Food Hydrocolloids 125 (2022) 107419

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Food Hydrocolloids
journal homepage: www.elsevier.com/locate/foodhyd

Biobased materials for active food packaging: A review

Omar Mohammad Atta a, b, 1, Sehrish Manan a, 1, Ajmal Shahzad a, Mazhar Ul-Islam c,
Muhammad Wajid Ullah a, d, **, Guang Yang a, *
a
Department of Biomedical Engineering, Huazhong University of Science and Technology, Wuhan, 430074, PR China
b
Department of Botany and Microbiology, College of Science, Al-Azhar University, Assiut Branch, Assiut, 71524, Egypt
c
Department of Chemical Engineering, College of Engineering, Dhofar University, Salalah 211, Oman
d
Biofuels Institute, School of the Environment and Safety Engineering, Jiangsu University, Zhenjiang, 212013, PR China

A R T I C L E I N F O A B S T R A C T

Keywords: A large portion of food is lost due to the damage caused by different environmental factors such as moisture,
Food safety and stability oxidation, irradiation, microbial contamination, and others. Thus, food should be protected from such damages
Biopolymers by developing strategies, such as packaging, to enhance its quality, stability, and shelf-life. The usage of con­
Edible films and coatings
ventional petroleum-based packaging materials is a great risk to health and environmental safety. In contrast, the
Biosafety
Food packaging
utilization of biobased films and coatings for food packaging applications could be a safe approach, both from
human health and environmental perspective. This review briefly overviews the desired properties of biobased
packaging materials. It mainly discusses the potential of different natural (polysaccharides, lipids, and proteins)
and synthetic polymers for their film and coating-forming abilities considering their abundance, biological
properties (biocompatible, biodegradable, non-toxic), and morphological and physiological features. It also
discusses the role of different additives and nanomaterials for their potential to impart additional structural and
functional properties to packaging materials.

1. Introduction environmental effects and associated risks to consumers health (Persin

Presently, the busy work-life demands food protection and improved
shelf-life to save the time of consumers. Packaging of food protects it
food from adverse environmental effects and preserves its structure for a
longer period, hence maintaining its flavor and nutritional values
(Campos, Gerschenson, & Flores, 2011). For decades, various methods
of food packaging have been applied to protect food from environmental
changes and microbial contamination. Even nature guides mankind
about food protection and safety before consumption by providing fruits
and vegetables in a natural cover (Spence, 2016). Currently, the prob­
lems associated with food safety and environmental protection are of
great concern in the food packaging industry. According to a UN report,
about 299 million tons of packaging materials were produced in 2013,
but the disposal rate was only 43% (Muscat, Adhikari, Adhikari, &
Chaudhary, 2012). The demand for traditional petroleum-based plastic
food packaging materials is decreasing due to their hazardous
et al., 2011). Moreover, most of the packaging materials become waste
after their use. Although modern packaging techniques such as dipping,
spraying, and brushing the food items can somehow overcome the
threats associated with petroleum-based packaging materials, there is
still a demand for the introduction of packaging materials that ensures
food safety and are economical, biodegradable, and
environment-friendly.
Biopolymers can be a good substitute for conventional plastic
packaging due to their biodegradable nature and safe consumption by
humans. Different biopolymers have been used to produce edible
biodegradable packaging films with high capability to resist moisture,
aroma, transfer of solvents, and preventing the oxidation of food items
for an extended time period (Aider, 2010). Such biopolymers-based
packaging materials are used as wrappers for various food items,
disposable knives, drinking mugs, over frames and laminating films, and
drinking straws (Gutiérrez & Alvarez, 2017). Among the different

* Corresponding author.
** Corresponding author. Department of Biomedical Engineering, Huazhong University of Science and Technology, Wuhan, 430074, PR China.
E-mail addresses: omarscience@yahoo.com (O.M. Atta), sehrish_manan@hust.edu.cn (S. Manan), ajmalshahzad917@yahoo.com (A. Shahzad), wajid_kundi@hust.
edu.cn (M. Ul-Islam), wajid_kundi@hust.edu.cn (M.W. Ullah), yang_sunny@yahoo.com (G. Yang).
1
These authors contributed equally to this manuscript.

https://doi.org/10.1016/j.foodhyd.2021.107419
Received 31 March 2021; Received in revised form 7 November 2021; Accepted 28 November 2021
Available online 30 November 2021
0268-005X/© 2021 Elsevier Ltd. All rights reserved.
O.M. Atta et al.
biopolymers-based packaging materials, the polysaccharides-based
packaging materials are receiving tremendous attention due to their
low production cost, biodegradability, wide availability, and multiple
usages (Xu, Chen, Rosswurm, Yao, & Janaswamy, 2016). Similarly,
lipid-based packaging materials comprised of waxes, acylglycerols, and
fatty acids are also used in the food industry (Meerasri & Sothornvit,
2020). Different proteins such as egg white protein, casein, soy protein,
collagen, wheat gluten, whey protein, fish gelatin, corn zein, myofi­
brillar protein, and keratin are also used in the development of edible
and biodegradable films (Galus & Kadzińska, 2015; Hosseini, Rezaei,
Zandi, & Ghavi, 2013). The multi-layer coating of thin biopolymers
sufficiently reduces the carbon dioxide emission and avoids thermal
degradation of active agents (Vartiainen, Vähä-Nissi, & Harlin, 2014).
Moreover, the surfaces of these biopolymers can be modified according
to the desired application through various surface modification tech­
niques (Rol, Belgacem, Gandini, & Bras, 2019; S.-H.; Yu, Tang, et al.,
2015). In recent years, the demand for the usage of biomaterials for food
packaging applications has been greatly increasing in comparison to the
chemically synthesized materials due to their biocompatible and
biodegradable nature and non-toxicity (Alves-Silva et al., 2013). In
addition to the intrinsic features of biomaterials, the introduction of
different functional groups, the addition of exogenous materials, and
grafting of bioactive polymers impart additional functionalities and
bioactivity to these biopolymers (Guo et al., 2018; Ullah, Ul-Islam, Khan,
Kim, & Park, 2016a; Wang, Lu, & Zhang, 2016; Yang, Xie, Deng, Bian, &
Hong, 2012; Zhou et al., 2018). The biopolymer-based food additives
not only enhance the shelf-life but also reduce the calories and enhance
the texture and flavor of food items (Deng, Jung, Simonsen, & Zhao,
2018; Guo et al., 2018; Tang et al., 2019). Table 1 summarizes the
development and utilization of different biopolymers-based edible films
and coatings by different methods for packaging different food items.
This review emphasizes the use of biopolymers-based biomaterials
over conventional petroleum-based packaging materials for developing
biologically safe and green films and coatings food packaging applica­
tions. It discusses the biological and physiological properties of food
packaging materials and discusses different classes of natural and syn­
thetic polymers in terms of their structure-properties relationship for
food packaging applications. It further overviews the role of different
additives and nanoparticles to impart functional properties to food
packaging materials. We propose further assessment of these packaging
materials related to the process evaluation, safety assessments, regula­
tion, marketing, and consumer response, which will pave the way for
commercialization of such biobased materials for food packaging
applications.
2. Properties of biobased packaging materials
The biobased materials are used in the preparation of films or coat­
ings for their use in food packaging applications. The films are first
formed and adhered to the surface of the product, while coatings are
directly formed on the surface of the food products (Guimarães,
Abrunhosa, Pastrana, & Cerqueira, 2018). Nevertheless, both films and
coatings are comprised of rigid matrices and demonstrate certain
physiological, biological, and other properties, as discussed below and
summarized in Fig. 1.
2.1. Biological properties
The materials used for food packaging applications must be
biocompatible, non-immunogenic, and non-toxic (Rukmanikrishnan,
Ramalingam, Rajasekharan, Lee, & Lee, 2020) and do not induce any
allergic reactions (Chandra, 1997) in the body after their intake with the
food products. Moreover, the edible films and coatings must be biode­
gradable (Siracusa, Rocculi, Romani, & Rosa, 2008), and their degra­
dation products should not cause any toxicity in the body. Ideally, the
materials used as films or coatings for food packaging are produced
2
Food Hydrocolloids 125 (2022) 107419
through ‘green’ approaches by the natural systems (Zahiri Oghani,
Tahvildari, & Nozari, 2021). Different green synthesized materials by
the microbial and non-microbial systems used for food packaging are
discussed in Section 3.1. In addition to the above-mentioned biological
properties of materials used for food packaging applications, these must
possess bioactive components such as antioxidants (Gómez-Estaca,
López-de-Dicastillo, Hernández-Muñoz, Catalá, & Gavara, 2014) and
antimicrobial agents (Appendini & Hotchkiss, 2002). The antioxidants
prevent the oxidation of food products, hence hindering the formation of
free radicals, which otherwise lead to chain reactions and damage the
food quality. Similarly, antimicrobial materials prevent the growth of
unwanted microorganisms and the formation of films or colonies on the
food surface, thereby preventing food spoilage. Although most of the
biopolymers used for food packaging applications do not possess anti­
microbial activity (antibacterial and antifungal), such features are
imparted to these polymers through the incorporation of antimicrobial
agents, such as nanoparticles (Espitia et al., 2012) and bioactive poly­
mers (Zahiri Oghani et al., 2021) into their matrices or surfaces.
Different classes of antimicrobial nanoparticles used for food packaging
applications are discussed in Section 5.2. Food packaging materials
could also be supplemented with probiotics, which are a class of useful
microorganisms and benefit the consumers when they reach the stomach
along with the packed food (Espitia, Du, de Jesús Avena-Bustillos,
Soares, & McHugh, 2014).
2.2. Physiological properties
Different physiological features of materials used in the development
of edible films or coatings contribute to the stability of food and increase
the shelf-life of food products. The food packaging materials must pro­
vide protection to food against UV light and other dangerous rays
(Debeaufort, Quezada-Gallo, & Voilley, 1998). Moreover, these should
allow the transport of different solutes (Falguera, Quintero, Jiménez,
Muñoz, & Ibarz, 2011), water vapors (Zhang, Wei, & Han, 2018), gases
(oxygen, carbon dioxide, ammonia, nitrogen, ethylene, and others)
(Falguera et al., 2011), and different organic molecules (e.g., vapors of
aromas and different solvents) (Debeaufort et al., 1998; Falguera et al.,
2011) between the food products and the environment. Furthermore,
these materials should allow mass transfer through different phenomena
such as diffusion, osmosis, permeation, and adsorption depending on the
morphological (such as porosity) and physiological properties of the
materials used for packaging application. The packaging materials must
serve as a barrier (Guimarães et al., 2018) and possess high mechanical
properties (elasticity, flexibility, and tensile strength) (Castro-Muñoz,
Martin-Gil, Ahmad, & Fíla, 2018; Zhang et al., 2008), and provide
protection against any physical damage such as a cut or a dent. In
addition, gelation is also considered an important property of the
packaging material. Gelation materials such as alginate (Xiao, Wang,
Yang, & Gauthier, 2012), starch (Veiga-Santos, Oliveira, Cereda, Alves,
& Scamparini, 2005), chitosan (Liu, Wang, Lan, & Qin, 2017), gelatin
(Khodaei & Hamidi-Esfahani, 2019), and others not only form physio­
logically stable hydrogels and encapsulation barriers to providing pro­
tection to food but are also biocompatible, biodegradable, and bioactive.
Thus, the gelation materials could be used in the development of edible
films and coatings. Besides the above-mentioned features, the optical
transparency (Petit, Velasco, & Spence, 2019), having no direct role in
enhancing the physiological features and stability of the food products,
is an important feature of the packaging material by allowing the im­
aging of any contamination or damage to the packed food.
2.3. Others
Besides the above-discussed features contributing to enhancing the
quality, stability, and shelf-life of food, there are several other factors to
be considered when choosing the materials for the development of films
and coatings. The packaging materials must be easily available and low-
O.M. Atta et al. Food Hydrocolloids 125 (2022) 107419

Table 1
The development and utilization of different natural polymers-based edible films and coatings by different methods for packaging of different foods. Table reproduced
from (Díaz-Montes & Castro-Muñoz, 2021) under Creative Common CC BY license.
Food Biopolymeric matrix Additives Coating Improved properties Reference
Technique

Fruits
Figs Chitosan Acetic acid, canola oil, cinnamon Spread Antioxidant capacity was preserved, Contreras Saavedra, Rosa,
essential oil, and Rosselle extract color change was delayed, and Ventura-Aguilar, Bautista-Baños,
growth of Alternaria alternata was and Barrera-Necha (2020)
inhibited
Bell pepper Chitosan Acetic acid, canola oil, glycerol, Spread Flavonoids and antioxidant capacity Hernández-López, Ventura-Aguilar,
and chitosan/α-pinene were not modified, and the growth of Correa-Pacheco, Bautista-Baños,
nanoparticles Alternaria alternata slowed down and Barrera-Necha (2020)
Papaya Papaya puree and alginate Glycerol and citric acid Dipped Shelf-life was extended Hamzah, Osman, Tan, and Ghazali,
(2013); Rangel-Marrón,
Mani-López, Palou, and López-Malo
(2019)
Carrageenan Glycerol and citric acid Dipped Ripening was delayed and shelf-life
was extended
Blueberries Alginate, chitosan, apple Glycerol, inulin, and oligofructose Dipped Sensory quality was improved, and Santos, Rostro-Alanís,
fiber, and orange fiber shelf-life was extended Parra-Saldívar, and Alvarez (2018)
Chitosan, calcium Glycerol and tween 20 Dipped Ripening was delayed, and flavor, Duan, Sun, Wang, and Yang (2011)
caseinate, alginate and texture, and visual appearance were
semperfresh™ maintained
Strawberries Chitosan Acetic acid, canola oil, cinnamon Wrapped Antioxidant capacity was increased, Ventura-Aguilar, Bautista-Baños,
essential oil, and Roselle extract and shelf-life was extended Flores-García, and Zavaleta-Avejar
(2018)
Chitosan and beeswax Glycerol and tween 80 Dipped Quality was preserved and shelf-life Velickova, Winkelhausen,
was extended Kuzmanova, Alves, and
Moldão-Martins (2013)
Chitosan and carotene- Glycerol and polyvinyl alcohol Dipped Microbial and fungal growth was Hajji, Younes, Affes, Boufi, and
proteins controlled, and antioxidant activity Nasri (2018)
was maintained
Chitosan and chitosan Glycerol, acetic acid, and propolis Dipped Total phenols, flavonoids, and Martínez-González et al. (2020)
nanoparticles extract antioxidant capacity were increased,
the ripening process and sensory
characteristics were not modified
Fish gelatin and citrus Glycerol and hydroxytyrosol-3,4- Dipped Mold growth was delayed, and shelf- Bermúdez-Oria,
pectin dihydroxy phenyl glycol life was extended Rodríguez-Gutiérrez,
Rubio-Senent, Lama-Muñoz, and
Fernández-Bolaños (2017)
Cassava starch Propolis extract Dipped Vitamin C content was promoted Thomas, Nassur, de, Boas, and Lima
(2016)
Fresh-cut Xanthan, alginate, and Glycerol and 1-methyl Dipped Microbial growth was inhibited, and Vargas-Torres et al. (2017)
jackfruit gellan gum cyclopropane shelf-life was extended
bulbs
Fresh-cut Cactus pear mucilage Glycerol and tween 20 Dipped Visual quality and flavor were Allegra et al. (2016)
kiwifruit improved, and shelf-life was
extended
Fresh-cut Whey protein Glycerol, citric acid, and Wrapped Shelf-life was extended Azevedo et al. (2018)
apples montmorillonite clay
Carboxymethyl cellulose Glycerol, calcium, and acid Dipped Vitamin C and antioxidant capacity Saba and Sogvar (2016)
ascorbic were maintained
Chitosan – Dipped Quality was enhanced Lustriane, Dwivany, Suendo, and
Reza (2018)
Alginate, gellan gum, Glycerol, ascorbic acid, and inulin Dipped Quality was enhanced and shelf-life Moreira, Cassani, Martín-Belloso,
pectin, and apple fiber was extended and Soliva-Fortuny (2015)
Chocolate and milk butter Polyglycerol polyricinoleate and Dipped Anti-aging effect was produced Khan, Cakmak, Tavman, Schutyser,
ascorbic acid and Schroёn (2014)
Olive oil and sunflower oil Lecithin and ascorbic acid Spread Anti-aging effect was produced Khan et al. (2014)
Whey protein, soy protein, Glycerol Dipped Physical changes were controlled, Ghavidel, Adl, Shawrang, Nejhad,
alginate, and carrageenan and shelf-life was extended and Abadi (2013)
Cassava starch and Glycerol and stearic acid Wrapped Physicochemical properties were Chiumarelli and Hubinger (2012)
carnauba wax improved
Soybean gum, jojoba, and Glycerol and paraffin oil Wrapped Quality was maintained El-Anany, Hassan, and Ali (2009)
Arabic gum
Red grapes Gelatin, corn starch, and Glycerol and sorbitol Dipped Quality was enhanced and shelf-life Fakhouri, Martelli, Caon, Velasco,
waxy maize starch was extended and Mei (2015)
Fresh-cut Alginate Glycerol, sunflower oil, lemongrass Dipped Quality was preserved and shelf-life Azarakhsh, Osman, Ghazali, Tan,
pineapple essential oil, calcium chloride, was extended and Adzahan (2014)
ascorbic acid, and citric acid
Fresh-cut Alginate Glycerol, sunflower oil, calcium Dipped Browning agent was delayed, and Robles-Sánchez, Rojas-Graü,
mangoes chloride, ascorbic acid, and citric shelf-life was extended Odriozola-Serrano,
acid González-Aguilar, and
Martin-Belloso (2013)
Fresh-cut Alginate, pectin, and Glycerol Dipped Texture was preserved and shelf-life Sipahi, Castell-Perez, Moreira,
watermelon calcium lactate was extended Gomes, and Castillo (2013)
(continued on next page)

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O.M. Atta et al. Food Hydrocolloids 125 (2022) 107419

Table 1 (continued )
Food Biopolymeric matrix Additives Coating Improved properties Reference
Technique

Vegetables, plants, and cereals

Saffron Maltodextrin and – Spread Physicochemical properties were Jafari, Bahrami, Dehnad, and
nanocellulose improved Shahidi (2018)
Potatoes Locust bean gum Glycerol Dipped Physical changes, microbial growth, Licciardello, Kharchoufi, Muratore,
and nutritional quality were and Restuccia (2018)
controlled
Taro corms Chitosan and starch Glycerol Dipped Quality was enhanced, microbial Bedolla-Cázares et al. (2017)
growth was inhibited, and shelf-life
was extended
Tomatoes Citrus peel pectin Glycerol and oregano oil Spread Antifungal effect was generated, and Bedolla-Cázares et al. (2017)
phenol content and antioxidant
activity were increased
Carnauba wax Mineral oil Spread Antioxidant activity was increased Dávila-Aviña et al. (2014)
Chitosan and zeolite Tween 80 and acid lactic Dipped Ripening was delayed García, Casariego, Diaz, and
Roblejo (2014)
Soy protein, Glycerol, ascorbic acid, and Dipped Physical characteristics were Nandane and Jain (2011)
carboxymethyl cellulose, sodium benzoate enhanced, and shelf-life was
and oleic acid extended
Cherry Hydroxypropyl Glycerol, tween 80, and oleic acid Dipped Growth fungal was reduced and Fagundes et al. (2015)
tomatoes methylcellulose and physical appearance was maintained
beeswax
Hydroxypropyl Glycerol and oleic acid Dipped Growth of Botrytis cinerea was Fagundes, Palou, Monteiro, and
methylcellulose and reduced and physical appearance Pérez-Gago (2014)
beeswax was improved
Shiitake Alginate Silver nitrate, sodium borohydride, Dipped Shelf-life was extended Jiang, Feng, Zheng, and Li, (2013)
mushrooms and polyvinylpyrrolidone
Broccoli Methylcellulose, Glycerol, tween 80, organic acids Dipped Growth of Escherichia coli, Salmonella Takala, Vu, Salmieri, Khan, and
polycaprolactone, and mixture, rosemary extract, Asian typhimurium, and Listeria Lacroix (2013)
alginate spice essential oil, and Italian spice monocytogenes was controlled
Spinach Agar, κ-carrageenan, and Glycerol Wrapped Freshness was maintained and shelf- Rhim and Wang (2013)
konjac life was extended
White Sodium carboxymethyl- Sucrose fatty acid ester, Dipped Weight loss was reduced, and quality Tzoumaki, Biliaderis, and
asparagus cellulose, whey protein polyethylene glycol, sorbitol, and was preserved Vasilakakis (2009)
isolate, and pullulan stearic acid
Animal and dairy products
Sausages Maltodextrin, alginate, Glycerol and Terminalia arjuna Wrapped Shelf-life was extended Kalem, Bhat, Kumar, Noor, and
and carboxymethyl Desai (2018)
cellulose
Gelatin and carrageenan Glycerol, lard, and beeswax Dipped Weight loss was reduced Tyburcy and Kozyra (2010)
Chicken meat Mango peel powder, Glycerol and polyvinyl alcohol Wrapped Shelf-life was extended Kanatt and Chawla (2018)
cyclodextrin, and gelatin
Gum Arabic Sorbitol, polyvinyl alcohol, and Wrapped Bioactive compounds were Muppalla and Chawla (2018)
Zanthoxylum rhetsa extract increased, and shelf-life was
extended
Linear low-density Cinnamon essential oil and silver- Wrapped Antimicrobial capacity was Ahmed et al. (2018)
polyethylene copper increased, and shelf-life was
extended
Butter Low-density polyethylene Yerba mate and carotenoid extracts Wrapped Antimicrobial and antioxidant Moura, de Souza, de Oliveira,
capacities were increased, and shelf- Lemos, and Druzian (2018)
life was extended
Ham slices Cassava starch, chitosan Glycerol Wrapped Shelf-life was extended Zhao et al. (2019)
and gallic acid
Fresh chicken κ-Carrageenan and Glycerol and oriental mustard Dipped Campylobacter jejuni was reduced and Olaimat, Fang, and Holley (2014)
breast chitosan extract shelf-life was extended
Chicken Alginate Calcium chloride Dipped Microwave heating was improved Harsing Jr et al. (2012)
nuggets
Bream fish Alginate Glycerol, vitamin C, and tea Dipped Bacterial growth was inhibited and Song, Liu, Shen, You, and Luo,
polyphenols sensory values were enhanced (2011)
Cheese Galactomannan and Glycerol, sorbitol, and oil corn Spread Shelf-life was extended Cerqueira et al. (2010)
chitosan
Poached Alginate, pectin, Nisin, novagard CB1, guardian Dipped Growth of Listeria monocytogenes was Juck, Neetoo, and Chen (2010)
turkey κ-carrageenan, starch, and NR100, sodium lactate, sodium inhibited
xanthan gum diacetate, and potassium sorbate
Bakery
Bread Pectin, alginate, and whey Glycerol and tween 20 Sprayed Moisture was decreased Chakravartula et al. (2019)
protein
Starch Glycerol and ε-poly-L-lysine Wrapped Shelf-life was extended Luz et al. (2018)

cost. For example, considering the high production cost of BC from the
chemically defined medium, several researchers have explored the po­
tential of different wastes and low-cost substrates as alternative carbon
sources for its production (Islam, Ullah, Khan, Shah, & Park, 2017;
Ul-Islam, Ullah, Khan, & Park, 2020). Similar strategies have been
developed for the production of other materials for their applications in
food packaging. Similarly, the packaging materials should remain stable
for an extended time and at varying temperatures during their transport.
3. Food packaging materials
Food packaging plays a vital role in protecting the food items during

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O.M. Atta et al. Food Hydrocolloids 125 (2022) 107419

Fig. 1. Characteristic features of biobased food packaging materials.

their supply chains to the consumer. Recently, the use of biomaterials-
based food packaging has been encouraged due to the abundance,
biocompatibility, biodegradability, and non-toxic nature of biomaterials
(Verghese, Lewis, Lockrey, & Williams, 2015). The biomaterials used for
packaging applications are derived directly or indirectly from a
renewable source. A summary of various biobased materials used in food
packaging is given in Table 2. The list of biopolymers that can be used
directly in packaging materials includes proteins, lipids, and poly­
saccharides (Fig. 2). These polymers are produced by plants, animals,
and microorganisms. In addition, some chemically synthesized poly­
mers, such as poly (lactic acid) (PLA), poly (glycolic acid) (PGA), and
several others, are also used for packaging application owing to envi­
ronmental permeability for bacteria, chemicals, organic matter, oxygen,
and water vapor (Arora & Padua, 2010).
3.1. Natural polymers
3.1.1. Polysaccharides
Polysaccharides represent the bulky molecules in the biosphere and
are the main structural elements of plants (Thakur & Thakur, 2016).
Several types of polysaccharides, such as chitosan, cellulose derivatives,
starch, and gums (Fig. 2), are used in the food packaging industry
(Elsabee & Abdou, 2013; Espitia et al., 2014). The biofilms developed
from these polysaccharides are used for food, medical, and other in­
dustrial applications (Freitas et al., 2014; McCarthy, Ullah, Booth, Pei, &
Yang, 2019). The polysaccharide-based films have excellent gas
permeability properties, thus contributing to improve the product life
without creating anaerobic conditions, unlike fat-based films, which
create an anaerobic environment and thus increase the risk of contam­
ination (Alkan, 2013). These polysaccharide-based biofilms are hydro­
philic and have low water barrier properties, high mechanical strength,
high gas (CO2 and O2) barrier properties (Galgano, 2015).
3.1.1.1. Cellulose. Cellulose is comprised of unbranched linear chains of
glucose monomers, which are linked through β-1,4-linkages. It is ob­
tained from different sources, including plants (Matharu et al., 2018),
animals (Bacakova et al., 2019), and microorganisms (Ahrem et al.,
2014; Ullah, Ul Islam, Khan, Shah, & Park, 2017), as well as synthesized
enzymatically such as by the cell-free enzyme systems (Kim, Viswana­
than, et al., 2019; Ullah, Ul-Islam, Khan, Kim, & Park, 2015, 2016b).

Table 2
Summary of biobased materials, their sources, and properties for food packaging applications.
Origin Polymer type Source Properties Reference

Plant Animal Microbial

Natural Polysaccharides Cellulose, starch, Glycogen Bacterial Biocompatibility, biodegradability, (Abral et al., 2020; Araújo, Ferreira, Torres,
pectin, and and cellulose, non-toxicity, thickening, gelation, Neves, & Freitas, 2020; Dou, Li, Zhang,
galactomannans chitosan chitosan, emulsification, stability, coating, Chu, & Hou, 2018; Freitas, Alves, Reis,
pullulan, and barrier, mechanical strength, Crespo, & Coelhoso, 2014; Niu, Shao, Chen,
alginate hydrophobicity, hydrophilicity & Sun, 2019; Soares et al., 2015)
Lipids Oils, fats, and Fats and – Protection, insulation, coating, (Hall, 2011; Romani et al., 2020, p. 106087;
waxes waxes barrier Seow, Yeo, Chung, & Yuk, 2014)
Proteins Soy protein Collagen, – Thickening, stability, foaming, (Jiang et al., 2020; Lara et al., 2020;
casein, and gelation, nutrition Samakradhamrongthai, Angeli, Kopermsub,
whey & Utama-ang, 2019; Wu et al., 2020; Yu
et al., 2018)
Others – – PHA and PHB Viscosity, resistance, flexibility, (Tan et al., 2020)
stability
Synthetic Poly (lactic acid), poly (glycolic) acid, poly (lactic-co-glycolic acid), poly (Mangaraj, Yadav, Bal, Dash, & Mahanti,
(propylene fumarate), Polycaprolactone 2019; Samavedi, Poindexter, Van Dyke, &
Goldstein, 2014)

5
O.M. Atta et al.
Fig. 2. Properties and structures of various polysaccharides used in the development of films and coatings for food packaging applications.
Cellulose and its derivatives are explored for their potential appli­
cations in the food industry, which impart stability and improve the
quality of food. For example, the addition of BC increased the strength of
Tofu and improved the texture of chocolate drinks (Jiazhi, Xiaoli,
Huang, & Dongping, 2013). Similarly, the addition of cellulose to ice
cream not only made the texture creamy and smooth but also reduced
the calories and improved its melting resistance (Guo et al., 2018).
Cellulose has been used in the development of transparent packaging
films. A study reported the development of antimicrobial transparent
cellulose film from ginger via chemical treatment and ultrasonication.
The developed films showed high cellulose content (88%), thermal
stability, moderate crystallinity, and low moisture resistance (Abral
et al., 2020). The findings of this study show a cost-effective approach of
using low-cost ginger fibers for the development of transparent and
bioactive food packaging materials for their application in the food in­
dustry. Studies have also shown that the reinforcement material can
improve the properties of a polymer through polymerization or other
chemical reactions. The modified polymers could be used as surface
coatings and adhesives (Falguera et al., 2011).
Researchers have manufactured cellulose-based biodegradable films
for food packaging (Isik, Sardon, & Mecerreyes, 2014). A
nanocellulose-based edible and biodegradable gel-like cover has been
manufactured for food packaging (Xavier, Babusha, George, & Ramana,
2015). Cellulose requires an additive to produce antimicrobial or anti­
oxidant biomaterials. Therefore, some studies have reported the use of
metallic nanoparticles to synthesize cellulose-based antimicrobial films
(Di, Shi, Ullah, Li, & Yang, 2017). In a study, a thermoplastic containing
the BC enhanced the properties of corn starch. The film showed
enhanced water and gas barrier properties and relative humidity up to
80% (Fabra, López-Rubio, Ambrosio-Martín, & Lagaron, 2016). In
another study, BC/bovine lactoferrin (BC/bLF) edible antimicrobial
films were developed to directly cover the fragile food items that are
easy to spoil. The BC/bLF films showed high water vapor permeability,
mechanical properties, and bactericidal efficacy against two pathogens,
coliform and staphylococcus aureus. The BC/bLF films also showed in
vitro and in vivo biocompatibility (Padrao et al., 2016).
3.1.1.2. Starch. Starch is an important storage component in plants. It
is present in leaves, stems, roots, seeds, and fruits (Manan, Ahmad, et al.,
2017). Amylose, a linear compound and a major component of starch,
typically comprises 20–25% of plant biomass. In a few species like
maize, its content ranges between 50 and 90% of total plant biomass
(Zhang, 2015). Starch-based films are odorless, colorless, non-toxic,
bio-absorbable, oil-resistant, and semi-permeable to CO2, and
non-permeable to O2. A starch-based film with less oxygen permeability
and high water solubility improves the storage period of food by
blocking the oxygen supply and thus hindering the microbial growth
(Mohamed, El-Sakhawy, & El-Sakhawy, 2020, p. 116178). Similarly, the
6
Food Hydrocolloids 125 (2022) 107419
short and branchy amylopectin chains can arrange into a spiral shape
and make a natural starch bead granule. These granules are highly hy­
drophilic due to the presence of hydrogen bonding between the OH
groups on the bead surface.
Starch is mainly obtained from different agricultural waste such as
corn residues, potato peels, wheat, and rice husk (Bradley, 2010; Pfister
et al., 2020). The thermal decomposition of starch takes place at a high
temperature, thus making it a suitable material for the production of
thermoplastic starch (TPS) (Li et al., 2011). TPS is manufactured by
shearing the native starch in water under controlled temperature and
pressure. Then it is processed into a filler or rigid plastic-like traditional
plastic. It is capable of molding into the desired shape for a specific
application such as cast film and bottle blowing. TPS and starch films are
semi-transparent, with high water vapor permeability and good gas
barrier properties (Mohammadi Nafchi, Moradpour, Saeidi, & Alias,
2013). TPS is not considered comparable to traditional plastic due to its
high hydrophilicity and limited mechanical strength; nevertheless, its
quality can be improved by mixing it with different materials, which are
usually fossil-derived biodegradable polymers. The content of starch in
such copolymer ranges between 30 and 80% by weight. The addition of
the reinforcement material allows a partial mixing of starch; neverthe­
less, the obtained copolymer is fully biodegradable. The development of
strong starch-based copolymers has been reported with PLA, PHA/B,
polypropylene, polyurethane (Bradley, 2010). Moreover, several phys­
ical or chemical approaches such as blending (Oliveira, Cunha, &
Andrade, 2010), derivative synthesis (Heinze, Haack, & Rensing, 2004),
and copolymerization (Worzakowska, 2018) have also been used for
improving the properties of starch (Ojogbo, Ogunsona, & Mekonnen,
2020). Maize-starch-based coatings with improved barrier properties
are used for food packaging (Fabra et al., 2016). Starch has a wide range
of applications in the food industry: for example, the starch blends are
used in the making of packaging films, film bags, disposable paper plates
and cups, and disposable foam trays (Beckles, 2010; Mohammadi Nafchi
et al., 2013).
3.1.1.3. Galactomannans. Galactomannan is a stored neutral sugar in
seeds of dicots, especially legumes (Cerqueira et al., 2011). The het­
erogeneous polysaccharide chains of galactomannans are composed of
β-(1–4)-D-mannan and α-(1–6)-D-galactose. The mannose/galactose
ratio (M/G) of galactomannan decides its food or non-food applications.
The commercially available galactomannans with variable M/G ratio
are gum (Cyamopsis tetragonolobo, M/G ratio: 2:1), Tara gum (Caesalpi­
nia spinosa, M/G ratio: 3:1), and locust bean gum (Ceratonia siliqua, M/G
ratio: 3.5:1) (Cerqueira et al., 2011; Pawar & Lalitha, 2014). Generally,
locust bean and guar gum are of great commercial interest due to their
easy availability and low price (Prajapati, Kaushik, Malik, & Vijay,
2013).
Due to their plant-origin, non-toxic nature, and good physical
O.M. Atta et al.
properties, galactomannans have been used for various applications
such as textile, food, medicine, and cosmetics (Soares et al., 2015). At
very low concentrations, galactomannans make highly viscous solu­
tions; however, this process is slightly affected by variation in pH, heat
treatment, and ionic strength. A high acidic and alkaline environment
causes the degradation of galactomannan at high temperatures (Cer­
queira et al., 2011). At above 60 ◦ C, galactomannans have a high initial
viscosity but poor stability (Prajapati et al., 2013). The viscosity of
galactomannans tends to remain constant at pH between 1 and 10.5. The
use of galactomannans as films or coatings has been little explored as
compared to the other sugars. However, some recent studies have
brought new insights into the nature and use of edible galactomannan
membranes/coatings. Although some properties of fine galactomannans
gum powders in food systems have been studies, a further evaluation of
the physiological and rheological behavior and structural properties of
the agglomerated guar gum and locust bean gum powders prepared by
fluidized bed agglomeration would provide a more clear picture about
their use in food packaing applications (Lee & Yoo, 2021; Lima et al.,
2010; Martins, Cerqueira, Souza, Carmo Avides, & Vicente, 2010).
Despite the non-toxic nature and permissible substance for human
consumption, pure galactomannan has some limitations in terms of
weak mechanical strength and poor water resistance. In recent years,
much work has been done to evaluate the utilization of various materials
and to mix them with different biopolymers to enhance the properties of
polysaccharide based-films/coatings (Cerqueira et al., 2010). The
galactomannan-based coating with corn oil and glycerol is applied on
cheese that minimizes the weight loss and also modifies its color due to
less water vapor permeability and oxygen transport across the mem­
brane (Cerqueira et al., 2011). In addition, the physical and chemical
modification of pure galactomannan successfully modified its features.
The water vapor permeability and hydrophilicity of pure galactomannan
were reduced by strong UV treatment. The UV radiations consume the
free –OH groups and reduce the hydrophilic property of the modified
films. The chemical modification of pure galactomannan films by
glutaraldehyde enhanced the tensile strength up to 15 times and
generated smooth surface films (Zhao et al., 2019). The tensile strength
of galactomannan films was increased with the addition of glycerol and
sorbitol during film formation (Mikkonen et al., 2007). Locust bean gum
and wax-coated citrus fruits remained fresh for a longer time with less
weight loss and produced juice with better taste compared to the
non-treated citrus (Conforti & Totty, 2007).
3.1.1.4. Pectin. Pectin is a natural heterogenous polysaccharide that
contains a good amount of soluble fibers. It is an important component
of a typical plant cell wall and is made up of α-(1,4)-D-galacturonic acid
(Casas-Orozco, Villa, Bustamante, & González, 2015; Munarin, Tanzi, &
Petrini, 2012; Paula Judith Pérez Espitia et al., 2014). Upon mixing with
water, it makes a gelatin-like structure. Being a good source of fiber, it
helps fight diabetes, lowers cholesterol levels, and supports weight loss.
Pectin can be a suitable candidate for the manufacturing of edible films
for food packaging due to its biodegradability, biocompatibility, edi­
bility, and many good chemical and physical properties (e.g., gelation,
selective gas permeability) (Espitia et al., 2014). FDA has already
declared pectin as ‘Generally Recognized As Safe’ (GRAS), and it is
widely used as a stabilizing, gelling, and thickening agent in a variety of
food items like yogurt, frozen desserts, jams, jellies, and various milk
products (Brejnholt, 2010, pp. 234–262). Active packaging is the best
packaging system that has attributes beyond the basic barrier properties
that are achieved by adding active ingredients within the packaging
material and/or using different functionally active polymers (Falguera
et al., 2011). Generally, pectin films are used for active food packaging.
Hence these need to be antimicrobial, and the film components should
be non-toxic. The features of the pectin films mainly depend on their
source, preparation conditions, and synthesis method. For instance, the
pure pectin films possess low tensile strength and high elongation at
7
Food Hydrocolloids 125 (2022) 107419
break value which leads to easy-to-torn films during their preparation
and storage period (Lorevice, Otoni, de Moura, & Mattoso, 2016). The
development of a range of functional properties requires the designing
of films with a range of characteristics. The technique of copolymer
synthesis was introduced to add flexibility and enhance the mechanical
properties of pectin films. Active pectin films are produced by adding
marjoram essential oil with citrus pectin. The formation of hydrogen
bonding between pectin and essential oil increased the mechanical
strength (Almasi, Azizi, & Amjadi, 2020). Likewise, the introduction of
thyme essential oil to pectin films reduced the elongation at break value
(Lin et al., 2020). The edible pectin films with essential oil have anti­
microbial activity and can have pharmaceutical and therapeutic po­
tentials (Ghasemi, Jafari, Assadpour, & Khomeiri, 2017). Some
researchers also attempted to increase the hydrophobicity of the pectin
films. The incorporation of gamma-aminobutyric acid and curcumin in
the pectin matrix reduced the hydrophilicity of the modified films. The
addition of curcumin also increased the thermal stability of the films up
to 112.42% compared to the pure pectin films (Ezati & Rhim, 2020;
Meerasri & Sothornvit, 2020). Sometimes transparent films are
preferred over the non-transparent ones, for instance, when these are
used as coatings to protect the original appearance of wrapped or coated
food. According to a previous study, a highly transparent film was
formed when pectin was combined with 23% by weight of beeswax
(Maftoonazad, Ramaswamy, & Marcotte, 2007). Antimicrobial activity
is an important feature of the coating system to minimize or completely
prevent the growth of microorganisms. A study reported the develop­
ment of edible pectin film with nisin protein via ionization radiation.
The developed film was used as the packaging material for meat to
prevent the growth of Listeria monocytogenes (Espitia et al., 2014).
Generally, the shelf-life of dairy products is very less. Citrus pectin and
fish gelatin-based films were developed to wrap Tunisian cheese. The
packaging material effectively controlled cheese dehydration and
reduced bacterial growth (Ezati & Rhim, 2020).
3.1.1.5. Chitosan. Food waste and loss and foodborne diseases are the
major concerns of the food industry. A significant reduction in food
spoilage can save billions of dollars for the world economy every year. In
addition to other biopolymers, chitosan is also receiving immense
consideration in the food industry. Chitosan is obtained from chitin
which is found in the outer structure of crustaceans as well as found in
the wall of fungus and other biological substances. It is mainly β-1,4-
linked 2-acetamido-2-deoxy-D-glucose. The high degree of deacetylation
and average molecular weight make chitosan an important candidate for
antimicrobial applications. Besides antimicrobial activity, chitosan films
are known for high mechanical strength, high water vapor transport,
and selective gas permeability (Tan, Ma, Lin, Liu, & Tang, 2013). These
distinctive properties of chitosan are important for the manufacturing of
edible films for the food industry. The physical properties of chitosan
can be further enhanced by combining it with neutral lipids, fatty acids,
and waxes (Lopez et al., 2017). Meanwhile, chitosan-based films are
unstable and have weak moisture barrier properties due to their high
hydrophilicity, which limits their utility in food packaging applications
(Ojagh, Rezaei, Razavi, & Hosseini, 2010). Furthermore, the incorpo­
ration of lipids into the chitosan-based films impairs the 3D network of
chitosan and adversely influences its mechanical properties (Santos,
dosSilva, Xavier, Leite, & Aroucha, 2017). In an earlier study, the
concept of developing blend or multilayer films from selected bio­
polymers has arisen as a viable technique for developing new sustain­
able packaging materials with enhanced features above
single-component films. In this context, a considerable improvement
in the mechanical characteristics and a decrease in the hydrophilicity of
the composite films composed of chitosan, CMC, and sodium alginate
were observed (Lan, He, & Liu, 2018). Recently, a multilayer film
comprised of chitosan with thyme essential oil was prepared. The
improved UV blocking ability and elongation at break was observed in
O.M. Atta et al. Food Hydrocolloids 125 (2022) 107419

the modified films but water vapor permeability was increased due to
more porous structure (Zhang et al., 2021). The antifungal and antimi­
crobial chitosan films are produced by enhancing their cationic nature.
In a study, spherical, small, and very stable chitosan nanoparticles were
prepared with lemon essential oil and grass carp collagen. The devel­
oped composite featured a higher tensile strength and a higher elonga­
tion at break. These films effectively prevented lipid oxidation and
microbial growth (Jiang et al., 2020). In another study, active films
based on natamycin-enriched chitosan were prepared by immersing the
films at various temperatures in 95% ethanol, and the antimicrobial
activity was evaluated. In the treated cheese samples, a substantial
decrease in yeasts and molds growth was noticed (Santonicola, Ibarra,
Sendón, Mercogliano, & de Quirós, 2017). Table 3 summarizes the ap­
plications of chitosan-based films in the food industry.
3.1.1.6. Alginate. Alginate is a natural polysaccharide present in the
cell wall of various brown algae (Ferreira, Alves, & Coelhoso, 2016;
Senturk Parreidt, Müller, & Schmid, 2018). It contains β-D-mannuronic
acid (M) joined to α-L-guluronic acid (G) joined through α-1,4-glycoside
linkage (Fig. 2) (Nadi et al., 2019). The properties of alginate depend on
the source and the ratio of M and G units in the polysaccharide chain
(Meng & Liu, 2013). Alginate has good colloidal properties, thickening
stability, gel-forming ability, and good moisture retention capability
(Dou et al., 2018). Besides, alginate has the ability to interact with di-
and trivalent cations during film formation. The crosslinking of alginate
with cations produces a highly stable 3D structure of films by estab­
lishing β-(1,4)-linkages between the G and M blocks and forming the
mannuronic acid form. The linear and flexible conformation is shown by
M block segments, although guluronic acid gives rise to α-(1,4) linkages
(G block), which serve to add a steric impediment around the carboxyl
groups. The G block provides folded and rigid structural conformations
responsible for the pronounced rigidity of the molecular chains. These
3D grid arrangements are known as ‘Egg box’ models (Yang, Xie, & He,
2011). Because alginate films are hydrophilic, these provide poor
moisture barrier properties; nevertheless, calcium limit the water vapor
permeability of these films and make them water-insoluble. Calcium has
the capability to crosslink with alginate by interacting with G. There­
fore, varying the number of G results in the formation of films with
varying water vapor permeability. With other edible films, the behavior
of alginate films is dependent on both the ambient relative humidity and
the plasticizer. Thus, evaluating the characteristics of alginate films
under various relative humidity settings and with various plasticizers is
critical for establishing whether these films are suitable for a particular
meal (Olivas & Barbosa-Cánovas, 2008). An alginate-based food gelling
agent is synthesized through crosslinking of alginate with calcium ions
(Cao, Lu, Mata, Nishinari, & Fang, 2020). This gelling agent is better
than gels prepared by alginate-manganese, aluminum, and ferrous ions
crosslinking. The efficiency of alginate as an antimicrobial agent can be
enhanced by incorporating antimicrobial compounds. For instance, the
addition of 3% potassium sorbate in sodium alginate coating signifi­
cantly enhanced the antimicrobial activity in cheese against Enterobacter
spp (Lucera et al., 2014). Alginate is already in use in the food industry
as a stabilizer, thickening, and gelling agent. For example, the preser­
vation of grapes after harvest is a well-established process for coating
grapes with alginate and CMC with brewer yeast (Yinzhe & Shaoying,
2013, p. 2013). A study also reported that coating of pineapple slices
with sodium alginate, lemongrass (0.3%), and glycerol prolonged the
freshness of fruit for more than 16 days after cutting (Azarakhsh et al.,
2014). Similarly, Chen et al. developed alginate and thymol films and
used them for preservation and maintaining the freshness of cut vege­
tables and fruits for a longer time (Chen et al., 2021). Alginate films
loaded with salicylic acid presented better bacterial growth inhibition
against P. aeruginosa, S. aureus, E. coli, and S. typhimurium (Kurczewska,
Ratajczak, & Gajecka, 2021). All these studies show that alginate-based
films could be useful candidates for the packaging of different food
items, both on small and industrial scales.
3.1.1.7. Pullulan. Pullulan, a water-soluble exopolysaccharide, was
first isolated from Aureobasidium pullulans, a ubiquitous fungus
commonly isolated from soil, water, and plant materials (Liang & Wang,
2015). It is a maltotriose trimer made up of α-(1,6)-linked (1,
4)-α-D-triglucosides. Due to the presence of both α-(1,6) and α-(1,4)
linkages, this polysaccharide is considered as intermediate of amylose
and dextran. This unique linkage combination gives pullulan a high
solubility in water and high flexibility (Trinetta & Cutter, 2016). The
edible pullulan powder is white in color, odorless, tasteless, non-toxic,
noncarcinogenic, and biodegradable (Oğuzhan & Yangılar, 2013). It
has good material forming properties such as high thermal stability,
good mechanical strength, non-hygroscopic, and is capable of forming
nanofibers, thin layers, nanoparticles, and coatings (Farris et al., 2012).
The pullulan films can be as thin as 5 μm, and are transparent with
excellent mechanical properties and oxygen-barrier characteristics
(Singh, Saini, & Kennedy, 2008). The use of pure pullulan films is not
suitable for packaging application due to their brittleness and high hy­
drophilicity. These limitations can be bypassed by preparing
pullulan-based composite films or blends to obtain multifunctional
packaging to ensure food quality and safety. pullulan has been combined
with essential oils, nanoparticles, cellulose, graphene oxide, gelatin, and
several other materials to prepare pullulan-based films and coatings for
various applications (Table 4). Pullulan-based edible films were devel­
oped to preserve the sensitive fruits such as strawberries and mangoes
(Yan et al., 2020; Zhou et al., 2021). A pullulan-based antimicrobial film

Table 3
Some chitosan sources and their use as a matrix for the reinforcement of different materials for various food applications.
Source Reinforcement materials Applications References

Arthropods Zinc oxide (ZnO) nanoparticles
Magnesium oxide (MgO)
Iron oxide (Fe3O4)
Silicon dioxide (SiO2)
Glycerol
Arthropods or Antimicrobial plant extracts
microorganisms
Purple yam starch (PYS) and
glycerol
Chinese chive root extract
Whey protein
Banana peels
Carboxymethyl cellulose
Xylan and carvacrol
Moringa oil
Laponite immobilized AgNPs
Lemon essential oil
Food preservative Packaging material
Food packaging
Food applications
Food processing and preservation
Food products preservation
Antimicrobial coating of vegetables and
fruits
Food biodegradable films
Bio-composite food packaging material
Oxidatively stable encapsulates for food
Apple coating
Fresh strawberries coating
Food packaging application
Packaging of cheese
Active food packaging
Food packaging
Franklin et al. (2007)
De Silva et al. (2017)
Shahbazi and Shavisi (2019)
Yu et al. (2012)
Epure, Griffon, Pollet, and Avérous (2011); Fajardo et al. (2010)
Park, Byun, Kim, Whiteside, and Bae (2013)
Martins da Costa, Lima Miki, da Silva Ramos, and Teixeira-Costa
(2020)
Riaz et al. (2020)
Lekshmi et al. (2019)
Ullah et al. (2020)
Shahbazi (2018)
Kamdem, Shen, and Nabinejad (2019)
Lin, Gu, and Cui, (2019)
Wu, Huang, Li, Xiao, and Wang (2018)
Jiang et al. (2020)

8
O.M. Atta et al. Food Hydrocolloids 125 (2022) 107419

Table 4 procedure, geographic territory, and stability under specific storage

Role of pullulan as a matrix for reinforcement material for various applications conditions (Mishra et al., 2020). Essential oils are widely used in food,
in the food industry. cosmetics, and pharmaceutical industries due to their low toxicity,
Reinforcement material Applications References natural origin, and low production cost. An active film is a characteristic
Chitosan Antimicrobial food- Li, Yi, Yu, Wang, and Wang
of food packaging, and it is important to thoroughly examine the me­
packaging (2020) chanical, optical, and barrier properties of the active film, in addition to
Rockrose essential oil Food packaging Luís, Ramos, and the mechanical strength, elasticity, and water vapor permeability
Domingues (2020) (Ramos et al., 2013). Several elements influence the mechanical prop­
AgNPs and essential oils Meat industry Khan, Kumari, Selamat,
erties of essential oils-loaded packaging films. The essential oil/­
Shameli, and Sazili (2020)
Tapioca starch Food Packaging Sheng et al. (2018) plasticizer or polymer matrix/essential oil ratio and the source and
Gelatin Food applications Zhang et al. (2019) properties of essential oil are the key factors that should be considered
Oil blend encapsulated Functional food Bakry et al. (2016) during the manufacturing of films loaded with essential oil for a specific
with whey protein applications application (Ramos et al., 2013). The yellow hydrophobic films with less
Whey protein nanofibers Food and Drosou, Krokida, and
pharmaceutical Biliaderis (2018)
water vapor permeability and average tensile strength were prepared by
industries combining glycerol-plasticized mesquite seed gum and palm fruit oil.
Capsaicin Antimicrobial food- Zhang et al. (2018) The developed composite films, due to their yellow appearance, can be
packaging used for orange and yellow fruits packaging (Rodrigues, Cunha, Brito,
CMC Fruit preservation Shao, Niu, Chen, and Sun
Azeredo, & Gallão, 2016). The edible films of chitosan and sunflower oil
(2018)
Cinnamon essential oil Antimicrobial film Chu et al. (2019) are used to enhance the quality of meat products. The
and Tween 80 chitosan-sunflower oil films modulated the oxygen permeability in
Chitosan Fresh Papayas coating Zhang et al. (2019) coated hamburgers compared to the pure chitosan films (Vargas, Albors,
Nano-TiO2 Food packaging Liu et al. (2019) & Chiralt, 2011). Another study reported the stable firm structure,
Seaweed extract Meat storage Seol, Lim, Jang, Jo, and Lee
conserved taste, and color of kiwi fruits with extended shelf-life when
(Carrageenan) (2009)
Sweet basil extract Apples storage Synowiec et al. (2014) coated with rice bran oil films (Hassani, Garousi, & Javanmard, 2012).
The lipophilic nature of essential oils helps them penetrate the bac­
terial membrane and interfere with the cell functions; hence they are
to prevent the growth of foodborne pathogens was developed by antimicrobial in nature. The incorporation of cinnamon essential oil into
combining nisin, thymol, lauric alginate, and polyethylene with pullulan chitosan film enhanced the antimicrobial activity of the film. On the
on the top. This pullulan-based packaging film showed good antimi­ other hand, the cinnamon essential oil level, water-solubility, water
crobial activity against E. coli, L. monocytogne, salmonella spp. and vapor permeability, and elongation at break were reduced (Seow et al.,
S. aureus in meat and poultry items (Hassan & Cutter, 2020). In another 2014; L.; Wang et al., 2011). Some researchers focused on the devel­
study, pullulan-based pickering emulsion with clove essential oil opment of edible films from fruit purees due to their great oxygen bar­
exhibited excellent water barrier properties, antioxidant activity, and rier. The water barrier properties of the films were enhanced by adding
improved mechanical properties (Shen et al., 2021). Pullulan is com­ essential oil, while their texture was enhanced by adding pectin and
bined with butyric anhydrous, propionic anhydride, and acetic anhy­ alginate. The modified films showed strong antimicrobial, good me­
dride to synthesize pullulan-butylate, pullulan-propionate, and chanical features, and enhanced moisture barrier characteristics when
pullulan-acetate with different concentrations of pullulan. The esteri­ applied on fresh-cut apples (Artiga-Artigas, Acevedo-Fani, & Martín-­
fied pullulan-based films slowed down the fruit ripening and thus Belloso, 2017; Hu, Jiang, Xiu, & Feng, 2018). Few studies have been
increased the shelf-life (Niu et al., 2019). In a study, edible and carried out to establish the effects of essential lemongrass oils loaded
eco-friendly packaging film was produced from pullulan and lysozyme with edible coats for fresh fruits (Azarakhsh et al., 2014). The antioxi­
microfibers. The casting of lysozyme in the pullulan matrix increased the dant activity of essential oils can also be controlled through the scav­
film-forming potential of pullulan and contributed to increasing the enging mechanism of reactive oxygen species. The terpenoids present in
mechanical strength of the film. In addition, the pullulan-lysozyme film essential oils possess high antioxidant activity (Hasheminya et al.,
showed good antimicrobial activity against S. aureus (Silva, Vilela, 2019). Starch-based active food packaging films incorporated with
Almeida, Marrucho, & Freire, 2018). The pullulan-based film also pre­ rosemary and oregano essential oils have high antimicrobial and anti­
vented the growth of L. monocytogenes in turkey meat during cold stor­ oxidant activity (Estevez-Areco, Guz, Famá, Candal, & Goyanes, 2019;
age for a longer time (Trinetta & Cutter, 2016). Medeiros et al., 2019). Further, the films with oregano, cinnamon, or
lemon essential oils presented a more smooth, porous, and uniform
3.1.2. Lipids surface. The films also possessed high plasticizing characteristics with
Lipids have non-polar chemical properties and are easily soluble in thick and less compact structures. During the manufacturing process of
non-polar solvents like hexane and chloroform (Mohamed et al., 2020, edible films supplemented with essential oils, the use of dry heating can
p. 116178). These originate from natural sources like plants, insects, and easily degrade the volatile compounds. Therefore, preventing the loss of
animals and are categorized into fatty acids, galactolipids, phospho­ useful volatile compounds is of great concern (Tongnuanchan & Ben­
lipids, glycerolipids, sphingolipids, and Vitamins (A, K, and D) based on jakul, 2014). To this end, the substitution of essential oils with
their structure and function (Manan, Chen, She, Wan, & Zhao, 2017). food-grade oleoresins could be a better choice for preserving the volatile
For decades, lipids have been used in the food industry to develop edible compounds with a positive impact on the food quality.
films and coatings for food preservation. The lipid-based coatings add a
glossy, shiny look to the fruits and vegetables and reduce the moisture 3.1.2.2. Waxes. Waxes are made from alcohol or esters of long-chain
loss due to their hydrophobic properties. Moreover, their production fatty acids and have a higher molecular weight. These act as the
process is cost-effective and minimizes the packaging complexity (Hall, covering to protect the plant and animal tissues and serve as a water
2011). barrier against harsh environmental conditions. Therefore, waxes can be
used as water-resistant edible coatings for food packing (Mohamed
3.1.2.1. Essential oils. Essential oils contain lipophilic and small volatile et al., 2020, p. 116178). Several researchers have used the insect-waxes
compounds such as aldehydes, phenols, terpenes, ketones, alcohol, and like bee-wax and plant-waxes like candelilla wax and carnauba wax for
ethers which are responsible for their biological properties. The flavor encapsulation and making water-resistant food coatings. Natural
composition of essential oils varies according to their source, extraction

9
O.M. Atta et al.
waxes have excellent rheology and microstructure. In the food industry,
waxes are also used as anticaking, lubricating, and flavor releasing
agents in the preparation of chewing gums, fresh fruit juices, sauces, soft
candies, and bakery items (Milanovic et al., 2010). Carnauba wax ob­
tained from the Brazilian palm tree is the hardest commercially avail­
able wax with a high melting temperature. It is highly elastic and
resistant but less viscous than the bee-wax (Shellhammer, Rumsey, &
Krochta, 1997). Carnauba wax is also used in the preparation of orga­
nogels in combination with soybean oil (Buitimea-Cantúa et al., 2021).
Organogels are defined as vegetable oil with a solid structure. These can
efficiently replace the trans-fats and highly saturated fats in a variety of
food products such as sausages, yogurts, bar cheese, creams, fillings, and
cookies (Chaves, Barrera-Arellano, & Ribeiro, 2018; Lim, Jeong, Oh, &
Lee, 2017). A water-resistant, low water permeability and good me­
chanical strength edible film was developed by combining bee-wax with
cassava starch and whey protein (Cortés-Rodríguez, Villegas-Yépez, Gil
González, Rodríguez, & Ortega-Toro, 2020). The films with cassava
starch and whey protein alone are not suitable for food coatings in the
humid environment due to their high hydrophilicity (Basiak, Lenart, &
Debeaufort, 2017). The addition of wax provides a water barrier due to
its hydrophobic nature. Brea gum collected from Cercidium praecox tree
gum is used for the development of a food emulsion by adding bee wax
and glycerol. The bee wax and glycerol act as the plasticizer and mois­
turizing buffer, whereas Brea gum provides the mechanical strength to
the emulsion (Spotti, Cecchini, Spotti, & Carrara, 2016). Further
research reported that cold plasma and the coating of carnauba wax are
effective in minimizing the water sensitivity of films made up of
myofibril proteins from fish. The fish protein films have promising
properties for use in food packaging; however, it has limited hydrophilic
activity. A combination of cold plasma and the coating of carnauba wax
could be an alternative to improve the packaging characteristics of
protein films that answer the need to minimize the accumulation of
synthetic plastics in nature using environmentally friendly tools and
technologies (Romani et al., 2020, p. 106087). The carnauba wax
coating on guava resulted in less affected flesh firmness, decreased
weight loss, decay, and chlorophyll degradation after 12 days at room
temperature. The edible coating of carnauba wax with sorbic acid
(0.1%) and triclosan (1%) actively maintained the post-harvest quality
of mango. The coated mangoes demonstrated better taste and compact
epidermis even after 35 days of storage. The wax coating prevented the
growth of yeast, molds, and mesophilic bacteria during storage at 10 ◦ C
and at room temperature. Carnauba wax coating also retained the high
level of antioxidants, anthocyanin, tanning, ascorbic acid content, and
sensory quality of pomegranate during storage of 60 days at 3–5 ◦ C
(Barman, Asrey, Pal, Kaur, & Jha, 2011). A 60% mixture of palm wax
with fish gelatin films showed enhanced flexibility, opaqueness, and
thickness. Also the incorporated palm wax improved the UV barrier
properties of films despite losing the appearance of colorless and
transparent gelatin film, which could be beneficial to preserving the
photosensitive food products by preventing their oxidation (Syahida,
Ismail-Fitry, Ainun, & Hanani, 2020). The addition of bee-wax in a
polysaccharide-based film decreased the tensile strength and Young’s
Modulus of the films (Spotti et al., 2016). Thus, it could be concluded
that waxes from different sources could be useful in making films and
coatings for their application in food packaging applications.
3.1.3. Proteins
Proteins are biopolymers with complex compositions and structures.
The high intermolecular binding ability of proteins makes them suitable
for multiple functions and applications. The capability of proteins to
interact with the neighboring molecules enable them to form strong,
viscoelastic, and cohesive films. The film properties are highly depen­
dent on molecular characteristics like molecular weight, flexibility,
charge, and conformation, and thermal stability of the protein molecule.
Moreover, the amino acid sequence, degree of elongation, and interac­
tion among the protein chains also influence the mechanical properties
10
Food Hydrocolloids 125 (2022) 107419
of the film (Calva-Estrada, Jiménez-Fernández, & Lugo-Cervantes,
2019). The raw materials used to produce protein-based films can be
of animal (collagen, casein, and whey protein) or plant (soy protein)
origin. For instance, the edible casein layer is attractive to food appli­
cations because of its high nutritional quality, excellent sensory prop­
erties, and adequate food protection regardless of the strong potential of
the surrounding environment. Gelatin is one of the first materials used to
form the walls of polymer capsules in microencapsulation (Samakrad­
hamrongthai et al., 2019). Soy and whey proteins are used along with
plasticizers in the manufacturing of films for food coating with less ox­
ygen permeability, transparency, and high solubility in water
(Pérez-Gago, Maria, & Krochta, 2012). Major proteins, their properties,
and their applications in the food industry are summarized in Table 5.
3.1.3.1. Casein. Casein is a common, cheap, non-toxic, highly stable,
and easily available group of proteins obtained from milk. It contains
αs1-casein (38%), αs2-casein (10%), β-casein (36%), and κ-casein
(13%). In the food industry, casein is generally used as an emulsifier and
dietary supplement (Bhat et al., 2016, pp. 1–17; Raghav, Agarwal, &
Saini, 2016). Casein proteins produce water-insoluble, opaque, and less
oxygen permeable films. Casein-based films or coatings easily dissolve in
water due to their accessible secondary structure, and such films are
easy to mold. In addition, casein films possess high consistency, which
has gained attention in recent years, largely as a result of the propensity
to supply by-products with high added value (Murrieta-Martínez et al.,
2018).
Natural proteins have good functional features suitable for making
food packaging films. However, some limitations such as low water
resistance, low mechanical strength, and high shear stress of most pro­
teins must be resolved before using them for making films. The polymer
network can be modified via crosslinking of polymer chains to enhance
film functionality with chemical and physical treatments (Bonnaillie
et al., 2014). As casein-based films are hydrophilic, these are highly
permeable to water vapors; the addition of hydrophobic elements such
as lipids into the hydrophilic films can enhance the moisture barrier
characteristics of the films (Bosquez-Molina, Guerrero-Legarreta, &
Vernon-Carter, 2003; Ohya et al., 2006). The packaging characteristics
of the casein-based film could also be improved by the dielectric barrier
discharge (DBD) cold plasma technique. A study showed the aggregation
and crystal structure of casein-based films (Wu et al., 2020). Films ob­
tained by blending the casein hydrolysates with polyvinyl alchohol are
recently evaluated as a protective carrier against active bacterium cul­
tures of Lactococcus lactis and Lactobacillus sakei. This approach can be
used to carry biocontrol agents against food pathogens in active pack­
aging films (Settier-Ramírez, López-Carballo, Gavara, & Hernández-­
Muñoz, 2021). An increment in the antimicrobial activity of ZnO
nanoparticles was achieved through their incorporation into casein films
through double polymerization that also enhanced the structural
morphology of the film (Ma et al., 2019). The combination of tannic acid
with casein improves the physical and chemical properties of films for
use in food applications (Picchio et al., 2018).
3.1.3.2. Whey. Whey is a by-product liquid obtained left after curdling
of milk during cheese preparation. According to an estimate, around 180
million tons of whey is produced annually. Its disposal is a serious
environmental concern because of its high organic matter content and
high demand for biological oxygen (Zhou, Hua, Huang, & Xu, 2019).
Whey is a nutritious material containing about 75% proteins, among
which 15%–20% are milk proteins, fats, minerals, and other organic
matters (Lappa et al., 2019). Whey is a rich source of essential and
branched-chain amino acids, which play a key role in skeletal muscle
protein synthesis (Hulmi, Lockwood, & Stout, 2010). Due to their hy­
drophilic nature, whey proteins do not form films of adequate moisture
barrier; nevertheless, such properties could be enhanced by the addition
of hydrophobic materials in the form of bilayer films, emulsion films, or
O.M. Atta et al.
Table 5
Summary of few major proteins and their properties used in the manufacturing of biomaterials for food applications.
Protein Properties Applications
Soy- Versatile, clear, cost-effective, Clear packaging films, biodegradable
protein lightweight plastic sheets, and adhesives
Whey Clear, durable, low moisture Flavor stabilizer, moisture, and oxygen
Proteins content, and high plasticizing resistant films, and films with high
ability strength
Collagen Good mechanical properties Food additives, dietary Supplements,
edible films, and coatings
Casein Cheap, non-toxic, flexible, and Emulsification and dietary supplement
highly stable
nanoparticles. The mechanical properties of edible films are determined
by protein-protein interactions in whey protein film matrices. By and
large, it appears as whey protein films have a low tensile strength than
conventional petroleum and polysaccharide-based films. The optical
properties of packaging materials are useful for observing the visual
characteristics of the primary packaging, and thus influences the con­
sumer preference and choice. To this end, the coatings of whey protein
improved visual quality (Janjarasskul & Tananuwong, 2019). Among
the different biopolymeric materials used for food packaging, whey
proteins are receiving immense consideration. Compared to the tradi­
tional packaging materials, whey proteins have specific advantages to
enhance the food quality and shelf-life and to develop new functions.
The whey proteins-based films have high clarity, durability but low
barrier properties against oil and gases. The film-forming tendency of
whey proteins depends upon the pH and temperature of the film-forming
solution. The plasticized whey-based films can be produced by heating
the 8–12% protein solution at 75–100 ◦ C for a few minutes. This treat­
ment causes irreversible denaturation of whey protein, hence preserving
the film structure (Chen et al., 2019). Several other chemical and
physical techniques can improve the properties of whey films. For
example, UV treatment of films with high whey protein content signif­
icantly improves the mechanical properties of the films, like tensile
strength, elastic modulus, and puncture deformation (Díaz, Candia, &
Cobos, 2016). Similarly, ultrasound treatment of whey films also makes
them strong, where the treatment duration directly affects the strength
of the films (Chen et al., 2019). The addition of glycerol in whey protein
isolates (WPI) plasticized the biofilms, and the inclusion of bergamot
and lemon essential oil improved the antimicrobial activity of these
plasticized biofilms (Çakmak, Özselek, Turan, Fıratlıgil, & Karban­
cioğlu-Güler, 2020). However, the characteristics of the water barrier in
whey protein-dependent films are weak, which could be enhanced by
using essential oils and lipids. For example, a study reported that the
addition of rapeseed oil reduced the water solubility of edible whey
films and increased the hydrophobic properties (Galus & Kadzińska,
2016). Similarly, a combination of polyvinyl alcohol with WPI increased
the water absorption capacity of the films (Lara et al., 2020). Whey
protein, pecan nut shell extract (PNSE), and glycerol-based active
packaging films inhibited the growth of foodborne pathogens like
Enterococcus faecalis, Salmonella enterica subsp. enterica ser., and Typhi­
murium. PNSE also improved the antioxidant properties of the films in a
water medium (Arciello et al., 2021).
Whey proteins-based membranes containing non-toxic natural anti­
oxidants could be safe alternative for preventing the oxidation of food
components, especially lipid oxidation. In a study, the WPI-coated films
showed high water vapor, better oxygen barrier characteristics than the
traditional films, and reduced the lipid oxidation of frozen meatloaves
after six months of storage (Song, Choi, Choi, Yoon, & Han, 2020).
Edible whey protein film is a good candidate for flavor carriers, thanks
to its distinct aroma and oxygen barrier. Whey proteins can capture and
stabilize the flavor during processing with fine and nano-encapsulation
techniques and control the release under certain conditions (Janjar­
asskul & Tananuwong, 2019). Whey proteins also serve as carriers for
11
Food Hydrocolloids 125 (2022) 107419
Ref.
(Calabria et al., 2012; Guo et al., 2018; Otoni, Avena-Bustillos, Olsen, Bilbao-Sáinz,
& McHugh, 2016; Yu et al., 2018)
(Ghasemi et al., 2017; Hassani et al., 2012; Janjarasskul & Tananuwong, 2019;
Lara et al., 2020; Soukoulis, Behboudi-Jobbehdar, Macnaughtan, Parmenter, &
Fisk, 2017; Zolfi, Khodaiyan, Mousavi, & Hashemi, 2014)
(Bhuimbar, Bhagwat, & Dandge, 2019; Chak, Kumar, & Visht, 2013;
Chattopadhyay & Raines, 2014; Hashim, Ridzwan, Bakar, & Hashim, 2015; Jiang
et al., 2020)
(Bhat, Dar, & Singh, 2016, pp. 1–17; Bonnaillie, Zhang, Akkurt, Yam, & Tomasula,
2014; Ma, An, Xu, Fan, & Wang, 2019; Picchio et al., 2018; Wu et al., 2020)
beneficial live microorganisms. For the protective supply of an appro­
priate amount of probiotics to the gut of consumers, the whey protein
matrix with alginate and pectin was developed (Soukoulis et al., 2014).
Another research group produced high thermally stable yellow color
whey protein films by adding alginate and pectin in the matrix (Chak­
ravartula et al., 2019).
3.1.3.3. Collagen. Collagen, a fibrous protein, is the most abundant
extracellular protein present in the animal kingdom. It provides support
to connective tissues because of its rigidity and resistance to stretching.
Such features are ideal for biomaterial production for different appli­
cations such as tissue engineering (Miranda-Nieves & Chaikof, 2017),
drug delivery (Yu, Tang, et al., 2015), and in the food sector (Qamar,
Asgher, Bilal, & Iqbal, 2020, p. 109625). The primary collagen is
extracted from the bone and skin of cattle and fish and is used in the
preparation of functional biomaterials having good biocompatibility
and biodegradability (Hashim et al., 2015). Research has already
documented that collagen films are better in terms of their optical
properties, as the brightness is greater than 80% in the visible spectrum.
A study showed that the light transmittance of collagen-based films was
improved to more than 90% with increasing wavelength and then
remained constant throughout the visible light range.
Collagen-based bioplastics are synthesized by the extrusion process
and possess good mechanical properties (Qamar et al., 2020, p. 109625).
In a study, the partially denatured collagen, water, and glycerol were
used to produce plasticized collagen to prepare pet food using the
molding technique (Meyer, 2019). Grass carp collagen films are syn­
thesized for the controlled release of lemon essential oil with high sta­
bility and efficiency. The collagen/lemon essential oil/chitosan-based
films demonstrated high tensile strength, low oxygen permeability,
antimicrobial activity, and sustained release of nanocapsules, and were
found useful for meat preservation (Jiang et al., 2020). The hydrogel
film prepared from silver nanoparticles (AgNPs), the extract of grape­
fruit seed, and ternary blend agar/alginate/collagen have high clarity,
tensile strength, water solubility, and antimicrobial activity (Wang &
Rhim, 2015). The fish-derived collagen films with chitosan and 5%
pomegranate peel extract surprisingly decreased the water solubility
and demonstrated antibacterial activity against foodborne pathogens
(Bhuimbar et al., 2019). A recent study reported the development of less
water vapor sensitive economic food packaging film by adding SiO2 with
alginate and hydrolyzed collagen blend (Marangoni Júnior, Silva,
Vieira, & Alves, 2021).
3.1.3.4. Soy protein. Soy protein has become one of the important
proteins for food packaging applications due to its worldwide abun­
dance. It is commercially available in three forms: flour (54%),
concentrate (72%), and isolates (90%) (Li, Zeng, Wang, Yang, & Wang,
2008). Soy proteins are an appealing alternative for food packaging
applications due to their great film-forming ability and low cost. The soy
protein-based films provide excellent oxygen barrier properties at low
relative humidity, which is critical for preventing the oxidative deteri­
oration of food quality within the packaging material (Umaraw &
O.M. Atta et al.
Verma, 2017). Moreover, these films are economical, sustainable, clear,
biodegradable, and biocompatible. However, the soy protein-based
films are usually brittle and have insufficient moisture barrier charac­
teristics (Tian et al., 2018). Glycerol is frequently used to plasticize the
soy protein films, which increases their flexibility but lowers their
moisture resistance further due to their hydrophilic nature (Rani &
Kumar, 2019). Other components, such as polysaccharides, lipids, or
plant extracts, have been incorporated into soy protein-based films to
improve their mechanical or physical properties (Cao, Fu, & He, 2007).
In some studies, cellulose nanocrystals and pine needle extract were
used to enhance the characteristics of soy protein-based film. The
phenolic compounds present in the pine needle extract exhibit strong
antioxidant activities; hence soy proteins-based films can be used as
active food packaging materials with increased mechanical strength and
antioxidant activity (Yu et al., 2018). Another study reported the addi­
tion of lactic acid along with cellulose nanocrystals and pine needle
extract to prepare biodegradable and mechanically strong films. The
developed film showed low sensitivity towards oxidation, which makes
it an ideal material for food packing (Yu et al., 2019). A two-layer soy
film with PLA was designed for high clarity, good adhesion, and anti­
microbial activity for use as the active food packaging material
(González & Igarzabal, 2013). Soy hydrogels can also be a suitable
carrier for bioactive compounds. Soy fibrils-epigallocatechin gallate
(EGCG) hydrogels have improved bio accessibility of EGCG, antioxidant
activity, viscosity, foam forming quality, and stability (Tong et al.,
2022).
3.1.4. Other polymers
3.1.4.1. Polyhydrooxyalkonate and poly-3-hydroxybutyrate. Poly­
hydrooxyalkonate (PHA) is a biopolymer produced by bacteria as an
intracellular carbon and energy storage compound (Fig. 3) (Aung, Shein,
Aye, & Nwe, 2018; Manikandan, Pakshirajan, & Pugazhenthi, 2020;
Pérez-Arauz et al., 2019; Tan et al., 2020; Zhang et al., 2018). PHA
Fig. 3. A comparison between PLA, PHA, and PLA/PHA composite in terms of their properties and applications in the food sector.
12
Food Hydrocolloids 125 (2022) 107419
attracts great scientific interest due to its excellent thermoplastic prop­
erties that range from transparent elastic material due to its solid and
opaque nature with high material strength. It is considered a good
replacement for petrochemical plastics. A variety of microorganisms
with diverse habitats can accumulate PHA as a product of several
metabolic pathways, including de novo fatty acid biosynthesis,
beta-oxidation, and tricarboxylic acid cycle (Jung, Lee, & Tam, 2010).
To date, about 167 PHA-producing microorganisms have been identified
(Foong et al., 2014; Koller, Salerno, & Braunegg, 2014), which use a
wide range of renewable substrates for the production of PHA (Tan et al.,
2020). PHA is widely used in many applications, such as for cell adhe­
sion and proliferation, as a plasticizer, and in bio-implants (Naveen
et al., 2015; Sin, Tan, Annuar, & Gan, 2014; Zhang et al., 2018). Peanut
oil was used to manufacture films of new PHA for use as biodegradable
packaging for use in the food industry. In the synthesized PHA, the
melting temperature decreased while the elongation increased during
intervals compared to the homopolymer PHB. In addition, the degra­
dation profile of PHA film in soil indicated a 75% weight loss in 3
months. The properties of PHA films allow their use in food packaging
and biotechnology industries (Pérez-Arauz et al., 2019).
Poly-3-hydroxybutyrate (PHB) is a polyester that falls under the PHA
category. The petrochemical plastics can be replaced by PHB, as these
closely resemble their physical and chemical properties. Although PHB
is versatile and its structure and composition can be modified, its high
production cost, high crystallinity, and low resistance to thermal
degradation are the main limitations for its direct use as a packaging
material. Therefore, several other materials such as nanowhiskers,
nanofibers, and plasticizers are combined with PHB to enhance its
packaging properties (Yeo, Tan, Bakar, & Ismail, 2010). A study re­
ported the preparation of PHB-based packaging films by combining PHB
with starch and plastic. The prepared material showed enhanced pack­
aging properties with a good moisture barrier (Cazón, Velazquez,
Ramírez, & Vázquez, 2017). In another study, silver nanoparticles were
incorporated into PHB to elevate its antimicrobial activity that provides
O.M. Atta et al.
protection against foodborne pathogens. This combination also
improved the oxygen barrier properties of the composite film. The
PHB-AgNO3 material can be used as a template for designing actively
biodegradable food packaging materials with improved antimicrobial
activity (Castro-Mayorga, Fabra, & Lagaron, 2016). The PHB and cel­
lulose nano-whiskers films possess good hydrophobicity (Song, Xiao, &
Zhao, 2014).
Some researchers blended and plasticized PLA and PHB with a nat­
ural terpene D-limonene (LIM) to increase the PLA crystallinity and
manufacture versatile films suitable for food packaging. The addition of
PHB to the PLA matrix increased the oxygen barrier and water resistance
properties of the surface of the composite film. The PLA–PHB–LIM films
were structurally and thermally more stable than PLA film. In addition,
the composite films showed enhanced morphological, thermal, me­
chanical, biocompatible, and biodegradable properties (Arrieta, López,
Hernández, & Rayón, 2014).
3.1.4.2. Fruits and vegetables pomace. Fruits and vegetable pomace have
significant potential as functional ingredients in a wide variety of food
products. The diversity and abundance of natural pomace components
and their health benefits seek attention for their industrial applications.
These natural materials can replace artificial additives, minimize food
waste disposal, and lower the health risks associated with artificial fla­
vors (Majerska, Michalska, & Figiel, 2019). The majority of food waste is
made up of fruit and vegetable by-products, where the industrial pro­
cesses such as the production of oil, juice, wine, and sugar significantly
contribute to this total. These residues are typically discarded as left­
overs and composted or used as feed, but these contain a wealth of
bioactive compounds such as polyphenols, vitamins, and minerals. Each
year, millions of tons of residues with the potential for reuse are wasted.
Hence numerous studies were carried out to reuse these priceless re­
sources. In this regard, their potential to improve the properties of food
packaging materials was evaluated. Several studies investigated fruit
pomaces such as grape, tomato, apple pomace, and others. The studies
show that these byproducts can enhance the physical, mechanical,
antioxidant, and antimicrobial properties of the packaging materials
(Dilucia, Lacivita, Conte, & Del Nobile, 2020). Grape pomace contains
30% neutral polysaccharides, 20% acidic pectic substances, and 15%
lignin, proteins, and structural phenols, all of which are related to the
structure of carbohydrate-lignin and essential fatty acids found in grape
seeds (Chemat et al., 2019). Thus, grape pomace is an excellent source of
natural antioxidants and food supplements that can be used in a variety
of processes (Garrido et al., 2019). Also, many byproducts of the tomato
processing industry are largely untapped or underutilized. Thus, re­
searchers studied the preparation of composite films of sodium
caseinate, glycerol, and a lipidic fraction of tomato pomace at different
concentrations. The incorporation of a lipidic fraction of tomato pomace
improved the thermal stability of sodium caseinate films and reduced
the water absorption (Aloui, Baraket, Sendon, Silva, & Khwaldia, 2019).
Additionally, studies have identified the flour substitutes and other
additives for enhancing the cereal products and make them more
tolerable for a broader range of consumers, including those with Celiac
disease. In addition to being the natural source of bioactive materials,
the addition of fruit or vegetable pomace may also improve the taste
properties of the packaging materials (Ścibor et al., 2015). The incor­
poration of apple pomace into the blends of sorghum and maize flour
improved the bioactive potential of pomace (Lohani & Muthukumar­
appan, 2017). A study used whey protein concentrate and apple pomace
extract to create a novel edible coating that extended the shelf-life of
fresh-cut apples. The apple slices were coated with various concentra­
tions of apple pomace and whey protein and stored at 5 ◦ C for 12 days. A
total of 15 phenolic compounds were found in apple pomace extract.
Additionally, a significant amount of apple pomace exhibited antioxi­
dant and antimicrobial activity and showed a negligible effect on the
sensory evaluation of apple slices (Hammad, Elsayed, & Elkashef, 2021).
13
Food Hydrocolloids 125 (2022) 107419
3.1.4.3. Bio-plastics. Petroleum-based plastic materials like poly­
propylene (PP), polyester (PET), polyethylene (PE), and polystyrene
(PS) have been used in plastic packaging for a long time (Salwa, Sapuan,
Mastura, & Zuhri, 2019). Bio-based plastics began trading in the early
1990s. These are part of our economies, highly efficient, and reduce the
negative impact on the environment. The natural biopolymers and
polymers synthesized/polymerized from natural feedstock monomers
are examples of bio-based plastics. Examples of bio-based plastics
include bio-based polyethylene (Bio-PE), bio-based polypropylene
(Bio-PP), and bio-based poly(ethylene terephthalate) (Bio-PET). The
biopolymers already exist in nature and are defined as polymeric com­
pounds found in plants (starch, cellulose, and zein), animals (milk pro­
teins), and microorganisms (cellulose, xanthan, and other
polysaccharide gums). Despite the low output of bio-based plastics
produced each year, it is predicted to go up to 2.43 million tons by 2024.
However, the bio-plastics are not fully biodegradable, and their rate of
degradation is largely determined by their source (Jariyasakoolroj,
Leelaphiwat, & Harnkarnsujarit, 2020).
For a majority of their applications, bio-based plastics are used in
food packaging, service ware, bags, fibers, and agricultural applications.
It is a priority to replace the conventional packaging materials that
produce a high carbon footprint with lower carbon footprint materials
made from renewable resources. Currently, the bio-PE and bio-PET are
used to produce flexible film and tough materials, respectively, for
various food packaging applications (Van den Oever, Molenveld, van
der Zee, & Bos, 2017). The structure, appearance, and qualities of
Bio-PET packaging are not different from the standard petroleum-based
PET products. For example, a study reported no significant difference in
gas permeable properties of bio-PET and conventional PET products
(Jariyasakoolroj et al., 2020). Indeed, the discovery of ways to manu­
facture PET using polymerization mechanisms involving monomers
drawn from biomass has opened the door to produce bio-PET, a form of
PET that can be manufactured using sustainable resources. All of these
accomplishments speak to the excellent way this polyester has been
utilized in the packaging industry because of its strength as a food
contact material (Nisticò, 2020, p. 106707). Another study examined
the feasibility of fabricating hybrid composites using one of the most
recent generations of Bio-PET in combination with basalt (10%) and
carbon fibers (10%). The injection-molded samples were characterized
for their morphological, mechanical, and processing properties. These
lightweight bio-based hybrid composites exhibited high tensile strength
and a nearly fourfold increase in modulus of elasticity molded in a wide
temperature range. Due to the high mechanical strength of hybrid ma­
terials, these can be used in numerous industries, especially automotive
industry, and household appliances (Kuciel & Mazur, 2019).
3.2. Synthetic materials
A variety of synthetic materials are also used in the manufacturing of
films and coatings for food packaging applications. Among the different
synthetic polymers, PLA is receiving immense considering. In addition
to its natural synthesis from plant sources such as corn, sugar cane, and
rice (Mangaraj et al., 2019) and microorganisms (Ren, 2011), it is also
synthesized from hydrogen cyanide and acetaldehyde. PLA synthesis is a
relatively complicated multistage process that begins with the assembly
of lactic acid, followed by the formation of lactate. Finally, PLA is
formed through the polymerization of individual units. The industrial
PLA-based resins are generally prepared from L-lactide and L-lactic acid,
being a semi-crystalline material characterized by a comparatively
extreme temperature of glass melting and glass transition (Auras, Lim,
Selke, & Tsuji, 2011). In addition to being biodegradable and produced
from renewable resources, PLA provides many other benefits, mainly
stabilization of CO2 (Sauceau, Fages, Common, Nikitine, & Rodier,
2011). The physical and chemical properties of PLA could be tuned via
blending, branching, interlocking, or lactation (Kakroodi, Kazemi, Ding,
Ameli, & Park, 2015). PLA is generally expensive than polyolefin;
O.M. Atta et al.
nevertheless, it offers high mechanical strength, adjustable heat capa­
bility, dynamic compatibility, simple enrichment, and monomer
regeneration. Additionally, PLA production yields a 15–60% lower
carbon emission and utilizes 25–55% less energy than other oil-based
polymers (Calabria et al., 2012).
PLA has been extensively used in the preparation of packaging ap­
plications. A study reported the development of biodegradable pack­
aging material comprised of PLA, starch, and proteins (Aung et al.,
2018). In addition, its potential in the development of antimicrobial
packaging has been evaluated in several studies (Jamshidian, Tehrany,
& Desobry, 2013; Li et al., 2012). Several patents associated with
PLA-based antimicrobial packaging materials have been issued (Liu,
Coffin, Hicks, & Jin, 2012; Yuzay, Auras, & Selke, 2010). PLA may be a
highly versatile biodegradable polymer that may be processed using a
standard industrial tool. Many polymer grades are customized to adapt
to a wide range of products. The plausible properties of PLA make it a
suitable candidate for many applications where product use, reuse, and
recovery are required (Siracusa & Ingrao, 2016). PLA has been classified
as ‘GRAS’ and approved by FDA for use in food packaging, together with
Fig. 4. Schematic illustration of the preparation of antimicrobial edible coating via dipping method on the surface of food.
14
Food Hydrocolloids 125 (2022) 107419
direct-contact applications. In addition, PLA could be a suitable candi­
date for a variety of packaging applications due to its high similarity
with industrial thermoplastics like PET (Scarfato, Avallone, Galdi, Di
Maio, & Incarnato, 2017).
4. Additives for food packaging films
Additives are chemical products that are added to the polymer to
enhance its innate features. Additives from natural renewable resources
are appealing feedstock for the future generation of eco-friendly prod­
ucts. The biopolymers-based additives are used to enhance the film
properties and produce packaging functions like colorants, antimicro­
bials, antioxidants, nutraceuticals, and flavors (Mihindukulasuriya &
Lim, 2014). Over the years, the food sector has been developing new
conservation techniques for food packaging using natural additives
because of the increased consumer demand for fresh and natural food­
stuffs (Miao et al., 2015). The incorporation of antioxidants and anti­
microbials into edible films is one way to treat new foods (Atta et al.,
2021). Some studies have established the applicability of chitosan
O.M. Atta et al.
membranes to olive oil residue extract to improve the durability of
shelf-life of some fruits (Khalifa, Barakat, El-Mansy, & Soliman, 2016).
Food packaging systems with antimicrobial properties may be instru­
mental in prolonging the storage duration of food products (Atta et al.,
2021).
4.1. Bioactive materials
The edible antibacterial membranes (Fig. 4) provide an efficient
means to monitor foodborne infections and harmful microbes, thereby
improving food safety and minimizing the damage to products. Different
antimicrobial agents used in food packaging include amino acids, bac­
teria, enzymes, alcohol, and fatty acids. Spice such as sage, thyme, clove,
cinnamon, onions, garlic, and their extracts are also used for minimizing
the risk of food spoilage, for example, meat (Al-Tayyar, Youssef, &
Al-Hindi, 2020). The use of edible films as antibacterial vectors is an
exciting strategy for the external fusion on the dietary surfaces of
vegetable mixtures. Some oils also contain antimicrobial components
(Aleksic & Knezevic, 2014). Similarly, volatile antioxidants and anti­
microbials are also used in the development of edible films, which
further contribute to enhancing the physiological properties of the
packaging materials (Du, Avena-Bustillos, Hua, & McHugh, 2011).
4.2. Nanoparticles
4.2.1. Gold nanoparticles
Gold nanoparticles (AuNPs) range in size from 1 to 100 nm, which
are also called colloidal gold when distributed in a liquid. AuNPs are
antifungal; however, these possess a poor antibacterial activity lower
than other metal nanoparticles such as silver and titanium (Table 6).
Some organic complexes of Au (I) and Au (III) ions possess antibacterial
activity at very high concentrations (Zheng, Setyawati, Leong, & Xie,
2017). Few studies have evaluated the pathogenic growth, inflamma­
tion, and invasion effect on AuNPs. Surprisingly, although AuNPs show
low toxicity to microbes like Pseudomonas aeruginosa and Candida albi­
cans, the nanoparticles prevented the formation of pathogenic biofilms
and the invasion of endodontic stem cells. Another study showed
attachment of AuNPs with pathogenic cells, which likely contributed to
preventing the biofilm formation (Yu et al., 2016). AuNPs are being used
in nano-packaging industries because of their non-toxic, inert nature,
antimicrobial characteristics, and therapeutic properties. These play an
important role in the food industry to minimize the microbial load in
food items; hence they can be applied in food packaging (Paidari &
Ibrahim, 2021). The utilization of Au and other NPs as sensing materials
could pave the pathway to design intelligent nano-biosensors for use in
the food industry, such as for monitoring and detection of food
contamination (Farooq et al., 2020; Jasim, Ullah, Shi, Lin, & Yang,
2017).
Table 6
A comparison between some properties, antimicrobial action mechanisms, activity, and food applications of some important classes of nanoparticles.
NPs Toxicity Antimicrobial mechanism
Au Non-toxic Increase the oxidative cell stress through
generation of ROS and release of
intracellular lactate dehydrogenase to the
extracellular medium
Ag Safe at low Cause membrane damage that leads to
concentration leakage of cellular contents and ultimately
bacterial death
ZnO Safe Disrupt the cell membrane and reduce the
hydrophobicity of cell surface as well as
affect the transcription process of genes
TiO2 Non-toxic at low Cause oxidation of entire cell membrane,
concentration alter the coenzymes, and cause DNA
damage
Food Hydrocolloids 125 (2022) 107419
4.2.2. Silver nanoparticles
Silver nanoparticles (AgNPs) are synthesized by physical, chemical,
and biological methods. The biological synthesis of AgNPs involves the
use of microbial and plant extracts, which represent a ‘green’ and
economical process (Balashanmugam & Kalaichelvan, 2015; Peiris,
Gunasekara, Jayaweera, Arachchi, & Fernando, 2017; Ullah et al., 2020;
Ullah, Shi, et al., 2017). Silver possesses good antimicrobial activity,
both in the form of metallic and nano-silver zeolite, where the latter is
used for protection of foodstuffs, disinfection, and decontamination
(Fortunati, Peltzer, Armentano, Jiménez, & Kenny, 2013). AgNPs
possess antifungal and antibacterial activity; however, their bactericidal
activity is more strong against Gram-negative bacteria. These show their
antibacterial activity by attacking the thick bacterial cell wall and
altering the permeability of the cell membrane, thus interfering with
bacterial growth (Marambio-Jones & Hoek, 2010). The effect of AgNPs
in food packaging materials to prevent microbial growth at stored food
items has already been evaluated. A recent study reported the packaging
of Olivier salad in polymer packaging with different concentrations of
AgNPs. After 15 days of storage, the packaged food showed better sen­
sory characteristics and less microbial growth (Valipour Motlagh,
Aghazamani, & Gholami, 2021). Biosynthesized AgNPs films from raw
banana peel reduced E. coli growth in represented samples (Ittiachen &
Babu, 2021). AgNPs offer electrochemical and bioluminescent proper­
ties that may be used as nano-sensors and for biological labeling
(Bhardwaj, Srinivasan, & McGoron, 2013). In addition to AgNPs,
Ag-based nanoscale structures are also receiving tremendous attention
for packaging application due to their attractive physico-chemical
properties in addition to antimicrobial activity (Ranjan et al., 2014).
4.2.3. Zinc oxide nanoparticles
Zinc oxide nanoparticles (ZnONPs) have gained significant attention
due to their antimicrobial activity and good mechanical and barrier
properties compared to other commercially available NPs (Huang, Mei,
Chen, & Wang, 2018; Ul-Islam, Khattak, Ullah, Khan, & Park, 2014).
ZnONPs are more biocompatible showing minimal human toxicity with
high photocatalytic activity (Sirelkhatim et al., 2015). ZnO in food is
commonly used to preserve color and prevent food spoilage (Table 6).
ZnONPs can efficiently inhibit the growth of both
Gram-positive/negative bacteria. Up to 95% growth inhibition was
observed in several Gram-positive bacteria such as E. fecal, S. Pyogenes,
and S. aureus (Sirelkhatim et al., 2015). Moreover, ZnONPs have great
antimicrobial activity against specific foodborne pathogens such as
L. monocytogenes, E. coli O157:H7, C. jejuni, and Salmonella spp. (Seil &
Webster, 2012). Therefore, ZnO particles were recently incorporated
into many polymers to enhance the antibacterial activities of the pack­
aging materials. In a study, ZnONPs were added to PLA, which improved
the barrier and antibacterial properties of the composite film (Murariu
et al., 2015). Another study reported improved thermal and physical
Antimicrobial activity Uses References
Moderate antibacterial Medical and food packaging (Mishra et al., 2012; Zheng et al.,
activity 2017).
Strong antimicrobial Medical devices and some (Gurunathan, Han, Kwon, & Kim,
activity food coating 2014; Khalandi et al., 2017;
Logeswari, Silambarasan, & Abraham,
2013).
High antimicrobials Preserve color and prevent (Pati et al., 2014; Seil & Webster,
activity against specific food spoilage 2012; Sirelkhatim et al., 2015).
food pathogens
Anti-biofilm and high Ingredient in food, (Kubacka et al., 2014; Li et al., 2016;
antimicrobial activity pharmaceutical, cosmetics, Seil & Webster, 2012; Weir,
against many pathogens clothing, and ceramics Westerhoff, Fabricius, Hristovski, &
Von Goetz, 2012).
15
O.M. Atta et al.
properties along with good UV-light barrier characteristics of PLA/ZnO
films (Kim, Viswanathan, et al., 2019). Similarly, the ZnO/PHB nano­
composites demonstrated appreciable tensile strength and antimicrobial
activity (Díez-Pascual & Díez-Vicente, 2014). Jayakumar et al. devel­
oped ZnONPs-based pH sensing antimicrobial films. The developed films
also showed UV-light resistance and water barrier features (Jayakumar
et al., 2019). This platform can help to prepare pH sensing and
pathogen-resistant food packaging materials. The addition of ZnONPs in
olive flounder bone gelatin films increased the tensile strength, anti­
microbial activity, prolonged the freshness and preserved the useful
contents of spinach such as Vitamin C. Meanwhile, it reduced the water
vapor permeability and water solubility of the packaging films (Beak,
Kim, & Song, 2017).
4.2.4. Titanium nanoparticles
Titanium dioxide (TiO2NPs) are synthesized globally for a wide
range of applications. Among the studied NPs, TiO2NPs have high
thermal stability and are inert. These are effective against popular
foodborne pathogens such as L. monocytogenes, V. parahaemolyticus, and
S. choleraesuis. The antimicrobial activity of TiO2NPs is activated only
under UV light. In the absence of light, the antimicrobial action of TiO2
indicates the direct cell contacts and adsorption on TiO2NPs, which may
lead to loss of membrane integrity, regardless of photocatalysis (Khan,
Ul-Islam, Khattak, Ullah, & Park, 2015; Seil & Webster, 2012; Shoukat
et al., 2019; Ullah et al., 2016). The low-cost production, non-toxicity,
antimicrobial activity, and high photostability make TiO2NPs an
emerging material for environmental and energy fields such as water
splitting, water purification, and self-cleaning surfaces (Yadav, Kim, &
Pawar, 2016). The ultrasonically dispersed TiO2NPs in ethylene-vinyl
alcohol copolymer films showed significant antimicrobial activity
against different microorganisms, including bacteria and yeast, which
are commonly involved in food spoilage (Cerrada et al., 2008). In
another experiment, the incorporation of TiO2NPs into polypropylene
film inhibited the growth of E.coli in fresh-cut lettuce (Chawengkijwa­
nich & Hayata, 2008). Similarly, the electrospun zein-TiO2 nanofibers
efficiently absorbed ethylene and prolonged the shelf-life of cherry to­
matoes. The addition of TiO2NPs reduced the diameter of nanofibers and
modified their structural and thermal properties (Böhmer-Maas, Fon­
seca, Otero, da Rosa Zavareze, & Zambiazi, 2020).
5. Future perspective of biobased materials in food packaging
Despite the great potential of using biobased materials for food
packaging applications, there are several factors to be considered to
attract investors and meet the market demand. For instance, several
biobased materials are not yet being approved by the Food and Drug
Administration (FDA) for their commercial use. Similarly, the produc­
tion of such materials through modified approaches such as through
genetic engineering of producers raises the concerns of general public
acceptance. Besides, safety assessments as well as in vivo degradation
and safety of metabolites produced should be further investigated. Thus,
the widespread development and applications of biobased food pack­
aging materials warrant the process evaluations, safety assessments,
toxicity assessments, regulatory assessments, and consumer studies to
packed food items would pave the way for commercialization of bio­
based materials for food packaging applications and commercialization.
Furthermore, the high cost of some biobased materials requires process
optimization and finding alternative raw materials for their production.
For example, the low-cost production of BC has been extensively
investigated by exploring the potential of different agro-industrial
wastes as carbon sources.
Biobased materials have huge potential to replace conventional
petroleum-based materials for packaging applications. For instance,
some additives exhibit favorable properties to serve as packaging and
coating materials by providing protection against microbial contami­
nation and remain non-toxic. Such packaging materials could be
16
Food Hydrocolloids 125 (2022) 107419
designed and manufactured on a large scale for use in the food industry,
particularly for coating applications. Additionally, natural materials can
be used in conjunction with other additives such as plant oils or yeast for
their use not only in food packaging but for cosmetic and medical ap­
plications. Similarly, the development of functional materials, like bio­
sensors, by using different bionanomaterials could benefit the food
industry for the early detection of pathogens and contamination.
Another future aspect could be the preparation of composites of bio­
polymers with natural and synthetic additives in forms other than
membranes. The development of advanced synthesis approaches like 3D
bioprinting, regeneration, in situ/ex situ, and using the cell-free enzyme
systems could lead to the preparation of packaging materials of
enhanced features and improved functionalities.
6. Conclusions
The food packaging industry is a thriving market that plays an
important role in a modern economy. The increasing consumer demands
and the development of new technologies are greatly contributing to the
development of the food industry. Food packaging plays a vital role in
preserving food quality and ensuring its storage and transportation. In
comparison to the traditional petroleum-based packaging for food
storage which has negative impacts on the global environment, the
development of bioactive packaging materials has greatly revolution­
ized the food industry, not only by preventing pathogen attacks and
extending the storage time by providing protection against the harsh
environment but also enhance the nutritional value of food products.
These bioactive food packaging materials eliminate the risk of food
contamination and avoid the risk of toxicity to consumers. Different
natural and synthetic polymers and nanomaterials discussed in this re­
view have a great potential to replace conventional food packaging and
overcome the hunger issue of third-world countries by preserving food
quality for an extended time.
CRediT author statement
Omar Mohammad Atta: Conceptualization, Literature review,
Writing- Original draft preparation Graphics and Softwares. Sehrish
Manan: Conceptualization, Literature review, Writing- Original draft
preparation Graphics and Softwares. Ajmal Shahzad: Graphics and
Softwares. Mazhar Ul-Islam: Writing- Reviewing and Editing.
Muhammad Wajid Ullah: Conceptualization, Supervision, Writing-
Original draft preparation, Reviewing and Editing. Guang Yang:
Conceptualization, Supervision, Writing- Reviewing and Editing.
Declaration of competing interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Acknowledgment
This work was supported by the BRICS STI Framework Programme
3rd call 2019 (2018YFE0123700), National Natural Science Foundation
of China (21774039, 51973076), China Postdoctoral Science Founda­
tion (2016M602291), and the Fundamental Research Funds for Central
Universities, Open Research Fund of State Key Laboratory of Polymer
Physics and Chemistry, and Changchun Institute of Applied Chemistry,
Chinese Academy of Sciences.
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