Green Chemistry: Sustainable Biodegradable Coatings For Food Packaging: Challenges and Opportunities

Green Chemistry
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Sustainable biodegradable coatings for food

Cite this: Green Chem., 2024, 26,
packaging: challenges and opportunities
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4934 a,b a,b

Fatemeh Jahangiri, Amar K. Mohanty and Manjusri Misra *a,b
This review article provides a thorough overview of barrier coating materials that have been used in food
packaging with a focus on biodegradable (bio-based or petroleum-based) materials, such as lipids, proteins,
polysaccharides, agriculture waste and polyesters. The goal is to provide an opportunity to acknowledge
progress made in this field, focusing on modifications made to coatings. These modifications aim
to address the shortcomings of biodegradable substrates (either plastic or paper) and improve their
performance, enabling them to compete with traditional petroleum-based food packaging materials. This
includes their barrier against water vapor and oxygen, mechanical and surface characteristics (sealability and
adhesion), as well as antimicrobial properties. The barrier of most biodegradable polymers underperforms in
comparison with petroleum-based non-biodegradable polymers, which possess either high water vapor
barrier or high oxygen barrier. Coating technology is a promising solution particularly in barrier improvement of
biodegradable polymers. Currently, there are only metallized, or inorganic nanosheet coatings available for bio-
degradable films that meet food packaging requirements. There are some challenges in this field, for example,
being able to retain the coating’s biodegradability despite applied modifications to improve it’s performance, the
large-scale fabrication of biodegradable coatings, the coating’s delamination and heat-sealability during service
time, and the migration of the coating into the packaged food. Moreover, green chemistry and its sustainability
Received 19th July 2023, needs in biodegradable polymeric coatings are also discussed regarding new ideas and possible directions for
Accepted 22nd January 2024
widespread application of coatings in food packaging. This is the first review that specifically summarizes bio-
DOI: 10.1039/d3gc02647g degradable coatings on plastic and paper substrates with a focus on coating modifications to improve the per-
rsc.li/greenchem formance of the base substrate to meet the required properties for food packaging applications.
1. Introduction the supply chain (∼17%),3 (IV) preparation and cooking and
(V) end-of-life.2 Food packaging is used worldwide to protect
1.1 From food waste to food packaging food against environmental contamination from outside
“We have woken up to plastic waste. Is food waste next?” (Liz sources such as odors, gases, aromas, humidity, light, physical
Goodwin).1 It is time to take the pledge to choose the health of damage, and microorganisms.4–6 Also, food packaging is the
our planet over plastic. Nowadays, it is evident to all that main contributor to ensuring the safety and quality of food, as
plastic waste has dreadful consequences for our planet. well as prolonging its shelf life, thereby lessening food wastage
Additionally, we are facing another equally urgent waste issue, and losses.6,7
which is food. According to the world counts website, one- Overall, plastic polymers, which are not biodegradable,
third of the world’s food is not only never consumed, but is have the largest amount of usage in the food packaging
wasted in each step of the food life cycle.2 This includes (I) industry.8,9 Petroleum-based plastics (e.g., polyvinyl chloride
agricultural production such as crops, that can be damaged in (PVC), polypropylene (PP), polyvinylidene chloride (PVdC),
farms by pests, diseases and factors linked to the weather, soil, polyethylene (PE), high- and low-density polyethylene (HDPE
climate, water availability, and natural disasters resulting in and LDPE), polystyrene (PS) and polyethylene terephthalate
1.2 billion tonnes of food waste per year ∼15%,3 (II) processing (PET)) are still commonly used in food packaging, while most
and manufacturing (food waste of ∼5%),3 (III) storage and dis- never see a second life and are associated with environmental
tribution that is food waste from retail to consumer stages of concerns.10 To be more precise, the biodegradation rate of pet-
roleum-based plastics ranges from tens to thousands of
a
years.11 In addition, these plastics can enter the ocean and bio-
School of Engineering, Thornbrough Building, University of Guelph, Guelph,
Ontario, N1G 2 W1, Canada. E-mail: [email protected]
degrade into microplastics, which end up in the stomach of
b
Bioproducts Discovery and Development Centre, Department of Plant Agriculture, marine organisms and eventually enter the human food
Crop Science Building, University of Guelph, Guelph, Ontario, N1G 2 W1, Canada chain.11 This is what triggers the urgent need for bio-
4934 | Green Chem., 2024, 26, 4934–4974 This journal is © The Royal Society of Chemistry 2024
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Green Chemistry Critical Review
degradable materials. The planet and its inhabitants would proposed in the available literature, for instance, development
benefit significantly from the prompt discovery of environmen- of biobased films and coatings,7,17 incorporation of nano-
tally friendly and sustainable alternatives to traditional plastic particles (e.g., reinforcement of biopolymers with nanoclay17,19),
food packaging materials. chemical modification20 (e.g., grafting fatty acid to improve the
water vapor barriers21), physical modification (e.g., heat treat-

1.2 Development of biodegradable food packaging – ment and irradiation22), and blending two or more biobased
limitations and strategies materials23 (Fig. 1). Among the aforementioned strategies, coat-
As reported by the IUPAC, “a bioplastic is a biobased polymer ings could add several advantages to the substrate such as resis-
derived from the biomass or issued from monomers derived tance against permeation of gases (i.e., O2, CO2), water vapor,
from the biomass and which, at some stage in its processing aromas, volatile organic compounds (VOCs), oils, and light (i.e.,
into finished products, can be shaped by flow”. Notably, using UV radiation). Furthermore, coatings can enhance the mechani-
the term bioplastic is discouraged, since it represents that any cal (e.g., friction resistance, tensile strength, and scratch resis-
polymer produced from biomass is ecofriendly. Hence, the tance), optical (gloss and haze), surface (adhesion and sealabil-
IUPAC proposes the term “biobased polymers”.12 Utilization of ity) and thermal (e.g., flame barrier) properties of the base sub-
biobased polymers as food packaging materials has seen strate. Finally, coatings can provide new functions for the packa-
various functional limitations over the past years, such as brit- ging such as antibacterial or antimicrobial properties.7 An “anti-
tleness, difficult heat sealability, thermal instability, low melt bacterial” material is defined as a substance that interferes with
strength, and poor barrier characteristics (i.e., high permeability bacterial growth and survival by selectively destroying bacteria.24
to water vapor and oxygen)13–16 (Fig. 1). These shortcomings In contrast, “antimicrobial” is a broader term, encompassing
restrain them from being a viable substitute for petroleum- materials that inhibit the growth of various microorganisms,
based plastics in food packaging applications.17,18 To enrich the including bacteria, fungi, and algae.25 Biobased coatings could
functional properties of biobased polymers, particularly barrier be made from different biopolymers, namely polyesters, poly-
capacities against gasses and water, several strategies have been saccharides, lipids and proteins (Fig. 1).
Fatemeh Jahangiri is currently Prof. Amar Mohanty is a

pursuing her PhD in the School Distinguished Research Chair in
of Engineering at the University Sustainable Biomaterials at the
of Guelph, under the supervision Ontario Agriculture College and
of Dr Amar K. Mohanty and the Director of the Bioproducts
Dr Manjusri Misra. She obtained Discovery and Development
her Bachelor’s and Master’s Centre. He is a Professor in the
degree in Pure Chemistry Department of Plant Agriculture
(2012–2016) and Polymer and School of Engineering at the
Chemistry (2016–2019), respect- University of Guelph, Ontario,
ively, at the University of Tehran, Canada. Dr Mohanty is the
Iran. Her PhD research focuses Editor-in-Chief of Sustainable
Fatemeh Jahangiri on development of biobased and Amar K. Mohanty Composites @ Composites Part
biodegradable coatings for food C – Open Access. He is one of
packaging applications. Her goal is to extend the shelf life of pack- the most cited researchers worldwide with more than 800 publi-
aged food by enhancing the barrier performance of biodegradable cations to his credit, including 475 peer-reviewed journal papers,
packaging materials. Successful completion of this project will 70 patents (awarded/applied), 6 edited books, 30 book chapters,
reduce our reliance on petroleum-based materials by providing a 300+ conference papers and over 160 plenary and keynote presen-
sustainable alternative where agricultural residues are used for tations. His Google-Scholar citations count is 56 271 and h-index
high-end value-added products in support of the circular economy. 109 (February 18, 2024). He has received many awards, the most
recent one being the prestigious Miroslaw Romanowski medal of
2021 for his significant scientific contributions to the resolution of
environmental problems from the Royal Society of Canada. He
also received the Synergy Award for Innovation from Natural
Sciences and Engineering Research Council of Canada (NSERC),
the Andrew Chase Forest Products Division Award from the
American Institute of Chemical Engineers (AIChE) and the
Lifetime Achievement Award from the BioEnvironmental Polymer
Society (BEPS).
This journal is © The Royal Society of Chemistry 2024 Green Chem., 2024, 26, 4934–4974 | 4935
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Critical Review Green Chemistry

Fig. 1 Biobased polymers’ limitations and strategies for food packaging applications.
1.3 Development of green coating alternatives to petroleum-

based coating
Synthetic polymeric barrier coating materials, such as poly-
Manjusri Misra is a professor fluoroalkyl (PFA) substances-coated paper wraps and epoxy-
and Tier 1 Canada Research based resin (bisphenol-A (BPA))26-coated canned goods cannot
Chair (CRC) in Sustainable be recycled or repulped and can have harmful effects on
Biocomposites in the School of human health.27,28 Polyvinyl alcohol (PVA) is a more environ-
Engineering and holds a joint mentally friendly option that is widely used as petroleum-
appointment in the Department based biodegradable coatings for flexible/rigid paper packa-
of Plant Agriculture at the ging to protect food against oxygen permeation.29 Bio-based
University of Guelph. She is also non-biodegradable polymers such as bio-polyethylene (Bio-PE)
the Research Program Director of and bio-polyethylene terephthalate (Bio-PET) have rarely been
the Bioeconomy Panel for the used as coatings for food packaging applications, and have not
Ontario Agri-Food Innovation been commercialized. An example of this application is the
Alliance, a program between the development of oxygen scavenger multilayer films using Bio-
Manjusri Misra Ontario Ministry of Agriculture PE as the food contact layer incorporating gallic acid as the
and Rural Affairs (OMAFRA) and oxygen scavenger.30 The greatest number of bio-based bio-
the University of Guelph. Dr Misra completed her Bachelor’s, degradable barrier coatings come from proteins, polysacchar-
Master’s, MPhil and PhD from Ravenshaw College at Utkal ides, lipids, and their composites.7 Protein coatings such as
University in India focusing on Chemistry with a specialization in the zein-based coating from FloZein Products31 have been
Polymer Chemistry and Natural Fibers during her graduate applied on cardboard containers for greasy food, on fresh/dried
program. Dr Misra’s current research focuses primarily on novel fruits and vegetables to provide a long-lasting moisture and
bio-based composites and nanocomposites from agricultural, for- microbial barrier as well as on fresh fish/meat to reduce oil
estry and recycled resources for the sustainable bioeconomy absorption during frying. Gum ghatti is a complex polysacchar-
moving towards the Circular Economy. She has authored more ide used in the paper industry as a moisture barrier coating.32
than 750 publications, including 450 peer-reviewed journal Paper and paperboard coated with Solenis TopScreen biowax
papers, 30 book chapters, and 55 patents. She was the editor or barrier coatings are available in the market. They are repulpab-
co-editor of 6 books in the area of biocomposites and nano- able, recyclable, and industrially compostable with EN 13432
materials. In 2020, she was selected as one of Canada’s Most certification.33 However, to the best of our knowledge, there are
Powerful Women: Top 100 Award Winner in the Manulife Science no other wax coating materials tested as biodegradable. More
and Technology category from the Women Executive Network. She research is needed to perform biodegradability tests on natural
is a Fellow of the Royal Society of Chemistry (UK), the American wax coating materials to ensure their biodegradability strictly
Institute of Chemical Engineers (AIChE), and the Society of Plastic under ASTM, ISO, European standard methods. Polyesters are
Engineers (SPE). also used as coatings for food packaging applications. For
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Fig. 2 Transition from synthetic non-biodegradable coatings to biobased biodegradable coatings for food packaging applications.
example, poly(lactic acid)-coated paper has been commercia- substrate. Various materials are used as a coating such as bio-
lized as stand-up bags for dried fruits, pulp molded trays and based biodegradable biopolymers (i.e., lipids, proteins, poly-
paper glasses for cold liquids.34 Polyhydroxyalkanoates and saccharides, biomass, and agriculture waste), bacterial poly-
starch-based aqueous coatings have shown odor/taste protec- mers (i.e., polyhydroxyalkanoates), and synthetic bio-
tion, oil/grease resistance, and gluability/heat sealability. degradable polymers ( polybutylene adipate-co-terephthalate
Nevertheless, aqueous coatings cannot provide high water/ (PBAT), polycaprolactone (PCL), polybutylene succinate (PBS)),
water vapor barrier properties.34 Overall, in both academic and which are reviewed in this paper. Through reviewing the pre-
industrial sectors, a significant transition is evident, moving vious strategies used to develop biodegradable coating
away from synthetic non-biodegradable coatings towards biomaterials, the pros/cons and efficiency of different coating
based, biodegradable alternatives (Fig. 2). Ongoing endeavors methods and the challenges of their commercialization are
are focused on improving the performance of environmentally summarized to guide the future design of coatings’ modifi-
friendly coatings for applications in food packaging. cations, widening their commercialized applications.
In summary, the development of biodegradable packaging
materials has attracted interest worldwide, as it is known to
lessen the environmental impact associated with traditional 2. Principle and stratagem to
petroleum-based plastic packaging. Nevertheless, getting developing green coatings
sufficient properties from biobased biodegradable polymers
that are required for food packaging applications is challen- One of the main strategies for improving the barrier properties
ging. Various technologies are being developed to compensate of biodegradable food packaging is surface coating. In prin-
for the biobased biodegradable deficiencies and enrich their ciple, applying an additional thin layer on one or both sides of
functional properties to be able to compete with traditional bio-based films or other packaging materials (i.e., paper,
plastic packaging. Coatings serve as an emerging technology to paperboard) is defined as a coating process.17 There are
improve the functional properties of the biodegradable sub- various coating techniques including chemical/physical
strate, particularly regarding barrier properties against oxygen vacuum deposition, solution coating (e.g., layer-by-layer assem-
and water vapor, thereby improving food shelf life. The manu- bly, slot-die coating, brush/bar coating, spray coating, spin
facture of paper, paperboard, cellulose thin films, plastic coat- coating and dipping), electrohydrodynamic processing (e.g.,
ings, fibrous fabric sheets, metallic foils, etc. are some of the electrospraying, electrospinning) and other techniques such as
main applications for coating technology. Using this techno- melt extrusion coating and hot pressing (Fig. 3). Coating tech-
logy, two or more layers with specific and complementary pro- niques are more versatile than lamination or coextrusion in
perties can be combined (i.e., multilayer) to obtain a single- terms of manipulating or developing multilayer structures
layer structure, resulting in enhancing the performance of the with different thicknesses from nano to millimeters.35
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Fig. 3 Different coating techniques for the preparation of single-layer or multilayer coatings. Schematic figures are adapted from the following
references. (A) Electrohydrodynamic processing including electrospinning, electrospraying; reproduced from ref. 46 with kind permission from John
Wiley and Sons, copyright 2020, open access. (B) Chemical vacuum deposition (CVD) is redrawn by the authors from ref. 47 with kind permission
from RSC, copyright 2016. Other techniques include (C) extrusion coating and (D) hot pressing48 and solution coatings including (E) layer-by-layer
assembly, (F) casting; (figure C–F are reproduced from ref. 48 with kind permission from Taylor & Francis, copyright 2021). (G) Slot-die coating,
reproduced from ref. 49 with kind permission from John Wiley and Sons, copyright 2020, open access. (H) Spin-coating, (I) spray-coating and (J)
dip-coating (figure H–J are reproduced from ref. 50 with kind permission from Springer Nature, copyright 2021, (license number 5581701004745)).
Coating materials include inorganic nanoparticles, small It is noteworthy that, although coatings and films are some-
organic molecules, and different macromolecules. Different times used as equally the same, their method of application is
coating materials and coating techniques along with their thoroughly different. A material that is obtained as a stand-
advantages/disadvantages have been reviewed and summar- alone solid laminate followed by applying it to foodstuff (or a
ized in previous literature.34–38 Here we have reviewed the coat- substrate e.g., paper/paperboard and biobased polymers) is
ings derived from specifically biodegradable polymers for known as a film. However, a coating is applied to food stuff (or
paper/plastic substrate and their corresponding modifications paper/paper board and biobased polymers) via a method that
to improve the performance of the substrate. may or may not contain a liquid and is not a stand-alone
In the biodegradable polymer field, coating technology structure.44,45 In the literature, this differentiation in defi-
can be divided into two categories: (1) coating a high nition has only been highlighted for edible films and coatings
barrier layer onto the biodegradable polymer film/sheet, and on food as the substrate. In the above description, we general-
(2) coating the high barrier biodegradable polymer (e.g., ized it to other substrates as well.
polyhydroxybutyrate-co-hydroxyvalerate (PHBV), bionanocom-
posites or waxes) on the paper/paper board. The interfacial
interactions between the substrate and the coating material 3. Different types of biodegradable
can significantly affect the barrier of the whole structure,
because the separation of coating and the matrix results in
coatings and their modifications
poor oxygen/water vapor barrier of the whole structure. 3.1 Coatings from nature
Interactions of molecular assembly deriving forces such as 3.1.1 Lipid-based coatings. A summary of all biopolymers
electrostatic39 and hydrogen bonding,40,41 corona treat- from nature that can be used as coating materials is shown in
ment,42 and silane hydrolysis43 have been studied so far to Fig. 4, which will be discussed throughout section 3.1.
improve the interface adhesion between the coating material Lipid-based materials have great potential in biopackaging
and the substrate. applications, due to their hydrophobic nature, which results in
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impressive barrier properties against moisture transfer.7,52 Functional properties, including barrier properties, of coat-
Lipid compounds are extracted directly from biomass originat- ings derived from lipid compounds are influenced by their
ing from animals, insects, and plants, which are considered chain length, saturation degree, physical state, structure (e.g.,
natural sources.44 degree of polarity), crystal dimensions, lipid distribution into
Lipids contain diverse functional groups such as mono-, di- the coating (e.g., homogeneity or heterogeneity), as well as
and triglycerides, fatty acids, fatty alcohols, phospholipids, ter- humidity and temperature.52 The high resistance of wax coat-
penes and cerebrosides.44,52 Fig. 4 shows the most common ings is due to either their hydrophobic nature (absence or low
lipids that have been used in coating formulations for food number of polar groups) or their molecular organization
packaging applications. Lipids, which are composed of fatty (waxes possess a tight orthorhombic crystalline arrangement,
acids, originate from vegetable oils, essential oils, and natural in which their direction is perpendicular to the gas flow and
waxes (e.g., candelilla or carnauba wax, and beeswax).44 therefore do not allow the gas transfer)58 (Fig. 5).
Soybean oil,53 corn oil,54 and sunflower oil55 are some of the Beeswax coating on whey protein isolate-cellulose (WPI-cell-
most common vegetable oils that are used as coatings for food ulose)-based film decreased the water vapor transmission rate
packaging applications. Among other lipid compounds, the (WVTR) by 92–95%, and was then coated on commercial cereal
high hydrophobicity of waxes makes them the most efficient box paper board.60 Although WPI has a good film-forming
barriers against water vapor permeation.7,52,56 property, its high WVTR in the presence of plasticizers limits
Pure lipid coatings are not commonly used as they are its applications. Incorporating a lipid component is a smart
mechanically weaker and have low structural integrity in modification for achieving a high barrier against moisture. A
contrast with proteins and polysaccharides.52 In this regard, biodegradable starch-based glue was used as an interfacial
composite coatings derived from hydrocolloids ( proteins or adherent between beeswax and the WPI layer.60 Biodegradable
polysaccharides) and lipids are more advantageous than the trays of thermoplastic starch/polylactic acid (TPS/PLA) coated
addition of lipids into proteins and polysaccharides, as the with 1% beeswax in ethyl alcohol and Tween80 emulsion
latter may cause low strength.52 Lipids play the role of a showed the lowest solubilisation capacity in water, which con-
barrier against moisture transfer and hydrocolloids play the tributed to water vapor permeation (WVP) being reduced by
role of a supporting matrix and provide a barrier against 97.46%.61 The concentration of beeswax emulsion showed a
gases in the composite structure. Lipids and hydrocolloids significant effect on the water vapor barrier properties of the
are processed by making either bilayers or emulsions52,57 trays, in which using 2–3% beeswax emulsion caused an
(Fig. 5). inferior adherence to the substrate and delamination.61 PLA
Fig. 4 A categorization of biopolymers obtained from biomass. Biopolymers are categorized in three main groups, namely proteins, lipids and poly-
saccharides. Some examples are shown under each categorization followed by their origin underneath. The typical chemical structure of each group
is drawn in ChemDraw by the authors. Proteins are made of a major building block called alpha amino acid. Triglycerides are the most common type
of lipids. Finally, polysaccharides are long chains of monosaccharides, of which the most common is glucose. Figure is redrawn from ref. 51, with
some added components by the authors with kind permission from MDPI, copyright 2020, (open access).
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Fig. 5 Characteristics of lipid-based coatings including their natural properties, processes of making coatings from lipids, their main functions and
factors affecting their functions. Data of iodin values for different types of oils are from ref. 59.
films coated with a crosslinked chitosan/beeswax layer had an Box 1 Biobased and biodegradable coating based on
increased water vapor/oxygen barrier as well as abrasion resis- waxes: Limitations and strategies
tance through a reduction of swelling in PLA films. This Limitations:
resulted from the crosslinked chitosan, which showed more • In solution coating methods, waxes are dissolved in a
profound effects on oxygen transmission rate (OTR) reduction. solvent, which is either chlorinated or non-chlorinated
A layer of beeswax coating reduced the WVTR further. hydrocarbons.64 To produce a sustainable biobased and
However, there was not a significant difference in OTR biodegradable coating, “green” solvents such as water,
between samples with or without beeswax coating.62 supercritical fluids, ionic liquids, liquid polymers and
Hydroxypropyl methylcellulose incorporating beeswax coatings biomass-derived solvents65 should be used.
showed improved moisture barrier from 20 to 50% compared • Most waxes have a low melting point (e.g., beeswax
to the formulation without beeswax. By increasing beeswax 45.5–70 °C,66 candelilla 54.5–76 °C (ref. 66)) and can
content from 20 to 60%, the moisture barrier improved signifi- leach away easily, which is a disadvantage for thermal
cantly, while the oxygen barrier and mechanical properties stability of coatings.
reduced.63 When considering materials with high hydro- • By increasing the wax content of the coating composition,
phobicity, particularly for use as robust barriers against water one can reduce water vapor permeation (WVP) for the packa-
vapor, waxes are the primary substances that come to mind.64 ging material; however, poor adhesion of waxes to the sub-
Nevertheless, there are still some issues that need to be con- strate limits their viable concentration in coating formulations.
sidered to create fully biobased and biodegradable coatings • A slight change in temperature can cause waxes to
based on natural waxes (Box 1). The strategies that have been become soft or brittle and suffer from low abrasion resis-
addressed in the literature are also summarized in Box 1. tance once coated on the substrate.64
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• The biodegradability of waxes needs to be studied formed in one step with no additional diluent, solvent, or oil
specifically according to standard methods, to ensure emulsifier. The film formation mechanism for polymeric solu-
the biodegradability of the whole packaging material tions through evaporation of the solvent/water results in volume
after being coated by natural waxes. A small number of shrinkage and film deformation or unwanted coating cracks on
studies have reported the effect of wax coating on biode- the surface.74 To increase the shelf life of guavas, coatings
gradability of the packaging material67 based on stan- based on cassava starch incorporating beeswax as a hydro-
dard methods. The biodegradability should be ≥90% (by philizing agent and sunflower oil as an emulsion former for
respirometer) after maximum 180 days for a material to coating formulations were developed. The coatings showed
be considered biodegradable (ASTMD6400). improved barrier against moisture and increased the guavas’
Strategies: shelf life.75
• Low melting point of waxes can also be considered as
Another category of lipid materials are essential oil com-

a positive aspect, as they can be easily emulsified with pounds derived from plants; these are known as naturally
water instead of using hydrocarbon solvents.64 occurring oils that have antimicrobial benefits.76 For example,
• To tackle the leaching problem of waxes, they can be cinnamaldehyde, a main ingredient of cinnamon bark oil,
mixed with other hydrophobic polymers such as polydi- showed antibacterial, antifungal, antiparasitic, insecticidal,
methylsiloxane68 for encapsulation and improve wax antiviral, anti-diabetic, anticancer, and pro-wound healing pro-
stabilization. In this regard, the wax’s desire to migrate perties.77 A summary of lipid-based coatings used to improve
to the surface results in improved coating barrier properties is listed in Table 1.
hydrophobicity.64 3.1.2 Protein-based coatings. In this section, we have sum-
• Dispersion of wax in alcohol is another positive point, marized a list of breakthroughs in protein-based coatings for
as it allows other polar compounds to be processed in food packaging applications. Protein-based coatings are
alcohol along with waxes.64 divided into two categories: proteins from plants and animals;
• By altering the crystallization of wax, it can act as a wheat gluten (WG), corn, soy proteins and zein as plant pro-
coating with rough surface similar to the lotus leaf.64 teins, and casein, whey, keratin, and gelatin as animal proteins
(Fig. 4). Biopolymers based on proteins are the most effective
due to their high gas barrier properties comparing with poly-
Oils derived from a wide range of annual plant seeds have saccharides and lipids. Soy-protein-based films showed 260-,
been used in the coating industry for centuries.71 The high 540-, 500- and 670-times reduced oxygen permeability in com-
importance of seed oils lies in their low cost, high availability, parison with low-density methyl cellulose, starch, polyethylene
renewability, and their high annual production across the and pectin, respectively. In addition, films based on proteins
world. Seed oils contain triglyceride molecules (Fig. 6) mixed possess better mechanical properties than those based on
with different fatty acid residues. The most common seed oils lipids or polysaccharides.79 The challenge of protein-based
are derived from soybean, tung, corn, linseed, and castor.72 coatings is their brittleness and intrinsic hydrophilicity, which
Fig. 6 shows the typical seed oil’s chemical composition con- causes poor barrier properties against water vapor.
taining esterified glycerol with 3 molecules of fatty acids as The strategies addressed for the above challenges of
well as the normal fatty acid composition of several of the protein-based coatings are categorized as follows in the pre-
most often used seed oils, along with their chemical designa- vious literature:80 (I) chemical modification of proteins using
tions, which are either saturated or unsaturated. In addition, chemical agents (e.g., glutaraldehyde, CaCl2) or inserting func-
fatty acid chains can contain various functional groups, such tional groups into protein side chains to form covalent and
as epoxy or hydroxyl. Fatty acid distribution determines the non-covalent crosslinking to improve their mechanical pro-
chemical/physical properties of seed oils. To explain further, perties; (II) addition of another polymer (e.g., chitosan, cell-
the position and number of CvC double bonds within the ali- ulose, alginate) or a plasticizer (e.g., sorbitol, glycerol) to
phatic chain has a noticeable effect on the final properties of improve their mechanical barrier properties and reduce costs;
the oil.73 The amount of iodine reacted by the double bonds in (III) addition of natural antioxidant (e.g., vitamin E) and anti-
100 g of oil corresponds to the average degree of unsaturation microbial agents (e.g., nisin) to proteins to improve the shelf
determined by the iodine value. There are three classifications life of packaged food; and (IV) modification of the protein’s
for oils depending on their iodine value,59 shown in Fig. 5. surface with lipid molecules, polysaccharides or proteins to
In industry, it is preferred to produce coatings with low improve barrier properties and interface adhesion. Protein-
solvent content. For instance, reducing the viscosity of the based coating/film processing is based on two standard
polymer is effective in decreasing the organic solvent content approaches: firstly, the “wet or solvent process”, in which pro-
in the coatings. Polymers with a narrowed molecular weight teins are dispersed or solubilized in a solvent, and secondly,
distribution or those with a low molecular weight can be used the “dry process”, which is based on forming a thermoplastic
to produce a low-viscosity coating composition.71 Moisture- followed by casting81 (Fig. 7).
resistant paper was prepared by coating silylated soybean oil The coating of plasticized whey protein over a commercial
(53.1% reduction in WVTR), which did not show any changes compostable plastic film based on PLA improved the resistance
in the oil’s viscosity and therefore the coating process was per- of PLA against oxygen permeation by 84.37%. Any modifications
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Fig. 6 (Top) Example of an unsaturated triglyceride in vegetable oils, which is composed of glycerol and fatty acids (figure on the top is redrawn
from ref. 69 with kind permission of the website owner). (Bottom) Chemical structure of some common fatty acids (figure on the bottom is redrawn
by the authors in ChemDraw from ref. 70 with kind permission from RSC, copyright 2010).
including denaturation, additive blending or crosslinking in (WG)-based multilayer system, PLA-WG-PLA (Fig. 8a and b).
natural polymers can influence their ultimate biodegradability. Moreover, WG coating thickness had a non-linear relationship
The biodegradability test revealed that the denatured whey with oxygen permeation (OP) (Fig. 8c), showing an exponential
protein within plasticizer degraded quickly even after applying decrease for thicknesses below 10–20 μm. The compatibility of
it to the commercial PLA film (i.e., fully mineralized during 20 PLA and WG layers in the fabrication of multilayers was
days of the test performed in liquid medium).82 Modification improved by hot pressing as well as a corona treatment. The
of whey protein isolate (WPI) with montmorillonite nanoplate- interface adhesion between layers is defined as the work of
lets and plasticizer (glycerol or sorbitol) produced WPI-based adhesion (Wa), which has determined values according to the
nanocomposite coatings with improved barrier against oxygen applications (Table 2). In a similar study using PLA-WG-PLA
permeation, while the elongation was reduced.83 laminate with hot-pressing, Cho et al.84 obtained Wa values that
Rocca-Smith et al.42 boosted the barrier properties of PLA were 2 orders of magnitude higher. However, they prepared WG
against water vapor and oxygen by developing a wheat gluten layers without using solvent as opposed to Rocca-Smith et al.42
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Table 1 Summary of lipid-based coatings
%Barrier improvement
Lipid-based coating and substrate Modifications Coating method WVP/WVTR/OP Ref.
Whey protein isolate-cellulose film- Using glutaraldehyde as crosslinking agent and Melt-brush coating 92–95% reduction in 60
coated beeswax for coating on glycerol as plasticizer and heating WVTR
paperboard compression
Beeswax-ethyl alcohol emulsion- Using Tween 80 as emulsifier Immersion coating 97.46% reduction in 61
coated trays of thermoplastic starch/ WVP
polylactic acid
Crosslinked chitosan/beeswax layer- Corona treatment of PLA surface, crosslinked Coating applicator 100% reduction in 62
coated PLA film chitosan with sodium tripolyphosphate prior to and hot melt roll WVTR
beeswax coating coater 23.77% reduction in
OTR
Hydroxypropyl methylcellulose Using glycerol as plasticizer Immersion coating 20–50% reduction in 63
incorporated with beeswax-coated WVP
plums Improved shelf life of
plums
Silylated soybean oil-coated paper Silane treatment of soybean oil by Laboratory roll-lab 53.1% reduction in 74
vinyltrimethoxysilane coater WVTR
Cassava starch incorporated with Using saponificated sunflower oil as surfactant Immersion coating 39% reduction in 75
beeswax-coated guavas (emulsion former of coating solution) WVTR
Improved shelf life of
guavas
Cinnamaldehyde-incorporated — Dip-coating Antibacterial properties 77
natural plant poly phenol coating
Epoxidized soybean oil and ZnO Epoxidized soybean oil cured with sebacic acid Dip-coating Reduced wettability 78
nanoparticle-coated paper/fabric as adhesive component, using stearic acid as and high
low energy modifier hydrophobicity
Fig. 7 Protein-based coatings, their properties and common processes as well as strategies for modification of proteins to improve their
performance.
This was explained by a hypothesis on evaporation of residual Zein and gelatin have been also extensively used for devel-
solvent, which could have an adverse consequence on the com- oping biodegradable coatings. Zein’s features include plas-
patibility and adhesion of PLA and WG layers. ticity, heat sealability, biodegradability13 and intrinsic hydro-
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Fig. 8 (a) Schematic of multilayer laminate PLA/wheat gluten (WG)/PLA and representative resistance against oxygen and water vapor permeation, (b)
the cross-section SEM image of multilayer laminate with total thickness of 60 μm, in which WG is 20 μm, (c) OP of multilayers versus WG coating thick-
ness (figure a–c are reproduced from ref. 42 with kind permission from ACS, copyright 2019, open access). (d) Stress–strain curve of PLA, bilayers and
Pickering emulsion films as well as confocal laser scanning microscopy (CLSM) of Pickering emulsion films (selective exciting either Nile blue A (red,
zein) or Nile red (green, oil) was used to take the micrographs), reproduced from ref. 89 with kind permission from Elsevier, copyright 2018.
Table 2 Theoretical work of adhesion for some of the industry film/

linker. The water resistance of PHA-coated films significantly
coating applications. Data are reported from ref. 90 improved, and crosslinked zein fibers maintained their fibrous
structure after 12 days of immersion in water.86 The intrinsic
Theoretical work of adhesion hydrophilicity of gelatin has restricted its application in food
Industry application value (Wa) packaging.87 Laminating gelatin with other polymers was
Latex painting applications to surfaces More than 70 mN m−1 reported to address this issue.87,88 Fish gelatin was used to
Organic applications to metals Around 65 mN m−1 develop multilayers of PLA/fish gelatin/PLA with improved
Printing paper and polymer films 60 mN m−1
oxygen barrier properties compared with neat PLA. The PLA
surface was modified by corona discharge to improve the inter-
face adhesion between layers. Fish gelatin was modified using
phobicity due to a high content of nonpolar amino acids.85 glycerol reinforced with CNC and antioxidant extract from
Therefore, it can be a better moisture barrier than other almond shell by-products. Hydrogen and covalent bonding
protein-based biopolymers.13 Although zein-based films are between the antioxidant and gelatin improved the ductility.87
reported to have great stability in high humidity and heat, they In similar work, fish gelatin’s water vapor permeability was
show high solubility and weak mechanical properties com- reduced by developing multilayers of PLA/fish gelatin/PBAT.88
pared to other proteins like gluten and fish protein.85 Zein Zhu et al.89 took the advantage of both proteins and poly-
fibers loaded with phenolic-rich orange chilto extracts were saccharide to develop a Pickering emulsion of zein–chitosan
electrospin-coated on PHA films followed by chemical modifi- complex suspension mixed with maize germ oil, which was
cation of the surface with glutaraldehyde vapor as a cross- then coated onto a PLA film. The miscible properties and
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interface interaction of chitosan and PLA (zein/chitosan than those of synthetic polymers. The way this issue has been
complex particles) was responsible for the increased strength addressed in the literature is to combine polysaccharides with
and extensibility of bilayer films compared with emulsion other biopolymers.93 The efficiency and functional behavior of
films (Fig. 8d). The oil was evenly distributed and filled polysaccharide-based coatings depend on the use of plastici-
throughout the zein–chitosan network matrix, according to zers, relative humidity, casting solvents, and the pH level.93,94
fluorescence laser scanning microscopy (Fig. 8d). Water vapor Using the LBL coating process, multilayer films (total of 30
permeation (WVP) was 1–2 orders of magnitude smaller than layers with final thickness of 4 μm) were created from sodium
films from only biopolymers (e.g., soy-protein isolate, chitosan alginate/polyethyleneimine (ALG/PEI) on biaxially oriented
films) and the protection against OP also improved.89 PLA films by Gu et al.95 (Fig. 9a and b). The OTR was 1.22 cm3
Overall, coatings based on proteins exhibit a good oxygen (m2 d atm)−1 and OP was less than 3.8 × 10−17 cm3 cm/cm2 s
barrier as well as medium mechanical behaviour. However, Pa. The latter was three orders of magnitude less than the
their sensitivity to water restricts their applications. Physical or BioPLA film. By increasing the number of coated layers, both
chemical post-treatment techniques can be used to improve tensile strength and elongation slightly increased as the
protein properties for coating applications. A summary of coating layers are too thin to have a significant effect on the
protein-based coatings is presented in Table 3. BioPLA film.95 Likewise, Dai et al.96 developed a transparent
3.1.3 Polysaccharide-based coatings and derivatives multilayer film based on cationic guar gum (CGG) and
3.1.3.1 General overview of polysaccharide-based coatings. TEMPO-mediated oxidised cellulose nanofibrils (TOCNs) using
Starch and its derivatives, cellulose derivatives, alginate, pectin, the LBL solution coating. The multilayer films showed WVTR
chitosan, and carrageenan are polysaccharides utilised in edible as low as 68.52 g (m2 d atm)−1 and OTR of 5.56 cm3 (m2 d
coating compositions71,91 (Fig. 4). Alginate and carrageenan can atm)−1 and resistance to canola dyed oil (Fig. 9c–e). The LBL
be applied as rather thick coatings on the surface of food to coating method has the advantage of electrostatic attraction
avoid moisture loss. As a result, until the coating dehydrates, between anion and cation and intermolecular hydrogen
the food does not lose significant moisture.81 Cellulose, starch, bonding, which densify the film structure and enhance the
chitosan, alginate and pectin are the main polysaccharide- mechanical and barrier properties.96 Cellulose nanocrystals
based materials for biodegradable coating applications. containing citric acid was developed as a biodegradable
At low relative humidity, polysaccharides provide an coating, in which the addition of up to 20% (by weight) citric
effective barrier to gases like carbon dioxide and oxygen, acid to CNC resulted in improved WVTR compared with neat
which lies behind their packed network structure of hydrogen- CNC. The improved WVTR occurred due to filling of free
bonding. However, their hydrophilic nature causes them to volumes in the coating matrix as well as citric acid’s higher
have a poor moisture barrier property.71,81,92 On the other hydrophobicity.97
hand, polysaccharides are rigid and brittle polymers. For Starch and derivatives of starch (e.g., hydroxypropylated high
example, the tensile strength of a film of chitosan or amylose amylose starch and amylose starch) have a reputation for being a
starch can be compared with other films based on HDPE. The low-cost packaging material, with great film-forming capabilities
main concerns are flexibility and elongation, which are far less and high water solubility.98,99 The mechanical strength, flexi-
Table 3 Summary of protein-based coatings
Protein-based coatings %Barrier improvement

and substrates Modifications Coating method WVP/WVTR/OP Ref.
Whey protein-coated PLA Addition of sorbitol Control coater OP reduced by 84% 82

Whey protein isolate-coated PET Addition of montmorillonite and Wired rod OP reduced by 91% for glycerol- 83
glycerol or sorbitol plasticized and 84% for sorbitol
plasticized
PLA-WG-PLA multilayers Addition of glycerol, high-pressure 1. Wet casting or OP reduced by 2000%, 42
homogenization and corona treatment spin-coating
2. Hot pressing WVP reduced by 20%
PLA-WG-PLA multilayers Addition of glycerol Hot pressing OP reduced by 99%, WVTR reduced 84
by 54%
Zein fibers loaded with orange Addition of glutaraldehyde as Electrospinning Improved water resistance 86
chilto extracts-coated PHA crosslinker and hot pressing
Zein–chitosan Pickering Casting WVP increased by 63%, OP reduced 89
emulsion and maize germ by 94%
oil-coated PLA
Fish gelatin + CNC coated PLA Corona discharge and addition of Laminating with OP reduced by 78% 87
CNC and antioxidant to fish gelatin thermo-compression
PLA/fish gelatin/PBAT Addition of glycerol Wet casting WVP reduced by 42%, reduced water 88
solubility
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Fig. 9 (a) LBL coating process in multilayer structure of ALG/PEI on BioPLA films. (b) A schematic of the multilayer film’s reduced free volume due
to strongly interdiffused ALG/PEI layers through electrostatic H-bonding, interpenetration and tangling of polymer chains. Therefore, the channel
for O2 diffusion via the layers was lengthened, contributed to better oxygen barrier of the films (figure a and b are reproduced from ref. 95 with kind
permission from Elsevier, copyright 2013). (c) and (d) A sandwiched structure including “saturated filter paper with canola dyed oil-film sample-
blank filter paper” was used for oil resistance test in CGG/TOCNs multilayer films and showed no discoloration. (e) The mechanism of oil-resistance
in multilayer films (figure c–e are reproduced from ref. 96 with kind permission from ACS, copyright 2017, open access).
bility, and transparency of starch-based films are impressive. lettuce.71,107 Additionally, CMC helps to preserve the flavour of
However, they have high WVTR, which might alter the inside fresh fruits and vegetables.71 This is achieved through the simu-
environment of the package, favoring microbe development and lation of a regulated atmosphere, in which the oxygen uptake is
resulting in product weight loss.99,100 Some other notable works reduced without any increase in carbon dioxide amount in the
have also been done on the utilization of thermoplastic starch in internal environment of coated apples and pears.71
various forms and combination of those with biodegradable Chitosan is one of the most efficient materials for coating
polyesters101–103 and alginate104 as well as proteins.105 fresh produce because of its great film-forming property and
In food applications, the most widely used cellulose deriva- adaptability with minerals, vitamins, and antimicrobial
tive is carboxy methyl cellulose (CMC).106 To create a barrier agents.108 Fruits that are highly perishable (e.g., strawberries,
against oxygen, moisture, and oil transfer, edible coatings made grapes, raspberries, mango) have been coated with chitosan-
from CMC, hydroxy propyl cellulose (HPC), methyl cellulose based coatings to protect from fungal decay.108 Chitosan coat-
(MC), and hydroxy propyl methyl cellulose (HPMC) have been ings combined with nanoemulsions have been studied for
used for vegetables and fruits.71 Among these, CMC is the most their bactericidal activity. For example, mandarin essential oil
applied coating for maintaining the crispness and firmness of has been loaded as nanoemulsion into chitosan coatings to
fruits including apples, peaches, berries, carrots, celery, and protect green beans against Listeria innocua through the
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application of UV-C, ozonated water treatments and tance, which avoided loss of molecular weight and tensile
γ-irradiation to enhance the antibacterial effect up to 3.3 log strength. Nanocellulose/nanochitin coating reduced the water
CFU per g. Although the bioactive coating combined with contact angle (from ∼87° for neat PLA to ∼65° for coated PLA)
γ-irradiation produced a synergistic and steady antibacterial due to increased hydrophilicity, but further treatment with micro-
impact with no negative effects on colour over the storage time, wave irradiation increased the water contact angle to ∼70° and
the reduction in sample firmness was a drawback. To overcome prevented the coating layers from peeling off the substrate.113
this problem, the combination of UV-C with bioactive packaging Flexible, transparent and gas impermeable coatings have
is a solution to avoid reducing the firmness during storage been based on cellulose nanofibers (CNFs) and chitin nano
time.109 Oil and water-repellent paper coatings were developed whiskers (CNWs) spray-coated in a layer-by-layer assembly
by the rod-coating of chitosan solution followed by further method on a PET substrate. The oxygen barrier of the multi-
layer (CNF/CNW)20 improved significantly (more than ∼65%)
modification of the paper surface with polydimethylsiloxane

(PDMS). Coated papers showed maximum fat resistance (kit compared with single layers of CNF or CNW. Further treatment
value of 12/12) and great water resistance (WCA of 95.2°).110 of PET-coated CNF/CNW through hot-pressing reduced the
Although polysaccharides have gained a lot of attention in OTR by ∼27%.117 In a similar study, the layer-by-layer coating
multilayer food packaging, there is not a clear approach to decide technique was used to coat nanocellulose/nanochitin on poly-
in which layer of bio-based multilayer packaging materials polypropylene films. A 20-layer coating of nanocellulose/nanochi-
saccharides should be used (i.e., outer or inner layer, facing-air tin with a total thickness of 60 µm decreased the OTR by
layer, intermediate layer).81 Another noteworthy point for polysac- ∼98% (from 1118 to 13 cc per m2 per day) due to the high crys-
charide-based coatings is regarding those derived from xylans tallinity of nanochitin and nanocellulose.118 It is important to
and mannans, which have shown low permeability of oxygen and note that further investigation of biodegradability for these
grease as well as good tensile strength.111 Therefore, biopolymer types of multilayers is needed to ensure that the biodegradabil-
blending and laminating using xylan/mannan can be used to ity of the coating alone is not disrupted after coating on a
develop novel multilayer composites. petro-based non biodegradable polymer such as PET or PP.
3.1.3.2 Nanocellulose and nanochitin-based coatings. Thermal treatment has produced significant improvement
Cellulose and chitin are the first and second most abundant in the case of nanochitin and nanocellulose coatings on cell-
polysaccharides112 and exhibit beneficial properties such as ulose acetate substrate. In a study, the spray-coated nanochi-
renewability, biodegradability and high crystallinity.113 tin/nanocellulose films were optimized in terms of spray
The chemical structure of chitin closely resembles that of coating temperature and thermal post-treatment temperature.
cellulose, with the key distinction being the presence of acet- By raising the spray temperature (from 40 to 100 °C) and the
amide groups in chitin, as opposed to the hydroxyl groups thermal temperature (from 40 to 140 °C), the OP reduced
found in cellulose.114 In the past few years, there has been a by 48% and 62%, respectively, reaching the optimal OP of
significant surge in research projects focused on nano-scaled 11.5 cm3 μm m−2 day−1 kPa−1, which is comparable to oriented
cellulose. Concurrently, there has been a growing interest in PET. The mechanical properties and WVP of the coated films
the isolation and extraction of nanosized crystalline chitin, exhibited an average enhancement of 20% and 11%, respect-
known as chitin nanocrystals or whiskers.114 ively, compared with neat cellulose acetate, with no significant
Cellulose-based nanoparticles are known as nanocellulose, influence observed from the temperatures.119
characterized by having at least one dimension measuring less The cellulose nanocrystal Pickering emulsion has been inte-
than 100 nm and length extending to several micrometers. grated into chitosan coatings to increase hydrophobicity on
Nanocellulose can be extracted from bio-sources like wood, hemp, pears during extended periods of cold storage. At 83% relative
linen, flax, tunicates and algae, and exists in three forms, namely humidity (RH), the ethylene production in commercial
nanocrystalline cellulose, nanofibrillated cellulose and bacterial Semperfresh™ coating and chitosan-reinforced CNC coated
nanocellulose.115 Common nanostructures for chitin are in the fruit tended to rise compared with those at 43% RH due to
form of nanofibrillar composites, nanofibers and nanowhiskers/ increased water absorption into the coating and reduced hydro-
nanocrystals, and can be extracted from mushrooms and shellfish phobicity. Conversely, fruit coated with Pickering emulsion CNC
as well as the mineralized structure of diatoms and sponges.114 incorporating chitosan stored at 83% RH exhibited no signifi-
PLA coated with multilayers of cationic chitin nanofiber and cant increase in ethylene production compared with those
anionic cellulose nanocrystals (CNC) using layer-by-layer spray stored at 43% RH. This indicates the greater hydrophobicity
coating improved the oxygen barrier properties of the final com- and stability at high RH of these coatings, effectively suppres-
posite films by 73%. PLA coated solely with chitin nanofiber or sing ethylene production, thereby delaying fruit ripening.120
CNC exhibited greater O2 permeability and haze compared with Cellulose nanofiber and nanocrystal (CNC) coatings have
PLA coated with multiple layers of both chitin nanofiber and demonstrated a reduction in the oxygen transmission rate
CNC. By increasing the coating thickness for 5 layers of chitosan (OTR) of the treated substrate.121,122 It is noteworthy, however,
nanofiber/CNC-coated PLA, a mutual interlayer destruction that the majority of studies have focused on self-standing cell-
caused a sharp decrease in ultimate tensile strength and breaking ulose films (fibers and/or crystals) or coatings applied to poly-
strength.116 In a similar study, PLA-coated nanocellulose/nanochi- meric substrates, as reviewed above, but a few studies are
tin using layer-by-layer assembly improved the hydrolysis resis- focused on porous substrate such as paper/paperboard.122,123
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Cellulose nanocrystals were applied to paper with small acidic chitosan coating technique was developed for preparing
(0.45 µm) and large (11 µm) pores using a layer-by-layer all-natural, biodegradable, and water-resistant paper coating.
method involving spinning and dipping. The paper with large Filter paper coated with CNW and soybean oil improved the
pores, coated with 10 layers of CNC (23 µm thickness), exhibi- WCA to more than 90° at zero time and water absorption of
ted the highest water contact angle WCA of 73°. The CNC less than 10% at 5 min.126
coating demonstrated low oxygen permeability, ranging from Reviewing the applications of nanochitin and nanocellulose
0.12 to 24 mL μm (m2 24 h kPa)−1, at 23% relative humidity coatings, it becomes apparent that utilizing these materials as
(RH). At 50% RH, the oxygen permeability (OP) was too high to polysaccharide-based substances can be considered as a sus-
measure, except for the dip-coated sample (with a thickness of tainable alternative in packaging applications.
23 μm), which exhibited an OP of 6.2 mL μm (m2 24 h kPa)−1 – Throughout section 3.1, we reviewed coatings from nature
lower than that of LDPE, PET, and PS. However, extended including lipid, protein, and polysaccharide-based coatings.
storage led to a decrease in OP, indicating a weakening of the Critical barrier properties and functions of edible coatings
coating’s barrier properties over time.122 from natural sources for fresh vegetables and fruits are sum-
A novel multilayer was developed by coating of CNC/CNW marized in Fig. 10. Coatings should have low permeability to
on one side of PET, and silica nanoparticles/CNW coated on water vapor to reduce the rate of desiccation and maintain the
the other side. The former side was treated with hot-pressing crunchy surface of the food. In addition, they should have a
and the latter side was impregnated with sunflower oil with low O2 permeability to reduce rate of respiration. However, O2
self-cleaning properties, and showed WVTR of 1.4 g m−2 day−1. permeability should not be too low to avoid anaerobic con-
The multilayer showed the WCA of maximum 154° with sig- ditions, production of ethanol, and off-flavor. Moreover, oxi-
nificant oxygen barrier properties of 0.1 mL per m2 per day.124 dation rates of the food can be reduced by barrier coatings
In another study, the CNW-CNC coating, in which CNW against UV light.127 Coatings can serve as a frying oil barrier,
was treated by aggressive deacetylation, demonstrated an so that the final oil content of the fried food remains low.
approximate ∼20% decrease in the WVTR compared with Finally, coatings have the capability to impart additional
uncoated cellulose acetate (CA) films by experiencing only a characteristics to the food such as a shiny and smooth surface,
marginal ∼10% reduction in ultimate tensile strength and no as well as providing antimicrobial and antioxidant properties.
noteworthy decline in failure strain. Multilayer films were All these contribute to extending the shelf life of food.128
achieved with a substantial 91–99% decrease in oxygen per- 3.1.4 Biomass and agriculture waste-based coatings.
meability (OP) as a result of tuning chitosan deacetylation, Packaging coatings/films should include at least two com-
compared with uncoated CA films.125 Interestingly, a non- ponents: a matrix (i.e., a macromolecule) that provides the
Fig. 10 Critical barrier properties and functions of an edible coating for fresh vegetables and fruits. The figure is drawn by the authors based on
contents in ref. 127 and 128.
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cohesive structure, and a plasticizer to reduce brittleness and eggs has been extended through immersion coating in cell-
rigidity. Other materials can also be added to coatings/films to ulose derivatives.139,140 Hemicellulose-based coating solutions
increase their physical, mechanical, and barrier character- are used to extend the shelf life of cheese by chemically modi-
istics127 (Fig. 11). fying chitosan and galactomannan in the presence of a plasti-
Biomass and agriculture waste, as renewable biorefinery cizer and corn oil.141 Pectin has been used for applications in
feedstocks, have also been used to develop coatings.127,129 food packaging as a coating on cut and fresh fruits or veg-
There are three generations of biorefineries, where the raw etables as well as in microencapsulating materials, with anti-
material is a feedstock obtained from a crop such as maize, oxidant and antimicrobial properties.51 In addition, pectin
corn, sugar beet, cassava and sugarcane (1st generation), cellu- coatings can be used in minimizing ripening and post-harvest
losic residue, forestry waste and agro-industrial waste (2nd rottenness, as well as enhancing tomatoes sensory character-
istics.142 Modifying the atmosphere around the fruit through
generation), and microalgae, CO2 capture and utilization (3rd

generation).130,131 Food waste is rich in carbohydrates, proteins applying a pectin-based coating impacts the oxygen level and
or lipids and therefore is a potential source of biopolymers.132 avoids ethylene production. Therefore, the physiological decay
Fig. 4 shows the main types of biopolymers that can be of the fruit will be postponed. Moreover, pectin was mixed
achieved from agricultural waste. For example, gelatin can be with corn flour to make a coating solution on fresh tomatoes
obtained from slaughterhouse wastes, which contain good and resulted in the formation of hydrophobic regions.142
sources of protein from animal origins.51 Gluten is a protein Among different biopolymers from by-products of the food
naturally found in some grains such as wheat and barley as a industry, fruit and vegetable residues are typically processed
by-product of wheat starch production.133 Lipid biopolymers into flour and have shown remarkable promise for flexible
could be obtained from natural sources like cutin extraction film/coating applications without the addition of plasticizers.
from tomato by-products.134,135 Polysaccharide biopolymers Andrade et al.143 created novel edible bilayers from flour that
such as pectin can be obtained from peels and seeds of are produced from a variety of residues (orange, watermelon,
different citrus fruits (mango, banana, orange) as well as from lettuce, carrot, spinach, mint, and cucumber) using the
juice manufacturing by-products51 and potato or cassava waste casting method. Furthermore, the incorporation of flour made
peels, which are a rich source of starch production.136 from the residue of potato skin enhanced the tensile strength.
Agricultural wastes such as corn straw, rice straw, wheat The high content of carbohydrates in potato skin resulted in
straw, sugarcane bagasse, and rice husk are the most abundant high flexibility but lower strength in comparison with films
type of biomass waste.137 Crop straw is produced from the dry made from fruit starch. The WVP values for the films made in
stem or stalk after removing the grain and chaff from the field. this study were lower than those found in films made from
The main constituents of crop straw are cellulose, hemi- banana puree (3.03 g mm m−2 h−1 kPa−1)144 but comparable to
cellulose, and lignin.138 The shelf life of avocados and fresh those found in films made from mango puree (2.66 g mm m−2
h−1 kPa−1).145
Abundant plant cell wall polysaccharides, namely xylan and
mannan, can be produced from by-products of the forestry
and agriculture industry.111 Edible coatings based on xylan
and mannan were tested on fruits.146,147 Apples coated with
arabinoxylan and β-glucan stearic acid ester showed reduced
weight loss and improved shelf life during storage time of
more than 30 days.147 Mikkonen et al.111 reported that coatings
derived from xylan’s and mannan’s biorefinery products have
oxygen barrier properties comparable to that of EVOH. In
addition, their mechanical strength was also comparable to
petro-based materials, though their stretchability was much
lower. Further studies are needed for the evaluation of safety
and quality of wastes derived from agricultural products.
Moreover, practical, and cost-effective ways for converting
wastes from biomass to raw materials should be developed to
allow industrial mass manufacturing.138
3.2 Polyester-based coatings

Fig. 11 Films and coatings derived from biomass should contain at
least two components: matrix (consist of a macromolecule that makes 3.2.1 Synthetic petroleum-based biodegradable polyester
the cohesive structure) and plasticizer (reduce brittleness and rigidity). coatings. In this section multilayer structures derived from
Other optional components are crosslinker and reinforcement to
synthetic oil-based biodegradable materials, such as PCL, PBS
improve physical characteristics of films/coatings. Some examples are
shown for each component in the boxes. Figure has been redrawn by
and PBAT, are summarized. Currently, PCL and PBAT are the
the authors from ref. 127 with kind permission from Elsevier, copyright most common synthetic biodegradable polymers that are used
2014. in the fabrication of multilayers.
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PCL and PBS are thermoplastic polyesters, which are syn- kg m−2 s−1 Pa−1) as well as interlayer adhesion. The films of
thesized by a condensation reaction.148 The melt transesterifi- paper/PHB fibers/PCL-PdNP and paper/PHB-PdNP fibers/
cation and melt polycondensation processes of poly(butylene PCL-PdNP indicated the best performance in oxygen scaven-
adipate) (PBA) and poly(butylene terephthalate) (PBT) produce ging. In fact, fibers and films from PCL rapidly remove oxygen
PBAT, an aliphatic–aromatic thermoplastic co-polyester.149 It from head space and are more efficient as a host for PdNP
has the same mechanical and thermal properties of some poly- than PHB for oxygen scavenging purposes.158 Overall, laminat-
ethylenes. Table 4 shows some of the characteristics of these ing and coating polyesters on each other showed a promising
polymers such as the appearance, melting point, solubility in outcome with regards to improving the performance of the
organic solvents, etc. All three polymers have an opaque final multilayer structure.
appearance due to their structures, which means they do not 3.2.2 Bio-based biodegradable polyester coatings. Herein,
allow light to pass through them.148 PBAT has a higher
we will review multilayer structures available today that have

melting point than PCL and PBS, although PBAT has a poorly been developed by coating biopolyesters such as PHAs, PLA,
crystalline nature compared with PCL and PBS. Although crys- PBS, etc. on polymeric substrates. Literature reviews show that
tallinity makes a polymer strong, it reduces the impact resis- several studies have concentrated on their blends159,160 or with
tance of the polymer, which is a significant characteristic in other agro-based polymers161 instead of coating or laminating
the application of food packaging. them with one another. However, effective coating techniques
A review of the literature on multilayers derived from syn- on biopolyesters have been demonstrated, with the main goal
thetic oil-based biodegradable polymers shows that the modifi- of improving their barrier and making them antioxidant or
cations include their blending with each other150,151 or with antibacterial for food quality preservation.81
polymers derived from agriculture.152 However, less work has For instance, Figueroa-Lopez et al.162 developed PHAs-based
been done on laminating these polymers over each other; active multilayers electrospin-coated with CNC and PHBV active
some of this is reviewed in this section. layer containing oregano essential oil (OEO) and ZnONPs (as
Multilayers of PBAT-coated PBAT/thermoplastic starch (TPS) antibacterial material) (Fig. 13a and b).162 Multilayers showed
blend and PBAT-coated PBAT/maleated thermoplastic starch an improved barrier against water vapor and D-limonene but the
(MTPS) blend showed barrier against oxygen and water oxygen barrier was not measured due to possible release of
vapor.157 The compression-moulded PBAT/TPS or PBAT/MTPS essential oil, which could damage the sensor. SEM (Fig. 13c–f)
blend film was dip-coated in PBAT. A rise of 664% and 329% showed that the fibers have a smooth surface with PHBV thick-
in shear strength was observed for 70TPS/30PBAT-coated PBAT ness of ∼0.6 µm. Mechanical parameters (tensile strength,
and 70MTPS/30PBAT-coated PBAT, respectively, as compared modulus, elongation) were reduced in comparison with PHA
with the TPS-coated and MTPS-coated films (Fig. 12a and b). monolayer due to delamination failure.162
This is a result of the fusion of PBAT coating into the blend Fabra et al.163 studied hydrophobic biopolyesters (i.e., PCL,
(Fig. 12c), which allows for MTPS-PBAT covalent bonding and PLA, and PHB) electrospin-coated on a thermoplastic corn
improved layer adhesion shown in SEM (Fig. 12d–g). PBAT starch (TPCS) film. The main shortcoming of starch-based
coating reduced WVP (59% for PBAT-coated PBAT/TPS and hydrophilic films is their high sensitivity to water, which
62% for PBAT-coated PBAT/MTPS), but slightly increased results in high plasticization.163,164 After electrospinning the
oxygen permeation film (8% for PBAT-coated PBAT/TPS and PCL, PLA, or PHB onto both sides of the TPCS films, the films
25% for PBAT-coated PBAT/MTPS) in comparison with the were heated between hot plates, resulting in continuous and
non-coated blend. Fig. 12h represents the adsorption, desorp- transparent outer layers. The WVP values of TPCS-coated PCL,
tion, and diffusion of water for these coated films.157 PLA, and PHB dropped by 83%, 88%, and 91%, respectively.
Cherpinski et al.158 prepared an oxygen-scavenging and water Accordingly, the O2 barrier of TPCS-coated PCL, PLA, and
barrier multilayered biopaper by electrospin-coating of polyhy- PHBV was improved by 91% for PCL and PLA and 95% for
droxybutyrate (PHB) and PCL fibers-containing Pd nano- PHB compared with neat TPCS film.163,164 Biodegradable ali-
particles (PdNP) over the paper. The multilayer was annealed, phatic polyester (PLA, PCL, polyesteramide (PEA), poly(hydro-
using a hydraulic press, resulting in a reduction of porosity xybutyrate-co-valerate) (PHBV) and poly(butylene succinate
and an improvement of barrier properties (WVP of 4.3 × 10−11 adipate) (PBSA)) were coated onto plasticized wheat starch
Table 4 Some characteristics of PCL, PBS and PBAT. The table is redrawn by the authors from ref. 148 with kind permission from MDPI, copyright
2021, open access, with added information (for PBAT) and some modifications for PCL and PBS. Tm, λc, %, Tg are melting temperature, percentage
crystallinity and glass transition temperature, respectively
Polymer Source Appearance Physical property Tm (°C) λc (%) Tg (°C) Ref.
PCL Oil-based Opaque Tough and flexible 70 77 −60 148 and 153
PBS Oil-based Opaque Tough and flexible 116 46 −25 148, 154 and 155
Bio-based
PBAT Oil-based Opaque Tough and flexible 120 23 −26 149, 151 and 156
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Fig. 12 (a) Interfacial shear strength of PBAT-coated films, (b) multilayers’ interfacial shear stress versus extension, (c) schematic of TPS/PBAT multi-
layers; SEM micrographs cross-section of fractured surfaces: (d) MTPS-coated, (e) TPS-coated, (f ) 70TPS/30PBAT-coated, (g) 70MTPS/30PBAT-
coated films, (h) Schematic diagram of moisture permeation through TPS/PBAT single-layer and multilayer films with PBAT coating. Figure is repro-
duced from ref. 157 with kind permission from Elsevier, copyright 2021.
(PWS). Polar amide groups in the PEA structure resulted in the were peeled away from the starch layer after 50 weeks. PWS/
high adhesion to the layer of PWS compared to other poly- PLA showed the most resistance to moisture and highest
esters. Coextruded films had a substantially higher adhesion hydrophobicity compared with other multilayers.165
(nearly twice) than compression-moulded films. However, the In a rare study, double-layers of PHBV/PBAT and PHBV/
strength of the adhesion varied over time and PHBV layers PBSebT (a composite based on PBS) were prepared by co-extru-
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Fig. 13 Schematic figure of active multilayer films, (a) with CNC coating and (b) without CNC coating, scanning electron microscopy (SEM) micro-
graphs of (c) the electrospun fibers of PHBV derived from cheese whey (CW) containing 2.5 wt% OEO + 2.25 wt% ZnONPs and of the active multi-
layer films (d and e) with cellulose nanocrystal (CNC) coating and (f ) without CNC coating (figures a–f are reproduced from ref. 162 with kind per-
mission from MDPI, copyright 2020, open access). (g) SEM image of a bi-layered blown film with blow-up ratio = 2.3 and take-up ratio = 4.1 with an
exterior layer of PBAT and (h) stress–strain curves of the double-layered film (with PHBV as the interior layer), PBAT film and PHBV film (figures g and
h are reproduced from ref. 166 with kind permission from John Wiley and Sons, copyright 2016).
sion film blowing.166 Under the same conditions, the thick- higher temperatures, whereas this elevated temperature can
ness variations in co-extrusion film blowing were half that of cause polysaccharides and proteins to bear thermal irre-
the blend. Delamination of two layers during SEM sample versible deterioration. Laminates or coatings on biopolye-
preparation was evidence of poor adhesion (Fig. 13g), which sters are a reliable and emerging way for producing light-
also created breaks in the stress–strain curve of bilayered films weight multilayer food packaging to minimize waste gene-
(Fig. 13h). PBAT/PHBV with PBAT serving as outer layer ration, reduce raw material use, and lower transportation
showed better resistance to water vapor 1.1–2.3 × 10−11 gm costs.81
m−2 s−1 Pa−1 as well as tear resistance (7.4–11.6 N) in compari- 3.2.2.1 Polyhydroxyalkanoate (PHA) coatings. PHAs are bio-
son with blends.166 degradable biopolyesters associated with “cradle-to-cradle”
Fossil-based hydrocarbons are cracked to produce olefins sustainability (versus “cradle-to-grave” dead end for oil-based
and further oxidized and derivatized to produce acrylates, resources)168,169 and are considered the carbon source syn-
which are then polymerized to produce polymers, resins, and thesized intracellularly by microorganisms.168 The most com-
coatings.167 Alkoxybutenolides were chemically synthesized by mercially available types of PHAs are poly(3-hydroxybutyrate-
using lignocellulose and converting it to furfural. Further co-3-hydroxyvalerate) (PHBV) and poly(3-hydroxybutyrate)
applying photooxidation (using visible light) resulted in robust (PHB).168 Thanks to PHAs’ intrinsic hydrophobicity, they are
uniform thin-film coatings as a bio-based alternative for acry- good barriers against water vapor.170 However, their mass pro-
late coatings for both glass and plastic materials.167 duction has been restricted due to the high price of raw
Compared with polysaccharides and proteins, melt and materials, separation of PHA from biomass and low microbial
thermal processability of biopolyesters can be performed at productivity (3–4 g PHA per 1 h).171,172
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Paper packaging is highly recommended with regards to sing, (2) forming uniform coatings, (3) negligible pinholes/
the harmful effects of plastic packaging, since paper is derived cracks, (4) solvent-free application.178
from renewable cellulose fibers. However, paper suffers from A biocomposite solution based on PHB incorporating addi-
having a low barrier against moisture, grease, and gas. tives (i.e., plasticizers, renewable fillers ( potato starch or ther-
Therefore, it is often coated or blended with petro-based mocell) and compatibilizer (stearic acid)) was coated on the
materials to fulfill the packaging requirements;7 however, this paper by a film applicator.181 The permeability of water vapor
excludes such packaging from biodegradability or repulpabil- is higher in papers coated with PHB containing starch than
ity.173 Therefore, investment in the PHA-coated paper industry those without starch due to starch’s hydrophilic property and
as well as using PHAs in biocomposite materials can help to the heterogeneous structure of the biocomposite.181 PHB/V
widen PHA applications and reduce their costs. was coated on the paper by extrusion-coating.182 Regardless of
Several biopolymers have been coated on paper to improve the typically used pre-treatments (corona and flame) in extru-
the barrier properties. However, biopolymers suffer from a low sion coating, PHB/V coated papers showed sufficient adhesion
oxygen and water vapor barrier.174,175 To address this issue, only when the substrate’s surface was pretreated with an
three main strategies are often used: (1) development of nano- acrylic primer. However, given that these primers are not bio-
composites, (2) functionalization of the biodegradable degradable, their applications will be restricted where com-
polymer, (3) coating paper with high barrier biodegradable postability is required.182 In the second part of the previous
polymers to develop multilayers.176 Multilayers typically study, WVTR and heat sealing of PHB/V coated paper were
contain two layers called “barrier” ( protects food against gas/ investigated. A higher crystalline melting point for PHB/V
water vapor) and “structural” ( protects food against mechani- (50 °C) compared with LDPE (40 °C) resulted in the high
cal stress) on the inside and outside, respectively.177 Another sealing temperature for PHB/V coatings on paper. PHB/V coat-
layer that can be included is the “active” layer.162 In addition, ings demonstrated four to six times poorer WVTR than that of
adhesives or “tie” layer177 resins are used to improve layers’ LDPE coatings. However, the addition of tall-oil rosin or wax
adhesion (Fig. 14). The manufacturing of such multilayer substantially improved the water vapor barrier properties.183
systems is essential, in which every layer targets a specific Using solvent casting to coat PHB on paper resulted in PHB
property in the final paper packaging. infiltration into the cellulose pores, thereby reducing the
Coating methods include melt-extrusion, solution coating, paper’s affinity to water molecules.184 Similarly, biodegradable
dispersion coating and lamination,173,178 of which extrusion bilayers were prepared by coating PHB on cardboard via com-
coating is the most industrially established one. The prepon- pression molding.185 Films containing 15% of PHB showed a
derance of extrusion coating is due to (1) continuous proces- marked drop in water permeation, moisture content, as well as
Fig. 14 Multilayered food packaging include printing layer, tie-layer, barrier layer, active layer and the food contact layer. The content of the figure
on the right for multilayers is from ref. 179 and 180 and the figure is redrawn from ref. 180 with kind permission from John Wiley and Sons,
copyright 2021.
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polarity. Moreover, the cellulose cardboard was functionalized paper at a bond strength of >1 N/15 mm, which shows the
with acetic acid, resulting in lower moisture absorption than sufficient bond strength between layers (Fig. 15c and d)189
those without treatment.185 Superhydrophobic papers were compared with polyethylene glycol (PEG)-plasticized PHBV-
prepared by immersing papers in PHB-CHCl3 solution and coated paper.
then in a coagulation bath consisting of water and ethanol.186 Overall, the paper coating industry, which has high-volume
To control the water flow through more wettable regions on production, is an appropriate field for utilizing PHA polymers
the paper, argon treatment was used (Fig. 15a). Paper-coated without concerns about their high production costs.181
PHB demonstrated higher WCA (i.e., 153.0°) compared with 3.2.2.2 Polylactide (PLA) and PLA blends coatings. For every
original paper (110.4°), which stemmed from PHB hydrophobi- researcher in the field of biopolymers, polylactide (PLA) has
city.186 Exfoliated layered nanocomposite (PHBV-nanoclay) was been considered as a favorable biodegradable polyester as its
polyester linkages come from 100% renewable resources.190
coated on pre-sprayed paper with a PHBV suspension to

enhance the resistance against water vapor.187 The WVTR of This makes PLA one of the most viable replacements for pet-
the coated paper decreased to as low as 26.4 g m−2 day−1 at roleum-based polymers in the paper packaging industry.191
90% relative humidity (RH) and 38 °C.187 However, a significant demand still exists for profitable routes
A PHA latex emulsion was coated onto kraft paper and then to improve PLA barrier properties, thermal stability and reduce
the coated papers were treated with a rapid pulse of photonic its brittleness.176 Methods to tailor the PLA gas barrier
energy.188 This treatment resulted in molten PHA particles include: (1) dispersing an additional phase(s) (e.g., bio-
forming a continuous film within milliseconds without polymer, inorganic materials, nanofiller, fiber) into PLA con-
degrading the substrate (Fig. 15b). WVTR was approximately tinuous matrix to produce bio/nano composite blends; (2)
the same for both photonic-dried and conventional oven-dried modifying the PLA surface through hot pressing, wet casting,
samples. However, 2-min Cobb values were higher for photo- electrospinning, and co-extrusion. The first approach results
nic-dried coated papers, which was due to pinholes in the in an intermediate barrier of the whole structure due to
coated film.188 The paper coated with triethyl citrate (TEC)- difficulty in dispersion and phase compatibility. However,
plasticized PHBV tore without releasing the coating from the the second approach results in a continuous blocking layer (or
Fig. 15 (a) A scheme representing the type of processed patterning on the superhydrophobic paper. The exposed area to argon plasma is limited
by glass slides, reproduced from ref. 186 with kind permission from Elsevier, copyright 2013. (b) Photonic energy heat treatment of PHA latex coated
paper resulted in coalescing and interdiffusion of PHA particles to make a continuous film, Reproduced from ref. 188 with kind permission from
TAPPI copyright 2018. (c) Bond strength of TEC-plasticized PHBV-coated paper and (d) PEG-plasticized PHBV coated paper, reproduced from ref.
189 with kind permission from MDPI copyright 2019.
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laminate) on the surface to act as a barrier against permeant coated baseboard.194 The schematic of the coating process is
molecules.42,192 shown in Fig. 16. The WVTR of the nanocellulose fiber-PLA
PLA solution was coated on paperboard for corrugated box nanocomposite (NCF-PLA)-coated paper depended on coating
liner applications. 3 w/v% of PLA solution resulted in the weight, temperature, and relative humidity.196 Applying 1%
highest water barrier property. Multilayer tensile strength modified NCF and higher coating weight resulted in lower
decreased compared with paperboard, while elongation at WVTR values (34 g (m2 24 h)−1) compared with non-coated
break slightly increased.193 Thin multilayers were produced by paper (1315 g (m2 24 h)−1).196
coating a solution of cationic starch on baseboard to enhance Low thermal instability of PLA is one of the major down-
the adhesion with the next layer, which was nanocellulose.194 sides of its usage in coating applications. To overcome this
Next, PLA was extrusion-coated on the paperboard. issue, the reinforcement of PLA with fillers (e.g., nanoscale sili-
cate) is needed.197 Also, it reduces the manufacturing costs of
Nanocellulose provides excellent oxygen resistance but a

limited water vapor barrier, while PLA has high water vapor the composite, enabling it to compete with low-cost poly-
and low oxygen barrier.194,195 The WVTR value of the multi- mers.197 Hectorite, saponite, sepiolite198 and montmorillo-
layer was lower than WVTR of PLA and the reference (LDPE) nite197 are some of the mainly used nanoclays incorporated
Fig. 16 (a) Illustration of the whole continuous line for coating of nanocellulose and PLA on baseboard, (b) cationic starch coating with reverse
gravure method; (c) extrusion coating of PLA or LDPE (as the control); (d) nanocellulose coating with a slot-die; and (e) final structure of the coated
paperboard, reproduced from ref. 194 with kind permission from ACS, copyright 2019 (open access) (https://pubs.acs.org/doi/10.1021/
acsami.9b00922, further permissions related to the material excerpted should be directed to the ACS).
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into PLA. Cheng et al.199 modified PLA with gelatin to improve from banana plants or water hyacinths. Banana plants and
the adhesion as well as facilitate the lamination process of water hyacinths were chopped, ground, cast and dried separ-
PLA on the paper substrate through enhancing the melt flow ately to make papers.203 To modify the paper against grease
rheology of the polymer. Thin PLA-coated coffee cups could penetration, the fluoro-free grease proof paper was prepared by
tolerate hot coffee or tea without any sign of leakage. The a non-toxic fluoro-free coating of sodium alginate (SA)/propy-
adhesion improved for PLA containing gelatin and the plastic lene glycol alginate and (SA)/sodium carboxymethyl cellulose.
coating played the role of a water barrier (WCA of 70.89°).199 The coating resulted in a kit-value of maximum 9, showing
So far, few researchers have paid attention to the “lotus leaf potential applications for paper packaging that requires direct
effect”, imitating this through surface roughness modification exposure to grease.204
to enhance water resistance/repellence properties in packaging Edible coatings are widely used in academia to improve the
materials. PLA electrospraying at 0.125% (w/v) over a pre- shelf life/safety of perishable fruits and vegetables, which tend
coated paper surface with 0.05 μm CaCO3 starch-based coating to see biochemical and physiological post-harvest losses in a
significantly increased the water contact angle (151.29°) and short time during transportation or storage. This issue results
improved WVTR, resulting in a superhydrophobic surface in economic loss and food wastage.205,206 For instance, a ligno-
through forming a surface roughness hierarchical structure.200 cellulosic nanofiber/wheat gluten hybrid composite solution
The PLA-PEG blend was coated on the kraft paper, using ethyl was dip-coated on six fruits (banana, cherry, grape, persim-
acetate to dissolve PLA instead of using hazardous halogen- mon, waxberry, and litchi). The coated fruits showed resistance
based solvents (chloroform/dichloromethane). The total crys- against microbes and UV as well as oxygen and water vapor
tallinity was increased due to PEG addition, which improved permeation in comparison with bare fruits.205 Dip-coating of
gas barrier properties compared with neat PLA. Furthermore, perishable fruits (orange, mango, waxberry, strawberry and
the barrier properties against water, oil-grease, and water cherry) with biomimetic hybrid material derived from shellac
vapor as well as heat sealing properties of coated paper membrane incorporating chitosan/poly(L-lactic acid) PLLA
improved.190 microspheres could improve the fruits’ shelf life. The coating
controlled gas (O2, CO2, H2O) permeability and CO2/O2 selecti-
3.3 Modifications of coatings vity. Further deposition of tannic acid on the microspheres
Coating technology is an emerging method towards the modi- imparted antioxidant and antibacterial properties to this
fication of surfaces to break limitations or meet challenges, hybrid coating material.207
particularly in food packaging applications. The modification Beeswax emulsion coating on tomato waste recycled cutin–
process can be simply applying one coating layer on top of the pectin membrane produced a superhydrophobic artificial
surface or manipulating the formulation of the coating material lotus leaf with an improved oxygen barrier. Further heating of
to improve its properties and then applying it on the surface. coated membranes at 55 °C improved the adhesion of the
Coating modifications are adopted to improve one or more pro- layers as well as the water vapor blocking ability. The heated
perties, some of which are summarized in this section. artificial lotus leaf showed anti-fouling ability against various
3.3.1 Environment resistance and barrier properties. The food liquids such as milk, tea, honey, coke, energy drinks and
resistance of the packaging material against surrounding yoghurt.208 Bovine albumin–chitosan oligosaccharide was
environmental factors such as water, oil, grease, UV, O2 and coated on a PLA biodegradable bag for strawberry preservation.
CO2 affects the final shelf life of packed food. Improving the The significant antibacterial properties of this coating post-
barrier properties of the packaging material against these poned the decay of strawberries and maintained their fresh-
environmental factors is of high interest for improving food ness and brightness.209
shelf life, thereby reducing food waste. Coating technology is PLA and cellulose possess the highest potential for com-
commonly used in this regard to modify the surface properties mercialization in food packaging among other biopolymers,
of the base substrate (e.g., paper, plastic) used for packaging, thanks to their abundant renewable natural resources.
as discussed earlier in sections 3.1 and 3.2. However, their commercialization is limited due to their high
In paper coating applications, the modification of the transparency to UV radiation. Surface modification of PLA and
coating with hydrophobic materials is performed to add water/ cellulose substrates by coating with p-coumaric acid and
oil repellency to the paper. For example, paper-coated chito- quinine improved their UV shielding property.210 Similarly, the
san-graft-castor oil improved paper hydrophobicity, originating coating of carbon-dot-based solution on PLA and cellulose
from castor oil and surface roughness due to the presence of substrate greatly increased the UV barrier for usage in food
microspheres. Therefore, chitosan coating modification packaging applications.211
through grafting with castor oil improved the water/oil repel- Overall, surface modification of paper, plastic or films as
lency of chitosan-graft-castor oil coated paper compared with well as foodstuff through coating technology or modification
chitosan-coated paper.201 Surface coating modification of of coating formulation and subsequent application on the
paper packaging, derived from oil palm fiber, with a beeswax– surface could effectively improve the surface functionality in
chitosan solution resulted in longer water absorbency time terms of resistance against environmental factors such as O2,
compared with uncoated paper.202 Biodegradable water-resist- H2O, CO2, UV, oil and grease. A summary of the recent litera-
ant paper was made by coating ethyl cellulose on paper made ture is presented in Table 5.
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Table 5 Application of coatings for improving the biodegradable polymeric substrate and food stuff against environmental factors
Substrate Coating Environment resistance Ref.
Paper Chitosan-graft-castor oil • Improved hydrophobicity 201

• Improved water/oil repellency

Paper from oil palm fiber Beeswax–chitosan solution • Longer water absorbency time 202
Paper from banana plant or Ethyl cellulose • Improved water resistance 203
water hyacinth
Paper Sodium alginate/propylene glycol alginate and sodium • Improved grease resistance 204
alginate/sodium carboxymethyl cellulose
• Resistance against microbes
Banana, cherry, grape, Lignocellulosic nanofiber/wheat gluten hybrid 205

persimmon, waxberry, litchi composite solution • UV shielding
• Resistance against oxygen and water vapor
Orange, mango, waxberry, Shellac membrane incorporated with chitosan/poly(L- • Controlled gas permeability (O2, CO2, 207
strawberry and cherry lactic acid) microspheres and tennic acid H2O) and O2/CO2 selectivity
• Antioxidant and antibacterial
Tomato waste recycled cutin– Beeswax emulsion • Superhydrophobic artificial lotus leaf 208
pectin membrane • Improved oxygen barrier
PLA packaging for strawberry Bovine albumin chitosan oligosaccharide • Antibacterial 209
• Maintained freshness/brightness of
strawberries
• Reduced spoilage of strawberries during
storage
PLA and cellulose p-Coumaric acid and quinine • Improved UV shielding 210
PLA and cellulose Carbon-dot-based solution • Improved UV shielding 211
3.3.2 Coating performance – adhesion and heat sealability inherent incompatibility that remains after the formation of the
3.3.2.1 Adhesion and coating delamination problem. To interface between coating and substrate.90 The major factors
improve adhesion between coating and the substrate, character- that affect the adhesion can be divided into two groups: physical
izing the physio-chemical adhesion energy and coating/sub- and chemical factors (Fig. 17). In addition, surface roughness,
strate interfacial tension is the key, and should be considered substrate wettability, and substrate preparation should be con-
simultaneously to improve the final adhesion between coating sidered,212 which are summarized below.
and substrate. In forming a bond between coating and sub- • Substrate preparation: Sufficient coating penetration into
strate, the researcher sacrifices both the coating surface (liquid) the substrate is necessary to make intermolecular forces. In
and the substrate surface (solid) and develops an interface. The this regard, the pre-treatment of the substrate with corona dis-
adhesion energy measures how energetically advantageous charge or chemical modifications is useful to remove any oil,
the formation of an interface is. Interfacial tension refers to the dirt, moisture, etc.212 For instance, PLA coating on biaxially
Fig. 17 Chemical and physical factors that affect the adhesion mechanism in polymer coatings. Physical factors include the smoothness of sub-
strate surface, surface tension, thickness, viscosity, and bond strength of coating to the substrate. In addition, the variance in thermal expansion of
coating and substrate affects the adhesion and a high difference results in weak bond strength during temperature variations. Chemical characters
include polarity of polymer coating, degree of polymerization, complexity of polymer adhesive molecule (chain length and molecular weight of
polymer coating) and pH. The figure is redrawn from ref. 212. Copyright (2020). From (Adhesion of Polymer Coatings) by (S. Verma and S. K. Nayak,
S. Mohanty/Sanjay Mavinkere Rangappa, Jyotishkumar Parameswaranpillai, Suchart Siengchin). Reproduced by permission of Taylor and Francis
Group, LLC, a division of Informa plc.
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oriented PET (BOPET) was developed as a biodegradable the freshness of food. Various factors are involved in the sealing
sealant layer to improve the sealability of the substrate. The process, which are classified in four groups: processing factors,
adhesion of the biodegradable PLA coating on BOPET was material characteristics, possible contaminant, and other
enhanced through corona treatment, resulting in the oxidation required processes (Fig. 18). These factors are described in
process and the presence of more polar groups.213 In another detail by Ilhan et al.;220 however, the material characteristics in
effort for substrate preparation, to improve interlayer adhesion Fig. 18 are briefly discussed below in order to bring insight to
between molded pulp (MP) food trays and cellulose nanofiber/ researchers working on the development of coating materials.
carboxymethyl cellulose (CNF/CMC), the MP was chemically • The molecular weight (MW) of the polymer used in flex-
modified by coating with chitosan solution. Chitosan provided ible packaging affects the sealing process. There is an indirect
electrostatic attraction with CNF/CMC, thereby improving the relationship between molecular weight and diffusion through
interlayer adhesion between CNF/CMC and MP.214 chain travel.220 As MW increased, stronger seals and better
• Surface roughness: This is to create a rigid substrate, with interfacial adhesion were achieved. Also, a more homogeneous
peaks and valleys, to enhance the mechanical interlocking of structure is provided by a narrow molecular weight distri-
the coating with the substrate.212 For example, modification of bution.221 For example, in corn starch/chitosan film formu-
acrylated epoxidized linseed oil with beeswax provided a stable lations, chitosan with medium molecular weight was selected
wax–oil emulsion coating for paper packaging. Beeswax to achieve better film-forming and heat-sealing properties
imparted microscale roughness on the surface of the coated rather than formulations with low molecular weight chito-
papers, which resulted in improved hydrophobicity, thereby san.222 However, the effect of low molecular weight chitosan in
reducing WVTR.215 Surface modification of paperboard with these formulations has not been discussed.
mineral-starch-based solution coating followed by electrospray- • The viscosity of a molten sealant layer reduces with a rise
ing of an additional PLA layer imparted microscale roughness. in temperature. If the sealant layer becomes too liquid, it
Moreover, PLA particle agglomeration during electrospraying squeezes out from the seal area by excessive pressure.
provided nanoscale roughness on the surface.200 Nevertheless, by adjusting the process temperature in accordance
• Wettability and spreadability: Complete wettability is with the properties of the polymer, the rheology of the melt
achieved when the grooves and roughness of the substrate are polymer during the sealing can be controlled.223 To prevent over-
filled with polymer coating rather than air. The air trapping causes heating and squeezing out, it is crucial to characterize the melt
a weak boundary layer on the substrate, which weakens the final viscosity or melt flow index of the sealant for the specific process
adhesion. In addition, the polymer coating should be able to flow circumstances.220,224 For example, celery paper was modified by
and spread at the micro/nanoscale onto the substrate to prevent soy-protein spray-coating to produce soy protein-celery composite
the formation of gas pockets.212 The synergy of coating rheology, paper with good heat-sealing properties. The shear thinning and
film formation after the coating application process and substrate viscoelastic behaviour of soy protein dispersion was the key to
properties are required to achieve a smooth and integrated coating improving the heat-sealing properties of the coated celery paper.
layer with sufficient flowability.216,217 For example, adding glycerol By increasing the soy protein concentration, its viscosity and seal
as a plasticizer to chitosan/carboxymethyl cellulose softened the strength increased.225
rigid crosslinked polymer network and showed shear thinning • The amorphous fraction of a melt polymer is correlated
behaviour, thereby a good coating coverage and homogeneity were with the seal strength of the polymer at a specific sealing temp-
achieved on the paperboard substrate.216 erature because the non-melted crystal macromolecules estab-
• Stresses: The applied stress on a coated substrate transfers lish a barrier to chain diffusion.226 Therefore, the heat sealabil-
from the coating layer to the substrate or from one coating to ity of a highly crystalline polymer, such as PHBV, is difficult and
another layer of coating in multilayers. This can be studied by tailoring its properties by blending or nanoparticle incorpor-
fracture mechanics, which covers crack propagation along the ation is necessary. Sealing in semi-crystalline polymers takes
coating–substrate interface, delamination, and failure.212 For place around the crystal melt temperature,227 since macro-
example, surface modification of paper by coating a low mole- molecule mobility rises at the melting point. For example, the
cular weight chitosan solution of 0.25 wt% increased the tensile heat-seal initiation temperature for PBAT was decreased by
strength and modulus. In fact, chitosan filled the paper pores either quenching (heat treatment) of PBAT or blending PBAT
due to the strong interaction of chitosan and paper, increasing with PLA. In both ways, the crystallinity of PBAT decreased,
the stress-transfer from one fiber to another.218 Environmental resulting in higher chain mobility and diffusion, thereby higher
stress including atmospheric conditions and weather changes adhesion strength at lower temperatures was achieved.228
can also impact the coating performance negatively.212 For • Surface characteristic of plastic coatings/films involves
instance, CNC coatings on PET surface showed a significant surface roughness and surface free energy. The wetting step of
reduction in CO2 barrier with increasing humidity from 0–80%, heat-sealing directly depends on the surface free energy of the
in which at 50% RH the CO2 permeance value was close to material. The ability of plastic to adhere to other plastic
uncoated PET. The same phenomenon occurred for the O2 increases, while having higher surface energy.220 Corona dis-
barrier of CNC-coated PET samples for RH >80%.219 charge has been used as a surface treatment to increase
3.3.2.2 Heat sealability. Flexible packaging needs to be surface free energy of materials as well as their wetting pro-
securely sealed to avoid leakage of food content and to maintain perties. On the other hand, surface treatment can give rise to
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Fig. 18 (a) Heat-sealing mechanism in flexible food packaging.220 (1 and 2) When two surfaces are melted and heated pressed, they make good
contact (wetting) over the seal area. (3) Then, the chain diffuses across the interface, leading to molecular entanglements. (4) Segments undergo
recrystallization after sealing, which binds the surfaces together and strengthens the seal. (b) Factors affecting final seal strength and seal integrity in
flexible packaging. Figure (a) is reproduced and (b) is redrawn from ref. 220 by the authors with some modifications, with kind permission from John
Wiley and Sons, copyright 2021.
surface roughness and results in improved wettability and gelatin/PLA films increased by increasing the ratio of fish
adhesion.220 Some examples of improving surface roughness gelatin layer thickness in fish gelatin/PLA bilayers.230
are discussed in section 3.3.2.1.
• Sealant layer thickness also has a major impact on heat
seal strength in barrier films because heat seal strength con- 4. Challenges for biodegradable
stantly rises with increasing sealant layer thickness above the coatings
seal initiation temperature.229 However, greater squeeze-out
issues are brought on by greater sealant thickness.223 4.1 Processing and application of green coatings on food or
Contaminated particles, joints, and corners must be con- food packaging
sidered as the most crucial sealing sites in packaging, which Polymeric coatings can be applied either on the food surface
need to be filled with enough sealant thickness.220 For or on the desired substrate, which will be further used in food
example, the seal strength and seal efficiency of bilayer fish packaging applications. In both cases, the coating can have
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direct or indirect contact with the food and the FDA (Food and Edible coatings with incorporated natural ingredients are
Drug Administration) information should be provided by the considered as a solution to tackle the loss of highly perish-
supplier of the food contact material. In addition, the func- able FFV by physical protection, reducing the pH losses,
tional barrier layer/component is responsible for the effective thereby extending shelf life.235 In addition, consumer
use of the coating. An appropriate efficient barrier blocks the demand for safe, sustainable, and healthy food, has resulted
migration of coating material to the food.7 For example, tech- in greater acceptance of natural edible coatings. On the
niques for assessing the migration of Ag and Cu nanoparticles other hand, a lack of standards and regulations, difficulties
(NP) from the coating and films to the food matrix have been in scale-up, environmental sustainability concerns, and
reviewed by Ahari et al.231 By using the titration method and limited market research on consumer ideas and purchase
the application of tetrazole with concentrated sulfuric acid, the intent, have limited the widespread application of edible
coatings.235 A recent survey on the consumer perception of
migration of AgNPs from a polyamide film coated with Ag into

caviar samples was investigated. No silver residual was found FFV with edible coatings showed that 79.3% of the respon-
from packages with different AgNPs concentrations.232 If the dents would buy edible-coated FFV if it is approved by the
coating material has not migrated to the food, it is not con- FDA.235,236
sidered a part of the food and therefore no regulations are For example, there are super hydrophobic edible coatings
applied to it. If there is no barrier layer/component between produced from FDA-approved (as generally recognized as safe
the food and the coating, the substrate must be revised for use (GRAS)) carnauba wax and beeswax for application on food
with food under the desired application conditions. In the containers to easily remove liquid food.237 Xanthan gum-based
case of a migration study, to ensure that the testing is coating on fresh cut lemon increased the storage time (at 4 °C)
sufficient to support a safety determination, migration studies to 21 days.238 In the US, most polysaccharides including
should be carried out in accordance with the FDA’s chemical xanthan gum that are used as major components in edible
and toxicological guidance documents.7 coatings are approved by the FDA.235 Chitosan/tannic acid/
corn starch bilayer films showed reduced WVP compared with
chitosan film, and coating of these bilayer films on banana
4.2 Food safety consideration in coating technology improved its storage time from 3 to 6 days.239 However, tannic
(migration issue) acid sensitivity to pH, light, and oxidation can cause a
Various compounds found in food contact materials have migration issue from the film.240 Coatings and encapsulation
the potential to migrate into the food and harm human of tannic acid have been reported to prevent its leaching and
health. Migrating substances can include non-intentionally migration from the film to the food.239,241 The edible coatings
added substances (NIAS) as well as intentionally added sub- on fruits may cause disorders such as core flush, flesh break-
stances (IAS). In manufacturing coatings, IAS are known as down, ethanol accretion and alcoholic off flavours, which are
commonly used ingredients, while NIAS are unknown detrimental to fruit quality.242,243 Transparent edible coatings
materials found in the coating.233 The toxicology information have a preferable appearance for fruits and vegetables as custo-
as well as in vitro/in vivo toxicology tests can be used to mers can assess the food’s external quality.242 For example,
identify the IAS and NIAS hazards and determine the safety whey protein-coated peanuts are reported to be darker than
levels. NIAS can either be (1) wholly unidentified com- uncoated ones.244
pounds, such as contaminants, degradation products, or Overall, edible coatings for FFV should be further explored
other reaction products, or (2) anticipated chemicals based in terms of their safety for human health, containing of aller-
on chemical reactions involved in the production of food gic components, and consumer attitude as well as discovering
contact materials.234 cheaper coating materials and processes.
Marin-Kuan et al.234 reported that it is not viable to use the
known time-consuming methods that entail the identification,
quantification, and toxicological evaluation of all chemicals 4.3 Processing of green coatings and their large scalability
that have the potential to migrate to the food. An effort is The various coating methods have their own advantages and
being made to combine data from analytics, bioassays, and disadvantages and not all are suitable for large-scale coating
in silico toxicology techniques for the risk evaluation of packa- production. Therefore, it is wise to select the coating method
ging materials in accordance with the International Life based on size and type of the substrate as well as surface
Sciences Institute (ILSI) and the European Union (EU) rec- roughness and final thickness of the thin film.245 For example,
ommendations on packaging materials. spray or spin coating of a hydrophobic material at a large scale
It is important to note that there is a great debate about may result in a non-uniform surface.37,246 Some of the advan-
the application of edible coatings on foodstuff like fresh tages and disadvantages of different coating methods which
fruits and vegetables (FFV). Cloete et al.235 highlighted that have hindered their scale-up manufacturing are listed in
there is a wide disparity across different regions of the world Table 6.
on established regulations for edible coatings, and con- To implement the laboratory-scale coating process in a
cluded that the industrial application of edible coatings are large-scale application, it is also necessary to thoroughly solve
not fully viable. the issues of safety material cost and long-term stability. It is
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Table 6 Advantages and disadvantages of coating methods
Coating method Advantage Disadvantage or limitation in mass production
Spraying • Minimal polymer use 245

• Thicker layer ends up with uneven layer245
• Any substrate size245 • Liquid biopolymers and base substrates with

−2
• Requires low coat weights (around 10 g m ) to obtain chemical or physical sensitivity may be subject to
the sufficient barrier properties (sometimes two layers are limitations in liquid media178
needed to remove the surface pinholes)a 178 • Drying and solvent evaporation is energy-
intensive178
Spinning • Simple and rapid to create uniform coatings245 • Difficult to control the coating thickness178,247
• Thickness of a few nm(s) to a few microns after solvent • Sometimes need high amount of the solvent to
evaporation245 245
prepare the coating solution
• Convenience and rather simple process setup • Solvent-based coating may cause any of below
178
appearances to the final coating:248
Dipping • Quick, affordable, easy, and high-quality coating W Blistering
245
• Applicable in both lab and industrial applications W Bubbling
W Sagging
W Solvent lifting
W Solvent popping
Roll coating • Most of the chemicals used in the roll-coating method • Limited coating thickness range249
are non-Newtonian fluids that behave in either a • Time consuming clean up for change over from one
pseudoelastic or viscoelastic manner245 coating to another249
• Limited speed range249
Extrusion coating • Continuous processing, minimal chances of pinholes • Requires high coat weight to obtain the required
and cracks, providing uniform coating178 properties178
• Solvent-free application178 • Melt instability of the polymer178
• Material-properties hinder the coating efficiency
and coating speed178
Blade coating • Good control over the coating thickness178 • Can be confined up to pilot scale or laboratory178
• Adaptable for solvent free applications245
• Large-area homogeneity245
• Little material waste245
• Interlayer dissolution prevention245
• Quick-drying step prevents the traditional solvent
annealing step245
Bar or rod coating • Better control over the thickness of the coating layer178 • Usually used on flat surfaces and may not work well
• The size of the groove or notch on the rod can be chosen on irregular surfaces250
to obtain desired coating thickness250 • Coating material viscosity and formulation affects
• Relatively simple and cost effective
250
performance of the coater instrument250
• Easy to clean the rod after coating250 • The operator skill and experience is critical to
• Versatility in applying coating of different materials achieve an even and consistent coating (in case of
including liquid250 coating manually)250
Other: physical/chemical • Pinhole-free and uniform high barrier coatings and can • Toxic gas can possibly be released from the
vapor deposition (PVD and provide chemical resistance and stress relaxation35,251,252 reaction47
CVD), etc. • High deposition rate and low deposition temperature47 • Substrate temperature may cause phase changes or
• CVD is the most popular method to obtain highly grain growth and diffusion of dopants in
uniform coatings on 3-D substrates47 microelectronic components47
• CVD provide multidirectional deposition253 • The corrosive gas can lead to poor adhesive
• PVD provides full control over growth, pristine film between coated film and substrate and contaminate
quality, large-scale fabrication, co-deposition flexibility, the film47
and controlling of the deposition temperature253 • Pricey vacuum environment and expensive
instrumentation245
• PVD provide only linear type of deposition253
a
Although this is true for generally solvent-based coatings methods, the thermoplastic polymer used in the coating can influence the required
coating weight. For example PLA coating by extrusion or solvent coating requires high coating weight to obtain necessary barrier properties,
while solvent or dispersion coating of other biopolymers need lower coat weight to get sufficient barrier properties.178
important to make sure that all components of the coating are reduce the number of nanoparticles that leak into the environ-
safe. For example, many different kinds of nanoparticles are ment. Further research and development can be performed to
still generally dangerous to human health and pose a threat to lower the loadings of relatively expensive nano additions or to
public safety. Creative engineering approaches can be used to find less expensive substitutes that can provide comparable
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qualities and performance to lower the cost of materials. The • Biosourced nanoparticles can operate as efficient
long-term chemical and physical stabilities of the materials Pickering stabilizers, providing potential alternatives to tra-
should also be enhanced considering that these coating ditional surfactants.256–258 Current research has demonstrated
materials would likely be exposed to outside natural factors that bio-surfactants are efficient in emulsion polymeriz-
such as heat, rain, humidity, and UV radiation for a long ation.259 Additionally, research is being done on innovative
period of time.37 ways to add starch nanoparticles directly to emulsion polymers
The development of various functional coating materials (latexes) to boost their bio-content.260,261
with desirable qualities and performance, as well as enhanced • Novel flame-retardant multilayer coating was developed
adoptability for large-scale applications in our everyday life, is by the incorporation of chitosan instead of bromine-based
anticipated to speed up through ongoing research in the materials.262
• There have been reports on bio-based, biodegradable
field of sustainable materials. However, scale-up requirements

and corresponding costs, technical feasibility for commercial thermosets made from epoxidized sucrose soyate, which is
viability, and life-cycle assessment as well as practical produced by epoxidizing sucrose ester resins obtained from
biodegradability are yet to be studied, discussed, and soybean oil fatty acids.263,264 Utilizing carboxylic acid-contain-
implemented. Some of the steps for these issues are addressed ing moieties from naturally occurring sources, such as fruit
below. juices, will result in crosslinking, producing an alternative to
• Manufacturing the multilayer coatings out of petroleum-based thermoset resin used in coatings.
biopolymers requires the appropriate materials and equip- Overall, using green chemistry principles, products that
ment, which are affordable and economically capable for mass enable biodegradation or make recycling easier at the end of
production. the product’s service life would be beneficial, and have the
• After multilayer packaging is successfully manufactured potential to be industrially commercialized.
on a large scale, its performance should be monitored during
storage, distribution, and consumption by customers to sys-
tematically analyze its quality and deficiencies. 5. Conclusion and future works
• It is also needed that government regulations develop in
a way that educates people about the advantages of novel In this review paper, we focused on the promising potential of
kinds of packaging materials in regards to the environment, biodegradable coatings to boost polymeric substrate properties
since consumer acceptance of these materials is an important to be used as a viable alternative for petroleum-based food
factor for their mass production. packaging materials. The modification of biodegradable sub-
strates, either paper or plastic, with a coating layer or modifi-
cation of coating formulation are reviewed with the focus on
4.4 Green chemistry and sustainability needs in polymeric the improved water vapour and oxygen barrier performance of
coatings the base substrate. In addition, the effect of coatings on the
Despite a substantial movement over the past few decades mechanical characteristics of the substrate or adding new
from solvent-based coatings to more ecologically friendly functional properties to the substrate (e.g., antimicrobial, anti-
water-based coatings, solvent-based coatings are still widely oxidant) are briefly discussed.
used in some applications. While high-end flexible packa- We have discussed various biodegradable coatings based
ging, such as that used for coffee and tuna food containers, on biopolymers from nature (i.e., lipids, proteins, polysacchar-
is predominantly solvent-based, low-end flexible packaging is ides, biomass, and agriculture waste), as well as bacterial poly-
now predominately water-based. Pressure-sensitive adhesives mers (i.e., PHAs) and synthetic/biobased biodegradable poly-
are primarily water-based, whereas industrial adhesives are esters that are used to tackle the shortcomings of bio-
predominately solvent-based. Flexible packaging materials degradable substrates for food packaging applications.
are similar to coatings in that they are made of a number of Firstly, in terms of barrier properties, coatings represent a
thin polymeric layers and are intended to protect its con- primary strategy for enhancing the barrier characteristics of
tents from environmental exposure.254 Some of the biodegradable substrates. To protect food against moisture,
developed green principles and new ideas are summarized hydrophobic materials are the most effective barrier coatings,
below. such as lipid, waxes and PHAs. Proteins and polysaccharides
• Utilization of biobased building blocks instead of petro- have a poor moisture barrier due to their hydrophilic nature.
chemical monomers. For example, a continuous, clear, and However, proteins and polysaccharides possess better barrier
water-resistant coating was achieved from evaporation of CO2 against gases compared with lipids. Secondly, in regards
and water from the cast film of carbon dioxide switchable poly- to mechanical properties, protein-based coatings exhibit
mers. During evaporation, these polymers switch from hydro- superior performance in comparison with coatings based on
philic to hydrophobic. Since these polymers are soluble in car- polysaccharides or lipids. In general, for coatings to improve
bonated water rather than natural water, they may keep the the barrier and mechanical properties, bonding and interlock-
VOC-free advantage of water-based coatings and are a substi- ing with the substrate is necessary and any delamination
tute for solvent-based coatings.255 failure can have a negative effect on the performance of
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the coated substrate. Lastly, coatings have the capacity to • Biopolymers from nature which are polar, such as cell-
impart antimicrobial or antioxidant attributes to the under- ulose, starch and protein, are easily permeated by water
lying substrate. In this context, examples include lipids (e.g., vapour, in particular at high humidity.269,270 Hence, for their
essential oils) and polysaccharides (e.g., chitosan and pectin), effective application as a coating on paper, their surface treat-
as well as the modification of coatings through the integration ment to act more hydrophobically is essential.268
of inorganic materials such as ZnO nanoparticles. • Biopolymers that are highly crystalline, such as micro/
Overall, multilayer packaging, compared with single-layer nanofilbrillated cellulose (MFC, NFC), showed excellent barrier
packaging, has more capacity to boost the performance of bio- properties, even better than conventional polymers for paper
degradable-based materials, particularly regarding barrier pro- substrates.178
perties. It is noteworthy to stress that, to meet sustainability In closing, it is worth emphasizing that polymeric coatings
goals, many companies that manufacture consumer packaged provide society with a variety of sustainability benefits by
goods have stated they will introduce new paper-based or other increasing product lifespans, lowering maintenance require-
sustainable bio-based polymer packaging by 2025–2030.34,265,266 ments, and/or defending our health and well-being. Due to the
Moreover, the challenges of biodegradable coatings such as manufacturing process of bi- or multilayer laminates, they
adhesion and delamination of layers, heat sealability, and have the ability to conceal certain undesirable shortcomings of
migration of coating material to the food, which hindered the biodegradable substrates while showcasing their desired pro-
mass production and application of coatings, are discussed, perties.81 The development and research on coating techno-
and possible ideas to tackle these challenges are provided. logy is in progress to make lightweight packaging materials;
Finally, a few recommendations for future research are given however, our review suggests that we still have a long way to go
separately below on the application of biodegradable coatings in developing packaging materials which can prove to be a
on paper and plastic packaging. great competitor for conventional plastics in terms of cost
effectiveness and consumer acceptability, besides being renew-
5.1 Biodegradable coatings on plastics substrates able, environmentally friendly and sustainable.
• Nowadays, PLA is commonly used in many kinds of flexible

bio-packaging. However, a coating or surface metallization is
required to boost its gas-barrier properties.81,267 After review- Abbreviations
ing the literature, we suggest that an appropriate natural
VOC Volatile organic compound
barrier coating would eliminate our reliance on petroleum-
UV Ultraviolet
based or metallized coatings.
PVdC Polyvinylidene chloride
• Cellulose and its derivatives have been applied as nano
PVC Polyvinyl chloride
coating or laminate layers with other biopolymers. However,
PE Polyethylene
there is room for exploring cellulose as a laminate layer with
PP Polypropylene
other biopolymers.81
LDPE Low-density polyethylene
• Lipid-based materials such as waxes that are intrinsically
HDPE High-density polyethylene
hydrophobic can be further explored as a coating layer on the
PS Polystyrene
biopolymers to improve their barrier against water vapor
PET Polyethylene terephthalate
permeation.
PHAs Polyhydroxyalkanoates
• Another untapped area is the creation of structured nano-
P3HB Poly(3-hydroxybutyrate)
particles from biopolymers such chitosan, alginate, and zein
PHBV Poly(3-hydroxybutyrate-co-3-hydroxy valerate)
as barrier coatings.
PBAT Poly(butylene adipate terephthalate)
• Coating or laminating biopolyesters on one another is
PLA Polylactic acid
another research area that needs to be explored more particu-
WG Wheat gluten
larly to improve the barrier of the final multilayer against
TPS Thermoplastic starch
oxygen and water vapour.
ASTM American Society for Testing and Materials
ESBO Epoxidized soybean oil
5.2 Biodegradable coatings on paper substrates PBS Polybutylene succinate
• Effective coating of non-polar biopolymers such as PLA, PHB PCL Polycaprolactone
and PHBV on paper improves its water barrier properties. PHB PVOH (PVA) Poly(vinyl alcohol)
in particular has shown the most comparable WVP to PE, PBSA Poly(butylene succinate adipate)
which is currently used as a petroleum-based coating for paper IUPAC International Union of Pure and Applied
packaging.178,268 Chemistry
• To further improve the barrier properties of hydrophilic BW Beeswax
biopolymers, one strategy is to make a blend of them with CW Carnauba wax
lipid-based biopolymers or hydrophobically modified biopoly- WPI Whey protein isolate
mers, or using these polymers as a filler.268 WVP Water vapour permeation
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WVTR Water vapour transmission rate 054449 and 800148); and (iii) the Natural Sciences and
OP Oxygen permeation Engineering Research Council of Canada (NSERC), Canada
OTR Oxygen transmission rate Research Chair (CRC) program ( project no. 460788).
RH Relative humidity
LBL Layer by layer

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Green Chemistry: Sustainable Biodegradable Coatings For Food Packaging: Challenges and Opportunities

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Green Chemistry: Sustainable Biodegradable Coatings For Food Packaging: Challenges and Opportunities

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Green Chemistry

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Sustainable biodegradable coatings for food

4934 a,b a,b

Green Chemistry Critical Review

water vapor barriers21), physical modification (e.g., heat treat-

Fatemeh Jahangiri is currently Prof. Amar Mohanty is a

Critical Review Green Chemistry

1.3 Development of green coating alternatives to petroleum-

Green Chemistry Critical Review

Critical Review Green Chemistry

Green Chemistry Critical Review

Critical Review Green Chemistry

Green Chemistry Critical Review

Another category of lipid materials are essential oil com-

Critical Review Green Chemistry

Green Chemistry Critical Review

Table 1 Summary of lipid-based coatings

Critical Review Green Chemistry

Table 2 Theoretical work of adhesion for some of the industry ﬁlm/

Green Chemistry Critical Review

Table 3 Summary of protein-based coatings

Protein-based coatings %Barrier improvement

Whey protein-coated PLA Addition of sorbitol Control coater OP reduced by 84% 82

Critical Review Green Chemistry

Green Chemistry Critical Review

modification of the paper surface with polydimethylsiloxane

Critical Review Green Chemistry

Green Chemistry Critical Review

generation), and microalgae, CO2 capture and utilization (3rd

3.2 Polyester-based coatings

Critical Review Green Chemistry

we will review multilayer structures available today that have

Polymer Source Appearance Physical property Tm (°C) λc (%) Tg (°C) Ref.

Green Chemistry Critical Review

Critical Review Green Chemistry

Green Chemistry Critical Review

Critical Review Green Chemistry

coated on pre-sprayed paper with a PHBV suspension to

Green Chemistry Critical Review

Nanocellulose provides excellent oxygen resistance but a

Critical Review Green Chemistry

Green Chemistry Critical Review

Substrate Coating Environment resistance Ref.

Paper Chitosan-graft-castor oil • Improved hydrophobicity 201

• Improved water/oil repellency

Banana, cherry, grape, Lignocellulosic nanofiber/wheat gluten hybrid 205

Critical Review Green Chemistry

Green Chemistry Critical Review

Critical Review Green Chemistry

migration of AgNPs from a polyamide film coated with Ag into

Green Chemistry Critical Review

Table 6 Advantages and disadvantages of coating methods

Coating method Advantage Disadvantage or limitation in mass production

Spraying • Minimal polymer use 245

• Any substrate size245 • Liquid biopolymers and base substrates with

Critical Review Green Chemistry

field of sustainable materials. However, scale-up requirements

Green Chemistry Critical Review