Food Eng Rev (2013) 5:200–216

DOI 10.1007/s12393-013-9072-5

REVIEW ARTICLE

Natural Additives in Bioactive Edible Films and Coatings:

Functionality and Applications in Foods
A. Silva-Weiss • M. Ihl • P. J. A. Sobral •

M. C. Gómez-Guillén • V. Bifani

Received: 28 January 2013 / Accepted: 5 August 2013 / Published online: 17 August 2013
Ó Springer Science+Business Media New York 2013

Abstract Incorporation of natural additives to active bioactive properties has not yet been characterized with
packaging systems or biopolymer-based edible films can respect to their ability to be applied directly on foods and
modify the film structure and, as a result, modify their used to develop active packaging or biopolymer-based
functionality and application to foods. This paper reviews edible films for preserving and adding value to foods. In
the effect of the incorporation of natural additives from addition, in vivo studies of the use of bioactive films to
plant extracts or their isolated active compounds and preserve the quality, shelf life, and nutritional value of
vitamins on the functionality of edible films and the foods remain limited.
application of these films to foods. The final functionality
of edible films is related to their bioactive properties (such Keywords Biopolymers
Bioactive compounds

as antioxidant, antimicrobial, and antibrowning activities) Plant-based products
Vitamins
Interactions
and functional properties (such as barrier to oxygen, carbon
dioxide, and UV–vis light); water vapor permeability;
tensile stress; elongation at break; and physical properties Introduction
(such as opacity and color). Several categories of natural
antioxidants found in plant, spices, and herbs (organic Natural additives from plant extracts, their isolated active
acids, plant natural extracts, and plant essential oils) have compounds, plant-based products, and vitamins can pro-
been incorporated into edible films and coatings, resulting vide antioxidant, antimicrobial, and/or antibrowning
in an improvement of the bioactive properties of the films. activity on edible films and coatings. However, the effect
However, a wide range of plant natural sources with of these active components on the structure and function-
ality of the films and food quality has not been analyzed
together.
A. Silva-Weiss (&)
Doctoral Program in Science of Natural Resources, Scientific The development of edible films and coatings is an
and Technological Bioresource Nucleus (BIOREN-UFRO), environmentally friendly technology that would permit a
Universidad de La Frontera, PO Box 54-D, Temuco, Chile reduction in the impact and disposal costs associated with
e-mail: acsilva@ufro.cl
synthetic polymer films. Edible films and coatings can be
M. Ihl
V. Bifani used as active packaging, extending the shelf life in a wide
Chemical Engineering Department, Universidad de La Frontera, variety of food applications by preventing dehydration,
PO Box 54-D, Temuco, Chile microbial growth, oxidative rancidity, surface browning,
and oil diffusion. The inherent biodegradability and edi-
P. J. A. Sobral
Food Engineering Department, University of São Paulo, PB 23, bility of these films and coatings must be maintained by the
Pirassununga, SP 13635-900, Brazil addition of food-grade ingredients in facilities that are
acceptable for food processing, in which the solvents used
M. C. Gómez-Guillén
are restricted to water and ethanol [121]. The ultimate
Instituto de Ciencia y Tecnologı́a de Alimentos y Nutrición
(ICTAN, CSIC), C/José Antonio Novais, 10, 28040 Madrid, functionality of edible films is related to their bioactivity
Spain (such as antioxidant, antimicrobial, and antibrowning) and

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Food Eng Rev (2013) 5:200–216 201

their functional (such as their ability to serve as a barrier to components [47]. Films or coatings also can be used as pou-
water vapor, oxygen, carbon dioxide, and UV–vis light), ches or wraps. The film-forming solution (FFS) can be applied
their mechanical (such as tensile stress and elongation at to food to generate an edible coating. If the FFS is applied as a
break) and physical (such as opacity and color) properties. thin layer on a flat surface and is allowed to dry, it is referred to
In addition, they can preserve or enhance the sensorial as an edible film, the physical and mechanical properties of
properties and may have the ability to modify the internal which can be studied separately from the coated material.
atmosphere of foods. Finally, manufacturers make a choice The methods used for the film formation are solvent
on the most appropriate type of packaging or edible films, casting (wet process) and extrusion (dry process). The
depending on the nature and requirements of the product, solvent casting is the most common technique used to form
the degree and nature of the protection need, the method of hydrocolloid edible films. Casting is a discontinuous pro-
distribution, the shelf life, and environmental impact. cess that requires polymer solubilization followed by a
Synthetic additives are being avoided more and more drying step to remove the solvent. The extrusion process
due to their potentially toxic effects [14, 84]. Plant-based uses thermoplastic biopolymers associated with plasticizers
bioactive agents are being incorporated in food as promi- and low levels of moisture. These techniques can be used
nent alternatives to chemical preservatives and additives. for large-scale production of edible films [51]. Extrusion
Their use in foods helps to address consumer demands for process is related to high temperatures, which could be
minimally processed natural products while providing affecting some sensible active compounds on films. When
some extra benefits to both food and the consumer [19, 20, comparing extrusion with solvent casting process, there can
83]. This contributes to the current demand, reported by be observed an increase in its elongation, although film
Food and Agriculture Organization (FAO) and the food solubility (36–40 %) did not change significantly between
industry, for fresh food products that are natural and easy to the different processes evaluated [2]. Films prepared by
consume, have specific advantages for health, are micro- casting are more homogeneous and transparent, with lower
biologically safe, and lack synthetic additives [27, 57]. opacity and water vapor permeability (WVP) values,
Research has shown that incorporation of extracts and compared to films prepared by other techniques [35].
natural components from plants, spices, and herbs on pack- The structural matrix of edible coatings and films is
aging, films, and coatings improves their active properties as developed from proteins, polysaccharides, and lipids or
antioxidants, antimicrobials, and/or antibrownings [44, 105, blends of them, called composite films. To create an edible
118]. The active additives on edible coatings can add value to coating or biodegradable packaging film, a base material in
food products by increasing their shelf life [38, 70, 117]. The solution must constitute a sufficiently cohesive structural
development of active packaging systems and edible films matrix [48]. Edible films and coatings must be uniform and
using natural additives, particularly those with antimicrobial without defects to optimize their functionalities [107]. Fatty
properties, has been studied on different subjects as for acids and other lipidic compounds, including natural fats,
example fresh-cut broccoli, grapes, fish, against listeria, and surfactants, and resins, can also be added. These can improve
fish spoilage bacteria [5, 28, 56, 70, 93, 94, 116]. the water barrier properties of the hydrocolloid matrix [114].
This paper discusses the development of active edible Surfactants can maximize the adhesion of the coating to the
films and coatings that incorporate natural additives from product [71]. To reduce the rigidity and glass transition
plant extracts, plant-based products, and vitamins. The top- temperature of the polymers, plasticizers rich in hydroxyl
ics of interest are as follows: (1) factors to consider when groups (such as glycerol, sorbitol, acetylated monoglyceride,
interactions occur between the natural additive and the polyethylene glycol, sucrose, and inverted sugars) can be
coating/film, and the active film and the food, and how these added. An appropriate concentration of plasticizer, between
interactions can affect film properties; (2) the effects of 15 and 30 % w/w of the total polymer weight, is needed
natural additives on the structure and consequently, on the depending on the biopolymer used [75, 77, 105]. Plasticizers
functionality and bioactive properties (antioxidant, antimi- increase flexibility but reduce the barrier to water vapor [45].
crobial, and antibrowning) of active edible films; and (3) the This is undesirable in foods with intermediate moisture,
effects of active edible films with natural additives on the which are characterized by a high water activity (from 0.65 to
bioactive properties and quality of fresh food products. 0.90) and a generally soft texture. An increase in the amount
of glycerol used as a plasticizer leads to a gradually
decreasing contact angle value of starch films due to glycerol
Edible Films and Coatings: Concept, Formulation, hydrophilicity [12], which enhances the distribution of the
and Requirements coating and contributes to the formation of a homogeneous
thickness above the food.
Edible films are defined as a thin layer of edible material To improve the appearance of coated foods, the adhe-
formed on a food as a coating or placed on between food sion, cohesion, and durability of edible coatings should be

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controlled [65]. The main functions of edible films and Interactions Among Additives, Film, and Food
coatings include the control of mass transfer (preventing
the loss of solutes and volatiles), mechanical protection, The interaction between the film and the foodstuff (solid/
and sensory appeal. The mechanical strength of an edible solid interface) depends on the molecular size of the bio-
film must be adequate to protect the integrity and thermal polymer (weight and volume), the chemical nature of the
insulation of both food and packaging during distribution compounds (polarity, planarity, etc.), the temperature and
[37, 48, 63]. process conditions, the film structure (crystallinity, plasti-
Currently, edible films and coatings are used in a variety cizing, morphology, glass transition temperature, etc.), the
of food applications. In case of fruit and vegetables, to thickness of the film, and the nature of the material. When
maintain the quality, edible films and coatings should a coating is in contact with a food, the coating evaporation
create a semi-permeable barrier against moisture migra- flux at the interface between the coating/environment
tion, carbon dioxide (CO2), aromas, and lipids from, and (liquid/air) should be evaluated, as well as the coating
the absorption of oxygen (O2) by, the foodstuff. The absorption flux on the food due to the interface between the
reduction of O2 availability and increased CO2 concentra- food/coating (solid/liquid) [62].
tions on fruits reduces ethylene levels, reducing ripening, Studies should specifically address the compatibility of
respiration rate, and water loss, increasing the shelf life. the coating agent and active compounds because the
The semi-permeable barrier regulates the atmosphere properties of the resulting film depend on their binary
around foods, preventing their desiccation and controlling combination and the ratio between them, which, in turn,
the migration of ingredients and additives in the food depends on the required dosage of active compounds in the
systems. In meat products, edible films and coatings can material (Table 1). According to the plant extract type that
also serve as carrier for antimicrobial, antioxidant, nutri- is incorporated in the films, the concentration of the plant
ents, color, herbs, and spices. Collagen films and sausage extract added to the biopolymer films should be analyzed,
castings are probably the most successful commercial since a high concentration could generate undesirable
application [110]. In fish, an extension of 8–10 days odors, turbidity, and/or compound precipitation on the
refrigerated shelf life has been obtained with tea and films and may promote oxidation in lipid systems [115].
rosemary extracts in chitosan coatings [70]. According to Cosgrove [25], the dose of the active com-
Ingredients in food packaging that may migrate to food pounds needs to be relatively low. In general, the compo-
are considered food additives and must meet food additive sition of a film strip can include 30 % active ingredient.
standards [34]. Additives are incorporated to contribute to Properties of films, coatings, and foods that can be affected
the overall quality, safety, nutritive value, organoleptic by the incorporation of natural additives are summarized in
characteristics (color, smell, and taste), convenience, and Table 2. The chemical or physical interactions between bio-
economy of foods [55]. Edible films and coatings can polymers and natural additives or bioactive compounds can
transport food additives to improve the mechanical affect their structure and, consequently, their functionality.
integrity and/or handling characteristics of the foods [65, The nature of the interaction between biopolymers and addi-
121]. They also can act as a vehicle to fortify foods with tives for preservation depends on the nature, chemical char-
vitamins such as folic acid and ascorbic acid as well as acteristics, concentration, and pH of both the biopolymer and
other nutrients such as omega-3 fatty acids [68, 103]. additives [30], as well as on the structural parameters of the
These films have the potential to control oxidation, which active compounds (stereochemistry, conformational flexibil-
causes browning and/or microbial spoilage [43, 70, 116]. ity, and molecular weight). Interactions between natural/
Thus, the new generation of edible films and coatings or active compounds and the film material may be identified by
active packaging has been specifically designed to the presence of new absorption bands in the UV–visible
increase functionality by incorporating bioactive/func- regions of the electronic absorption spectra of the natural/
tional natural additives. According to AIMPLAS [3], new active compounds [94].
active compounds from plant extracts could improve the In a food packaging system, three phases should be con-
shelf life of perishable fresh foods by 20 percent. The sidered: the food, the edible coating/film, and the environ-
quality of a food product whose useful life is short ment (Fig. 1). Most biopolymers are semi-crystalline. Mass
(4–5 days) could be extended by one or two additional transport through semi-crystalline materials can be consid-
days through the use of this new type of active packaging, ered to occur via the amorphous region of the material.
minimizing losses from spoilage through better conser- Interactions or mass transfer among the film/foodstuff/
vation and durability; taking into account, however, the environment can be classified as permeation, sorption, and
incorporation of additives increases the number of stages migration. In permeation, compounds from the environment
required for processing, implying a higher production (such as volatiles, gases, vapors, or liquids) are transported to
cost. the film/material in contact with the food and vice versa.

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Table 1 Active compounds added to biopolymer-based edible films: concentration and effect
Active compounds Concentration Biopolymer-based film References
Effects of active compounds

Vitamins and/or acidulants [167 mg g/g polymer Methylcellulose Ayranci and Tunc [11]
Increases the WVP of films at higher concentrations
a-Tocopherol \100 mg/kg meat Chitosan Georgantelis et al. [38]
Has pro-oxidative effects on meat at higher
concentrations
Gallic acid, ferulic acids and/or 3 mg/cm2 film Zein films Arcan and Yemenicioğlu [8]
flavonoids such as catechin, Catechin, gallic acid, p-hydroxybenzoic acid and
flavone or quercetin ferulic acid eliminate film brittleness and increase
their flexibility to 189 %
Rosemary extracts \1.0 g/L FFS Chitosan Wambura et al. [115]
Confers an undesirable odor at higher concentrations
Tea extract \2.5 g/L FFS Chitosan Wambura et al. [115]
Induces turbidity at higher concentrations
Murta extracta 20 mL/g polymer or Chitosan–starch Silva-Weiss et al. [104]
81 mg GAE/g Increases the thickness and turns from yellow to
polymer slight orange color thickness and turns from
yellow to slight orange color
Rosemaryb 20 mg/g polymer Chitosan Georgantelis et al. [38]
Improve antioxidative effect.
Kiam wooda 300–1,500 mg/L HPMC Chana-Thaworn et al. [21]
Increases WVP and film solubility. Decreases
mechanical properties. Darkens film color and
decreases transparency
Garlic oil 100 lL/g polymer Chitosan Pranoto et al. [95]
At these levels, the films were physically acceptable
in term of appearance, mechanical and physical
properties
Sodium carboxymethylcellulose (CMC), hydroxypropyl methylcellulose (HPMC), gallic acid equivalent (GAE), film-forming solution (FFS)
a
Aqueous extract
b
Ethanol:water extract (1:8)

Transport of small molecules or compounds through the film edible films incorporating garlic oil were compared by Pra-
can be explained by sorption, diffusion, and desorption noto et al. [95] with conventional food preservative potas-
mechanisms. The sorption of solutes from the environment sium sorbate and bacteriocin nisin, showing an increase in its
or from foodstuff compounds, such as flavor, aroma, or dyes, antimicrobial efficiency against Escherichia coli, Staphylo-
that interact with biopolymers, depends on the charge density coccus aureus, Salmonella typhimorium, Listeria monocyt-
of the polymer and pH of the polymer network as well as on ogenes, and Bacillus cereus. The incorporation of garlic oil
the dielectric constant of the media [111]. This reveals the into chitosan films showed desirable characteristics as a
importance of electrostatic interactions, in which negatively physical and antimicrobial barrier to food contamination.
charged chain biopolymers can absorb positively charged According to Perez-Perez et al. [91], the migration of com-
compounds. The sorption of solutes on the film matrix can pounds from chitosan, like organic acids, is a complex
also occur by hydrophobic interactions and H-bonding on the phenomenon that involves many factors such as electrostatic
extreme surface of the film or coating. Migration represents interactions, ionic osmosis, and structural changes in the
the mass transfer of compounds, originally present in the polymer, induced by the presence of the acids.
film, to the food or vice versa (negative migration). A
function of films and coatings is decreasing the migration of
moisture and aromas, among other compounds, from foods. Functionality of Edible Films
Moreover, the migration of particular active agents from the
film, such as antioxidants and antimicrobial agents, could The functionality of edible films depends on their bioactive
improve the shelf life of the product. For example, chitosan and physical properties. Bioactive properties include

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Table 2 Properties of coatings,

Interactions
films, and food that could be
affected by interactions with Natural additive—coating Natural additive—film Active film/coating—food
active agents or natural
additives Properties
Compatibility and stability Physico-mechanical Surface
Temperature and pH Resistance and elasticity Adhesion
Turbidity Color, gloss, light Wettability
Moisture content
Rheological Barrier Physiological
Temperature and pH O2 and CO2 permeability Respiration rate
Shear rate Water vapor permeability Nutrient concentration
Concentration UV light barrier
Viscoelasticity
Thermal Control delivery and bioavailability
Glass transition temperature Temperature and pH
Crystallization point
Melting point
Decomposition point
Morphology and structure
Crystallinity
Bond type
Shape
Sensorial
Texture, color, odor, flavor, etc.
Biological
Antioxidant, antimicrobial and antibrowning activities

Fig. 1 Natural additive

molecules (gray circle): e.g.,
bioactive compounds or plant
extracts, plant-based products,
and vitamins; food molecules:
e.g., flavorings (gray triangle)
and vitamins (black square);
environmental molecules: e.g.,
oxygen and/or odor (black
circle)

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antioxidant, antimicrobial, and antibrowning activities. reaching 16 % after 6 weeks, depending on the fish gelatin
Among the physical properties are barrier to oxygen, car- source. The interaction between gelatin and vitamin E
bon dioxide, and UV–vis light, water vapor permeability reduces the elongation of the gelatin-based film to 33 %
(WVP), tensile stress (TS), elongation at break (EB), after 6 weeks of storage. The reduction in the film’s
opacity, and color. The incorporation of the natural addi- mechanical properties occurs because the interaction
tives to active packaging systems or biopolymer-based between vitamin E and fish gelatin decreases the movement
edible films can modify the film structure and, as a result, of macromolecules in the biopolymer film [60].
modify their functionality and application to foods. Changes in the mechanical properties of biopolymer-
based films, when natural extracts are added, are presented
Mechanical Properties in Table 3. Green tea water extract (GTE) slightly increa-
ses the mechanical resistance (or TS) and extensibility (or
Tensile strength and elongation at break are parameters that EB) of chitosan-based films [105] but decreases the TS and
are related to the film’s mechanical properties and chemical EB of both agar and agar–gelatin films [40], negatively
structure [79]. The tensile strength (TS, MPa) is the max- affecting the film’s mechanical properties. The mechanical
imum strength measuring the resistance of the film, properties of chitosan film did not significantly change
whereas the percentage of elongation at break (EB, %) is a when the GTE concentration increased from 0 to 5 % but
measure of the stretching capacity or flexibility of the film significantly increased when the GTE concentration chan-
prior to breaking [65]. ged from 5 to 20 % [105]. The improvement in the
The addition of vitamin E to films, based on fish skin mechanical properties of the films containing GTE may be
gelatin from Priacanthus macracanthus and Lutjanus vitta, attributed to the interaction between the chitosan matrix
modifies film’s mechanical properties over time [60]. Ini- and the polyphenolic compounds from the GTE. In general,
tially, vitamin E decreases the film tensile strength to 14 %, the incorporation of polyphenol-rich aqueous extracts

Table 3 Effects of plant aqueous extracts and phenolic compounds on the physical properties of edible films
Additive Biopolymer
Thickness (lm) Mechanical properties References
TS (MPa) EB (%)

Chitosan
– 70.7 ± 5.0 29.69 ± 1.89 45.10 ± 1.40 Silva-Weiss et al. [104]
Murta leavea 77.5 ± 3.5 n.d. n.d. Silva-Weiss et al. [104]
– 62.1 ± 6.3 23.66 ± 2.63 54.62 ± 3.12 Siripatrawan and Harte [105]
Green teaa 62.1 ± 6.3 25.13 ± 1.91 58.14 ± 4.24 Siripatrawan and Harte [105]
– *80 24.00 ± 3.00 29.00 ± 2.00 Moradi et al. [83]
Grape seeda *80 16.00 ± 0.60 21.00 ± 3.00 Moradi et al. [83]
– *75 *18 Rivero et al. [96]
Tannic acid (40 mg/g chitosan) *95 *25 Rivero et al. [96]
Chitosan–starch
– 72.0 ± 2.4 20.56 ± 1.78 13.52 ± 2.85 Silva-Weiss et al. [104]
Murta leavea 126 ± 12 17.13 ± 1.22 6.57 ± 2.43 Silva-Weiss et al. [104]
– 73.5 ± 3.9 *42 *57 Mathew and Abraham [76]
Ferulic acid 78.9 ± 4.3 *49 *60 Mathew and Abraham [76]
Agar
– 18.48 ± 1.28 62.35 ± 2.49 Giménez et al. [40]
Green teaa 7.88 ± 1.02 51.69 ± 3.92 Giménez et al. [40]
Agar-fish gelatin
– 15.03 ± 1.50 77.60 ± 5.76 Giménez et al. [40]
Green teaa 6.88 ± 1.46 59.05 ± 3.20 Giménez et al. [40]
TS tensile strength (MPa), EB elongation at break (%), n.d. non-determinate. Different superscript letters in the same column represent significant
differences (P \ 0.05)
a
Aqueous extract

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reduces the mechanical properties (TS and EB) of the films crosslinkings between protein chains and/or the protein and
[40, 83, 104]. However, the addition of phenolic acid to the vitamin E during storage and the re-crystallization of the
film has been shown to slowly increase these properties gelatin in the matrix of the film [9], which produces a
[76, 96]. However, there is a negative relationship between matrix that is less permeable and more dense.
the concentration of phenolic compounds in the plant Chitosan coatings have been widely used in postharvest
extract and the film’s mechanical properties: extracts studies of fruits and vegetables because they maintain food
containing a higher concentration of phenolic compounds, quality and reduce the respiration rate (O2 barrier), ethyl-
murta leaves extract of ecotype SC, strongly reduced the ene production, and transpiration [31–33, 69, 87, 116]. As
tensile stress and elongation at break of gelatin-based films, another benefit, the addition of chitosan reduces the WVP
while films containing the murta leaves extract of ecotype and solubility of starch films [12, 113].
SG behaved similarly to the control film [44]. In other studies, red natural pigment (betalain) added to
HPMC-based films increased their WVP when they were
Water Vapor and Gases Barrier Properties measured at 38 °C and at a 90 % RH gradient. Besides, this
permeability did not change significantly after 20 days of
For food applications, the oxygen (O2), carbon dioxide light exposure [4]. Active compounds in the film could
(CO2), and water vapor (WVP) permeability of biomate- remain constant over time, because the red color of betalain
rials should be considered. Due to the hydrophilic nature of increased the film’s light barrier, thereby maintaining the
films, its barrier properties are dependent on the sur- stability of the film properties over time.
rounding relative humidity conditions [72]. For this reason,
tests should be carried out at constant storage conditions, % Light Barrier Properties and Appearance
RH, and temperature. Increasing the polarity, hydrogen
bond forces, and crystallinity decreases the free volume of Transparent packaging induces the oxidation and degra-
the film, enhances the cohesion, and reduces the flexibility, dation of nutritional compounds, because light acts as a
thereby increasing the barrier properties of the polymer catalyst for these processes. Therefore, opaque packaging
[74]. However, the differences in the oxygen barrier and packaging containing specific compounds that absorbs
properties depend mainly on the chemical composition, light in the UV–Vis spectrum have been developed to
molecular structure of the polymers [82], as well as water prevent these reactions. The light barrier property is related
content, which reduce the interactions of hydrogen bonds to the color and opacity of the edible films. For fruits and
between the hydroxyl groups of the polymer chains. The vegetables, gloss is an expected sensorial characteristic of
effects of antioxidants on the oxygen permeability of edible edible coatings. Therefore, the relation between the opacity
films have been reviewed by Bonilla et al. [17]. and gloss factors must be evaluated in vivo on the product
In general, most biopolymers possess good properties as to obtain an equilibrium between the sensory and nutri-
semi-permeable barriers to gases, but they are weak bar- tional qualities of the food.
riers to water vapor. The transfer of water vapor is gener- Liposoluble vitamins such as vitamin E increase the
ally due to the hydrophilic portion of the film and depends transparency of films during storage, allowing the normal
on the ratio of hydrophilic to hydrophobic compounds in passage of light, which catalyzes the rancidity of fats.
the film [50]. To prevent or diminish the dehydration of However, film gloss is not affected by the incorporation of
foods, films used as packaging or coatings must control the vitamin E. In hydrocolloid matrices of fish gelatin, vitamin
transfer of humidity from the product to the environment; E interacts with proteins through bridging hydrogen links,
hence, the WVP of these films must be as low as possible causing an increase in the absorption of UV–visible light
[73]. [60].
The films providing a semi-permeable barrier to oxygen/ Plant extracts are commonly used to provide color and
carbon dioxide could prevent the leaching of vitamins opacity to polymers [53], and as a result, films containing
during food washing [103]. However, hydrophilic com- plant extracts are less transparent than films without plant
pounds could increase the WVP of films and water loss extracts [44, 118]. Thus, the incorporation of plant extracts
from food products [72, 98]. The hydrophobic molecules of in films provides an adequate barrier to light, which is also
a-tocopherol (vitamin E) can reduce the WVP of bio- important for preventing the degradation of ascorbic acid
polymeric films, as has been proven with calcium caseinate and, consequently, browning. These results confirm the
[80] and fish skin gelatin [60]. In the last case, incorpo- beneficial effects of adding antioxidant to the applied
rating vitamin E into a fish skin gelatin film initially packaging. For instance, films of fish skin and bovine
reduces the WVP by 38 %, achieving a further reduction of gelatin enriched with polyphenol-rich aqueous extracts
approximately 11–16 % in 6 weeks. This reduction in the from rosemary and origanum display improved light bar-
film’s WVP could be caused by an increase in the rier properties and antioxidant activity, irrespective of the

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type of gelatin employed [41]. Tuna gelatin films enriched recently, the antifungal effect on grapes of origanum
with PEML display similar effects [44]. The light absorp- essential oil in chitosan coating was published [28].
tion in the limit of the visible spectrum at a wavelength of The process of browning results from both the enzy-
400 nm was 6 times higher for the film containing the matic and non-enzymatic oxidation of phenolic com-
murta extract than that without the extract, while in the UV pounds. Enzymatic browning consists of the oxidation of
spectrum, this difference was even more pronounced. phenolic substrates to colored ortho-quinones, depending
on the type of polyphenol that acts as a substrate [7]. To
prevent browning by the chemical reduction of quinones to
Edible Films and Coatings with Incorporation colorless ortho-diphenol reduction agents, antioxidants and
of Natural Additives: Applications enzymatic inhibitors can be used effectively [78]. Phenolic
acids, such as gallic acid, exhibit antioxidant and antibr-
The main techniques to apply coatings on foods are owning activity that has been attributed to their capacity to
spraying and dipping. Edible films and coatings based on reduce ortho-quinones (colored) to the corresponding col-
polysaccharides (such as chitosan, starch, carrageenan, orless phenolic compounds [66]. Thus, it may be reason-
pectin, and gellan) and proteins (such as whey protein able to assume that flavonoids with one or more OH groups
concentrate and fish skin, pigskin, and bovine skin gelatin) in their structure will display similar antibrowning activity.
reduce the spoilage of some fresh foods, but a potential Studies have demonstrated that flavonoids such as quer-
storage improvement has been observed when antioxidant, cetin, rutin, and morin have significant antioxidant activity
antimicrobial, and/or antibrowning compounds are intro- [18, 22]. Because antioxidants control the diffusion of
duced into these biopolymers. oxygen through membranes or films by diminishing their
The selection of natural additives and their application permeability [11, 92], these antioxidant flavonoids, when
depends on their bioactive properties (antioxidant, antimi- incorporated in edible films or coatings, might act as an-
crobial, and/or antibrowning), availability, cost effective- tibrowning compounds by delaying the contact of oxygen
ness, and effect on the sensory attributes of the final with the enzyme polyphenoloxidase (PPO). Onion extract,
product, as well as on consumer awareness [88]. which possesses bioactive compounds such as flavonol
Antioxidants are necessary to prevent the oxidative quercetin and quercetin derivates, can be used as an addi-
losses of lipids, essential oils, liposoluble vitamins (vitamin tive to prevent browning [64, 99]. In addition, some
A, D, E, and K) and pigments [112]. Polyphenols are the flavonoids have also been found to protect ascorbic acid
major plant compounds with antioxidant activity. Chiefly, from degradation [101].
among these compounds are flavonoids, which have potent Another possibility to prevent browning in fresh prod-
antioxidant activities and positive effects on human health ucts is to use packaging, films, or coatings that prevent the
[89]. Natural antioxidants found in plants have been stud- oxygen diffusion produced by mechanical damage during
ied as alternatives or complements to synthetic antioxidants transport, storage, and distribution. Browning is inhibited
[15, 52, 67, 123]. Plant extracts, such as basil, laurel, in atmosphere containing less than 1 kPa of oxygen [46],
rosemary, and tea leaf extracts, slow down the oxidation of so that the incorporation of plant extracts on films or
several oils more effectively than synthetic antioxidants, coatings is expected to enhance the oxygen and light bar-
such as BHA and BHT [52, 115]. The antioxidant activity rier, preventing oxygen from coming in contact with PPO
of rosemary extract is associated with the presence of and maintaining the stability of ascorbic acid in the food.
several phenolic diterpenes, which break free radical chain Spice oleoresins are natural plant extracts that constitute
reactions by hydrogen donation. Carnosic acid and ros- the essence of spices in their most concentrated form and
marinic acid are the main bioactive compounds present in contain volatile as well as non-volatile components (such
rosemary extracts, but whole rosemary extract is more as carotenoids, steroids, alkaloids, anthocyanins, and gly-
active than rosmarinic acid [36]. cosides). Food-grade oleoresins are obtained by alcohol
The bioactive compounds and plant extracts can have steam distillation from fresh vegetables. Ponce et al. [93]
also antimicrobial activity [6]. In the last 10 years, natural studied chitosan coatings containing different natural ole-
antimicrobials from spices, herbs, and oils for food systems oresins. Films applied to butternut squash slices (Cucurbita
(fresh and fresh-cut fruits, vegetables, meat, poultry, fish, moschata) displayed an antioxidant effect that inhibited
rice, and dairy products) that can be potentially incorpo- POD activity when the films contained oleoresins of
rated into edible films and coatings have been reviewed rosemary, olive, or blueberry, in decreasing order, while
[97, 109]. In relation to essential oils, the physical prop- PPO activity was significantly reduced when the chitosan
erties and applications of edible films containing plant coating contained olive, garlic, and pepper oleoresins. The
essential oils in food systems, to control pathogens and chitosan coatings containing rosemary and olive oleoresins
spoilage bacteria, have also been reviewed [29]. More improved the antioxidant properties of fresh-cut butternut

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squash, delaying the browning reactions that generally effect on the inhibition of lipids oxidation [60]. In addition,
result in fruits and vegetables quality loss. These chitosan chitosan, alone or constituted as film, exerts an antibr-
films containing oleoresins also significantly inhibit PPO owning effect and can be beneficial in reducing browning
enzymatic activity in lettuces, although the independent on fruits [58, 59]. The application of chitosan coating
application of chitin and rosemary is more efficient. (1–2 % w/v) in litchi (Litchi chinensis Sonn cv. Huaizhi)
Table 4 shows the effects of vitamins added to edible partially delays their decay and changes produced by
films on the functional and bioactive properties of films and browning [122], results also found in chitosan coatings on
their application on foods. Ascorbic acid can be used into strawberries [116]. This is reflected in the preservation of
films as browning inhibitors. Vitamin and/or acidulant the anthocyanin contents, flavonoids, and total phenolic
concentrations in an edible film should not be higher than compounds, as well as the decrease in PPO activity and
0.5 g/3 g biopolymer because higher concentrations of weight loss of the food. However, an increase in the
these molecules increase the WVP [11]. Therefore, the chitosan concentration in the coating did not significantly
antibrowning effects of edible films and coatings contain- increase the beneficial effects of the chitosan on spoilage
ing ascorbic acid depend on the biopolymer type and the and browning of the fruit. In addition, chitosan coatings
vitamin concentration added. Ouattara et al. [86] studied (2 % w/v) help to preserve the concentration of ascorbic
the shelf life of ground meat after the addition of 5 % (w/ acid in tissues, which inhibits enzymatic browning [59, 87].
w) ascorbic acid and a protein-based edible coating con- The effects of aqueous plant extracts and plant-based
taining a mix of 3 % (w/w) of natural spices (thyme, products on the functional and bioactive properties of films,
rosemary, and sage). They found that the combination of as well as their potential applications on food, are pre-
ascorbic acid and edible films with natural spices signifi- sented in Table 5. Plant extracts are complex systems that
cantly inhibited the lipid oxidation of ground meat during contain bioactive compounds at different concentrations.
storage, when compared to samples containing ascorbic The primary purpose of adding natural extracts containing
acid or control samples without natural additives. In antioxidants to a film or coating is to delay the onset of
addition, under refrigeration in the dark, films containing oxidation and the accumulation of oxidative products
ascorbic acid have been shown to retain their ascorbic acid [115]. The addition of plant extracts provide certain
concentration [26], whereas vitamins such as a-tocopherol, physicochemical modifications and bioactivity to biopoly-
included in fish skin gelatin films, did not have a significant mer materials such as chitosan [28, 70, 104, 108, 119] and

Table 4 Functionality and bioactive properties of films containing vitamins: applications

Natural additive Biopolymer base Effect of vitamin on Active film application References
film

Ascorbic acid Methylcellulose Increases O2 barrier Mushrooms and cauliflower: controls Ayranci and Tunc [10],
and citric acid and reduces PPO browning and reduces vitamin C loss Ayranci and Tunc [11]
activity
Ascorbic acid WPC Fresh-cut potatoes and apples: controls Perez-Gago et al. [90]
(1 % w/w) browning. Coating application did not
reduce weight loss in fresh-cut apples,
most likely due to the high relative
humidity of the product
Ascorbic acid CMC Apple and potato: controls browning Baldwin et al. [13]
a-Tocopherol Fish skin gelatin Increases TS, Bacon: lipidic oxidation control Jongjareonrak et al. [60]
(0.02 % w/w) transparency and
WVP. Reduces EB
a-Tocopherol Chitosan Strawberries and raspberries: reduces Han et al. [49]
weight loss, increases nutritional value,
and prolongs shelf life
a-Tocopherol Xanthan gum Baby carrot: improves desirable surface Mei et al. [81]
(0.2 % w/w) color without affecting taste, texture,
and 5 % fresh aroma and flavor, except for a
calcium slightly slippery surface. The b-carotene
level is not affected by the edible
coating
Shown in parentheses: vitamin concentration
AOX Antioxidant, TS tensile strength (MPa), EB elongation at break (%), WVP water vapor permeability, CMC sodium carboxymethylcellulose,
WPC whey protein concentrate

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Food Eng Rev (2013) 5:200–216 209

Table 5 Incorporation of plant extracts into edible films

Plant extract Biopolymer base Effects of natural additive on film properties/ References
Potential applications

Kiam wooda HPMC Increases WVP and film solubility. Decreases TS Chana-Thaworn et al. [21]
and EB. Darkens film color and decreases
transparency/Antimicrobial film to extend the
shelf life of foods
Betacyanin HPMC Enhances barrier to oxygen and WVP Akhtar et al. [4]
Oregano and rosemarya Fish skin and Bovine Increases AOX activity and UV light barrier/ Gómez-Estaca et al. [41]
gelatin Inhibiting oxidative rancidity
Murta leaves SC and SG Fish skin gelatin SC: Increases AOX activity and UV light barrier. Gómez-Guillén et al. [44]
(283.2 and 224.2 lg eq. Increases cohesiveness and reduces TS, EB, and
gallic acid/mL, WVP. SG: Increases AOX activity and UV light
respectively)a barrier/inhibiting oxidative rancidity
Green teaa Agar and Agar–fish Increases film water solubility and decreases TS Giménez et al. [40]
gelatin and EB in both films
Ginsengb Alginate Retarding lipid oxidation induced by UV light in Norajit, Kim and Ryu [85]
food systems
Borageb (1,542 g eq. Sole skin gelatin/and Increases AOX activity, irrespective of the type of Gómez-Estaca et al. [42]
caffeic acid/mL) commercial fish gelatin employed, to a level higher than films
gelatin with tocopherol and BHT. Minor changes in
physicochemical properties
Murta leaves SGa CMC Decreases WVP, forms a selective barrier to gases Bifani et al. [16]
(CO2/O2)/increasing the shelf life of fresh
products with a high respiratory metabolism
Murta leaves SCa CMC Increases O2 barrier Bifani et al. [16]
Green teaa Chitosan Increases AOX activity and polyphenolic content. Siripatrawan and Harte [105]
Increases mechanical properties and reduces the
WVP/active packaging for food products
Tea polyphenolsa Chitosan Increases AOX activity and water solubility. Wang et al. [119]
Decreases the WVP and increases the opacity
and color of chitosan films
Grape seeda Chitosan Strong scavenging activity Moradi et al. [83]
a
Acacia seed Galactomannan Increases radical-scavenging activity and the Cerqueira et al. [23]
phenolic content of the film
Effects on film functionality and bioactive properties. Perspectives
Shown in parentheses: total phenolic content (TPC). AOX antioxidant, TS tensile strength (MPa), EB elongation at break (%), WVP water vapor
permeability, CMC sodium carboxymethylcellulose, HPMC hydroxypropyl methylcellulose
a
Aqueous extract
b
Ethanol: water extract

thus could expand their overall applications. However, the films may decrease, as observed for a chitosan-based film
choice of the bioactive agent could be restricted by the containing a tea polyphenol extract whose antioxidant
incompatibility of the agent with the packaging material or activity was reduced by 33–43 % after 3–4 weeks [118].
by its heat instability during processing [91]. Therefore, the This behavior is most likely due to the loss of total phenolic
light barrier properties that these extracts of murta, rose- compounds in the film, because of oxidation. Therefore,
mary, and origanum leaves confer to the edible films kinetic studies of active compound delivery from films and
contribute to reducing the rancidity of lipids (Table 6) and of the film’s antioxidant activity should be performed
preserving the nutritional value of foods, particularly under the conditions of application and food storage.
ascorbic acid, which helps to inhibit browning. Chitosan offers real potential for applications in the food
Film antioxidant activity increases when flavonoids are industry as a preservative coating due to its specific
added to the films. The increase in the antioxidant activity physicochemical properties (such as good oxygen and
of the film depends on the compound type used (e.g., fla- carbon dioxide barrier and mechanical properties), rapid
vonoid type) and their concentration [108]. However, the biodegradability, biocompatibility with human tissues,
antioxidant activity (free radical-scavenging activity) of antimicrobial and antifungal activities, and non-toxicity.

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Table 6 Natural plant extracts as additives in edible films and their application on foods
Natural additive Biopolymer Effects of plant extracts on film characteristics/Food: protective References
effects of active natural films on food

Borage seedb Fish gelatin Horse mackerel (Trachurus trachurus) patties: protective effects Giménez et al. [39]
on lipid oxidation throughout frozen storage
Oregano and Rosemarya Pigskin Antioxidant activity/Sardines: controls lipid oxidation Gómez-Estaca et al.
[43]
Murta leavesa CMC Increases oxygen barrier/Apricot: reduces weight loss Ihl et al. [54]
Rosemarya CMC Antioxidant activity/Roasted peanuts: increases oxidative Wambura et al. [115]
stability compared to coating containing tea leaf extract and
vitamin E
Green teaa Chitosan 95 % DS Enhances the antimicrobial and antioxidant properties of the film/ Siripatrawan and
Pork sausages: inhibits lipid oxidation and microbial growth, Noipha [106]
extends shelf life
Rosemary Chitosan 88 % DS Antioxidant activity/Beef Burgers: retains red color, best Georgantelis et al. [38]
antioxidant effects
Rosemary Chitosan 85 % DS Antioxidant activity/Fish (Pseudosciaena crocea): reduces lipid Li et al. [70]
oxidation and microbial spoilage, improves sensorial properties
compared with control sample
Tea polyphenols Chitosan 85 % DS Fish (Pseudosciaena crocea): reduces microbial spoilage, Li et al. [70]
improves sensorial properties compared with control sample
Tea polyphenols Chitosan 95 % DS Mango (Mangifera indica L.): enhances their sensory quality, Wang et al. [117]
reduces weight loss and respiration rate and inhibits chlorophyll
degradation in fruit peels
Olive, garlic and pepperc Chitosan Butternut squash (Cucurbita moschata Duch): controls PPO Ponce et al. [93]
activity
Rosemary and olivec Chitosan Butternut squash (Cucurbita moschata Duch): improves Ponce et al. [93]
antioxidant protection, prevents browning reactions, reduces
quality loss and does not introduce deleterious effects on the
sensorial acceptability of squash
Rosemaryc Chitosan Romaine lettuce: controls PPO activity Ponce et al. [93]
DS Degree of deacetylation, AOX antioxidant, TS tensile strength (MPa), EB elongation at break (%)
a
Aqueous extract
b
Ethanol: water 50:50 (v:v)
c
Oleoresins

The applications for active bio-based chitosan film pro- Green tea-derived polyphenols have been reported to
duction and its potential in the food industry have been exhibit strong antioxidant properties in numerous studies.
reviewed by Aider [1]. In contrast to plant extracts, the They can act as antioxidant by donating a hydrogen atom,
antioxidant activity of chitosan is not a result of its accepting free radicals, and interrupting chain oxidation
reduction power but rather its capacity to prevent the for- reactions or by chelating metals. Green tea extract has been
mation of reactive oxygen species (ROS) through the added to films based on chitosan [105, 106] and agar–
chelation of metals [61] and direct capture of ROS [120]. gelatin [40]. Chitosan–gelatin composite coatings, in con-
The strong scavenging activity observed on chitosan trast to gelatin coatings containing rosemary or origanum
films containing an aqueous extract of tea polyphenols extracts, do not inhibit oxidative rancidity but instead
[118], grape seed [83], and rosemary [38] might be due to reduce the growth of microorganisms in sardines [43].
an increase in intermolecular interactions, primarily weak The inclusion of origanum and rosemary extracts in
interactions such as hydrogen bonding between phenolic pigskin gelatin-based edible films [43] yields antioxidant
compounds and chitosan [105]. Films containing tea and activities similar to those of the original film, in spite of the
rosemary aqueous extracts display greater antioxidant difference in the polyphenol content. This result indicates
effects on the lipidic food storage stability of foods, such as that the antioxidant activity of the film depends on the type
peanuts, beef, and fish, than that displayed by synthetic a- and concentration of the polyphenolic compounds present
tocopherol [70, 115], and films containing a borage extract in the extracts. These active films increase the shelf life of
display higher antioxidant activities than films containing sardines (Sardina pilchardus) by slowing lipid oxidation.
a-tocopherol and BHT [42]. Furthermore, when combining these coatings with high

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Food Eng Rev (2013) 5:200–216 211

pressures, microbial spoilage is delayed due to the libera- proportion of quercetin than of myricetin [16]. This is
tion of bioactive compounds from the film to the food. relevant because myricetin (3 OH groups on the B ring)
contains one more OH group than does quercetin (2 OH
groups on the B ring), which allows PEML SC, with a high
Effect of Murta Leaf Extract on the Structure myricetin concentration, to react with more other
and Properties of Active Films: A Case Study compounds.
The extracts, PEML SC and PEML SG, affected the
Murtilla or murta (Ugni molinae Turcz) is an endemic structure of gelatin films in different ways. In comparison
shrub in central-southern Chile that belongs to the Myrta- with the gelatin film–PEML SG and with the film without
ceae family. Polyphenol-rich aqueous extracts from murta extract, the gelatin film–PEML SC presented a compact
leaves (PEML) display high antioxidant activity in vitro structure, which denotes a greater cohesiveness between
[100] and antimicrobial activity against foodborne micro- the polymeric chains and compatibility between the bio-
organisms [102]. Phenolic acids such as gallic acid, as well polymer and the polyphenolic compounds of the PEML
as flavonoid aglycones and glycosides from quercetin and SC.
myricetin, are among the main compounds found in those Both extracts affect the WVP of a CMC-based film,
extracts [16, 100], being the proportion of phenolic acids although in different ways [16]. The WVP decreased sig-
higher than that of flavonoids in the PEML, being the nificantly upon the incorporation of PEML SG but not
proportion of phenolic acid in the PEML is higher than that PEML SC in the film (P [ 0.05). These results could be
of flavonoids. related to the structural modification of the CMC network
The increase in the total phenolic compounds and rad- produced by the polyphenolic extract because the WVP of
ical-scavenging activity is generally proportional to the the film increases with the number of available polar (–OH)
amount of extract added to the edible films [23]. However, groups on the polymer [24]. This could explain the lower
a high concentration of phenolic compounds can change WVP of the films containing PEML SG. In the case of fish
the film structure and consequently modify its functionality gelatin film, PEML SC does not have any effect on the
by affecting its barrier, mechanical and thermal properties. WVP, while PEML SG slightly reduces the WVP, although
The effect of the PEML of two leaf ecotypes, SC and SG, not significantly [44]. The stability of the properties of the
on the barrier and mechanical properties of films based on WVP in both biopolymers can be explained by means of
fish skin gelatin [44] (Fig. 2) and carboxymethylcellulose the higher cohesion of the polymeric chains that can be
(CMC) [16] has been studied. The compositions of PEML obtained, quantitatively and qualitatively, via the active
SC and PEML SG are quantitatively and qualitatively compounds of PEML SC.
different. A higher antioxidant activity and concentration Regarding to gas barrier properties, the PEML SC and
of total phenolic compounds are present in PEML SC PEML SG increase the oxygen barrier properties of CMC-
(283.2 lg equivalent gallic acid/mL extract) compared to based films, while the PEML SG reduces the film’s CO2
PEML SG (224.2 lg equivalent gallic acid/mL extract) barrier properties [16]. This indicates that a CMC-based
[44]. The PEML SC also shows a larger amount of my- film with PEML SG possesses a selective permeability to
ricetin than of quercetin, while PEML SG contains a higher CO2 and O2, and thus, films containing PEML SG permit

Fig. 2 Edible films based on fish skin gelatin with added polyphenol- SG: 224.2 lg equivalent gallic acid/mL extract). F-SG: Film with
rich extract from murta leaves (PEML). Extracts from the two murta PEML SG, F-SC: Film with PEML SC, F-C: the control film without
leaf ecotypes (SC and SG), which contain different concentrations of extract
total phenolic compounds, were studied (PEML SC: 283.2 and PEML

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the release of a higher amount of CO2 than entering oxy- Plant extracts are complex systems. Therefore, to eval-
gen. This suggests that films with PEML SG could be used uate their contribution to the bioactive and functional
as coatings for fruits with high respiration rate, to achieve a properties of edible films, the main bioactive compounds
delay in ripening. from the plant extracts should be identified, and the prop-
The PEML also has been added to chitosan and chito- erties of the films containing the plant extract should be
san–starch composite films [104]. Pure chitosan films are evaluated in two ways: (1) incorporating the main bioactive
generally cohesive and compact, with a smooth surface compounds separately and in different concentrations and
without pores or cracks. In the cross-sections of chitosan (2) incorporating a plant extract concentration equivalent to
films, chains are arranged in a horizontally ordered form at the concentration of the bioactive compounds present in the
pH \ 5.0. However, upon the incorporation of the PEML, extract. Such an evaluation establishes whether the changes
several elongated horizontal pores of approximately in the functional properties and bioactivity of the edible
1–4 lm are observed. This indicates that an increase in the films are due to the chemical structure, the active com-
diffusion of gases such as oxygen and carbon dioxide could pound concentration in the extracts and/or a synergic effect
occur, as the diameter of oxygen is 1.2 9 10-4 lm while of the plant extract compounds.
that of carbon dioxide is 3.6 9 10-4 lm. The incorporation of natural extracts from plants, spices,
The polyphenolic nature of the PEML extract with and herbs and the incorporation of vitamins C and E, alone
chitosan renders an extremely high reactive agent. Thus, or combined, represents a promising approach for the
PEML induced great discontinuity in chitosan–PEML film development of bioactive edible films/coatings with new
matrix due to excessive chitosan crosslinking. The perfor- and improved bioactive, mechanical and physicochemical
mance of chitosan–PEML can be improved when starch is properties and applications.
added. In studies about starch–chitosan film blend [104], When incorporated in biopolymer matrices, several nat-
starch stabilizes the interaction between chitosan and PEML, ural plant additives provide antioxidant activity, barriers to
and then chitosan–starch–PEML renders a more continuous UV–visible light, and beneficial properties for the reduction
and homogeneous film structure than only chitosan–PEML. of lipid oxidation and the browning of foods. However,
in vivo studies of their capacity to preserve the quality, shelf
life, and nutritional value of foods remain limited. Further-
Final Remarks more, there are a wide range of plant natural sources with
bioactive properties that remains to be investigated, regu-
Food safety and quality can be influenced by the chemical lated for application directly on foods, and used for the
interactions between biopolymer packaging materials and development of active packaging or biopolymer-based edi-
foods. There is evidence that natural additives such as poly- ble films for preserving and adding value to foods.
phenol-rich extracts from plants, can change the structure and
morphology of edible films and coatings and that there is a close
relationship between the incorporation of plant extracts and References
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