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Antimicrobial Coatings for Food Contact Surfaces:

Legal Framework, Mechanical Properties, and


Potential Applications
Eduardo Torres Dominguez, Phong H. Nguyen, Heather K. Hunt , and Azlin Mustapha

Abstract: Food contact surfaces (FCS) in food processing facilities may become contaminated with a number of
unwanted microorganisms, such as Listeria monocytogenes, Escherichia coli O157:H7, and Staphylococcus aureus. To reduce
contamination and the spread of disease, these surfaces may be treated with sanitizers or have active antimicrobial
components adhered to them. Although significant efforts have been devoted to the development of coatings that improve
the antimicrobial effectiveness of FCS, other important coating considerations, such as hardness, adhesion to a substrate,
and migration of the antimicrobial substance into the food matrix, have largely been disregarded to the detriment of their
translation into practical application. To address this gap, this review examines the mechanical properties of antimicrobial
coatings (AMC) applied to FCS and their interplay with their antimicrobial properties within the framework of relevant
regulatory constraints that would apply if these were used in real-world applications. This review also explores the various
assessment techniques for examining these properties, the effects of the deposition methods on coating properties, and the
potential applications of such coatings for FCS. Overall, this review attempts to provide a holistic perspective. Evaluation
of the current literature urges a compromise between antimicrobial effectiveness and mechanical stability in order to
adhere to various regulatory frameworks as the next step toward improving the industrial feasibility of AMC for FCS
applications.
Keywords: antimicrobial, coatings, food, surfaces, regulations

Introduction There are numerous sanitary practices intended to prevent mi-


The World Health Organization (2019) estimates that 600 crobial contamination of food products and FCS, but the practice
million people fall ill and 420,000 die each year due to con- per excellence is prevention. With this in mind, the Food Safety
taminated food. Contaminated food contact surfaces (FCS) may, Modernization Act (FSMA) was passed in the United States in
in part, be responsible for such incidences. For instance, coliforms January 2011, changing the focus of the U.S. food safety system
were found on product contact surfaces at a broiler slaughter plant from a responsive strategy to a preventative one (FDA, 2007a).
in Taiwan with concentrations ranging from 104 to 106 CFU/cm2 This reform was passed in response to changes observed in the
(Ho, Huang, & Chen, 2004). At two red pepper powder pro- global food trade system. Australia has also responded, not only
duction facilities at South Korea, Bacillus cereus was found in 1 to ensure the safety of food imported from its closest neighbor,
of 35 samples obtained by swabbing machinery surfaces (Oh, New Zealand, but also to facilitate food trade by the homologa-
Koo, & Kim, 2012). At two different peeled-shrimp processing tion of the food safety standards between both countries (FSANZ,
plants in Iceland, 11.2% of 695 samples taken from conveyer belts, 2018). Similar to other preventative strategies, the use of antimi-
tubs, and forklifts throughout the entirety of the cooking process crobial coatings (AMCs) for FCS is impacted by these regulatory
tested positive for Listeria monocytogenes. Notably, however, no L. changes by the jurisdiction under which they must be observed
monocytogenes were found in samples taken from the final prod- and by the minimum safety features they must possess. For practi-
uct due to sanitation and prevention efforts (Gudmundsdóttir, cal applications, AMCs must meet not only a variety of stringent
Gudbjörnsdóttir, Einarsson, Kristinsson, & Kristjansson, 2006). regulatory requirements, but also performance metrics related to
functionality and use.
The ideal AMC is potent, chemically resistant, mechanically re-
CRF3-2019-0093 Submitted 4/14/2019, Accepted 8/29/2019. Authors Torres sistant, chemically stable, nonabsorbent, innocuous, inexpensive,
Dominguez, Nguyen, and Hunt are with Dept. of Biomedical, Biological & Chemical and easy-to-clean when placed in complex environments (Provder
Engineering, Univ. of Missouri, Columbia, MO 65211, U.S.A. Author Mustapha & Baghdachi, 2007). However, in the pursuit of this ideal, the pri-
is with Food Science Program, Univ. of Missouri, Columbia, MO 65211, U.S.A. mary focus of most AMC development has been on improving
Direct inquiries to authors Hunt and Mustapha (E-mail: hunthk@missouri.edu,
mustaphaa@missouri.edu) the coatings’ antimicrobial properties. This has been detrimental
to the field due to the lack of focus toward developing AMCs


C 2019 Institute of Food Technologists®

doi: 10.1111/1541-4337.12502 Vol. 0, 2019 r Comprehensive Reviews in Food Science and Food Safety 1
Antimicrobial coatings for food contact . . .

that adhere to regulatory standards, which out of necessity include because they cannot be considered as coatings due to their lack of a
their chemical and mechanical stability. An AMC that does not rigid or semi-rigid substrate. Readers interested in the mechanical
adhere to these regulatory limits cannot be applied to real food properties of active and antimicrobial free-standing films for food
applications, even if that coating exhibits most of the ideal an- packaging should consult other published work (Barros-Velazquez,
timicrobial properties. Because AMCs exhibiting all of these ideal 2016; Bastarrachea, Dhawan, & Sablani, 2011; Kuorwel, Cran,
characteristics are not currently available, assessing the degree of Orbell, Buddhadasa, & Bigger, 2015).
compliance with those ideals (most of which are regulated by We also note that the classification given in Table 1 below
laws) would allow us to quantify the progress attained in the field is only one logical grouping; other groupings may be found in
of AMCs for FCS. the literature. For instance, Bastarrachea et al. (2011) classified
This review seeks to present a broad perspective on the progress antimicrobial packaging systems into four different groups based
of development of AMCs, with a particular focus on their under- on how the antimicrobial agent is immobilized or implanted into
explored mechanical properties. This perspective will include dis- the material, namely:
cussions on how the mechanical properties are assessed, what met-
rics must be achieved, how the mechanical properties impact their (i) The antimicrobial substance is directly incorporated into the
usability, and the regulations that impact AMC development and matrix of the substrate
use (Brotzen, 1994). These factors are interrelated and complex, (ii) The antimicrobial agent is released from an inner/outer layer
and although the assessment of mechanical properties for AMCs and migrates across a secondary layer before arriving at the
is accomplished in a similar fashion around the globe, the AMC food matrix
regulatory framework is a country-specific matter. Therefore, this (iii) The antimicrobial agent is released from a coating
portion of the topic is presented in this article for a variety of (iv) The antimicrobial substance is immobilized on top of the
countries (Australia, the European Union [EU], Mexico, and the substrate’s surface (Bastarrachea et al., 2011).
United States) to give the reader a global context, and to allow the
reader to understand the complexity that needs to be considered Although more precise than the classifications presented in this
when developing AMCs for FCS. This review will contribute to document, the categorizations from Bastarrachea et al. (2011) are
the current field of AMCs for FCS by presenting a summary and less useful for discussing regulatory issues, particularly assessments
analysis of the progress in the development of AMCs in relation of antimicrobial agent migration into food (Bastarrachea et al.,
to the global regulatory perspective. It should be noted that this 2011). We suggest that the classifications presented here that sort
review focusses on supported AMCs. Free-standing films, or films antimicrobial agents used on FCS according to their applications
that do not possess substrates or are removed from their substrates, will help the reader frame AMCs in terms of their legal require-
are beyond the scope of this review. ments.
In this classification framework, a food additive is an ingredient
FCS in the Food Processing Industry intentionally added to foods to maintain or improve their safety,
AMCs must withstand decontamination methods for FCS cur- freshness, nutritional value, taste, or appearance (FDA, 2010).
rently in use or intended to be used in the food processing indus- When an antimicrobial substance is intentionally added to a pack-
try because: (i) it is highly risky to rely on one decontamination aging material’s composition or onto its surface, the antimicrobial
method only, (ii) each method has a different range of action and it substance is expected to migrate, partially or completely, into the
is wise to decontaminate the FCS in a range as ample as econom- food, where the preservative effects take place. Because the an-
ically feasible, and (iii) cross-contamination can adopt different timicrobial agent is consumed together with the food product, the
forms, and it is unrealistic to expect that an AMC will prevent all substance is regarded, for this specific group of circumstances, as a
forms of cross-contamination. In this section, AMCs are placed in food additive (Lück, 1997).
the context of decontamination of FCS and the implications for The same is not true for the antimicrobial substances used to
AMCs in terms of decontamination strategies. clean, sanitize, and sterilize surfaces. In this case, the primary pur-
poses of the antimicrobial substances are for controlling foodborne
Overview of FCS pathogen populations, decontaminating the surfaces, and comply-
FCS are surfaces present on equipment, utensils, and containers ing with microbiological occurrence regulations (Miller, 2009).
for the production, processing, and packaging of food. The most Because the ingestion of such substances may present a threat to
common FCS are made of stainless steel, copper, plastic, rubber, consumer health, they must be completely removed with a final
ceramic, glass, and wood (Skåra & Rosnes, 2016). It is impossible rinse treatment, and any antimicrobial substance that remains on
to compile a complete list of FCS because surface types depend on the food is therefore considered a food contaminant (Dunsmore,
the processing facility, the type of process, and the different alloys Twomey, Whittleston, & Morgan, 1981). Food contamination
that make up the process equipment. However, common exam- by antimicrobial substances can be avoided with careful design
ples of such process equipment include conveyors, filler hoppers, of equipment/facilities and with appropriate cleaning/sanitation
slicers, blenders, cutting boards, dishes, cutlery, waxed cardboard, programs (Miller, 2009). For example, research on the mitigation
and food containers (Chen et al., 2009). When FCS are treated of the contamination of food products by antimicrobial substances
with an antimicrobial agent, there are three general intended pur- as a result of FCS sanitation processes has led to the development
poses (see Table 1): of cleaning programs that use natural essential oils as an alterna-
tive to chemically prepared disinfectants (Falcó, Verdeguer, Aznar,
(i) To improve the properties of food packaging
Sánchez, & Randazzo, 2018). However, although essential oils
(ii) To decontaminate the surface
pose less of a health risk, they are still considered contaminants
(iii) To induce antimicrobial properties at the surface.
when they contact food products, because the essential oils affect
It should be noted that free-standing antimicrobial films, mostly the organoleptic characteristics of food, such as flavor and aroma
used for food packaging purposes, are excluded from this review, (Vital et al., 2018).

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Antimicrobial coatings for food contact . . .

Table 1–Classifying the antimicrobial agents used on FCS by their specific applications is useful in discussions of antimicrobial agent migration and
legal requirements.

Antimicrobial
Antimicrobial regulatory
FCS application presence in food classification Example of antimicrobial Example of surfacea
Food packaging Intentionally added Food additive Silver ion (El Arrassi et al., 2017) Bulk food storage containers, paperboard
cartons, jars, and bottles with
antimicrobial action
Ongoing effect from Unintentionally added Food contamination Titanium dioxide (Veerachandra Cutting boards, conveyor belts, and other
the surface or residue K. Yemmireddy & Hung, 2017) food processing equipment with
antimicrobial action
Decontamination of Unintentionally added Food contamination Peracetic acid (Dinu et al., 2010) Countertops, table tops, cutlery,
the surface or residue dishware, cookware, and other
processing equipment
decontaminated by antimicrobial
substances
a For the purposes of this review, free-standing films (films with no substrate) for packaging purposes are excluded in this classification.

Similarly, the unintentional diffusion of antimicrobial substances cross-contamination and the mechanisms involved in the spread
from FCS to food products is also considered contamination. of foodborne pathogens along the food processing chain (see
However, in this case, the migration of the active agent occurs Figure 1 and Table 2). At broiler and slaughter plants, for in-
due to a failure, because the antimicrobial substance is expected stance, microorganisms were found on food products, such as
to remain adhered to the FCS and to exert its action from the carcasses, even before any secondary processing step has occurred
surface upon which it remains. The facile detachment of active (Ho et al., 2004). Depending on the specific steps involved in the
coatings from their substrates and their low durability when sub- process, the bacterial counts on food and FCS vary, but they in-
jected to complex environments are some of the main reasons crease when the process includes evisceration (Wang et al., 2014).
for the scarcity of AMCs observed in commercial applications The tools employed in food processing activities, such as knives,
(Yemmireddy & Hung, 2017). Given this, surface adhesion has table-tops, operators’ gloves, and handlers, are important sources
been a subject of multiple investigations (Bera, Rout, Udayab- of cross-contamination (Ho et al., 2004; Remya, Sunil, Latha, K.,
hanu, & Narayan, 2016; Karbay, Budakoglu, & Zayim, 2015; Lv & Kumar, 2014). The contamination at processing facilities is then
et al., 2018). aggravated by the presence of pathogens resistant to benzylpeni-
As is apparent from Table 1, whether an AMC is applied to cillin, imipenem, and fusidic acid (Sala et al., 2016). Once the
protect the food or the surface dictates whether the antimicrobial food leaves the processing center, it may be further contaminated
substance is considered a food additive (preservative) or a food in transport or in retail stores, and or from contact with workers’
contaminant once the antimicrobial agent reaches the food prod- shoes, aprons, and cutting tools (Kim & Yim, 2017). In some cases,
uct. This difference defines the regulatory stipulations applicable the microbial counts from meat samples are higher at the retail
to the antimicrobial substance. shops than at the abattoir, suggesting that the hygienic procedures
are less stringent when it comes to handling meat outside of in-
dustrial environments (Pradhan et al., 2018). Finally, even though
The need for microbial control on FCS foodborne pathogens are kept under control at processing facilities
Food is among the most basic of human necessities. When and in retail environments, foodborne pathogens may arise within
safety requirements are not met during the food production pro- the consumer’s domestic purlieu because of nonhygienic handling
cess, foodborne illnesses are likely to result (Trachman et al., 2014). of food at home (Kilonzo-Nthenge, Chen, & Godwin, 2008).
Harmful microorganisms, such as bacteria and viruses, and chem- In the instances described above, FCS are always involved, al-
icals, such as toxins and pesticide residues, are the primary causes though the specific nature of the food process influences contami-
of foodborne illness. The improper handling of food has led to nation in complex ways. For example, consider the contamination
approximately 48 million cases of foodborne illness and 3,000 of polyethylene-based FCS, which has an unsteady process of at-
deaths per year in the United States alone (Scallan, Griffin, An- tachment of L. monocytogenes to the FCS (Beltrame et al., 2014).
gulo, Tauxe, & Hoekstra, 2011). Foodborne pathogens are also In another example, differences in surface finishing may not in-
a public health threat, as they can lead to large-scale outbreaks fluence the degree of contamination of stainless steel surfaces, but
with potentially devastating impacts to human health, as well as the proportion of different microbial species on the surface of the
the food industry (Hussain & Dawson, 2013). As an example, a FCS does influence the degree of contamination (Guobjornsdottir,
Salmonella outbreak that occurred in the United States in 2009 Einarsson, & Thorkelsson, 2005). Finally, consider how abrasive
led to the recall of peanut products, ultimately resulting in an es- cleaning treatments applied to rubber surfaces may disinfect the
timated economic loss of $70 million for the producer involved surface, but also increase surface roughness due to wear. This may
(Hussain & Dawson, 2013). More recently, the U.S. Food and degrade the ability of the surface to resist bacterial adhesion over
Drug Administration (FDA) and Centers for Disease Control and time (Santos et al., 2011). Table 1 lists more details on the studies
Prevention (CDC) closed investigations, concluding that between on cross-contamination and foodborne pathogens found on FCS,
March 3, 2019 and May 1, 2019, a Salmonella outbreak originating despite cleaning and sanitation efforts.
at a precut melon packaging facility in Indiana infected 137 peo-
ple in Georgia, Illinois, Indiana, Kentucky, Michigan, Missouri,
North Carolina, and Ohio (CDC, 2019). Current FCS cleaning practices
Due to their potential to cause large-scale public health The primary purpose of cleaning practices is to reduce cross-
and economic threats, the occurrence of foodborne pathogens contamination in foodstuffs. As can be observed in Table 2, specific
in food is subject to intense research, especially on tracing decontamination methods cover varying ranges of contamination,


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Antimicrobial coatings for food contact . . .

Food Harvesting Handling and Storage Processing and Distribution and Market Consumption
• Agricultural • Bacterial Packaging • Bacterial growth during • Contact between
chemicals contamination from • Bacterial storage raw and
(pesticides, fouled process contamination from • Contact between raw and processed food
herbicides, equipment fouled process processed food • Pests (insects,
fungicides, • Bacterial growth equipment surfaces • Cross-contamination of rodents, etc.)
fertilizers, etc.) during storage • Bacterial growth foods with allergy inducing • Improper food
• Crop infestation • Equipment during storage foods (e.g., peanuts, containers (e.g.
(disease, maintenance • Contact between raw shellfish, milk, etc.) non-reusable
parasites, etc.) substances (e.g. and processed food • Cross-contamination from containers)
• Dirt, husks, and equipment oil) • Cross-contamination utensils (knives, cutting • Improper storage
other organic • Inadequate waste of foods with allergy boards, wash cloths, etc.) conditions (e.g.,
residuals
control inducing foods (e.g., • Improper storage conditions humidity,
• Improper peanuts, shellfish, (e.g. humidity, temperature) temperature)
decontamination milk, etc.) • Migration of contaminants • Inadequate waste
(removal of food • Equipment from storage materials control
harvesting maintenance • Personal hygiene (from • Migration of
contaminants) substances (e.g. clothing, hair, unwashed contaminants from
• Improper storage equipment oil) hands, etc.) storage materials
conditions (e.g., • Inadequate waste • Pests (insects, rodents, etc.)
humidity, temperature) control • Pest control agents
• Migration of • Migration of • Petrol and diesel fumes from
contaminants from contaminants from transport
storage materials storage materials • Residual kitchen cleaning
• Pests (insects, • Pests (insects, agents
rodents, etc.) rodents, etc.)

Figure 1–Steps during food processing and where contamination might occur from various sources.

Table 2–Recent studies of cases where foodborne pathogens have been found on food contact surfaces.

Facility/surface/equipment Pathogen/indicator Occurrence Main testa Reference


Broiler slaughter plant E. coli and other coliforms 104 to 106 CFU/cm2 Occurrence on surface Ho et al. (2004)
Fish and shrimp processing Pseudomonas and 27% to 66% of the Occurrence in situ and Guobjornsdottir et al. (2005)
plant Aeromonas samples were positive adhesion ex situ
Domestic refrigerators Listeria and Not detected to 8.39 log Occurrence on surface Kilonzo-Nthenge et al. (2008)
Enterobacteriaceae CFU per sample
Dairy, fish, and meat facilities L. monocytogenes 15% of 258 samples Occurrence on surface Kovacevic, McIntyre,
positive Henderson, and Kosatsky
(2012)
Table tops and knives at meat Listeria 3% of 100 samples Occurrence on surface Remya et al. (2014)
processing facilities positive
Rubber and silicone surfaces Streptococcus agalactiae Reduction from 4.5 to Hydrophobicity and Santos et al. (2011)
of milk machine 2.5 CFU/cm2 after bacteria detachment
treatment
Chicken slaughter line Salmonella 23 isolates from 104 Occurrence on surface Wang et al. (2014)
samples
Polyethylene cutting boards L. monocytogenes 6.11 to 6.92 log CFU/cm2 Microbial adherence to Beltrame et al. (2014)
surface
Pig slaughterhouse L. monocytogenes 25.8% of 97 samples Occurrence on surface Sala et al. (2016)
positive
Retail outlets: raw meat, Salmonella and L. From nondetectable to Occurrence on surface Losito et al. (2017)
fishery products, deli, monocytogenes >500 CFU/cm2
pastry, and dairy products
Meat processing plants Aerobic plate count 23.5% of the samples Occurrence on surface Kim and Yim (2017)
equipment were positive
Retail meat shops and Coliforms and S. aureus 1.98 to 5.69 log CFU/cm2 Occurrence on surfaces Pradhan et al. (2018)
abattoirs
a Occurrence on surfaces was determined by swabbing unless stated otherwise.

namely, there is no single decontamination method capable of and other chemical contaminants (FDA, 2018b). There are differ-
covering the entire range of decontamination levels. ent degrees of decontamination: cleaning, sanitization, and steril-
Decontamination can be understood as a group of actions ex- ization. Cleaning is the removal of visible fouling (Li et al., 2014).
erted to partially or completely eliminate harmful substances from Sanitization, also known as disinfection, denotes the reduction of
FCS by means of cleaning, sanitizing, and/or sterilizing such sur- the number of microorganisms to a safe level. Finally, sterilization
faces (Miller, 2009). The harmful substances may be pathogens can be interpreted as the complete destruction of microorganisms
(bacteria, viruses, and parasites), pesticides, natural toxins, metals, (Miller, 2009). The different approaches to the decontamination

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of FCS can be classified into five methods: thermal, mechani- Table 3–Classification of disinfection methods by decontamination level.
cal, chemical, physical (Otto et al., 2011), and biological (Dinu
Decontamination level (increasing from
et al., 2010). It should be noted that this review focuses on the left-to-right)
removal or inactivation of microorganisms only, although clean- Sanitizing
ing procedures in general may focus on the elimination of other Cleaning (disinfection) Sterilizing
contaminants too. Biological √
Decontamination via cleaning methods. Current investigations Chitosan, Lactobacillus
bacteriocins, and phages √ √
on FCS cleaning methods focus primarily on alternatives to those Detergents with enzymes
methods that rely on the use of water and/or hazardous disinfec- Chemical √
tants. Widely found in industrial food processing facilities, clean- Detergents √
in-place (CIP) systems deactivate microorganisms on equipment Ethylene oxide √
Hydrogen peroxide √
surfaces using rinse cycles and aqueous solutions of cleaners. For Ozone and chlorine dioxide √ √
instance, Clostridium perfringens, adhered to stainless steel, was de- Peracetic acid, iodine
activated using different CIP regimes by adding sodium hydroxide compounds, and chlorine
compounds
(NaOH) as an active cleaning agent (Alzubeidi, Udompijitkul, Mechanical √ √
Talukdar, & Sarker, 2018). However, CIP systems are not always Brushing and water jet √
effective. For instance, Khamisse, Firmesse, Christieans, Chassaing, Rinsing
Physical √ √
and Carpentier (2012) found that an industrial cleaning and disin- Gamma rays √ √
fection system at a ricotta facility did not significantly reduce the Dry ice, ice pigging, and
total cell counts from stainless steel and PVC surfaces, although ultrasound √ √
Gas plasma √
the surfaces appear visually clean after the cleaning procedure UV light
(Khamisse et al., 2012). Furthermore, some cleaning agents accel- Thermal √
erate the deterioration of rubber and silicon surfaces, such as those Autoclave √ √
Hot water √ √ √
encountered in milking machines (Santos et al., 2011). Perhaps Steam
more importantly, there are a large number of food commodi-
ties (cereals, dry seasonings, infant formulas, peanut butter, and
so on) that must be handled in low-moisture environments to
control Salmonella (NAMI, 2015) that do not permit the use of enumerating the effects of the surface properties and food prod-
conventional CIP systems based on water and cleaning agents. ucts’ components on the effectiveness of mechanical–chemical
Therefore, alternative methods, such as ice blasting, UV irradi- methods. For example, the application of aqueous NaOH on
ation, and ultrasound, have been tested on dairy surfaces, ceramic stainless steel plates followed by rinsing with an aqueous chlo-
tiles, and bamboo cutting boards, with results comparable to those rine compound was proposed as an alternative disinfecting process
obtained by radiation, vapor blasting, and brushing (Witte et al., (Jiménez-Pichardo et al., 2016). In another study, Park and Kang
2017). For example, the use of UV light has been evaluated to (2017) found that the effectiveness of chlorine dioxide gas was
reduce Salmonella populations on different FCS (Lim & Harri- negatively correlated to the contact angle observed on FCS made
son, 2016). In some instances, these alternative methods are paired of silicon, TeflonR
, rubber, stainless steel, and PVC, and that the
with conventional cleaning agents when the adherence strength of average roughness had a less pronounced effect on the gas’ antimi-
bacterial biofilms to the FCS is so great that a combination of con- crobial activity (Park & Kang, 2017).
ventional cleaning agents and an alternative, such as ultrasound, is Physical methods of sanitization, listed in Table 6, such as UV
more effective than using a conventional method only (Fink, Oder, and white light irradiation or plasma treatment, have received sig-
Stražar, & Filip, 2017). For example, Kuda et al. (2011) found that nificant attention in research studies. For instance, a 2-s treatment
removing dried egg plasters from the FCS before washing the completely deactivated viruses on surfaces and in aqueous sus-
FCS via CIP increased the cleaning efficacy (Kuda et al., 2011). pensions. However, the addition of a small quantity of organic
A standing issue is the proper disposure of the waste water con- matter simulant to the surface or to the suspensions reduced the
taining spent cleaning agents. Therefore, environmentally friendly effectiveness of the treatment (Jean, Morales-Rayas, Anoman, &
enzymes have been studied as substitutes for chemical decontam- Lamhoujeb, 2011). The results suggest that UV light is more effec-
ination methods, but with limited effectiveness (Lequette, Boels, tive when inactivating microorganisms placed on abiotic surfaces
Clarisse, & Faille, 2010). than on food surfaces (Haughton et al., 2012; Sommers & Sheen,
Decontamination via sanitizing methods. As a more effective 2015). These findings are in agreement with the accepted fact
method of decontamination, sanitizing or disinfecting can be ac- that UV light has low penetrating power into food matrices and
complished by mechanical, physical, chemical, thermal, and/or surfaces (Jay, Loessner, & Golden, 2005). Comparable results (see
biological means (Table 3 to 8). Mechanical and chemical meth- Table 6) to those obtained with UV light irradiation can be ob-
ods can, in fact, be regarded as a single disinfection method because tained with nonthermal plasmas using air (Niemira, Boyd, & Sites,
rinsing (see Table 3) and detergents or disinfectants (see Table 4) 2014) and nitrogen (Dasan et al., 2016) as feed gases. Both meth-
are synergistically employed together in practice. The effectiveness ods, UV light irradiation and nonthermal plasma, are convenient
of electrolytic solutions (Guentzel, Liang Lam, Callan, Emmons, methods when the presence of moisture in the processing envi-
& Dunham, 2008), strong bases or acids (Furukawa, Akiyoshi, Ko- ronment is a concern or when the FCS cannot withstand high
moriya, Ogihara, & Morinaga, 2010), and the effects of detergent temperatures.
concentration, water temperature, and surface material have been When the presence of water and high temperatures are not lim-
extensively investigated (Reynisson, Guobjornsdottir, Marteins- iting constraints, thermal methods of disinfection are acceptable
son, & Hreggviosson, 2009). Recent research has focused on de- (see Table 7). Steam is an inexpensive sanitizing agent that is read-
veloping combinations of less toxic sanitizing solutions, as well as ily available in most industrial food processing plants (McCann,


C 2019 Institute of Food Technologists® Vol. 0, 2019 r Comprehensive Reviews in Food Science and Food Safety 5
Antimicrobial coatings for food contact . . .

Table 4–Selection of publications on mechanical decontamination of food contact surfaces.

Decontamination Decontamination Intended


Surface Microbe level method Treatment result Variables tested application Reference
Stainless steel E. coli O26, P. Cleaning and Rinsing with water The bactericidal The effect of Food-related Kuda, Yano, and
dishes aerugi- sanitation and application effect rinsing before environ- Kuda (2008)
nosa, and S. of disappeared the application ments
aureus benzalkonium because of food sanitizer
chloride residues
Stainless steel and Not identified Cleaning Rinsing regime 0.8 to 1.5 log CFU Effectiveness of an Cutting at beef Khamisse et al.
PVC reductions actual cleaning processing (2012)
and disinfection facilities
regime
Wood, triclosan- Salmonella Cleaning and No treatment, From 1.90 to 2.80 Effectiveness of Food contact Soares et al.
treated plastic, Enteritidis sanitation rinsing, and log to each treatment surfaces, in (2012)
glass, and application of undetectable on different general
stainless steel sanitizers materials
cutting boards

Sheridan, McDowell, & Blair, 2006). It has been shown that it surfaces. These FCS may modify, to some extent, the quality of
takes less than a minute to inactivate foodborne pathogens from the final food product. The limits of changes to a food product’s
FCS made of stainless steel or PVC using steam at 75 to 85 °C quality due to its contact with surfaces is something that neither
(Park & Kang, 2013). food producers nor consumers can fairly set or predict, because
Prey–predator relationships and different abilities to compete both consumers and producers have competing economic interests
for limited resources have been suggested as the working princi- (Boulding, 1945) that are more related to changes in market prices
ples of biological methods to disinfect FCS (see Table 8). Tomat, than food safety. Therefore, a third factor, a central government
Quiberoni, Mercanti, and Balagué (2014) achieved different de- and/or a regulator, must enter the scene to set strict requirements
grees of decontamination on FCS by means of phages inoc- (Cooper & Tice, 2001) that not only ensures consumers’ safety,
ulated into populations of foodborne microorganisms (Tomat, but also allows producers the flexibility to develop profitable and
Quiberoni, Mercanti, & Balagué, 2014), whereas Gomes, Piard, safe food processes.
Briandet, and Mergulhão (2017) reported that colonization and A central government is able to establish statutory requirements
biofilm formation on FCS by Escherichia coli is retarded by pur- through a congress or a group of peoples’ representatives. Ap-
posely added Pseudomonas grimontii. In both cases, further investi- pointed by a central government, regulators are then autonomous
gations are needed to assess these biological methods’ compatibil- entities that are granted authority to stipulate regulatory require-
ity with commonly used practices of sanitizing FCS, as chemical, ments. Both regulatory and statutory requirements form the legal
physical, mechanical, and thermal disinfection methods do not framework that oversee the use of AMCs in FCS. Globally, the
discriminate among microbial species. Because of this, the effec- Food and Agriculture Organization of the United Nations (FAO)
tiveness of biological methods might be diminished when used in and the World Health Organization (WHO) are recognized food
combination with other disinfection approaches, because the bio- safety regulators. These organizations produce international food
logical methods described above rely on the existence of specific standards and help to regulate food production, including shipment
living microbial strains. and intake, among countries (FAO, 2018). Among countries, reg-
Decontamination via sterilizing methods. Sterilization of FCS ulations and statutory laws vary greatly (see Table 9). For instance,
is routinely accomplished by autoclaving, gamma ray radiation, in Mexico and the United States, the rules and laws related to
or washing with hydrogen peroxide or concentrated solutions of AMCs for FCS are established by different but complimentary
strong acids or bases (Jay et al., 2005). However, plasma treat- institutions; this is not the case in Australia. The antimicrobial
ment has been explored as an alternative of those routine meth- component of any existing or novel AMC must be listed in at least
ods. Deilmann, Halfmann, Bibinov, Wunderlich, and Awakowicz one of the following, depending on which jurisdiction the FCS is
(2008) reported sterilization of PET bottles using plasma from a beholden to:
mixture of nitrogen, oxygen, and hydrogen, with results compa-
rable to that obtained by hydrogen peroxide washing. Sen and r Australia: ANZFS Code, Chapter 1, part 1.3, Standard 1.3.1;
Mutlu (2012) reported water vapor as the most effective gas for Schedule 15 and Schedule 20.
sterilization purposes using glow discharge plasma. In both cases, r EU: Regulation (EU) No. 1130/2011, Regulation (EC) No.
the inherent nature of the plasma sterilization process required the 10/2011, and Regulation (EC) No. 450/2009.
use of a chamber or reactor to accomplish the plasma formation r Mexico: Codex Alimentarius.
described above. r USA: Code of Federal Regulations, Title 21, part 182, and
In this context, AMCs can be listed among the chemical meth- U.S. Code, Title 21, Chapter 9, Subchapter IV, section 346a.
ods for cleaning and sanitizing FCS and may be used simultane-
ously, depending on the specific application, with other chemical, In the same manner, the AMC, as an integral part of the FCS,
mechanical, physical, or thermal methods. In such cases, AMCs must comply with at least the following:
must be able to synergistically interact with different cleaning r Australia: ANZFS Code, Chapter 3, Part 3.2, Standard 3.2.3
practices. r EU: Regulation (EC) No. 1935/2004 and Regulation (EC)
No. 450/2009.
Legal Framework Pertaining to FCS r Mexico: Mexican Official Standard, NOM-251-SSA1-2009.
The process by which food is harvested, processed, and deliv- r USA: Code of Federal Regulations, title 21, subchapter B,
ered to the consumer involves unavoidable contact with multiple part 110.

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Table 5–Selection of chemical decontamination research studies of food contact surfaces.

Decontamination Decontamination Intended


Surface Microbe level method Treatment result Variables tested application Reference

C 2019 Institute of Food Technologists®


Food service areas E. faecalis, E. coli, Sanitation Hypochlorous acid 79% to 100% Concentration of sanitizer Food contact Guentzel et al. (2008)
S. aureus, L. reduction of surfaces
monocytogenes, and microbial growth
S. Typhimurium
Plastic and stainless steel Gammaproteobacteria Sanitation Washing protocol with 99.9% of bacterial Water, temperature, and Fish processing Reynisson et al. (2009)
coupons detergents removal detergent plant
Antimicrobial coatings for food contact . . .

concentration
Stainless steel, wood, and Alicyclobacillus Sanitation Chlorine dioxide and Reductions from 0 to Time of treatment and Food handling and Friedrich,
rubber conveyor sodium hypochlorite 4.5 log CFU/ concentration of processing Goodrich-Schneider,
material coupon sanitizers surfaces Parish, and Danyluk,
(2009)
Stainless steel plates S. aureus and E. coli Cleaning and Cleaning in place agents Reduction from 107 to Different cleaning agents Food processing Furukawa et al. (2010)
sanitation containing NaOH, KOH, 106 CFU/cm2 and food additives plants
nitric acid, phosphoric
acid, and sodium
hypochlorite
Glass dishes S. Typhimurium and Cleaning and Benzalkonium chloride The bactericidal effect The effect of the presence Food-related Kuda et al. (2011)
S. aureus sanitation and alkyldiaminoethyl- of sanitizers of dried and adhered environments
glycine disappeared in the egg compounds on
hydrochloride presence of yolk treatment efficacy
and whole egg
Stainless steel and PP S. aureus Sanitation Peracetic acid and sodium Cell detachment The efficacy of the Food service da Silva Meira, de
hypochlorite around 3 log CFU/ sanitizers surfaces Medeiros Barbosa,
cm2 Alves Aguiar Athayde,
de Siqueira-Júnior, and
de Souza (2012)
Rubber and silicon S. agalactiae Cleaning and 1.5% sodium hydroxide 2.5 to 4.5 CFU/cm2 The relation between Milking machine Santos et al. (2011)
surfaces sanitation coupon adhesion and contact surface
angle
Stainless steel coupons C. perfringens Sanitation Ethanol, iodophore, 0.33 to 2.70 log Treatment time, Food industry Udompijitkul, Alnoman,
quaternary ammonium reductions disinfectant, and environments Paredes-Sabja, and
compounds, and Decon microbial species Sarker (2013)
Spore
(Continued)

Vol. 0, 2019 r Comprehensive Reviews in Food Science and Food Safety 7


Table 5–Continued.

Decontamination Decontamination Intended


Surface Microbe level method Treatment result Variables tested application Reference
PE and ceramic dishes B. cereus spores, Sanitation Benzalkonium chloride Reductions of around The effect remnants of Food industry Li, Kuda, and Yano (2014)
P. aeruginosa, S. and alkyldiaminoethyl- 3 and 4 log food on efficacy of environments
aureus, and E. coli glycine CFU/dish were treatment at different
O26 hydrochloride obtained concentrations
Buna and PVC chips Cronobacter Sanitation Sodium hypochlorite Reduction of 3 log Surface material, Conveyor belt Song, Chon, Kim, Park,
concentration of and Seo (2014)
sanitizer, and pH
Antimicrobial coatings for food contact . . .

PE cutting boards L. monocytogenes Sanitation Organic acids, peracetic For all contact times The efficacy of the Surfaces of cutting Beltrame et al. (2014)
acid, sodium tested, biofilm sanitizers on used and boards
hypochlorite, and formation was new cutting boards
chlorhexidine avoided
Rubber, glass, stainless Human norovirus Sanitation Ethanol, sodium Reductions of <1 log Concentration of Surfaces in Liu et al. (2015)
steel, PVC, wood, and hypochlorite, sodium sanitizers and different general
ceramic tile disks metasilicate, and surface materials
quaternary compounds
Stainless steel coupons E. faecalis and Cleaning and Several detergents and Reductions of below Detergent and sanitizer Ricotta processing da Silva Fernandes,
Enterococcus faecium sanitation sanitizers 0.4 log CFU/cm2 combinations facility Kabuki, and Kuaye

8 Comprehensive Reviews in Food Science and Food Safety r Vol. 0, 2019


(2015)
Stainless steel coupons P. aeruginosa, E. Cleaning and Alkaline electrolyzed Reduction of 3.20 to Concentration of Dairy industry Jiménez-Pichardo et al.
faecalis, and sanitation water and neutral 3.90 log CFU sanitizers, time, and (2016)
Micrococcus luteus electrolyzed water temperature
Silicon, Teflon, rubber, S. Typhimurium, E. coli Sanitation Gaseous chlorine dioxide 5.91 to 6.81 log CFU Time of treatment and Food contact Park and Kang (2017)
stainless steel, and PVC O157:H7, and L. reduction surface material surfaces
monocytogenes
Biofilms on dairy surfaces Bacillus subtilis, Sanitation Iodophore, sodium 550 to 650 ppm were Microbial biofilm Dairy niches Makwana, Ram Grover,
Salmonella, hypochlorite, and required eradicating and Kumar (2018)
Pseudomonas, benzalkonium chloride concentration and
Listeria, and E. coli effectiveness minimum inhibitory
concentration
Stainless steel, HDPE, L. monocytogenes Sanitation Phosphoric acid, Biofilm formation was Temperature and Fishery facility Dhowlaghar et al. (2018)
Buna N, and dodecylbenzene lower in Buna than concentration of catfish surfaces
polyurethane sulfonic acid, in the other mucus on FCS


quaternary ammonium materials
compounds, hydrogen
peroxide, peracetic
acid, octanoic acid, and
sodium hypochloride

C 2019 Institute of Food Technologists®



Table 6–Selection of physical decontamination investigations of different food contact surfaces.

Decontamination Decontamination Intended


Surface Microbe level method Treatment result Variables tested application Reference
PET bottles Bacillus atrophaeus and Sterilization Low-pressure microwave Reduction of 105 and Treatment time and Aseptic filling of Deilmann et al. (2008)
Aspergillus niger plasma 104 CFU plasma reactor design beverages
Stainless steel knife L. monocytogenes and E. Sanitation White light Total deactivation of Time and type of meat Food contact Rajkovic et al. (2010)
coli O157:H7 6.5 log CFU/side of product surfaces

C 2019 Institute of Food Technologists®


knife
Stainless steel and PVC Murine norovirus Sanitation UV light 3 to 5 log CFU Timing, distance of Drinking water or Jean et al. (2011)
disks (MNV-1) and irradiation, and food-handling
hepatitis A virus presence of bovine surfaces
(HAV) serum
Stainless steel and PVC Campylobacter jejuni Sanitation UV light No microorganisms Treatment time and Chicken contact Haughton et al. (2012)
Antimicrobial coatings for food contact . . .

coupons 1136 DF were recovered distance of irradiation surfaces


after treatment
Stainless steel and PE E. coli K12 Sterilization Nonthermal plasma 7 log CFU reduction Different plasma Food contact Sen and Mutlu (2012)
coupons parameters surfaces
Glass slides Salmonella biofilms Sanitation Cold plasma Reduction up to 2.13 Time of treatment and Conveyor belt Niemira et al. (2014)
log CFU/mL distance from plasma
emitter
HDPE, PE, and stainless Yersinia pestis Sanitation UV light and freezing >6 log was eliminated Power of irradiation, Food contact Sommers and Sheen
steel chips at 1 J/cm2 surface material, and surfaces in (2015)
effect of freezing general
Plastic jerry cans Coliforms Cleaning Detergents 40% to 96% Occurrence after cleaning Milk handling Wafula, Matofari, Nduko,
microbial load of surface and Lamuka (2016)
reductions
Stainless steel, HDPE, Salmonella Cleaning Rinsing and detergents Reduction of 1.91 to Occurrence on surface Tomato handling Lim and Harrison (2016)
PVC, and waxed 3.50 log facility
cardboard CFU/coupon
Stainless steel, silicone, S. epidermidis and E. coli Sanitation Non-thermal plasma Reduction of 2.95 to Effectiveness of different General surfaces Dasan et al. (2016)
and PET 4.43 log CFU/mL sanitizers
Polyurethane conveyor B. cereus Cleaning Ultrasound and cleansers Reduction from 0.47 Effectiveness of the Bakery facility Fink et al. (2017)
belts to 0.205 of biofilm’s combination of both
optical density methods
Ceramic tiles, and Micrococcus roseus R4 Cleaning and Dry ice blasting Approximately 90% CO2 quantity, pressure, Food production Witte et al. (2017)
materials of smear sanitizing removal of bacteria pellet size, and equipment
robots bacterial concentration
Stainless steel dishes Saccharomyces Sanitation UV light and sanitizers Reductions from 6 to Effects of food residues on Processed food Shikano, Kuda, Takahashi,
cerevisiae and De- <2 and 3 to 4 log the survival rates industries and Kimura (2017)
baryomyces CFU/dish,
hansenii
Knifes Enterobacteriaceae, S. Sanitation Ultrasound, detergents, Migration rate of The method was Cattle slaughter Brasil et al. (2017)
aureus, molds, and and chlorinated water residues: 1.61 It compared to a process
yeasts should be conventional method
mg/L.min

Vol. 0, 2019 r Comprehensive Reviews in Food Science and Food Safety 9


Antimicrobial coatings for food contact . . .

Table 7–Selection of thermal decontamination investigations of food contact surfaces.

Decontamination Decontamination Variables Intended


Surface Microbe level method Treatment result tested application Reference
Stainless steel and E. coliO157:H7, Sanitation Steam 1.78 to 3.0 log Stream tem- Steam pas- Park and Kang
PVC coupons S. Typhimurium, CFU/coupon perature teurization (2013)
and reductions and
L. monocytogenes treatment
biofilms timing
Peanut processing Salmonella Sanitation Hot oil and 60% <0.16 log Effectiveness Peanut butter Grasso, Grove,
equipment isopropanol ± CFU/cm2 of cleaning pilot plant Halik, Arritt,
quaternary and and Keller
ammonium sanitation (2015)
compounds procedure
Wooden boards Listeria innocua Sanitation Steam 2 log CFU Different tem- Cheese manu- Imhof,
reduction peratures facturing Schwendi-
mann, and
Riva
Scettrini
(2017)

Table 8–Selection of biological decontamination studies of food contact surfaces.

Decontamination Decontamination Intended


Surface Microbe level method Treatment result Variables tested application Reference
Stainless steel Pseudomonas Cleaning Polysaccharidases Serine proteases Seven enzymes tested Clean-in-place Lequette et al.
slides fluorescens and proteolytic removed Bacillus to remove biofilms for food (2010)
and B. cereus enzymes and from 16 bacterial industries
polysaccharidases species
removed P.
fluorescens biofilms
more efficiently
Glass slides E. coli Sanitation Myoviridae phages Viable cell Three different Food Tomat et al.
and concentration phages as a cocktail processing (2014)
stainless decreases from 1.2 or on surfaces surfaces
steel chips to 5.4 log CFU/mL
Bare and E. coli Sanitation Competitive The biovolume of E. Time of growth and Food contact Gomes et al.
coated with microbe, coli was lower in surface coating surfaces (2017)
diamond- Pseudomonas presence of P.
like carbon grimon- grimontii 13A10
stainless tii 13A10
steel
coupons
Stainless steel S. aureus Sanitation Oregano essential Decrease of ≥2 log Time of treatment and Surfaces of Rodrigues et al.
coupons oil CFU/cm2 concentration of stainless (2018)
essential oil steel
Stainless steel E. coli O157:H7, Sanitation Thyme and tea Decrease of biofilm Minimum Food industry Sadekuzzaman,
and rubber L. monocyto- tree oils cells up to 3.5 log concentration for surfaces Mizan, Kim,
genes, CFU/cm2 biofilm eradication Yang, and Ha
and Salmonella (2018)

Despite these variations, the intended goal of all such regulations food statutory and regulatory requirements. Therefore, from a le-
is to guarantee safe food for consumers through prevention, moni- gal perspective, the antimicrobial agent must be regarded not as
toring, and enforcement. Correctly identifying the regulatory and a component of the coating, but as a food component (Lück,
statutory laws for a given scenario is a necessary first step toward 1997). The other two modes of control, risk assessment and good
the commercial adoption of AMCs for FCS. Understanding this manufacturing practices, are defined by governmental institutions
framework can allow researchers to appropriately design AMCs or by organizations, committees, and institutions whose technical
that, from the beginning, meet the requirements, thus simplifying experience and expertise lend them a certain level of authority
the process of translation outside the laboratory. Unfortunately, within the industry; that is, risk assessment and good manufac-
the requirements are often so complex that many researchers do turing practices are self-regulations. Good practices for equipment
not take these into consideration when designing new AMCs. surfaces (Chen et al., 2009) or good practices for equipment de-
Here, we present an overview of the legal framework that governs sign (NAMI, 2015) for food processing plants are examples of
AMCs for FCSs both globally and in our specific case studies of good practices relating to FCS.
the United States, Mexico, the EU, and Australia. Table 10 and 11 give a general view of the legal requirements
expected to be met by FCS and antimicrobial substances, respec-
Legal requirements for AMCs tively. These requirements, intended for national and regional
Globally, FCS are controlled in four different ways: statutory applications, are nonnegotiable and enforceable. Thus, descrip-
requirements, regulatory requirements, risk assessment, and good tions of laws should be both general enough to facilitate their
manufacturing practices (Assent, 2016). Because antimicrobial practical use and sufficiently specific to prevent voids in what is
agents adhered to FCS will migrate from the coatings’ surfaces and is not allowed regarding FCS and AMCs. Although many of
to food products and become a constituent of the food prod- the mechanical requirements for FCS listed in Table 10 are qual-
uct (a contaminant), the antimicrobial substance is regulated by itative guidelines, such as easy to clean, smooth, nonabsorbent,

10 Comprehensive Reviews in Food Science and Food Safety r Vol. 0, 2019 


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Antimicrobial coatings for food contact . . .

Table 9–Legal classifications of antimicrobial agents and governing bodies in various regions of the world.

Antimicrobial legal Mexican


FCS application classification Australian authority EU authority authority U.S. authority
Food packaging Food additive Territories and state authorities, Food European Food Safety Cofeprisb Food and Drug
Standards Australia New Zealande Authority Administration
Ongoing effect Food contamination Territories and state authorities, European Food Safety Cofeprisb Environmental
from the surface or residue Department of Agriculture and Authority Protection
Water Resourcesa , Food Standards Agency
Australia New Zealande
Decontamination Food contamination Territories and state authorities, European Food Safety Secretarı́a de Environmental
of the surface or residue Australian Pesticides and Authority Saludc Protection
Veterinary Medicines Authority, Agencyd
Food Standards Australia New
Zealande
a For imported food.
b Federal Commission for the Protection Against Sanitary Risk. Decentralized regulator supervised by the federal Secretariat of Health.
c Secretariat of Health.
d Except when the antimicrobial is used to disinfect food packaging materials, in which case, jurisdiction belongs to the Food and Drug Administration.
e Develops and administers the Food Standards Code, does not have enforcement responsibilities.

Table 10–List of legal mechanical requirements for FCS by country or region and the corresponding regulation that establishes such requirements.a

Country/region Legal requirement Mechanical requirement Comments Reference


Australia ANZFS Code, Chapter Made of innocuous materials. Easy to clean Chapter 3 applies to Australia Food Standards
3, Part 3.2, and to sanitize if needed. Incapable of only, while the rest of the Australia New
Standard 3.2.3. absorbing soil and water. Standard is applicable in New Zealand (2016)
Zealand as well. State-level
regulations also apply.
EU Regulation (EC) No. Does not transfer components to food at Provides the guidelines for European Parliament
1935/2004 harmful levels. Does not alter food quality. harmlessness for all food (2004)
contact surfaces.
Regulation (EC) No. Active and intelligent materials exempted Applies to active and intelligent European Parliament
450/2009 from the rule that prohibits releasing of materials that absorb or (2009)
substances into food. release compounds to or from
the food or the surroundings.
Mexico Rules for innocuous Rules for food packaging. Describes the chemical and Presidencia de la
control of products physical characteristics food República, 1999
and services, title packaging must meet.
27
Mexican Official Must be smooth, washable, and crack free. The standard is mandatory Secretarı́a de Salud
Standard, NOM- Must resist effective washing and across all Mexican territory (2010)
251-SSA1-2009 disinfection. for food, beverages, and food
supplements production
processes.
USA Code of Federal Food process equipment manufactured to The FDA establishes sanitation U.S. Congress (2011a)
Regulations, title allow its disassembly for cleaning and requirements and inspects
21, subchapter B, sanitizing. Rough finishes are not allowed food processors (all food
part 110. Accumulation of food, debris, and water excluding meat, poultry, and
must be prevented. Must be able to resist egg products).
standard cleaning chemicals.
a The requirement statements have been paraphrased to reduce wording size.

and resistant to chemical attack, special attention should be paid For Mexico, the Rules for Innocuous Control of Products
to European Regulation (EC) No. 1935/2004 and Regulation and Services makes reference to the WHO’s Codex Alimenta-
(EC) No. 450/2009, because these documents clearly separate the rius (FAO, 2018) as the official list of approved antimicrobial sub-
difference in requirements between protective coatings for FCS stances and their limits in food applications. For the United States,
and active coatings for FCS, which is not the case for Australian, several lists exist. However, they can be classified into two main
Mexican, and American laws. groups: those for food additives (U.S. Congress, 1999) and those
On the other hand, Table 11 lists legal requirements with large for chemical pesticides (U.S. Congress, 2015).
amounts of quantitative content. For Australia, approved antimi-
crobial substances and their dose limits are given by the Australia Legal compliance
New Zealand Food Authority (Australia New Zealand Food Au- Compliance to legal requirements must be demonstrated for
thority, 2016). For the EU, three main lists are available: both the surface and the antimicrobial substance to authorities,
regulatory bodies, or third-party authorized agents. Legal com-
pliance is demonstrated by documented evidence collected by an
(i) Regulation (EU) No. 1130/2011, which lists approved an- authority’s agents or its authorized representatives during site vis-
timicrobial substances and their maximum levels in food its, and/or submission of required documentation or applications
(European Commission, 2011b) (Australian Government, 2003; European Parliament, 2004; Presi-
(ii) Regulation (EC) No. 10/2011, listing polymers for coatings dencia de la República, 1999; U.S. Congress, 2011a). The specific
of cans for food products aspects of compliance of FCS and AMC regulations are discussed
(iii) Regulation (EC) No. 450/2009, which lists the require- in the following sections.
ments to consider a material as an intelligent component of Legal compliance of the FCS. All the legal requirements per-
food packaging. taining to FCS characteristics emphasize the surfaces’ ability to


C 2019 Institute of Food Technologists® Vol. 0, 2019 r Comprehensive Reviews in Food Science and Food Safety 11
Antimicrobial coatings for food contact . . .

Table 11–List of legal requirements for antimicrobials for food applications by country or region and the requirements’ corresponding regulation.a

Country/region Legal requirement Scope/Content Comments Reference


Australia ANZFS Code, Chapter Substances permitted as food The considered antimicrobial substances Australia New
1, Part 1.3, additives for food purposes are: sorbic acid, Zealand Food
Standard 1.3.1; benzoic acid, sodium, potassium, Authority (2016)
Schedule 15 calcium benzoates, sulfur dioxide,
among others.
Australian Total Diet Evaluation of the intake or Lists chemicals, dietary exposure, risk FSANZ (2016)
Study dietary exposure to food management, and qualifiers (food
contaminants in Australia tested).
ANZFS Schedule 20 Maximum residue limits in Lists the maximum residue limits of Australian Pesticides
foodstuff agricultural or veterinary chemical and Veterinary
residue that is legally allowed in a food Medicines
product. Authority (2018)
EU Regulation (EC) No. Materials allowed for food Indicates how to manage active and European Parliament
1935/2004 contact intelligent materials not inert by (2004)
design. It also establishes the safety
assessments used to manufacture FCS.
Regulation (EC) No. Polymers and their articles for Regulates the composition of the European
10/2011 food contact purposes polymers permitted as FCS material of Commission,
construction. (2011a)
Regulation (EC) No. Active and intelligent This regulation does not apply to the European Parliament
450/2009 materials food contact materials considered in (2009)
Regulation (EC) No. 1935/2004
Regulation (EU) No. Substances approved for food The considered antimicrobial substances European
1130/2011 applications as additives for food purposes are: sorbic acid, Commission,
sulfur dioxide, sodium benzoate, (2011b)
among others.
Register of substances Lists more than 40 substances Activated carbon, bentonite, silicon European Parliament
under Regulation with potential use as active dioxide, sodium hydroxide, talc, and so (2009)
(EC) No. 450/2009 and intelligent material, on. No maximum levels are given.
but the specific application
has to be approved by the
European Food Safety
Authority.
Mexico Rules for innocuous Food additives Lists the types of food additives allowed Presidencia de la
control of products and their general definitions. República, 1999
and services, title
23
Mexican Official Disinfection with chlorine, Applies to potable water quality Secretarı́a de Salud
Standard, NOM- chlorine compounds, ozone, parameters and water purification (1994)
127-SSA1-1994 or UV light are allowed. processes
Mexican Official The maximum levels allowed A guideline to establish maximum levels SAGARPA (2017)
Standard, of chemical pesticides of chemical pesticides allowed for
NOM-082-SAG- found in human food must agriculture in the Mexican territory.
FITO/SSA1-2017 comply those established
by the Food and
Agriculture Organization
(FAO) and the World
Health Organization (OMS).
USA Code of Federal Status List for food additives Establishes the general principles for U.S. Congress (2016)
Regulations, Title evaluating the safety of food additives.
21, and Part 170
Code of Federal Lists the food additives Applies when the substance is added U.S. Congress (1999)
Regulations, Title generally recognized as intentionally to food.
21, part 182 safe (GRAS) in food.
Code of Federal Lists the substances affirmed Applies when the substance is added U.S. Congress (2011b)
Regulations, Title as GRAS in food. intentionally to food.
21, part 184
Code of Federal A list with almost 700 This regulation applies to antimicrobial U.S. Congress (2014)
Regulations, Title pesticide chemicals with substances on food contact surfaces.
40, Part 180, tolerances are given.
Subpart C
Code of Federal Substances affirmed as GRAS Applies when the substance is added U.S. Congress (2000)
Regulations, Title for use in food packaging intentionally to food.
21, part 186
U.S. Code, Title 21, Lists the maximum levels of Describes the cases for which the U.S. Congress (2015)
Chapter 9, pesticides in food and the tolerances must be met and those for
Subchapter IV, substances exempted from which an exemption can be requested.
section 346a this classification.
U.S. Code, Title 7, An antimicrobial pesticide is Details the requirements for cleaning and U.S. Congress (2017)
Chapter 6, intended to protect objects, sanitizing of food contact utensils.
Subchapter II. industrial processes or
systems, surfaces, and so on
from microorganisms
a The requirement statements have been paraphrased to reduce wording size.

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Antimicrobial coatings for food contact . . .

Table 12–Suggestions for the refinement of the legal terms into mechanical property designations and the techniques that can be applied to quantify
them (see Table 10 and 11).a

Regulatory requirement Translation into mechanical property Characterization techniques


Easy to clean Hydrophobicity and porosity Contact angle analysis, microscopy, and adsorption
test
Unable to absorb water or dirt
Smooth finishing Roughness Profilometry
Withstand cleaning Abrasion, adhesion, hardness, fracture Crosscut test, curvature test, indentation testing,
toughness, and stress pencil hardness, scratch test, scotch tape test,
rubbing test, sand test, and Taber test
Migration into food (as contaminant or as Adhesion and migration Crosscut test, extractability test, indentation testing,
additive) scratch test, and scotch tape test
a Adherence to these suggestions does not guarantee the satisfaction of regulatory statutes. Their interpretation must be carefully reviewed to determine compliance with standards set forth by various governing
bodies.

withstand microbial contamination. Although not explicitly stated, conditions, and the mechanical forces to which the equipment
the material of construction and the finish of the surface must be will be subjected, scientists and engineers should be able to de-
selected in such a way as to avoid microbial attachment. This se- sign equipment with surfaces meeting regulatory statutes. Table 12
lection relies on the fact that microbial adherence to surfaces varies shows the interpretation of the general quantitative requirements
considerably with both the surface composition and structure and listed in Table 10 and the more specific quantitative parameters
the microbial genera (Cunault, Faille, Dubois, & Bénézech, 2018; listed in Table 11. The interpretations allow researchers to express
Lopes, Morin, Oliveira, & Melo, 2005; Storgards, Simola, Sjöberg, requirements, such as ease of cleaning and smooth finish, in quan-
& Wirtanen, 1999). For instance, removal of bacteria is easier from titative, measurable quantities. On the other hand, it should be
stainless steel than from polyvinyl chloride (PVC) and high den- noted that although the quantities of antimicrobial additives and
sity polyethylene (HDPE) (Sommers & Sheen, 2015). Following contaminants in food are clearly defined, the actual amount of any
this reasoning, compliance with FCS regulations may be met by additive or contaminant that migrates from an AMC to the food
demonstrating that the material of construction, as well as the has to be assessed for each specific application, because, as will be
finish of the surface, discourage bacterial deposition and/or facil- shown in the coming sections, the transport of active substances
itates bacterial detachment. As mentioned previously, authorities from the FCS to the food’s matrix is a multivariable process. All the
or authorized third-party companies judge compliance by means regulations contained in Table 11 set stipulations for the migra-
of on-site inspections and/or document records. It is generally tion of food additives or contaminants into food. Therefore, these
accepted that stainless steel grade 316 with 2B finishing and food regulations make no distinctions among the assessment methods
grade HDPE both meet FCS regulations in general terms (Sarava- of migration, except for release, which should be thought of as a
cos & Kostaropoulos, 2016). controlled ejection of the active substance into the surroundings.
Legal compliance of antimicrobial agents. The steps to assess
compliance of AMC on FCS are, in general terms, the following Mechanical Properties of AMCs
(Assent, 2016): FCS are those surfaces present on equipment, utensils, and con-
(i) Assess which surfaces come into contact with food tainers for the production, processing, and packaging of food. This
(ii) Determine which surfaces’ materials of construction (in- definition is useful in identifying the FCS at the process facility
cluding the antimicrobial substance) are already in the level and simplifies the analysis of the regulatory framework. In the
approved-substances lists in the country or region of interest present section, an AMC is defined as a liquid mixture, solution,
(iii) Track parts whose materials of construction and active in- or suspension that is applied to a surface and undergoes solidifica-
gredients are unknown to their suppliers to verify the parts’ tion afterward (Hochberg, 1979) with the purpose of sanitizing,
materials of construction and active ingredients compliance disinfecting, reducing, or mitigating microbial growth on FCS
(iv) Gather support documentation regarding materials’ compli- (U.S. Congress, 2017). The coating layer is defined as the region
ance where the coating’s properties can be distinguished from those of
(v) Perform migration tests through an authorized third-party its substrate. In this section, different techniques for characteriz-
if documentation is not available. ing the AMC coating layers are explored, listed, and contrasted.
Additionally, some of the results that have arisen from investiga-
Regardless of whether the antimicrobial substance is considered tions using the characterization techniques given in Table 13 are
under a statutory or a regulatory system, the amount of antimi- discussed.
crobial that has migrated, intentionally or unintentionally, into the
food has to be determined quantitatively (Codex Alimentarius, Mechanical properties of AMCs for FCS
1995a, 1995b). For AMCs to be an industrially viable option, they must en-
dure and perform in a variety of conditions inherent to both food
Translation of legal requirements into mechanical property and cleaning processes, namely, over time, at variable tempera-
requirements for AMCs tures, and be compatible with both the food and cleaning process.
Following from the previous section, if an AMC is to be applied Firstly, an AMC must adhere most strongly to its substrate. Second,
on a FCS, the coating should be in compliance with antimicrobial the coating must be durable and lasting; high abrasion resistance is
regulations and keep the surface in compliance with applicable desirable in maximizing the operating lifetime of a coating. Hard-
regulations for FCS. From a design perspective, the AMC should ness, fracture toughness, and other related properties are directly
be considered as a component of the food processing equipment related to how coatings perform over time and with exposure to
at the early stages of the equipment’s design. With information mechanical stressors. Hydrophobicity, a property describing the
about the equipment’s specific application, the food processing coating’s affinity for water, is frequently reported, although no


C 2019 Institute of Food Technologists® Vol. 0, 2019 r Comprehensive Reviews in Food Science and Food Safety 13
Antimicrobial coatings for food contact . . .

Table 13–Common methods to characterize various mechanical properties of coatings.

Characterized
Mechanical property Characterization technique Equipment parameter Standard/Approved method
Abrasion Rubbing test Cotton fabric or hard Resistance against DIN norm 58196-5
eraser abrasion
Sand test Sand cradle/sand slide Haze and light ASTM D F735-17, DIN
scattering 52348:1985-02
Taber test Spinning wheels with Haze of the coating ISO 3537:2015
abrasives
Tribological testing Test rig Friction force and –
surface damage
Air blast Air blast abrasive Resistance to abrasion ASTM D 658–91
Adhesion Adhesion test Tensiometer rig Surface energy –
Adhesion test Dynamic load cell Force needed to tear DIN EN ISO 4624
off the coating
Crosscut test Pressure-sensitive tape Surface energy ASTM D 3359-09, BS
and cutting tool 3900-E6:2007, ISO
2409:2007, and (JIS) K5400
Indentation testing Nanoindenter Interfacial cracking –
Fracture toughness Indentation testing Nanoindenter Critical load of –
cracking
Hardness and elastic Indentation testing Nanoindenter Local plastic –
properties deformation
Pencil hardness Calibrated pencils Local plastic ASTM norm D 3363-05 and JISK
deformation 5400 norm
Scratch test Indenter Local plastic ASTM G 171-03
deformation
Hydrophobicity Contact angle Goniometer Surface energy –
Migration Extractability test Extraction cell Mass transfer rate CD 82/711/EEC, CD
85/572/EEC, and FDA
Guidance for industry 2007
Porosity Nitrogen adsorption Gas sorption system –
Scanning electron microscopy Scanning electron Distribution and –
microscope energy of scattered
electrons
Surface roughness Total integrated scattering Helium laser scatter Light scattering ASTM F1048-87 1999a
Stylus profiling Stylus profilometer Vertical deflection of ISO 4288:1996
stylus
Scanning electron microscopy Scanning electron Distribution and –
microscope energy of scattered
electrons
Scanning tunneling –
microscope
Stress Indentation testing Indenter Local plastic –
deformation
Curvature test Tensile and –
compressive
stresses
Thickness Ellipsometry and scanning Ellipsometry and scanning Refractive indexes and –
electron microscopy electron microscope direct measurement
from the generated
image
a Withdrawn in 2003.

definitive correlation between hydrophobicity and cell adhesion Aegerter (2017) suggests using easy, inexpensive, and standardized
to FCS has been demonstrated. In terms of performance and methods as screening tests and before proceeding further to obtain
compatibility, the coating microstructure not only influences the more accurate data with more sophisticated and sensitive equip-
coating’s antimicrobial activity, but also the migration of antimi- ment to study coatings that already meet the expectations for the
crobial substances from the coating into food. As will be discussed intended application (Aegerter, 2017).
in the subsequent section, the microstructure of a coating is largely The existence and availability of several methods to assess the
dependent, not only on the chemical composition and defects of same mechanical property also influences the selection of charac-
the coating, but also the deposition method. Last, the impact of a terization equipment (for example, the case of abrasion, with at
coating on its substrate’s surface roughness must be evaluated, as a least five different characterization techniques that may be used
coating will tend to make the substrate smooth, thus influencing to quantify abrasion). Porosity of AMCs, for example, can be ex-
the tendency of bacteria to adhere to the modified surface. pressed as percentage of surface area covered by pores and deter-
Characterization of coating mechanical properties. The selec- mined by microscopic observation (Ctibor et al., 2012). Porosity
tion of mechanical property characterization equipment for coat- is also reported as percentage of the coating total volume cor-
ings depends on three parameters: the type of investigation con- responding to pores (Liu, Wang, Yang, & Yang, 2008). Better
ducted, the availability of multiple methods to assess the same yet, porosity of AMCs can be described with a combination of
property, and the amount of detectable response from the coating multiple characterization technique results, such as average pore
when perturbed by the characterization tool. Research experi- size and pore surface coverage from scanning electron microscopy
mentation requires more precise (and more expensive) instrumen- (SEM) and transmission electron microscopy (TEM) imaging and
tation, whereas field and industrial studies are performed by less pore volume percentage from H2 O/D2 O exchange experiments
exact equipment and, often, with more repeatable procedures. (Atefyekta et al., 2016).

14 Comprehensive Reviews in Food Science and Food Safety r Vol. 0, 2019 


C 2019 Institute of Food Technologists®
Antimicrobial coatings for food contact . . .

The amount of detectable response is a third factor to con- formation of the coating due to a compressive force using a tip of
sider when choosing the characterization equipment. For instance, well-defined geometry (Le Bail, Benayoun, & Toury, 2015). The
Anne Pauline, Kamachi Mudali, and Rajendran (2013) deter- tip moves down in the vertical direction and indents the coating
mined that the incorporation of strontium (Sr) into porous titania (see Figure 4). For the scratch test, a tip of known geometry is used
(TiO2 ) gave the same adhesion level, namely, no failed regions, to apply an increasing normal force on the coating. The tip moves
whereas Palanivelu and Kumar (2014) found that the addition of in the direction parallel to the evaluated surface at a given veloc-
TiO2 and hydroxyapatite to alumina (Al2 O3 ) coatings showed ad- ity, creating a scratch. The measurement of the forces involved
hesion values that varied up to 30%, depending on the amount in the process allows the calculation of the adhesion coefficients
of TiO2 and hydroxyapatite incorporated into the coating. These (Aegerter, 2017). For a comprehensive and detailed description of
differences in the results of the two studies may be attributed to these techniques, refer to the ASM Handbook (Brotzen, 1994).
differences in the sensitivity of the characterization methods used, Please see Table 14 for a list of studies that report adhesion val-
namely, adhesion by tape and nanoindentation, respectively. When ues in conjunction with the coating material, substrate material,
choosing a characterization technique, the desired level of accu- deposition method, and adhesion assessment method.
racy should be known, and the option chosen should be evaluated Abrasion. Abrasion is a process that consists of the movement
to ensure that the technique provides adequate resolution. of a particulate or bulk solid tangentially to a solid surface under a
The characterization techniques given in Table 12 are further certain force. Abrasion is closely related to wear. Wear is the pro-
segmented and matched to specific testing equipment in Table 13. gressive damage of a surface that comes from the relative motion
Often, one mechanical property can be assessed with different between the surface being worn and another solid. The outcome
equipment and with different characterization parameters. Equip- of these two processes, namely, abrasive wear, is the loss or dis-
ment and tests that have found applications at industrial levels are placement of the material from the surface subjected to abrasion
already standardized, which is advantageous when comparing the (Tylczar, 1992). The abrasive may take the form of a cotton fabric,
same mechanical property of different coatings. The main dis- sand grains, a spinning wheel’s surface, or a flow of a mixture of
advantage of standardized characterization methods is that they air and solid powders. The effects of abrasion are then estimated
provide little, if any, fundamental information to explain the ob- assessing a measurable change in any surface property, such as mass
served antimicrobial activity. loss and volume loss, and in instances where the volume or mass
Adhesion. Adhesion is the force of attraction between two sur- of a coating is difficult to determine, the degree of wear is often
faces that keep them attached together. Adhesion characterization assessed by the reflection and transmission of light from surfaces
techniques work based on the principle that under certain cir- (Aegerter, 2017). The Taber test is the technique most frequently
cumstances, it is possible to measure the energy required to sep- used to evaluate the wear of coatings (Le Bail et al., 2015). This
arate two attached surfaces. Adhesion can be expressed in units test consists of the cyclic application of a fixed load on the coat-
of energy per surface area, force, or in terms of a value taken ing using wheels whose external surfaces possess a well-defined
from an arbitrary scale that reflects the level of adhesion (namely, abrasive material. The abrasive material is then put in contact with
the cross-cut test scale). The classification of adhesion assessment the coating by means of rotating the wheels a certain number of
methods can be separated into two groups: macroscopic and mi- times or cycles. Then, the coating’s surface is examined under a
croscopic. The crosscut and adhesive tape tests belong to the first microscope to quantify the wear.
group, whereas indentation and scratching correspond to the sec- The availability of studies on the mechanical wear of AMC is
ond group. Macroscopic techniques are inexpensive, simple, and very limited and even more limited for specific applications on
are useful in selecting coatings for industrial applications. The ad- FCS, despite the importance of this parameter in the implemen-
vantage of using microscopic techniques is that these techniques tation of AMC in real food-processing environments. Hung and
provide quantitative information, whereas macroscopic techniques Yemmireddy (2015) have reported the assessment of wear of AMC
often do not (Aegerter, 2017). intended for use on FCS. TiO2 nanoparticles were mixed with dif-
The crosscut and the tape test consist of placing an adhesive ferent polymeric binders and applied on stainless steel coupons.
tape on the coating to be evaluated. In the tape test, the adhesive Then, the coatings were repeatedly used for antimicrobial test-
film is placed directly onto the coating’s surface, whereas in the ing. After 1, 3, 5, and 10 cycles of antimicrobial action and rinse,
crosscut test, perpendicular incisions are first cut into the coating the coatings’ mechanical and antimicrobial parameters were as-
to form a grid and subsequently, an adhesive tape is placed on sessed. The outcome of the investigation was that depending on
the sample. Uniform force is applied to adhere the tape to the the binder used, the loss of antimicrobial activity can be as high
sample surface and then firmly removed. The coating is inspected, as 73% due to the diminution of the coatings’ thickness and pho-
and the amount of coating substance removed is graded according tocatalyst exposed area. Hung and Yemmireddy (2015) concluded
to a graphical scale. Following ASTM D 3359-09, Hung and that the decrease of antimicrobial activity was due to coating dam-
Yemmireddy (2015) rated the adhesion of AMCs with different age. In the second experiment, Hung and Yemmireddy (2015)
binders and TiO2 nanoparticles to stainless steel according to the quantified the wear of the AMC using an abrasive reciprocating
cross cut test scale, from 2B to 4B (Hung & Yemmireddy, 2015). apparatus that exerted force with sponges and brushes on coatings
Microscopic techniques, such as indentation and scratch meth- prepared with different types of binders. Later, Yemmireddy and
ods, are more sophisticated than the macroscopic evaluations, and Hung (2017) explored the effect of multiple washes and use cycles
require a nanoindenter, similar in many respects to those used on HDPE cutting boards covered by TiO2 nanoparticles. The cut-
in the Vickers and Brinell hardness tests. The main difference ting boards showed similar or decreased antimicrobial activity after
between nanoindentation and other common hardness tests is repeated use (Yemmireddy & Hung, 2017). These studies suggest
that with nanoindentation, mechanical properties are extracted that the reduction in the efficacy of AMCs over several use cy-
by sampling from the surface to nanometer depths, whereas com- cles is a challenge that still needs to be addressed. Unfortunately,
mon indenters work deeper in the solid body (Brotzen, 1994). results reported by Yemmireddy and Hung (2017) are difficult to
Nanoindentation relies on the characterization of the plastic de- compare, not only because of the lack of similar studies, but also


C 2019 Institute of Food Technologists® Vol. 0, 2019 r Comprehensive Reviews in Food Science and Food Safety 15
Antimicrobial coatings for food contact . . .

Table 14–Selection of results from studies on adhesion of coatings to their substrates.

Macroscopic techniques
Coating Substrate Deposition method Adhesion technique Adhesion Reference
TiO2 Stainless steel Spin coating of sol gel Cross cut test 5B Anne Pauline et al. (2013)
TiO2 Stainless steel Dip coating with Cross cut test 4B Hung and Yemmireddy
polymeric binder (2015)
TiO2 Stainless steel Dip coating with Cross cut test 4B Yemmireddy, Farrell, and
polymeric binder Hung (2015)
AlO3 nanoparticles Stainless steel Dip and spin coating Adhesion tape 170 to 200 N Hesselbach et al. (2018)
with polymeric
binders
Microscopic techniques
Coating Substrate Deposition method Adhesion technique Adhesion Reference
AlO3 Stainless steel Sol–gel Peeling test 73 J/m2 Xie and Hawthorne (2003)
TiO2 Titanium Plasma spray Micro scratch 19.7 N Palanivelu and Kumar (2014)
TiO2 Stainless steel Sol–gel spraying Micro scratch Not Momeni, Saghafian,
determined. Golestani-Fard, Barati, and
No delami- Khanahmadi (2017)
nation
occurred.

because of the use of made-in-house assessment methods. With


this in mind, standard methods, such as ISO 11640:1993 (leather,
color fastness to cycles of to-and-fro rubbing) are available and
have been used to evaluate the abrasion resistance of an AMC on
leather against E. coli and Staphylococcus aureus.
The lack of information published on wear and abrasion of
AMC for FCS may be mitigated with results found in studies on
wear and abrasion of coatings and surfaces for medical applica-
tions. Lazzeri et al. (2006) have proposed methods to quantify the
mechanical degradation of polymer coatings for medical devices
using the tip of atomic force microscopes as a tool to induce wear
on the coatings. Wear of the surface can be subsequently quanti-
fied by measuring the size of the damaged areas with the use of
microscopic imaging techniques (Ilie, 2010; Wang, Peng, Wang, Figure 2–Nano indentation analysis requires a precise knowledge of the
& Jiang, 2013; Yuan, Jin, Tipper, & Yan, 2010). Wear not only nanoindenter tip’s geometrical features. Once the tip touches the coating
at the contact point, the coating is indented until the highest load is
depends on the material used to fabricate the coating, but also
detected. In addition, the indentation depth parameters, hr , hc , A, As ,
on the fabrication conditions, such as the sintering temperature roughly estimated using a load indentation curve, can be determined by
in the case of firing sol–gel coatings. As the temperature of cal- means of microscopic measurements of the indenter.s tip at max load and
cination of the coatings was increased up to 900 °C, the lowest max depth.
wear rate obtained was around 3 × 10−4 mm3 /Nm (Çomaklı,
Yetim, & Çelik, 2014). The addition of tungsten oxide (WO3 ) nique. Details on the nanoindentation technique can be found in
to TiO2 coatings, deposited by electrophoresis, increased the vol- the ASM Handbook (Brotzen, 1994).
ume of wear compared to coatings of pure TiO2 , but the wear Plastic deformation is studied using stress relaxation and creep
volume, measured using scratch tests, decreased as the amount of tests. Stress relaxation tests consists of measuring the change in
WO3 increased among TiO2 –WO3 composite coatings (Hafedh, load while the coating is pressed with the indenter at a con-
Kaouther, & Ahmed, 2017). Another study demonstrated that stant rate during a specified length of time. On the other hand,
pure titanium surfaces coated using plasma spray deposition, with during the creep test, the penetration rate is recorded while the
Al2 O3 (13 wt% TiO2 ), displayed a decrease in wear rate of 1.7 indenter load is kept constant. Graphs of plastic depth (usually
times (Palanivelu & Kumar, 2014). Similar results were obtained given in nm) as a function of time (usually given in seconds) at
by coating pure titanium with TiO2 using sol–gel and ionic post different constant loads can be plotted. Beam-bending methods
treatment methods. Evaluation of the wear ratio using a Taber- are useful to determine elastic and yield properties of coatings,
like test indicated that the wear ratio decreased by almost half with such as the Young’s modulus, E. Though different from scratch
respect to the uncoated titanium surface (Çomaklı et al., 2018). and indentation tests, a nanoindenter can also be used to bend a
Hardness, fracture toughness, and related properties. Fracture micromachined-cantilever beam. The free end of the beam, fixed
toughness, hardness, plastic deformation, and other related prop- from one of its ends, is forced downward by the indenter’s tip, and
erties are conveniently assessed by nanoindentation techniques the deflection, δ, is recorded. The Young’s modulus can be deter-
(Brotzen, 1994). Depending on the specific property that needs mined from the slope of the curve δ(P), where P is the applied
to be evaluated, the tip is used to indent or to scratch the up- load. Then, the Young’s modulus of the coating can be determined
per layer of the coating, usually no deeper than one-tenth of by comparing the Young’s modulus of the bare substrate and that
the total thickness. The main requisite of the indentation test is of the coated substrate.
that the tip should not interact with the substrate during testing The mechanical properties of coatings vary depending on the
. Figures 2 and 3 further elaborate on the nanoindentation tech- coating material, the deposition method, and the resultant mi-

16 Comprehensive Reviews in Food Science and Food Safety r Vol. 0, 2019 


C 2019 Institute of Food Technologists®
Antimicrobial coatings for food contact . . .

Table 15–Hardness and elastic properties of selected coatings with potential application as antimicrobial coatings.a

Young’s
Hardness—H modulus—E Effective elastic
Coating Deposition method Structure description (GPa) (GPa) modulus—Er (Gpa) Reference
ZrO2 Dip coating sol–gel Nonporous 5.0 220 – Garcı́a-Heras et al.
(2003)
ZrO2 -SiO2 Dip coating sol–gel Nonporous 4.9 85 – Garcı́a-Heras et al.
(2003)
SiO2 Dip coating sol–gel Nonporous 4.8 70 – Garcı́a-Heras et al.
(2003)
SiO2 Spin coating sol–gel Mesoporous disordered – – 3.2 Williford et al.
structure (2005)
SiO2 Spin coating sol–gel Mesoporous hexagonal – – 3.5 Williford et al.
structure (2005)
TiO2 Electrophoretic 21 nm average particle 1.03 108 – Hafedh et al. (2017)
deposition size
TiO2 Dip coating sol–gel Anatase and rutile, dense 7.8 to 8.8 – – Çomaklı et al.
coating with grain size (2018)
approximately 20 to
40 nm
TiO2 doped with Fe Chemical vapor Dense rutile 8.9 to 12.3 Approximately – Sobczyk-Guzenda
or Cu/F deposition 150 to 180 et al. (2018)
PTFE/ Spray gun Polymer from free radical 0.06 – 10 Yeo and Polycarpou
Pyrrolidone-1 polymerization (2013)
PTFE/ Spray gun Polymer from free radical 0.05 – 3.6 Yeo and Polycarpou
Pyrrolidone-2 polymerization (2013)
PTFE/MoS2 Spray gun Polymer from free radical 0.05 – 3.5 Yeo and Polycarpou
polymerization (2013)
a When possible, TiO was chosen as the AMC’s material of construction to facilitate comparisons.
2

quently the methods of choice when depositing a sol–gel based


coating, depending on the viscosity of the precursor. Dip coating
is typically employed for more viscous precursors, as it is more
difficult to achieve uniform coatings with highly viscous inks us-
ing spin coating. The hardness of spin-coated/dip-coated coatings
varies, with typical hardness values from 5 to 9 GPa (Çomaklı
et al., 2018; Garcı́a-Heras, Rincón, Romero, & Villegas, 2003;
Williford et al., 2005). Finally, less common deposition methods
include electrophoretic deposition and chemical vapor deposi-
tion, among others (Hafedh et al., 2017; Sobczyk-Guzenda et al.,
2018). Table 15 lists the results of various coating materials, depo-
sition methods, microstructures and their corresponding hardness,
Young’s modulus, and effective elastic modulus.
Hydrophobicity. Liquids have deformable boundaries. The
force that acts on a liquid body’s surface to minimize its exter-
nal surface area is called surface tension. When a liquid substance
contacts a solid surface, there are three forces that act on a molecule
at the point where the liquid, the solid, and the surrounding at-
mosphere meet: the surface tension at the liquid–gas (atmosphere)
interface, liquid–solid interface, and the solid–gas interface. The
Figure 3–The information recorded during a nanoindentation test can be
summarized in a load versus indentation curve. The measurement starts mathematical expression describing the relationship between the
at the contact point with zero load. Load is continuously increased forces is, γ lg cos θ = γ sg – γ ls , where γ lg , γ ls , and γ sg are the
through the indenter.s tip until “breaking” the coating. Then the indenter surface tensions at the liquid–gas (atmosphere) interface, liquid–
tip is continuously unloaded until its complete separation from the solid interface, and the solid–gas interface, respectively, and θ is the
coating. The max load depth, the maximum load, and the effective elastic
modulus (calculated form the tangent S line) can be determined from
contact angle (see Figure 4). From θ , the coating can be described
theplotted data. qualitatively as hydrophobic or hydrophilic, depending on whether
the coating shows repulsion or affinity for water, respectively.
In 1989, Kirtley and McGuire (1989) proposed the measure-
ment of contact angle as a descriptor of the liquid–solid interac-
crostructure. Furthermore, these parameters are not independent.
tions on FCS. Subsequently, McGuire and Sproull (1990) exam-
For instance, the desired microstructure is frequently the parameter
ined the influence of temperature on the same parameter for food
optimized, with the coating material fixed. As such, the deposi-
contact applications. From there, many articles have been pub-
tion method is often chosen to achieve the desired microstructure.
lished with a variety of different results. Analysis of these articles
Consider polytetrafluoroethylene (PTFE) coatings produced by
indicates a pattern, namely, the contact angle and the surface free
spray gun application. The precursors are typically nonviscous,
energy cannot be correlated with the attachment of bacteria on
and the resultant coatings have significant effective elastic modu-
FCS. Experiments studying the attachment of L. monocytogenes and
lus, Er , but possess low values of hardness, H (Yeo & Polycarpou,
Salmonella on stainless steel and polymers (Sinde & Carballo, 2000),
2013). On the other hand, dip coating and spin coating are fre-


C 2019 Institute of Food Technologists® Vol. 0, 2019 r Comprehensive Reviews in Food Science and Food Safety 17
Antimicrobial coatings for food contact . . .

deposition, were investigated by optical microscopy, transmission


electron microscopy (TEM), and X-ray diffraction (Ctibor et al.,
2012).
Ellipsometry is employed to estimate the thickness of antimi-
crobial TiO2 coatings (Cao et al., 2014) and has been proposed as
a method to determine cleanliness of FCS (McGuire, Al-Malah,
Bodyfelt, & Gamroth, 1990). In the study presented by Cao et al.
(2014), different FCS were covered with milk and washed after-
ward following different cleaning procedures, and the refractive
indices of the surfaces before and after the washing treatments
were compared and used as a quantitative indicator of cleanliness.
It was found that the substrate’s microstructure played a significant
Figure 4–Contact angle analysis involves the measurement of the angle role in the cleanliness achieved.
formed between the liquid surface and the solid surface. The amplitude of The porous volume of various semiconductor-based AMC has
the measured angle, θ , serves as a quantitative parameter to classify the been quantified by nitrogen sorption (Liu et al., 2008). Although
solid surface as hydrophobic (bad wetting) or hydrophilic (good wetting).
the use of rough and absorbent surfaces is restricted by FCS regula-
tions (Australia New Zealand Food Authority, 2016; Secretarı́a de
L. monocytogenes on stainless steel, different kinds of rocks, glass, Salud, 2010; U.S. Congress, 2011a), a positive correlation has been
and polypropylene (Silva, Teixeira, Oliveira, & Azeredo, 2008), demonstrated between the active area of photocatalytic coatings
and Salmonella Enteritidis and L. monocytogenes on two different and their antibacterial action (Zhang, Tu, Zhang, Zheng, & Yang,
types of stainless steel (Casarin et al., 2016), all concluded that 2014). Given this, efforts have been devoted to increase the specific
there was no correlation between the substrates’ hydrophobic- surface area by means of the formation of porous structures.
ity and bacterial attachment. Additionally, Perera-Costa, Bruque, Migration. Migration refers to the mass transport of the antimi-
Gonzalez-Martin, Gomez-Garcia, and Vadillo-Rodriguez (2014) crobial substance from the AMC structure into the food and/or
claim that reductions in cell adhesion to textured surfaces occur to the head space inside a closed container by means of molecu-
regardless of surface hydrophobicity. Spores of B. cereus and Bacillus lar, convective, or a combination of both types of transport under
subtilis attach in similar amounts to surfaces, irrespective of the sur- storage conditions. The rate of migration is affected by the envi-
faces’ hydrophobicity (Faille et al., 2002). However, this tendency ronmental conditions at which the coating-food system is kept, the
cannot be taken as definitive because there are results that show nature of the food, the coating’s mechanical and chemical prop-
that E. coli (Faille et al., 2002) and Staphylococcus epidermidis (Cerca, erties, and its antimicrobial characteristics (Nerin, Silva, Manso,
Pier, Vilanova, Oliveira, & Azeredo, 2005) adhere more readily & Becerril, 2016). To measure rates of migration, food simulants
on hydrophobic surfaces as compared to hydrophilic surfaces. In are placed in contact with the coating to be evaluated under con-
conclusion, the contact angle, though intuitively relevant, is not ditions of temperature and elapsed time that resemble or exceed
a good parameter with which to assess whether a surface is easy those to be expected during the actual use of the coating. The
to clean or prevents the adhesion of bacteria. Therefore, surface concentration of the components of the coatings that migrate into
topography is the preferred characteristic to correlate with the the food simulants is usually determined by chromatography.
ease-of-decontamination of FCS.
A typical migration test consists of three steps:
Microstructure. The microscopic structure of a coating is de-
fined by several interrelated properties, including porosity, di-
mension and form of grain, phase composition, surface rough- (i) Preparation of the food sample and surface sample
ness, thickness, and coatings defects. Coating properties, such as (ii) Contacting the actual foodstuff or a simulant and the mate-
hardness, surface energy, and wear resistance, are influenced by rial to be tested at specified test conditions and for specified
the coating’s microscopic structure, chemical composition, and durations
the presence of impurities (Aegerter, 2017). Additionally, the (iii) Assessment of the amount of mass transferred from the FCS
microstructure is highly influenced by the coating’s deposition to the food or the simulant food using approved analytical
method, as will be shown in the following section. techniques.
The characterization of microstructure properties relies on the
observation of a coating’s surface under a microscope, the assess- EU directives 82/572/EEC and 82/711/EEC mandate that ref-
ment of the surface of a coating using a fine stylus, or by adsorption erence samples are exclusively plastic, food simulants vary (typi-
of nitrogen or water into the coating’s voids for the specific case of cally, distilled water, dilute acetic acid, ethanol, and rectified olive
porosity and porous volume. Consider the following case studies oil or some combination thereof), typical testing temperatures are
that list typical microstructure characterization techniques and the from 5 to 121 °C, testing times range from 30 min to 10 days,
associated data provided by the various techniques. In one experi- and analytical methods to determine contaminant concentration
ment, the incorporation of chelating agents allowed the deposition in the food product are not specified. In contrast, the guidelines
of relatively thick (1.2 µm) barium titanate (BaTiO3 ) crack-free in the United States specify the test equipment as a migration cell
coatings on glass using a sol–gel dip coating method (Kozuka, with the reference sample being a plaque with known proper-
Kajimura, Hirano, & Katayama, 2000). Thickness was measured ties (FDA, 2007b). Food samples vary (10% to 50% ethanol and
using contact profilometer, and crack formation was observed by food oil) with the testing temperature being set at the most severe
SEM and surface profilometry, whereas internal stress was mea- conditions expected and the testing time being the longest time
sured using a bending-substrate technique. In another experiment, period expected in real applications. The analytical method to be
pore size and shape, crystal phase, and the microstructure of TiO2 used to determine contaminant concentration is also unspecified,
coatings, deposited on stainless steel substrates by plasma spray but the accuracy, precision, and selectivity must be provided.

18 Comprehensive Reviews in Food Science and Food Safety r Vol. 0, 2019 


C 2019 Institute of Food Technologists®
Antimicrobial coatings for food contact . . .

Table 16–Overview and comparison of migration tests within the European Union and the United States of America.

Migration test Extractant analytical


rules Test equipment Test sample Food sample Test temperature Testing time method
82/572/EEC and Not specified Exclusively made of Depending on the Depending on the Depending on the Not specified.
82/711/EEC plastic intended food intended intended
application. application: application:
Distilled water, 3% from 5 121 °C. from 30 min to
(w/v) acetic acid, 10 days.
15% ethanol, and
rectified olive oil.
Guidance for Migration cell A plaque of known Food simulants should The most severe The longest period Not specified, but
industry: formulation, be used depending condition of time should be described
preparation of thickness, surface of the intended expected, or expected or its accuracy,
premarket area, and food application. depending on 10 days. precision, and
submissions for polymeric 10% to 50% the intended selectivity.
food contact properties (if ethanol and food oil application:
surfaces. applicable) from 20 to
40 °C.

Table 17–Selection of results from migration tests of plastic additives regarded as food contamination.

Migration Detection method in


Contaminant Legal limit observed extracting medium Food Surface Reference
Di(2-ethylhexyl) 50 µg/kg of food Up to 1,500 Gas chromatography Rice, starch, barley, Cardboard boxes (Fiselier et al., 2009)
maleate µg/kg noodles, spaghetti, without functional
pizza, frozen fish, barrier
biscuits, among
others.
Mainly epoxidized The sum of all Up to 1,314 Liquid and gas 411 different food Gasket of lids (McCombie et al.,
soybean oil migrated mg/kg chromatography products 2012)
(ESBO) and plasticizers <60
other 19 mg/kg of food
different
plasticizers
Melamine and Melamine: 2.5 mg/kg; Melamine: not Liquid Food simulant: acetic Melamine plastic Garcı́a Ibarra et al.
formaldehyde formaldehyde: detected to chromatography acid 3% (w/v) kitchenware (2016)
15 mg/kg of food 13.5 mg/kg
Formaldehyde:
0.165 to
150 mg/kg

Table 18–Selection of results obtained from migration investigations of antimicrobial substances considered as food additives.

Detection method in
Additive Migration observed extracting medium Food Surface Reference
Cinnamon and clove 0.88 to 1.19 mg/g UV–Vis spectroscopy Distilled water Cassava starch Souza et al. (2013)
essential oils
Ethyl lauryl arginate 0.93 to 1.62 µg/g Liquid Simulants: ethanol Polyethylene Aznar et al. (2013)
chromatography 10% and 95% v/v,
and chicken
Silver 1.66 to 31.46 ng/cm2 Mass spectrometry Simulants: 1.66 to Food containers Echegoyen and Nerin
31.46 ng/cm2 (2013)
Silver <0.1 to 28 ng/cm2 Voltammetry Pure and acidified Poly (lactic acid) Martinez-Abad,
water (pH 2.5) Lagaron, and Ocio
(2014)

Several case studies show the application of these guidelines 2016). These results are summarized in Table 17. Several studies of
to both general food contaminants and antimicrobial substances the migration of antimicrobial substances into food exist, such as
considered as food contaminants. Fiselier, Rutschmann, McCom- studies of the migration of essential oils (Souza, Goto, Mainardi,
bie, and Grob (2009) studied the migration of di(2-ethylhexyl) Coelho, & Tadini, 2013), ethyl lauryl arginate (Aznar, Gomez-
maleate from cardboard boxes into various food products, includ- Estaca, Velez, Devesa, & Nerin, 2013), and silver (Echegoyen &
ing rice, frozen fish, and biscuits, among others (Fiselier et al., Nerin, 2013) from various substrate materials of construction,
2009). The established legal limit of the contaminant is 50 µg/kg including cassava starch, polyethylene, and polylactic acid, respec-
of food; however, gas chromatography revealed that the contam- tively (see Table 18).
inant concentration was as high as 50 µg/kg of food. Other ex- Regulatory agencies demand toxicology data from antimicrobial
amples of general contaminant migration into food are available, agents used on FCS, depending on the substance and its classifica-
including an extensive study of the migration of plasticizers from tion according to Table 1. Regardless of whether the antimicrobial
lid gaskets into 411 different food products, characterized with liq- agent is considered as an additive or food contaminant, the reg-
uid and gas chromatography (McCombie et al., 2012), and a study ulatory agencies, tolerance levels, monitoring, enforcement, and
of melamine and formaldehyde from plastic kitchenware into a the characterization methods suggested and approved vary greatly
dilute acetic acid solution, characterized with liquid chromatog- by region, as explained in section 3 (Legal Framework Pertain-
raphy (Garcı́a Ibarra, Rodrı́guez Bernaldo de Quirós, & Sendón, ing to Food Contact Surfaces). Regardless of those variations, all


C 2019 Institute of Food Technologists® Vol. 0, 2019 r Comprehensive Reviews in Food Science and Food Safety 19
Antimicrobial coatings for food contact . . .

legal frameworks require knowledge of a food component’s toxi- posited. However, it is expected that the coating would smooth
city, which in general terms, can be classified as acute, subacute, the FCS after its application because that is one of the require-
or chronic (Watson, 2004). Additionally, these three toxicity ap- ments stated by FCS regulations. Smooth and rough are relative
proaches can be performed in three modes: in vitro (microor- concepts, but 0.1 to 100 µm are frequently used in practice. Am-
ganisms, cells, and biological molecules), in vivo (whole, living plitude in the z-direction (height variation) and spatial frequency
organisms), and in silico (computer simulation) (Watson, 2004). in x- and y-directions are the main features to consider when
From these, in vivo testing (that is, feeding studies in laboratory measuring surface roughness. Hence, to compare roughness val-
animals) is generally required by regulatory agencies (Armstrong, ues measured with different equipment, the ranges of spatial fre-
1992; FDA, 2007a; OECD, 2019). However, in vivo testing is time quencies in x and y must be the same, because roughness is a
consuming; therefore, in vitro tests, in general, and cytotoxicity relative measurement. When that is not the case, roughness data
tests, in particular, are used as prerequisite tests before specific are presented in terms of a power spectral density function (PSD)
toxicological studies and in vivo testing are carried out (Cetin & and their values can be compared even if the data come from
Bullerman, 2005). Cytotoxicity is a measure of the ability of a different methods, equipment, or if different spatial frequencies
substance to cause damage to cells due to its toxic properties. Cy- were used. The cutoff, namely, the low-frequency limit of the
totoxicity bioassays can be subdivided into the following types, measurement, must be clearly stated as well. The spatial frequency
with regard to the specific cellular damage resulting from the toxic that is used as a reference to assign roughness values is called the
effect: exclusion/inclusion dye, extracellular release of intracellular special frequency footprint. The roughness is expressed in propor-
marker, cell proliferation, RNA synthesis inhibition, and inhibi- tion to the footprint or by means of the PSD. When the spatial
tion of boar spermatozoan motility (Severin, Souton, Dahbi, & frequency footprint is fixed by means of the scan area or cut-
Chagnon, 2017). off length, the surface topography can be expressed as an average
For the specific case of coatings, any of the cytotoxicity bioas- roughness Ra . The reader should refer to ISO 4287:1997 for de-
says mentioned above are performed with the extracts obtained tailed descriptions of terms and definitions of texture descriptors
from the migration tests (Migration). Because there are innu- (ISO, 1997).
merable antimicrobial agents that can migrate from the AMCs Cunault et al. (2018) argue that roughness (Ra ) alone is
to the food matrices (see Table 11), it is impossible to list cyto- not enough to establish coherent relations between bacterial
toxicity bioassays for each antimicrobial agent. It should be men- detachment and surface topography. Instead, Cunault et al. (2018)
tioned that Mittag et al. (2006) specifically addressed the migration suggest the use of reduced valley depths and reduced peak heights
of chemical components from FCS coatings and corresponding as better descriptors. Previously, Crawford, Webb, Truong, Hasan,
cytotoxicity bioassays, although the coatings were not intended and Ivanova (2012) suggested that the minimum topographical
for antimicrobial purposes. In their study, Mittag et al. (2006) parameters that must be reported for microbiological adhesion
evaluated the migration of multiple agents from can coatings to surfaces are the root mean square (RMS) roughness, the
with different bioassays, including those related to cytotoxic- summit density, and the developed area ratio. The discussion of
ity, mutagenicity, and aquatic toxicity. Strong variations in the the importance of choosing sufficient roughness parameters to
cytotoxicity effects were detected depending on the cell type describe a coating may come from attempts to explain intuitively
tested. contradictory results. Truong et al. (2010) found that both S.
In summary, the guidelines provided in Table 16 are useful, al- aureus and Pseudomonas aeruginosa ATCC 9025 were retained
beit vague. A survey of migration tests suggests that experiments in higher amounts on extremely polished commercial purity
should be modeled as closely to real applications as possible, with titanium surfaces than on less smooth surfaces made of the same
food simulants and surfaces giving an adequate representation of material. In 2005, a study found that the size of pits intention-
mass transfer of contaminants into real food products. Similarly, ally placed on titanium coatings and the cells’ size influence
the testing temperature and time should be representative of the bacteria retention on titanium coatings (Whitehead, Colligon,
temperatures and time that the actual food product will be ex- & Verran, 2005). Subsequent papers on purposely textured
posed to the contaminant. Popular analytical methods to quantify coatings report inhibition of biofilm formation on textured
contaminant concentration include liquid and gas chromatogra- films (Xu & Siedlecki, 2012), that bacteria adhere selectively
phy; however, other suitable methods are UV–Vis spectroscopy, depending on the topographical pattern encountered on the
mass spectrometry, and voltammetry, as demonstrated by the case coatings (Perera-Costa et al., 2014), that microbial retention
studies listed in Table 17 and 18. is affected by the surface chemistry and features of different
Surface roughness. Stainless steel is the most commonly used metal surfaces (Whitehead et al., 2015), and that the initial cell
material of construction for food processing equipment (Sarava- adhesion process starts at the surface’s peaks (Ludecke et al., 2016).
cos & Kostaropoulos, 2016). The arithmetic roughness of stainless These investigations suggest that patterned textures can alter
steel surfaces varies widely based on the method employed to finish bacterial adhesion on coatings by reducing the area of contact
the surface (Brotzen, 1994). To assess roughness, the mechanical between surfaces and cell walls, but those treatments alone are not
stylus (profilometer) is the instrument most widely used for indus- enough to completely prevent bacterial deposition. The results
trial purposes, whereas microscopic techniques, such as SEM and of various investigations on the effect of surface topography on
scanning tunneling microscopy (STM), are much more common the adhesion of bacteria to surfaces (some of which are also
in research laboratories. Light scattering is another technique that mentioned above) are shown in Table 19. It can be observed that
is frequently used in both production and research environments. the surface roughness and the bacterial genus exert influence on
Figure 5 shows a more detailed graphical list of the equipment the cells’ attachment. However, cell attachment also seems to be
that are used to perform surface topography, commonly known as dependent on more than surface roughness and bacterial genus
profilometry, measurements. alone.
Intuitively, the AMC average roughness is, in part, dependent To supplement the results reported in Table 19, a com-
on the average roughness of the surface upon which it is de- parison of the materials and methods reported is shown in

20 Comprehensive Reviews in Food Science and Food Safety r Vol. 0, 2019 


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Antimicrobial coatings for food contact . . .

Figure 5–Graphical representation of the characterization techniques used to assess mechanical parameters comprised under the general term
“profilometry”. Contact and pseudo contact techniques are widespread for characterizing coatings that are not transparent.

Table 20. The detachment procedure is the most important pa- Influence of deposition method and coating material
rameter listed in Table 20, because detachment/attachment values on mechanical properties of AMCs
are the final outcomes reported in the listed investigations. A closer Deposition methods strongly influence the coating’s microstruc-
look at the methods of determination of adherent bacterial cells ture because each procedure yields differences in grain size, phase
on the studied surfaces reveals that the values reported are not composition, crystalline structures, crosslinked structures, amount
comparable, as every research group uses profoundly different and size of pores, size of cracks, and other defects. Additionally,
methods to evaluate detachment values even if the reported val- each deposition method has several operational parameters that
ues have the same units. For instance, results obtained by directly allow nuances in the final coating obtained. In addition to mi-
observing the attached bacteria on sample surfaces, after rinsing crostructure, the surface topography and hardness of coatings also
them with water for 30 min following the bacterial inoculation depend on the deposition method. As such, the technology used
(Whitehead et al., 2005; Whitehead et al., 2015), are not compa- to deposit the AMC on substrates also plays an important role in
rable to those results from direct observation of adhered bacteria the resulting rates of migration of the AMC into food. The avail-
after rinsing with water for 11 hr following the initial inocula- ability of multiple techniques to deposit coatings, the numerous
tion (Ludecke et al., 2016; Truong et al., 2010), nor those results materials of construction exhibiting antimicrobial activity, and the
for which the inoculation time is not reported (Schlisselberg & many units that express coatings’ mechanical properties leads to
Yaron, 2013), as bacterial population is a time-dependent quan- the conclusion that reported values of hardness for AMCs are the
tity. Therefore, comparisons among numerical values reported for only values suitable for comparison when analyzing the influence
attachment results from roughness studies should be done with of the deposition method on the mechanical properties of AMCs.
caution and with special attention given to the details of specific Overview of deposition methods. The deposition methods listed
experiments. in Table 21 are different, primarily in the way that the coating


C 2019 Institute of Food Technologists® Vol. 0, 2019 r Comprehensive Reviews in Food Science and Food Safety 21
Antimicrobial coatings for food contact . . .

Table 19–Comparison of results obtained in different studies relating surface roughness and bacterial attachment.

Gudmundsdóttir et al. (2006)


Ra (µm) Rz (µm) Rpk (µm) Microorganism Attachment (log/sample)
0.7 to 8 5.4 to 6.5 – L. monocytogenes and Serratia liquefaciens Approximately 1.8
0.16 to 0.22 1.3 to 1.9 – L. monocytogenes and S. liquefaciens Approximately 2.2
0.16 to 0.22 1.3 to 1.9 – L. monocytogenes and S. liquefaciens Approximately 2.2
Truong et al. (2010)
Ra (nm) Rq (nm) Rpk (nm) Microorganism Attachment (×104
cells/mm2 )
222 223 – P. aeruginosa 0.37
83 84 – P. aeruginosa 0.06
222 223 – S. aureus 31
83 84 – S. aureus 15
Schlisselberg and Yaron (2013)
Ra (nm) Rz (nm) Rpk (nm) Microorganism Initial attachment (cells/cm2 )
106 1,907 115 S. Typhimurium Approximately 110
30 301 41 S. Typhimurium Approximately 110
13 145 21 S. Typhimurium Approximately 35
4 67 8 S. Typhimurium Approximately 35
Ludecke et al. (2016)
Ra (nm) Rq (nm) Rpk (nm) Microorganism Surface coverage (%)
1.6 2.0 – E. coli Approximately 40
1.8 2.3 – E. coli Approximately 35
2.4 3.0 – E. coli Approximately 30
4.8 6.1 – E. coli Approximately 18
1.6 2.0 – S. aureus Approximately 55
1.8 2.3 – S. aureus Approximately 18
2.4 3.0 – S. aureus Approximately 29
4.8 6.1 – S. aureus Approximately 32
Ra : average roughness.
Rz : peak-to-peak height.
Rpk : reduced summit height.
Rq : square mean roughness.

material is transformed into a fluid, a solution, or a suspension to produced by subjecting the coated substrate to a high tempera-
make it suitable for coating substrate surfaces. For instance, elec- ture heating process (around 500 to 1,000 °C; Brinker & Sherer,
trodeposition requires the coating’s material of construction to be 1990). Another method, thermal spraying, uses melted particles
dissolved in the form of ions to allow their migration to the surface of the coating material of construction to form coatings by collid-
where they form the actual coating through a reduction–oxidation ing the particles with a target substrate (Tucker, 2015). When the
reaction initiated by an applied voltage (Myung, 2006). Because drops of melted material reach the substrate’s surface, they adhere
the coating is formed from dissolved ions and controlled with an and solidify, forming the coating. Therefore, the coatings obtained
applied voltage, the coatings can be fine-tuned to a high extent. in this manner tend to be lamellar (Bull, 2011). Finally, the spray-
However, the deposition of the ions cannot be directed, and the ing, dipping, and brushing methods are the simplest. Spraying and
particles randomly deposit on the surface, which can lead to the dipping are especially useful for the industrial application of poly-
formation of aggregates (Bull, 2011). A more recent technique, meric coatings and are also feasible options when the coating’s
vapor deposition, in general, and atomic layer deposition, in par- material of construction is heat sensitive (Zeno & Frank, 2013).
ticular, relies on the displacement of gaseous molecules of highly Figure 6 is a schematic representation of the various coating de-
reactive precursors (Londergan, 2006). A stoichiometric quantity position methods.
of another reactive component, such as water, is deposited on Overview of coating materials. The material of construction
the uncoated substrate. The gaseous precursor is then allowed to of the coating also affects its mechanical properties. Therefore,
reach the substrate where the precursor readily reacts with the pre- to obtain some useful insight on the influence of the deposition
viously deposited reactants. The reaction leads to the formation of method on the mechanical properties of coatings, the material of
a one-molecule thick coating on the substrate. When the process construction should be considered. Because TiO2 has been exten-
is repeated, uniform and fine coatings can be obtained, although sively studied as the main constituent of AMCs deposited using
the coating process can take several hours when relatively thick different methods, it was chosen as the main constituent of the
coatings are needed (Collins, 2012). Another method that uses a AMCs that are compared in Table 22. The direct comparison of
chemical reaction of precursors, the sol–gel method, can be in- values shown in Table 22 is not straightforward due to the vari-
terpreted as a liquid-state analog of the vapor deposition process ety of units employed to measure the same mechanical property
(Collins, 2012). However, the sol–gel technique does not allow (this comes from the diversity of characterization equipment and
control of the coating thickness at the molecular level, because the techniques available, shown in Table 13) and also because very
liquid components must first react until the desired microstructure few studies have been conducted to comprehensively assess the
in the gelled mixture has been achieved. The gel is then applied mechanical properties of AMCs. However, it can be observed that
on the substrate by dipping or spin coating. The final coating is sol–gel coatings are much more resistant to wear when annealed

22 Comprehensive Reviews in Food Science and Food Safety r Vol. 0, 2019 


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Antimicrobial coatings for food contact . . .

Table 20–Overview of the investigations where the surface topography has been modified to observe the effect on the adherence of microorganisms.

Topography
Surface Treatment characterization Detachment
Coating/surface treatment method method Microorganism determination Result Reference
Titanium on silicon Regularly Magnetron Atomic force S. aureus, P. Directly Cells were Whitehead et al.
spaced pits sputtering microscopy aeruginosa, observing the retained (2005)
and features and surface after according to
Candida rinsing with their size and
albicans water after the pits’ size.
30 min of
inoculation.
Stainless steel Untreated, – Stylus Mixed culture Swabbing and The three different Guobjornsdottir
polished, and profilometer of L. mono- plating after surface et al. (2005)
glass beaded cytogenes 120 hr of treatments
and Gram- contact time. showed the
negative same level of
bacteria cell attachment
Pure titanium Polished and Equal channel X-ray S. aureus CIP Counted directly Around two times Truong et al.
unpolished angular photoelectron 65.8 and P. from the more cells were (2010)
pressing spectroscopy, aeruginosa surface after attached to the
atomic force ATCC 9025 rinsing with polished surface
microscopy, and water after than the rough
optical 11 hr surface.
profilometry
Stainless steel Polished and Bright-Alum, Atomic force S. Ty- Counted directly Four times less Schlisselberg
unpolished electro microscopy phimurium on the coupon initial and Yaron
polishing, after sensing attachment on (2013)
and sand with saline Bright-Alum
polishing solution and electro
polishing
surfaces than
the other
treatments.
Polydimethylsiloxane Geometrical Soft Atomic force S. epidermidis, Directly Cell adhesion Perera-Costa
on silicon patterns lithography microscopy E. coli, and observing the reduction of et al. (2014)
B. subtilis surface after 30% to 45%
dipping the with respect to
coatings twice the smooth
in phosphate control surface
buffered
saline solution
after 30 min
of inoculation.
Gold, titanium, Different Magnetron Light scattering L. monocyto- Directly The topography Whitehead et al.
molybdenum, silver, coatings sputtering and atomic genes, E. observing the did not (2015)
and iron on silicon material force coli, and S. surfaces after influence
yielded microscopy aureus rinsing with microbial
different water after 30 adhesion.
topography. min of
inoculation
Titanium on glass Variation of Physical vapor Atomic force E. coli and S. Microscopy Adhesion Ludecke et al.
deposition deposition microscopy aureus observations reduction of (2016)
rate and after 1, 3, 5, 7, 56% for E. coli
coating 9, and 11 hr and 41% for S.
thickness aureus.

at higher temperatures. Çomaklı et al. (2014) reported increasing whether the wear and abrasion values come from the deposition
values from 7.9 to 11.5 GPa and from 176 to 206 GPa for hardness method, the composition of the coating, or a combination of those
and elastic modulus, respectively, when the annealing temperature two variables. Finally, a large difference between the hardness of
of TiO2 was increased from 500 to 900 °C. Çomaklı et al. (2014) coatings based on polymeric binders (Hung & Yemmireddy, 2015)
observed this same trend for abrasion and wear. This behavior is and sol–gel coatings can be observed. Sol–gel coatings are much
explained by the fact that TiO2 crystal structure shifts from the harder than polymeric coatings.
anatase phase to the rutile phase as temperature increases. It can
also be observed that sol–gel and dipping methods (specifically,
successive ionic layer adsorption and reaction) gave close values of Studies and Potential Applications of AMCs for Food
wear and roughness, although the same is not true for grain size. Contact Applications
Larger grain size resulted in harder and more wear-resistant AMC. The potential applications of AMCs can be classified based on
It should be noted that for this specific study, the dipping method five working principles that cover the entire range of interactions
was repeated 80 times to produce a coating of the same thickness with microorganisms that lead to the prevention of bacterial pro-
as that produced by the sol–gel method. Then, both coatings were liferation on FCS: anti-adhesion, antimicrobial-loaded, contact
annealed at 700 °C (Çomaklı et al., 2018). γ Al2 O3 /rutile TiO2 inactivation, photocatalytic, and multifunctional (Zhang, 2017;
coatings show comparable hardness values (Palanivelu & Kumar, see Table 23). Although several representative publications are re-
2014) to those found by Çomakli et al. (2018), but completely dif- viewed in this section and more have been mentioned in the pre-
ferent values for wear and abrasion. It is not possible to determine vious sections, only one study was identified where AMCs were


C 2019 Institute of Food Technologists® Vol. 0, 2019 r Comprehensive Reviews in Food Science and Food Safety 23
Antimicrobial coatings for food contact . . .

Table 21–Classification and overview of the methods used to deposit antimicrobial coatings on food contact surfaces.

Parameters
Deposition General working influencing Coatings’ Advantages of the Disadvantages of the
methods principle microstructure microstructure method method Reference
Electrodeposition Reduction of metallic Composition of the Fine-grained coating Extremely fine coatings Limited to metallic Bull (2011)
ions at the surface electrolyte, or three- can be obtained. Fine electrolytes. Inhibitors
of the substrate current intensity, dimensional particles can be can be added to control
(cathode) of an bath crystalline incorporated into the coating’s structure to a
electrolytic cell. temperature, and structures. coating. certain extent. Larger
presence of cracks on coatings are
growth inhibitors frequent.
on the substrate’s
surface.
Spraying, dipping, Usually, a liquid Composition of the Amorphous or Versatility to adhere to Limited to organic Zeno and Frank
brushing, and mixture of resins, liquid mixture, crystalline plastics and metal coatings. Limited (2013)
hand rolling. volatile carrier, and viscosity of the structures. surfaces. Relatively control over
additives are placed mixture, and Crosslinked or simple to apply. High microstructure. Some
on the substrate’s molecular weight branched coating speeds. coatings use flammable
surface where of the resins. structures. Possibility to solvents.
evaporation of the incorporate different
carrier enhances solid materials into
the completion of the matrix of the
polymeric reactions. coating.
Sol-gel: dipping Coating’s chemical Type and Porous, dense, and Coatings with high Precursors are limited to Brinker and
and spinning. precursors are concentration of geometrically surface areas certain metal oxides Sherer (1990)
mixed with polar precursors, ordered structures obtainable. Obtained components. Relatively
solvents, forming a solvents, and can be obtained. by liquid phase long process comprising
suspension (sol) catalysts, aging reactions at room of several steps. Some
that gelates (gel). time of gel, temperature or close precursors are
The gel is suitable dipping and to room temperature. hazardous materials.
for coating the spinning rates, Precise composition
substrate. and annealing of coating can be
temperature of obtained.
the gel.
Thermal spraying: The powder coating Degree of particle’s Flat, lenticular Extremely fine Coatings may contain Bull (2011)
flame, particles are heated melting, viscosity particles. microstructures can voids and oxidized
high-velocity up to their melting of the liquid, and Anisotropic be achieved. The particles. Not suitable
combustion, point and ejected wetting of the lamellar structure. crystal phase can be for flammable coatings.
and plasma. against the surface. controlled to a certain
substrate’s surface. extent. The coating’s
thickness can be
controlled precisely.
Vapor deposition: The coating’s Nucleation of the Anisotropic array of Very even, highly dense, Substrate’s surface Bull (2011)
atomic layer, components are components, closely packed uniformly distributed extremely clean before
physical, evaporated at surface structure, columns coatings can be deposition. Hazardous
chemical, and vacuum pressure and evaporation perpendicular to obtained. process due to
sputtering. and then rate. the surface. flammable vapors.
condensed on the Vacuum chambers are
substrate’ surface. needed.

tested under actual degradation conditions arising from the de- as a coating, its legal status corresponds to those AMCs with on-
contamination methods (namely, rinsing, washing with chemical going effects from the surface, namely, its migration into the food
agents, and brushing) that are routinely used on FCS at a brewing must be considered as contamination (see Table 1). This classi-
facility. However, the researchers concluded that the presence of fication can be avoided when repellent properties are induced
the AMC did not affect microbial populations occurring in situ by specific surface topography, although legal requirements man-
(Priha et al., 2015). date that surfaces must be both smooth and nonabsorbent (see
Table 10).
Anti-adhesion
The anti-adhesion working principle consists of modifying the Antimicrobial-loaded
FCS in such a way that the microorganisms are repelled from When the coating’s matrix is loaded with an antimicrobial agent,
the surface. The surface modification may consist of the appli- the antimicrobial substance must diffuse into the food and/or the
cation of polymers, such as polyethylene glycol (Desai, Hossainy, environment to be effective. The diffusive process may occur in-
& Hubbell, 1992), carboxybetaine polymer (Cheng et al., 2009), discriminately, as in the case of the simple release, or controlled
or the modification of the surface topography (Whitehead et al., by a stimulus, as in the controlled release mechanism of action
2005). Although it remains uncertain whether the hydrophobicity (Figure 7). In the simple release case, the AMC agent depletes
of surfaces made of uncoated FCS (namely, PVC, stainless steel, faster than the stimulation-sensitive AMC agent, where the ac-
natural rock, and so on) prevent bacterial adhesion, the applica- tive agent is mobile only when certain circumstances are met.
tions shown in Table 23 claim favorable results for S. epidermidis, Atefyekta et al. (2016) developed a highly porous TiO2 coating
S. aureus, and Pseudomonas when an active element (namely, the on stainless steel in which gentamicin, vancomycin, and dapto-
polymers) is applied to the FCS. This is in contrast to those cases mycin were embedded to prevent postsurgery infections after the
mentioned previously (see section “Hydrophobicity”), where the implantation of medical devices. The antimicrobial efficacy was
surfaces investigated were bare. Because the antimicrobial agent demonstrated against S. aureus and P. aeruginosa. The depletion
on the FCS is not intended to migrate into the food but remain time was not considered as part of their investigation. On the

24 Comprehensive Reviews in Food Science and Food Safety r Vol. 0, 2019 


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Antimicrobial coatings for food contact . . .

Figure 6–Schematic representation of the different coating deposition methods. (A) Electrodeposition: the substrate serves as a working electrode,
meaning that it is the electrode to be coated, while the counter electrode closes the electric circuit. The reference electrode is used to measure the
electrical potential (V) with the aid of an ammeter; the electric current (I) is generated by means of an electrical source. (B) Spraying, brushing, and
roller deposition methods all involve laying down a coating on the substrate through different mechanical means. (C) Thermal spraying uses a spray
gun to mix the coating material with the media supply, which increases the mixture temperature to the melting point of the coating material and
ejecting it to the substrate or target, where the coating material solidifies. (D) Sol–gel method: In the dip-coating technique, the substrate is
submerged into the gelled sol and pulled upward to form the coating due to the force of gravity and the force induced by the shear stress present, and
by the continued polymeric reactions occurring. In the spin-coating method, the force of gravity is replaced by centrifugal force that spreads the
coating material, originally dispensed at the center of the substrate, to its edges. Shear stress and polymeric reactions are responsible for the coating
formation.

other hand, a polypeptide coating was deposited on titanium to Photocatalytic


be released in response to the concentration of blood components AMCs based on the photocatalytic working principle aim to re-
(Kazemzadeh-Narbat et al., 2013). Both AMCs were intended for solve the issue of the depletion of the active substance. TiO2 is the
medical implant applications. Consider the case where these two flagship component of photocatalytic AMCs due to its high rate
coatings are applied to FCS: the migration of the active and in- of reactive oxygen species production (Li, Zhang, Niu, & Chen,
ert components of the AMC, namely, the TiO2 , the antibiotics, 2012). TiO2 and the other photoactive semiconductors, such as
and the peptide, into the food must be evaluated and compared zinc oxide (ZnO), magnesium oxide (MgO), and copper oxide
to the legal limits appearing in the corresponding regulations (see (CuO), require the simultaneous presence of a source of water
Table 11). and UV light to generate hydrogen peroxide (H2 O2 ), which is
Contact inactivation responsible for the antimicrobial effect. Priha et al. (2015) placed
The working principle of contact inactivation relies on the dam- stainless steel coupons coated with TiO2 on equipment in a brew-
age that certain long-chain molecules can exert on microorganisms ing facility to observe the effects of the cleaning procedures of
when the active molecules attached contact the microorganisms. the equipment on the wear of the AMCs. Although the coatings
Under this principle, the coating’s active agent must remain at- resisted the rinsing, washing, and brushing cleaning procedures,
tached to the surface to exert its antimicrobial action. Murata, the antimicrobial efficacy of the TiO2 could not be demonstrated
Koepsel, Matyjaszewski, and Russell (2007) describe their coating for the naturally occurring bacterial populations at the brewing
as a polymeric brush that disrupts E. coli cell walls due to surface facility. In this application, TiO2 must be approved by legislation
charges rather than the length of the polymer chains used to fab- as an antimicrobial substance exerting its effects from the surface
ricate the molecular brush. Glinel et al. (2009) also refer to their (see Table 11).
coatings as polymeric brushes that prevent biofouling and exhibit
antimicrobial activity due to the incorporation of magainin I into Multifunctional
the brushes. These coatings were successfully tested against Listeria The working principles described above can be combined into
ivanovii and Bacillus cereus. Peptide and magainin I are listed in the a single AMC to synergize the effects of individual working prin-
references given in Table 11, under the classification of substance ciples. For instance, Whitehead et al. (2015) modified the sur-
with ongoing effects from the surface. face topography of silver coatings to reduce cell attachment while


C 2019 Institute of Food Technologists® Vol. 0, 2019 r Comprehensive Reviews in Food Science and Food Safety 25
Antimicrobial coatings for food contact . . .

Table 22–Selection of mechanical properties measurements from different research groups’ investigations.a

Mechanical property
Deposition Surface Contact Abrasion and
method Coating topographyb angle wear Adhesion Hardness (GPa) Microstructure Migration Reference
Dipping TiO2 and – – 1.53 to 14.0 mg 2B to 4B 0.14 to 1.08 Compact structures, – Yemmireddy et al.
binders with or without (2015)
aggregates; 61% to
79% of TiO2
coverage area;
thickness: 50 to
107 µm
TiO2 Ra : 0.21 µm – Approximately – 7.8 Grain size: 21 nm; – Çomaklı et al.
anatase 1.75 × 10−3 thickness: 1.8 µm (2018)
and mm3 /Nm
rutile
Sol–gel TiO2 Ra : 0.19 µm – Approximately – 8.8 Grain size: 42 nm; – Çomaklı et al.
anatase 1.2 × 10−3 thickness: 1.8 µm (2018)
and mm3 /Nm
rutile
TiO2 Ra : 0.16 to – 2.5 to 8.5 × – 7.9 to 11.5 Thickness: 1.2 to 2.1 – Çomaklı et al.
anatase 0.23 µm 10−4 µm (2014)
and mm3 /Nm
rutile
TiO2 Ra : 10.17 to <5° – – – Thickness: – Atefyekta et al.
anatase 19.74 nm approximately 200 (2016)
and (0.5 × 0.5 to 700 nm; pore
antibi- µm) size: 4.0 to 7.08 nm;
otics pore surface
coverage: 18% to
42%
Thermal γ Al2 O3 - Ra : 8.94 µm – 6.9 × 10−9 17.34 N 5.45 Spherical particles – Palanivelu and
spraying 13wt% mm3 /Nm with Kumar (2014)
rutile agglomerations.
TiO2 TiO2 completely
melted, Al2 O3
partially melted.
TiO2 Rq : 10 to 39 10 to – – – Thickness: 0.9 to 1.6 – De Falco et al.
anatase nm 33° µm; grain size: 30 (2018)
nm
Vapor TiO2 – – – – – Grain size: 50 to 100 – Zhang, Cooke,
deposition anatase nm; thickness: Carmichael, and
and approximately 800 Parkin (2013)
rutile nm
TiO2 – – 0.5 to 1.5 wear 21.2 N 3.43 to 6.67 Thickness: 2.50 to – Chung et al.
anatase index 7.50 µm; columnar (2009)
grain
a Titanium dioxide was the only material of construction listed to allow for more direct comparison among the results obtained when the deposition method was changed.
b Values of R are not directly comparable.
a

inactivating L. monocytogenes, E. coli, and S. aureus by the release of Given this need, it is imperative that researchers have a good
silver ions. In another case, chitosan released from a photocatalytic understanding of the legal framework of AMCs used in FCS. A
ZnO coating was tested against Salmonella enterica, E. coli, and deeper understanding will allow researchers to set performance
S. aureus with positive results (Al-Naamani, Dobretsov, & Dutta, objectives during the initial design of the AMC, allowing the
2016). Although a good approach in theory, multifunctional coat- coating to be prepared in such a way that it meets as many of
ings are more complex to fabricate. In practice, it is simpler to the performance metrics as possible for real-world application.
obtain synergistic effects from different decontamination methods Unfortunately, many studies overlook this opportunity, resulting
(UV irradiation, washing with detergents, and so on) rather than in a lack of detailed studies examining the mechanical stability
trying to unite more than one working principle in a single AMC. and mechanical properties of AMCs in favor of demonstrating the
coatings’ antimicrobial effects. Although the antimicrobial activity
Conclusions is important, the AMC must be developed to maintain microbial
As this review discusses, the assessment of the antimicrobial levels under regulatory specifications, as a component working in
properties of AMCs for FSC is a necessary step to demonstrate tandem with processing conditions and other FCS decontamina-
the coatings’ effectiveness. However, this alone is not enough, tion methods.
particularly when researchers are interested in translating a novel Therefore, the AMC must be regarded not as an isolated el-
AMC to commercial applications. In these cases, the assessment ement that entirely solves the issue of microbial contamination,
must be made in conjunction with appropriate mechanical stability but rather, as an interacting element of a group of physical
tests under conditions similar to those of the expected application and chemical hygienic actions, of which the AMC must syn-
conditions, including those conditions that arise from the use of ergize with and withstand. The mechanical stability of AMCs
complementary decontamination methods. Doing so ensures that is explicitly constrained by national and regional legal require-
the AMCs under investigation not only meet the performance ments. AMC researchers/designers must remain aware of the
metrics required in terms of antimicrobial activity, but also comply composition and features allowed for the coatings in the re-
with the legal framework surrounding the use of AMCs for FCS. gions where it is expected to be applied to facilitate the

26 Comprehensive Reviews in Food Science and Food Safety r Vol. 0, 2019 


C 2019 Institute of Food Technologists®

Table 23–Selection of publications on antimicrobial coatings with potential applications for food contact surfaces.a

Substrate/Type of
Working principle Mechanism of action Limitations Working agent application Microorganism tested Reference
Anti-adhesion Passive repellence by changing Stability of the surface property Polyethylene glycol PET/Ongoing effect from S. epidermidis, S. aureus, Desai et al. (1992)
surface energy the surface and P. aeruginosa
Carboxybetaine polymer Glass/Ongoing effect P. aeruginosa and P. Cheng et al. (2009)
from the surface putida

C 2019 Institute of Food Technologists®


Surface topography Silicon/Ongoing effect S. aureus, P. aeruginosa, Whitehead et al. (2005)
modification from the surface and C. albicans
Antimicrobial-loaded Simple release. The antimicrobial Indiscriminate leaching of the Low molecular weight Stainless steel/Ongoing S. aureus and P. Atefyekta et al. (2016)
agent charged into coating’s antimicrobial substance. Depletion antibiotics effect from the surface aeruginosa
matrix transfers continuously until of the antimicrobial agent.
Antimicrobial coatings for food contact . . .

depletion Emergence of new resistant


microorganisms
Silver metal Glass/Ongoing effect E. coli, L. monocytogenes, Roldan et al. (2014)
from the surface C. perfringens, and B.
anthracis
Nisin, allyl isothiocyanate, Glass/Packaging Salmonella enterica Jin and Gurtler (2011)
and zinc oxide
Controlled release. The antimicrobial The optimal amount of release HHC-36 Titanium/Ongoing effect S. aureus and P. Kazemzadeh-Narbat et al.
agent charged into the coating’s depends on multiple factors. (KRWWKWWRR-NH2 ) from surface aeruginosa (2013)
matrix transfers in response to Depletion of the antimicrobial peptide
stimuli until depletion. agent. Emergence of new resistant
microorganisms
Ponericin G1 peptide Silicon/Ongoing effect S. aureus Shukla et al. (2010)
from the surface
Olygo (ethylene glycol) Silicon/Ongoing effect L. ivanovii and E. coli Laloyaux et al. (2010)
methacrylate from the surface
Contact inactivation Cell disruption by contact with active The coating’s action is mass-transfer Quaternary ammonium Glass/Ongoing effect E. coli Murata et al. (2007)
agent limited, to the layer which the polymers from the surface
antimicrobial agent reaches.
Magainin I peptide Silicon/Ongoing effect L. ivanovii and B. cereus Glinel et al. (2009)
from the surface
Photocatalytic Continuous generation of reactive Poor action under natural light. UV Titanium dioxide Stainless steel/Ongoing Acinetobacter sp., lactic Priha et al. (2015)
oxygen species to damage the light is required to enhance the effect from the surface acid bacteria, and
cell’s wall photocatalytic effect. enterobacteria
Zinc dioxide Glass/Ongoing effect S. aureus and E. coli ATCC Evstropiev et al. (2017)
from the surface 25922
Multifunctional A combination of two or more Optimization is not straightforward Silver metal and Silicon/Ongoing effect L. monocytogenes, E. Whitehead et al. (2015)
mechanisms of action topography from the surface coli, and S. aureus
modification
Chitosan and ZnO PE/Packaging S. enterica, E. coli, and S. Al-Naamani et al. (2016)
aureus
a Some of the coatings have been developed with medical applications in mind. Application types correspond to classifications given in Table 1.

Vol. 0, 2019 r Comprehensive Reviews in Food Science and Food Safety 27


Antimicrobial coatings for food contact . . .

EPA Environmental Protection Agency


F load
FCS food contact surface(s)
FDA Food and Drug Administration
GRAS generally recognized as safe
h indentation depth or displacement
H hardness
HDPE high density polyethylene
PE polyethylene
PET polyethylene terephthalate
PP polypropylene
PSD power spectral density
PTFE polytetrafluoroethylene
PVC polyvinyl chloride
R wear resistance
Ra average roughness
Rpk reduced summit height
Rq square mean roughness
Rz peak to peak height
S tangent line to nanoindentation up-loading curve
SEM scanning electron microscopy
STM scanning tunneling microscopy
TEM transmission electron microscopy
UV ultraviolet
Figure 7–Schematic illustration of the two different diffusion mechanisms
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