1 s2.0 S2215038221002004 Main 5

Colloid and Interface Science Communications 46 (2022) 100560
Contents lists available at ScienceDirect
Colloid and Interface Science Communications

journal homepage: www.elsevier.com/locate/colcom
Strategies applied to modify structured and smooth surfaces: A step closer

to reduce bacterial adhesion and biofilm formation
A. Uneputty a, 1, A. Dávila-Lezama a, b, 1, D. Garibo c, d, A. Oknianska e, N. Bogdanchikova d, J.
F. Hernández-Sánchez f, A. Susarrey-Arce a, *
a
Mesoscale Chemical Systems, MESA+ Institute, University of Twente, Drienerlolaan 5, 7522 NB Enschede, the Netherlands
b
Facultad de Ciencias de la Salud, Universidad Autónoma de Baja California, Blvd. Universitario número 1000, Valle de las Palmas, 22260 Tijuana, México
c
Cátedras Conacyt, Universidad Nacional Autónoma de México, Centro de Nanociencias y Nanotecnología, Km 107 Carretera Tijuana-Ensenada, Ensenada, BC, Mexico
d
Universidad Nacional Autónoma de México, Centro de Nanociencias y Nanotecnología, Km 107 Carretera Tijuana-Ensenada, Ensenada, BC, Mexico
e
School of Pharmacy and Biomedical Sciences, University of Central Lancashire, Preston, UK
f
Instituto de Ciencias Aplicadas y Tecnología, Universidad Nacional Autónoma de México, Circuito Exterior S/N, Ciudad Universitaria, 04510 Mexico City, Mexico
A R T I C L E I N F O A B S T R A C T
Keywords: Nearly a century has passed since the discovery of the first antibiotics. With each passing decade, more bacterial
Antibacterial surfaces strains developed resistance towards existing antibiotics. Alternative methods to reduce contamination by bac
Biofilm teria and biofilms have arisen to reduce the pressure on existing or currently developed antibiotics. This review
Coatings
highlights promising approaches to prevent bacterial contamination of the surface. Special attention is paid to
Topographies
antibiotic-free antibacterial strategies that are not affected by bacterial resistance. The approaches have been
divided into four categories: (i) anti-adhesive, (ii) contact active, and (iii) biocide attached/biocide release,
which can be integrated with (iv) topographical modification. Anti-adhesive approaches can reduce the adhesion
between bacteria and a solid surface to prevent bacteria from contacting and contaminating the surface. Contact
active approaches provide antibacterial activity by attachment of antibacterial agents to the substratum. Biocide
attached/biocide release integrates contact-release of toxic chemicals to bacteria attached to the surface. Lastly,
topographical modification relies on approaches to produce small structural features capable of matching cellular
components killing bacteria. Combining one or more antibacterial strategies can lead to a more robust approach
to deal with dangerous pathogenic bacterial species. In this case, a way forward is by combining various coatings
onto topographically modified surfaces, enabling multifunctionality to reduce adhesion and biofilm formation. A
perspective on the current antibacterial surface challenge is provided.
1. Introduction methods, bacterial contamination can be reduced by developing single

or multi-level functionalization steps over surfaces to achieve excep
Since the discovery of penicillin by Alexander Fleming in 1928, tional antiseptic potential [5], preferably at the early stages of bacterial
humankind has been using antibiotics to treat infections [1]. Nearly a adhesion before the biofilm is formed [6].
century has passed, and first-line antibiotics cannot cope with the In view of the variety of single or multi-level functionalization
adaptation mechanisms of bacteria, which ultimately develop antibiotic strategies, in the current paper, we categorize antibacterial surfaces as
resistance [2]. The world needs to change the way of prescribing and anti-adhesive, contact active, and biocide attached/biocide release.
overusing antibiotics [3]. Even if the new generation of antibiotics Anti-adhesive surfaces can reduce the adhesion between bacteria and a
prevails, still providing antibacterial protection, antibiotic resistance solid surface to remove bacteria before bacterial adherence and prolif
will remain a significant human threat [3]. An urgent quest for alter eration. Anti-adhesive surface strategies in this report include ap
native methods to reduce surface contamination by bacteria species has proaches using passive polymers, hydrogels, and poly-zwitterionic
arisen to minimize antibiotic dependency [4]. In these alternative polymers. The active contact approach displays antibacterial activity by
* Corresponding author.
E-mail address: a.susarreyarce@utwente.nl (A. Susarrey-Arce).
1
Equal contribution.
https://doi.org/10.1016/j.colcom.2021.100560
Received 23 August 2021; Received in revised form 18 November 2021; Accepted 19 November 2021
Available online 6 December 2021
2215-0382/© 2021 The Author(s). Published by Elsevier B.V. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/).
A. Uneputty et al. Colloid and Interface Science Communications 46 (2022) 100560
attachment of antibacterial agents to the substratum’s surface. Contact interaction and attachment. The attachment of planktonic cells to the
active surface strategies include approaches on active action polymers, surface is not permanent. Cell locomotion with the use of flagella or pili
quaternary ammonium compounds, surface-attached antimicrobial is granting preferential selection for surface attachment. In Stage 2,
peptides, and quorum sense inhibitors. Unlike the active contact biofilm formation, irreversible attachment, and cell wall deformation
approach, the biocide attached/biocide release approach integrates a over the substratum surface are typically observed. This process is
toxic bacteriostatic or bactericidal substance. It can, therefore, be mediated by the expression of quorum-sensing signaling molecules and
considered toxic by design. Attached/Released chemical or biological by the formation of extracellular polymeric material. Stage 3 involves
components, which are known to be prone to bacterial resistance, are the formation of a mature biofilm with a 3D structure containing cells
not considered. The main focus of the presented paper is to provide a packed in clusters with channels between the clusters that allow trans
general overview of existing antibacterial strategies (e.g., coatings) port of water and nutrients and waste removal. Unpredictable properties
applied to topographies. These functionalization approaches linked to like resistance to external chemicals are an adaptative biological process
topographical designs might be the stepping stone to reduce bacterial of bacteria and are probably supported by the 3D network. Once the 3D-
contamination, proliferation, and dangerous human infections [7–9]. In structured biofilm network is created, stage 4 takes place. Here,
this respect, such functional topographies should reduce bacteria cell detachment and dispersion of cells from the biofilm and initiation of new
viability or cause cell death without promoting bacterial resistance. biofilm formation occurs. Dispersed cells are morphologically more
Despite the antibacterial mechanism imposed by topography, dead similar to planktonic cells than mature biofilm cells, which can initiate
bacteria can always build up on the surface, inactivating bacterial killing the biofilm development process again [19]. In other words, the
properties of the surface [10]. Therefore, multipotent platforms to spreading of infectious bacterial cells might commence.
reduce cell adhesion and biofilm formation have yet to be found, In the following steps, we explore surface modification approaches
particularly for long-term applications. Promising strategies that employing anti-adhesive, contact active, and biocide attached/biocide
combine self-cleaning properties and bacteria-killing are an example of release strategies. Surface modification strategies (mainly chemical) are
multipotent antibacterial platforms [11–15]. With such platforms, both then connected to functionalization parameters that can be end-
bacterial killing and active bacterial detachment could be expected, compatible with topographical micro-/nano-structures fabricated
maintaining the surface bacteria-free without the need for antibiotics using physical modification approaches presented in Table 1. In some
and other hazardous chemicals to be released to the environment. cases, such topographies possess inherent antibacterial properties as
Similar multipotent platforms that combine single or multi-level func well. In both cases, chemical and physical approaches are shown in
tionalization strategies are assessed. Strategies applied over topogra Fig. 2, where the common goal is to reduce bacterial attachment or
phies, particularly for long-term applications in the health care setting, prevent biofilm formation. The implemented level of functional strate
are the main focus. Finally, a perspective on the current long-term gies is described below.
antibacterial surface challenge is provided.
2.1. Surface modification strategies
2. Biofilm formation
Biofilm formation is the survival strategy of microorganisms wherein
The long-term application of antibacterial surfaces is threatened by microbial cells adapt to their environment and to a multicellular lifestyle
irreversible bacterial attachment, leading to biofilms. Biofilms have in which bacterial cells are self-immobilized in a matrix of extracellular
been identified as a possible source of infection. Verderosa et al. defined polymeric substance (EPS) [19,20]. The bacteria inside this matrix are
biofilms as complex three-dimensional communities of microorganisms shielded against antibacterial compounds and are up to 1000 times less
adhering to a surface and encased in a protective extracellular polymeric susceptible to antibiotics [21]. Thus, the prevention of the early stages of
substance (EPS). EPS is composed of protein (<1-2%), DNA (<1%), biofilm should be the primary focus (i.e., stages 1 & 2 during biofilm
polysaccharides (1-2%), RNA (<1%), and water (up to 97%), being the formation, shown in Fig. 1).
main source for flow of nutrients inside a biofilm matrix [16]. Arunasri A key issue identified for the recently developed chemical strategies
et al. mentioned the development from planktonic bacterial cells into is that, as time goes by, the substratum's degradation occurs as a result of
sessile aggregates known as biofilm [11]. The proposed biofilm growth chemical agent depletion or loss of structural surface integrity. Conse
mechanism is divided into four biofilm formation stages, as shown in quently, an opportunity for bacteria to adhere to and proliferate is
Fig. 1 [17,18]. created. Biofilm formation can occur on virtually any surface. Most of
In stage 1, the reversible attachment of bacterial cells to a surface the strategies shown in Table 1 render to surface contamination. In the
occurs. During this stage, the free-floating planktonic cells identify a ideal case, most of the surfaces should last long. Nevertheless, very few
surface, where once landed, they can initiate the process of surface of them have been identified to retain their antibacterial properties over
extended periods [22].
As shown in Fig. 2, an overview of the division of antibacterial
strategies is given. Here, a division is made between physical and
chemical strategies. Chemical strategies, such as anti-adhesive (AA),
contact active (CA), and biocide attach/release (BAR), include
treatment-induced on the surface, i.e., polymerization and surface
functionalization. The second group includes physical treatment
involving modification of the surface topography (TM), changing sur
face properties, and creating a superhydrophobic or hydrophobic
interface for self-cleaning or slippery interfaces. Each of the identified
antimicrobial strategies contains several subgroups listed in Table 1.
This table describes AA, CA, BAR, and TM approaches with a general
remark when integrated to topography, such as functionalization
compatibility.
The main themes identified can be formulated as follow:
Fig. 1. Process of biofilm formation: reversible attachment, (i) irreversible
attachment, (ii) 3D biofilm formation (iii), biofilm dispersion (iv) adapted from
Maunders et al. [17,18].
2
Table 1
Multifunctional chemical and physical strategies required to reduce bacterial attachment and biofilm formation.
Strategy Subcategory Approach Remark Compatibility with References
topographies
Chemical Anti-adhesive Passive polymers, Hydrogels, Poly- Mechanisms based on steric exclusion repulsion, Yes, as a coating. [23–26]
Strategies zwitterionic polymers. electrostatic repulsion, and low surface energy.
Contact active Quaternary ammonium compounds, Contact active agents induce bacterial cell death or reduce Yes, as a coating. [27–29]
Surface attached antimicrobial peptides, the metabolic activity of bacteria, minimizing their
Quorum sensing inhibition. pathogenic effect in their biological environment.
Biocide release Nanoparticle Metals; Release of an active agent inducing bacterial cell death or Yes, as a [30]
interferes with bacterial cellular interactions. composite.
Physical Topographic Superhydrophobic moieties, Hydrophobic Inhibition of biofilm formation through superhydrophobic Yes, but [31,32]
Strategies modification moieties. hydrophobic interaction. complicated
Fig. 2. Surface modification strategies for antibacterial application.
(i) AA: involves mainly passive action polymers, hydrogels, zwit when polymers attached to coating surfaces provide physical barriers to
terions motives, the action of which is based on steric exclusion proteins from the bacteria cell wall [23]. Another mechanism is elec
repulsion, electrostatic repulsion, and low-surface energy. trostatic repulsion, where repulsion occurs due to charges on coatings
(ii) CA: relates mainly quaternary ammonium cations, antimicrobial preventing the attachment of microbes [24]. Lastly, the mechanism of
proteins, and peptides, and quorum sensing inhibition, the action low surface energy where reduction of external microbial adhesion oc
of which is based on the covalent attachment of agents which can curs due to low energy surfaces [25,26]. With these three main mech
induce bacterial cell death or can reduce bacterial metabolic anisms in mind, strategies on anti-adhesive approaches like passive
activity. action polymers, hydrogels, poly-zwitterionic polymers are next intro
(iii) BAR: involves mainly nanoparticles, which is based on the duced. Each of the strategies relies on one or a combination of low en
loading and release of an activity that can kill bacteria or reduce ergy and repulsion mechanism.
its metabolic activity.
(iv) TM: addresses hydrophobic or superhydrophobic moieties based 3.1.1. Passive action polymers
on the inhibition of bacteria due to hydrophobic interaction. Today, various types and subclasses of bacterial adhesins are
described in the literature as active polymers [33]. Bacterial adhesion
3. Chemical strategies depends primarily on intramembranous structural proteins found on
hair-like appendages such as pili, fimbria, and nanofibers, which pro
With the use of chemistry, surfaces can be modified to provide a vide a scaffold upon which several extracellular adhesins may be
specific function. In this section, various methods and development attached [33,10]. In many cases, these adhesins are minor subunit
regarding the fabrication of antibacterial biocide-free surfaces are proteins at the tip of fimbria [33,34]. It is possible to reduce bacterial
described. Three of the four main strategies are approaches connected protein adsorption on its surface with passive polymers, thereby pre
with chemical modification techniques. venting bacterial adhesion. Passive polymers generally include self-
healing, slippery liquid-infused porous surface (SLIPS) [35,36], un
charged polymers [23], charged polyampholytes, and zwitterionic
3.1. Anti-adhesive principle polymers[37].
Among the passive polymers, Poly(ethylene glycol) (PEG) is the most
The principle of an anti-adhesive surface is an effective strategy to commonly used. The use of surface-immobilized PEG and its derivatives
reduce biofilm formation. Anti-adhesive surfaces can reduce the adhe for antifouling activity are assessed. Chirife et al. hypothesized the
sion force between the bacterium and the substratum, preventing bio antibacterial action of PEG-400, attributing to two effects, lowering the
film formation. The mechanism of repulsion of bacteria, as shown in water activity and the specific action of PEG-400 molecules on bacterial
Table 2, is based on exclusion steric repulsion, where repulsion occurs cells [38]. Afterward, Jeon et al. proposed that repulsive forces hinder
bacterial proteins, which can most probably be electrostatic forces [39],
Table 2 resulting from highly mobile PEG chain compression on functionalized
Physicochemical anti-adhesive mechanisms. surfaces. Furthermore, this theory proposes that the compression of
Mechanism Based on
polymer chains would need the thermodynamically unfavorable
removal of water molecules from the hydrated polymer. This would
Exclusion steric Repulsion by physical barriers to proteins, cells, and
result in a formation of a tightly bound water layer interacting with the
repulsion microbes.
Electrostatic repulsion Repulsion by electrostatic charges of molecules/coatings. grafted polymer, acting as a physical barrier to the adsorption of protein
Low surface energy Reduction of external microbial adhesion due to low- and bacteria [40]. Benčina et al. reported that a precise antibacterial
energy surfaces. repellence mechanism of surface-immobilized PEG is still not fully
3
elucidated. However, various studies report numerous properties of the inherently antimicrobial activity where the matrix itself displays anti
grafted polymer, including grafting density, chain length/thickness of bacterial activity [54]. The main advantage of using hydrogels is the
the polymer layer, conformation, and wettability which play an essential control of specific properties such as morphology by controlling the
role in resisting protein adhesion [25]. number of crosslinkers and monomers in the hydrogel network [56],
Ali-Ani et al. demonstrated a reduction of adhesion by tuning the thereby influencing the ability of dispersion of loaded agents and its
grafting density of PEG chains. In this study, (3-Aminopropyl) antibacterial activity. Wang et al. described that the active antifouling
triethoxysilane-grafted silicon wafers were used to attach PEG chains of mechanism strongly depends on the environment media due to the
different densities covalently. Here, a systematic method of grafting complicated interactions between the fouling agent (foulant), anti
density is demonstrated, linking the polymer density to the solution's fouling materials, and the solvent media. However, whether a surface
salt concentration (K2SO4), fabricating the highest possible density at will be antifouling toward the adsorption of a foulant is understood by
0,6M/60 ◦ C. These PEG-modified surfaces showed less bacterial adher standard thermodynamic considerations [36]. In this case, the free en
ence than Si and APTES surfaces concluding that this reduction is ergy of the adsorption process contains an enthalpic component
attributed to the hydrophilicity of covalently grafted PEG. The results describing the strength of interactions between the foulant, solvent, and
are in agreement with experiments where APTES is used to functionalize surface [36]. Hydrogels with inherently antibacterial properties include
Si or SiO2. The results demonstrate that regardless of the hydrophilic hydrogels made of chitosan, peptides, and polymers [57,58]. In this
character of the functionalized with APTES, bacteria still adherence and work, peptide-based hydrogels will not be discussed further.
proliferate [41]. In the case of eukaryotic cells, such as mesenchymal
stem cells [42] and MG63 human osteosarcoma cell attachment was 3.1.2.1. Chitosan-based hydrogels. Chitosan (CS) is a linear poly
increased at low and medium PEG-polymer densities [42]. Jiang Wu saccharide. CS is able to polymerase by cross-linkage in the presence of
et al. investigated the effect of molecular weight of PEG and mass ratios anions and polyanions [59]. A common method to make CS is by
of PEG: proteins on the interactions between PEG and proteins in deacetylation of Chitin (CT) [60]. CS-based hydrogels have shown
aqueous solution. In this work, Jiang Wu et al. concluded that long-chain properties such as self-healing, antibacterial activity, biocompatibility,
PEG could interact with proteins in an aqueous solution. PEG–protein and biodegradability [22,61,62]. Ravishankar et al. divided chitosan-
interactions induce conformational changes to relatively open structures based hydrogels into three generations: the first generation comprises
with increased hydrophobic cavities, provide multiple binding sites of chemically and metal coordinated cross-linked hydrogels. These cross-
proteins to PEG, and facilitate a PEG–protein complexes formation. The linked hydrogels result in fair-to-good mechanical properties. Howev
effect is often neglected for long-chain PEG. However, short-chain PEG er, the majority of the first generation is toxic. The second generation
behaved differently and indicated little tendency to protein interaction comprises physically cross-linked hydrogels utilizing physical forces,
due to its inability to form multiple binding sites [43]. Zhang concludes such as electrostatic interactions, H-bonding, and hydrophobic interac
that though the antifouling property of PEG displays better functionality tion. In contrast to the first generation, the second generation hydrogels
than most other hydrophilic polymers, the stability of PEG is impaired are non-toxic, demonstrating low-to-moderate mechanical properties.
due to oxidation of its intrinsic ether linkage. Lastly, the third generation comprises extensive physical cross-links
PEG has shown reliability in various applications in the medical field across the chitosan chains. These hydrogels demonstrate very high
owing to its antifouling properties, biocompatibility, and excellent stiffness and exceptional environmental stability, overcoming the
safety [44–46], and is used, e.g., for coating of implants [47]. Although drawbacks of the second generation. Common examples of third-
PEG is one of the most commonly used passive polymers, known for its generation hydrogels include polyanions having a large molecular
properties regarding PEG-protein interaction in aqueous solution, its weight and a net charge ratio. This generation can be shaped as nano
mechanism of action and antibacterial properties are not fully under particles end-having a negatively charged surface. However, it should be
stood and should be investigated more thoroughly. An interesting aspect noted that the third generation needs further research as the antibac
to explore is the dependence of PEG stability on chain length, particu terial mechanism of action is not fully elucidated [63].
larly when imparting antifouling functionality. Eventually, PEG can find CS can inhibit bacterial growth through positively charged amino
application in the health care setting used, e.g., indoor handles, linen, groups interacting with the negatively charged cell outer membrane
and clothing [48]. PEGylation (attachment of PEG to surfaces) has been [64]. The ability to attach CS hydrogels to surfaces might represent an
a “golden standard” to resist nonspecific protein adsorption [49]. exciting option to achieve antibacterial properties using surface func
However, it has been reported that the hydrophobic character tested in- tionalization approaches. For example, methods to covalent attach
vivo, particularly with highly immunogenic protein conjugated to PEG, hydrogels to a surface can vary. He et al. reported a bilayer hydrogel
can generate PEG-specific antibodies. The generation of these antibodies coating that can switch from a cell-adhesion mode of action to an
in term causes the complete elimination of subsequent doses of PEGy antibacterial mode of action. To create the coating, firstly, a CS hydrogel
lated agents [49–51]. Although recent studies have identified the thin film is covalently attached to a thiol-modified substrate via the
chemical origin of PEG, the exact biological mechanism of PEG immu thiol-one click reaction of an ene-functionalized copolymer of poly
nogenicity is not completely clear [51]. As a result, PEG might not be (sulfobetaine methacrylate-acrylate acid-2-hydroxyethyl methacrylate)
safe for all applications in health. PEG’s immunogenicity might limit the (P(SBMA-AA-HEMA)). After that, heparin-mimicking polymer chains
scope, and more research must be in place to overcome its limitations were grafted onto the hydrogel thin film layer via surface-initiated atom
[52]. transfer radical polymerization [65]. In a later study, He et al. demon
strated a robust method to covalently attach multifunctional hydrogel
3.1.2. Hydrogels thin layers onto substrates showing reliable stability. Thin hydrogel
Hydrogels are three-dimensional (3D) polymer networks cross- layers were formed and covalently immobilized onto substrate surfaces,
linked by physical or covalent bonds [53]. These gels are a class of as shown in Fig. 3, by two steps: double bonds introduced onto the
highly hydrated material finding use in a diverse medical application for substrate providing the surface with anchoring points for hydrogel
its general biocompatibility properties. As a result, hydrogels make a layers, and the formation and simultaneously attachment of hydrogel
convenient platform to develop selectively active antimicrobial mate layers onto the substrate surface by cross-linking copolymerization for
rials [54]. Hydrogels have, compared to other types of biomaterials, the double bonds and functional monomers. Here, hydroxyl groups on
distinct properties such as high water content, controllable swelling polyethersulfone (PES) substrates were prepared by cross-linking poly
behavior, and biocompatibility [55]. Salome Veiga et al. described two merization of HEMA followed by a phase inversion technique. Via the
types of antimicrobial hydrogels: hydrogels either encapsulating or co reaction of acryloyl chloride and the hydroxyl groups, double bonds
valent immobilizing antimicrobial agents or hydrogels with an
4
Fig. 4. Schematic procedure for the preparation of AgNPs hybrid supramo

lecular hydrogels [80].
linked by both pseudopolyrotaxane crystallization and AgNPs, which

showed temperature responsiveness properties. Due to hybridization,
Fig. 3. A thin hydrogel layer with anticoagulant, antifouling, and antibacterial the hydrogels showed excellent antibacterial properties against S. aureus
functions. The synthesis procedure of surface-attached hydrogel thin layers is and E. coli bacteria showing potential applications as injectable anti
highlighted [66]. bacterial materials [80]. Garcia-Astrain et al. developed a bio-
nanocomposite hydrogel based on gelatin and chondroitin sulfate with
were introduced, which provided anchor points for the hydrogel layers. covalently attached AgNPs. In this study, Garcia-Astrain reported using
Then, various precursor solutions were added to coat the double bond maleimide-coated AgNPs as cross-linkers to prepare a bio-
surface-covered PES substrates, respectively, and cross-linking copoly nanocomposite gelatin-based hydrogel via Diels− Alder cycloaddition
merization was executed at 365 nm to attach the hydrogels covalently. to furan-modified gelatin [81]. Despite their biocompatibility, toxicity
Calculations of the residual masses of the samples were made to evaluate was not entirely reduced. The results indicate that synthetic methods
the stability of the layers. The results indicated high stability as residual can change NPs toxicity and should be tunable to maintain antibacterial
masses remained unchanged after seven cycles of treatment. Interest activity and reduce cytotoxicity towards human cells [75]. The advan
ingly, He et al. noted that for metal and inorganic substrates, anchoring tages of incorporating NPs into hydrogel have great potential to increase
sites can be provided by dopamine chemical coating or treatment with material functionality in the clinical setting.
fresh piranha. Thereby showing the versatility of this technique [66]. In
a different research, Bidhari et al. covalently bond antifouling thin layer 3.1.3. Poly-zwitterionic polymers
hydrogels on 3-ethoxybenzophenonesilane-modified inorganic or bare Zwitterionic polymers refer to a family of materials with equal cat
organic substrates by irradiation under UV light. Due to irradiation, ions and anions along their polymer chains [82]. These polymers
photo-active benzophenone molecules enabled the generation of the contain positive- and negative charged groups incorporated into their
polymer network and the attachment of the network onto the substrates. structure, making them highly hydrophilic antifouling compounds [83].
In general, the covalent attachment of hydrogels to surfaces has been Classified by anions, the zwitterionic groups can be classified into sul
proven successful by various strategies. The ability to covalently attach fobetaine (SB), carboxy betaine (CB), phosphorylcholine (PC). Zheng
thin hydrogels may provide surfaces an antifouling or antibacterial et al. report that due to the favorable antifouling capacities provided by
functionality depending on the hydrogel used. Moreover, the addition of the chemical groups, zwitterionic materials could have applications in
thin layer hydrogels may increase the antibacterial functionality of biomedical devices, implants, drug delivery, separation membranes, and
inherent antifouling or antibacterial surfaces. Ultimately, properties, e. marine coating. However, the application is still made at a laboratory
g., biocompatibility and tunable biodegradability, can be provided to scale, and applications at the industrial scale still see many challenges
these surfaces showing their versatility for the medical setting. How [82].
ever, further optimization of these techniques is needed [67], especially SB-based polymers are commercially available monomers and with
when applied to topographical surfaces. more applications found in the literature. CB-based polymers have
shown excellent antifouling properties [84] and biocompatibility [85].
3.1.2.2. Nanoparticle incorporated hydrogels. For antibacterial surface PC-based polymers show excellent biocompatibility [37,82] compared
applications, nanoparticle incorporated hydrogels are an option of to SB- and CB-based polymers. Zwitterionic hydrogels exhibit unique
choice, particularly when in contact with the body (i.e., wound dress behaviors and properties, including “anti-polyelectrolyte” behavior,
ings). These materials could also include antibiotics. However, in this unusual pH sensitivity, and temperature sensitivity [82]. Research has
paper, antibiotics will not be described as it is not the focus of the cur shown that polyzwitterion's antifouling action cannot be correlated to
rent literature review. Bodnenberger et al. describe the use of NP ap the type of zwitterion used but due to their exact chemical structure
plications in hydrogels. In this case, the hydrogel is loaded with NPs [86]. Shen et al. demonstrated that soft and wet drag-reducing zwit
enabling to increase antibacterial efficacy [68]. Among metal NPs, silver terionic hydrogel coatings have weak swelling in saline solution and are
NPs (AgNPs) have attracted much research due to their antimicrobial effective against E. coli and S. aureus. The antibacterial activity and weak
properties [69,70]. AgNPs in solution, at the surface or composite, can swelling were obtained by the combination of using the anti-
lead to various antibacterial mechanisms, e.g., the generation of reactive polyelectrolyte effect of poly-N-(3-sulfopropyl)-N-(methacryloxyethyl)-
oxygen species (ROS), which are harmful to bacteria [71]. ROS, such as N,N-dimethylammonium betaine (PSBMA) and the typical poly
superoxide, hydrogen peroxide, and hydroxyl radical, can cause several electrolyte effect of polyacrylic acid (PAA) [87]. Although PSBMA
types of intracellular damage in bacterial cells [72]. When in contact exhibited antifouling properties, PSBMA has an anti-polyelectrolyte ef
with mammalian cells, some formulations of AgNPs can be cytotoxic, fect, which mechanism is shown in Fig. 5 [88], causing swelling and
limiting their application in humans [73,74]. However, exceptions exist shrinkage behavior when transferred from water to a saline solution.
in the literature for AgNPs alone [75–78] and AgNPs-hydrogels nano However, this effect was suppressed by using PAA, improving the me
composites with non-cytotoxic effects [79]. chanical properties of the hydrogel [87]. Huang et al. increased the
Niu et al. reported the preparation of supramolecular hydrogels hy durability of zwitterionic polymers by blending networked zwitterionic
bridized with AgNPs by in-situ reduction of AgNO3 stabilized by microgels with the PES polymer matrix. For both E.coli and S.aureus a
PPEGMA-ran-PAA followed by complexing with α-cyclodextrins reduction in bacterial attachment has been observed. Furthermore, the
(α-CDs), as shown in Fig. 4. These hydrogels were physically cross- antibacterial property was maintained after challenges with harsh
5
active antimicrobial polymer is functionalized with positively charged

quaternary ammonium [94].
3.2.1.1. Quaternary ammonium compounds. Quaternary ammonium

compounds (QACs) are positively charged polyatomic ions [95]. They
are among the most commonly used disinfectants in the food industry
for long-term stability and effectiveness against bacterial biofilms [27].
QACs consist of 4 alkyl groups attached to a central cationic nitrogen
atom [95]. By nature, QACs are perpetually charged, regardless of the
pH solution [95]. Various known factors contribute to the antibacterial
effect of QACs. For instance, the antibacterial efficacy depends on their
chain length and can be grouped into long- and short-chained [96]. In
this review, the definition of long-chained QACs by Li et al. [97] and
Kaur et al. [96] is where their alkyl substitution reaches longer than six.
The optimum chain length for antibacterial activity of QACs for gram-
positive bacteria is 12-14 carbons and a length of 14-16 carbons for
gram-negative bacteria [98,99]. However, the exact mode of action of
immobilized QACs has yet to be explained. It is known that a threshold
of molecular charge density of immobilized QACs is required to induce
cell death [99,100]. The charge density threshold (quaternary amine
units/cm2) for contact killing in high-division conditions (i.e., log-
phase) is 1012 and 1013 N+/cm2 for E. coli and S. epidermis [101]. As
for low-division conditions (i.e. stationary pahse) it is 1014 N+/cm2 for
Fig. 5. Mechanism of anti-polyelectrolyte effect of zwitterionic polymer both E. coli and S. epidermis [101].
brushes [88]. To covalently integrate QACs onto biomaterial surfaces, various
methods have been developed, which include the sol-gel process via
chemical environments [89]. covalent hydrolyzable ester linkage, atom transfer radical polymeriza
An attractive system is the combination of polyzwitterions and PEG, tion, plasma polymerization, and layer-by-layer deposition [102–107].
which has shown antifouling property [90–93]. However, the exact The approach is effective to impart permanent active contact antimi
mechanism has not been elucidated. A deeper understanding of non- crobial activity on surfaces [105,108–114]. In 2013, Asri et al. demon
fouling performance is needed. Leng et al. compared the surface hy strated a coating of covalently tether QACs in a hyperbranched
dration of antifouling zwitterionic and PEG materials in contact with configuration onto silicon (Si) surfaces. As shown in Fig. 6, these sur
proteins. Results suggested that surface hydration for PEG-coated sur faces were prepared by covalently attaching hyperbranched polyurea
faces and NPs, are relatively strong and resist protein adsorption. This is (HB) coatings to glass slides. Polyethyleneimine (PEI) was added to
due to surface hydration that is disrupted to a certain degree. Free- couple covalently with the polyurea branches. By consecutive alkylation
floating in solution PEG showed bondage with proteins which reduces with 1-bromohexane and iodomethane the coatings were converted into
hydration. SB-coated surfaces, or free-floating SB, showed strong hy hydrophobic polycationic species creating. As a result, a-Si-HB-PEI+
dration in contact with proteins [93]. As evident from the research coating. Here, two concentrations of PEI was used, 10 wt% and 20 wt%
studies, zwitterionic polymers show antibacterial and antifouling [115]. Evaluation by confocal microscopy showed that coatings made
properties achieved by their strong hydration in contact with proteins. with a 10 and 20 wt% concentration of PEI showed a charge density of 6
The diversity of zwitterionic polymers used is still limited. More × 1015 and 4 × 1015 N+ cm− 2, respectively. The 20 wt% Si-HB-PEI+
research is needed to broaden the existing structural diversity of poly coating displayed >99%, >99,9% and 99,99% contact-killing at bacte
zwitterions for antifouling optimization. The next generation of zwit rial challenges of 16, 160 and 1600 CFU/cm of S.epidermidis.
terionic polymers should take into account mechanical stability at the In 2019, Dong et al. demonstrated similar research of immobilized
surface over a prolonged time without losing antifouling properties. robust hyperbranched antibacterial coatings on poly(dimethylsiloxane)
When applied in the clinical setting, specifically in contact with the (PDMS) [116]. These coatings showed exceptional antibacterial activity
human body, biocompatibility should be assessed. against various Gram-positive and Gram-negative bacteria. Interest
ingly, by utilizing EDTA as a permeabilizer, the antibacterial activity
was strongly enhanced by weakening the molecular interactions of the
3.2. Contact active principle lipopolysaccharide constituent of the outer cell membrane [117], dis
playing similar effectiveness for both Gram-positive and Gram-negative
Unlike the anti-adhesive principle, where antifouling mechanisms bacteria [116]. Unlike tethering QACs to hyperbranched polymers,
reduce bacterial adhesion, the active contact approach focuses on Villanueva et al. concluded that medical grade poly(vinyl chloride)
immobilizing antibacterial agents onto the surface through covalent (PVC) is able to transform into antibacterial plastics with high anti
bonds that kill bacteria on contact. Strategies based on the principle of bacterial activity against both gram-positive and gram-negative micro
active contact include the use of active action polymers, quaternary organisms. Here, a coating comprising of QACs and aliphatic moieties
ammonium cations, and antimicrobial proteins & peptides. was formed on PVC. Mercaptopropyltrimethoxysilane and amino
propyltriethoxysilane were grafted onto PVC. Then betaine and dodecyl
3.2.1. Active action polymers succinic anhydride (DDSA) were bonded to free amino groups. Sur
In contrast to passive polymers, which are based on their antifouling prisingly, surfaces treated with betaine and DDSA showed low bacterial
ability, active polymers are based on killing bacteria that adhere to the attachment. The mode of action of the coated PVC is concluded to be
polymer surface [94]. Typically, these polymers are functionalized with related to the interaction between cationic and aliphatic moieties and
an antibacterial agent that kills or reduces the metabolic activity of microbial cells [118].
bacteria, minimizing their pathogenic effect in their biological envi Although QACs are commonly used, there remains a lack of knowl
ronment. The exact mechanisms of these functionalized polymers, edge on the toxicity of surface-immobilized QACs, which should be
however, depend on the active agent. Nowadays, the most widely used
6
Fig. 6. Schematics of the preparation of covalently attached hyperbranched polyurea coatings, tethering of polyethyleneimine and two-step alkylation of PEI that
was covalently coupled onto hyperbranched polyurea coatings [115].
crucial to research for creating and designing intelligent materials. functionalized surface [124].
QACs, though are simple in structure but are complex as various vari Yasir et al. elucidated the mechanism of action of surface-
ables attribute to their antibacterial effect. However, the charge density immobilized antimicrobial peptides Melamine and Mel-4 against
of immobilized QACs, in particular, has proven to be crucial. As P. aeruginosa. Melimine and Mel-4 are chimeric cationic peptides
mentioned earlier, to induce cell death, a threshold charge density has to inhibiting a broad- spectrum of antimicrobial activity. The two peptides
be met. Therefore, investigation for optimizing attachment density are highly biocompatible and have been tested in human clinical trials.
should be focused on. Surface immobilized QACs show high potential as Yasir et al. concluded that both immobilized melamine and Mel-4 show
an antibacterial surface strategy. However, the use of surface- similar mechanisms of action immobilized as in their solution-phase: the
immobilized QACs is still in the development stage. Therefore, the ability to bind bacterial lipopolysaccharides, cause membrane disrup
toxicity and safety application in medical settings remains uncertain and tion, and facilitate the release of ATP and subsequently DNA/RNA from
should focus on future research. cells [125].
He et al. developed an immobilization method of AMPs with stable
3.2.2. Surface attached antimicrobial peptides activity by combining initiated atom transfer radical polymerization on
Antimicrobial peptides (AMP) are oligopeptides composed of silicon surfaces (SI-ATRP) and click chemistry [121]. Generally,
cationic and hydrophobic amino acids [28,119]. AMPs play a crucial attachment of AMPs to a surface has limitations as stability is impaired
role as potent antibiotics in innate immunity. They are categorized by due to degradation of the peptide by enzymes and antibacterial activity
their secondary structure in four groups, which include β-sheet, α-helix, could be impaired if the AMPs are not correctly orientated due to surface
extended, and loop [119]. The use of AMPs has emerged as a promising energy [122,123,126]. By using a spacer molecule, as shown in Fig. 7,
strategy in the combat against biofilm-related infections because they
show high potency against biofilms. However, AMPs are limited in the
clinical setting by a couple of factors, e.g., bio-degradation and lack of
knowledge on the multiple mechanisms of action [28]. In recent studies,
many mechanisms of action of AMPs have been described [120].
Although, it has yet to be determined whether the multiple mechanisms
of AMPs are independent of one another [120]. It is hypothesized that
surface attachment of AMPs can be target specific to the cell membrane
[28]. However, unlike other antimicrobial agents, AMPs only exhibit
antibacterial activity if orientated adequately on the surface [121–123].
Dutta et al. immobilized the antimicrobial peptides, LL-37, mel
amine, lactoferricin, and Mel-4 onto poly-hydroxyethyl methacrylate
(pHEMA) surfaces to achieve an antibacterial effect. These findings
indicated that a threshold concentration of immobilized AMPs on
pHEMA is crucial to achieving antimicrobial activity. Furthermore,
outcomes showed that the inhibition is highly sensitive to the attach
ment technique used. Interestingly, Dutta et al. noted that the contact Fig. 7. Schematic diagram for the chemical immobilization of PraAMP to Si
area between the AMP and the bacteria affects the efficacy of the AMP surface [121].
7
poly[2-(methacryloyloxy)ethyl]dimethyl-(3-sulfopropyl)ammo
niumhydroxide (polySBMA), enzymolysis stability of the surface was
increased. Furthermore, by modifying the antimicrobial peptide HHC36
with L-propargylglycine (PraAMP) and attaching the PraAMP to the
spacer molecule, salt-tolerant properties were enhanced. The surface
exhibited antimicrobial activity against E. coli, S. aureus, and
P. aeruginosa and exhibited negligible cytotoxicity to mouse bone
mesenchymal stem cells.
Novel techniques to combat biofilm formation have risen. Among the
most promising antibacterial strategies, surface-attached AMPs are
strategies with the most potential, as they have shown high potency
against biofilm formation and good biocompatibility. Moreover, AMPs Fig. 8. Chemical structures of synthetic DHP derivatives [134].
have shown high sensitivity to techniques used for surface attachment.
In addition, the efficacy of AMPs has been revealed to be affected by chemistry for specific covalent surface attachment of the QSI DHP. The
contact area and orientation. Therefore, to gain more knowledge, for structural orientation of DHP can influence antibacterial activity.
improvement and optimize efficacy, the diversity of AMPs should be Therefore, it is imperative to show the importance of the orientation and
tested on various attachment techniques and correlated AMPs attach location where QSIs attachment occurs. However, before a clinical
ment to the specific action mechanism. To date, AMPs in the clinical and application, research is crucial as surface-immobilized QSIs are a novel
medical application will stay limited unless the mode of action against strategy that has yet to be fully understood. Nevertheless, the ability to
specific bacterial strains is better understood. Yasir et al. has shown immobilize QSIs on surfaces represents a potential approach as an
great steps in elucidating the mechanism of action of surface- antibacterial coating for effective biofilm formation prevention,
immobilized Melamine and Mel-4 where results conclude that the reducing the risk for the development of bacterial resistance.
immobilized form of both AMPs exhibits a similar mode of action to its
soluble form. Nevertheless, the use of surface-attached AMPs may set a
new standard in long-term antibacterial and even broader antimicrobial 3.3. Biocide attached/release principle
functionality for its potency and its intrinsic ability to combat biofilm.
The biocide attachment and release approach integrates the release
3.2.3. Quorum sensing inhibition of a toxic substance to bacteria upon attachment [135]. There are
Quorum sensing (QS) is a bacterial cell-to-cell communication pro multiple strategies where biocides can be attached and released to
cess that relies on the production, sensing, and response to extracellular eradicate bacteria from the surface [130–135]. Some of them can be
signaling molecules that allow bacterial communities to share infor considered toxic by design, as in metals and other complex organic
mation about their changing environment [127–129]. QS alters specific substances. Only a few of these approaches are not toxic [136], such as
gene' expression in a population [129,130]. For example, QS in gram- antifouling-based principles for marine applications. However, in the
negative bacteria makes use of the release of chemical signal mole clinical setting, selective pathogenic bacteria-killing remains an issue.
cules called autoinducers. Gram-negative bacteria use acyl-homoserine Efforts have started to appear for fungi using metal nanoparticles [70].
lactone (AHL) as an autoinducer [128,131]. When the population den Similar strategies should be applied for the design of multifunctional
sity of a bacterium reaches a specific “quorum,” the corresponding level surfaces selective to pathogenic bacteria. Besides the uniqueness of the
of AHL concentration can induce activation of transcriptional activators, proposed approaches, we will focus on metal nanoparticles attached/
which in turn activate transcription of genes and modify physiological released from the surface and the principles of these processes in this
functions [128,132]. section.
3.2.3.1. Surface immobilized quorum sense inhibitors. Surface immobi 3.3.1. Nanoparticle metals
lized QS-inhibitors (QSIs) rely on inhibition of QS, resulting in blockage In this section, surface immobilization with metal nanoparticles is
of bacterial communication rather than inducing bacterial death. Ho discussed [137]. Depending on the NP type, the antibacterial mecha
et al. demonstrated the reduction of bacterial surface adhesion up to nism might vary [30]. A broadly accepted mechanism is the generation
97% for both P. aeruginosa and S. aureus by covalent attachment of the of reactive species (ROS) that can end-compromising the cell membrane
QSI, dihydropyrrolones (DHPs). DHPs were immobilized on glass sur integrity, as depicted in Fig. 9. Another critical parameter to evaluate is
faces via copper-catalyzed azide-alkyne 1,3-dipolar cycloaddition click the antibacterial activity of metal ions in solution from metal nano
reaction. This click-DHP coating displayed an exceptional reduction in particles which is generally non-specific, displaying a broad spectrum of
bacterial adhesion and biofilm formation in vitro over 48 hours[29]. activity [138], e.g., AgNPs.
Taunk et al. compared the immobilization of various DHPs and furanone To provide antibacterial functionality to a surface, metal NPs can be
(FU) compounds on azide-functionalized glass surfaces. The results either covalently immobilized or coated onto surfaces. Moreover, NPs
suggest that non-specific attachment of FUs and DHPs to highly reactive can be loaded into hydrogels and then be coated onto a surface to an
azide-groups does not impair the antibacterial activity of the com antibacterial mode of action. Materials frequently used are silver, cop
pounds, indicating that the compounds retain their activity even after per, gold, iron, and zinc in the form of NPs. In Fig. 9, hypothesized
attachment[133]. In later work, Taunk et al. demonstrated the impor mechanisms of AgNPs and silver ions are displayed [139]. The generally
tance of the structural orientation of DHPs for S. aureus activity. Results accepted phenomenon is based on NPs causing damage to bacterial cell
displayed better antibacterial activity with surface attachment to the N- membranes or cause detrimental alterations to organelles [53]. Yeray
position opening the phenyl group (Fig. 8) rather than the attachment of et al. developed a versatile method of synthesis in situ of silver NPs with
C-4 position of the phenyl of DHP. However, results showed no differ a well-defined size using maleimide as a single crosslinker and polyvinyl
ence in activity for P. aeruginosa [134]. alcohol [140]. Yeray et al. concluded that the cross-linking degree of
In general, the immobilization of QSI’s on surfaces has shown to be a hydrogel networks regulated and stabilized the NP size in their work. In
novel strategy with a high potential for antibacterial application. The this study, the encapsulated AgNPs have demonstrated antibacterial
precise mechanisms of action of surface-immobilized QSI’s have yet to activity against S. aureus owing to the release of the AgNPs. Moreover,
be elucidated. Ho et al. has demonstrated the utilization of CuAAC click the antibacterial activity against S. aureus depends on NP size, where the
antibacterial effect increases as the nanoparticle size diameter decrease
8
hydrophobic, and superhydrophobic topographies.
4.1. Wettability and the contact angle (θ)
Wettability is a key physical parameter used to characterize anti

bacterial surfaces. The wettability of a surface can be evaluated by
measurements of the apparent contact angle (CAo) of a sessile droplet
[145,146]. As shown in Table 3, the CAo range can aid in identifying the
wettability property of the surface. From the CAo, (super)water repel
lency [147] or hydrophilicity [148] can be characterized. In most cases,
(super)water repellent surfaces can prevent bacterial attachment
[149–151]. On the contrary, hydrophilic surfaces might increase bac
teria attachment [152] to the surface unless the surface is coated with a
slippery material, which in essence retain its hydrophilicity over time
[152].
4.1.1. Hydrophobicity and superhydrophobicity

Traditionally, a surface is considered hydrophilic when the CAo is
lower than 90o, hydrophobic when CAo is larger than 90o and smaller
Fig. 9. Schematic representation of the known mechanisms of antibacterial than 150o. Drops with angles lower than 90o tend to adhere to smooth
action of silver [139]. surfaces. While drops with larger angles than 90o tend to slide more
easily [153]. When the CAo of a drop is larger than 150o, the surface is
[140]. considered superhydrophobic [145,154]. Sessile drops on super
Huang et al. developed an antibacterial silver NP surface- hydrophobic surfaces take almost spherical shapes. Super
functionalized with d-cysteine. The surface exhibited excellent anti hydrophobicity may not be achieved without micro(nano)topography
bacterial activity against E.coli, P.aeruginosa PA01, and S.aureus. d- unless superhydrophobic coatings are used. Chemical techniques
Cysteine inhibited the maturation of biofilm and suppressed bacteria in enabling superhydrophobic functionality over a surface include chemi
a dispersed and planktonic unicellular state. Furthermore, d-Cystine cal etching, templating, sol-gel processing, electro-spinning, anodic
increased the lethality of silver NPs to bacteria. This combination of oxidation, layer-by-layer assembly, electrochemical deposition, and
AgNPs and the biofilm-dispersing properties of d-cysteine achieved chemical vapor deposition [48]. Once superhydrophobicity is achieved,
more durable and more effective antibacterial ability [141]. In contrast a sessile drop might slide off from the surface[154]. Such characteristics
to previous research, Sun et al. reported the design and synthesis of can be used to produce self-cleaning materials, providing an additional
perfluoroalkyl attached silica nanoparticles. By adding these NPs into advantage to reduce bacteria attachment [155,156]. However, under
curable coatings, high wear-resistance and antibacterial activity against standing wetting properties on antibacterial surfaces is not trivial as
E.coli and S.aureus were achieved due to the particle self-migration to complex patterns or other wetting properties can emerge [157,158].
the surface [142]. Another point is understanding the action mechanism during self-
Gadkari et al. developed a silver-loaded CS NP coating by using the cleaning because micro(nano)features decorating surfaces are far from
layer-by-layer (L-B-L) technique and applied this on cotton fabric. The smooth. In fact, they are rough, which makes the understanding of the
silver-loaded chitosan (CS-Ag) was prepared by adding an aqueous so wetting properties challenging and difficult to characterize. The influ
lution of AgNO3 to a CS nanoparticle suspension. This L-B-L coating ence of the surface micro(nano)structure on the CAo of droplets is usu
exhibited 100% antibacterial activity against both Gram-positive and ally explained by the Wenzel model [159], which applies to wetted
Gram-negative bacteria. In comparison, the CS-Ag coated fabric showed surfaces. In other words, the liquid fills in the space between the surface
only 72% and 68% effectiveness against S. aureus and E. coli [143]. micro(nano)structures. In the Cassie-Baxter model [160], the liquid lies
In view of the afore-stated research, the effect of silver NPs can atop the micro(nano)structure, it leaves air between the interspace of
enhance the existing antiseptic properties of materials. Yeray et al. have the micro(nano)structures under the droplet, and the surface can be
shown the importance of NP size, where the decrease in nanoparticle considered hydrophobic. A detailed description of the Wenzel and
size relates to an increase in antibacterial activity [140]. However, it Cassie-Baxter is addressed below.
should be noted that smaller particles also exhibit higher cytotoxicity to
the host cells. Moreover, Ferdous et al. conclude that biological inter 4.1.1.1. The Young model. The interaction between the solid surface
action and toxicity are dependent on particle number and surface area and the liquid drop has been modeled using a number of equations.
for the same mass of an NP [144]. Huang et al. have shown the impor Assuming that the surface is ideal, i.e., smooth, isotropic and physico
tance of combining multiple mechanisms and/or approaches to improve chemically homogenous, the CAo can be modeled with the Young
antibacterial activity effectiveness. Further research should focus on equation
minimizing the load of NPs for optimal antibacterial activity in combi ( )/
cosθ = γsg − γsl γlg
nation with complementary strategies, such as functionalizing silver
with d-cysteine. These complementary strategies can increase efficacy,
which may lower the concentration of silver NPs needed for optimal Table 3
antibacterial activity [141]. Wettability label, range of CAo, and physical observation. These intervals have
been modified to adjust to the CAo observed in nature.
4. Physical strategies Wettability Contact angleo Observation
(θ)
In this section, the properties of wetted surfaces are first examined, Hydrophilic 0o≤ CAo≤90o The water drop wets the surface. For
followed by the antibacterial properties of textured surfaces. Exclusive angles close to zero, the drop spreads on
attention is paid to fabricated surfaces that are antibacterial by design the surface.
Hydrophobic 90o<CAo≤150o The water drop partially wets the surface.
free of biocides. The strategies include the fabrication of hydrophilic,
Superhydrophobic CAo>150o The water drop does not wet the surface.
9
where γsg, γsl, γlg are the energies in the solid-gas, solid-liquid, and 4.2.2. Antibacterial skin
liquid-gas interfaces. The Young model does not take into account the Similar to leaves, the skin of some animals evolved to develop anti-
influence of surface roughness [161]. Regardless of the topography, the biofouling properties, such as micro- and nano-structures and wax. For
effect of microstructures during wetting Cassie-Baxter and Wenzel example, the skin of sharks is covered with micro-structures called rib
models are usually employed to understand droplet-structured surface lets. Compared to plants, the typical diameter of riblets is larger than the
interaction [147]. diameter of the bumps on leaves, between 100 to 300 μm [169,170].
Other topographical surfaces, such as the feet of Gecko, show micro-
hairs, called setae, with diameters comprehended between 30 and 130
4.1.1.2. The Cassie-Baxter model. The Cassie–Baxter model describes
μm [171]. Other surface topographies like the wing of butterflies display
the CAo of a drop sitting on top of the microstructures, leaving an air
scales similar to shingles, with width between 30 and 50 μm and length
layer under the droplet and around the microstructure. In other words,
between 58 and 146 μm [164]. On a smaller scale, Cicada wings are
the Cassie-Baxter can be used to describe a (super)hydrophobic solid;
covered with nanopillars of conical shape [172,173]. It has been found
typically, the surface below the drop consists of a fraction of air [147].
on the wings of cicadas and dragonflies bio-wax [164]. Such bio-wax
Here, it is assumed that the CAo on the purely solid surface can be
might play a role in enhancing antibacterials properties along with an
estimated with the Young equation and can be written as
increase in hydrophobicity, end-interacting with proteins and lipids
cosθ* = ϕs (1 + cosθ) − 1 components of the cell membrane [174].
To avoid bio-fouling, the surface of leaves developed super-
where θ* is the apparent CAo corresponding to the state of stable equi hydrophobicity with contact angles comprehended between 142o and
librium, θ is the equilibrium contact on the Young equation, and ϕs is the 159o [164]. Meanwhile, the skin of some animals may have considerably
fraction of the liquid interface in contact with the solid. lower angles than plants comprehended between 76o up to 147o [164].
Grooming possibly explains such a different range of angles [175], as
4.1.1.3. The Wenzel model. The Wenzel model describes the CAo when plants cannot clean their leaves and bio-fouling components remain
the liquid has filled the space below the drop. In other words, a sessile longer on their surfaces. When a structured surface is super-hydrophilic
drop in a Wenzel state has been impaled on the micro-structures. Unlike (CAo=0o), a thin layer of water covers the surface, resulting in a force of
the Cassie-Baxter model, the Wenzel model leads to highly adhesive attachment to another surface. When a surface is hydrophobic, van der
forces in the solid-liquid interface. The Wenzel model can be written as Waals forces produce a tiny force of attachment as well. It has been
argued that the numerous structures on the feet of Gecko evolved to
cosθ* = rcosθ optimize the use of both of these forces to attach to walls at will [176].
where r is the dimensionless roughness defined as the ratio between the
4.3. Effects of surface modification, micro-, and nano-structures
area of the wet surface and the total surface under the droplet [159]. The
presented models are the basis for the understanding of surface wetting
4.3.1. Fabrication of hydrophobic surfaces
properties, essential for antibacterial surfaces.
Schwibbert et al. [177] investigated the effect of irregular nano-
structures during E. coli and S. aureus colonization. In this investiga
4.2. Antibacterial surfaces in nature
tion, the nano-structures have been fabricated on polyethylene surfaces
using a femtosecond laser. The irregular nano-structures fabricated on
After millions of years of evolution, nature has created unparalleled
the surface led to an increase in the CAo from 65o to 121o. While the
antibacterial surfaces. Researchers have attempted to mimic hierarchies
topographical surface reduced the adhesion of E. coli, the coverage of
from nature by employing physical structuring using fabrication
S. Aureus remained unaltered. Schwibbert et al. [177] concluded that
methods. Fabrication methods from microelectronics are typically used
bacterial repellence might not only be attributed to wetting properties
to mimic the antibacterial effect in nature. Interestingly, the importance
but the shape and size of the bacteria and the pillars play a role as well.
of naturally occurring antibacterial surfaces lies in the fact that such are
Specifically, S. aureus is small enough to fit within the valleys of the
not coated with biocides [41].
surface, unlike E. Coli. This allowed the S. aureus to adhere to the sur
face. Nevertheless, the femtosecond laser process has endowed the
4.2.1. Antibacterial leaves
polyethylene surface with an outstanding antibacterial effect on E.coli by
Plants evolved to avoid biofouling on their leaves. Hydrophobicity is
impeding bacterial adherence [177].
their first line to combat the attachment of water drops at the surface.
Peter et al. [32] used direct laser interference patterning (DLIP) to
The leaves of plants, such as Taro and Lotus, secrete wax [162–164].
fabricate periodic arrays of cones and holes separated about 850 nm in
Surfaces covered with bio-wax are hydrophobic, typically displaying
stain steel. The presence of these structures modified the contact angle of
contact angles between 74o [164] up to 106o [165]. Such property is
stainless steel from 77±3o to 154±3o for cones and 148±5o for holes.
thanks to the bio-wax and micro(nano)structure surface features. For
The presence of these structures resulted in a considerable reduction of
example, Taro and Lotus leaves have elliptical bumps whose diameter is
retention of E. coli and S. aureus. On E. Coli, the retention reduction was
around 20 μm [162,163,166]. Such bumps further increase the CAo,
about 99.8% for cones and 99.4% for holes. On S. aureus, the retention
making the surface superhydrophobic [163,166,167]. Hierarchical fea
reduction was about 70.6% for cones and 79.1% for holes. However, this
tures, whose size is on the order of nanometers, can increase hydro
nano-fabrication process did not produce superhydrophobic surfaces as
phobicity over leaves [162–164]. By removing the nanocrystals in Lotus
drops only slide when the tilting angle reached 90o [32]. Gupta et al.
leaves, the CAo decreased about 16o [164]. In addition, nano-bio-wax
[178] produced stainless steel surfaces with enhanced roughness using a
can enhance superhydrophobicity, achieving contact angles up to 142o
nanosecond pulsed laser. In this investigation, pulses of 100 ns with an
for the Lotus leaves and up to 150o for the Taro leaves. Furthermore, it
energy of 7.5 mJ were used to enhance the contact angle from untreated
has been demonstrated that a higher density of such nanostructures
surfaces from 40◦ up to 110◦ after treatment. It was concluded that the
improves the reduction rate of bacteria and bacteria attachment even
laser treatment produced a dual-scale patterning. The first scale is on the
under water [162,164,168]. Thus, water drops on the surface of leaves
micron size, while the second scale is on the nano size. The antibacterial
slide and fall with relative ease. Self-cleaning arises as an unprecedent
properties of these surfaces were tested with gram-negative P. aeruginosa
strategy because biofouling components may attach to drops rather than
and gram-positive B. subtilis. Fluorescent staining on the biofilms of the
staying on the leaves.
treated and untreated surfaces confirmed bacterial inactivation and
adherence.
10
Despite not having the self-cleaning attribute of superhydrophobic 4.4. Physical grounds behind the bactericidal effect
surfaces, changes in topography on the micro and nanoscale may pro
vide hydrophobic and anti-adhesive properties to stainless steel sur The biocidal effects of topographical surfaces have been investigated
faces. Future research should focus on combining micro-and nano- deeply. Some of these studies have focused on natural surfaces, while
fabrication with chemical modification techniques to search for syner others mimic surfaces from nature. Recently, the skin of sharks inspired
gistic strategies [41,177]. the fabrication of antibacterial surfaces [183–185]. These topographical
surfaces consist of millions of uniquely ordered micropatterns that
4.3.2. Fabrication of superhydrophobic surfaces provide antibacterial and antifouling properties [184]. In some cases
Jalil et al. [31] have produced superhydrophobic surfaces on gold creating bacterial patterns over the structured surface [157]. It has been
with femtosecond laser pulses. After treatment, the surface exhibited observed that micropatterns similar to the sharkskin strongly inhibit the
different surface structures on scales of the order of micro and nano- biofilm formation of P. aeruginosa and S. aureus [183] without using
meters. Some of the shapes were conic, 1D-rods of less than ≤6 μm, toxic compounds [184]. The microtopography of shark skin not only
and spherical nano-structures with a diameter of ≥10 nm. The results inhibits the attachment of bacteria in an early stage but also inhibits
indicated that the femtosecond laser-induced changes in the wettability, biofilm formation [186]. Bacterial loads are reduced due to the effect of
going from hydrophilic to superhydrophobic. With this technique, longitudinal vortices formed on the grooves of the riblets [185]. Such
treated surfaces demonstrated the reduction of E. coli compared to non- vortices are the result of a turbulent flow induced by non-uniform
treated surfaces [31]. grooves. In reverse osmosis membranes, the optimal length of shark
Freschauf et al. [179] developed a shrink method for producing lets and the space between them has been optimized at 2 μm [187].
superhydrophobic surfaces using consumer plastics without chemical Moving on from shark-like riblets, cicada wings containing nano
modification. The method consists of pre-stressed polyolefin (PO) pro structures have also been proposed as a powerful alternative applied in
cedure that fabricates rough surfaces with multiscale structures of the field of antibacterial surfaces [188,189]. The conical nanopillars on
extreme aspect ratio [180]. PDMS is used to cast such a structure on a cicada wings are protruding upward from the surface. Biophysical
mechanically and thermally stable medium. PDMS molds are used to models of the bactericidal activity reported that the cell wall attaches to
endow various hard plastics with the initial topography. Results indi these conical pillars during drying. As the drying process continues, the
cated that the superhydrophobic surfaces exhibit a significant reduction cell wall is ruptured due to extension stress [189,190]. The stress con
in bacterial growth of E. coli over flat surfaces. The ability to endow centrates in the regions suspended between the pillars, ultimately
superhydrophobic structures to plastics may be a method that is tearing the membrane. These natural surfaces more effectively kill gram-
compatible with roll-to-roll manufacturing and scale-up production negative bacteria than gram-positive bacteria. It is believed that gram-
[179]. Tripathy et al. [181] designed flexible superhydrophobic surfaces positive bacteria are more resistant due to the higher stiffness of their
decorated with copper hydroxide nanowires. These nanowires are cell wall [164,191]. Another investigation of E. coli on the wings of
grown separately and transferred onto a polydimethylsiloxane (PDMS) dragonflies demonstrated that the membrane is damaged even before
surface by mechanical peeling, allowing non-planar 3D structured sur direct contact with the structures takes place [192]. This investigation
faces to be fabricated. These surfaces have shown antibacterial effects, demonstrated that membrane damage results from a combination of
blood repellence, hemocompatibility, making them suitable for health strong adhesion between the nanopillars and the extracellular polymeric
care applications [181]. substance. An additional shear force appears when immobilized bacteria
Wang et al. [182] fabricated a robust superhydrophobic surface attempt to colonize these topographies.
(Fig. 10) for possible long-term applications in the health care setting.
Here, both of these apparently opposite characteristics are achieved by 5. Multifunctional antibacterial strategies: coatings and
fabricating a micro-structured armor around the nano-structures. While topographies
the nano-structures provide superhydrophobicity, the micro-structured
armor provides durability. The micro-structured armor is an inter Multiple functions can enhance antibacterial properties at the sur
connected frame containing ‘pockets’ with water-repellent and me face to combat biofilm formation and prevent bacterial infections.
chanically fragile nanostructures. When such composite structures are Cloutier et al. have categorized multifunctional antibacterial surface
fabricated on the surface of various materials such as silicon, ceramic, strategies into multiapproach, multiagent release, and multi-property
metal, and transparent glass, super-hydrophobicity has persevered after surfaces [193]. In this review, we focus on multiapproach and multi-
abrasion. Silicon inverted-pyramidal microstructures were manufac property surfaces. An additional level of multifunctionality is added
tured by photolithography. However, ceramic, metal, and transparent with the integration of physical structuring, addressed in the perspective
glass inverted-pyramidal microstructures were manufactured by section.
embossing technology. Interestingly, the produced structures showed
high mechanical stability as superhydrophobic interaction was main 5.1. Multi-approach surface
tained after extreme harsh conditions [182].
This is a novel strategy with high potential in antibacterial coatings.
The approach uses multiple functional routes, such as CA, BAR, and AA,
to improve antibacterial efficacy. Various efforts have been made to
develop multi-approach surfaces over the last few decades [194]. One of
the main disadvantages of BAR, AA, and TM is that dead bacteria can
build up and start biofilm formation [10]. Townsend et al. have devel
oped a dual approach coating consisting of two types of AMPs for im
plants. This dual system consists of electrostatic released peptides that
can sterilize surrounding tissue in the short term and works in tandem
with covalently attached peptides for long-term bacterial inhibition
[195]. He et al. demonstrated an outstanding novel antibacterial and
antifouling strategy whereby a surface structure, consisting of a CA
Fig. 10. Strategy for enhancing the mechanical stability of the super upper-layer and an AA sub-layer, is made. This surface is prepared by
hydrophobic surface by housing water-repellent nanostructures within a pro casting gemini quaternary ammonium salt (GQAS) waterborne poly
tective microstructure ‘armor’ [182]. urethanes over layered PEG and hydrophobic blends. The authors
11
speculate that GQAS brushes are deployed at the polymer-air interface zwitterionic, releasing the bacteria from the surface [206]. Q. Yu et al.
forming an antibacterial upper-layer. The combination of GQAS and the have developed a nanopatterned thermoresponsive surface (Fig. 11).
antifouling sub-layers, such as PEG, endow long-lasting antifouling The nanopattern is composed of a thermoresponsive polymer, poly(N-
properties and maintain bacterial killing efficiency close to 99%. This is isopropylacrylamide) (PNIPAAm), and a QAC that act as a biocide
a dual approach of AA and CA principles that can promote surface [216]. The patterned QAC does not only modulate the killing of the
roughness [196]. However, the roughness obtained by GQAS/PEG/hy bacteria using QAC as a tethered biocide, but PNIPAAm aids to release
drophobic surface does not compare to physical structuring methods, the bacteria from the nanotopography. Therefore, PNIPAAm can be
such as laser patterning [31] or microfabrication [197], which have classified as a fouling-release polymer [228,229]. Besides the function
more control over the micro/nanoscale. Advancements in the field can ality given by the PNIPAAm and QAC, the effect of topography (Fig. 11)
be made by combining AA and CA with physical structuring methods. might also play an important role during bacteria-killing [230] or
For instance, structuring could enhance water repellency, enabling release [216].
higher biofouling, maintaining AA and CA bacteria-killing properties
active. 5.2. Multi-property surfaces
5.1.1. Switchable surfaces Multi-property surfaces can display several properties simulta
Antibacterial switchable surfaces are based on the ability to switch neously, such as self-healing, anti-frost, anti-fog properties, or increased
functions, and therefore can be considered within multi-approach. Such mechanical strength. Wei et al. developed a universal strategy by
a level of multifunctionality can, for example, promote bacteria-killing alternating L-B-L deposition of a polyanion, poly(acrylic acid-co-1-
and bacteria-releasing [198,199]. Bacterial-killing and bacteria-release adamantan-1-ylmethyl acrylate) [P(AAco- adamantane)] with guest
properties can be activated by either temperature or light [200,201]. adamantane groups, and a polycation, poly-(allylamine hydrochloride)
The application of an electrical field or other substances such as salt and (PAH). The guest adamantane groups served as anchor points for the
sugar or variations in pH are important stimuli that enable switching immobilization of functional host molecules by supramolecular forming
between antibacterial functions [202–204]. In Table 4, a summary of the host-guest complexes with β-cyclodextrin (β-CD) and derivatives modi
most representative switching functionalities found in the literature is fied with quaternary ammonium salt groups (CD-QAS). In conclusion,
provided. This table shows the great variety of switching approaches due to the nature of non-covalent host-guest interaction, versatility in
that can modulate bacterial viability at the surface. incorporating bio-molecules without impairing functionality was ach
A few examples are described in the following lines to highlight the ieved. In addition, dead bacteria are easily removed, and CD-QAS and its
bacteria-killing and bacteria-release properties modulated using tem derivates can be regenerated [231]. Guo et al. developed a multifunc
perature or pH. For other stimuli than temperature and pH, the reader tional antibacterial self-cleaning surface coating. This novel coating is
should consult the references listed in Table 4. G. Cheng et al., demon developed by grafting poly(N-vinylpyrrolidone-co-maleic anhydride)
strated that a change in pH could trigger switchable properties. In this (poly(NVP-co-MA)) co-polymer on glass slides. This multifunctionality
case, the coating located at the surface has bacteria-killing and anti is achieved due to PMA segments attaching covalently to the glass sur
fouling properties. The antibacterial agent was a cationic pCBMA-1 C2. face to enhance long-term stability, whereas PVP segments enable anti-
Then, by changing the pH, the cationic deviated is hydrolyzed to a fog, anti-frost, antibacterial, and self-cleaning properties. The coating
exhibited antibacterial activity against E.coli and S.aureus, robustness,
Table 4 durability, and could shield the surface from fog, frost, and oil-based
Switching functionalities that promote bacteria-killing and bacteria-release contaminants [232].
[205]a.
Bacterial killing Bacterial Mechanism of bacterial Reference 6. Perspective: towards long-term antibacterial activity
Release release
Cationic CB esters CB esters pH [206,207,208] At first, future research should address the standardization of
SA [209] methods used to address challenges such as long-term antibacterial ac
Cationic Arg-Est Arg-Est [210] tivity and stability, reduced toxicity, increased biocompatibility, and
Cecropin B PMAA [211] wettability. Another issue is the gap of knowledge on surface-attached
Lysozyme [212]
Cationic ONB esters UV light [213,214]
QACs AMPs and QSI. Mentioning QAC specifically, its use is constant
precursors in surfaces because of the antibacterial effectiveness it presents for long
Cationic PSBEDOT Electrical potential [215] periods [185]. AMPs studies only mention effectiveness after 24 hours of
PSBEDOT-Ox exposed bacteria, and more studies are needed to check how various
QAC PNIPAAm Temperature [216,217]
antimicrobial surfaces perform over a longer time [186]. As for nano
Lysozyme [218,219]
AgNPs [220,221] particles, the antibacterial effectiveness has been assessed until day 7
Cationic PTMAEMA Counterion [222] [187,188]. Although these strategies show high potential for their long-
PTMAEMA term stability and high efficacy, longer times are required.
TCS or PolyTA PDVBAPS Salt [223,224] It is also important to understand that, while studies have combined
CD-QAC PBA/CD-QAC Fructose [225]
TRGO Ada/ManCD AdCNa [226]
the principles of AA, CA, and BAR in recent years, few have investigated
GNPL PTLF Vc [227]
a
Abbreviations: Ada, adamantine; AdCNa, sodium adamantine carboxylate;
Arg-Est, L-arginine methyl ester–methacryloylamide; CB, carboxybetaine; CD,
β-cyclodextrin; GNPL, gold nanoparticle layer; ManCD, heptamannosylated CD;
ONB, o-nitrobenzyl; PBA, phenylboronic acid; PDVBAPS, poly(3-(dimethyl(4-
vinylbenzyl)ammonium)propyl sulfonate); PMAA, poly(methacrylic acid);
PNIPAAm, poly(N-isopropylacrylamide); PSBEDOT, poly(sulfobetaine-3,4-
ethylenedioxythiophene); PSBEDOT-Ox, oxidized PSBEDOT; PTLF, phase-
transitioned lysozyme film; polyTA, poly[2-(tert-butylamino) ethyl methacry
late]; PTMAEMA, poly((trimethylamino)ethyl methacrylate chloride); QAC, Fig. 11. Depiction of the procedure for the preparation of nanopatterned
quaternary ammonium salt; SA, salicylate acid; TCS, triclosan; TRGO, thermally PNIPAAm surfaces (Steps 1 and 2) and nanopatterned PNIPAAm/QAC surfaces
reduced graphene oxide; Vc, vitamin C. (Steps 1–3) [216].
12
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Colloid and Interface Science Communications 46 (2022) 100560

Contents lists available at ScienceDirect

Colloid and Interface Science Communications

Strategies applied to modify structured and smooth surfaces: A step closer

1. Introduction methods, bacterial contamination can be reduced by developing single

Fig. 2. Surface modification strategies for antibacterial application.

Fig. 4. Schematic procedure for the preparation of AgNPs hybrid supramo

linked by both pseudopolyrotaxane crystallization and AgNPs, which

active antimicrobial polymer is functionalized with positively charged

3.2.1.1. Quaternary ammonium compounds. Quaternary ammonium

hydrophobic, and superhydrophobic topographies.

4.1. Wettability and the contact angle (θ)

Wettability is a key physical parameter used to characterize anti

4.1.1. Hydrophobicity and superhydrophobicity

You might also like

1 s2.0 S2215038221002004 Main 5

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1 s2.0 S2215038221002004 Main 5

Uploaded by

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Original Title

Copyright

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1 s2.0 S2215038221002004 Main 5

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Colloid and Interface Science Communications 46 (2022) 100560

Contents lists available at ScienceDirect

Colloid and Interface Science Communications

Strategies applied to modify structured and smooth surfaces: A step closer

1. Introduction methods, bacterial contamination can be reduced by developing single

Fig. 2. Surface modification strategies for antibacterial application.

Fig. 4. Schematic procedure for the preparation of AgNPs hybrid supramo­

linked by both pseudopolyrotaxane crystallization and AgNPs, which

active antimicrobial polymer is functionalized with positively charged

3.2.1.1. Quaternary ammonium compounds. Quaternary ammonium

hydrophobic, and superhydrophobic topographies.

4.1. Wettability and the contact angle (θ)

Wettability is a key physical parameter used to characterize anti­

4.1.1. Hydrophobicity and superhydrophobicity

You might also like

Fig. 4. Schematic procedure for the preparation of AgNPs hybrid supramo

Wettability is a key physical parameter used to characterize anti