coatings

Review
Edible and Functionalized
Films/Coatings—Performances and Perspectives
Sorin Marius Avramescu 1,2, * , Claudia Butean 3 , Claudia Valentina Popa 1,4 , Alina Ortan 1, * ,
Ionut Moraru 5 and Georgeta Temocico 1
1 University of Agronomic Science and Veterinary Medicine, 011464 Bucharest, Romania;
popa_vali2006@yahoo.com (C.V.P.); gtemocico@gmail.com (G.T.)
2 Department of Organic Chemistry, Biochemistry and Catalysis, Faculty of Chemistry,
University of Bucharest, 50663 Bucharest, Romania
3 Department of Chemistry and Biology, North University Centre of Baia Mare Technical University of
Cluj-Napoca, 430122 Cluj-Napoca, Romania; dee1168@yahoo.com
4 Medical-Military Scientific Research Center of Bucharest, Bucharest, 3-5, Institutul Medico-Militar street,
010919 Bucharest, Romania
5 SC Laboratoarele Medica SA, Frasinului 11, 075100 Otopeni, Romania; ionutmoraru@pro-natura.ro
* Correspondence: sorin.avramescu@g.unibuc.ro (S.M.A.); alina_ortan@hotmail.com (A.O.);
Tel.: +40-74-517-2435 (S.M.A.); +40-77-132-3216 (A.O.)




Received: 6 May 2020; Accepted: 11 July 2020; Published: 16 July 2020


Abstract: In recent years, food packaging has evolved from an inert and polluting waste that
remains after using the product toward an active item that can be consumed along with the food it
contains. Edible films and coatings represent a healthy alternative to classic food packaging. Therefore,
a significant number of studies have focused on the development of biodegradable enveloping materials
based on biopolymers. Animal and vegetal proteins, starch, and chitosan from different sources
have been used to prepare adequate packaging for perishable food. Moreover, these edible layers
have the ability to carry different active substances such as essential oils—plant extracts containing
polyphenols—which bring them considerable antioxidant and antimicrobial activity. This review
presents the latest updates on the use of edible films/coatings with different compositions with a
focus on natural compounds from plants, and it also includes an assessment of their mechanical
and physicochemical features. The plant compounds are essential in many cases for considerable
improvement of the organoleptic qualities of embedded food, since they protect the food from different
aggressive pathogens. Moreover, some of these useful compounds can be extracted from waste such
as pomace, peels etc., which contributes to the sustainable development of this industry.

Keywords: edible films; edible coatings; starch; chitosan; egg white protein; whey protein essential
oils; plant extracts; polyphenols

1. Introduction
The food market represents a large part of the global economy and is growing at an alert pace
every year. It is a common fact that food waste reaches around 1.3 billion tons each year [1]. An average
consumer from Europe or the USA produces about 95–115 kg/year of food waste, and the average
consumer from Africa and South/Southeast Asia produces about 6–11 kg/year [1]. These figures
represent the ready-to-eat products and do not include the waste generated in the cultivation of plants,
animal breeding, and processing steps. Considering the life cycle of food manufacturing, it can be
stated that this industry is the most polluting among anthropogenic activities. The main reason for food
waste production in less developed countries is the absence or poor infrastructure and technological
means for preservation or distribution [2]. The high carbon footprint, which accelerates global climate

Coatings 2020, 10, 687; doi:10.3390/coatings10070687 www.mdpi.com/journal/coatings

Coatings 2020, 10, 687 2 of 45

change and all sorts of environmental burdens, is another negative aspect of producing this particular
waste. In addition, human health is highly endangered by food spoilage; about 600 million people per
year become ill after consuming contaminated food [3]. Another important aspect is the food packaging,
which also largely contributes to worldwide pollution by generating a high amount of waste: plastic,
paper, metal, glass, etc. Especially plastics of any type and shape are under the scrutiny of public
concern due to their ubiquitous spread in all environmental compartments and contamination of
the ecosystems. Microplastic is considered an insidious type of plastic pollution [4]. In 2015, more than
300 million tons of plastic waste was generated, and 79% of this was deposited in landfills [5]. It is also
estimated that 46,000 plastic pieces are floating on each square mile of ocean, and because of these
materials, 1 million sea birds, 100,000 sea mammals, and a large amount of fish are killed. In addition,
some packaging contains harmful compounds (e.g., bisphenol A); therefore, a replacement of them is
beneficial for human health.
Consumer habits are difficult to change significantly; therefore, developing strategies for
diminishing this trend is indisputably necessary. A not-so-healthy alternative to increase the shelf life
of food is to introduce preservatives in their recipes. In some cases, this is an inevitable choice, but in
most situations, the types and amounts of preservatives exceed the safety rules. Another important
approach for addressing simultaneously the packaging load and the food squandering from related
industries is represented by edible films that can substitute for the classical packaging, concomitantly
with protecting for a longer time any kind of food from adulteration and subsequent disposal to waste.
Edible film alternatives are not new in the food industry; they represent a full and mature technology
with highly renowned results in terms of efficiency and versatility. In addition, some of the food
industry wastes can be successfully used in film preparation, bringing a supplementary reduction of
overall waste. Improvements and innovations in the last decade have expanded both the number of
applications and the quality of these products [6]. This review will center on the latest work on new
edible films and coatings with advanced features, with an emphasis on the utilization of plant extracts
containing polyphenols and some essential oil components for enhancing antimicrobial components.

2. Historical Consideration, Definition, Quality Parameters, and Technical Requirements of

Edible Films/Coatings
Edible films/coatings are essentially a food package for food. This type of wrapping was used
empirically, without scientific knowledge of their role, in food preservation from a long time ago
(being documented for 12 centuries in China). In 1922, the method of waxing fruits was introduced to
increase their commercial appeal.
As a definition, edible films or coatings are materials used for encapsulating different foods to
preserve their properties and could be consumed alongside the food. Films and coatings are sometimes
replaceable terms and fulfill the same role, but they represent different concepts. Films are prefabricated
by various methods and used to embed food, while coatings are applied on the food surface using a
viscous liquid. From the particularities of edible envelopments appear the incontestable advantages
of these materials: eco-friendly since they are consumed and, when it is not the case, biodegradable;
the solid waste amount is considerably reduced; the organoleptic properties of food are improved,
the nutritional properties are enhanced by adding adjuvants; they bring the possibility of wrapping
individual items avoiding bulk packaging issues, antimicrobial properties, and the possibility of using
a series of byproducts (e.g., agricultural waste) from different activities.
Edible coating and films are used in the same way as any other packaging to preserve the properties
of original food, and for that, they have to present some specific features:

• Generally Recognized as Safe (GRAS) labeling or GRAS/FS (some compounds are safe for use in
food industry; however, their concentrations is limited by currently used standards). In this respect,
the main goal is to avoid toxic, allergic, and/or non-assimilable components [7–15];
• Comply with good manufacturing practices (GMP) [16,17];
Coatings 2020, 10, 687 3 of 45

• Acknowledgment about a food additive for which a regulation was issued as a result of public
statements (e.g., petitions);
• Adequate mechanical properties for preventing the damaging of food surfaces during manipulation
from field to supermarket;
• Adherent to food surface;
• Agreeable taste or tasteless;
• Stability in time and especially avoidance of mold development;
• Reduce water depletion of the enveloped product;
• Maintain an adequate gas transfer, especially for oxygen and carbon dioxide and to avoid the loss
of components that are responsible for aroma, flavor, and nutritional value;
• Enhancement of structural properties;
• Appearance—overall presentation of the final product requires attaining classical package
performances in terms of design. Otherwise, the product can be rejected by consumers;
• Costs—in order to justify a major change in food industry paradigm, the costs need to be lower than
other approaches. In some areas, this technology has already attained maturity and the expenses
are considerably lower;
• Application devices/methods—distribution of film/coatings formulations on different products
in a consistent, efficient, and competitive manner is mandatory. The apparatus used for film
preparation must be similar with the classic apparatus. The method of application must be
compatible with current equipment;
• Manufacturing processes have to be easy and economically viable. Maintenance and cleaning of
the devices used has to be easy to perform.

The difficulties of complying with the above criteria represent the main reason for the small number
of companies in the beginning (around 10 in 1986) comparing with over 600 in 1996 [18]. The tremendous
progress in the field accomplished in recent years has led to an important increase of businesses related
to edible coatings, and the market for these products was evaluated in 2018 to attain around 727.6
million USD with the CAGR (Compound Annual Growth Rate) projected to be 6.2% [19]. The important
players in the field are Tate and Lyle, DuPont, Ashland, Koninklijke DSM N.V., Cargill Inc., Devro Plc,
Kerry Inc, Innoteq, Watson, Biofilm Limited, ODF Pharma, Proinec, MonoSol, Umang Pharmatech,
ProLiant Inc., American Casein Company, The Solae Company, Cargill, etc. There is still more room
for growth of this market, since there is a large part of the world (South America, Africa, South East
Asia, and Australia) where these products are scarcely extended [20].

3. Building Blocks of Edible Coatings/Films Formulations

Applying edible films on food is somehow a straightforward task, since numerous biomaterials
can be used with good results. Edible films contain four components: basic materials, plasticizers,
additives, and solvents.

3.1. Basic Materials

The basic materials generally used belong to three categories of natural products: proteins,
polysaccharides, and lipids. They come either from vegetal or animal sources and can be used in
the pristine state or after a preliminary modification.

3.1.1. Proteins
Proteins as raw materials are extracted from milk (casein, whey), other animal sources
(collagen, gelatin), corn (zein), wheat (gluten), soy, eggs (white egg), sorghum, pea, rice bran,
cottonseed, peanut, keratin, etc. Proteins are known as natural polymers composed of amino acids in
different proportions that vary from source to source.
 Coatings 2020, 10, 687 4 of 45

Coatings 2020, 10, x FOR PEER REVIEW 4 of 48

Protein film formation occurs through the denaturation of the initial material by heat, solvent
utilization, and pH. In general, biopolymers are not thermoplastic and are liquefied only by adding
some plasticizers. The absence of plasticizers leads to thermal degradation [21]. Temperatures above
some plasticizers. The absence of plasticizers leads to thermal degradation [21]. Temperatures
the glass transition (Tg) (Figure 1) undergo the transformation of proteins by molecules disaggregation,
above the glass transition (Tg ) (Figure 1) undergo the transformation of proteins by molecules
unfolding,disaggregation,
dissociation, and straightening;
unfolding, dissociation, andmolecules
straightening;are reuniting
molecules through
are reuniting otherother
through links
linkswhile the
material becomes soft, elastic,
while the material and
becomes configurable
soft, in any shape.
elastic, and configurable in anyThe cooled
shape. material
The cooled acquires
material acquiresimproved
properties and structure due to the new covalent, hydrogen, ionic links formed. Operational parameters
improved properties and structure due to the new covalent, hydrogen, ionic links formed. Operational
such as temperature, plasticizer (type and concentration), pH, etc. are important in film formation.
parameters such as temperature, plasticizer (type and concentration), pH, etc. are important in
film formation.

Figure 1. Variation of polymers state with temperature.

Figure 1. Variation of polymers state with temperature.
Some of the most used proteins are:
Some of the mosta protein
Gelatin, used proteins
obtainedare:through the hydrolysis of collagen and other insoluble proteins,
is an important candidate for films/coatings production [7,22–33]. It is mainly formed from proline,
Gelatin, a protein obtained through the hydrolysis of collagen and other insoluble proteins, is an
hydroxyproline, and glycine. Gelatin is used in different mixtures for preserving meat food and even
importantforcandidate
improving the forrecipes.
films/coatings
Krishna et al.production
developed films [7,22–33].
from fish It gelatin
is mainly formed
by extrusion from proline,
or casting
hydroxyproline, and glycerol
using 20–25% glycine. as Gelatin is used
a plasticizer in different
at 110–120 ◦ mixtures
C [34]. Extruded filmsfor preserving
were more flexiblemeat food and even
and thicker
for improving the with
compared recipes.
thoseKrishna
formed by etcasting.
al. developed
Fang et al.films from fish
used gelatin gelatin
coatings by extrusion
for reducing the salt or casting using
amount
20%–25% glycerol as a plasticizer at 110–120 °C [34]. Extruded films were more flexible[35].
in sausages, and as a result, preventing the risk of high salt concentration in food for human health and thicker
They prepared coating solutions from gelatin–NaCl solutions (1.5–15%) and applied them on non-salted
compared with those formed by casting. Fang et al. used gelatin coatings for reducing the salt amount
sausages. The original recipe of this product contain 2% NaCl. In terms of pH, color, texture analysis,
in sausages,
andand as a evaluation,
sensory result, preventing
the coatedthe andrisk
not of highproducts
coated salt concentration
are the same,in food
but for human
the coated producthealth [35].
They prepared
containcoating
overall 50% solutions
less salt. from gelatin–NaCl solutions (1.5%–15%) and applied them on non-
salted sausages. The original
Formulations containingrecipe of this product contain
gelatin–chitosan–extracts from grape2% seedNaCl.
with orIn terms
without of(apH,
nisin color, texture
polycyclic
analysis, and sensory evaluation, the coated and not coated products are the same, butfor
antibacterial peptide) [22] were used for coating fresh pork chunks to evaluate their usefulness the coated
preserving the freshness. The results obtained permitted establishing the influence and amount required
product contain overall 50% less salt.
for each component. Hence, the antioxidant properties increased significantly from simple mixtures to
Formulations
complex ones: containing
1% chitosangelatin–chitosan–extracts
< 1% chitosan + 3% gelatin < 1% from grape
chitosan + 3%seed with
gelatin orgrape
+ 0.5% without
seed nisin (a
polycyclicextract.
antibacterial
Zhang et al.peptide) [22] were
used a combination used (3%)
of gelatin for with
coating fresh porkincorporated
ZnO nanoparticles chunks toin ginger
evaluate their
usefulnessessential
for preserving the were
oil [31], which freshness.
appliedThe results
on beef obtained
patties. Some ofpermitted
the mechanicalestablishing
properties the influence and
(thickness
amount required for each component. Hence, the antioxidant properties increased significantly
and elongation) increased, while others (tensile strength and gel strength) decreased. Ginger essential oil from
reduces the water vapor permeability, and lipid oxidation can be avoided.
simple mixtures to complex ones: 1% chitosan < 1% chitosan + 3% gelatin < 1% chitosan + 3% gelatin +
Gelatin–turmeric combinations improved the elongation at break (EAB) of some edible films [36].
0.5% grape seed Liangextract. Zhang
et al., (2017) [37] et al. used
obtained a combination
a homogeneous of gelatin
film from sturgeon(3%) with ZnO
skin-derived nanoparticles
gelatin in
incorporated in ginger
combination withessential
esculine (aoil [31], which
coumarin glucoside)were applied onagents.
as antimicrobial beef patties.
The filmsSome of the
have good mechanical
tensile
propertiesstrength
(thickness
(TS), goodandwaterelongation) increased,
vapor permeability (WVP), while othersantioxidant
and higher (tensile activity
strength due and gel strength)
to esculine,
decreased. Ginger essential oil reduces the water vapor permeability, and lipid oxidation can be
but with an accentuated yellow color and lower elongation at break (EAB).
avoided.
Gelatin–turmeric combinations improved the elongation at break (EAB) of some edible films [36].
Liang et al., (2017) [37] obtained a homogeneous film from sturgeon skin-derived gelatin in
combination with esculine (a coumarin glucoside) as antimicrobial agents. The films have good tensile
strength (TS), good water vapor permeability (WVP), and higher antioxidant activity due to esculine,
Coatings 2020, 10, 687 5 of 45

Mahdu et al., measured the moisture sorption isotherms of sugarcane jaggery portions coated
with different edible layers based on whey, gluten, gelatin, zein, and arabic gum at different
concentrations (0.5%, 1.5%, and 2.5%) [38], and they applied different models to the experimental data.
The Guggenheim–Anderson–de Boer (GAB) model was the best fitting one, and gelatin and gluten gave
the best results regarding moisture prevention.
Casein represents a family of phosphoproteins (αS1, αS2, β, κ) that can be found in different
proportions in human or animal milk. A complex film produced from casein, alginate, pectin, glycerol,
and probiotic Enterococcus faecium Rp1 was developed by Namratha et al., [39]. This film was tested
and showed important antimicrobial and antioxidant properties and good physicochemical features
for about 60 days, while E. faecium Rp1 was still viable. Regarding the efficacy of films incorporating
probiotics against S. aureus, E. coli, and S. flexneri, there was a low survival rate of these bacteria:
20%, 5%, and 10% respectively. In contrast, in the case of probiotic-free films, the survival rate was
about 90% for all three microorganisms. The biopolymer coating for processed apples was performed
by Volpe et al. [40] using chitosan–caseinate coatings, which increased the shelf life by four days,
and the fruit properties were thoroughly preserved. Pella et al., [24] studied the effect on guava fruits
of films based on cassava starch, casein, and gelatin with sorbitol (30% w/w) as a plasticizer. The films
were prepared using a factorial design (23 , three central points). The fruits remain unchanged for
nine days, which could also be observed from harvest index (HI), titratable acidity (TA), and vitamin
C measurements. Vitamin C values were initially 98.04%, and after 9 days, they were 85.42% for
non-coated fruit and 98.24% for coated products.
Whey is a by-product of cheese manufacturing that consists of the liquid remaining after casein
coagulates at a pH value of 4.6 and around 20 ◦ C. Whey proteins present hydrophobic, charged/polar
amino acids evenly distributed along the chain in contrast to casein proteins. Therefore, the whey
hydrophobic groups are hidden within molecules. These proteins can be used in different commercial
purposes, and “edible films” is an important direction with good results, especially since large
amounts of dairy products are used constantly. Whey is much more used in the edible film/coatings
field, probably because it is a by-product that in most cases needs disposal, since the global
cheese production is 24 million tons/year and consequently 21.6 million tons/year of whey [41].
This by-product is ecologically difficult to manage, so the edible films are a good alternative for its
use [42–55]. As with casein, whey has to be molded along with several other adjuvants such as
chitosan and alginate [42], whey protein concentrate/wheat cross-linked starch composite film [43],
Iprovit Bacterial Milk–Yogurt Starter™–sodium alginate–whey–glycerol [52], the microorganism
Bifidobacterium animalis subsp. Lactis BB-12–whey protein isolate–alginate [44], whey–glycerol
(30–60% w/w of whey) [45], maltodextrin–Arabic gum–whey [53], green tea/rosemary extract–whey [46],
whey–glycerol (5–15% w/w)—rosemary and thyme extracts [47], etc. It was found that the produced films
act as a barrier for different microorganisms [42,46,50–52,54] and present improved physicochemical
properties [42,43,53,55].
Egg white is a complex mixture of globular proteins [56]: ovomucin, ovotransferrin, ovalbumin,
ovomucoid, lysozyme, G2 globulin, G3 globulin, and avidin. The content of the main constituents
from total proteins are ovalbumin—54%, ovotransferrin—12%, and ovomucoid—11%. For edible
film preparation, the –SH groups, which exist only in ovalbumin and the S–S bonds encountered in
lysozyme, ovomucoid, and ovotransferrin are very important in reticulation processes. Mixtures of
pullulan (Pu)–egg white (EW)–glycerin (Gly) [57] lead to the formation of edible films with superior
properties due to hydrogen bond rearrangements. These changes were assessed by Fourier-transform
infrared spectroscopy (Nicolet 380 FT-IR Spectrometer, Thermo Fisher Scientific, Waltham, MA, USA)),
XRD (D8 Advance, Bruker AXS, Karlsruhe, Germany), secondary structures, and free amino group
analysis. The highest values of the TS (329.48 MPa) and EAB (10.33%) were obtained for the Pu:EW = 1:1
ratio. Increased TS can also be obtained by adding oleic acid probably due to the increased negative
charges and exposure to –SH groups [58], while the use of dialdehyde starch increases water solubility
and mechanical strength [59]. Alkaline pH (10–12) is required for homogeneous films [60], while
Coatings 2020, 10, 687 6 of 45

UV radiations increase the reticulation of polymer chains, resulting in a low solubility and improved
mechanical strength [61]. Sothornvit et al., [62] prepared three types of edible films from soy,
egg white proteins, and whey proteins, respectively. Whey films presented a better water vapor
permeability compared with egg white films. In another paper [63], edible films were prepared using
egg white–succinylated casein with and without transglutaminase (TGase) treatment. Films treated
with TGase (concentrations of 15 U/g protein) showed maximum mechanical strength and lower
values of WVP. Another interesting combination for edible film preparation was obtained using
egg white and κ-carrageenan [64]. When the percentage of egg white increased, the EAB and light
transmission improved to 10.85% and 53.3%, respectively. In addition, in another paper [65], egg
white lysozyme was incorporated into zein–glycerin films to obtain food packaging with antimicrobial
properties against B. subtilis and L. plantarum. Moreover, the films containing in addition disodium salt
of ethylenediaminetetraacetic acid (EDTA) are efficient against E. Coli. Its antimicrobial feature
is manifested even at low lysozyme concentrations. Aguilar et al. [66] produced edible films
and microparticles by ionic gelation using pectin–alginate blend followed by electrostatically coating
with whey or egg white proteins. A thorough characterization of films and particles was made in terms
of calcium content, thickness, adsorbed protein, moisture, WVP, structure, and mechanical properties.
As the authors suggest, the difficult part of the synthesis was obtaining a homogeneous drying of
the films; this aspect require further studies.

3.1.2. Polysaccharides
Polysaccharides represent, besides proteins, another important pillar of the biological kingdom.
These compounds are ubiquitous and therefore compatible with the natural products that are supposed
to be protected by edible films/coatings. Moreover, the possibility of chemically modifying this natural
and biodegradable polysaccharide increases significantly the range of compounds eligible for biocoatings.
The main polysaccharides used to produce edible barriers are starch (natural or modified) [67], modified
cellulose (carboxy methylcellulose [68], hydroxypropylcellulose [69], hydroxypropylmethylcellulose [70]),
inulin (Jerusalem artichoke) [44], sodium alginate (brown seaweed) [71], chitosan (crustacean shells
deacetylation) [72], pectin [7,73], carrageenan [64], pullulan [74], gellan [75], xanthan [76], etc.
Starch (Figure 2) is an abundant natural compound that is present in all plant components
(stem, seeds, fruits, roots, etc.). It is the plant “battery” since it represents energy storage in chemical
form, but also the main energy source for animals and humans (60–70% of the human caloric
intake comes from starch). Starch consists of two different polysaccharides: amylose composed of
D-glucose residues with α-(1→4) linkages—linear and amylopectin formed and α-(1→4) linkages
and approximately 6% α-(1→6) linkages as branches from the parent molecule. Both are comprised
of water-insoluble granules with different shape, morphology, and crystallinity for different sources.
Starch possesses thermoplastic characteristics in the presence of plasticizers, high temperatures,
and mechanical pressing. In this respect, starch is similar to other synthetic polymers; hence,
the operation implemented to other polymers can be applied to starch also. Therefore, to give starch a
new shape, a thermomechanical process is needed (extrusion, injection, kneading, molding, casting,
all in the presence of heat, water, and appropriate plasticizers). A novel and efficient approach [77] to
obtain thermoplastic starch consists of using sodium hexametaphosphate (SHMP)/polyvinyl alcohol
fibers (PVAF) as cross-linking agents and the following procedure: SHMP and PVAF are mixed in
solution, starch and glycerol were added to solution, the mixture was submitted to extrusion, granules
were obtained, and granules were molded in films. In this process, SHMP produces cross-linking
between starch molecules and PVAF.
Coatings 2020, 10, x FOR PEER REVIEW 7 of 48
Coatings 2020, 10, 687 7 of 45

Figure 2. Starch structure emphasizing the two main components: amylose and amylopectin.
Figure 2. Starch structure emphasizing the two main components: amylose and amylopectin.
In addition, the degree of polymerization varies significantly among sources [78–92]. There are
some methods for fractionation, separation, and chemical modification to comply with edible
In addition, the degree of polymerization varies significantly among sources [78–92]. There are
films/coatings formulation. There are several advantages to use starch, such as its low cost,
some methods for fractionation, separation, and chemical modification to comply with edible
large availability, non-toxic nature, and versatility in processing (as flexible as polyethylene and rigid as
films/coatings formulation. There are several advantages to use starch, such as its low cost, large
polystyrene), but it also has disadvantages. For example, raw starch is brittle, too hygroscopic, and has
availability, non-toxic nature, and versatility in processing (as flexible as polyethylene and rigid as
low mechanical properties. To eliminate these drawbacks, plasticizers can be used, and different
polystyrene), but it also has disadvantages. For example, raw starch is brittle, too hygroscopic, and has
sources of starch can be taken into consideration.
low mechanical properties. To eliminate these drawbacks, plasticizers can be used, and different
Andean blueberries [93] were protected using starch–glycerol films, the starch source being
sources of starch can be taken into consideration.
Colombian native potatoes: pacha negra, mora, and alcarrosa. For all three types of starch, the reduction
Andean blueberries [93] were protected using starch–glycerol films, the starch source being
in gas exchange was found to be approximately 27%. Corn starch, with hydroxypropyl methylcellulose,
Colombian native potatoes: pacha negra, mora, and alcarrosa. For all three types of starch, the reduction
Uncaria gambir extract, and glycerol were used as the main ingredients for edible film preparation [94].
in gas exchange was found to be approximately 27%. Corn starch, with hydroxypropyl methylcellulose,
To assess the influence of gambir extract to edible film parameters, an experimental design and statistical
Uncaria gambir extract, and glycerol were used as the main ingredients for edible film preparation [94].
analysis were used. It was observed that the optimal operational parameters are a 40% concentration
To assess the influence of gambir extract to edible film parameters, an experimental design and
of Uncaria analysis
statistical gambir and 1000used.
were rpm It centrifugation
was observed forthat
separation.
the optimal operational parameters are a 40%
Other authors prepared films based on arrowroot starch–cranberry powder (0–55%) [95].
concentration of Uncaria gambir and 1000 rpm centrifugation for separation.
Arrowroot authors arundinaceae
Other (Maranta prepared films L.) was selected
based due to it containing
on arrowroot good starch
starch–cranberry properties:
powder (0–55%)high [95].
amylose content, digestibility, and gelling ability. Cranberry powder was selected due to its large
Arrowroot (Maranta arundinaceae L.) was selected due to it containing good starch properties: high
amount
amylose of anthocyanins,
content, proanthocyanidins,
digestibility, and gelling ability.organic acids, glycosides,
Cranberry powder was flavonoids,
selectedphenolic
due to itsacids,
large
and ascorbic
amount acids, whichproanthocyanidins,
of anthocyanins, confer remarkable antioxidant
organic acids, properties
glycosides,to prepared
flavonoids, films. Despite
phenolic their
acids, and
beneficial activity,which
ascorbic acids, increasing the remarkable
confer cranberry content to over 45%
antioxidant leads to to
properties brittle, rough, films.
prepared and irregular
Despite films.
their
In an activity,
beneficial experimental design
increasing the[67] with two
cranberry factors—starch
content to over 45% type (cassava,
leads arrowroot,
to brittle, and irregular
rough, and canna)
and starch
films. percentage of (3%, 4%, 5%) (v/v)—the quality of prepared edible films was assessed. Sorbitol
was used
In anas a plasticizer.design
experimental In terms
[67]of tensile
with two strength, Canna type
factors—starch edulis(cassava,
showed arrowroot,
higher values,
and while
canna)for and
elongation, arrowroot
starch percentage gave
of (3%, better
4%, 5%) results.
(v/v)—theIt isquality
not surprising,
of preparedsince thesefilms
edible two was
parameters areSorbitol
assessed. inversely was
proportional. For another
used as a plasticizer. important
In terms parameter,
of tensile WVP,
strength, the authors
Canna found lower
edulis showed highervalues in while
values, case offor
arrowroot-type starch for all experimental concentrations. Therefore, in this paper, it was shown that
the starch type is paramount for the film quality.
arrowroot-type starch for all experimental concentrations. Therefore, in this paper, it was shown that
the starch type is paramount for the film quality.
Another interesting starch provenience is elephant foot yam (EFY), which is one of the natural rich
sources of starch. Nagar et al. used starch from this tropical tuber crop to obtain edible
Coatings 2020, 10, 687 8 of 45
films in
conjunction with hydrocolloids–xanthan (XG) and/or agar–agar (AA) [96]. It was found that the WVP
values decreased with increasing concentrations of AA and XG. The hydrophilic nature of
Another interesting starch provenience is elephant foot yam (EFY), which is one of the natural
hydrocolloids facilitates water molecules to bond with polymer chains and form microcavities. Hence
rich sources of starch. Nagar et al. used starch from this tropical tuber crop to obtain edible films in
, atdiminished content of agar–agar (AA) and /or xanthan (XG) the films present higher WVP (suitable
conjunction with hydrocolloids–xanthan (XG) and/or agar–agar (AA) [96]. It was found that the WVP
forvalues
packaging where moisture is needed) and for higher AA and /or XG content the films
decreased with increasing concentrations of AA and XG. The hydrophilic nature of hydrocolloids
presentreduced
facilitates waterWVP (when
molecules to sealing
bond with is required).
polymer chains and form microcavities. Hence, atdiminished
The protection of Huangguan
content of agar–agar (AA) and /or xanthan (XG) pear (Pyrus pyrifolia),
the films present which is a (suitable
higher WVP new species with superior
for packaging
properties (larger,issmoother,
where moisture needed) and sweeter)
for higher was
AAmade
and /orthrough a new
XG content theapproach first reported
films presentreduced WVP in(when
the literature:
edible
sealingfilms prepared from cross-linked (with adipic acid) cassava starch reinforced by starch
is required).
nanocrystals (SNCs)of
The protection [97]. The authors
Huangguan prepared
pear (Pyrus the films
pyrifolia), whichfor
is aparameter
new speciestesting, and the
with superior same solutions
properties
were used for coatings. The study involved also the impact of grading operations previous
(larger, smoother, sweeter) was made through a new approach first reported in the literature: to coating,
edible
since these fruits are very sensitive. The results showed that coatings containing 6% SNC presented the
films prepared from cross-linked (with adipic acid) cassava starch reinforced by starch nanocrystals
(SNCs) [97]. The authors prepared the films for parameter testing, and the same solutions were used
best performance, and the fruits were significantly protected, especially when a graded process occurs
for coatings. The study involved also the impact of grading operations previous to coating, since these
after coating.
fruits are very sensitive. The results showed that coatings containing 6% SNC presented the best
Chitosan (Figure 3) is a well-known polysaccharide derived from chitin with countless uses due
performance, and the fruits were significantly protected, especially when a graded process occurs
to its properties
after coating. [98–100]: it is a natural linear polymer that is non-toxic and therefore safe for the food
industry, biodegradable,
Chitosan (Figure 3) antitumoral,
is a well-known fungistatic, hemostatic,
polysaccharide derivedanticholesteremic, antioxidant,
from chitin with countless uses antacid,
colon
duetargeting, analgesic,
to its properties etc. Chitosan
[98–100]: is mainly
it is a natural insoluble
linear polymer thatiniswater, but and
non-toxic it becomes
thereforesoluble
safe forin acidic
solutions
the food(acetic acid,
industry, formic acid,antitumoral,
biodegradable, etc.). If the deacetylation degree exceeds
fungistatic, hemostatic, 50%, the solubility
anticholesteremic, antioxidant, increases,
too.antacid,
Whencolon chitosan is analgesic,
targeting, introduced etc. in the acidic
Chitosan is mainlymedia, the inchain-linked
insoluble amino soluble
water, but it becomes groups in become
protonated, and the
acidic solutions chitosan
(acetic shiftsacid,
acid, formic into a cationic
etc.). state. Hence,
If the deacetylation positive
degree exceedscharged
50%, thechitosan
solubilityacquires
antimicrobial properties since it interacts with the negative surface of cell membranes,
increases, too. When chitosan is introduced in the acidic media, the chain-linked amino groups becomeleading to
protonated, and
bacteria deactivation. the chitosan shifts into a cationic state. Hence, positive charged chitosan acquires
antimicrobial properties since it interacts with the negative surface of cell membranes, leading to
bacteria deactivation.

Figure 3. Comparison among cellulose, chitin, and chitosan structures.

Figure 3. Comparison among cellulose, chitin, and chitosan structures.
The diverse features of chitosan make it a good candidate for the preparation of edible coatings
andThe diverse
films, solelyfeatures of chitosan
or in various make itChitosan
formulations. a good candidate
edible film for the preparation
coatings of edible coatings
were also investigated
and films, solely or in various formulations. Chitosan edible film coatings
for the protection of food qualities of sweet cherry (Prunus avium L.) [101]. wereparameters
Several also investigated
of for
sweet cherry such as its total carbohydrate content, titratable acidity, total soluble solids, water activity,
the protection of food qualities of sweet cherry (Prunus avium L.) [101]. Several parameters of sweet
and pH were preserved using chitosan coatings. The authors used four types of chitosan: two
cherry such as its total carbohydrate content, titratable acidity, total soluble solids, water activity, and
prepared by themselves from shrimp wastes with different deacetylation degrees and two commercial
pHones.
wereThepreserved using chitosan coatings. The authors used four types of chitosan: two prepared by
chitosan prepared by reaction with 40% sodium hydroxide at 120 ◦ C for 300 min (CH-1,
themselves from
deacetylation shrimp
78.2%, wastes
182 kDa) with different
provided deacetylation
a longer shelf degrees
life for studied fruits.and two commercial ones. The
chitosan prepared
Pectin by reaction
is an important with 40% sodium
polysaccharide hydroxide
considering at 120 °C
the structural rolefor
in300 min
plant (CH-1,
tissues. deacetylation
Pectin’s
78.2%, 182 kDa)
biological provided
function a longerthe
is to reticulate shelf life for
cellulose studied
and fruits. fibers, producing a more resistant
hemicellulose
structure. It is found in almost all plants in different concentrations mainly in the middle lamella layer
between cells (Figure 4). Pectin is a generic name for a family of polymers which differ in terms of
molecular weight, chemical configuration, and types and abundance of monosaccharide subunits:
 Pectin
Pectin is anis animportant
importantpolysaccharide
polysaccharide considering
considering the thestructural
structuralrole role
in in plant
plant tissues.
tissues. Pectin’s
Pectin’s
biological
biologicalfunction
function is isto toreticulate
reticulatethethecellulose and hemicellulose
cellulose and hemicellulosefibers,
fibers, producing
producing a more
a more resistant
resistant
structure. It isItfound
structure. is found in inalmost
almostall allplants
plantsinin different concentrations
different concentrations mainly
mainly in the
in the middle
middle lamella
lamella layerlayer
between
betweencells (Figure
cells (Figure 4).4).Pectin
Pectinisisaageneric
generic name
name for for aafamily
familyofofpolymers
polymers which
which differ
differ in terms
in terms of of
Coatings 2020, 10, 687 9 of 45
molecular
molecular weight,
weight, chemical
chemicalconfiguration,
configuration, and types types andandabundance
abundanceof of monosaccharide
monosaccharide subunits:
subunits:
(rhamnogalacturonan I, rhamnogalacturonan II, and homogalacturonan)
(rhamnogalacturonan I, rhamnogalacturonan II, and homogalacturonan) [102]. In a simply way, pectin [102]. In a simply way, pectin
is a ischain
a chain of alpha -1,4,-linked galacturonic acid
acid subunits
subunits(Figure
(Figure5) 5)that
(rhamnogalacturonan I, rhamnogalacturonan II, and homogalacturonan) [102]. have an an
In a simply“accordion-like”
way, pectin
of alpha -1,4,-linked galacturonic that have “accordion-like”
is
conformationa chain of
which alpha -1,4,-linked
result in galacturonic
molecules with acid
extensiblesubunits (Figure 5)
characteristics. that have an “accordion-like”
conformation which result
conformation which in molecules
result with
in molecules extensible
with extensible characteristics.
characteristics.

Figure 4. Structure of the plant tissue and the zone where the middle lamella is situated.
Figure 4. Structure of the plant tissue and the zone where the middle lamella is situated.
Figure 4. Structure of the plant tissue and the zone where the middle lamella is situated.

Figure 5. Structure
Figure ofofgalacturonic
5. Structure galacturonic acid andpectin.
acid and pectin.
Galacturonic acid is a sugar acid that is a product from the oxidation of D-galactose. The acid groups
Galacturonic acid is a sugar acid that is a product from the oxidation of D-galactose. The acid
along the chain are esterified with methoxy groups in different proportions. In addition, some of
groupsthealong the chain Figure 5. Structure of galacturonic acid and pectin.
hydroxy groupsare areesterified
acetylated.with methoxy
The chemistry groups
of pectinin different
is quite proportions.
complex In addition,
and possesses numeroussome
of the hydroxy
properties, groups
but theare mainacetylated. The chemistry
uses are gelling, of pectin
thickening, and as aisstabilizer
quite complex
agent inandfoodpossesses numerous
[73,102–104].
Galacturonic
properties, Pectin type E440i (contain different levels of methyl esters on polygalacturonic acid chain)The acid
but acid
the is
main a sugar
uses are acid
gelling,that is a
thickening,product
and from
as a the oxidation
stabilizer agent in of D-galactose.
food [73,102–104].
groups along
Pectin the
typechain
and E440ii E440i
(containare esterified
(contain
amides groupswith
different methoxy
levels
along groups
of methyl
with methyl in different
esters
esters areproportions.
on polygalacturonic
groups) largely usedacid Inchain)
in addition,
the food and Esome
of the hydroxy
440ii (contain groups
industry. amidesare
Regarding acetylated.
groupsthe along with
safety of The chemistry
this methyl esters
compound, of pectin
the groupsis) are
European quite complex
largely
Food Safety usedand possesses
in the
Authority numerous
food industry.
Panel agrees
Regarding
with the
the safety
fact thatof this
this compound,
compound the
lowers European
the Food
cholesterol Safety
level of Authority
properties, but the main uses are gelling, thickening, and as a stabilizer agent in food [73,102–104].
adults if the Panel
daily agrees
dose with
reaches the
6 g fact
that this type
Pectin compound
(for
E440i lowers
infants, there are
(contain
nothedifferent
cholesterol
data available). level of
levels of methyl
adults if esters
the dailyondose reaches 6 g (foracid
polygalacturonic infants, there
chain) and E
Due to the significant role in plant biology and already being an important ingredient in the food
are no data
440ii (contain available).
amides
industry, pectingroups
is a good along withformethyl
candidate esters
edible films groups ) are largely used in the food industry.
coatings/preparation.
Due to the significant role in plant biology and already being an important ingredient in the food
Regarding theNatural
safety sources
of thisof compound, the European
pectin with different extractionFood
yieldSafety Authority
are represented Panel agrees
by different with the fact
agricultural
industry, pectin is a good candidate for edible films coatings/preparation.
that this compound
wastes: apple lowers
pomace the(4.2–19.8%),
cholesterol level
citrus peelof(13.4–37.52%),
adults if thesugardailybeet
dose reaches
pulp 6 g (for
(23–24.87%), infants, there
tomato
Natural sources of pectin with differentwatermelon
extraction yield are represented by different agricultural
are no dataapple
available).
waste
wastes:acidic
(7.55–32.6%),
pomace
mango
(4.2%–19.8%),
peel (17.15%), rinds (19–21%), etc. Extraction is made in hot
(pH = 1.5–2) water solutioncitrusfollowed peelby(13.4%–37.52%),
vacuum concentration sugarand
beet pulp (23%–24.87%),
precipitation with differenttomato
Due to
waste the significant
(7.55%–32.6%), mangorolepeel
in plant biology
(17.15%), and already
watermelon rinds being an important
(19%–21%), etc. ingredient
Extraction is made ininthe
hotfood
agents (mostly alcohols). Microwave, ultrasound, and supercritical-assisted extraction processes are
industry,
acidic pectin ispectin
(pH =for1.5–2)
used a good
water candidate
solution
separation for edible
[105].followed byfilms
vacuum coatings/preparation.
concentration and precipitation with different
Natural sources ofetpectin
Tumbarski with
al., used different
celery-based extraction
pectin (1%) aloneyield
or in are represented
combination by different
with bacteriocin agricultural
(Bacillus
wastes: apple pomace (4.2%–19.8%),
methylotrophicus citrusapeel
BM47) for preparing (13.4%–37.52%),
coating sugar beet[73].
for blackberries preservation pulp (23%–24.87%),
Comparing with a tomato
waste (7.55%–32.6%), mango peel (17.15%), watermelon rinds (19%–21%), etc. Extraction is made in hot
acidic (pH = 1.5–2) water solution followed by vacuum concentration and precipitation with different
agents (mostly alcohols). Microwave, ultrasound, and supercritical-assisted extraction processes are
used for pectin separation [105].
Tumbarski et al., used celery-based pectin (1%) alone or in combination with bacteriocin (Bacillus
methylotrophicus BM47) for preparing a coating for blackberries preservation [73]. Comparing
Coatings 2020, 10, 687 10 of 45
with a
control (not-coated fruits), the coating preserved all the initial properties of the blackberries (loss of
weight, decay, total soluble solids, titratable acidity, pH, organic acids, sugars, total phenolic content,
control (not-coated
total anthocyanins, andfruits), the coating
antioxidant preserved
activity). all theacid
Ascorbic initial
is properties
one of theofmost
the blackberries
important (loss of
parameters,
weight, decay, total soluble solids, titratable acidity, pH, organic acids, sugars, total phenolic content,
and it remains at the same level compared to the initial moment for 16 days (57.5 mg/100 g for the
total anthocyanins, and antioxidant activity). Ascorbic acid is one of the most important parameters,
pectin-based coating and 58.8 mg/100 g for pectin and bacteriocin).
and it remains at the same level compared to the initial moment for 16 days (57.5 mg/100 g for
Ngo et al., conducted a study in which they used pectin and nanochitosan (in different ratios) and
the pectin-based coating and 58.8 mg/100 g for pectin and bacteriocin).
tried to elucidate
Ngo et al.,the influence
conducted of each
a study component
in which and
they used ratioand
pectin between them on
nanochitosan the mechanical
(in different ratios) and
barrier
andproperties. The results
tried to elucidate showedof
the influence that a ratio
each of 50:50
component andobtained the best
ratio between results:
them on thetensile strength of
mechanical
8.96 and
MPa, water solubility decrease to 37.5%, water vapor permeability (WVP)
barrier properties. The results showed that a ratio of 50:50 obtained the best results: tensile to 0.2052
g·mm/m 2 ·day·kPa,
strength of 8.96and oxygen
MPa, waterpermeability (OP) to to
solubility decrease 47.67 cc·mm/m
37.5%, 2 ·day [106].
water vapor permeability (WVP) to
Yeddes et al., prepared gelatin–chitosan–pectin edible films improved with rosemary essential oil
0.2052 g·mm/m 2 ·day·kPa, and oxygen permeability (OP) to 47.67 cc·mm/m2 ·day [106].

[7]. The preparation

Yeddes et al.,process
prepared was optimized using a edible
gelatin–chitosan–pectin Doehlert
filmsmatrix
improved(an with
advanced
rosemaryresponse
essentialsurface
methodology superior to other design, such as composite central and Box–Behnken) [107]. Hence, the
oil [7]. The preparation process was optimized using a Doehlert matrix (an advanced response surface
methodology superior to other design, such as composite central and Box–Behnken) [107]. Hence,
mechanical and textural properties were improved, and the optimal composition was found to be 10%
the mechanical and textural properties were improved, and the optimal composition was found to
chitosan, 24.3% gelatin, 65.2% glycerol, and 0.5% pectin, while the antioxidant activity was enhanced
be 10% chitosan, 24.3% gelatin, 65.2% glycerol, and 0.5% pectin, while the antioxidant activity was
for the addition of 1.996 mg/g rosemary oil.
enhanced for the addition of 1.996 mg/g rosemary oil.

3.1.3. 3.1.3.
Lipids, Waxes,
Lipids, andand
Waxes, Resins
Resins

Lipids (saturated,
Lipids monounsaturated,
(saturated, monounsaturated, polyunsaturated
polyunsaturatedfatfatacids)
acids) [108],
[108], waxes [68] (Figure
waxes [68] (Figure6),
6), and
resinsand
(wood
resinsrosin,
(woodshellac) [109] [109]
rosin, shellac) represent another
represent important
another importantarea
areaof
of edible coatings/films
edible coatings/films either as
either
primary components
as primary or as or
components plasticizers. Shellac
as plasticizers. is is
Shellac produced
producedbyby insects Lacciferlacca
insects Laccifer lacca
andand contains a
contains
a complex mixture of aliphatic alicyclic hydroxy acid polymers i.e., aleuritic, bucolic, shellolic,
complex mixture of aliphatic alicyclic hydroxy acid polymers i.e., aleuritic, bucolic, shellolic, and jalaric
and jalaric acids).
acids).

Figure 6. Main
Figure typestypes
6. Main of compounds
of compounds included
includedin in
waxes: hydrocarbons
waxes: hydrocarbons(n-alkanes where nn== 22–36),
(n-alkanes where 22–36), fatty
alcohols
fatty(R length(Rislength
alcohols 12–34iscarbon atoms),
12–34 carbon fattyfatty
atoms), acids (R length
acids is is12–34
(R length 12–34carbon), long-chain
carbon), long-chain esters (R1
esters
(R and R =
and R2 =1 10–202 carbon atoms in length).
10–20 carbon atoms in length).

3.2. Plasticizers
3.2. Plasticizers
Plasticizer choices encompass a large range of molecules: water, xylitol, mannitol, propylene glycol,
Plasticizer choices
glycerol, sorbitol, encompass
polyethylene a large
glycol, range
sucrose, of molecules:
polypropylene water,
glycol, xylitol,
triethylene mannitol,
glycol, propylene
ethylene glycol, cornglycol,
glycerol,
syrup,sorbitol,
1.4 butanepolyethylene
diol, 1,6 hexaneglycol, sucrose,
diol, triacetin, polypropylene
glucose, glycol,
urea, diethanolamine, triethylene
dibutyl phthalate,glycol, ethylene
tributyrate,
glycol, corn citrate,
tributyl syrup,diethyl
1.4 butane
tartrate,diol, 1,6 hexane
acetylated diol, triacetin,
monoglycerides, glucose,
fatty acids urea, lauric,
(oleic, stearic, diethanolamine, dibutyl
etc.), lactic acid,
phthalate, tributyrate,
deep eutectic solventstributyl
[110], etc.citrate,
Some ofdiethyl
them aretartrate,
removed andacetylated
others aremonoglycerides, fatty acids (oleic,
introduced in the manufacturing
stearic, lauric, etc.), lactic acid, deep eutectic solvents [110], etc. Some of them are removed
process in accordance with updated food regulations [111,112]. Plasticizers are generally requiredand in aothers
are introduced in the manufacturing process in accordance with updated food regulations [111,112].
proportion of 10% to 65% as a function of polymer rigidity. They improve the process of polymer formation,
and for a final product (films or coatings), these molecules allow a larger temperature range for their use,
Plasticizers are generally required in a proportion of 10% to 65% as a function of polymer rigidity. They
impart flexibility, lower the brittleness, and increase the hardness of the film. In addition, the main role of
Coatings 2020, 10, x FOR PEER REVIEW 11 of 48

improve the process of polymer formation, and for a final product (films or coatings), these molecules
allow a larger temperature range for their use, impart flexibility, lower the brittleness, and increase the
Coatings 2020, 10, 687 11 of 45
hardness of the film. In addition, the main role of these compounds is to diminish the intermolecular
forces between polymer chains (Figure 7), which increases the free volume and movement of the
these compounds is to diminish the intermolecular forces between polymer chains (Figure 7), which increases
polymeric chains.
the free volume and movement of the polymeric chains.

Figure 7. Activity of plasticizer between protein chains.

Figure 7. Activity of plasticizer between protein chains.
As for the classification of these molecules, there are two types of plasticizers [113]: internal
As for
andthe classification
external, of these molecules,
which is terminology taken from polymerthere science.
are twoInternal
typesplasticizers
of plasticizers [113]: internal and
(co-polymers
or compounds that interact with polymer chain) increase the steric hindrance of chains followed
external, bywhich is terminology taken from polymer science. Internal plasticizers (co-polymers or
increased free volume and flexibility. As a consequence, the glass transition temperature (Tg )
compounds that modulus
and elastic interact(EM)with polymer
decrease, whilechain)
the whole increase
polymer the steric
become hindrance
softer. of chains
External plasticizers do followed by
increasednotfree volume
react and flexibility.
with polymer chains; theyAs actaon
consequence,
protein chains the glass transition
by solvation temperature
and lubrication, (Tg) and elastic
and also as
modulus (EM) decrease, while the whole polymer become softer. External plasticizers do not react with
agents to lower the glass transition temperature and increase free volume. The most important features
of plasticizers are compatibility, efficiency, and permanence. Compatibility means that plasticizers
polymer have
chains; they act on protein chains by solvation and lubrication, and also as agents to lower the
a similar chemical structure, and they are also low volatility, non-harmful, and free of aromas.
glass transition
Efficiencytemperature
is attained if theand increase
plasticizer freeits
fulfills volume. The concentration
role at lower most important features
and presents of plasticizers are
a higher
compatibility,
diffusionefficiency,
capacity intoand permanence.
the polymer matrix. WeCompatibility
encounter in this means that plasticizers
matter a delicate balance betweenhave a similar
chemical structure, and they are also low volatility, non-harmful, and free of aromas.
diffusivity and volatility; therefore, the size of the molecules involved is crucial. The permanence of Efficiency is
plasticizers is also related to their molecule size, but likewise, polarity and hydrogen bonds play an
attained if the plasticizer fulfills its role at lower concentration and presents a higher diffusion capacity
important role. The correlation of plasticizers amount and type with Tg variation is less easy to obtain
into the for
polymer matrix. since
natural polymers, We biopolymer
encounterchains in this matter
are less mobile a due
delicate
to chainbalance between
interactions, diffusivity and
hydrogen
volatility;bonding,
therefore,ionic the size of and
interactions, theS–S
molecules involved
bonds. Plasticizers is crucial.
generally The permanence
bring superior of plasticizers is also
mechanical properties
related to their molecule size, but likewise, polarity and hydrogen bonds play an important role. The
to the mixture, but their hygroscopic properties (for most of them) increase the water vapor permeability
and decrease the blocking properties of coatings for gases, moisture, and aroma compounds.
correlation of plasticizers amount and type with Tg variation is less easy to obtain for natural polymers,
since biopolymer chains are less mobile due to chain interactions, hydrogen bonding, ionic interactions,
3.3. Additives
and S–S bonds. Plasticizers
Additives play manygenerally bring
important roles superior
in the mechanical
film/coatings matrix andproperties
include variousto compounds
the mixture, but their
hygroscopic properties
such as (for
antioxidants, most of them)
nutraceuticals, increase antimicrobials,
pharmaceuticals, the water vapor permeability
nutrients, and decrease the
flavors, fragrances,
blocking properties of coatings for gases, moisture, and aroma compounds.
colors, probiotics, emulsifiers, cross-linking agents, browning inhibitors [114–116], etc.
Antimicrobial molecules are used in order to prevent the decaying of foodstuffs. Commonly used
agents are benzoic acid, potassium sorbate, propionic acid, sodium benzoate, clove bud oil, sorbic acid,
3.3. Additives
etc. The antimicrobial properties come from the ability of undissociated organic acids molecules to
penetrate bacterial walls and disrupt the cell’s development. Other antimicrobial components of
Additives play many important roles in the film/coatings matrix and include various compounds
natural sources are grapefruit seed extracts, allyl isothiocyanate, hinokitiol, nisin, pediocin, natamycin,
such as antioxidants, nutraceuticals,
and reuterin (Figure 8). pharmaceuticals, antimicrobials, nutrients, flavors, fragrances,
colors, probiotics, emulsifiers, cross-linking agents, browning inhibitors [114–116], etc.
Antimicrobial molecules are used in order to prevent the decaying of foodstuffs. Commonly used
agents are benzoic acid, potassium sorbate, propionic acid, sodium benzoate, clove bud oil, sorbic acid,
etc. The antimicrobial properties come from the ability of undissociated organic acids molecules to
penetrate bacterial walls and disrupt the cell’s development. Other antimicrobial components of natural
sources are grapefruit seed extracts, allyl isothiocyanate, hinokitiol, nisin, pediocin, natamycin, and
reuterin (Figure 8).
Coatings 2020, 10, x FOR PEER REVIEW 12 of 48
Coatings 2020, 10, 687 12 of 45

Figure 8. Natural antioxidants used in edible films/coatings preparation.

Figure 8. Natural antioxidants used in edible films/coatings preparation.

Antioxidants and antibrowning agents retard discoloration, rancidity [53], and the degradation
of food. The most commonly used are ascorbic acid, scorbyl palmitate, butylated hydroxyanisole
Antioxidants and antibrowning agents retard discoloration, rancidity [53], and the degradation of
(BHA), butylated hydroxytoluene (BHT), citric acid, propyl gallate, tertiary butylhydroquinone
food. The most commonly used are ascorbic acid, scorbyl palmitate, butylated hydroxyanisole (BHA),
(TBHQ), tocopherols, Maillard reaction products, rosemary, and sage extracts. Maillard compounds
butylated hydroxytoluene (BHT), citric acid, propyl gallate, tertiary butylhydroquinone (TBHQ),
(hundreds of them) results from a sequence of non-enzymatic reactions (Figure 9), which start from
tocopherols, Maillard reaction products, rosemary, and sage extracts. Maillard compounds (hundreds
sugars and an amino group (typically from an amino acid or protein) through room temperature
of them) results from a sequence of non-enzymatic reactions (Figure 9), which start from sugars and an
to approximately 200 ◦ C. These compounds are very good antioxidants, but they are usually
amino group (typically from an amino acid or protein) through room temperature to approximately
associated with cooking processes (some of them) such as the flavors, aroma, and brown color
200 °C. These compounds are very good antioxidants, but they are usually associated with cooking
released by baked food. Essential oil contains mainly terpenic compounds that are responsible
processes (some of them) such as the flavors, aroma, and brown color released by baked food. Essential
for the antibacterial and antioxidant properties of films: monoterpenes (limonene, tricyclene,
oil contains mainly terpenic compounds that are responsible for the antibacterial and antioxidant
α-thujene, α-pinene, camphene, sabinene, β-pinene, β-myrcene, 3-carene, α-terpinene, α-phellandrene,
properties of films: monoterpenes (limonene, tricyclene, α-thujene, α-pinene, camphene, sabinene, β-
p-cymene, υ-terpinene, α-terpinolene), oxigenated monoterpene (1,8-cineole (Z)-sabinenehydrate,
pinene, β-myrcene, 3-carene, α-terpinene, α-phellandrene, p-cymene, υ-terpinene, α-terpinolene),
linalool, d-fenchylalcohol, α-campholenal, camphor, borneol, 4-terpineol, α-terpineol, bornylacetate),
oxigenated monoterpene (1,8-cineole (Z)-sabinenehydrate, linalool, d-fenchylalcohol, α-campholenal,
sesquiterpene hydrocarbon (α-copaene, aromadendrene α, (E)-caryophyllene, alpha-amorphene,
camphor, borneol, 4-terpineol, α-terpineol, bornylacetate), sesquiterpene hydrocarbon (α-copaene,
7-cadinene, δ-cadinene), oxygenated sesquiterpene (caryophyllene oxide, α-eudesmol) [12,117–126].
aromadendrene α, (E)-caryophyllene, alpha-amorphene, ɤ-cadinene, δ-cadinene), oxygenated
sesquiterpene (caryophyllene oxide, α-eudesmol) [12,117–126]
Coatings 2020, 10, x FOR PEER REVIEW 13 of 48
Coatings 2020, 10, 687 13 of 45

alkaline conditions acidic conditions

OH O
O
C C C C HO
HO C O
HO C C C C C
C C O
OH OH OH

fission products reductones hydroxymethylfurfural

Figure 9. Maillard reactions that are the source of efficient antioxidants.

Figure 9. Maillard reactions that are the source of efficient antioxidants.
These molecules comply with the Code of Federal Regulations; they are GRAS, GRAS/FS, GMP,
These
and are verymolecules
effective,comply
but their with
use the Code of
is subject to Federal Regulations;
controversy in the foodthey are GRAS,
industry, andGRAS/FS,
replacements GMP,
andneeded
are are very(except
effective,
for but
the their useproduct,
natural is subject to controversy
and even for them, in the
the food
use isindustry,
allowed andonlyreplacements
after a carefulare
needed (except
evaluation for the natural product, and even for them, the use is allowed only after a careful
of effects).
evaluation of effects).
Nutrients, flavors, and colorants such as calcium lactate [127], vitamin E [128], and beta
Nutrients,
carotene flavors,
[129] can and colorants
be embedded such as calcium
in coatings/films andlactate
bring[127], vitamin E improvement
an important [128], and betaofcarotene
food
[129] can be embedded
quality protection. in coatings/films and bring an important improvement of food quality
protection.
Cross-linking agents (formaldehyde [130], glutaraldehyde [131], transglutaminase [63], citric
Cross-linking
acid [132], genipinagents
[133], (formaldehyde [130], glutaraldehyde
lactic acid [52], tannic acid [134], ionized [131], transglutaminase
calcium, [63], enhance
or UV radiation) citric acid
[132], genipin [133], lactic acid [52], tannic acid [134], ionized calcium, or UV radiation)
the reticulation of biopolymers, resulting in significant changes of the properties: decreased solubility, enhance the
reticulation
increased of biopolymers,
mechanical resulting
resistance, etc. in significant changes of the properties: decreased solubility,
increased mechanical
Emulsifiers resistance, etc.
are surface-active agents that allow a good dispersion of precursors in order to obtain
Emulsifiers
and stabilize are surface-active
protein/lipid agents that allowcomposites
or polysaccharide/lipid a good dispersion of precursors
and improve in order to
their adherence to food
obtain
and stabilize
surfaces. Addingprotein/lipid
emulsifiers, orthe
polysaccharide/lipid
hydrophilic–lipophilic composites
balance of and improve
mixtures cantheir adherence
be tailored to food
according
surfaces.
to Adding
the required emulsifiers,
lower water vapor the permeability
hydrophilic–lipophilic
(WVP). Commonbalanceemulsifiers
of mixturesused can in
bethe
tailored according
food industry
to the
are required monoglycerides,
acetylated lower water vapor permeability
ammonium (WVP).
lauryl Common
sulfate, emulsifiers
ethylene used in the food
glycol monostearate, industry
glycerol
are acetylated oleic
monostearate, monoglycerides,
acid, linoleicammonium
acid, potassium lauryloleate,
sulfate, ethyleneglycol
propylene glycolmonostearate,
monostearate,sodiumglycerol
monostearate, oleic acid, linoleic acid, potassium oleate, propylene glycol monostearate,
alkyl sulfate, sodium oleate, sorbitan monostearate (Spans), lecithin, stearic acid, sucrose stearate, sodium alkyl
sulfate, sodium (20),
polyoxyethylene oleate, sorbitan
sorbitan monostearate
monolaurate (Tween(Spans),
20), etc. lecithin, stearic acid, sucrose stearate,
polyoxyethylene (20), sorbitan monolaurate (Tween 20), etc.
3.4. Solvents
Solvents are the media for dispersing all films/coatings components and need to be adapted to the
chemicalCoatings
nature of these ingredients. Aqueous solutions of ethanol with different concentrations
2020, 10, 687 14 of 45
are
generally used, since they can provide an adequate solvation power, a lower microbial growth, and a
rapid drying process after application. Examples of alcohol-soluble proteins are wheat gluten and fish
3.4. Solvents
myofibrillar Solvents
proteins. are The hydration
the media of protein
for dispersing facilitates
all films/coatings their solubilization.
components Rarely, toacetone or
and need to be adapted
isopropanol can be used, but more often, acidic solutions (acetic and lactic acid) at lower pH (2.5–3) are
the chemical nature of these ingredients. Aqueous solutions of ethanol with different concentrations
employed for some proteins or chitosan (insoluble in neutral solutions). Other compounds such as
are generally used, since they can provide an adequate solvation power, a lower microbial growth,
and a rapid drying process after application. Examples of alcohol-soluble proteins are wheat gluten
cotton seed proteins require highly alkaline solutions (pH = 8–12), temperature 20–60 °C, and solvent
and fish myofibrillar proteins. The hydration of protein facilitates their solubilization. Rarely, acetone
content in
or the 10%–50%
isopropanol can range.
be used, but more often, acidic solutions (acetic and lactic acid) at lower pH (2.5–3)
are employed for some proteins or chitosan (insoluble in neutral solutions). Other compounds such as
3.5. Plantcotton
Extracts
seed proteins require highly alkaline solutions (pH = 8–12), temperature 20–60 ◦ C, and solvent
content in the 10–50% range.
The whole picture of films/coatings composition is far from complete, and the quest for new
improvements
3.5. PlantisExtracts
ongoing. In recent years, the utilization of plant extracts in edible formulations has
increased at Thea rapid
wholepace. The
picture reason for this
of films/coatings is the complex
composition is far fromcomposition
complete, andof theextracts
quest forthat
newmimic the
properties of different additives already in use. Moreover, the high selection basis of plants and
improvements is ongoing. In recent years, the utilization of plant extracts in edible formulations
solvents,has increased at a rapid pace. The reason for this is the complex composition of extracts that mimic
development of advanced extraction, separation and purification techniques, and/or
the properties of different additives already in use. Moreover, the high selection basis of plants
analyticaland
methods allow the selection and design of customized fractions from initial concentrate. A
solvents, development of advanced extraction, separation and purification techniques, and/or
special case is Centrifugal
analytical methods allowPartition Chromatography
the selection (Figure 10),
and design of customized whichfrom
fractions avoids the
initial use of solid phase
concentrate.
separation columns
A special (which
case is are Partition
Centrifugal expensive and prone to
Chromatography degrade
(Figure sensitive
10), which avoidscompounds) with a rotor of
the use of solid phase
special construction that allows the simultaneous utilization of a liquid stationary phase and
separation columns (which are expensive and prone to degrade sensitive compounds) with a rotor of a liquid
mobile phase [105,135–137]. Table 1 presents various applications of plant extracts for a wide range of
special construction that allows the simultaneous utilization of a liquid stationary phase and a liquid
mobile phase [105,135–137]. Table 1 presents various applications of plant extracts for a wide range
foods. of foods.

Figure 10. Centrifugal

Figure 10. Partition
Centrifugal Chromatography:
Partition a preparative
Chromatography: a preparative scale
scale method forplant
method for plant extract
extract fractionation.
fractionation.

Table 1. Application of plant extracts in food preservation.

Product
Plant Extract Film/Coating Base References
Preserved
Fish Red radish anthocyanins extract gelatin/gellan gum [3]
Rosemary
glycerol, gelatin, chitosan,
essential oil— Rosemary essential oil [7]
pectin
enriched films
Alginate
Trout fillet Zataria multiflora Boiss essential oil [9]
coarse/nanoemulsions
Coatings 2020, 10, 687 15 of 45

Table 1. Application of plant extracts in food preservation.

Product Preserved Plant Extract Film/Coating Base References
Fish Red radish anthocyanins extract gelatin/gellan gum [3]
Rosemary essential oil—enriched
Rosemary essential oil glycerol, gelatin, chitosan, pectin [7]
films
Trout fillet Zataria multiflora Boiss essential oil Alginate coarse/nanoemulsions [9]
Pullulan and polymeric nanocapsules
Table grapes (Vitis vinifera L.) Thymus vulgaris L. essential oil [12]
containing essential oil
Edible film Nitrite and garlic essential oil Gelatin–chitosan [28]
Microemulsion nanofilms: Tilapia fish
Meat Ginger essential oil [31]
skin gelatin and ZnO nanoparticles
Edible film against food spoilers Oregano, clove, tea tree, coriander, mastic
Whey protein isolate [50]
and foodborne pathogens thyme, laurel, rosemary, and sage essential oils
Edible films Yerba mate extract Cassava starch [86]
Edible films - Water chestnut starch–chitosan [88]
Edible films Thyme essential oil/apple skin polyphenols Acai puree, pectin [116]
Lamb meat Thyme and garlic essential oils Alginate [117]
Tomato Sage essential oil Aloe vera gel [118]
In vitro and in the food model
Caraway and juniper essential oils - [119]
(polenta).
Ready-to-cook barbecue chicken Ginger essential oil and citric acid Cellulose nanofibers coating [120]
Papaya (Carica papaya L.) Mentha essential oils Chitosan [122]
Rainbow trout fillets Lemon and sage essential oil Quinoa [125]
Pork loin Oregano essential oil, resveratrol nanoemulsion Pectin [138]
Rainbow trout fillets Ferulago angulata essential oil Chitosan [139]
biopolymer Nanoemulsions of Lepidium
Soybean oil Hyssop (Hyssopus officinalis L.) extract [140]
perfoliatum and Orchis mascula
Beef Myristica fragrans essential oil Agar [141]
Rainbow trout Lemon verbena extract/essential oil Chitosan [142]
Zataria Multiflora Boiss and Bunium persicum
Turkey meat Chitosan [143]
Boiss essential oils
Antibacterial films Rheum ribes L. extract Methylcellulose film [144]
Cucumber Cinnamon essential oil and cinnamaldehyde chitosan [145]
Guava fruit Cinnamon essential oil Gum arabic, oleic acid [146]
Papaya Clove essential oil Manioc starch [147]
Beef Cumin essential oil Shahri Balangu seed mucilage [148]
Edible film Clove essential oil Millet starch [149]
Free or nano-encapsulated Paulownia
Pork chops Chitosan [150]
Tomentosa essential oil
Tambaqui (Colossoma macropomum)
Clove essential oil Chitosan [151]
fillets
Apple, tomato, and persimmon Lecithin-encapsulated thyme essential oil Starch–gellan [152]
Combining, pectin, and chitosan
Edible films Cupuassu (Theobroma grandiflorum) Puree [153]
nanoparticles
Edible films Extracts of green apple (Granny Smith) skin Methylcellulose [154]
Yuba, carboxymethyl cellulose, beeswax,
Edible films Oxidized ferulic acid [155]
sodium pyrophosphate
nano emulsion-based edible coating
Chicken breast fillets Ginger (Zingiber officinale) essential oil [156]
containing
Guava (Psidium guajava L.) Ruta graveolens Essential Oil Chitosan [157]
Mango cultivar Tommy Atkins Mentha piperita L. essential oil Chitosan [158]
Banana Clove essential oil titratable Cassava starch, polyvinyl polychloride [159]
edible film Microencapsulation of Thai rice grass extract Carboxymethyl cellulose [160]
Edible films Aloe vera gel Banana starch–chitosan [161]
Meat products Asparagus racemosus Calcium alginate edible film [162]
Macadamia skin (Macadamia tetraphylla),
Edible films Pea starch–guar gum Biocomposite [163]
banana peel, blueberry ash extracts
Nile tilapia fillets Pomegranate peel extract as edible coating Chitosan [164]
Fish skin gelatin, palm oil, different
Edible films Basil essential oil [165]
surfactants
Tomatoes Oregano (Lippia graveolens) essential oil Pectin [166]
Coatings 2020, 10, 687 16 of 45

Table 1. Cont.
Product Preserved Plant Extract Film/Coating Base References
Kashar cheese Orange essential oil Egg white protein [167]
Caesalpinia decapetala and Caesalpinia spinosa
Ground beef patties gelatine [168]
(Tara) extracts
Edible films Ginger essential oil nanoemulsion Gelatin, montmorillonite [169]
Edible films Hydrolysable chestnut tannin Pigskin gelatin films [170]
Organic leafy greens in sealed
Carvacrol and cinnamaldehyde Apple, carrot, and hibiscus [171]
plastic bags
Clove bud (Syzygium aromaticum)/oregano
Sliced bread Methylcellulose [172]
(Origanum vulgare) nanoemulsions
Apples Satureja hortensis L. extracts Pullulan [173]
Edible films Grape pomace extract Chitosan [174]
Edible films Ginja extract cherry Methylcellulose [175]
Extracts of chives (Allium schoenoprasum), sage
(Salvia pratensis, Lamiaceae), European
Edible films Atelocollagen [176]
elderberry (Sambucus nigra, Caprifoliaceae),
dandelion (Taraxacum officinale)
Edible films Red raspberry extract Soy protein isolate [177]
Ham Carvacrol and cinnamaldehyde Pectin-based apple, carrot, and hibiscus [178]
Zataria multiflora Boiss essential oil /grape seed
Edible films Chitosan [179]
extract

4. Preparation and Characterization of Edible Films/Coatings

4.1. Techniques for Preparing Edible Films/Coatings

The preparation phase has to follow some previously tested formulations for obtaining products
with the desired properties (strength, solubility, flavor, texture, strength, compatibility between
components, film stability, etc.). When new components or different concentrations of additives
are introduced, the features of coating/films mixtures can change significantly. In order to attain
the optimal configuration with the minimum number of trials, some advanced statistical methods
(response surface methodology) are implemented. Challenges encountered in preparing and using
films/coatings generally are as follows.

• Using essential oil in the formulation due to the low miscibility in protein or polysaccharides
solution. For this problem, an adequate emulsifier is used in an appropriate concentration;
• The casting method is not so easy to apply at the industrial level compared with the extrusion
method. In this respect, maintaining the required concentration of essential oil in the film is an
aspect that requires further studies;
• Obtaining a complex material at a low price with high resistance to surrounding factors;
• Choosing the right material for film preparation from a wide range of options

Film/coatings are formed as a result of a multitude of chemical and physical processes blended in a
manner that assures a suitable output. An important aspect is to figure out in what order the ingredients
are added, which include the temperature regime and pH of the solution. The process of mixing
usually starts with water and surfactants followed by the main ingredients (proteins, polysaccharides,
lipids) and active ingredients (antimicrobial, antioxidants, etc.). Finally, water is added for adjusting
components’ concentrations, viscosity, pH, etc.
Different techniques are used for the efficient production of edible barriers. To a certain
extent, the preparation of films and coatings follows the same path: obtaining the complex mixture,
homogenization, degassing, and stabilization. In the case of films, the first step is to process the liquid
by casting (the liquid is poured on solid surfaces), lamination, or extrusion. The second step is drying
carefully until the material reaches a certain values of humidity, and the final step is application on food.
In the case of coatings, the liquid is dispersed on food surfaces in different ways: spraying, dipping,
brushing, panning, fluidized bed, foaming, etc. The process parameters are thoroughly controlled in
order to obtain the desired products and are related with the food characteristics (temperature, shape,
 Coatings 2020, 10, 687 17 of 45

size, diameter variation, hygroscopicity, surface tension) or to the coating liquid itself (solvent type,
composition, viscosity, surface tension, etc.). The food particle size and shape are the main factors that
decide the choice of method (Figure 11).
Coatings 2020, 10, x FOR PEER REVIEW 18 of 48

Figure 11.11.
Figure Influence ofofmaterial
Influence materialsize
size on coatingselection
on coating selection techniques.
techniques.

All these
All these materials
materials combined
combined giveaa final
give final product
productwithwithenhanced
enhanced properties. There
properties. are also
There are also
coatings in a multi-component or composite manner, which are based on complementary or synergistic
coatings in a multi-component or composite manner, which are based on complementary or synergistic
approaches. Usually, there is some association between hydrophobic and hydrophilic structures.
approaches. Usually, there is some association between hydrophobic and hydrophilic structures. These
These are prepared by two methods: (1) superposing two layers—hydrophobic on top of a hydrophilic
are prepared by two methods: (1) superposing two layers—hydrophobic on top of a hydrophilic layer
layer or (2) emulsion-type composite lipids dispersed in a hydrophilic support. Layer-by-layer
or (2) deposition
emulsion-type
(LbL) composite lipids
permits better dispersed
control over theinfeatures
a hydrophilic
of ediblesupport. Layer-by-layer
coating; especially, deposition
its thickness
(LbL) and
permits better
is more control
adapted over the features
to automated of edible
manufacturing coating;
[180]. especially,
The ionic its thickness
self-assembly method isand is more
based
adapted to automated
on successive layersmanufacturing [180]. polymers
of positively charged The ionic(chitosan)
self-assembly method ischarged
with negatively based polymers
on successive
layers of positively charged polymers (chitosan) with negatively charged polymers (polyanionic
(polyanionic cellulose, pectin, etc.).
cellulose, pectin, etc.).
4.2. Characterization of Edible Films/Coatings
4.2. Characterization of Edible Films/Coatings
The characterization of edible films/coatings is a complex process, since it addresses a large range
of features and is intended to give a thorough overview of the product’s qualities. The diversification of
The characterization of edible films/coatings is a complex process, since it addresses a large range
characterization methods is necessary since in some cases, introducing different ingredients in certain
of features and iscan
parameters intended to give a thorough
lead to antagonistic overview
variations: of the
for example, product’s
when qualities.
the tensile strengthThe
(TS)diversification
increases,
of characterization methods is necessary
the elongation at break (EAB) decreases. since in some cases, introducing different ingredients in
certain parameters can lead to
After preparation, theantagonistic variations:are
product’s properties for thoroughly
example, when the tensile
evaluated strength (TS)
by measuring
increases, the elongationand
the physicochemical at biological
break (EAB) decreases.
parameters, such as water vapor permeability (WVP), elastic modulus
After preparation,
(EM), elongation the (EAB),
at break product’s propertiesoptical
microstructure, are thoroughly evaluatedand
properties, antioxidant byantimicrobial
measuring the
physicochemical and biological parameters, such as water vapor permeability (WVP), elastic
activity, etc. Adequate values of these parameters assure to some extent the preservation of modulus
the food’s
(EM), elongation at break (EAB), microstructure, optical properties, antioxidant and antimicrobial
original properties.
activity, etc.Wettability
4.2.1. Adequateofvalues
Coatingsof Formulations
these parameters assure
on Food to some extent the preservation of the food’s
Surface
original properties.
An important aspect of edible coatings is their compatibility in terms of wettability [181,182]
between the formulation and the food surface. Mismatch between coating formulation and surface
4.2.1. Wettability of Coatings Formulations on Food Surface
results in inconsistencies in film properties (thickness and uniformity). In most cases, the adhesion of
An important
coatings aspect
to the food of edible
surface coatings
is inadequate dueistotheir compatibility
chemical in terms
differences, which of wettability
generally [181,182]
increase when
between the formulation and the food surface. Mismatch between coating formulation and surface
results in inconsistencies in film properties (thickness and uniformity). In most cases, the adhesion of
coatings to the food surface is inadequate due to chemical differences, which generally increase when
the coated object consist of slices of fresh cutted fruits. The fast adsorption of the liquid included in
formulations on fruit surfaces prevents the formation of an edible barrier. Improving the wettability
 Coatings 2020, 10, 687 18 of 45

the coated object consist of slices of fresh cutted fruits. The fast adsorption of the liquid included in
formulations on fruit surfaces prevents the formation of an edible barrier. Improving the wettability
requires the surface tension of the solid surface to be similar to that of liquid, and matching those
usually
Coatings 2020, 10, xrequires
FOR PEERsurfactants
REVIEW such as Tween 80. When a liquid is spread on a solid surface (Figure 12), 19 of 48
the spreading coefficient (Ws ) is close to zero, meaning that the liquid is optimal for covering.
The wetting capacity of the liquid depends on the right balance between the adhesion coefficient Wa
(accounting for forces that expand the liquid on the surface) and the cohesion coefficient Wc (accounting
(accounting for forces that expand the liquid on the surface) and the cohesion coefficient Wc (accounting
for forcesforthat keep
forces thatliquid contracted).
keep liquid contracted).

Figure 12. Equilibrium of forces acting at solid–liquid–gas interfaces.

Figure 12. Equilibrium of forces acting at solid–liquid–gas interfaces.

Ws , Wa , Wc can be described by Equations (1)–(3), and the value of Ws can be zero or negative:
Ws, Wa, Wc can be described by Equations (1)–(3), and the value of Ws can be zero or negative:
Ws = Wa − Wc = γSV − γLV − γSL (1)
Ws = Wa – Wc = γSV − γLV − γSL (1)
Wa = γLV (1 + cos θ) (2)
Wa = γLV (1 + cos θ) (2)
Wc = 2γLV (3)
W = 2γ
c LVγ (3)
The contact angle results from interfacial tensions: SV (solid–vapor), γLV (liquid–vapor), γSL
The contact angle results from interfacial tensions: γSV the
< (solid–vapor), γLV (liquid–vapor),
◦ above 90◦
(solid–liquid). Values of θ 90 show that the liquid is wetting surface, while values γSL
show the opposite. When θ is near zero, the liquid wettability is at its maximum. Contact angle
(solid–liquid). Values of θ < 90° show that the liquid is wetting the surface, while values above 90° show
measurements are influenced by factors such as droplet size, temperature (maintained up to 8 ◦ C),
the opposite. When θ is near zero, the liquid wettability is at its maximum. Contact angle measurements
surface roughness, and surface impurities. Generally, Ws can be obtained from the contact angle
are influenced by factors
and surface tension such
values. asThe
droplet
contactsize, temperature
angle is determined (maintained
by the sessileup tomethod
drop 8 °C), surface
[183–186]roughness,
and surface impurities.
(a droplet Generally,
on the food surface is Wmeasured
s can be obtained from
by an optical the contact
system equippedanglewith aand surface tension values.
high-performance
The contact angle is determined by the sessile drop method [183–186] (a droplet on the food surface is
video camera and a software) or by the immersion method [187] (using a tensiometer).
measured byAn animportant parameter in the physicochemistry of surfaces is surface tension, which stands as
optical system equipped with a high-performance video camera and a software) or by
the amount of energy required to increase the surface per area unit (J m−2 ). Surface tension (γLV ) is
the immersion method [187] (using a tensiometer).
determined using the De Noüy platinum ring method.
An important parameter
Surface tension in theof physicochemistry
is a measure adhesion between liquid ofandsurfaces
solid andisissurface
calculatedtension,
from the which
contact stands as
the amountangleof energy required
measurements to increase
of a standard liquid onthe
the surface per area
surface. Another unit (Jparameter
important m−2). Surface tension (γLV ) is
is the critical
determined using
surface the[152,181]
tension De Noüy platinum
of the food to be ring method.
coated. This parameter is obtained using the extrapolation
of Zisman plot [152] (cos θ against the surface tension of different liquids on the studied surface) until
Surface tension is a measure of adhesion between liquid and solid and is calculated from the
intercept of the curve at cos θ = 1.
contact angleTherefore,
measurements of a standard liquid on the surface. Another important parameter is the
for a good compatibility (liquid–solid), two conditions must be fulfilled: wettability
critical surface tension [152,181] of the food to be coated. This parameter is obtained using the
and adhesion.
extrapolationSapper
of Zisman
et al.,plot
[152][152] (cos θ the
evaluated against the surface
influence tension of different
of coating-forming liquids ononthe studied
liquids composition
surface) until intercept of the curve at cos θ = 1.
the wettability/spreading coefficient, contact angle, and surface tension values. In addition, the interaction
Therefore, for a good compatibility (liquid–solid), two conditions must be fulfilled: wettability and
of these liquids with persimmon, tomato, and apple surface fruits was assessed. The liquid coatings
formulations used were obtained from different compounds: starch–gellan, starch–gellan with emulsified
adhesion.essential oil, and starch–gellan with lecithin-encapsulated essential oil. To these formulations were added
Sapper et concentrations
different al., [152] evaluated
of Tween 85. the It wasinfluence
found that inofthecoating-forming
absence of essential oil liquids composition
in the liquid coatings, on the
wettability/spreading coefficient,
Tween 85 has a beneficial effect,contact
improving angle, and surface
the spreading tension
coefficient values.
(values almostIn addition,
zero). the interaction
The addition
of these liquids with persimmon, tomato, and apple surface fruits was assessed. The liquid coatings
formulations used were obtained from different compounds: starch–gellan, starch–gellan with
emulsified essential oil, and starch–gellan with lecithin-encapsulated essential oil. To these
formulations were added different concentrations of Tween 85. It was found that in the absence of
Coatings 2020, 10, 687 19 of 45

of essential oil also shows a good impact on surface tension, but not with Tween 85 in the formulations.
As can be seen from Figure 13, the contact angle decreases at higher Tween 85 concentration, which shows
the beneficial effect of surfactant. The influence of the food surface nature is emphasized by the lower
Coatings 2020, 10, x FOR PEER REVIEW 20 of 48
values of contact angles of persimmon compared with apple and tomato.

Figure 13. Variation of θ with Tween 85 concentration for three coating mixtures.
Figure 13. Variation of θ with Tween 85 concentration for three coating mixtures.
 Coatings 2020, 10, 687 20 of 45

Ortiz et al. [183] observed that in a formulation containing chitosan, glycerol (10%), and Tween 20,
the Ws coefficient increases from −28.24 to −20.63 when the Tween 20 content increases from 5% to
15%. Gelatin-based films prepared with mint essential oil (0%, 0.06%, 0.13%, 0.25%, 0.38%, 0.50%)
present a significant improvement of coating properties in terms of hydrophobicity (the contact angle
of the water on the coating surface increases from 49.0◦ to 63.1◦ ).

4.2.2. Film/Coating Thickness, Mechanical, and Gas BARRIER properties

Film/coating thicknesses generally have a large variability in a range from 2 to about 3000 µm [188]
depending on application/preparation techniques and the composition of formulation. Film thicknesses
are measured with digital micrometers in several repetitions and at different positions.
The incorporation of clove essential oil (0.8% w/v) increases the thickness from 43 to 51 µm.
This is attributed to the higher free volume of the film [159]. The same situation was observed by
Han et al. [189] when cinnamon essential oil was added to into sodium alginate/carboxymethyl cellulose.
Another beneficial effect of essential oil is that film rigidity decreases and the mechanical properties
are improved [124]. However, higher values of thickness often lead to higher surface roughness [97],
which may impair the gas barrier properties.
Organic acids (citric, lactic, malic, or tartaric) play a major role in increasing the thickness of a
complex mixture containing nisin incorporated in soy protein [190]. Organic acids were introduced in
different concentrations (0–2.5%), and the thickness reaches a maximum within that interval. Without
malic acid in the composition, the thickness is 25 µm, and with 1.6% organic acid, the thickness reaches
35 µm.

4.2.3. Mechanical Properties

These properties are important, since they assure the physicochemical integrity of the protected
food by film/coatings and are generally measured using a texture analyzer. Figure 14 shows three
mechanical parameters that are taken into consideration for the characterization of films/coatings in
terms of resistance at stress: tensile strength (TS), elongation at break (EAB), and modulus of elasticity
(EM). Figure 14 represents a typical curve of these parameters’ evolution (the shape of the curve can
change significantly with the quality or type of materials). The range of mechanical parameters out of
those already mentioned are larger, including compression, puncture, tearing strength, burst, abrasion,
Coatings 2020, 10,but
etc., x FOR
thesePEER REVIEW
parameters are not the object of this paper. 22 of 48

Figure 14. Mechanical parameters considered for the evaluation of edible films/coatings.
Figure 14. Mechanical parameters considered for the evaluation of edible films/coatings.

4.2.4. Barrier parameters

Water vapor permeability (WVP) is a parameter that directly affects the freshness of the product
embedded in films/coatings, since the water depletion significantly changes their organoleptic
properties. The usual determination method for WVP is gravimetrically according to ASTM E96M-10
at 75% relative humidity (RH) (or other RH if required):
 Coatings 2020, 10, 687 21 of 45

Tensile strength can be calculated using the below equation, and the results are expressed in MPa.

Fmax
TS = (4)
LW
where Fmax is the maximum tensile force at rupture (N), L is the thickness of the film (mm), and W is
the width of the film (mm). Elongation at break can be expressed as:

DL
EAB = 100 (5)
L
FigureL 14.
where Mechanical
is the parameters
initial length considered
of the filmsample (mm), for
andthe
∆L evaluation of edible
is the difference films/coatings.
between the final and initial
lenght of sample (mm).
4.2.4. Barrier parameters
The values of these mechanical indicators are categorized in quality ranges such as inferior,
marginal, good, and superior. In this way, the users of films/coatings can objectively assess
Water the
vapor permeability
compatibility (WVP)with
of a coating is a the
parameter
food thatthat directly
needs affects the
to be protected. freshness
Table of some
2 presents the product
embedded values
in films/coatings, sincestudies
obtained in different the and
waterwithdepletion significantly
different materials that showchanges their
the influence organoleptic
of certain
properties. The usual determination method for WVP is gravimetrically according to ASTM E96M-10
ingredients on mechanical strength.
at 75% relative
4.2.4.humidity (RH) (or other RH if required):
Barrier Parameters
Water vapor permeability (WVP) is 𝑊𝑊𝑊𝑊𝑊𝑊
𝑤𝑤 that
𝑥𝑥 directly affects the freshness of the product
=
a parameter
(6)
𝐴𝐴 significantly
embedded in films/coatings, since the water depletion ∆𝑝𝑝 changes their organoleptic properties.
The usual determination method for WVP is gravimetrically according to ASTM E96M-10 at 75%
where x is the film thickness (m), A is the permeation area (m2), Δp is the difference in vapor pressure
relative humidity (RH) (or other RH if required):
across the film (Pa), and w is the weight of water gained by the film in the capsule per hour (g h−1).
wx
The water permeability has to be restricted in both
WVP = directions, since the key of food preservation (6)
A ∆p
is to keep the food as it is. In general, the main ingredients of film coatings are proteins and
polysaccharides
where with
x is thehydrophilic
film thicknesscharacter,
(m), A is theand in order
permeation areato(mlower the WVP, some lipid products are
2 ), ∆p is the difference in vapor pressure
−1 ).
used [151,162,191].
across theOther hydrophobic
film (Pa), additives
and w is the weight suchgained
of water as vitamin E decrease
by the film the WVP
in the capsule [192].
per hour (g hIn addition,
The water permeability has to be restricted in both directions, since the key of food preservation is to
the introduction of chitosan biguanidine (Figure 15) into a ternary system composed of carboxymethyl
keep the food as it is. In general, the main ingredients of film coatings are proteins and polysaccharides
cellulose/sodium alginate/chitosan
with hydrophilic character, andbiguanidine (CMC/A/CBg)
in order to lower the WVP, someinlipid a progressive manner
products are used decreases the
[151,162,191].
WVP from 330Othertohydrophobic
178 (g/m /day)
2 [193].
additives suchThis occurs
as vitamin due to the
E decrease higher
the WVP reticulation
[192]. In addition, and the cross-linking
the introduction
reactions among CMC, CBg, and alginate.
of chitosan biguanidine (Figure 15) into a ternary system composed of carboxymethyl cellulose/sodium
The main barrier in water
alginate/chitosan depletion
biguanidine is the hydrophobic
(CMC/A/CBg) in a progressive substances,
manner decreases andthe
the
WVPuseful
from indicator
330 to for
178 (g/m2 /day) [193]. This occurs due to the higher reticulation and the cross-linking reactions among
selecting them is presented in Figure 16.
CMC, CBg, and alginate.

Figure 15. Compounds used for edible films with lower water vapor permeability (WVP).
Figure 15. Compounds used for edible films with lower water vapor permeability (WVP).
 Coatings 2020, 10, 687 22 of 45

The main barrier in water depletion is the hydrophobic substances, and the useful indicator for
Coatings 2020, 10, x FORthem
selecting PEERis REVIEW
presented in Figure 16. 23 of 48

Figure 16. Substances used for obtaining lower values of WVP ranked in terms of hydrophobicity.
Figure 16. Substances used for obtaining lower values of WVP ranked in terms of hydrophobicity.
Oxygen and CO2 Permeability
Oxygen and COOxygen
2 Permeability
and CO2 are important gases that affect the integrity of any food during storage. Usually,
these parameters are measured using ASTM D 3985–02 (2002) or the new permeability meters
Oxygenprovided
and CO are important
by2different producers.gases
Edible that affect the
films/coatings integrity
preserve of any
the initial food
state of foodduring storage. Usually,
by restricting
these parameters areofmeasured
the access these gases.using ASTM vitamin
For example, D 3985–02 (2002)
C, which is anorimportant
the newdietary
permeability
componentmeters
of provided
by different producers. Edible films/coatings preserve the initial state of food by restricting the access
some foods, is depleted inside product if the coating is too permissive to O2 or even CO2 at higher
concentrations. On the other hand, films with a high permeability of oxygen favor the production of
of these gases. Forand
ethylene example, vitamin
the fruits ripen C,while
quickly, which filmsiswith
an too
important dietary
low permeability component
allow fermentation of some foods, is
[115].
depleted inside product
In addition, if the coating
is important is too permissive
to acknowledge that water andto oxygen
O2 or even CO2 atinhigher
permeability concentrations.
most cases are On
the other hand, filmsrelated;
inversely with hence,
a highedible
permeability
films must of be oxygen
prepared favor
in ordertheto production of ethylene
fulfill both features [128,194].and the fruits
Low O2 permeability allows preventing discoloration, which is an important organoleptic property for
ripen quickly, while films with too low permeability allow fermentation [115]. In addition, is important
consumers. Some polymers used for edible films show lower O2 permeability compared with classic
to acknowledge that
polymers water
such as lowand oxygen
density permeability
polyethylene (LDPE). Filmsinbased
mostoncases aresuch
additives inversely related;
as chitosan, alginate, hence, edible
films must be preparedand
carrageenan, in order to fulfill
pectin present goodboth
gas features [128,194].
barrier properties. Some Low O2 permeability
functional allows
groups attached to preventing
biopolymer chains induce lower permeability for gases: –OH, –CN, –Cl, –F and –COOCH3 (from higher
discoloration, which is an important organoleptic property for consumers. Some polymers used for
to lower) [13,16,81,124,154]. Table 2 presents some of the permeation characteristics of the different
edible filmsformulations
show lower used toO 2 permeability
prepare edible films. compared with classic polymers such as low density
polyethylene (LDPE). Films based on additives such as chitosan, alginate, carrageenan, and pectin
present good gas barrier properties. Some functional groups attached to biopolymer chains induce lower
permeability for gases: –OH, –CN, –Cl, –F and –COOCH3 (from higher to lower) [13,16,81,124,154]. Table 2
presents some of the permeation characteristics of the different formulations used to prepare edible films.
Coatings 2020, 10, 687 23 of 45

Table 2. Examples of formulations where mechanical and barrier parameters are changing as a function of composition.
WVP 1010 CO2 109 O2
Thickness Tensile Strength Moisture
Formulation Composition EAB (%) EM (MPa) (g m−1 s−1 Pa−1 ) (cm3 /m s Pa) 1010 References
(µm) (MPa) Content (%)
(cm3/m s Pa)
0% 90.59 18.1344 78.2348 6.42
Fish skin gelatin (FSG), zinc oxide nanoparticle 10% 104.9 15.5879 101.364 6.31
(ZnONP), ginger essential oils (GEO) different 20% 112.34 14.4574 111.028 - 5.94 - - - [31]
concentrations, Tween 20, glycerol 40% 122.96 13.0296 120.421 5.22
80% 134.1 10.846 132.463 4.93
Extrusion 20%
450 2.41 282.6 99 1.51 21.4
(110 ◦ C)
Extrusion 20%
580 1.51 256.3 118 1.97 19.4
Fish gelatin, glycerol, water, extrusion and casting (120 ◦ C) - - [34]
Extrusion 25%
410 1.92 293.4 84 2.43 16.1
(110 ◦ C)
Extrusion 25%
340 1.87 237.2 132 2.92 27.7
(110 ◦ C)
Casting 20% 100 17.8 27.4 482 1.91 24.7
Casting 25% 100 7.7 49.4 259 2.5 21.4
Control 57.05 26.27 53.83 2.71
0.3% esculin 55.82 34.26 52.37 - 2.67 - - -
Gelatin from sturgeon skin, glycerol, solution [37]
0.6% esculin 57.25 35.42 49.55 1.72
0.9% esculin 56.92 35.87 42.86 1.32
FP + WPC 3.75 112.7 32.8 9.4 6.7 10.8
Microparticles containing sunflower oil, alginate, FP + OVA 3.50 107.4 27.6 13.2 - 8.9 - - 11.4
[66]
pectin coated in protein FP3.75 81.1 28.2 5.9 11.5 17.1
FP3.50 73.4 32.6 3 11.8 17
Cassava - -
3% 60 0.54 127.16 0.172 15.05
4% 90 0.093 107.47 0.214 11.34
5% 100 1.102 130.91 0.184 16.3
Arrowroot - -
Starch (3%, 4% and 5%) from cassava, arrowroot, 3% 700 1.716 67.85 - 0.161 - - 16.94 [67]
and canna edulis 4% 85 1.633 84.37 0.157 11.34
5% 650 1.827 141.36 0.124 15.2
Canna edulis - -
3% 125 4.064 61.19 0.167 45.27
4% 90 2.438 52.23 0.225 43.39
5% 115 3.998 42.94 0.176 20.4
Thermoplastic starch (TPS) reinforced with TPS 2.02 125.66
hexametaphosphate (SHMP) and polyvinyl 2% PVAF/TPS - 2.62 83.618 - - - - - [77]
alcohol fiber (PVAF) SHMP/PVAF/TPS 5.75 114.02
Coatings 2020, 10, 687 24 of 45

Table 2. Cont.
WVP 1010 CO2 109 O2
Thickness Tensile Strength Moisture
Formulation Composition EAB (%) EM (MPa) (g m−1 s−1 Pa−1 ) (cm3 /m s Pa) 1010 References
(µm) (MPa) Content (%)
(cm3/m s Pa)
Fvr/P = 10:0 27 31.38 3 2.45
Fvr/P = 8:0 28 30.51 3 2.48 - - -
Vegetable residue (FVR) and potato skin (P) flours Average: 242 [87]
Fvr/P = 8:2 70 32.01 3 2.6
Fvr/P = 8:4 84 34.49 4 2.78
(10:70:20) 80.53 27.09 4.73 1.41 5.04 4.13 1.41
Native starch, acetylated starch, glycerol (% (80:5:15) 75.97 16.25 2.59 - 0.88 2.66 2.08 0.88
[89]
w/w/w) (75:5:20) 122.93 10.31 20.14 1.31 4.13 3.31 1.31
(15:70:15) 129.42 23.99 6.14 1.2 3.85 2.98 1.2
Extract concentration -
Corn starch, Uncaria gambir Roxb 20% 110 14.78 2.42
- - - - - [94]
extract, glycerol 30% 119 15.11 2.46
40% 124 15.67 2.5
EFYS 0% 163 15.81 23.96 54.08 1.91 1.036 23.66
AAG 0.5% 186 17.3 19.75 60.81 1.2 4.49 25.3
AAG 1% 194 17.64 15.36 63.43 1.29 7.36 25.38
AAG 1.5% 197 17.85 13.62 65.08 1.16 5.39 25.62
Elephant foot yam starch, hydrocolloids xanthan
AAG 2% 199 20.14 13.34 58.03 1.1 - 1.06 26.42 [96]
(XG) and agar–agar (AA)
XG 0.5% 158 19.27 21.52 56.15 2.47 7.59 25.21
XG 1% 173 19.1 17.4 58.28 9.09 1.09 22.83
XG 1.5% 186 19.34 15.36 64.03 1.04 1.19 23.17
XG 2% 187 19.48 14.69 69.77 9.34 5.48 24.36
Cassava starch CS 43 - - - 0.37 - - 18.3
[159]
CS + 0.8% EO
Casava starch + clove essential oil 51 0.3 16.24
W/V
Control 3.17 48.91 1.34
WP 0.2% 2.65 35.49 0.86
Starch–glycerol whey protein (emulsifying) WP 0.4% ~3000 2.02 34.66 0.7 - - - - [188]
WP 0.6% 1.8 32.02 0.6
WP 0.8% 1.81 31.74 0.64
5%/2%/0% 10.17 2.75
Starch, sorbitol, mango peel, (NaOH solution up - - - - - -
5%/2%/2% 15.2 5.53 [195]
to 100%)
5%/2%/4% 13.45 6.69
Ag 27.5 19.7 992 8.47 13.95
Ag/Ln 19.5 14.5 970 6.1 7.47
Agar or/and alginate, glycerol, Larrea nitida Alg - 22.4 17.8 793 8.3 - 1.77 - [196]
extract Alg/Ln 10.3 10.6 784 6.04 4.16
Ag/Alg 24 23.7 615 7.83 1.89
Ag/Alg/Ln 12.9 21.4 477 6.06 3.76
Coatings 2020, 10, 687 25 of 45

Table 2. Cont.
WVP 1010 CO2 109 O2
Thickness Tensile Strength Moisture
Formulation Composition EAB (%) EM (MPa) (g m−1 s−1 Pa−1 ) (cm3 /m s Pa) 1010 References
(µm) (MPa) Content (%)
(cm3/m s Pa)
Zein 115.4 10.73 3.69 648.28
Zein + Gallic acid 115.66 8.59 3.52 428.5
Zein + Vanillic - - - -
Zein protein, polyphenols, and/or essential oil 124.98 6.99 2.75 445.49 [197]
acid
Zein + Carvacrol 129.7 4.68 8.76 226.82
Zein + Eugenol 134.63 7.56 7.83 344.05
Zein + Citral 157.8 4.32 1.21 412.16
SA/Pul/Cap–0% 32 46.34 4.7 1.18 21.69
SA/Pul/Cap–2% 33 53 3.58 1.93 19.4
sodium alginate/pullulan/capsaicin SA/Pul/Cap–4% 35 54.1 3.22 - 1.99 - - 17.4 [198]
SA/Pul/Cap–6% 36 54.41 3.16 2 16.72
SA/Pul/Cap–8% 38 55.25 3.08 3.06 15.2
CH:S - 9.5 90 17 9.6 - 6.6 -
Chitosan, starch, thyme extract [199]
CH:S:TE 8.2 47 51 8.8 4.3
Chitosan 388.73 20.39 7.89
Chitosan, lactoperoxidase with or without iodine Chitosan/LPOS - 574.42 18.31 - 5.61 - - - -
Chitosan/LPOSI 580 17.8 6
HDM pectin 76.67 28 1.08 1990.29
Nwax10 104.23 28.99 3.23 885.53
HDM, high methylester pectin; L232, polymer for
Nwax20 112.7 29.02 3.17 721.86
industrial seed coating; Noil, nanocomposite of
Nwax30 96.98 29.49 3.84 668.47 - - - - [200]
pectin and neem oil; Nwax, nanocomposite of
pectin and carnauba wax. HDM pectin Noil10 112.14 29.86 3.38 525.99
Noil20 101.34 30.5 3.8 497.74
Noil30 123.28 30.28 4.28 493.19
CM25 0.054 0.054 0.131 18.18
Chia mucilage (CM) hydrocolloid glycerol (25%, - - - -
CM50 0.056 0.056 0.325 32 [201]
50%, and 75% w/w)
CM75 0.06 0.06 0.442 41.88
Coatings 2020, 10, 687 26 of 45

4.2.5. Other Characterization Methods of Edible Films/Coatings

Color
Color is an important organoleptic parameter, and at first glance, the success of coating it is
represented by final product color. Color is measured usually with a Portable Colorimeter Reader.
Evaluations are made on L* (luminosity), a* (+red, −green), and b* (+yellow, −blue), which represent
the color parameters of the CIELab scale. Generally, color parameters were measured in five points on
an edible film surface. Hue (qualitative attribute) and Chroma (quantitative attribute) were calculated
following Equations (7) and (8), respectively [159]:

b∗
!
−1
Hue = tan (7)
a∗
p
Chroma = a∗2 + b∗2 (8)

These values can be used to calculate the browning index [195], which is an efficient parameter
for monitoring product freshness:
[100(X − 0.31)]
BI = (9)
0.172
(a∗ + 1.75L∗ )
X = . (10)
(5.645 L∗ + a∗ − 3.02b∗ )
Increasing the plant extract in mixtures formed from starch and mango peel extract causes the color
to turn yellow, as indicated by Hue and Chroma, and this is attributed to the higher concentrations of
carotenoid and flavonoid compounds [195]. Alves et al., [159] found that little changes in color are
observed by introducing essential oil in combination. Values of a* and b* are near zero, which gives
the film a gray color.

Thermogravimetric Analysis
Similar to any polymers, biopolymers are sensitive to temperature; hence, thermostability
represents an important parameter. In fact, thermogravimetric analysis stands as the thermal
fingerprint of edible films/coatings. The thermogravimetric curves (TG—thermogravimetric analysis
and DTG—differential thermal analysis) usually used in the film characterization of the films
are recorded on a thermogravimetric analyzer under different atmospheres (more often nitrogen).
The samples were heated from near ambient temperature to 500–800 ◦ C at x ◦ C/min. A typical
thermogram is presented in Figure 17. From these curves, the moment of water desorption, plasticizer
volatilization, and at higher temperature, the polymer decomposition can be specified [202]. It is an
important tool to assess the differences between formulations in a series or when the basal formulation
is preserved and only some ingredients are added [96,124,200,203,204].

Film Morphology
The morphology of composite edible films is examined using a scanning electron microscope
(SEM) under 500 magnifications or higher. It is a very useful technique for taking a closer look
at the surface of edible barriers in order to observe any cracks, breaks, openings on the surfaces,
or particular morphologies that can appear by mixing several ingredients [33,93,198,201,205–208].
The goal is to obtain a homogeneous surface without defects.
Coatings 2020, 10, 687 27 of 45
Coatings 2020, 10, x FOR PEER REVIEW 29 of 48

Figure 17. Typical thermal analysis of edible films.

Figure 17. Typical thermal analysis of edible films.
FTIR Spectroscopy
FTIRFourier-transform
Spectroscopy infrared spectroscopy (FTIR) is a very useful method to record the infrared
spectrum of prepared films.
Fourier-transform infrared Anspectroscopy
FTIR spectrometer (FTIR) is collects
a veryhigh-definition
useful method data in a large
to record range
the infrared
of
spectrum of prepared films. An FTIR spectrometer collects high-definition data in a large range or
spectra, and the operating parameters are attenuated total reflection (ATR) mode, absorption of
transmission −1 (room temperature, x = 110–120
spectra, and mode, wavenumber
the operating ranging
parameters arefrom 4000 tototal
attenuated 400 cm reflection (ATR) mode, absorption or
number of accumulated
transmission scans, resolution
mode, wavenumber ranging cm−1 ).4000
of 4from Fourier-transform
to 400 cm −1 (room infrared spectroscopy
temperature, x =(FTIR) is
110–120
used to identify the absorption bands that result from the vibrations of
number of accumulated scans, resolution of 4 cm ). Fourier-transform infrared spectroscopy (FTIR)
−1 functional groups presented in
macromolecules.
is used to identifyUsually in the case
the absorption of polysaccharides
bands that result from butthealso in the case
vibrations of all compounds
of functional groupscontaining
presented
–OH groups, a strong band at approximately 3300 cm −1 is observed. If water is trapped in the film
in macromolecules. Usually in the case of polysaccharides but also in the case of all compounds
structure, a band can appear at 1750–1540 −1 . Polysaccharides adsorb cm−1
containing –OH groups, a strong band atcm approximately strongly If
3300 cm−1 is observed. inwater
the 1200–900
is trapped in
region due to C–O–C glycosidic linkage [91,177,209–211]. In chitosan and
the film structure, a band can appear at 1750–1540 cm . Polysaccharides adsorb strongly in the 1200–
−1 proteins, stronger bands
appear
900 cm−1atregion
approximately
due to C–O–C cm−1 , 1547linkage
1651 glycosidic cm−1 , [91,177,209–211].
and 1320 cm−1 correspondingIn chitosan andtoproteins,
C=O stretching
stronger
(amide I), N–Hatbending
bands appear (amide 1651
approximately II), and
cmto −1, C–N
1547 stretching
cm−1, and 1320 (amide cm−1III) [174,177,212].toThe
corresponding C=Opositions of
stretching
these
(amide I), N–H bending (amide II), and to C–N stretching (amide III) [174,177,212]. The positions in
bands are subject to shift due to new bond formation in the frame of complex mixtures used of
edible films/coatings.
these bands are subject This technique
to shift due toisnew verybonduseful to assessinthe
formation thedifferences betweenmixtures
frame of complex formulations if
used in
some
edibleingredients are changed,
films/coatings. as observed
This technique is very byuseful
Zhangtoetassessal. [97].
the differences between formulations if
some ingredients are changed, as observed by Zhang et al. [97].
X-ray Difraction
X-ray Difraction
X-ray diffraction is a characterization technique for different materials that permits the identification
of crystal structures
X-ray diffraction and is
interatomic distances. technique
a characterization That is possible, since the materials
for different X-ray wavelength is similar
that permits the
to the distances between atoms. The analysis can be applied using an X-ray
identification of crystal structures and interatomic distances. That is possible, since the diffractometer, which is
X-ray
usually
wavelengthprovided with to
is similar a tube, a copper between
the distances anode, and a detector
atoms. operating
The analysis canatbe40–45 kV and
applied 30–40
using mA,
an X-ray
and the range of 2θ and speed are selected according to applications. Diffractograms
diffractometer, which is usually provided with a tube, a copper anode, and a detector operating at of edible
films
40–45(single
kV and or 30–40
multi-component)
mA, and thereveal
range aofcombination
2θ and speed between amorphous
are selected and crystalline
according areas
to applications.
(Figure 18) with high
Diffractograms variations
of edible depending
films (single on some factors, including
or multi-component) the biopolymer
reveal a combination type and
between sources,
amorphous
plasticizers, film drying regime, moisture content, etc. Chitosan diffractograms present
and crystalline areas (Figure 18) with high variations depending on some factors, including the semi-crystalline
features
biopolymerwith type
two diffraction peaks
and sources, (2θ = 11◦ and
plasticizers, 20◦drying
film ) [213]. regime,
In addition, a partially
moisture crystalline
content, pattern
etc. Chitosan
was observed in a large number of finished films/coatings, which suggests that
diffractograms present semi-crystalline features with two diffraction peaks (2θ = 11° and 20°) is the main feature
[213].
of these materials [57,95,193,204,214]. Usually by mixing different ingredients, the diffraction
In addition, a partially crystalline pattern was observed in a large number of finished films/coatings, bands
existing in diffractograms
which suggests sustain
that is the mainsome attenuation,
feature of these diminishing, scattering, and broadening,
materials [57,95,193,204,214]. Usually by which are
mixing
all clear indications of the crystallinity lowering.
different ingredients, the diffraction bands existing in diffractograms sustain some attenuation,
diminishing, scattering, and broadening, which are all clear indications of the crystallinity lowering.
Coatings
Coatings 10, x10,
2020,2020, FOR687PEER REVIEW 28 of 30
45 of 48

Figure 18. X-ray diffraction patterns of starch films emphasizing the amorphous and crystalline area.
Figure 18. X-ray diffraction patterns of starch films emphasizing the amorphous and crystalline area.
Antioxidant and Antimicrobial Activity
Antioxidant andevaluation
For the Antimicrobial Activityactivity, some global parameters measured through colorimetric
of antioxidant
methods are used:
For the evaluation of antioxidant activity, some global parameters measured through
colorimetric
• Totalmethods
phenolic are used:(TPC) (Folin–Ciocalteu reagent) data are expressed in equivalents of mg
contents
of gallic acid for 100 g of film (mg GAE/100 g film) [78,118–120,155,156,215–228].
• Total phenolic contents (TPC) (Folin–Ciocalteu reagent) data are expressed in equivalents of mg
• Total flavonoids (aluminum chloride reagent) data are expressed in mg of quercetin equivalents
of gallic acid for 100 g of film (mg GAE/100 g film) [78,118–120,155,156,215–228].
for 100 g of film (mg QE/100 g film) [46,140,163,188,216,217,229–233]
• Total flavonoids (aluminum chloride reagent) data are expressed in mg of quercetin equivalents
• DPPH method (1,1-diphenyl-2-picrylhydrazyl radical reagent–DPPH) data are expressed in mg of
for 100 g ofacid
ascorbic filmequivalents
(mg QE/100 g film)
for 100 [46,140,163,188,216,217,229–233]
g of film (AAE/100 g of film) [30,32,37,47,72,160,162,163,169,199,233–239]
• DPPH
• method (1,1-diphenyl-2-picrylhydrazyl radical reagent
ABTS (2,20-azino-bis (3-ethylbenzothiazoline-6-sulphonic - DPPH) data
acid reagent–ABTS) dataare
areexpressed in mg
expressed in
of mg ascorbic
of ascorbicacid equivalents
acid equivalents for 100 gfor 100
of film g gofof film)
(AAE/100 film[32,47,166,174,211,235,239,240]
(AAE/100 g of film)
[30,32,37,47,72,160,162,163,169,199,233–239]
• ABTS Antibacterial activity(3-ethylbenzothiazoline-6-sulphonic
(2,20-azino-bis is performed by the assessment of the acidzone of inhibition
reagent – ABTS) assay on are
data
a solid medium placed in Petri dishes and containing specific media for each microorganism
expressed in mg of ascorbic acid equivalents for 100 g of film (AAE/100 g of film)
tested [74,125,129,141,171,176,179,187,213,238,241–259].
[32,47,166,174,211,235,239,240]
Strawberries, as one of the most highly consumed and also perishable fruits, require
Antibacterial
special attentionactivity
in termsis performed by the assessment
of edible coatings. Composite of the obtained
films zone of inhibition assay on a solid
using chitosan–banana
medium placed in Petri dishes and containing specific media for each microorganism
starch–Aloe vera gel (optimum value 20%) permit an important increase in shelf life up to 15 days tested
in the case of refrigerated strawberries
[74,125,129,141,171,176,179,187,213,238,241–259]. [260]. A special case [188] is the use of a nanoemulsion of
water in oil (W/O), which is composed from orange essential oil (70%), xoconostle cactus pear extract
Strawberries, as one of the most highly consumed and also perishable fruits, require special
(10%), and liquid soy lecithin (20%) incorporated into a starch–glycerol–whey protein film formulation.
attention in terms of edible coatings. Composite films obtained using chitosan–banana starch–Aloe
Different amounts of nanoemulsion (0–0.8%) were introduced into the films to evaluate their antioxidant
vera gel
and (optimum
antibacterialvalue 20%)
activity permit
as well an important
as mechanical increase
properties, and it inwas
shelf life that
found up to0.8%15ofdays in the case of
nanoemulsion
refrigerated strawberries
was the optimal value. [260]. A special case [188] is the use of a nanoemulsion of water in oil (W/O),
which is composed from orange
Egg white–sorbitol essential essential
(3% w/w)–orange oil (70%),oil xoconostle
(2% v/v) filmscactus pear extract
were prepared for the (10%), and liquid
preservation
soy lecithin
of ‘kashar(20%)
cheese’incorporated
for 30 days atinto4 C a[167].
◦ starch–glycerol–whey
The orange essential protein film formulation.
oil composition consists mainly Different
of
amounts
limoneneof nanoemulsion
(84.2%), sabinen(0–0.8%) were introduced
(3.2%), myrecene (1.2%), etc.,into
which the
arefilms
known tofor
evaluate their antioxidant
their antimicrobial activity. and
antibacterial activity
Three cheese as well
samples wereasartificially
mechanical properties, with
contaminated and dangerous
it was found that 0.8%
bacteria E. coli,ofL.nanoemulsion
monocytogenes, was
the optimal value.
and S. aureus. Two of them were covered with prepared films (with and without essential oil), while one
remained as the control. It was found that in the essential oil-treated
Egg white–sorbitol (3% w/w)–orange essential oil (2% v/v) films were prepared sample, the bacterial growth was for the
inhibited rapidly (7 days for L. monocytogenes and S. aureus and 15 days for E. coli), while for the sample
preservation of ‘kashar cheese’ for 30 days at 4 °C [167]. The orange essential oil composition consists
without essential oil, the growth decreased more slowly. As expected, the bacterial growth remained
mainly of limonene (84.2%), sabinen (3.2%), myrecene (1.2%), etc., which are known for their
high in the unprotected sample.
antimicrobial activity. Three cheese samples were artificially contaminated with dangerous bacteria
For Turkish ‘lor cheese’ protection, Kavas et al. [261] used an edible film based on egg white
E. coli, L. monocytogenes,
proteins. The testing of and S. aureus.
the prepared Twosolutions
coating of themwas were covered
performed bywith preparedlorfilms
contaminating cheese (with
with and
without essential
E. coli O157: H7 oil),
(ATCCwhile one remained
43895), as the(ATCC
L. monocytogenes control. It was
19118), andfound that(ATCC
S. aureus in the 6538):
essential oil-treated
‘lor cheese’
sample, theimmersion
(50 g), bacterialintogrowth was (15
inoculum inhibited rapidly
min), first (7 days
immersion into for L. monocytogenes
coating and in
solution (90 s), hold S. air
aureus and 15
(3 min),
days for E. coli), while for the sample without essential oil, the growth decreased more slowly. As
expected, the bacterial growth remained high in the unprotected sample.
For Turkish ‘lor cheese’ protection, Kavas et al. [261] used an edible film based on egg white
proteins. The testing of the prepared coating solutions was performed by contaminating lor cheese
with E. coli O157: H7 (ATCC 43895), L. monocytogenes (ATCC 19118), and S. aureus (ATCC 6538): ‘lor
Coatings 2020, 10, 687 29 of 45

second immersion into coating solution (60 s), drying (10 ◦ C/4–5 h), and storage at 4 ◦ C for 30 days.
The coating thickness was higher for samples with balm oil (2%), and therefore, the WVP was lower.
The presence of bactericidal compounds in coatings stopped the development of the microorganisms
from day one, and the optimal concentration of essential oil was 2%.
Garlic and oregano oils were used as adjuvants to “achira” starch (Canna indica L.) coatings
for double cream cheese protection during storage at 5 ◦ C for 42 days [262]. Comparing with
control, the two types of films were suitable to preserve the product and eliminate the presence
of pathogenic microorganisms. Oregano oil-based films convey lower hardness to cheese samples
compared with garlic oil treatment and control.
Mango fruits were preserved from getting spoiled by using starch solutions (2%) from the pulp of
banana, soursop, and stenospermocarpic mango (a fruit smaller than normal mango) [263]. The starch
extends the shelf life of fruits up to 15 days with no signs of losing the organoleptic characteristics.
Millet starch-based edible films incorporating clove oil (60% eugenol as the main ingredient)
in different amounts (1%, 2%, and 3%) have bactericidal activity toward different microorganisms:
Syzygium aromatic, Staphylococcus aureus, Escherichia coli, Pseudomonas aeruginosa, Enterobacter sp.,
and B. cereus [149]. A Box–Behnken experimental design (BBD) was used to optimize the preparation
process of edible coating for protecting ‘Cripps pink’ apples [224]. The independent variables were
percent of starch, carrageenan, sucrose fatty acid ester, and glycerol, while the dependent variables
were thickness, WVP, solubility, TS, and EAB. Response surface methodology gave the optimum
solution for preserving apple qualities: starch 2.5% carrageenan 1.5%, sucrose fatty acid ester 2%,
and glycerol 1.5%.
The antioxidant activity of starch films was also improved using microencapsulated ascorbic
acid [264], embedding carvacrol and citral [184], the addition of nystose from Bacillus subtilis natto [265],
Aloe vera gel [161], turmeric [36], thyme extracts [199], natural plant extracts (epigallocatechin gallate,
blueberry ash, fruit extract, macadamia peel extract, and banana peel extract [163,266].
Gelatin films containing chitosan nanoparticles enriched with tea polyphenols were proven to
be suitable for food protection, especially in the context of an innovative electrospray preparation
method [23]. This technique is suitable for the better incorporation of polyphenols in chitosan, which is
known as a good carrier for different compounds. The preparation of chitosan microcapsules was
followed by incorporation in gelatin and film preparation. The gelatin used was provided by grass
carp skin, which is one of the main by-products of fish processing in China.
Ferulago angulata essential oil (1–3%) and chitosan (approximately 450 kDa) were used as coatings
for preserving trout during 16 days storage at 4 ◦ C [139]. The formulation with 3% essential oil
presented superior properties.
Aloe vera gel [142,161,260,267,268] represents an important ingredient in chitosan-based
formulations, since this extract has multiple benefits: anti-inflammatory, detoxifying, lowering
cholesterol, improving metabolism, anti-ulceration, improving oral health, fighting cold and cough,
etc. Therefore, besides edible coatings, aloe vera gel is both food and medicine, which is probably due
to the content of glycosides aloin A and B (15–40%) [269].
Other adjuvants for improving the properties of chitosan edible coatings were also used. Pickering
emulsions formed by chitosan–cellulose nanocrystals–oleic acid (10 or 20 g oleic acid/kg emulsion)
were used for ‘Bartlett’ pears ripening prevention [270]. Chitosan–lemon verbena extract/essential oil
for trout (Oncorhynchus mykiss) preservation [142].
Mango fruit was protected against fungi (Phomopsis sp. RP257 and Pestalotiopsis sp.) using a
system composed of chitosan and lactoperoxidase [242].
Strawberries were protected by a mixture of chitosan–chitosan nanoparticles–propolis
extract (10–30%) [217]. Chitosan nanoemulsions prepared by high-energy or low-energy
methods represent an advanced edible coating for food [129]. In addition, it was found that
chitosan–beeswax–carboxymethylcellulose are very efficient coatings for Kinnow mandarin fruits [68].
An interesting approach [27] was to produce coatings from mixtures of gelatin–furcellaran–pu-erh
Coatings 2020, 10, 687 30 of 45

tea extract–green tea extract (GTE). Furcellaran is a naturally occurring polysaccharide that can
be extracted from red seaweeds (Rhodophyceae). Jamróz et al. evaluated the coating properties:
physical (color, swelling, thickness, water content), antioxidant (TPC, DPPH, ABTS), antimicrobial
(Staphylococcus aureus, Escherichia coli, Henseniaspora uvarum and Candidia albicans). Tensile strength
increased from 9.62 to 24.14 when GTE was introduced, and a significant inhibition zone of 25 mm
appeared against S. aureus. Moreover, it can be considered an intelligent film due to the capability
of color changing at different pH values (no color at pH = 3 and orange at pH = 12). This feature is
important for fish preservation tests.

5. Statistical Analysis. Design of Experiments (DOE)

In order to manage complex mixtures and processes for obtaining edible films/coatings,
it is necessary to optimize the process, and this task require several steps:
Screening–where the factors that influence significantly the preparation are identified (modality
of completion: fractional factorial [107])
Improvement–a process through which the near optimum parameters are founded by changing
the factor settings (modality of completion: Box/simplex or steepest ascent approach)
Optimization–where optimal settings are founded (modality of completion: response surface
designs such as CCD or Box–Behnken [126]).
Response surface design stands for an advanced design of experiments (DOE). Several types
of software are used for fulfilling these tasks: JMP, Minitab, Design Expert, etc. These programs
have implemented the methodology to perform the laborious statistical analysis required. Basically,
these procedures offer information of the effect of input variables/factors (temperature, pH, composition
etc.) to output variables/response (thickness, TS, WVP, EM, EAB, etc.) and also the reciprocal effects of
independent variables (taken two at a time) on the final product quality (Figure 19). Factors can take
only a few potential values called factor levels. Response surface methodologies are divided in two
categories:

• Central composite designs;

• Box–Behnken designs.
Coatings 2020, 10, x FOR PEER REVIEW 33 of 48

Figure19.
Figure 19. Example
Example ofof response
response surface
surface plots
plots emphasizing
emphasizing the
the influence
influence of
ofindependent
independentvariables
variables
(factors) interaction on the output variables (response).
(factors) interaction on the output variables (response).

6. Conclusions
Edible films/coatings are efficient ways to prevent the spoilage of different foods. Important
achievements in this industry are exponentially increased by the number of ingredients and their
combinations, which can be used and tailored to adapt to any kind of edible protection for fast/slow
Coatings 2020, 10, 687 31 of 45

Central composite designs are used because they provide a uniform precision of estimates effect,
unlike Box–Behnken designs, which are less precise but need fewer design points and consequently
are less expensive to run using an equal number of factors such as CCD.
Box–Behnken designs can use up to 3 levels per factor, while CCD can use up to 5.
For predicting the experimental output, a second-order polynomial model is usually used.
Xk Xk Xk X Xk
Ŷ = β0 + βi Xi + βii Xi + βii Xi2 + βij Xi X j (11)
i=1 i=1 i=1 i< j = 1

where Y is the predicted value of the response; β0 , βi , βii , and βij are the regression
coefficients; k is the number of independent parameters; and Xi and Xj are the coded levels of
the experimental conditions.

6. Conclusions
Edible films/coatings are efficient ways to prevent the spoilage of different foods. Important
achievements in this industry are exponentially increased by the number of ingredients and their
combinations, which can be used and tailored to adapt to any kind of edible protection for fast/slow
perishable food. The investigations pursued by different research teams aim to optimize the formulation
compositions. Particular attention is attributed to mechanical properties, which require a delicate
harmonization between resistance and elasticity. In addition, antioxidant and antimicrobial features
are mandatory for these ecological envelopments; hence, numerous studies report the utilization of
diverse types of essential oils and plant extracts. The possibility of obtaining an edible layer from other
ready-to-use waste (shrimp shell, fruits peels, pomace, etc.) significantly increases the practice of food
protection in this manner.
Experimental designs are extensively used to obtain the best result from complex edible coatings
and to carefully assess the beneficial or detrimental role of each component. Along with matrix
characteristics, application methods represent an important challenge, especially when the transition
from lab scale to industrial scale is required.
Another challenge in achieving effective edible layers on food is the increasingly frequent
introduction of different types of nanoparticles (silver, ZnO, silica, etc.), which, besides beneficial effects,
can bring new issues regarding consumer protections. Regulatory requirements for the presence of
nanoparticles in this field may become a difficult task for researchers in the future.

Author Contributions: Conceptualization, S.M.A., A.O., I.M.; formal analysis, S.M.A., C.B., C.V.P., and I.M.;
funding acquisition, S.M.A., A.O.; investigation C.B., C.V.P.; methodology, S.M.A., A.O., and G.T.; supervision
S.M.A.; writing—original draft, S.M.A., A.O., C.B., C.V.P., and G.T.; writing—review and editing, S.M.A., A.O.,
and I.M. All authors have read and agreed to the published version of the manuscript.
Funding: This research was funded by the project SusMAPWaste, SMIS104323, Contract No. 89/09.09.2016,
from the Operational Program Competitiveness 2014–2020, project co financed from the European Regional
Development Fund.
Conflicts of Interest: The authors declare no conflicts of interest.

References
1. Gustavsson, J.; Cederberg, C.; Sonesson, U. Global Food Losses and Food Waste–Extent, Causes and Prevention;
FAO: Rome, Italy, 2011.
2. Fierascu, R.C.; Fierascu, I.; Avramescu, S.M.; Sieniawska, E. Recovery of natural antioxidants from
agro-industrial side streams through advanced extraction techniques. Molecules 2019, 24, 4212. [CrossRef]
[PubMed]
3. Zhai, X.; Li, Z.; Zhang, J.; Shi, J.; Zou, X.; Huang, X.; Zhang, D.; Sun, Y.; Yang, Z.; Holmes, M.; et al.
Natural biomaterial-based edible and pH-sensitive films combined with electrochemical writing for intelligent
food packaging. J. Agric. Food Chem. 2018, 66, 12836–12846. [CrossRef] [PubMed]
Coatings 2020, 10, 687 32 of 45

4. Enfrin, M.; Dumee, L.F.; Lee, J. Nano/microplastics in water and wastewater treatment processes–Origin,
impact and potential solutions. Water Res. 2019, 161, 621–638. [CrossRef] [PubMed]
5. Jang, Y.-C.; Lee, G.; Kwon, Y.; Lim, J.-H.; Jeong, J.-H. Recycling and management practices of plastic packaging
waste towards a circular economy in South Korea. Resour. Conserv. Recycl. 2020, 158. [CrossRef]
6. Fierascu, R.C.; Sieniawska, E.; Ortan, A.; Fierascu, I.; Xiao, J. Fruits by-products–A source of valuable active
principles. A short review. Front. Bioeng. Biotechnol. 2020, 8. [CrossRef]
7. Yeddes, W.; Djebali, K.; Aidi Wannes, W.; Horchani-Naifer, K.; Hammami, M.; Younes, I.; Saidani Tounsi, M.
Gelatin-chitosan-pectin films incorporated with rosemary essential oil: Optimized formulation using mixture
design and response surface methodology. Int. J. Biol. Macromol. 2020, 154, 92–103. [CrossRef]
8. Valerio, F.; Volpe, M.G.; Santagata, G.; Boscaino, F.; Barbarisi, C.; Di Biase, M.; Bavaro, A.R.; Lonigro, S.L.;
Lavermicocca, P. The viability of probiotic Lactobacillus paracasei IMPC2.1 coating on apple slices during
dehydration and simulated gastro-intestinal digestion. Food Biosci. 2020, 34. [CrossRef]
9. Khanzadi, S.; Keykhosravy, K.; Hashemi, M.; Azizzadeh, M. Alginate coarse/nanoemulsions containing
Zataria multiflora Boiss essential oil as edible coatings and the impact on microbial quality of trout fillet.
Aquac. Res. 2020, 51, 873–881. [CrossRef]
10. Shamshina, J.L.; Kelly, A.; Oldham, T.; Rogers, R.D. Agricultural uses of chitin polymers. Environ. Chem. Lett.
2019, 18, 53–60. [CrossRef]
11. Puscaselu, R.; Gutt, G.; Amariei, S. Rethinking the future of food packaging: Biobased edible films for
powdered food and drinks. Molecules 2019, 24, 3136. [CrossRef]
12. Pina-Barrera, A.M.; Alvarez-Roman, R.; Baez-Gonzalez, J.G.; Amaya-Guerra, C.A.; Rivas-Morales, C.;
Gallardo-Rivera, C.T.; Galindo-Rodriguez, S.A. Application of a multisystem coating based on polymeric
nanocapsules containing essential oil of thymus vulgaris L. to increase the shelf life of table grapes (Vitis
Vinifera L.). IEEE Trans. Nanobiosci. 2019, 18, 549–557. [CrossRef] [PubMed]
13. Jeevahan, J.; Chandrasekaran, M. Nanoedible films for food packaging: A review. J. Mater. Sci. 2019, 54,
12290–12318. [CrossRef]
14. Sofi, S.A.; Singh, J.; Rafiq, S.; Ashraf, U.; Dar, B.N.; Nayik, G.A. A comprehensive review on antimicrobial
packaging and its use in food packaging. Curr. Nutr. Food Sci. 2018, 14, 305–312. [CrossRef]
15. Singh, S.; Singh, G.; Arya, S.K. Mannans: An overview of properties and application in food products. Int. J.
Biol. Macromol. 2018, 119, 79–95. [CrossRef] [PubMed]
16. Umaraw, P.; Munekata, P.E.S.; Verma, A.K.; Barba, F.J.; Singh, V.P.; Kumar, P.; Lorenzo, J.M. Edible films/coating
with tailored properties for active packaging of meat, fish and derived products. Trends Food Sci. Technol.
2020, 98, 10–24. [CrossRef]
17. Imeson, A.P. Carrageenan and furcellaran. In Handbook of Hydrocolloids; Woodhead Publishing Limited:
Cambridge, UK, 2009; pp. 164–185.
18. Pavlath, A.; Orts, W. Edible films and coatings: Why, what, and how? In Edible Films and Coatings for Food
Applications; Springer: New York, NY, USA, 2009; pp. 1–23. [CrossRef]
19. Available online: https://www.grandviewresearch.com/industry-analysis/edible-packaging-market (accessed
on 14 July 2020).
20. Available online: https://www.mordorintelligence.com/industry-reports/edible-films-and-coating-market
(accessed on 14 July 2020).
21. Hernandez-Izquierdo, V.M.; Krochta, J. Thermoplastic processing of proteins for film formation—A review.
J. Food Sci. 2008, 73, R30–R39. [CrossRef] [PubMed]
22. Xiong, Y.; Chen, M.; Warner, R.D.; Fang, Z. Incorporating nisin and grape seed extract in chitosan-gelatine
edible coating and its effect on cold storage of fresh pork. Food Control 2020, 110. [CrossRef]
23. Wang, Y.; Zhang, R.; Qin, W.; Dai, J.; Zhang, Q.; Lee, K.; Liu, Y. Physicochemical properties of gelatin films
containing tea polyphenol-loaded chitosan nanoparticles generated by electrospray. Mater. Des. 2020, 185.
[CrossRef]
24. Pella, M.C.G.; Silva, O.A.; Pella, M.G.; Beneton, A.G.; Caetano, J.; Simoes, M.R.; Dragunski, D.C. Effect
of gelatin and casein additions on starch edible biodegradable films for fruit surface coating. Food Chem.
2020, 309, 125764. [CrossRef]
25. Khojah, S.M. Bio-based coating from fish gelatin, K-carrageenan and extract of pomegranate peels for
maintaining the overall qualities of fish fillet. J. Aquat. Food Prod. Technol. 2020, 1–13. [CrossRef]
Coatings 2020, 10, 687 33 of 45

26. Scartazzini, L.; Tosati, J.V.; Cortez, D.H.C.; Rossi, M.J.; Flores, S.H.; Hubinger, M.D.; Di Luccio, M.;
Monteiro, A.R. Gelatin edible coatings with mint essential oil (Mentha arvensis): Film characterization
and antifungal properties. J. Food Sci. Technol. 2019, 56, 4045–4056. [CrossRef] [PubMed]
27. Jamroz, E.; Kulawik, P.; Krzysciak, P.; Talaga-Cwiertnia, K.; Juszczak, L. Intelligent and active
furcellaran-gelatin films containing green or pu-erh tea extracts: Characterization, antioxidant
and antimicrobial potential. Int. J. Biol. Macromol. 2019, 122, 745–757. [CrossRef] [PubMed]
28. Handayasari, F.; Suyatma, N.E.; Nurjanah, S. Physiochemical and antibacterial analysis of gelatin–chitosan
edible film with the addition of nitrite and garlic essential oil by response surface methodology. J. Food
Process. Preserv. 2019, 43. [CrossRef]
29. Char, C.; Padilla, C.; Campos, V.; Pepczynska, M.; Calderón, P.D.; Enrione, J.I. Characterization and testing of
a novel sprayable crosslinked edible coating based on salmon gelatin. Coatings 2019, 9, 595. [CrossRef]
30. Belan, D.L.; Flores, F.P.; Mopera, L.E. Optimization of antioxidant capacity and tensile strength
of gelatin-carboxymethylcellulose film incorporated with bignay (Antidesma bunius (L.) Spreng.) crude
phenolic extract. AIP Conf. Proc. 2018. [CrossRef]
31. Zhang, L.; Liu, A.; Wang, W.; Ye, R.; Liu, Y.; Xiao, J.; Wang, K. Characterisation of microemulsion nanofilms
based on Tilapia fish skin gelatine and ZnO nanoparticles incorporated with ginger essential oil: Meat
packaging application. Int. J. Food Sci. Technol. 2017, 52, 1670–1679. [CrossRef]
32. Yang, H.-J.; Lee, J.-H.; Lee, K.-Y.; Bin Song, K. Application of gelatin film and coating prepared from
dried alaska pollock by-product in quality maintanance of grape berries. J. Food Process. Preserv. 2017, 41.
[CrossRef]
33. Wang, W.; Wang, K.; Xiao, J.; Liu, Y.; Zhao, Y.; Liu, A. Performance of high amylose starch-composited gelatin
films influenced by gelatinization and concentration. Int. J. Biol. Macromol. 2017, 94, 258–265. [CrossRef]
34. Krishna, M.; Nindo, C.I.; Min, S.C. Development of fish gelatin edible films using extrusion and compression
molding. J. Food Eng. 2012, 108, 337–344. [CrossRef]
35. Xiong, Y.; Deng, B.; Warner, R.D.; Fang, Z. Reducing salt content in beef frankfurter by edible coating to
achieve inhomogeneous salt distribution. Int. J. Food Sci. Technol. 2020. [CrossRef]
36. Tosati, J.V.; Messias, V.C.; Carvalho, P.I.N.; Rodrigues Pollonio, M.A.; Meireles, M.A.A.; Monteiro, A.R.
Antimicrobial effect of edible coating blend based on turmeric starch residue and gelatin applied onto fresh
frankfurter sausage. Food Bioprocess. Technol. 2017, 10, 2165–2175. [CrossRef]
37. Liang, C.; Jia, M.; Tian, D.; Tang, Y.; Ju, W.; Ding, S.; Tian, L.; Ren, X.; Wang, X. Edible sturgeon skin gelatine
films: Tensile strength and UV light-barrier as enhanced by blending with esculine. J. Funct. Foods 2017, 37,
219–228. [CrossRef]
38. Madhu, B.; Jagannadha Rao, P.V.K.; Patel, S. Moisture sorption isotherms of edible coated solid sugarcane
jaggery. Sugar Tech. 2019, 22, 319–327. [CrossRef]
39. Namratha, S.; Sreejit, V.; Preetha, R. Fabrication and evaluation of physicochemical properties of probiotic
edible film based on pectin–alginate–casein composite. Int. J. Food Sci. Technol. 2020, 55, 1497–1505.
[CrossRef]
40. Volpe, S.; Cavella, S.; Torrieri, E. Biopolymer coatings as alternative to modified atmosphere packaging for
shelf life extension of minimally processed apples. Coatings 2019, 9, 569. [CrossRef]
41. Lopes, A.C.A.; Eda, S.H.; Andrade, R.P.; Amorim, J.C.; Duarte, W.F. New alcoholic fermented
beverages—potentials and challenges. In Fermented Beverages; Woodhead Publishing Limited: Cambridge,
UK, 2019; pp. 577–603.
42. Fernandes, L.; Pereira, E.L.; Do Céu Fidalgo, M.; Gomes, A.; Ramalhosa, E. Physicochemical properties
and microbial control of chestnuts (Castanea sativa) coated with whey protein isolate, chitosan and alginate
during storage. Sci. Hortic. 2020, 263. [CrossRef]
43. Song, J.; Jiang, B.; Wu, Y.; Chen, S.; Li, S.; Sun, H.; Li, X. Effects on surface and physicochemical properties of
dielectric barrier discharge plasma-treated whey protein concentrate/wheat cross-linked starch composite
film. J. Food Sci. 2019, 84, 268–275. [CrossRef]
44. Pereira, J.O.; Soares, J.; Monteiro, M.J.P.; Amaro, A.; Gomes, A.; Pintado, M. Cereal bars functionalized
through Bifidobacterium animalis subsp. lactis BB-12 and inulin incorporated in edible coatings of whey
protein isolate or alginate. Food Funct. 2019, 10, 6892–6902. [CrossRef]
45. Galus, S.; Lenart, A. Optical, mechanical, and moisture sorption properties of whey protein edible films.
J. Food Process. Eng. 2019, 42. [CrossRef]
Coatings 2020, 10, 687 34 of 45

46. Castro, F.V.R.; Andrade, M.A.; Sanches Silva, A.; Vaz, M.F.; Vilarinho, F. The contribution of a whey protein
film incorporated with green tea extract to minimize the lipid oxidation of salmon (salmo salar L.). Foods 2019,
8, 327. [CrossRef]
47. Andrade, M.A.; Ribeiro-Santos, R.; Costa Bonito, M.C.; Saraiva, M.; Sanches-Silva, A. Characterization of
rosemary and thyme extracts for incorporation into a whey protein based film. LWT 2018, 92, 497–508.
[CrossRef]
48. Azevedo, V.M.; Borges, S.V.; Marconcini, J.M.; Yoshida, M.I.; Neto, A.R.S.; Pereira, T.C.; Pereira, C.F.G. Effect
of replacement of corn starch by whey protein isolate in biodegradable film blends obtained by extrusion.
Carbohydr. Polym. 2017, 157, 971–980. [CrossRef] [PubMed]
49. Ahmed, Z.S.; Badr, K.R.; ElGamal, M.S. Evaluation of the antimicrobial action of whey protein edible films
incorporated with cinnamon, cumin and thyme against spoilage flora of fresh beef. Int. J. Agric. Res. 2014, 9,
242–250. [CrossRef]
50. Fernandez-Pan, I.; Royo, M.; Ignacio Mate, J. Antimicrobial activity of whey protein isolate edible films with
essential oils against food spoilers and foodborne pathogens. J. Food Sci. 2012, 77, M383–M390. [CrossRef]
[PubMed]
51. Gadang, V.P.; Hettiarachchy, N.S.; Johnson, M.G.; Owens, C. Evaluation of antibacterial activity of whey
protein isolate coating incorporated with nisin, grape seed extract, malic acid, and EDTA on a Turkey
frankfurter system. J. Food Sci. 2008, 73, M389–M394. [CrossRef]
52. Gregirchak, N.; Stabnikova, O.; Stabnikov, V. Application of lactic acid bacteria for coating of wheat bread to
protect it from microbial spoilage. Plant. Foods Hum. Nutr. 2020. [CrossRef]
53. Chasquibol, N.A.; Gallardo, G.; Gomez-Coca, R.B.; Trujillo, D.; Moreda, W.; Perez-Camino, M.C.
Glyceridic and unsaponifiable components of microencapsulated sacha inchi (Plukenetia huayllabambana L.
and Plukenetia volubilis L.) edible oils. Foods 2019, 8, 671. [CrossRef]
54. Soukoulis, C.; Yonekura, L.; Gan, H.H.; Behboudi-Jobbehdar, S.; Parmenter, C.; Fisk, I. Probiotic edible films
as a new strategy for developing functional bakery products: The case of pan bread. Food Hydrocoll. 2014, 39,
231–242. [CrossRef]
55. Yu, D.; Regenstein, J.M.; Xia, W. Bio-based edible coatings for the preservation of fishery products: A review.
Crit. Rev. Food Sci. Nutr. 2019, 59, 2481–2493. [CrossRef]
56. Lacroix, M.; Vu, K.D. Edible coating and film materials. In Innovations in Food Packaging; Elsevier Science &
Technology Books: Amsterdam, The Netherlands, 2014; pp. 277–304.
57. Han, K.; Liu, Y.; Liu, Y.; Huang, X.; Sheng, L. Characterization and film-forming mechanism of egg
white/pullulan blend film. Food Chem. 2020, 315, 126201. [CrossRef]
58. Handa, A.; Gennadios, A.; Froning, G.W.; Kuroda, N.; Hanna, M.A. Tensile, solubility, and electrophoretic
properties of egg white films as affected by surface sulfhydryl groups. J. Food Sci. 1999, 64, 82–85. [CrossRef]
59. Gennadios, A.; Handa, A.; Froning, G.W.; Weller, C.L.; Hanna, M.A. Physical properties of egg
white—Dialdehyde starch films. J. Agric. Food Chem. 1998, 46, 1297–1302. [CrossRef]
60. Gennadios, A.; Weller, C.L.; Hanna, M.A.; Froning, G.W. Mechanical and barrier properties of egg albumen
films. J. Food Sci. 1996, 61, 585–589. [CrossRef]
61. Rhim, J.W.; Gennadios, A.; Fu, D.; Weller, C.L.; Hanna, M.A. Properties of ultraviolet irradiated protein films.
LWT–Food Sci. Technol. 1999, 32, 129–133. [CrossRef]
62. Sothornvit, R. Edible film formation and properties from different protein sources and orange coating
application. Acta Hortic. 2005, 682, 1731–1738. [CrossRef]
63. Peng, N.; Gu, L.; Li, J.; Chang, C.; Li, X.; Su, Y.; Yang, Y. Films based on egg white protein and succinylated
casein cross-linked with transglutaminase. Food Bioprocess Technol. 2017, 10, 1422–1430. [CrossRef]
64. Huang, X.; Luo, X.; Liu, L.; Dong, K.; Yang, R.; Lin, C.; Song, H.; Li, S.; Huang, Q. Formation mechanism of
egg white protein/κ-Carrageenan composite film and its application to oil packaging. Food Hydrocoll. 2020,
105. [CrossRef]
65. Mecitoğlu, Ç.; Yemenicioğlu, A.; Arslanoğlu, A.; Elmacı, Z.S.; Korel, F.; Çetin, A.E. Incorporation of partially
purified hen egg white lysozyme into zein films for antimicrobial food packaging. Food Res. Int. 2006, 39,
12–21. [CrossRef]
66. Aguilar, K.C.; Tello, F.; Bierhalz, A.C.K.; Garnica Romo, M.G.; Martínez Flores, H.E.; Grosso, C.R.F. Protein
adsorption onto alginate-pectin microparticles and films produced by ionic gelation. J. Food Eng. 2015, 154,
17–24. [CrossRef]
Coatings 2020, 10, 687 35 of 45

67. Rondhi, M.; Utami Hatmi, R.; Apriyati, E.; Cahyaningrum, N.; Addy, H.S. Edible coating quality with three
types of starch and sorbitol plasticizer. E3S Web Conf. 2020, 142. [CrossRef]
68. Baswal, A.K.; Dhaliwal, H.S.; Singh, Z.; Mahajan, B.V.C.; Kalia, A.; Gill, K.S. Influence of carboxy
methylcellulose, chitosan and beeswax coatings on cold storage life and quality of Kinnow mandarin
fruit. Sci. Hortic. 2020, 260. [CrossRef]
69. Rinaudo, M. Physicochemical behaviour of semi-rigid biopolymers in aqueous medium. Food Hydrocoll.
2017, 68, 122–127. [CrossRef]
70. Joerger, R.D. Antimicrobial films for food applications: A quantitative analysis of their effectiveness.
Packag. Technol. Sci. 2007, 20, 231–273. [CrossRef]
71. Iñiguez-Moreno, M.; Ragazzo-Sánchez, J.A.; Barros-Castillo, J.C.; Sandoval-Contreras, T.; Calderón-Santoyo, M.
Sodium alginate coatings added with Meyerozyma caribbica: Postharvest biocontrol of Colletotrichum
gloeosporioides in avocado (Persea americana Mill. cv. Hass). Postharvest Biol. Technol. 2020, 163. [CrossRef]
72. Kaya, M.; Khadem, S.; Cakmak, Y.S.; Mujtaba, M.; Ilk, S.; Akyuz, L.; Salaberria, A.M.; Labidi, J.;
Abdulqadir, A.H.; Deligöz, E. Antioxidative and antimicrobial edible chitosan films blended with stem, leaf
and seed extracts of Pistacia terebinthus for active food packaging. Rsc Adv. 2018, 8, 3941–3950. [CrossRef]
73. Tumbarski, Y.; Petkova, N.; Todorova, M.; Ivanov, I.; Deseva, I.; Mihaylova, D.; Ibrahim, S.A. Effects of
pectin-based edible coatings containing a bacteriocin of bacillus methylotrophicus bm47 on the quality
and storage life of fresh blackberries. Ital. J. Food Sci. 2020, 32, 420–437.
74. Synowiec, A.; Gniewosz, M.; Kraśniewska, K.; Przybył, J.L.; Baczek, ˛ K.; W˛eglarz, Z. Antimicrobial
and antioxidant properties of pullulan film containing sweet basil extract and an evaluation of coating
effectiveness in the prolongation of the shelf life of apples stored in refrigeration conditions. Innov. Food Sci.
Emerg. Technol. 2014, 23, 171–181. [CrossRef]
75. Danalache, F.; Carvalho, C.Y.; Alves, V.D.; Moldao-Martins, M.; Mata, P. Optimisation of gellan gum edible
coating for ready-to-eat mango (Mangifera indica L.) bars. Int. J. Biol. Macromol. 2016, 84, 43–53. [CrossRef]
76. Golly, M.K.; Ma, H.; Sarpong, F.; Dotse, B.P.; Oteng-Darko, P.; Dong, Y. Shelf-life extension of grape (Pinot
noir) by xanthan gum enriched with ascorbic and citric acid during cold temperature storage. J. Food Sci.
Technol. 2019, 56, 4867–4878. [CrossRef]
77. Yin, P.; Dong, X.; Zhou, W.; Zha, D.; Xu, J.; Guo, B.; Li, P. A novel method to produce sustainable biocomposites
based on thermoplastic corn-starch reinforced by polyvinyl alcohol fibers. RSC Adv. 2020, 10, 23632–23643.
[CrossRef]
78. Kim, H.Y.; Lamsal, B.; Jane, J.l.; Grewell, D. Sheet-extruded films from blends of hydroxypropylated
and native corn starches, and their characterization. J. Food Process. Eng. 2019, 43. [CrossRef]
79. Islam, M.Z.; Saha, T.; Monalisa, K.; Hoque, M.M. Effect of starch edible coating on drying characteristics
and antioxidant properties of papaya. J. Food Meas. Charact. 2019, 13, 2951–2960. [CrossRef]
80. Ferreira, D.C.M.; Molina, G.; Pelissari, F.M. Effect of edible coating from cassava starch and babassu flour
(orbignya phalerata) on brazilian cerrado fruits quality. Food Bioprocess Technol. 2019, 13, 172–179. [CrossRef]
81. Castillo, L.A.; Lopez, O.V.; Garcia, M.A.; Barbosa, S.E.; Villar, M.A. Crystalline morphology of thermoplastic
starch/talc nanocomposites induced by thermal processing. Heliyon 2019, 5, e01877. [CrossRef]
82. Ulyarti, U.; Maryana, E.; Rahmayani, I.; Nazarudin, N.; Susilawati, S.; Doyan, A. The characteristics of yam
(dioscorea alata) starch edible film. J. Penelit. Pendidik IPA 2018, 5. [CrossRef]
83. Sun, S.; Liu, P.; Ji, N.; Hou, H.; Dong, H. Effects of various cross-linking agents on the physicochemical
properties of starch/PHA composite films produced by extrusion blowing. Food Hydrocoll. 2018, 77, 964–975.
[CrossRef]
84. Désiré, A.Y.; Charlemagne, N.; Achille, T.F.; Anne-Catherine, D.; Georges, A.N.; Marianne, S. Water vapor
permeability of edible films based on improved cassava (manihot esculenta crantz) native starches. J. Food
Process. Technol. 2017, 8. [CrossRef]
85. Saberi, B.; Thakur, R.; Vuong, Q.V.; Chockchaisawasdee, S.; Golding, J.B.; Scarlett, C.J.; Stathopoulos, C.E.
Optimization of physical and optical properties of biodegradable edible films based on pea starch
and guar gum. Ind. Crop. Prod. 2016, 86, 342–352. [CrossRef]
86. Jaramillo, C.M.; Gutierrez, T.J.; Goyanes, S.; Bernal, C.; Fama, L. Biodegradability and plasticizing effect of
yerba mate extract on cassava starch edible films. Carbohydr. Polym. 2016, 151, 150–159. [CrossRef]
87. Andrade, R.M.; Ferreira, M.S.; Goncalves, E.C. Development and characterization of edible films based on
fruit and vegetable residues. J. Food Sci. 2016, 81, E412–E418. [CrossRef]
Coatings 2020, 10, 687 36 of 45

88. Mei, J.; Yuan, Y.; Guo, Q.; Wu, Y.; Li, Y.; Yu, H. Characterization and antimicrobial properties of water
chestnut starch-chitosan edible films. Int. J. Biol. Macromol. 2013, 61, 169–174. [CrossRef] [PubMed]
89. López, O.V.; Zaritzky, N.E.; Grossmann, M.V.E.; García, M.A. Acetylated and native corn starch blend films
produced by blown extrusion. J. Food Eng. 2013, 116, 286–297. [CrossRef]
90. Gao, W.; Dong, H.; Hou, H.; Zhang, H. Effects of clays with various hydrophilicities on properties of
starch–clay nanocomposites by film blowing. Carbohydr. Polym. 2012, 88, 321–328. [CrossRef]
91. Chaléat, C.M.; Halley, P.J.; Truss, R.W. Study on the phase separation of plasticised starch/poly (vinyl alcohol)
blends. Polym. Degrad. Stab. 2012, 97, 1930–1939. [CrossRef]
92. Bello-Pérez, L.A.; Agama-Acevedo, E.; Zamudio-Flores, P.B.; Mendez-Montealvo, G.; Rodriguez-Ambriz, S.L.
Effect of low and high acetylation degree in the morphological, physicochemical and structural characteristics
of barley starch. LWT–Food Sci. Technol. 2010, 43, 1434–1440. [CrossRef]
93. Medina-Jaramillo, C.; Estevez-Areco, S.; Goyanes, S.; Lopez-Cordoba, A. Characterization of starches isolated
from colombian native potatoes and their application as novel edible coatings for wild andean blueberries
(vaccinium meridionale swartz). Polymers 2019, 11, 1937. [CrossRef]
94. Santoso, B.; Hazirah, R.; Priyanto, G.; Hermanto, D.; Sugito, D. Utilization of Uncaria gambir Roxb filtrate in
the formation of bioactive edible films based on corn starch. Food Sci. Technol. 2019, 39, 837–842. [CrossRef]
95. Matta Fakhouri, F.; Nogueira, G.F.; De Oliveira, R.A.; Velasco, J.I. Bioactive edible films based on arrowroot
starch incorporated with cranberry powder: Microstructure, thermal properties, ascorbic acid content
and sensory analysis. Polymers 2019, 11, 1650. [CrossRef]
96. Nagar, M.; Sharanagat, V.S.; Kumar, Y.; Singh, L. Development and characterization of elephant foot yam
starch-hydrocolloids based edible packaging film: Physical, optical, thermal and barrier properties. J. Food
Sci. Technol. 2020, 57, 1331–1341. [CrossRef]
97. Dai, L.; Zhang, J.; Cheng, F. Cross-linked starch-based edible coating reinforced by starch nanocrystals and its
preservation effect on graded Huangguan pears. Food Chem. 2020, 311, 125891. [CrossRef] [PubMed]
98. Zhao, D.; Yu, S.; Sun, B.; Gao, S.; Guo, S.; Zhao, K. Biomedical applications of chitosan and its derivative
nanoparticles. Polymers 2018, 10, 462. [CrossRef] [PubMed]
99. Saikia, C.; Gogoi, P. Chitosan: A promising biopolymer in drug delivery applications. J. Mol. Genet. Med.
2015, S4. [CrossRef]
100. Zhao, F.; Yao, D.; Guo, R.; Deng, L.; Dong, A.; Zhang, J. Composites of polymer hydrogels and nanoparticulate
systems for biomedical and pharmaceutical applications. Nanomaterials 2015, 5, 2054–2130. [CrossRef]
[PubMed]
101. Tokatlı, K.; Demirdöven, A. Effects of chitosan edible film coatings on the physicochemical and microbiological
qualities of sweet cherry (Prunus avium L.). Sci. Hortic. 2020, 259. [CrossRef]
102. Chan, S.Y.; Choo, W.S.; Young, D.J.; Loh, X.J. Pectin as a rheology modifier: Origin, structure, commercial
production and rheology. Carbohydr. Polym. 2017, 161, 118–139. [CrossRef]
103. Hua, X.; Wang, K.; Yang, R.; Kang, J.; Zhang, J. Rheological properties of natural low-methoxyl pectin
extracted from sunflower head. Food Hydrocoll. 2015, 44, 122–128. [CrossRef]
104. Guo, X.; Han, D.; Xi, H.; Rao, L.; Liao, X.; Hu, X.; Wu, J. Extraction of pectin from navel orange peel assisted
by ultra-high pressure, microwave or traditional heating: A comparison. Carbohydr. Polym. 2012, 88, 441–448.
[CrossRef]
105. Dranca, F.; Oroian, M. Extraction, purification and characterization of pectin from alternative sources with
potential technological applications. Food Res. Int. 2018, 113, 327–350. [CrossRef] [PubMed]
106. Ngo, T.M.P.; Nguyen, T.H.; Dang, T.M.Q.; Tran, T.X.; Rachtanapun, P. Characteristics and antimicrobial
properties of active edible films based on pectin and nanochitosan. Int. J. Mol. Sci. 2020, 21, 2224. [CrossRef]
107. Ferreira, S.L.; Dos Santos, W.N.; Quintella, C.M.; Neto, B.B.; Bosque-Sendra, J.M. Doehlert matrix:
A chemometric tool for analytical chemistry-review. Talanta 2004, 63, 1061–1067. [CrossRef]
108. Mohamed, S.A.A.; El-Sakhawy, M.; El-Sakhawy, M.A. Polysaccharides, protein and lipid-based natural
edible films in food packaging: A review. Carbohydr. Polym. 2020, 238, 116178. [CrossRef]
109. Akin, M.; Saki, N.; Buyukbayram, M. Shellac and Carnauba Wax Based Edible Films Coating for Fruit
Applications. In Proceedings of the International Science and Applications of Thin Films, Conference &
Exhibition (SATF 2018), Izmir, Turkey, 17–21 September 2018.
110. Zdanowicz, M.; Johansson, C. Mechanical and barrier properties of starch-based films plasticized with two-
or three component deep eutectic solvents. Carbohydr. Polym. 2016, 151, 103–112. [CrossRef] [PubMed]
Coatings 2020, 10, 687 37 of 45

111. Fromme, H.; Bolte, G.; Koch, H.M.; Angerer, J.; Boehmer, S.; Drexler, H.; Mayer, R.; Liebl, B. Occurrence
and daily variation of phthalate metabolites in the urine of an adult population. Int. J. Hyg. Environ. Health
2007, 210, 21–33. [CrossRef] [PubMed]
112. Heudorf, U.; Mersch-Sundermann, V.; Angerer, J. Phthalates: Toxicology and exposure. Int. J. Hyg. Environ.
Health 2007, 210, 623–634. [CrossRef] [PubMed]
113. Sothornvit, R.; Krochta, J.M. Plasticizers in edible films and coatings. In Innovations in Food Packaging;
Han, J.H., Ed.; Academic Press: London, UK, 2005; pp. 403–433.
114. Sahraee, S.; Milani, J.M.; Regenstein, J.M.; Kafil, H.S. Protection of foods against oxidative deterioration
using edible films and coatings: A review. Food Biosci. 2019, 32. [CrossRef]
115. Otoni, C.G.; Avena-Bustillos, R.J.; Azeredo, H.M.C.; Lorevice, M.V.; Moura, M.R.; Mattoso, L.H.C.;
McHugh, T.H. Recent advances on edible films based on fruits and vegetables-A review. Compr. Rev.
Food Sci. Food Saf. 2017, 16, 1151–1169. [CrossRef]
116. Espitia, P.J.; Avena-Bustillos, R.J.; Du, W.X.; Chiou, B.S.; Williams, T.G.; Wood, D.; McHugh, T.H.; Soares, N.F.
Physical and antibacterial properties of acai edible films formulated with thyme essential oil and apple skin
polyphenols. J. Food Sci. 2014, 79, M903–M910. [CrossRef]
117. Guerrero, A.; Ferrero, S.; Barahona, M.; Boito, B.; Lisbinski, E.; Maggi, F.; Sanudo, C. Effects of active edible
coating based on thyme and garlic essential oils on lamb meat shelf life after long-term frozen storage. J. Sci.
Food Agric. 2020, 100, 656–664. [CrossRef]
118. Tzortzakis, N.; Xylia, P.; Chrysargyris, A. Sage essential oil improves the effectiveness of aloe vera gel on
postharvest quality of tomato fruit. Agronomy 2019, 9, 635. [CrossRef]
119. Kocić-Tanackov, S.; Dimić, G.; Jakšić, S.; Mojović, L.; Djukić-Vuković, A.; Mladenović, D.; Pejin, J. Effects of
caraway and juniper essential oils on aflatoxigenic fungi growth and aflatoxins secretion in polenta. J. Food
Process. Preserv. 2019, 43. [CrossRef]
120. Khaledian, Y.; Pajohi-Alamoti, M.; Bazargani-Gilani, B. Development of cellulose nanofibers coating
incorporated with ginger essential oil and citric acid to extend the shelf life of ready-to-cook barbecue chicken.
J. Food Process. Preserv. 2019, 43. [CrossRef]
121. Ekrami, M.; Emam-Djomeh, Z.; Ghoreishy, S.A.; Najari, Z.; Shakoury, N. Characterization of a
high-performance edible film based on Salep mucilage functionalized with pennyroyal (mentha pulegium).
Int. J. Biol. Macromol. 2019, 133, 529–537. [CrossRef]
122. Dos Passos Braga, S.; Lundgren, G.A.; Macedo, S.A.; Tavares, J.F.; Dos Santos Vieira, W.A.; Camara, M.P.S.;
De Souza, E.L. Application of coatings formed by chitosan and Mentha essential oils to control anthracnose
caused by Colletotrichum gloesporioides and C. brevisporum in papaya (Carica papaya L.) fruit. Int. J. Biol.
Macromol. 2019, 139, 631–639. [CrossRef] [PubMed]
123. Bolívar-Monsalve, J.; Ramírez-Toro, C.; Bolívar, G.; Ceballos-González, C. Mechanisms of action of novel
ingredients used in edible films to preserve microbial quality and oxidative stability in sausages—A review.
Trends Food Sci. Technol. 2019, 89, 100–109. [CrossRef]
124. Benbettaieb, N.; Karbowiak, T.; Debeaufort, F. Bioactive edible films for food applications: Influence of
the bioactive compounds on film structure and properties. Crit. Rev. Food Sci. Nutr. 2019, 59, 1137–1153.
[CrossRef]
125. Alak, G.; Guler, K.; Ucar, A.; Parlak, V.; Kocaman, E.M.; Yanık, T.; Atamanalp, M. Quinoa as polymer in edible
films with essential oil: Effects on rainbow trout fillets shelf life. J. Food Process. Preserv. 2019, 43. [CrossRef]
126. Senturk Parreidt, T.; Muller, K.; Schmid, M. Alginate-based edible films and coatings for food packaging
applications. Foods 2018, 7, 170. [CrossRef]
127. Valdés, A.; Burgos, N.; Jiménez, A.; Garrigós, M. Natural pectin polysaccharides as edible coatings.
Coatings 2015, 5, 865–886. [CrossRef]
128. Silva-Weiss, A.; Ihl, M.; Sobral, P.J.A.; Gómez-Guillén, M.C.; Bifani, V. Natural additives in bioactive edible
films and coatings: Functionality and applications in foods. Food Eng. Rev. 2013, 5, 200–216. [CrossRef]
129. Chaudhary, S.; Kumar, S.; Kumar, V.; Sharma, R. Chitosan nanoemulsions as advanced edible coatings for
fruits and vegetables: Composition, fabrication and developments in last decade. Int. J. Biol. Macromol. 2020,
152, 154–170. [CrossRef]
130. Mhd Haniffa, M.A.C.; Ching, Y.C.; Abdullah, L.C.; Poh, S.C.; Chuah, C.H. Review of bionanocomposite
coating films and their applications. Polymers 2016, 8, 246. [CrossRef] [PubMed]
Coatings 2020, 10, 687 38 of 45

131. Honarkar, H.; Barikani, M. Applications of biopolymers I: Chitosan. Mon. Für Chem. Chem. Mon. 2009, 140,
1403–1420. [CrossRef]
132. Ganduri, V.S.R. Evaluation of pullulan-based edible active coating methods on Rastali and Chakkarakeli
bananas and their shelf-life extension parameters studies. J. Food Process. Preserv. 2020. [CrossRef]
133. Nesic, A.; Cabrera-Barjas, G.; Dimitrijevic-Brankovic, S.; Davidovic, S.; Radovanovic, N.; Delattre, C. Prospect
of polysaccharide-based materials as advanced food packaging. Molecules 2019, 25, 135. [CrossRef]
134. Yang, W.; Li, X.; Jiang, J.; Fan, X.; Du, M.; Shi, X.; Cao, R. Improvement in the oxidative stability of flaxseed
oil using an edible guar gum-tannic acid nanofibrous mat. Eur. J. Lipid Sci. Technol. 2019, 121. [CrossRef]
135. Kim, M.I.; Kim, J.H.; Syed, A.S.; Kim, Y.M.; Choe, K.K.; Kim, C.Y. Application of centrifugal partition
chromatography for bioactivity-guided purification of antioxidant-response-element-inducing constituents
from atractylodis rhizoma alba. Molecules 2018, 23, 2274. [CrossRef] [PubMed]
136. Schwienheer, C.; Krause, J.; Schembecker, G.; Merz, J. Modelling centrifugal partition chromatography
separation behavior to characterize influencing hydrodynamic effects on separation efficiency. J. Chromatogr.
A 2017, 1492, 27–40. [CrossRef]
137. Issaadi, H.M.; Tsai, Y.C.; Chang, F.R.; Hunyadi, A. Centrifugal partition chromatography in the isolation of
minor ecdysteroids from Cyanotis arachnoidea. J. Chromatogr. B 2017, 1054, 44–49. [CrossRef]
138. Xiong, Y.; Li, S.; Warner, R.D.; Fang, Z. Effect of oregano essential oil and resveratrol nanoemulsion loaded
pectin edible coating on the preservation of pork loin in modified atmosphere packaging. Food Control 2020,
114. [CrossRef]
139. Shokri, S.; Parastouei, K.; Taghdir, M.; Abbaszadeh, S. Application an edible active coating based on chitosan-
Ferulago angulata essential oil nanoemulsion to shelf life extension of Rainbow trout fillets stored at 4 degrees
C. Int. J. Biol. Macromol. 2020, 153, 846–854. [CrossRef]
140. Savadkouhi, N.R.; Ariaii, P.; Langerodi, M.C. The effect of encapsulated plant extract of hyssop (Hyssopus
officinalis L.) in biopolymer nanoemulsions of Lepidium perfoliatum and Orchis mascula on controlling
oxidative stability of soybean oil. Food Sci. Nutr. 2020, 8, 1264–1271. [CrossRef] [PubMed]
141. Kiarsi, Z.; Hojjati, M.; Behbahani, B.A.; Noshad, M. In vitro antimicrobial effects of Myristica fragrans
essential oil on foodborne pathogens and its influence on beef quality during refrigerated storage. J. Food Saf.
2020. [CrossRef]
142. Rezaeifar, M.; Mehdizadeh, T.; Langroodi, A.M.; Rezaei, F. Effect of chitosan edible coating enriched with
lemon verbena extract and essential oil on the shelf life of vacuum rainbow trout (Oncorhynchus mykiss).
J. Food Saf. 2020. [CrossRef]
143. Keykhosravy, K.; Khanzadi, S.; Hashemi, M.; Azizzadeh, M. Chitosan-loaded nanoemulsion containing
Zataria Multiflora Boiss and Bunium persicum Boiss essential oils as edible coatings: Its impact on microbial
quality of turkey meat and fate of inoculated pathogens. Int. J. Biol. Macromol. 2020, 150, 904–913. [CrossRef]
[PubMed]
144. Kalkan, S.; Otag, M.R.; Engin, M.S. Physicochemical and bioactive properties of edible methylcellulose films
containing Rheum ribes L. extract. Food Chem. 2020, 307, 125524. [CrossRef] [PubMed]
145. Istúriz-Zapata, M.A.; Hernández-López, M.; Correa-Pacheco, Z.N.; Barrera-Necha, L.L. Quality of cold-stored
cucumber as affected by nanostructured coatings of chitosan with cinnamon essential oil and cinnamaldehyde.
LWT 2020, 123. [CrossRef]
146. Etemadipoor, R.; Dastjerdi, A.M.; Ramezanian, A.; Ehteshami, S. Ameliorative effect of gum arabic, oleic
acid and/or cinnamon essential oil on chilling injury and quality loss of guava fruit. Sci. Hortic. 2020, 266.
[CrossRef]
147. De Vasconcellos Santos Batista, D.; Reis, R.C.; Almeida, J.M.; Rezende, B.; Braganca, C.A.D.; Da Silva, F.
Edible coatings in post-harvest papaya: Impact on physical-chemical and sensory characteristics. J. Food Sci.
Technol. 2020, 57, 274–281. [CrossRef]
148. Behbahani, B.A.; Noshad, M.; Jooyandeh, H. Improving oxidative and microbial stability of beef using
Shahri Balangu seed mucilage loaded with Cumin essential oil as a bioactive edible coating. Biocatal. Agric.
Biotechnol. 2020, 24. [CrossRef]
149. Al-Hashimi, A.G.; Ammar, A.B.; G, L.; Cacciola, F.; Lakhssassi, N. Development of a millet starch edible film
containing clove essential oil. Foods 2020, 9, 184. [CrossRef]
150. Zhang, H.; Li, X.; Kang, H. Chitosan coatings incorporated with free or nano-encapsulated Paulownia
Tomentosa essential oil to improve shelf-life of ready-to-cook pork chops. LWT 2019, 116. [CrossRef]
Coatings 2020, 10, 687 39 of 45

151. Vieira, B.B.; Mafra, J.F.; Bispo, A.S.D.R.; Ferreira, M.A.; Silva, F.D.L.; Rodrigues, A.V.N.;
Evangelista-Barreto, N.S. Combination of chitosan coating and clove essential oil reduces lipid oxidation
and microbial growth in frozen stored tambaqui (colossoma macropomum) fillets. LWT 2019, 116. [CrossRef]
152. Sapper, M.; Bonet, M.; Chiralt, A. Wettability of starch-gellan coatings on fruits, as affected by the incorporation
of essential oil and/or surfactants. LWT 2019, 116. [CrossRef]
153. Melo, P.T.S.; Nunes, J.C.; Otoni, C.G.; Aouada, F.A.; De Moura, M.R. Combining cupuassu
(theobroma grandiflorum) puree, pectin, and chitosan nanoparticles into novel edible films for food
packaging applications. J. Food Sci. 2019, 84, 2228–2233. [CrossRef]
154. Matta, E.; Tavera-Quiroz, M.J.; Bertola, N. Active edible films of methylcellulose with extracts of green apple
(Granny Smith) skin. Int. J. Biol. Macromol. 2019, 124, 1292–1298. [CrossRef] [PubMed]
155. Kim, N.; Seo, E.; Kim, Y. Physical, mechanical and water barrier properties of yuba films incorporated with
various types of additives. J. Sci. Food Agric. 2019, 99, 2808–2817. [CrossRef]
156. Khanzadi, S.; Hashemi, M.; Keykhosravy, K. Antimicrobial and antioxidant efficiency of nano emulsion-based
edible coating containing ginger (Zingiber officinale) essential oil and its effect on safety and quality attributes
of chicken breast fillets. Food Control 2019, 106. [CrossRef]
157. Tovar, C.D.G.; Delgado-Ospina, J.; Porras, D.P.N.; Peralta-Ruiz, Y.; Cordero, A.P.; Castro, J.I.; Valencia, M.N.C.;
Mina, J.H.; Lopez, C.C. Colletotrichum gloesporioides inhibition in situ by chitosan-ruta graveolens
essential oil coatings: Effect on microbiological, physicochemical, and organoleptic properties of guava
(Psidium guajava L.) during room temperature storage. Biomolecules 2019, 9, 399. [CrossRef]
158. De Oliveira, K.Á.R.; Da Conceição, M.L.; De Oliveira, S.P.A.; Lima, M.d.S.; De Sousa Galvão, M.;
Madruga, M.S.; Magnani, M.; De Souza, E.L. Postharvest quality improvements in mango cultivar Tommy
Atkins by chitosan coating with Mentha piperita L. essential oil. J. Hortic. Sci. Biotechnol. 2019, 95, 260–272.
[CrossRef]
159. De Figueiredo Sousa, H.A.; De Oliveira Filho, J.G.; Egea, M.B.; Da Silva, E.R.; Macagnan, D.; Pires, M.;
Peixoto, J. Active film incorporated with clove essential oil on storage of banana varieties. Nutr. Food Sci.
2019. [CrossRef]
160. Rodsamran, P.; Sothornvit, R. Microencapsulation of Thai rice grass (O. Sativa cv. Khao Dawk Mali 105)
extract incorporated to form bioactive carboxymethyl cellulose edible film. Food Chem. 2018, 242, 239–246.
[CrossRef] [PubMed]
161. Pinzon, M.I.; Garcia, O.R.; Villa, C.C. The influence of Aloe vera gel incorporation on the physicochemical
and mechanical properties of banana starch-chitosan edible films. J. Sci. Food Agric. 2018, 98, 4042–4049.
[CrossRef] [PubMed]
162. Noor, S.; Bhat, Z.F.; Kumar, S.; Mudiyanselage, R.J. Preservative effect of Asparagus racemosus: A novel
additive for bioactive edible films for improved lipid oxidative stability and storage quality of meat products.
Meat Sci. 2018, 139, 207–212. [CrossRef]
163. Saberi, B.; Vuong, Q.V.; Chockchaisawasdee, S.; Golding, J.B.; Scarlett, C.J.; Stathopoulos, C.E. Physical,
barrier, and antioxidant properties of pea starch-guar gum biocomposite edible films by incorporation of
natural plant extracts. Food Bioprocess. Technol. 2017, 10, 2240–2250. [CrossRef]
164. Alsaggaf, M.S.; Moussa, S.H.; Tayel, A.A. Application of fungal chitosan incorporated with pomegranate
peel extract as edible coating for microbiological, chemical and sensorial quality enhancement of Nile tilapia
fillets. Int. J. Biol. Macromol. 2017, 99, 499–505. [CrossRef] [PubMed]
165. Tongnuanchan, P.; Benjakul, S.; Prodpran, T.; Pisuchpen, S.; Osako, K. Mechanical, thermal and heat sealing
properties of fish skin gelatin film containing palm oil and basil essential oil with different surfactants.
Food Hydrocoll. 2016, 56, 93–107. [CrossRef]
166. Rodriguez-Garcia, I.; Cruz-Valenzuela, M.R.; Silva-Espinoza, B.A.; Gonzalez-Aguilar, G.A.; Moctezuma, E.;
Gutierrez-Pacheco, M.M.; Tapia-Rodriguez, M.R.; Ortega-Ramirez, L.A.; Ayala-Zavala, J.F. Oregano
(Lippia graveolens) essential oil added within pectin edible coatings prevents fungal decay and increases
the antioxidant capacity of treated tomatoes. J. Sci. Food Agric. 2016, 96, 3772–3778. [CrossRef] [PubMed]
167. Kavas, N.; Kavas, G. Physical-chemical and antimicrobial properties of Egg White Protein Powder films
incorporated with orange essential oil on Kashar Cheese. Food Sci. Technol. 2016, 36, 672–678. [CrossRef]
168. Gallego, M.G.; Gordon, M.H.; Segovia, F.; Pablos, M.P.A. Gelatine-based antioxidant packaging containing
caesalpinia decapetala and tara as a coating for ground beef patties. Antioxidants 2016, 5, 10. [CrossRef]
Coatings 2020, 10, 687 40 of 45

169. Alexandre, E.M.C.; Lourenço, R.V.; Bittante, A.M.Q.B.; Moraes, I.C.F.; Sobral, P.J.D.A. Gelatin-based films
reinforced with montmorillonite and activated with nanoemulsion of ginger essential oil for food packaging
applications. Food Packag. Shelf Life 2016, 10, 87–96. [CrossRef]
170. Pena-Rodriguez, C.; Martucci, J.F.; Neira, L.M.; Arbelaiz, A.; Eceiza, A.; Ruseckaite, R.A. Functional properties
and in vitro antioxidant and antibacterial effectiveness of pigskin gelatin films incorporated with hydrolysable
chestnut tannin. Food Sci. Technol. Int. 2015, 21, 221–231. [CrossRef]
171. Zhu, L.; Olsen, C.; McHugh, T.; Friedman, M.; Jaroni, D.; Ravishankar, S. Apple, carrot, and hibiscus edible
films containing the plant antimicrobials carvacrol and cinnamaldehyde inactivate Salmonella Newport on
organic leafy greens in sealed plastic bags. J. Food. Sci. 2014, 79, M61–M66. [CrossRef] [PubMed]
172. Otoni, C.G.; Pontes, S.F.; Medeiros, E.A.; Soares Nde, F. Edible films from methylcellulose and nanoemulsions
of clove bud (Syzygium aromaticum) and oregano (Origanum vulgare) essential oils as shelf life extenders
for sliced bread. J. Agric. Food Chem. 2014, 62, 5214–5219. [CrossRef] [PubMed]
173. Kraśniewska, K.; Gniewosz, M.; Synowiec, A.; Przybył, J.L.; Baczek, ˛ K.; W˛eglarz, Z. The use of pullulan
coating enriched with plant extracts from Satureja hortensis L. to maintain pepper and apple quality and safety.
Postharvest Biol. Technol. 2014, 90, 63–72. [CrossRef]
174. Ferreira, A.S.; Nunes, C.; Castro, A.; Ferreira, P.; Coimbra, M.A. Influence of grape pomace extract
incorporation on chitosan films properties. Carbohydr. Polym. 2014, 113, 490–499. [CrossRef]
175. Campos, D.; Piccirillo, C.; Pullar, R.C.; Castro, P.M.; Pintado, M.M. Characterization and antimicrobial
properties of food packaging methylcellulose films containing stem extract of Ginja cherry. J. Sci. Food Agric.
2014, 94, 2097–2103. [CrossRef]
176. Lopez-Garcia, J.; Kucekova, Z.; Humpolicek, P.; Mlcek, J.; Saha, P. Polyphenolic extracts of edible flowers
incorporated onto atelocollagen matrices and their effect on cell viability. Molecules 2013, 18, 13435–13445.
[CrossRef]
177. Wang, S.; Marcone, M.; Barbut, S.; Lim, L.T. The impact of anthocyanin-rich red raspberry extract (ARRE) on
the properties of edible soy protein isolate (SPI) films. J. Food Sci. 2012, 77, C497–C505. [CrossRef]
178. Ravishankar, S.; Jaroni, D.; Zhu, L.; Olsen, C.; McHugh, T.; Friedman, M. Inactivation of Listeria
monocytogenes on ham and bologna using pectin-based apple, carrot, and hibiscus edible films containing
carvacrol and cinnamaldehyde. J. Food Sci. 2012, 77, M377–M382. [CrossRef]
179. Moradi, M.; Tajik, H.; Rohani, S.M.R.; Oromiehie, A.R.; Malekinejad, H.; Aliakbarlu, J.; Hadian, M.
Characterization of antioxidant chitosan film incorporated with Zataria multiflora Boiss essential oil
and grape seed extract. LWT–Food Sci. Technol. 2012, 46, 477–484. [CrossRef]
180. Lara, G.R.; Uemura, K.; Khalid, N.; Kobayashi, I.; Takahashi, C.; Nakajima, M.; Neves, M.A. Layer-by-layer
electrostatic deposition of edible coatings for enhancing the storage stability of fresh-cut lotus root (Nelumbo
nucifera). Food Bioprocess. Technol. 2020, 13, 722–726. [CrossRef]
181. Lima, Á.M.; Cerqueira, M.A.; Souza, B.W.S.; Santos, E.C.M.; Teixeira, J.A.; Moreira, R.A.; Vicente, A.A.
New edible coatings composed of galactomannans and collagen blends to improve the postharvest quality
of fruits–Influence on fruits gas transfer rate. J. Food Eng. 2010, 97, 101–109. [CrossRef]
182. Novel sources of edible films and coatings. Stewart Postharvest Rev. 2010, 6, 1–8. [CrossRef]
183. De Elguea-Culebras, G.O.; Bourbon, A.I.; Costa, M.J.; Muñoz-Tebar, N.; Carmona, M.; Molina, A.;
Sánchez-Vioque, R.; Berruga, M.I.; Vicente, A.A. Optimization of a chitosan solution as potential carrier for
the incorporation of Santolina chamaecyparissus L. solid by-product in an edible vegetal coating on ‘Manchego’
cheese. Food Hydrocoll. 2019, 89, 272–282. [CrossRef]
184. Dhumal, C.V.; Ahmed, J.; Bandara, N.; Sarkar, P. Improvement of antimicrobial activity of sago starch/guar gum
bi-phasic edible films by incorporating carvacrol and citral. Food Packag. Shelf Life 2019, 21. [CrossRef]
185. Torres-León, C.; Vicente, A.A.; Flores-López, M.L.; Rojas, R.; Serna-Cock, L.; Alvarez-Pérez, O.B.; Aguilar, C.N.
Edible films and coatings based on mango (var. Ataulfo) by-products to improve gas transfer rate of peach.
LWT 2018, 97, 624–631. [CrossRef]
186. Terpilowski, K.; Hołysz, L.; Rymuszka, D.; Banach, R. Comparison of contact angle measurement methods of
liquids on metal alloys. Ann. UMCS, Chem. 2016, 71, 89. [CrossRef]
187. Souza, V.G.L.; Pires, J.R.A.; Rodrigues, C.; Coelhoso, I.M.; Fernando, A.L. Chitosan composites in packaging
industry-current trends and future challenges. Polymers 2020, 12, 417. [CrossRef]
Coatings 2020, 10, 687 41 of 45

188. Medina-Pérez, G.; Hernández-Uribe, J.P.; Fernández-León, D.; Prince, L.; Fernández-Luqueño, F.;
Campos-Montiel, R.G. Application of nanoemulsions (w/o) with active compounds of cactus pear fruit in
starch films to improve antioxidant activity and incorporate antibacterial property. J. Food Process. Eng. 2019,
42. [CrossRef]
189. Han, Y.; Wang, L. Sodium alginate/carboxymethyl cellulose films containing pyrogallic acid: Physical
and antibacterial properties. J. Sci. Food Agric. 2017, 97, 1295–1301. [CrossRef] [PubMed]
190. Eswaranandam, S.; Hettiarachchy, N.S.; Johnson, M.G. Antimicrobial activity of citric, lactic, malic, or tartaric
acids and nisin-incorporated soy protein film against listeria monocytogenes, escherichia coli O157:H7,
and salmonella gaminara. J. Food Sci. 2004, 69, FMS79–FMS84. [CrossRef]
191. Fabra, M.J.; Talens, P.; Gavara, R.; Chiralt, A. Barrier properties of sodium caseinate films as affected by lipid
composition and moisture content. J. Food Eng. 2012, 109, 372–379. [CrossRef]
192. Amarante, C.; Banks, N.H. Postharvest physiology and quality of COATED fruits and Vegetables.
In Horticultural Reviews; John Wiley & Sons, Inc.: Bridgewater, NJ, USA, 2000.
193. Salama, H.E.; Abdel Aziz, M.S.; Alsehli, M. Carboxymethyl cellulose/sodium alginate/chitosan biguanidine
hydrochloride ternary system for edible coatings. Int. J. Biol. Macromol. 2019, 139, 614–620. [CrossRef]
[PubMed]
194. Campos, C.A.; Gerschenson, L.N.; Flores, S.K. Development of edible films and coatings with antimicrobial
activity. Food Bioprocess. Technol. 2010, 4, 849–875. [CrossRef]
195. Rojas-Bravo, M.; Rojas-Zenteno, E.G.; Hernández-Carranza, P.; Ávila-Sosa, R.; Aguilar-Sánchez, R.;
Ruiz-López, I.I.; Ochoa-Velasco, C.E. A potential application of mango (Mangifera indica L. cv Manila)
peel powder to increase the total phenolic compounds and antioxidant capacity of edible films and coatings.
Food Bioprocess. Technol. 2019, 12, 1584–1592. [CrossRef]
196. Moreno, M.A.; Bojorges, H.; Falcó, I.; Sánchez, G.; López-Carballo, G.; López-Rubio, A.; Zampini, I.C.;
Isla, M.I.; Fabra, M.J. Active properties of edible marine polysaccharide-based coatings containing Larrea
nitida polyphenols enriched extract. Food Hydrocoll. 2020, 102. [CrossRef]
197. Alkan, D.; Yemenicioğlu, A. Potential application of natural phenolic antimicrobials and edible film technology
against bacterial plant pathogens. Food Hydrocoll. 2016, 55, 1–10. [CrossRef]
198. Zhang, S.; Wei, F.; Han, X. An edible film of sodium alginate/pullulan incorporated with capsaicin. New J.
Chem. 2018, 42, 17756–17761. [CrossRef]
199. Talon, E.; Trifkovic, K.T.; Nedovic, V.A.; Bugarski, B.M.; Vargas, M.; Chiralt, A.; Gonzalez-Martinez, C.
Antioxidant edible films based on chitosan and starch containing polyphenols from thyme extracts.
Carbohydr. Polym. 2017, 157, 1153–1161. [CrossRef]
200. Castro e Silva, P.; Oliveira, A.C.S.; Pereira, L.A.S.; Valquíria, M.; Carvalho, G.R.; Miranda, K.W.E.;
Marconcini, J.M.; Oliveira, J.E. Development of bionanocomposites of pectin and nanoemulsions of carnauba
wax and neem oil pectin/carnauba wax/neem oil composites. Polym. Compos. 2019, 41, 858–870. [CrossRef]
201. Dick, M.; Costa, T.M.; Gomaa, A.; Subirade, M.; Ade, O.R.; Flores, S.H. Edible film production from
chia seed mucilage: Effect of glycerol concentration on its physicochemical and mechanical properties.
Carbohydr. Polym. 2015, 130, 198–205. [CrossRef] [PubMed]
202. Yang, H.; Wang, D.; Deng, J.; Yang, J.; Shi, C.; Zhou, F.; Shi, Z. Activity and structural characteristics of
peach gum exudates. Int. J. Polym. Sci. 2018, 2018, 1–5. [CrossRef]
203. Bonilla, J.; Bittante, A.M.Q.B.; Sobral, P.J.A. Thermal analysis of gelatin–chitosan edible film mixed with
plant ethanolic extracts. J. Therm. Anal. Calorim. 2017, 130, 1221–1227. [CrossRef]
204. Breda, C.A.; Morgado, D.L.; Assis, O.B.G.; Duarte, M.C.T. Processing and characterization of chitosan films
with incorporation of ethanolic extract from “pequi” peels. Macromol. Res. 2017, 25, 1049–1056. [CrossRef]
205. Ghadermazi, R.; Hamdipour, S.; Sadeghi, K.; Ghadermazi, R.; Asl, A.K. Effect of various additives on
the properties of the films and coatings derived from hydroxypropyl methylcellulose—A review. Food Sci.
Nutr. 2019, 7, 3363–3377. [CrossRef] [PubMed]
206. Aisyah, Y.; Irwanda, L.P.; Haryani, S.; Safriani, N. Characterization of corn starch-based edible film
incorporated with nutmeg oil nanoemulsion. IOP Conf. Ser. Mater. Sci. Eng. 2018, 352. [CrossRef]
207. Funami, T. In vivo and rheological approaches for characterizing food oral processing and usefulness of
polysaccharides as texture modifiers—A review. Food Hydrocoll. 2017, 68, 2–14. [CrossRef]
208. Fuertes, S.; Laca, A.; Oulego, P.; Paredes, B.; Rendueles, M.; Díaz, M. Development and characterization of
egg yolk and egg yolk fractions edible films. Food Hydrocoll. 2017, 70, 229–239. [CrossRef]
Coatings 2020, 10, 687 42 of 45

209. Hosseini, S.F.; Rezaei, M.; Zandi, M.; Farahmandghavi, F. Fabrication of bio-nanocomposite films based on
fish gelatin reinforced with chitosan nanoparticles. Food Hydrocoll. 2015, 44, 172–182. [CrossRef]
210. Wang, Z.; Zhou, J.; Wang, X.-X.; Zhang, N.; Sun, X.-X.; Ma, Z.-S. The effects of ultrasonic/microwave assisted
treatment on the water vapor barrier properties of soybean protein isolate-based oleic acid/stearic acid blend
edible films. Food Hydrocoll. 2014, 35, 51–58. [CrossRef]
211. Akhtar, M.J.; Jacquot, M.; Jasniewski, J.; Jacquot, C.; Imran, M.; Jamshidian, M.; Paris, C.; Desobry, S.
Antioxidant capacity and light-aging study of HPMC films functionalized with natural plant extract.
Carbohydr. Polym. 2012, 89, 1150–1158. [CrossRef] [PubMed]
212. Romano, N.; Tavera-Quiroz, M.J.; Bertola, N.; Mobili, P.; Pinotti, A.; Gomez-Zavaglia, A.
Edible methylcellulose-based films containing fructo-oligosaccharides as vehicles for lactic acid bacteria.
Food Res. Int. 2014, 64, 560–566. [CrossRef] [PubMed]
213. Alotaibi, M.A.; Tayel, A.A.; Zidan, N.S.; El Rabey, H.A. Bioactive coatings from nano-biopolymers/plant
extract composites for complete protection from mycotoxigenic fungi in dates. J. Sci. Food Agric. 2019, 99,
4338–4343. [CrossRef] [PubMed]
214. Criado, P.; Fraschini, C.; Salmieri, S.; Lacroix, M. Cellulose nanocrystals (CNCs) loaded alginate films against
lipid oxidation of chicken breast. Food Res. Int. 2020, 132. [CrossRef]
215. Tahir, H.E.; Zhihua, L.; Mahunu, G.K.; Xiaobo, Z.; Arslan, M.; Xiaowei, H.; Yang, Z.; Mariod, A.A. Effect of gum
arabic edible coating incorporated with African baobab pulp extract on postharvest quality of cold stored
blueberries. Food Sci. Biotechnol. 2020, 29, 217–226. [CrossRef]
216. Sakooei-Vayghan, R.; Peighambardoust, S.H.; Hesari, J.; Peressini, D. Effects of osmotic dehydration (with
and without sonication) and pectin-based coating pretreatments on functional properties and color of hot-air
dried apricot cubes. Food Chem. 2020, 311, 125978. [CrossRef]
217. Martínez-González, M.D.C.; Bautista-Baños, S.; Correa-Pacheco, Z.N.; Corona-Rangel, M.L.;
Ventura-Aguilar, R.I.; Del Río-García, J.C.; Ramos-García, M.D.L. Effect of nanostructured chitosan/propolis
coatings on the quality and antioxidant capacity of strawberries during storage. Coatings 2020, 10, 90.
[CrossRef]
218. Luo, P.; Li, F.; Liu, H.; Yang, X.; Duan, Z. Effect of fucoidan-based edible coating on antioxidant degradation
kinetics in strawberry fruit during cold storage. J. Food Process. Preserv. 2020. [CrossRef]
219. Emamifar, A.; Bavaisi, S. Nanocomposite coating based on sodium alginate and nano-ZnO for extending
the storage life of fresh strawberries (Fragaria × ananassa Duch.). J. Food Meas. Charact. 2020, 14, 1012–1024.
[CrossRef]
220. El-Mogy, M.M.; Parmar, A.; Ali, M.R.; Abdel-Aziz, M.E.; Abdeldaym, E.A. Improving postharvest storage
of fresh artichoke bottoms by an edible coating of Cordia myxa gum. Postharvest Biol. Technol. 2020, 163.
[CrossRef]
221. Valencia, G.A.; Zare, E.N.; Makvandi, P.; Gutiérrez, T.J. Self-assembled carbohydrate polymers for food
applications: A review. Compr. Rev. Food Sci. Food Saf. 2019, 18, 2009–2024. [CrossRef]
222. Ulutasdemir, T.; Cagri-Mehmetoglu, A. Effects of edible coating containing Williopsis saturnus var. saturnus
on fungal growth and aflatoxin production by Aspergillus flavus in peanuts. J. Food Saf. 2019, 39. [CrossRef]
223. Totad, M.G.; Sharma, R.R.; Sethi, S.; Verma, M.K. Effect of edible coatings on ‘Misty’ blueberry (Vaccinium
corymbosum) fruits stored at low temperature. Acta Physiol. Plant. 2019, 41. [CrossRef]
224. Thakur, R.; Pristijono, P.; Scarlett, C.J.; Bowyer, M.; Singh, S.P.; Vuong, Q.V. Starch-based edible coating
formulation: Optimization and its application to improve the postharvest quality of “Cripps pink” apple
under different temperature regimes. Food Packag. Shelf Life 2019, 22. [CrossRef]
225. Tarazona, A.; Gomez, J.V.; Mateo, E.M.; Jimenez, M.; Mateo, F. Antifungal effect of engineered silver
nanoparticles on phytopathogenic and toxigenic Fusarium spp. and their impact on mycotoxin accumulation.
Int. J. Food Microbiol. 2019, 306, 108259. [CrossRef] [PubMed]
226. Tang, F.; Aldridge, D.C. Microcapsulated biocides for the targeted control of invasive bivalves. Sci. Rep. 2019,
9, 18787. [CrossRef]
227. Khoshnoudi-Nia, S.; Sedaghat, N. Effect of active edible coating and temperature on quality properties of
roasted pistachio nuts during storage. J. Food Process. Preserv. 2019, 43. [CrossRef]
228. Khodaei, D.; Hamidi-Esfahani, Z. Influence of bioactive edible coatings loaded with Lactobacillus plantarum
on physicochemical properties of fresh strawberries. Postharvest Biol. Technol. 2019, 156. [CrossRef]
Coatings 2020, 10, 687 43 of 45

229. Barreto, M.R.; Aleixo, N.A.; Silvestre, R.B.; Fregonezi, N.F.; Barud, H.D.S.; Dias, D.D.S.; Ribeiro, C.A.;
Resende, F.A. Genotoxicological safety assessment of puree-only edible films from onion bulb (Allium cepa L.)
for use in food packaging-related applications. J. Food Sci. 2020, 85, 201–208. [CrossRef]
230. Zhao, L.; Fan, H.; Zhang, M.; Chitrakar, B.; Bhandari, B.; Wang, B. Edible flowers: Review of flower processing
and extraction of bioactive compounds by novel technologies. Food Res. Int. 2019, 126, 108660. [CrossRef]
231. Sicari, V.; Loizzo, M.R.; Pellicanò, T.M.; Giuffrè, A.M.; Poiana, M. Evaluation of Aloe arborescens gel as
new coating to maintain the organoleptic and functional properties of strawberry ( Fragaria × ananassa cv.
Cadonga) fruits. Int. J. Food Sci. Technol. 2019, 55, 861–870. [CrossRef]
232. Rastegar, S.; Khankahdani, H.H.; Rahimzadeh, M. Effectiveness of alginate coating on antioxidant enzymes
and biochemical changes during storage of mango fruit. J. Food Biochem. 2019, 43, e12990. [CrossRef]
[PubMed]
233. Talmaciu, A.I.; Ravber, M.; Volf, I.; Knez, Ž.; Popa, V.I. Isolation of bioactive compounds from spruce bark
waste using sub- and supercritical fluids. J. Supercrit. Fluids 2016, 117, 243–251. [CrossRef]
234. Jacotet-Navarro, M.; Laguerre, M.; Fabiano-Tixier, A.S.; Tenon, M.; Feuillere, N.; Bily, A.; Chemat, F. What is
the best ethanol-water ratio for the extraction of antioxidants from rosemary? Impact of the solvent on yield,
composition, and activity of the extracts. Electrophoresis 2018. [CrossRef] [PubMed]
235. Ganiari, S.; Choulitoudi, E.; Oreopoulou, V. Edible and active films and coatings as carriers of natural
antioxidants for lipid food. Trends Food Sci. Technol. 2017, 68, 70–82. [CrossRef]
236. Ramos, M.; Valdés, A.; Beltrán, A.; Garrigós, M. Gelatin-based films and coatings for food packaging
applications. Coatings 2016, 6, 41. [CrossRef]
237. Koubaa, M.; Barba, F.J.; Grimi, N.; Mhemdi, H.; Koubaa, W.; Boussetta, N.; Vorobiev, E. Recovery of colorants
from red prickly pear peels and pulps enhanced by pulsed electric field and ultrasound. Innov. Food Sci.
Emerg. Technol. 2016, 37, 336–344. [CrossRef]
238. Choulitoudi, E.; Bravou, K.; Bimpilas, A.; Tsironi, T.; Tsimogiannis, D.; Taoukis, P.; Oreopoulou, V.
Antimicrobial and antioxidant activity of Satureja thymbra in gilthead seabream fillets edible coating.
Food Bioprod. Process. 2016, 100, 570–577. [CrossRef]
239. Bonilla, J.; Sobral, P.J.A. Investigation of the physicochemical, antimicrobial and antioxidant properties
of gelatin-chitosan edible film mixed with plant ethanolic extracts. Food Biosci. 2016, 16, 17–25. [CrossRef]
240. Haddar, A.; Sellimi, S.; Ghannouchi, R.; Alvarez, O.M.; Nasri, M.; Bougatef, A. Functional, antioxidant
and film-forming properties of tuna-skin gelatin with a brown algae extract. Int. J. Biol. Macromol. 2012, 51,
477–483. [CrossRef]
241. Zhang, L.; Kou, X.; Huang, X.; Li, G.; Liu, J.; Ye, J. Peach-gum: A promising alternative for retarding
the ripening and senescence in postharvest peach fruit. Postharvest Biol. Technol. 2020, 161. [CrossRef]
242. Mohamed, C.; Elise, N.G.; Etienne, T.V.; Loiseau, G.; Montet, D. Antifungal activity of edible coating made
from chitosan and lactoperoxidase system against Phomopsis sp. RP257 and Pestalotiopsis sp. isolated from
mango. J. Food Saf. 2020. [CrossRef]
243. Maringgal, B.; Hashim, N.; Amin Tawakkal, I.S.M.; Muda Mohamed, M.T.; Hazwan Hamzah, M.; Ali, M.M.;
Abd Razak, M.F.H. Kinetics of quality changes in papayas (Carica papaya L.) coated with Malaysian stingless
bee honey. Sci. Hortic. 2020, 267. [CrossRef]
244. Li, D.; Karsli, B.; Rubio, N.K.; Janes, M.; Luo, Y.; Prinyawiwatkul, W.; Xu, W. Enhanced microbial safety of
channel catfish (Ictalurus punctatus) fillet using recently invented medium molecular weight water-soluble
chitosan coating. Lett. Appl. Microbiol. 2020. [CrossRef] [PubMed]
245. Arroyo, B.J.; Bezerra, A.C.; Oliveira, L.L.; Arroyo, S.J.; Melo, E.A.; Santos, A.M.P. Antimicrobial active edible
coating of alginate and chitosan add ZnO nanoparticles applied in guavas (Psidium guajava L.). Food Chem.
2020, 309, 125566. [CrossRef]
246. Zheng, K.; Xiao, S.; Li, W.; Wang, W.; Chen, H.; Yang, F.; Qin, C. Chitosan-acorn starch-eugenol edible film:
Physico-chemical, barrier, antimicrobial, antioxidant and structural properties. Int. J. Biol. Macromol. 2019,
135, 344–352. [CrossRef]
247. Lu, Y.; Zhao, X.; Fang, S. Characterization, antimicrobial properties and coatings application of gellan gum
oxidized with hydrogen peroxide. Foods 2019, 8, 31. [CrossRef]
248. Kulawik, P.; Jamróz, E.; Özogul, F. Chitosan role for shelf-life extension of seafood. Environ. Chem. Lett. 2019,
18, 61–74. [CrossRef]
Coatings 2020, 10, 687 44 of 45

249. Shen, Z.; Kamdem, D.P. Antimicrobial activity of sugar beet lignocellulose films containing tung oil
and cedarwood essential oil. Cellulose 2015, 22, 2703–2715. [CrossRef]
250. Severino, R.; Ferrari, G.; Vu, K.D.; Donsì, F.; Salmieri, S.; Lacroix, M. Antimicrobial effects of modified
chitosan based coating containing nanoemulsion of essential oils, modified atmosphere packaging and gamma
irradiation against Escherichia coli O157:H7 and Salmonella Typhimurium on green beans. Food Control
2015, 50, 215–222. [CrossRef]
251. Emam-Djomeh, Z.; Moghaddam, A.; Yasini Ardakani, S.A. Antimicrobial activity of pomegranate
(Punica granatum L.) peel extract, physical, mechanical, barrier and antimicrobial properties of pomegranate
peel extract-incorporated sodium caseinate film and application in packaging for ground beef. Packag. Technol.
Sci. 2015, 28, 869–881. [CrossRef]
252. Sanchez-Ortega, I.; Garcia-Almendarez, B.E.; Santos-Lopez, E.M.; Amaro-Reyes, A.; Barboza-Corona, J.E.;
Regalado, C. Antimicrobial edible films and coatings for meat and meat products preservation. Sci. World J.
2014, 2014, 248935. [CrossRef]
253. De Lacey, A.M.L.; López-Caballero, M.E.; Montero, P. Agar films containing green tea extract and probiotic
bacteria for extending fish shelf-life. LWT–Food Sci. Technol. 2014, 55, 559–564. [CrossRef]
254. Iturriaga, L.; Olabarrieta, I.; De Maranon, I.M. Antimicrobial assays of natural extracts and their inhibitory
effect against Listeria innocua and fish spoilage bacteria, after incorporation into biopolymer edible films.
Int. J. Food Microbiol. 2012, 158, 58–64. [CrossRef]
255. Deng, Q.; Zhao, Y. Physicochemical, nutritional, and antimicrobial properties of wine grape (cv. Merlot)
pomace extract-based films. J. Food Sci. 2011, 76, E309–E317. [CrossRef] [PubMed]
256. Gomez-Estaca, J.; De Lacey, A.L.; Lopez-Caballero, M.E.; Gomez-Guillen, M.C.; Montero, P.
Biodegradable gelatin-chitosan films incorporated with essential oils as antimicrobial agents for fish
preservation. Food Microbiol. 2010, 27, 889–896. [CrossRef] [PubMed]
257. Ponce, A.G.; Roura, S.I.; Del Valle, C.E.; Moreira, M.R. Antimicrobial and antioxidant activities of edible
coatings enriched with natural plant extracts: In vitro and in vivo studies. Postharvest Biol. Technol. 2008, 49,
294–300. [CrossRef]
258. No, H.K.; Meyers, S.P.; Prinyawiwatkul, W.; Xu, Z. Applications of chitosan for improvement of quality
and shelf life of foods: A review. J. Food Sci. 2007, 72, R87–R100. [CrossRef]
259. Rudra, J.S.; Dave, K.; Haynie, D.T. Antimicrobial polypeptide multilayer nanocoatings. J. Biomater. Sci.
Polym. Ed. 2006, 17, 1301–1315. [CrossRef]
260. Pinzon, M.I.; Sanchez, L.T.; Garcia, O.R.; Gutierrez, R.; Luna, J.C.; Villa, C.C. Increasing shelf life of
strawberries (Fragaria ssp) by using a banana starch-chitosan-Aloe vera gel composite edible coating. Int. J.
Food Sci. Technol. 2019, 55, 92–98. [CrossRef]
261. Kavas, G.; Kavas, N. Use of egg white protein powder based films fortified with sage and lemon balm
essential oils in the storage of lor cheese. Mljekarstvo 2016, 66, 99–111. [CrossRef]
262. Molina-Hernández, J.B.; Castro, A.E.; Martinez-Correa, H.A.; Andrade-Mahecha, M.M. Edible coating based
on achira starch containing garlic/oregano oils to extend the shelf life of double cream cheese. Rev. Fac. Nac.
Agron. Medellín 2020, 73, 9099–9108. [CrossRef]
263. Hernández-Guerrero, S.E.; Balois-Morales, R.; Palomino-Hermosillo, Y.A.; López-Guzmán, G.G.;
Berumen-Varela, G.; Bautista-Rosales, P.U.; Alejo-Santiago, G. Novel edible coating of starch-based
stenospermocarpic mango prolongs the shelf life of mango “ataulfo” fruit. J. Food Qual. 2020, 2020,
1–9. [CrossRef]
264. Martínez-Ortiz, M.A.; Palma-Rodríguez, H.M.; Montalvo-González, E.; Sáyago-Ayerdi, S.G.; Utrilla-Coello, R.;
Vargas-Torres, A. Effect of using microencapsulated ascorbic acid in coatings based on resistant starch
chayotextle on the quality of guava fruit. Sci. Hortic. 2019, 256. [CrossRef]
265. Bersaneti, G.T.; Garcia, S.; Mali, S.; Colabone Celligoi, M.A.P. Evaluation of the prebiotic activities of edible
starch films with the addition of nystose from Bacillus subtilis natto. LWT 2019, 116. [CrossRef]
266. Saberi, B.; Chockchaisawasdee, S.; Golding, J.B.; Scarlett, C.J.; Stathopoulos, C.E. Characterization of pea
starch-guar gum biocomposite edible films enriched by natural antimicrobial agents for active food packaging.
Food Bioprod. Process. 2017, 105, 51–63. [CrossRef]
267. Shah, S.; Hashmi, M.S. Chitosan–aloe vera gel coating delays postharvest decay of mango fruit. Hortic. Environ.
Biotechnol. 2020. [CrossRef]
Coatings 2020, 10, 687 45 of 45

268. Khatri, D.; Panigrahi, J.; Prajapati, A.; Bariya, H. Attributes of Aloe vera gel and chitosan treatments on
the quality and biochemical traits of post-harvest tomatoes. Sci. Hortic. 2020, 259. [CrossRef]
269. Sahu, P.; Giri, D.; Singh, R.; Pandey, P.; Gupta, S.; Shrivastava, A.; Kumar, A.; Pandey, K. Therapeutic
and medicinal uses of aloe vera: A review. Pharmacol. Pharm. 2013, 4, 599–610. [CrossRef]
270. Rosenbloom, R.A.; Wang, W.; Zhao, Y. Delaying ripening of ‘Bartlett’ pears (Pyrus communis) during
long-term simulated industrial cold storage: Mechanisms and validation of chitosan coatings with cellulose
nanocrystals Pickering emulsions. LWT 2020, 122. [CrossRef]

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