Basic and Applied Concepts of Edible Packaging for Foods

CHAPTE R 1

Basic and Applied Concepts of Edible Packaging for Foods Jorge A. Aguirre-Joya*, Miguel A. De Leon-Zapata*, Olga B. Alvarez-Perez*, Cristian Torres-León*, Diana E. Nieto-Oropeza*, Janeth M. Ventura-Sobrevilla*, Miguel A. Aguilar**, Xochitl Ruelas-Chacón†, Romeo Rojas‡, María Elena Ramos-Aguiñaga*, Cristóbal N. Aguilar* *Autonomous University of Coahuila, Saltillo, Coahuila, Mexico; **Center for Research and Advanced Studies of the National Polytechnic Institute (CINVESTAV-IPN), Saltillo, Coahuila, Mexico; †Antonio Narro Agrarian Autonomous University (UAAAN), Saltillo, Coahuila, Mexico; ‡Autonomous University of Nuevo León, San Nicolás de los Garza, Nuevo León, Mexico

1 Introduction Food packaging has an important role in chain supplies and it is an important part of the final process. Edible films and coatings are one of the emerging strategies for food-quality optimization. Their usefulness is based on the capacity to maintain the quality, to extend the shelf life, and to contribute to the economic efficiency of packaging materials (Arismendi et al., 2013). In addition, consumers demand high-quality products containing only natural ingredients. Over the years, several techniques have been used to preserve, being edible coatings for composite of the method to greater results (Bosquez-Molina et al., 2003). New packaging materials have been developed and characterized by scientists from natural sources; but despite that, this information is available for the preparation of food covered, it is not universal for all products, which poses a challenge for the development of specific coatings and films for each food. A package has to satisfy various requirements effectively and economically; for this reason a modern food package should be optimized and integrated effectively with the food supply chain. Changes in the way that distribution chain function, such as the production, distribution, stored and retailed products, reflect the continuing increase for these materials, and also it is intended that the packaging is fulfilling its function and can offer safety foods (Ahvenainen, 2003). There are various patents and scientific papers regarding the manufacture of edible packaging. Certainly, edible packaging can be used to encapsulate some antioxidant (Cheng et al., 2015; Realini and Marcos, 2014) and antimicrobial agents (Arismendi et al., 2013), Food Packaging and Preservation http://dx.doi.org/10.1016/B978-0-12-811516-9.00001-4

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2  Chapter 1 aroma compounds or nutritional substances (Vanderroost et al., 2014; Zambrano-Zaragoza et al., 2014). The characteristics required for edible films and coatings depend for the most part on the application of the food product, which might be coated. Consequently, low oxygen permeability is needed for oxidation sensitive products. The properties of mass transfer selectivity allow fruit and vegetable respiration to limit dehydration during storage of avoiding solute penetration. Fruits and vegetables are greatly perishable during the postharvest management; there are considerable losses due to microbes, insects, respiration, and transpiration (Barbosa-Pereira et al., 2014; Janjarasskul et al., 2014). There are also external factors that include O2 and CO2 content, stress factor, ethylene ratios, and temperature, among others; and internal factors, such as the species, cultivar and its growth stage, that greatly affects the product quality and the risk to the consumers because of the presence of pathogenic microorganism (BosquezMolina et al., 2003). The fresh products quality factors are important to ensure marketability. The postharvest losses of fresh products are important issues due to their rapid decay during handling, transportation, and storage. Mainly, the purpose of edible coatings is to increase the natural barrier of fruits and vegetables. Likewise, a very important fact of edible coatings is that these may be safely eaten as a part of the products and are environment-friendly at the same time as they extend shelf life of fresh products (Ali et al., 2010). The aim of this book is to provide basic, technical, and applied knowledge concerning the development, characterization, and uses of edible coatings in food science.

2  Natural Polymers Based Edible Films and Coatings 2.1 Introduction Current consumer demands and needs about more natural, high-quality, and safer foods around the world have changed the global market. Actually, they also ask for food packages that do not increase pollution, and are made by sustainable processes, all of these in a cheap way. For this reason companies and researchers have focused on developing sustainable, biodegradable, and edible materials that improve the productivity, food quality, freshen, and provide food safety (Mahalik and Nambiar, 2010). Biopolymers have been studied for researchers as an alternative to traditional (petroleum) food packaging regarding their film-formation properties to produce biodegradable and edible films and coatings for food packaging (Azeredo et al., 2009). Biopolymers formulate edible films and coatings are structuring ones, such as polysaccharides, proteins, and lipids (Espitia et al., 2014a). A definition for edible films and coatings is that they are a primary packaging made from edible materials. Also, it is possible to apply a thin layer of edible packaging directly in the

Basic and Applied Concepts of Edible Packaging for Foods  3 food by immersion, spraying, and drenching (coating) or by being previously formed into a film and after are used as a food wrap without changing the process method of the coating and the ingredients used (Galus and Kadzińska, 2015). So the difference between an edible film and coating is that coatings are applied in liquid forms while films are obtained as solid laminates and then applied to food stuff (Falguera et al., 2011). In actuality, most researchers have focused on composite or multicomponent films and coatings to improve the final characteristics of the packaging, by summarizing their individual components advantages and by minimizing their disadvantages (Galus et al., 2013; Kurek et al., 2014). For that reason most of the composite packaging are mixtures of a hydrophilic structural matrix and of a hydrophobic (lipid) compound, these mixtures have resulted in better moisture barrier properties than the pure hydrocolloid films. Galus and Kadzińska (2015) mentioned that composite materials can be obtained as bilayers or emulsions. The lipid dispersed in the biopolymer matrix forms an emulsion. In the case of the bilayer system it is necessary to create first a thin layer of protein or polysaccharide and over this the second layer of lipids. Despite providing good barriers against water vapor, bilayers are less popular in the food industry as they require two casting and two draying stages (Debeaufort and Voilley, 1995).

2.2  Polysaccharide-Based Edible Films Polysaccharides, such as pectin, alginate, carrageenan, gum xantan, and starch, have been used in recent years as biopolymer compounds to create edible films and coatings in order to reduce traditional plastic packages (Espitia et al., 2014b). One of the materials that have been recently used as a sustainable compound for edible film formation are lignocellulosic ones (Mellinas et al., 2016). Next we describe some of the most used polysaccharides in edible films and coatings formulation. Characteristics of polysaccharides are that they are not toxic and wily available compounds in nature, and have selective permeability to oxygen and carbon dioxide (Erginkaya et al., 2014). This characteristic permits polysaccharide-based edible films and coatings to prolong shelf life of fruits, but polysaccharide solely packages have the disadvantage of low water permeability. 2.2.1  Animal origin polysaccharides Chitin and chitosan. Chitin is after cellulose, the second most often occurring biopolymer in nature. It is found in the exoskeleton of crustaceous, in fungal cell walls, and other biological materials. By the deacetylation of chitin, chitosan is obtained [poly-β-(1→4)-N-acetyl-dglucose-amine], a major component of the shells of crustaceans. Chitosan is a high molecular weight cationic polysaccharide with reported antibacterial and antifungal activities, as well as great film-forming capacities (Campos et al., 2011; Ferreira et al., 2009). Due to its characteristics, such as biodegradability, nontoxicity, and biocompatibility, it has been used in

4  Chapter 1 the food, chemical, and biomedical industries (Erginkaya et al., 2014). Chitosan is insoluble in water but soluble in acidic solvents, such as diluted hydrochloride, formic, and acetic acids. Moreira et al. (2011) reported that the antibacterial activity of chitosan could be due to the polycationic nature of the molecule, which permits interaction and forms polyelectrolyte complexes with polymers that produce at the bacteria cell surface. Chitosan is used due to their capability not only as an antimicrobial agent but also to reduce water loss by creating a semipermeable barrier that controls gas exchange, maintaining vegetable products for extended periods (Alvarez et al., 2013). 2.2.2  Plant origin polysaccharides Cellulose and cellulose derivatives. Cellulose is the major component of the plant cell, so it is the most abundant organic compound on earth. It is formed by d-glucose units linked through β-1,4 glycoside bonds. Cellulose derivatives are mainly used to form natural, biodegradable, or edible films as they are tasteless, odorless, and biodegradable substances with a low application cost (Erginkaya et al., 2014). Most used cellulose derivatives are carboxymethylcellulose (E466, CMC), methylcellulose (E461, MC), and hydroxypropyl metylcellulose (E464, HPMC) (Çag˘rı et al., 2002). In particular, carboxymethylcellulose (CMC) has been reported to be a water-soluble polymer with thermal gelatinization and excellent film-forming properties (Almasi et al., 2010). Nevertheless cellulose derivative films present poor water vapor barriers due to the inherent hydrophilic nature of this compound. Starch. Starch is a polysaccharide composed of amylase (25%) and amylopectin (75%) (Bourtoom, 2008) widely available in nature and is produced to fabric biodegradable films as starch films are transparent or translucent, flavorless, colorless, and tasteless (Skurtys et al., 2011). The largest source of starch is corn (maize), but also it can be obtained from wheat, tapioca, potato, and rice. Starch is the major carbohydrate reserve, present in plant tubers, where it is found as granules. High amylose starch films exhibit oxygen impermeability, oil resistance, heat-sealeabity, and water solubility and other physical characteristics similar to plastic films, and can retard microbial growth by lowering water activity (edible films from polisaccha cap lib). Pectin. Pectins are a group of plant-derived polysaccharides found in fruits and vegetables, the majority extracted from citrus peel and apple pomace (Dhanapal et al., 2012). Pectin (E440) is an anionic polysaccharide with structural backbone of (1→4)-linked α-dgalacturonic acid unit and used in food as gelling, stabilizing, and thickening agent in products, such as yogurts, jams, milk, and ice-cream (Espitia et al., 2014a,b). Pectin is divided into two categories; depending on their degree of methylation these are low-methoxyl pectin

Basic and Applied Concepts of Edible Packaging for Foods  5 (LMPs) and high-methoxil pectins (HMPs), with a respectable degree of methoxylation lower and higher than 50%. This degree of methoxylaion has a decisive effect on the mechanism of gelation (Altenhofen et al., 2009). Arabic gum. Gum arabic is obtained from stems of various Acacia species and is the most industrial employed polysaccharide because it presents unique emulsification, film-forming, and encapsulation properties (Ali et al., 2013) and it is composed of galactose, arabinose, rhamnose, and glucoronic acid (Anderson et al., 1991). In actuality, it is used in food industries for flavoring, confectionary, and bakery, and also in pharmaceutical and cosmetics industries (Maqbool et al., 2011). It has been applied in tomatoes, bananas, and papayas to improve quality and shelf life (Ali et al., 2010; Maqbool et al., 2010, 2011). 2.2.3  Marine origin polysaccharides Alginate. Alginates are a natural polysaccharide extracted from the marine brown algae from the family Phaeophyceae; they are compounded by units of R-d-mannuronate (M) and a-lguluronate (G) at different ratios and distributions in the chain (1–4); in general the sequences of M and G in the chain depends on the source of alginate and the age of the plant (Erginkaya et al., 2014). Formation of gels by the addition of calcium ions involves the G blocks, so the higher concentration of G units the higher gel strength (Albert et al., 2010). Nevertheless, alginate-based coatings can present good quality and preserve food shelf life by increasing the water barrier, maintaining the flavor, and retarding fat oxidation; they may be used as carriers for imicrobals and antioxidants to achieve a high concentration of preservatives in foods (Song et al., 2011). Carragenan. Another marine origin polysaccharide is the carrageenan that are sulfated water soluble polymers extracted from various red seaweeds of the Rhodophyceae family. They are used in food, dairy, and pharmaceutical industries, such as gelling, emulsifying, and stabilizing ingredients (Seol et al., 2009). Three major types of carrageenans are: k, ι, and λ-carragenans, depending on the number and position of sulfate groups that respectable are 20, 33, and 41% (w/w) (Fabra et al., 2008). Karbowiak et al. (2006) reports that the mechanism of carrageenan film formation includes gelation during moderate temperature drying, leading at solid film formed by polysaccharide-double helices after solvent evaporation. 2.2.4  Microbial polysaccharides Gellan. Gellan is a class of polysaccaride produced by the bacterium Sphingomonas elodea (also known as Pseudomonas elodea) and presents unique colloidal and gelling properties and good ability to form coatings (Moreira et al., 2015). The use of gellan in the food industry is increasing where it is used as a texturizing and gellin agent (Rojas-Graü et al., 2008) and also as a carrier for food additives, such as antibrowning and antimicrobial agents, colorants, flavors, and nutraceuticals (Oms-Oliu et al., 2010; Robles-Sanchez et al., 2013). Gellan gum-based edible coatings have been effectively applied over fresh cut vegetables,

6  Chapter 1 such as apples, mangoes, melons, and pears to improve shelf life and quality (Dalanche et al., 2016; Oms-Oliu et al., 2008; Perez-Gago et al., 2005; Rojas-Graü et al., 2008). Xantan Gum. Xantan gum is an exopolysaccharide synthetized by the bacteria Xanthomonas campestris, is a generally recognized as safe (GRAS) compound (FDA, 2013) as food stabilizer, thickener, and emulsifier. The viscous solution that it forms in cold or hot water is stable at a high range of pH and temperature and also is stable to enzymatic degradation (Sharma and Rao, 2015). It has a structure of 1,4-linked β-d-glucose residues and a side chain of trisaccharide bound to an alternating d-glucose residues. The trisaccharide chain is formed by β-d-mannose-1-4-β-d-galacturonic acid—1-2-α-d-mannose (ZambranoZaragoza et al., 2014). Xantan gum-based edible coatings have been used recently to improve quality and shelf life, also as a carrier of bioactive compounds of minimally processed prickly pear (Mohamed et al., 2013) and fresh cut apples (Freitas et al., 2013), among other fruits. In the classification we described earlier, some of the most commonly used polysaccharides for film and coating production, are only packaging material and are also carriers, holders, and physical barriers against moist loss and spoilage. Nevertheless, there are not the unique polysaccharides used, because scientifics and industries are always in the development and search for cheaper, functional, sustainable, and available sources of ingredients. Table 1.1 summarizes other examples of natural polysaccharides used alone or combined to create edible films and coatings.

Table 1.1: Polysaccharide-based edible films and coatings. Polysaccharide

Food Application

Specific Functionality

References

Agar

Fish

López de Lacey et al. (2014)

Polycaprolactone/ alginate film

Broccoli

Pullulan

Baby carrot

Cactus (Opuntia ficus-indica) mucilage/ gelatin/beeswax Gum cordia

—

Fucoidan

—

Delay growth of microorganisms by green tea extract addition Inhibition of S. typhymoroum by addition of organic acids and essential oils Reduction of Botritis cinerea growth by addition of caraway essential oil To obtain viable edible films with alternative polysaccharides Shelf life improvements by apllication of the gum cordia film and cordia myxa extract Characterization of fucoidan edible film as alternative functional polysaccharide

Chilgoza (Pinus gerardina) nuts

Takala et al. (2013)

Perdones et al. (2012)

Lira-Vargas et al. (2014)

Haq et al. (2013)

Chang and McClements (2015)

Basic and Applied Concepts of Edible Packaging for Foods  7

2.3  Lipid-Based Edible Coatings Lipids are compounds that have the capability for miscible or nonpolar organic solvents, but few of them contain hydrophilic and hydrophobic part forming micelle (Fig. 1.1). The diversity of the group is made up by monoglycerides, diglycerides, triglycerides, cerebrosides, phosphatide, phospholipids, terpenes, fatty acids, and fatty alcohol (Akoh and Min, 2008; Belitz et al., 2009; Chow, 2008). They are in natural sources such as plants, animals, and insects. In recent years, the food industry has focused on lipids to apply them in edible films and coatings for preservation, however, benefits for adding on food are huge. Akoh and Min (2008) described how lipids in edible film and coatings provide many features, for example, they minimize moisture loss, provide gloss, reduce complexity, and cost of packaging. The presentation of lipids may affect some features in film or coating and food, the moisture barrier being the most affected. Animal and plant waxes have a higher efficiency barrier moisture than resins, monoglycerides, diglycerides, fatty alcohols, emulsifiers, and surface active agents (Huber and Embuscado, 2009). 2.3.1  Oils and fats Oils and fats are mixtures where the major compounds are triglycerides; they come from plants and animals, respectively. This mixture is chemically similar but differs physically, as oils are liquids and fats are solids (Igoe, 2011; Wool and Sun, 2005). Fig. 1.2 represents chemically the lipids compounds that are common on different oils, such as canola oil, olive oil, palm oil, corn oil, cottonseed oil, rice bran oil, soybean oil, sunflower oil, palm oil; only butter cocoa, coconut oil, and peanut oil are exempt of linolenic (Chow, 2008).

Figure 1.1: Behavior of Lipids (Micelle) on Aqueous Solution and Organic Solvent.

8  Chapter 1

Figure 1.2: Essentials Fatty Acids From Plants.

Rodrigues et al. (2016) made a film palm fruit oil with favored water vapor barrier, water resistance, elongation, and transparency (Table 1.1). They described how their films look in scanning electron microscopy liked discontinuous appearance with uniform droplets. These films can be tried on food, for example, Vargas et al. (2011) and Hassani et al. (2012). Vargas et al. put sunflower oil in edible coatings and on pork meat hamburgers for increasing the quality of food, because on meat it was important to modulate water vapor and oxygen to prevent an undesirable reaction; but Hassani et al. tried rice bran oil for extending the shelf life of kiwifruit. Fruits were preserved principally on firmness, taste, and color, however, chemistry values were down. 2.3.2  Essential oils Essential oils are extracts rich in hydrophobic and volatile compounds. They contain an important antimicrobial activity due to terpenes, terpenoids, and aromatic constituents of, which they are formed (Han, 2014). Listeria monocytogenes, S. enteric, Staphylococcus aureus and Escherichia coli O157:H7 are principal pathogens we can find on contaminated food. Randazzo et al. (2016), Moradi et al. (2016), and Du et al., 2009 tested various essential oils in films to evaluate antimicrobial effect and properties of matrix. Randazzo et al. (2016) used citrus essential oils of peels from orange, mandarin, and lemon. They checked the oils applied on chitosan or methylcellulose films were present antilisterial activity. Chitosan film

Basic and Applied Concepts of Edible Packaging for Foods  9 with essential oils presented better incorporation of oil. Then Moradi et al. (2016) suggested a film with zein, 3% Zataria multiflora Boiss essential oil and 1% monolaurin because this film presented synergism of compounds and consequently had effect on bacterial load. Finally, Du et al. (2009) used allspice, cinnamon, and clove bud essential oils. Films had antibacterial activity but water vapor and tensile properties had no effect over them. 2.3.3 Waxes Waxes have higher molecular weight because they are formed by esters of a long chain acid and long chain alcohol. The origin of waxes are animal and vegetal; they have a function of protective covering tissues. These are useful on edible films or coatings for efficiency reducing moisture permeability for high hydrophobicity (Akoh and Min, 2008; Huber and Embuscado, 2009; Sikorski and Kolakowska, 2011). Saucedo-Pompa et al. (2007) designed an edible coating with candelilla wax and Aloe vera gel, applied on fresh-cut fruits. They concluded that candelilla coatings were an alternative for the preservation of food, in this case apples, avocados, and bananas. They observed it was helpful in firmness, weight loss, and appearance and lightness values compared to fruits without coating. However, edible coatings or films with waxes suffer disadvantages, such as brittle or form a rigid matrix; this depends a lot on the other components and concentrations of wax. Kowalczyk (2016) created films with 5% (w/w) aqueous biopolymer solutions containing 3% (w/w) sorbitol, 0.5% (w/w) candelilla wax, and 0.35% (w/w) Tween 40 for carrier ascorbic acid. Candelilla wax interacted differently with aqueous biopolymers affecting solubility, with sodium carboxymethyl or soy protein isolate present in full solubility and oxidized potato starch or pork gelatin solubility were partial. Spotti et al. (2016) mixed brea gum, beeswax, and glycerol, but they concluded that beeswax did not help in this film because of decreased mechanical properties, water vapor permeability, and microstructure. Nevertheless, waxes are not bad materials for films; for example, Chiumarelli and Hubinger (2014) presented a film with amazing properties, having good barrier, good mechanical, thermal, physical, and structure, and it was composed for cassava starch, glycerol, carnauba wax, and stearic acid. They tested different concentrations of carnauba wax but finally they took a low concentration because with a higher concentration of wax, the matrix showed a rigid structure. 2.3.4 Resins Resins are substances that plant cells produce for response to injury or infection in trees and shrubs; and some insects can produce them, which is the case of Laccifer lacca that produces shellac resin. Major of resins are translucent with yellowish-brown tones and physically are solid or semisolid (Baldwin et al., 2012). Chauhan et al. (2015) and Chitravathi et al. (2014) improved edible coatings on a base of shellac; they applied it on tomatoes and green chillies, respectively. Both groups of researchers found those films showed glossiness, transparency, quick drying nature, and sound emulsion stability, but then when applied on food, the

10  Chapter 1 coatings were optimal barriers of gases and water vapor and prevented senescence. They could extend shelf life by 12 days of these foods. Even so, shellac resin has a problem of esterification, so because of that, pharmaceutical industries decline to use this resin. Soradech et al. (2013) tried to stabilize a film; it had shellac resin with gelatin, a diverse concentration to protect the actives sites of shellac. 2.3.5 Plastificizers Plasticizers are compounds with low molecular weight that increase flexibility and strength of a material. The addition of plasticizers on film or coating help increase permeability to water and gases due to capacity for reduction of intermolecular forces in a polymer. Glycerol and polysorbates are popular plasticizers (Han, 2014; Rahman, 2007). The addition of diverse plasticizers lipidic to film or coating have a positive affect , which is the case glycerol-sage seed gum film, where demonstrated plasticizers increase thickness, moisture content, moisture uptake (Mohammad et al., 2015), but mechanical properties (elongation and tensile strength) were influenced by concentration, hydrophobic tail of compound, and stirring of emulsion that was the case of films with glycerol-chia seed mucilage and glycerol-chitosan (Dick et al., 2015; Santacruz et al., 2015). About morphology, glycerol-crees seed gum edible films were homogeneous and smooth without cracks, as described by Jouki et al. (2013). 2.3.6 Emulsifiers Emulsifiers are macromolecular stabilizers of character ionic that can reduce surface tension between two immiscible phases at their interface, allowing them to become miscible. The principal function is preventing syneresis or phases separation, because they keep hydrophilic–lipophilic balance (Badui, 2006; Igoe, 2011; Rahman, 2007). Important emulsifiers are lecithins; they are a mixture or fractions of phospholipids, they originate in animal-like egg lecithin or vegetal-like soybean lecithins (Whitehurst, 2004). Soy lecithin has effects on edible films or coatings, for example, color, opacity, solubility, and in microstructure. Fadini et al. (2013) related opacity and color yellow of the coatings for soy lecithin but Andreuccetti et al. (2011) associated action of lecithin with solubility and microstructure. Andreuccetti et al. (2011) observed that lecithin films, on study of microscopy, had the highest concentration of lecithin in film presented; small globules on the surface indicate heterogeneity in protein network.

2.4  Protein-Based Edible Films The edible packages proposal is based on using biopolymers. The goal is to join the principal characteristics and qualities of each one and that way obtain the best result, which can be proteins, lipids, or polysaccharides (Quintero et al., 2010). Also, other objectives of the EF is

Basic and Applied Concepts of Edible Packaging for Foods  11 to gather enough qualities so it can nourish the foodstuff and also protect it from unhealthy microorganism by antimicrobial release (Lin and Zhao, 2007). The EF are defined as a thin layer placed over food (it needs to be preformed). Its goal is to limit the interchange of biogas, pigments, scents, and so on, between the food and its environment, and to work as a vehicle for nutrients, such as antioxidants, antimicrobials, flavors, and colorants, improving the mechanical integrity or characteristics of foodstuff (Krochta and De Mulder-Johnston, 1997). It is important to settle the difference among films and coatings; the coatings can be defined as a prolonged and thin matrix, which has structures surrounding the foodstuff normally by immersion on the coat solution (while edible films are a prefractured moldable matrix that adjusts to the food it will surround). A composed EF is made of lipids and combined hydrocolloids (hydrolytic polymers that contain hydroxyls –OH of vegetal, animal, or microbial origin. In the food industry, they are used as additives with the purpose of thickening and coagulating) (Ramos-García et al., 2010) to get a conglomerate (Krochta and De Mulder-Johnston, 1997). The EF production is contemplated with the task of leverage of every compound property and the synergy of every component implemented, because the mechanical and barrier properties depend on the compounds that form the polymer matrix (Altenhofen et al., 2009) (Fig. 1.3).

Figure 1.3: Schematic Representation of Edible Packaging and Its Functions.

12  Chapter 1 2.4.1 Proteins Proteins can be found in a natural way, as globular proteins or fibrous proteins; the fibrous ones are bonded to each other on parallel, and globulars are rolled over their selves (Badui, 2006). Caseinate, the lactic serum, collagen and seine are among the proteins that can be used for EF (Fig. 1.4). Caseinate is good for the production of emulsified films, because of its amphiphilic nature, (a product that contains in its molecule one or many hydrophilic groups and one or many lipophilic groups), its disordered structure, and the ability to form hydrogen bridges. Lactic serum is a good barrier for CO2 even though it is fragile. To solve this problem, various investigations proved that its mechanical properties improve after the addition of a plasticizer agent like glycerol. For the fabrication of films, the first step is to get a concentrated solution of proteins over which heat is applied to denaturalize the proteins. After this, it gets refrigerated to eliminate the enclosed gas and obtain the package material. In collagen, the EF obtained were used from long ago in meat products, such as cold cuts. The benefit of this kind of coating is to avoid the humidity loss and give a uniform aspect to the product, improving its structural properties (AINIA, in press). Zein is a prolamin and the principal protein from the corn. It is characterized for being a relative hydrophobic and also a thermoplastic material because it is strong, shiny, resistant to bacteria, water insoluble, antioxidant, and adhesive film.

Figure 1.4: Schematization of Proteins Incorporation Into Edible Films.

Basic and Applied Concepts of Edible Packaging for Foods  13

3  Edible Packaging: A Vehicle for Functional and Bioactive Compounds 3.1 Introduction Edible packagings increase the shelf life and improve quality of foods (De León-Zapata et al., 2015; Saucedo-Pompa et al., 2009). The most commonly used natural polymers for formulation of edible packagings include polysaccharides (starch, cellulose, and its derivatives, chitosan, alginate, gellan gum), proteins (collagen, zein, soybean, and gluten proteins, milk proteins), and fats (beeswax, candelilla wax, carnauba wax, fatty acids, and glycerols) (Bravin et al., 2006; Casariego et al., 2008; De León-Zapata et al., 2015; Pommet et al., 2003; SaucedoPompa et al., 2009). The edible packagings are carriers of antimicrobial substances, antioxidants, dyes, and vitamins, thus improving the sensory properties of food products (Krasniewska and Gniewosz, 2012). Components of edible packagings depend on the nature of the food product and the specific function in the food. One of the main functions of edible packagings is their use as carriers of antimicrobials agents to increase shelf life of foods (Saucedo-Pompa et al., 2009). This chapter discusses edible packagings as matrices for additives antimicrobials of natural origin as plant extracts, oils, enzymes, bacteriocins, and polysaccharides for application in foods.

3.2  Active and Intelligent Packaging Food packaging technology is continually increasing in the last few years in response to growing challenges from a modern society (Realini and Marcos, 2014). This material goes from simple preservation to the analysis of the addition of safety food additives and contributes to reducing environmental pollution. Active and intelligent packaging systems are a modern innovation that goes beyond the traditional functions in which exists an interaction among the product and its environment to extend the shelf life of food, improving sensory properties maintaining the quality of the packed food (Han, 2013). Active and intelligent packaging should not to be confused; active packaging causes a modification of the conditions of the packed food to extend shelf life, maintaining the quality of final product while an intelligent packaging system monitors the condition of packaged foods to give information about the quality products during transport and storage (Ahvenainen, 2003). Both systems can function synergistically to realize what is called smart packaging, providing a total packaging solution using each of their advantages. Besides this, active, intelligent, and smart packaging concepts are often used interchangeably in literature. Some types of smart packaging allow the controlled release of bioactive substances (antimicrobials or antioxidants) or can be added with encapsulated compounds (Lee, 2010) (Tables 1.2 and 1.3).

3.3  Incorporation of the Active Substances Into the Packaging Film 3.3.1  Use of natural antimicrobials Food safety is a global priority and one of the major objectives of the current food legislation due to microbiological risks of food products and are one of the main sources

14  Chapter 1 Table 1.2: Examples of lipid-based edible films and coatings. Carbohydrates or Protein Compounds

Lipids Compounds Beeswax/tween 80/glycerol Candelilla wax/tween 40

Brea gum Oxidized potato starch, soy protein isolate, sodium carboxymethyl cellulose, or pork gelatin Palm fruit oil/tween 80 or Span 80 Mesquite seed gum Citrus essential oils Chitosan or methylcellulose Glycerol/Z. multiflora Boiss essential Corn zein oil/glycerol monolaurate Glycerol Chia seed mucilage Glycerol/tween 20 or tween 80 Chitosan Glycerol Sage seed gum Shellac/oleic acid Aloe gel Oregano essential oil/glycerol Citrus peel pectin Shellac Starch Carnauba wax/glycerol/stearic acid Cassava starch Cocoa butter/soy lecithin Pectin/hydrolyzed collagen Glycerol Cress seed gum Shellac Gelatin Rice bran oil/glycerin Whey protein Sunflower oil Chitosan Soy lecithin Gelatin/protein Cinnamon oil/allspice oil/clove Apple puree bud oil/glycerol Candelilla wax A. vera gel

References Spotti et al. (2016) Kowalczyk (2016)

Rodrigues et al. (2016) Randazzo et al. (2016) Moradi et al. (2016) Dick et al. (2015) Santacruz et al. (2015) Mohammad et al. (2015) Chauhan et al. (2015) Alvarez et al. (2014) Chitravathi et al. (2014) Chiumarelli and Hubinger (2014) Fadini et al. (2013) Jouki et al. (2013) Soradech et al. (2013) Hassani et al. (2012) Vargas et al. (2011) Andreuccetti et al. (2011) Du et al. (2009) Saucedo-Pompa et al. (2007)

Table 1.3: Protein-based edible films and coatings. Protein

Additives

Applications

Functions

Wheat gluten (7.5%) Soy (5%)

No

Cheese and tomato

No

Gelatin (4%)

Corn oil (2.5%) and olive oil (5%)

Apple, potatoes and carrots Sausage

Permeability to O2 avoiding oxidation Permeability to water and other gasses Antioxidant mechanical properties and permeability to water and other gasses Permeability to O2 avoiding oxidation

Calcium No caseinate (5%)

Potato and apple

Storage Life Expectation 14 days at 10°C

References

Origin

5 days at 25°C

Tanada Palmu Vegetal and Grosso (2003) Shon and Choi Vegetal (2011)

35 days at 25°C

Castro et al. (2010)

Animal

130 min at 20°C

Thian et al. (2012)

Animal

Basic and Applied Concepts of Edible Packaging for Foods  15 of food-borne illnesses. Traditionally, antimicrobial agents are directly mixed into the initial food formulations, but excessive amounts may change the taste of the food caused by direct addition of antimicrobial components (Nguyen Van Long et al., 2016; Uz and Altinkaya, 2011), which may result in an inactivation due to food components or dilution below active concentration or evaporation of these compounds (Quintavalla and Vicini, 2002). The main reason for incorporating this compond into the packaging is to prevent surface growth in foods where a large portion of spoilage and contamination occurs; this may reduce the addition of great quantities of antimicrobials (Nguyen Van Long et al., 2016). A possible solution to controlling the growth of phytopathogens in fruits during postharvest shelf life (Junqueira-gonçalves et al., 2013), and to extend the safety and shelf life of ready-to-eat foods (Moditsi et al., 2014), it is the use of antimicrobials compounds. Antimicrobial packaging can be effective during the storage period, handling or transport, and once the package is opened, the antimicrobial film will still be active (Baños-Guevara et al., 2004). The antimicrobials embedded in films can also be transferred to the food surface for further action, and relatively low amounts are required to achieve a target shelf life (Nguyen Van Long et al., 2016). The relative humidity environment and the moisture content of the product can influence the antimicrobial property of edible packagings. This can induce condensation of moisture on the food surface, increasing the possibility for microbial growth (Torres et al., 1985). Edible packagings, when incorporated with antimicrobial compounds, have the potential to be used as antimicrobial active packaging to control foodborne pathogens and spoilage microorganisms, thus enhancing food safety (Pérez Espitia et al., 2014). The selective action of such films consists in the release during food storage of an appropriate active substance that affects microorganisms (Lopez–Rubio et al., 2006). Tables 1.4–1.7 show recent studies exploring the application and efficiency of natural antimicrobial compound incorporation into edible films for the prevention of food spoilage. 3.3.2  Antioxidant packaging Increasing interest and research has been focused on biodegradable packaging materials as antioxidant packaging systems that allow the incorporation of natural antioxidants into a biodegradable matrix. Oxidative processes are one of the primary mechanisms of quality deterioration of foods. The incorporation of antioxidants in food formulations may affect food quality parameters, such as color, odor, or taste, and consumer preference (Barbosa-Pereira et al., 2014). Active packaging represents an innovative strategy to incorporate antioxidants in a polymer matrix to prevent oxidative processes and extend the shelf life of food products (Realini and Marcos, 2014). Traditionally, synthetic antioxidants, such as polyphenol, and thioester compounds have been used, although the potential toxicity derived from their migration into food products is making their application questionable, and for that reason plant extracts, and essential oils from herbs, such as Rosemary (Bolumar et al., 2016), oregano (Camo et al., 2011), and

16  Chapter 1 Table 1.4: Investigated applications of edible films with natural antimicrobials in foods. Matrix SPC + glycerol

Natural Antimicrobial Clove essential oil

CFP + glycerol + tween 20 Clove bud oil

Glycerol

DMM+ myrosinase

Protein + SCSG + chitosan Oregano, cinnamon, and anise essential oils PSM + red algae Lemongrass, rosemary, and clove bud essential oils Coconut Green tea oil + glycerol + starch Maize zein + carnauba Catechin, wax+ soybean l-αgallic acid and lecithin + glycerol lysozyme MC + HPMC + PG400 Nisin

Food

Target Microorganism

References

Minced sardine muscle

Total mesophiles, H2S producer microorganism, luminiscent colonies, Pseudomonas spp., lactic bacteria, and Enterobacteriaceae L. monocytogenes and S. enteritidis

Salgado et al. (2013)

Sliced cheddar cheese Slices of cold smoked salmon Carp

Lee et al. (2015a)

L. monocytogenes, KCTC 3569 Lee et al. (2012)

Total aerobic

Wu et al. (2014)

Pork sausage

L. monocytogenes (ATTC 19111)

Song et al. (2015)

Tomatoes

Bacterias and yeast

Das et al. (2013)

Fresh Kashar cheese Cold smoked salmon

L. monocytogenes ATCC 7644

Unalan et al. (2013)

Five L. monocytogenes strains, PSU1 (serotype 1/2a), PSU21 (serotype 4b), PSU9 (serotype 1/2b), F5069 (serotype 4b), and Scott A (serotype 4b)

Neetoo and Mahomoodally (2014)

CFP, Chicken feed protein; HPMC, hydroxypropylmethylcellulose; M, methylcellulose; PG400, polyethylene glycol 400; PSM, perilla seed meals; SCSG, silver carp skin gelatin; SPC, sunflower protein concentrate; WPI, whey protein isolate .

tea (López De Dicastillo et al., 2011), are of great interest as natural antioxidants. In most cases they can offer health benefits, and their use is becoming highly relevant. Due to the nature of the compounds and in order to achieve an adequate distribution in the matrix, it is very important to consider all the chemical characteristics of antioxidants compounds to be incorporated to achieve a highly compatibility (Decker, 1998). One of the important features to consider when we add antioxidants in the formulation is the solubility, which can determine its effectiveness into the matrix, so it is essential to know that these compounds should be selected depending on the type of food. In that way, polar antioxidants are more

Table 1.5: Investigated effects of natural compounds on the antimicrobials properties of edible films. Film

Natural Compound

Microorganisms Tested

SPC + glycerol

Clove essential oil

HMP + papaya puree + tween 80

Cinnamaldehyde

HMWFG + sorbitol + glycerol

Sodium lignosulfonate from eucalyptus wood (molecular weight of 7085 Da and low sugar content (4% reducing sugars) Coliphage T4 Marjoram oil, coriander oil and clove bud oil Mustard essential oil Oregano, cinnamon, and lemongrass essential oils

Salgado et al. (2013) Lactobacillus acidophilus CETC 903, Salmonella cholerasuis CECT 4300, L. innocua, CECT 910, Citrobacter freundii CECT 401, E. coli CECT 515, Shigella sonnei CECT 4887, P. aeruginosa CECT 110, Yersinia enterocolitica CECT 4315, Brochothrix thermosphacta CECT 847, S. aureus CECT 240, Bacillus cereus CECT 148, L. monocytogenes CECT 4032, Clostridium perfringens CECT 486, Aeromonas hydrophila CECT 839T, Photobacterium phosphoreum CECT 4192, Shewanella putrefaciens CECT 5346T, P. fluorescens CECT 4898, Vibrio parahaemolyticus CECT 511T, B. coagulans CECT 56, Bifidobacterium animalis subespecies lactis DSMZ 10140, B. bifidum DSMZ 20215, Enterococcus faecium DSM 20477, L. helveticus, DSM 20075, Debaryomyces hansenii CECT 11364, Aspergillus niger CECT 2088, Penicillium expansum DSMZ 62841 Otoni et al. (2014a) E. coli (ATCC 11229), S. aureus (ATCC 6538), L. monocytogenes (ATCC 15313), and S. enterica serovar Choleraesuis (ATCC 10708) Nuñez-Flores et al. D. hansenii CECT 11364 (2013)

WPI + glycerol CFP + glycerol + tween 20

NaCS + beta-cyclodextrin + glycerol + tween 80 Amaranth flour + chitosan + starch + glycerol + tween 20

E. coli BL21 E. coli O157:H7 (NCTC 12079), S. aureus (KCTC 1621), L. monocytogenes (ATCC 19111), and S. enteritidis (KCTC 2930) E. coli, S. aureus, B. subtilis, and A. niger A. niger and P. digitatum

References

Vonasek et al. (2014) Lee et al. (2015a)

Chen and Liu (2016) Ávila-Sosa et al. (2012) (Continued)

Table 1.5: Investigated effects of natural compounds on the antimicrobials properties of edible films. (cont.) Film Porcine MBM protein + fructose + tween 20

Alginate

Microorganisms Tested E. coli O157:H7 (NCTC 12079) and L. monocytogenes (ATCC 19111) S. aureus ATCC 25923, B. cereus PTCC 1154, E. coli ATCC 25922, P. aeruginosa ATCC 27853, and S. typhimurium ATCC 14028 DMM L. monocytogenes KCTC 3569 Carvacrol S. aureus ATCC 25922 and E. coli ATCC 25923 Lysozyme Micrococcus sp. Z. multiflora Boiss S. aureus ATCC 25923, B. cereus PTCC 1154, E. coli and Mentha pulegium ATCC 25922, P. aeruginosa ATCC 27853, and S. essential oils typhimurium ATCC 14028 Thyme essential oil S. marcenscens, A. hydrophila, A. faecalis, A. denitrificans, L. innocua Oregano essential oil E. coli, S. enteritidis, S. aureus, L. monocytogenes

Pectic extract

Lime essential oil

CMC + glycerol + tween 80

Glycerol Sodium caseinate + glycerol LMAP + glycerol SSPS + glycerol + tween 80

Chitosan

Carrageenan Mucilage

Metylcellulose Sodium caseinate Hake protein

Natural Compound Coriander oil and tannic acid Z. multiflora essential oil

E. coli O157:H7, S. typhimurium, S. aureus, B. cereus, and L. monocytogenes Satureja hortensis S. aureus, B. cereus, E. coli, P. aeruginosa, S. essential oil typhimurium Oregano essential oil L. monocytogenes, S. typhimurium, B. cereus, Y. enterocolitica, P. aeruginosa, S. aureus, E. coli, E. coli O157:H7, S. putrefaciens, and V. cholera Oregano and thyme P. fluorescens, A. hydrophila/caviae, L. innocua essential oils Matricaria recutita L. monocytogenes, S. aureus, and E. coli O157:H7 essential oil Citronella, coriander, B. thermosphacta, E. coli, L. innocua, L. monocytogenes, tarragon and thyme P. putida, S. typhimurium, S. putrefaciens essential oils

References Lee et al. (2015b) Dashipour et al. (2015) Lee et al. (2012) Arrieta et al. (2014) Bayarri et al. (2014) Salarbashi et al. (2014) Ruiz-Navajas et al. (2013) Benavides et al. (2012) Sanchez-Aldana et al. (2015) Shojaee-Aliabadi et al. (2013) Jouki et al. (2014)

Iturriaga et al. (2012) Aliheidari et al. (2013) Pires et al. (2013)

Gelatin

Bergamot and lemongrass essential oils Sodium caseinate + glycerol Hen egg white lysozyme BHGTB + glycerol Genipin and lysozyme Açaí pectin + glycerol, ascorbic acid + citric acid Apple skin polyphenol poder and thyme essential oil PPRA + sucrose Grapefruit seed extract and cinnamaldehyde Tapioca starch + HPMC + glycerol Nisin Brewers spent grain protein + glycerol

Chitosan

CSMP + fructose + sorbitol Maize zein + glycerol + oleic, linoleic, and lauric acids Methylcellulose + tween 80 and tween 20

Carvacrol Lysozyme and catechin Clove bud (Syzygium aromaticum) and Oregano (O. vulgare) essential oils

E. coli, S. typhimurium, P. aeruginosa, L. monocytogenes, S. aureus

Ahmad et al. (2012)

M. luteus CIP A270

Colak et al. (2015)

B. subtilis (ATCC 6633)

Ma et al. (2013)

L. monocytogenes

Pérez Espitia et al. (2014)

E. coli, O157:H7 and L. monocytogenes

Jo et al. (2014)

L. innocua (CIP 8011, CCMA 29), and Z. bailii (NRRL 7256) L. monocytogenes (ATCC 19111), S. aureus (KCTC 1621), S. Typhimurium (KCTC 2514), and E. coli O157:H7 (NCTC 12079) E. coli O157:H7 L. innocua (NRRL B-33314)

Basch et al. (2013)

A. niger (ATCC 16404) and P. sp. (ATCC 2147)

Lee et al. (2015c)

Jo et al. (2012) Arcan and Yemenicioglu (2014) Otoni et al. (2014b)

BHGTB, Bovine hide gelatin type B; CFP, chicken feed protein; CMC, carboxymethyl cellulose; CSMP, cotton seed meal protein; DMM, defatted mustard meal; FSG, fish skin gelatin; HMP, high methylester pectin; HPMC, hydroxypropylmethylcellulose; HMWFG, high molecular weight fish gelatin; LMAP, low methoxyl amidated pectin; NaCS, sodium cellulose sulfate; PPRA, persimmon peel/red algae; SSPS, soluble soybean polysaccharide; WPI: whey protein isolate.

20  Chapter 1 Table 1.6: Investigated applications of edible coatings with natural antimicrobials in foods. Matrix Chitosan Alginate WPI + glycerol+

Pectin + calcium chloride + tween 20 + glycerol QSM + glycerol

Tween 80 + acetic, lactic and levulinic acids + Hemicellulose A and B Articoat-DLP is a commercially available antimicrobial edible coating Tapioca starch + glycerol Sodium alginate + glicerol

Natural Antimicrobial

Food

Microorganisms Tested

References

Lemon essential oil Lemongrass essential oil Cinnamom, cumin, and thyme essential oils Chitosan and transcinnamaldehydeCD Oregano and thyme essential oils

Strawberry

B. cinerea

Apple Freshly cut beef

E. coli, psychrophilic bacteria, and yeast Total viable count (TVC)

Perdones et al. (2012) Salvia e Trujillo et al. (2015) Badr et al. (2014)

Fresh-cut papaya (Carica papaya L. cv “Maradol”)

Total aerobic plates, Brasil et al. psychrotrophics, yeast, and (2012) molds counts

Fish (Oncorhynchus mykiss)

Chitosan

Turkey deli meat

Total viable bacterial count, psychrophilic bacterial count, Enterobacteriaceae, Pseudomonas spp., H2Sproducing bacteria (including S. putrefaciens), and LAB Three L. innocua strains (ATCC 33090, 33091, 51742)

Jouki et al. (2014)

Guo et al. (2015)

Lactic acid, Fresh skinless TVC, Pseudomonas, B. acetic acid, and chicken breast fillets thermosphacta, lactic acid sodium diacetate bacteria (LAB), coliforms, and E. coli

RodríguezCalleja et al. (2012)

Nisin and natamycin Carvacrol and methyl cinnamate

Ollé-Resa et al. (2014) Peretto et al. (2014)

Port Salut Cheese Strawberry

S. cerevisiae (CBS 1171), L. innocua (CIP 80.11) E. coli O157:H7 and B. cinerea

CFP, Chicken feed protein; HA, hemicellulose A; HB, hemicellulose B; QSM, quince seed mucilage; SPC, sunflower protein concentrate; WPI, whey protein isolate.

suitable for foods with a high lipid content (Gómez-Estaca et al., 2014). Decker (1998) mention that it is called “antioxidant paradox.” This is a phenomenon where hydrophilic free radical scavengers (FRS) are more effective antioxidants than hydrophobic ones in oils, while hydrophobic FRS are more effective in emulsified oils. This effect was observed at the oil–air interface of bulk oils due to the ability of polar FRS with a prevalent oxidation (Decker, 1998). Also, other authors mention that the main mechanism of action

Basic and Applied Concepts of Edible Packaging for Foods  21 Table 1.7: Investigated effects of natural compounds on the antimicrobial properties of edible coatings. Matrix

Natural compound

Microorganisms Tested

NaCS + betacyclodextrin + glycerol + tween 80 Whey protein

Mustard essential oil E. coli, S. aureus, B. subtilis, and A. niger Chitosan and E. coli and S. aureus lysozyme obtained from the protein of chicken egg whites PLA and nisin Mesophilic and B. edulis wild edible psychrophilic bacteria mushrooms + LDP + tributyl citrate

References Chen and Liu (2016) Lian et al. (2012)

Han et al. (2015)

LDP, Low-density polyethylene; NaCS, sodium cellulose sulfate; PLA, poly(l-lactic acid).

is the reduction of the oxygen transmission rate, as well as the possibility of incorporating antioxidant compounds in the edible film or coating matrix. In the last decade there have been many inquiries about active films using various polymer matrices, as well as different sources of antioxidant compounds.

3.4 Conclusions Currently the new trend in food packaging, such as films and coatings, is the addition of natural bioactive compounds with antimicrobial properties against microorganisms of food interest, due to the indiscriminate use of synthetic chemicals in food, so that the consumer has tried to avoid such substances. It is important to consider the type of natural bioactive compound to be used in an edible packaging, depending on whether you want to apply as a solid matrix (film) or as a liquid matrix (coating) in the food.

4  Food Surface Properties for Edible Packaging Application 4.1 Introduction Packaging is widely used for preserving, distributing and marketing foods, and is often used in combination with other preservation methods (Hoover, 1997). However, the disposal of packaging materials leads to ecological problems and additional recycling costs (Tzoumaki et al., 2009; Viña et al., 2007). A natural alternative to extend shelf life of these products during storage is the use of edible coatings, which is defined as a cover material that is applied to edible food to improve appearance, being an effective barrier to transmission of gases, solving problems of migration of moisture, oxygen, carbon dioxide, and aromas (Cuq et al., 1995; Fernández-Álvarez, 2000; Krochta and De Mulder-Johnston, 1997), reducing maturation process, prolonging life, and quality of food (Vernon et al., 1999). The study of surface properties of edible packagings, mainly coatings based on the type of food surface, has led to the prediction of the efficacy of the coating in the same (Souza et al., 2010). The

22  Chapter 1 effectiveness of edible coatings for protection of food depends primarily on controlling the wettability of the coating solutions, which affects the coating thickness (Park, 1999; Souza et al., 2010) and must be wet and spread uniformly on the foods surface and, upon drying, a coating that has adequate adhesion, cohesion, and durability to function properly must be formed (Krochta and De Mulder-Johnston, 1997). This chapter reviews the parameters of wettability, surface tension in edible packagings for determining food surface properties by determining the contact angle of coating in the surface of food.

4.2  Wettability of Coatings in the Surface of Foods 4.2.1 Wettability The wettability, or spreading coefficient (Ws), is the ability to have a given liquid spread on a solid surface (Ribeiro et al., 2007) where higher values of Ws (closer to zero) are considered the most suitable to coat the surface (Carneiro-da-Cunha et al., 2009). To determine the wettability of a solution on a solid surface the coefficient of adhesion (Wa) is taken into account, which represents the force that promotes the expansion of the liquid on a solid surface and the cohesion coefficient (Wc), which represents the force that promotes the contraction of the liquid on a solid surface. The wetting behavior of the solutions will mainly depend on the balance between these forces (Lima et al., 2010). 4.2.2  Importance of application of edible coatings in foods 4.2.2.1 Cheese Edible coatings can improve shelf life and cheese quality by providing good and selective barriers to moisture transfer, oxygen uptake, lipid oxidation, losses of volatile aromas and flavors, better visual aspect, and reduction of microbiological contamination (NísperosCarriedo, 1994). Cheese is a complex food product consisting mainly of casein, fat, and water (Cerqueira et al., 2009a). Fresh cheeses are packaged in a modified atmosphere with N2 and/ or CO2 replacing the O2 in the package (Mannheim and Soffer, 1996). However, spoilage caused by yeast and especially bacteria may still occur even at very low O2 and elevated CO2 levels (Westall and Filtenborg, 1998). Semisoft and hard cheeses have a relatively high respiration rate, which require a packaging material somewhat permeable to CO2 to avoid an expansion of the packaging (Cerqueira et al., 2009a). Meanwhile, O2 must be kept out to avoid fungal spoilage and oxidation of the cheese (Cerqueira et al., 2009a). Instead, these products require a balanced oxygen and carbon dioxide atmosphere to prolong their shelf life (Haasum and Nielsen, 1998). In semihard cheeses, the factor that most affects cheese stability is water activity (aw), which depends mainly on moisture and salt contents (Cerqueira et al., 2009a). During ripening, aw is not constant but decreases until the cheese surface is in equilibrium with the surrounding atmosphere, thus influencing the microbiological and chemical evolution of the cheese

Basic and Applied Concepts of Edible Packaging for Foods  23 (Saurel et al., 2004). All of these factors affect not only the cheese’s physical characteristics but also its flavor during storage (Cerqueira et al., 2009a). 4.2.2.2  Fruit and vegetables

Coatings on fruits and vegetables that exceed a critical thickness can cause detrimental effects of reduced internal O2 concentration and increasing CO2 concentration from anaerobic fermentation (Choi et al., 2002). That is why edible-coating formulations must be wet and spread on the fruit’s surface uniformly and upon drying form a coating that has adequate adhesion, cohesion, and durability to function properly (Krochta and De MulderJohnston, 1997) without exceeding the critical thickness of formed film on the surface of the fruit. 4.2.2.3 Fish

Fresh fish is a rich source of nutrients, however, this is a very perishable food product (Souza et al., 2010). Postharvest damage is mainly due to biochemical and microbiological changes (Duran et al., 2008). Therefore, to prevent lipid oxidation and microbial growth it is very important to maintain freshness and increase shelf life in fish (Remya et al., 2017). Inadequate postcapture handling induces both microbial and endogenous enzyme activities and muscle autolysis, leading to protein degradation and loss of functionality. In particular, seafood products contain high levels of polyunsaturated fatty acids that are easily attacked by oxygen-derived free radicals, resulting in lipid peroxidation and meat rancidity (Huang and Weng, 1998). Furthermore, lipid oxidation causes fish rancidity, rendering the product unacceptable for human consumption (Souza et al., 2010). The increasing demand for fresh refrigerated seafood with an extended shelf life has intensified the search for technologies that support fresh fish utilization (Abbas et al., 2008). One of the main developments is the utilization of edible coatings for improved shelf life and fish quality by providing good and selective barriers to moisture transfer, avoiding lipid oxidation (Huang and Weng, 1998), better visual aspect, and reduction of microbiological contamination (Duran et al., 2008). Several authors have reported the improvement of Ws and contact angle of coatings in foods with the addition of plasticizers and surfactants (Table 1.8). 4.2.3  Variables that affect the wettability of coatings at nanoscale level At nanoscale level, the conjugation of variables, such as the degree of aminolyzation, number of layers, pH of each layer, and the polymer present in each layer will then be crucial for layer binding and therefore will affect film wettability (Carneiro-da-Cunha et al., 2010). The wettability of a surface depends on the nature of the outermost layer and not on the initial substrate film; however, the interpenetration of layers may cause some influence on that property (Fu et al., 2005). Changes in pH of coatings can significantly affect wettability

24  Chapter 1 Table 1.8: Mainly investigated applications of wettability of edible coatings in food. Contact Angle θ (degree)

Coefficient of Spreading (Ws) References

Matrix of Coating

Food

Chitosan + tween 80 Starch + sorbitol

88.9 83

−66.8 −44

Choi et al. (2002) Ribeiro et al. (2007)

86

−45

Ribeiro et al. (2007)

80

−38

Ribeiro et al. (2007)

Chitosan + GFGT + AFGB + corn oil + glycerol/sorbitol + tween 80 GFAP + glycerol

“Fuji” apple skin Strawberry (Fragaria ananassa cv. Camarosa) Strawberry (F. ananassa cv. Camarosa) Strawberry (Fr. ananassa cv. Camarosa) “Regional” cheese of Portugal Acerola

—

−28 to −59

—

−29 to −47

GFAP + glycerol

Cajá

—

−27 to −36

GFAP + glycerol

Mango

—

−29 to −37

GFAP + glycerol

Pitanga

—

−26 to −44

GFAP + glycerol

Seriguela

—

−23 to −37

GFCP + glycerol

Acerola

—

−32 to −58

GFCP + glycerol

Cajá

—

−27 to −47

GFCP + glycerol

Mango

—

−45 to −77

GFCP + glycerol

Pitanga

—

−35 to −58

GFCP + glycerol

Seriguela

—

−36 to −51

POLICAJU + tween 80

Apples Golden delicious Atlantic salmon (Salmo salar) Ricotta cheese

—

−26 to −53

—

−4 to −13

Cerqueira et al. (2009a) Cerqueira et al. (2009b) Cerqueira et al. (2009b) Cerqueira et al. (2009b) Cerqueira et al. (2009b) Cerqueira et al. (2009b) Cerqueira et al. (2009b) Cerqueira et al. (2009b) Cerqueira et al. (2009b) Cerqueira et al. (2009b) Cerqueira et al. (2009b) Carneiro-da-Cunha et al. (2009) Souza et al. (2010)

—

−22 to −47

Martins et al. (2010)

Carrageenan + glycerol Chitosan + tween 80

Chitosan + tween 80 GFGT + corn oil + nisin + glycerol

AFGB, Agar from G. birdiae; GFAP, galactomannan from A. pavonina seed; GFCP, galactomannan from C. pulcherrima seeds; GFGT, Galactomannan from G. triacanthos; POLICAJU, polysaccharide from A. occidentale L. tree gum.

of a surface, because they can change the film structure (Carneiro-da-Cunha et al., 2010). At higher pH values the chains of polymer are more weakly charged and adopt a loopier and globular conformation than those at lower pH values, those chains present a smoother surface, adopting more flat structures thus leading to a thinner polymer layer (Fu et al., 2005; Yoo et al., 1998).

Basic and Applied Concepts of Edible Packaging for Foods  25

4.3  Contact Angle of Coatings in the Surface of Foods The hydrophobic effect is properly understood as a phenomenon dominated by the strong self-association of water molecules that excludes association with, and solubilization of, nonpolar solutes (Vogler, 1998). Contact angle (θ) of films is one of the indicators for direct determination of the hydrophilic or hydrophobicity of films (Galus and Kadzińska, 2016; Lenart et al., 2013). When the lipid content is increased, the contact angle is increased due to the hydrophobic character of films by the increase of lipid molecules. The swelling effect of water droplets deposited on the hydrocolloids films through time is related to the hydrophilic nature of such materials (Kokoszka et al., 2010). This phenomenon is due to the solubility of the film surface in contact with water. In general, films with higher θ values exhibit a higher surface hydrophobicity (Ramos et al., 2013; Tang and Jiang, 2007); quantitative differentiation between hydrophobic and hydrophilic surfaces is indeed based on whether θ > 65 degree or θ < 65 degree, respectively (Vogler, 1998). This property is also determined in the outer surface (skin) of the fruits, such as apples (Carneiro-da-Cunha et al., 2009; Ramírez et al., 2012), and mango (Vicente et al., 2012) to know the interactions with liquids through dispersion forces to demonstrate the ability of surface to participate or not in nonpolar interactions. This property (θ) is measured at the intersection by the angle between the tangent of the spherical part of the liquid/vapor interface and the solid interface (Wang et al., 2016). Probably, it is the most important parameter of surface science, which is used to characterize the wettability of solid surfaces, drop condensation or evaporation, icing, drop impact phenomena, adhesion between drops and solid surfaces, and may be the other practical application. For this reason, an accurate measurement of the contact angle is of fundamental importance and can be affected by impurities in the fluid, line tension, adsorption of the vapor onto the solid phase, electrostatic potential, surface roughness, or chemical heterogeneity (Biolè et al., 2016). The most widely used technique to date is the Axisymmetric Drop Shape Analysis (ADSA) method (Bateni et al., 2004; Hoorfar and Neumann, 2006; Kalantarian et al., 2009; Rotenberg et al., 1983).

4.4  Surface Tension of Coatings 4.4.1  Surface tension According to Zisman (1964), in systems having a surface tension lower than 100 mN/m (low-energy surfaces), the contact angle formed by a drop of liquid on a solid surface will be a linear function of the surface tension of the liquid, YLV, (were phase V is air saturated with the vapor of the liquid, L). Zisman’s method is applicable only for low-energy surfaces; therefore, it is necessary to determine the surface energy of the apple. For a pure liquid, if polar YLp and dispersive YLd interactions are known, and if θ is the contact angle between

26  Chapter 1 that liquid and a solid, the interaction can be described in terms of the reversible work of adhesion, Wa (Eq. 1.1), as:

(

)

Wa = Wad + Wap ↔ Wa = 2 ⋅ YSd ⋅ YLd + YSp ⋅ YLp (1.1) where YSp and YSd are the polar and dispersive contributions of the surface of the studied solid. Rearranging Eq. 1.1, yields (Eq. 1.2): 1 + cos θ YL Yp ⋅ = YSp ⋅ Ld + YSd (1.2) 2 YL YLd The contact angle determinations of at least three pure compounds: bromonaphthalene (Merck, Germany), formamide (Merck, Germany), and ultrapure water, on the surface (skin) of the apple combined with the respective dispersive and polar component values, will Yp allow the calculation of both the independent variable, Ld and the dependent variable, YL 1 + cos θ YL ⋅ from Eq. (1.2). 2 YLd The surface tension, the dispersive, and the polar component are, respectively, 72.10, 19.90, and 52.20 mN/m for water, 44.40, 44.40, and 0.00 mN m−1 for bromonaphthalene and 56.90, 23.50, and 33.40 mN m−1 for formamide (Busscher et al., 1984). The surface tension of a coating solution is typically determined using a pendant drop technique, together with the Young–Laplace equation (Song and Springer, 1996). 4.4.2  Critical surface tension The estimation of the critical surface tension (Yc) was performed by extrapolation from Zisman plots (Zisman, 1964) obtained by plotting the cosine of the contact angle of pure liquids on a solid surface to be studied against the surface tension of the same series of liquid. The critical surface tension (Yc) (Eq. 1.3) is defined as: Yc = lim YLV , as θ → 0 (1.3) The intercept of the curve at cos θ = 1 is known as critical surface tension. Critical surface tension is a fictitious value of YSV, which is often used to describe surface wettability (Lima et al., 2010). Several authors have reported the critical surface tension for improvement of Ws of coatings in foods with the addition of plasticizers and surfactants (Table 1.9). 4.4.3  Surface-free energy Surface-free energy is a characteristic thermodynamic quantity for each substance associated with the equilibrium state of the atoms in a surface layer of matter (Moncayo et al., 2013).

Basic and Applied Concepts of Edible Packaging for Foods  27 Table 1.9: Investigated applications more important of critical fruit skin (food) surface tension. Fruit

Critical Surface Tension (mN/m) T (°C)

References

Apple Strawberry Strawberry Tomato Apple Hog plum Cajá Mango Redcurrant Plum “Regional” cheese of Portugal Mango Apple Atlantic salmon (S. salar) Waxed cranberry Unwaxed cranberry Waxed apple: Granny smith Apple Quince

18.70 18.8 18.84 17.4 25.4 9.39 23.92 26.68 13.42 19.62 18.33 19.5 25.4 30.13 26.8 34.1 39.7 18.56 18.71

Choi et al. (2002) Castro (2005) Ribeiro et al. (2007) Casariego et al. (2008) Carneiro-da-Cunha et al. (2009) Cerqueira et al. (2009b) Cerqueira et al. (2009b) Cerqueira et al. (2009b) Cerqueira et al. (2009b) Cerqueira et al. (2009b) Cerqueira et al. (2009a) Lima et al. (2010) Lima et al. (2010) Souza et al. (2010) Skurtys et al. (2011) Skurtys et al. (2011) Velásquez et al. (2011) Ramírez et al. (2012) Ramírez et al. (2012)

— 19 19 20 21.1 21.3 21.3 21.3 21.3 21.3 21.3 20 20 20 21 21 21 25 25

One of the important applications of the contact angle measurement is the assessment of the surface-free energy of the solid (Kwok and Neumann, 1999). The well-known Young Eq. 1.4) describes the balance at the three-phase contact of solid– liquid and gas. YSV = YSL + YLV cos θ Y (1.4) The interfacial tensions, YSV, YSL, and YLV, form the equilibrium contact angle of wetting, many times referred as Young contact angle θY (Siboni et al., 2004). The Young equation assumes that the surface is chemically homogenous and topographically smooth (Volpe et al., 2004). In Eq. 1.4, the surface-free energy of the solid is described by using the contant angle θY, surface tension of the liquid YLV and interfacial tension between solid and liquid YSL (Siboni et al., 2004). The first two are easily measured but the problem is the unknown YSL, which cannot be measured directly. To be able to solve the equation, more assumptions of the relationship between YSV, YSL, and YLV has to be made (Volpe et al., 2004). Surface-free energy of the solid is equivalent to surface tension of the liquid and the unit is the same mN/m (=dynes/cm). This represents the specific state of nonequilibrium intermolecular interactions in the boundary phase between two media (Moncayo et al., 2013). Although the contact angle itself also gives indications on the wetting properties of the surface, the contact angle always depends also on the liquid used for the measurements

28  Chapter 1 Table 1.10: Methods for determining a liquid’s surface free energy and various indirect methods used for determining the surface free energy of solids. Methods

Description

References

Fowkes

Divides surface energy into dispersive and polar components and uses a geometric mean approach for combining their contributions Consists of determining dispersion and polar surface free energy components on the basis of the Berthelot hypothesis Accepted to idea of Owen and Wendt to divide the SFE into polar and dispersive components. Requires the use of at least two liquids, one mainly polar and one dispersive. Water and diiodomethane are again often used. From a theoretical point of view, the geometric mean is more accurate than the harmonic one Is used to define so-called critical surface tension, which is the surface tension of the liquid needed to completely wet the solid (contact angle between the solid and liquid is zero). This critical surface tension value differs from the surface free energy of the solid, and is not divided into dispersive and polar components. In theory, only two measurement points would be needed but in practice using just few different liquids will lead to incorrect results. Even negative values are often seen Is based on the assumption that there is a relationship between surface energy free of a solid, surface energy free of the liquid wetting the solid surface, and surface energy free of the solid–liquid interface The acid-base approach. The polar component is further divided into acid and base components. Acid-base method is one of the most recent developments in the field of SFE calculations. It has a potential to give more in depth information about surface properties of the solid but has been criticized by its sensitivity to even small variations in the contact angle measurements or properties of liquids used

Lu et al. (2012)

Owens-Wendt

Wu

Zisman plot

Newman

Van OssChaudhury-Good

Rudawska and Jacniacka (2009) Volpe et al. (2004)

Siboni et al. (2004)

Zenkiewicz (2007)

Kwok and Neumann (1999)

(Volpe et al., 2004). In Table 1.10 we describe some of the reported methods to determine surface-free energy in liquids and solids.

4.5 Conclusions The effectiveness of edible coatings for protection of fruit and vegetables and extend product shelf life depends primarily on controlling the adhesion and wettability of the coating

Basic and Applied Concepts of Edible Packaging for Foods  29 solutions spread uniformly on the fruit’s surface. Surface tension varies, depending on the fruit skin composition.

5  Edible Packaging for Food Application 5.1 Introduction The quantity of packaging materials has been increased by 8% annually (Muizniece-Brasava et al., 2011; Tavassoli-Kafrani et al., 2015). Less than 5% of all plastics are recycled, leading to a high accumulation of plastics in the environment (Espitia et al., 2014a,b). Continuous removal of these plastics (nonbiodegradable), to generate a growing tendency to replace petroleum-based polymers with biodegradable materials, these biodegradable polymers have been used mainly to formulate edible films and coatings (De Azeredo et al., 2014). Edible films and coatings have been assessed in various types of food, with excellent results in prolonging the shelf life (Falguera et al., 2011). Here are some applications on fruits and vegetables, dairy products, meat and poultry, and the main results that are obtained.

5.2  Fruits and Vegetables Fresh and minimally processed fruits and vegetables are highly perishable (Jung and Zhao, 2016), so they need optimal postharvest technologies in order to maintain their storage and stability. To prolong the food shelf life there are several types of biopackaging made from natural polymers, such as starch (Chiumarelli and Hubinger, 2014), pectin (Taqui and Stamatin, 2014), chitosan (Elsabee and Abdou, 2013), galactomannans (Cerqueira et al., 2011), alginate (Guerreiro et al., 2015), proteins (Belyamani et al., 2014), and wax (Ochoa et al., 2011). Edible films (F) and coatings (C) have been considered a technology with great potential to extend the shelf life of fruits and vegetables (Cerqueira et al., 2011). Emulsions have proved to be effective to increase stability of a variety of fresh or processed fruits, vegetables, cheeses, and other food products (Galus and Kadzińska, 2015). In Table 1.11 we describe some of the applications for edible packaging and also the main components used.

5.3  Fresh-Cut Fruit and Vegetables In recent years, consumers have shown a growing interest in the consumption of fresh produce, healthy and nutritious products that bring health benefits, so the demand for freshcut fruits and vegetables is very high. However, the peeling and cutting operations may accelerate the metabolic activities of plant tissue (Chiumarelli and Hubinger, 2012), making the minimally processed product more perishable than intact fruits and vegetables. A solution for increasing the shelf life of fresh and minimally processed fruits and vegetables is coating with edible film (Table 1.12) (Ciolacu et al., 2014).

30  Chapter 1 Table 1.11: Summary of different applications of edible coatings and films in fresh fruit and vegetables: components, and primary findings. Application

Components

Primary Findings

References

Arbutus unedo

Alginate with the essential oils compounds: eugenol and citral. (C) Chitosan and A. vera extract (C) carboxymethyl cellulose and chitosan (C)

Preserved sensory and nutritional attributes and reduced microbial spoilage The shelf life was extended 5 days

Guerreiro et al. (2015)

Blueberry Citrus fruits

Red Crimson grapes

Pumpkin

Apples

Avocado

Tomato fruits

Green bell peppers

Baby carrots

Coatings notably improved all quantified parameters of fruit quality 21 days storage under refrigerated conditions

Cornstarch and gelatin, plasticized (glycerol or sorbitol) (C) k-Carrageenan, tapioca starch The products obtained were safe from microbiological view point and (C) presented a satisfactory color and texture Candelilla wax, ellagic acid, Edible film on apples extends jojoba (C) oils their shelf life and elevates the antioxidant potential, as well as their nutritional quality Ellagic acid, candelilla wax (C) Edible films were able to reduce significantly the damage caused by C. gloeosporioides, also significantly reducing the change in appearance and weight loss in fruit Chitosan, acetic acid (F) The tomato coatings can prevent weight loss and maintain freshness. The nutritional value was increased by iodide supplementation Pectin, arabic and xanthan The edible coating significantly gums, candelilla wax, jojoba extended shelf life of green bell oil, and a crude extract of pepper polyphenols (C) Chitosan, acetic acid, glycerol Chitosan-based coatings delayed microbial spoilage in carrots and exhibit positive effects on the color and texture of carrots

Vieira et al. (2016) Arnon et al. (2015) Fakhouri et al. (2015) Genevois et al. (2015)

Ochoa et al. (2011)

SaucedoPompa et al. (2009)

Limchoowong et al. (2016)

Ochoa et al. (2013)

Leceta et al. (2015)

C, Coating; F, film.

5.4  Dairy Products Milk and dairy products are an important source of the nutrients required for growth in children and for maintaining health in adults (Cardador and Gallego, 2016). Cheese is the most diverse group of dairy products; however, the shelf life of cheeses is limited by the action of microorganisms. Antimicrobial coatings applied to the cheese surface is one way

Basic and Applied Concepts of Edible Packaging for Foods  31 Table 1.12: Summary of different applications of edible coating and films in fresh-cut fruit and vegetables: components and primary findings. Mechanical Properties

Permeability

Primary Findings

References

Alginate coating and malic acid (C) Cassava starch, glycerol, carnauba wax, and stearic acid (F, C)

—

—

14 days storage

Elastic modulus: 0.221 (MPa)

Increase in the water vapor resistance and reduction in weight loss

Citric acid, calcium chloride, cassava, starch, and glycerol (C) Apple pectin, oleic acid, tween 80, citric acid, calcium chloride Fruit and vegetable residues (F)

—

CO2: 6.13 mL/kg h water vapor resistance: 44.51 s/cm —

Salinas et al. (2016) Chiumarelli and Hubinger (2012)

—

—

Tensile strength: 0.14 MPa

—

Edible coating inhibited the growth of food-borne human pathogens in inoculated persimmons The data demonstrate the potential of a multicomposite vegetable matrix for producing coatings and packaging materials The bioactive coating inhibits L. monocytogenes after 7 days of storage at 4°C The composite bags were found to protect vegetables against S. aureus activity by serving as a good barrier and as an antimicrobial agent

Application

Components

Fresh-cut mango Fresh-cut apples

Fresh-cut mango

Fresh-cut “Rojo Brillante” persimmon Fresh-cut carrot

Precut cauliflowers

Fresh-cut: asparagus, baby corn, and Chinese cabbage

Lactic acid, — citrus extract, lemongrass, and tween 80 (C) Chitosan, glycerol, Tensile banana flour (F) strength: 5.19– 4.22 MPa; elongation: 1.64%–2.59%

—

Water permeability: 38.81– 41.66 g(mm/ m2 day kPa)

Coating was efficient Dussán et al. to maintain the quality (2014) during 24 days of storage Sanchís et al. (2016)

Fai et al. (2016)

Boumail et al. (2016)

Pitak and Rakshit (2011)

C, Coating; F, film.

to limit negative changes, which can be promoted during handling and storage (Galus and Kadzińska, 2015). Table 1.13 summarizes different applications of edible coating and films in dairy products.

5.5  Meat and Poultry Meat is characterized as a food with tissue structure and is often treated by different kinds of technological processes that favor the development of microorganisms. Antimicrobial and intelligent packaging has emerged as a food-safety hurdle technology in recent years.

32  Chapter 1 Table 1.13: Summary of different applications of edible coatings and films in dairy products: components and primary findings. Application

Components

Cheese

Semi-hard cheese

Galactomannan, glycerol and corn oil (C) Chitosan and natamycin (F)

Ricotta cheese

Chitosan and whey protein (F)

Cheese

Whey protein isolate, glycerol, guar gum, sunflower oil, and tween 20 (C) Chitosan, sodium alginate, and soy protein isolate (C)

Mozzarella cheese

Permeability

Primary Findings

References Cerqueira et al. (2010)

O2: 7.68 × 10–15 g/ (Pa/s m), CO2: 64.58 × 10–14 g/ (Pa/s m) O2: 21.3 g/(mm/ m2 day2 kPa2) CO2: 17.7 g/(mm/ m2 day2 kPa2)

Significantly reduced the O2 consumption and CO2 production rates decreased on molds/yeasts of 1.1 log (CFU/g–1) compared to control after 27 days of storage The coating delayed the development of undesirable acidity, better maintained the texture, and did not seem to modify sensory characteristics Reduction in the water loss, hardness, and color change

Sodium alginate coated cheese possessed best overall properties during storage

Zhong et al. (2014)

Fajardo et al. (2010)

Di Pierro et al. (2011)

Ramos et al. (2012)

C, Coating; F, film.

Also, considering large volumes and varieties of ready-to-eat meat and poultry industry there is need for alternative methods to control food-borne pathogens and to improve the shelf life in their products (Guo et al., 2014). By this way, edible films and coatings have been used to improve the gas and moisture barriers, mechanical properties, and sensory perceptions of meat products (Galus and Kadzińska, 2015). The application that has been used is by foaming, dipping, spraying, casting, brushing, individual wrapping, or rolling (Ustunol, 2009). In recent years there have been generated various forms of combined meat preservers using bioactive edible films and coatings (Table 1.14). 5.5.1 Fish Fresh and minimally processed fish is highly perishable during storage mainly due to rapid microbial growth of microorganisms naturally present in the fish or from contamination, which can occasionally result in either economic or health-related problems (Gómez-Estaca et al., 2010; López de Lacey et al., 2014). For conservation, some strategies have been recently developed. One of these strategies is the design and application of edible films and coatings to improve the safety and shelf life of fish. Several polysaccharides have been used, such as chitosan, agar, starch, whey protein isolate. Also, other techniques are used to prolong the shelf life, such as marinating (Van Haute et al., 2016) to create an additional sensorial value. A summary of some of the advances in research during the last years is presented in Table 1.15.

Basic and Applied Concepts of Edible Packaging for Foods  33 Table 1.14: Summary of different applications of edible coating and films in meat and poultry: components and primary findings. Mechanical Properties

Permeability

Shelf Life

References

Chitosan (2%), chitosan (2% and 1.5% clove oil)

No response

No response

Lekjing (2016)

Gelatin (3 g/100 g protein), 50 g/100 g of glycerol (based on protein content), catechin and lysozyme (1:1) Whey protein isolate (100 g/kg), glycerol (50 g/kg), oregano oil (10 g/ kg), clove oil (20 g/ kg)

Tensile strength: 5.05 ± 0.59 MPa, elongation at break: 200.16 ± 15.56%

4.25 ± 0.11×10–6 g/(mm h cm Pa)

Retards the lipid oxidation and extends the shelf life up to 20 days under refrigeration Reduces discoloration, thiobarbituric acid reactive substances, weight loss, and microbial growth

No response

No response

FernándezPan et al. (2014)

Pork meat Chitosan tea patties polyphenol

No response

No response

Roasted turkey

No response

No response

The use of oregano oil increases the shelf life from 6 (control) to 13 days, keeping the total mesophilic aerobic, Pseudomonas spp., and lactic acid bacteria counts under the microbiological limits recommended for distribution and consumption The shelf life is extended for 6 days at 4°C. Slows the increase of thiobarbituric acidreactive substances and metmyoglobin with acceptable sensorial attributes The best edible film is pectin combined with commercial antimicrobials. L. monocytogenes is reduced 1.1 log CFU/cm2 during the next 8 weeks after having been frozen 4 weeks

Product

Components

Cooked pork sausages

Minced pork

Chicken breast fillets

Starch (15% w/v), chitosan (2% w/v), alginate (1% w/v), pectin (1% w/v), sodium lactate (3.5 g), sodium diacetate (0.44 g)

Kaewprachu et al. (2015)

Qin et al. (2013)

Jiang et al. (2011)

34  Chapter 1 Table 1.15: Summary of different applications of edible coatings and films in fish: components, and primary findings. Application

Components

Golden pomfret (Trachinotus blochii)

Tilapia fish gelatin, chitosan (C)

Mechanical Properties

Permeability

Primary Findings

References

No response

No response

Inhibition of weight loss during 17 days. pH, TVB-N, and TVC remained stable at 6.1, 13.56 mg/100 g, and 4 log CFU/100 g during cold storage 84.83%–100% inhibition of E. coli at 96 h. Reduce the increase of free fatty acids, peroxide value, and aerobic plate count

Feng et al. (2016)

Reduction of H2Sproducing bacteria counts and total viable bacteria throughout the storage period (15 days). The quality is maintained within the limits of acceptability The film retains the quality and the shelf life of fish samples during refrigerated storage, and shows an antioxidant effect

López de Lacey et al. (2014)

Improves the water holding capacity, drip loss, and textural properties. Slows the deterioration up to 8 days (5 days for untreated fish) 1.5% sodium alginate/10% glycerin/5% vitamin C is the best treatment due to the reduction of chemical spoilage, the slowing of water loss, and the increase in global sensory quality

Mohan et al. (2012)

Tilapia steaks Low density polyethylene, chitosan (F)

Fillets of defrosted hake (Merluccius capensis)

Rainbow trout (Oncorhynchus mykiss) fillets

Fillet of sardine (Sardinella longiceps)

Bream (Megalobrama amblycephala)

Tensile strength 1.24 −3.73 (MPa). Elongation at break (%) machine direction (111.96–243.03). Heat seal strength (MPa) (1.71–3.17) Agar, glycerol, No response glucose, green tea extract (Camellia sinensis L.)

Oxygen transmission rate 2189–2487 (mL/m2/day). Water vapor transmission rate (g/m2/day) (2.88–4.19) No response

Chitosan (1% w/v) in 1% v/v acetic acid, gelatin (3% w/v), glycerol (0.75 mL/g) Chitosan (1–2%)

No response

No response

No response

No response

Sodium alginate (1.5%), calcium chloride (2%), vitamin C, and tea tocopherols

No response

No response

Reesha et al. (2015)

Nowzari et al. (2013)

Song et al. (2011)

Basic and Applied Concepts of Edible Packaging for Foods  35

6  Regulatory Aspects and Commercialization of Edible Packaging 6.1  Edible Packaging Legislation and Consumer Behavior Since the decade of the 1970s the European Union (EU) has established a regulatory policy for analysis and quality control of food packaging and all food contact materials for consumer health protection and commercial reasons, which includes steel, wood, aluminum, cellulose, paper and plastics, and active and intelligent materials (Silano and Rossi, 2015). In the case of the USA, the legislation is regulated by the Food and Drug Administration (FDA). But, why in the last 20 years has edible and active packaging become so important? Well, it is because it is considered an imperative strategy of the actual effort to accomplish food safety around the world (Barone et al., 2015). The FDA establishes differences between a Food Contact Substance (FCS), Food Contact Material (FCM), and Food Contact Article (FCA). FCS is defined as any substance that is intended for use as a component of materials used in manufacturing, packing, packaging, transporting, or holding food, if such use of the substance is not intended to have any technical effect in the food. FCM is a single substance, such as a polymer or an antioxidant in a polymer. As a substance, it is reasonably pure. The FCA is the finished film, bottle, dough hook, tray, or whatever is formed out of the FCM. The definitions can be a little confusing; however, each one has a single but substantial difference. To better understand these definitions we can say that an FCM is made with FCS and other substances where the composition can be variable, often it is a mixture like an antioxidant in a polymer. The evaluation of food active and/or intelligent packaging follows the same principles for any FCM, regarding exposure assumptions of toxicological data. Nevertheless, the specific information about the functions of the substance or active ingredients in the packaging must be provided. Additionally, migration testing may be effectuated with the specific conditions specially selected and designed for the intended use of the packaging. However, a large quantity of new materials, such as adhesives, rubber, and coatings have not been evaluated yet for the European legislation, so for this reason there is a lack of information for many of the substances found in these materials that makes this area of food safety particularly challenging. In an attempt to have a worldwide applicable regulation the Food and Agriculture Organization of the United Nations (FAO), and the World Health Organization (WHO) created a document to guide all the countries uniform about food legislation and standards, the Codex Alimentarius (FAO, 2016a,b). Edible, natural, and smart packaging regulations should follow the legislation of the country that is going to be sold to the final consumer. Each country is responsible for the guarantee of

36  Chapter 1 the safety of the consumers. The specific characteristics of materials and treatments for those packages depends on the country where they will be sold, but it is also important to label the coated foods with the correct information of about ingredients used, processing technologies, and final functionality of the package. Consumers have the right to be always informed about the food and in general the products that they are buying. It is said that edible films and coatings should be classified as food additives because they are made intentionally to be eaten with the food. For the EU, edible food packages are included in the regulations for food additives, which says “in order to protect human health, the safety of additives for use in foods for human consumption must be assessed before they are placed on the community market,” so in the formulation of edible films it only can be used ingredients that appears in the community list of authorized substances (EC 1331/208). Moreover, the use of food additives must be always technologically justified and also why the technological effect cannot be accomplished by any other economically substance, and the substance add should not mislead the consumer, of course. Enough information is needed to confirm that the additive used is safe for the consumers, such as probes of toxicity and acceptable daily intake (EU 234/2011). In the USA, the FDA provides a list of ingredients that must be used as part of the coatings and emulsions. This regulation permits the use of only the listed components at certain concentrations. The list is practically composed of GRAS substances and other provided safe ingredients. The entire list is in the subpart C: “Substances for use as components of coatings” in the section “Indirect Food Additives: Adhesives and Components of Coatings” (FDA, 2015). The USA regulation also mentions that in the case of fresh fruits and vegetables that have a coating, they should be labeled to give the information to the consumers; consumers are really informed about their food, which is an excellent point for quality food commercialization. Natural films can be made not to be eaten, for example, in the case of those to be used as biodegradable wraps, active and/or intelligent (smart) packaging. One difference between biodegradable coatings or wraps and active packages is that the first ones are inert to food; it means that its mechanism of action is due to the creation of a modified atmosphere in the surface of the foodstuff and permeation to water vapor (WV), oxygen, and other gases. Active packaging is an intentional design to directly interact with the foodstuff and/or the surrounding environment to make it active; most scientists have been incorporating natural extracts in the films (Pereira de Abreu et al., 2011). Active packaging has received special attention during the last years because it is one of the most promising technologies to traditional packaging, where antioxidants are added to reduce oxidation in foodstuff, which is one of the main causes of deterioration (López-de-Dicastillo et al., 2012).

Basic and Applied Concepts of Edible Packaging for Foods  37 In the aspect of consumer behavior, it is undeniable that the edible packaging area is a hot topic in science the last 20 years because the consumer demands a high quality and fresh or minimally processed foods, edible packages, and active ones that offer this possibility, improving the microbiological quality (Fuciños et al., 2016). In addition, consumers are increasingly concerned about the environmental pollution in which traditional plastics (made from petroleum) represent a huge source of contamination due to traditional plastics that are not biodegradable and remain in nature as waste for a long time, representing a risk for human health and the environment. The Director General of the Environment of the European Commission (Official Journal of the European Union, 2008) reported that the total plastic waste postconsumer in the EU, Norway, and Switzerland was of 24.9 Mt. Plastics from packaging represent by far the largest contributor with 63% of the input of plastic waste (Official Journal of the European Union, 2011). Edible films have been formulated in most of cases with biopolymers that make a biodegradable and ecofriendly package, motivated again by the position and interest of the consumers, in the actuality represents a viable alternative to traditional plastics at least for food packaging (Atarés and Chiralt, 2016; Cerqueira et al., 2012). On the other hand, in some countries, such as Mexico, there is still a lack of information about edible functional, bioactive, and intelligent packaging, where there is no specific legislation for this type of material. For this reason some consumers disapprove uses of edible films and waxes in fruits, but the correct information about edible films, their composition and benefits will change current opinion. Creation of specific norms for these types of materials is also needed to achieve this goal.

6.2  Economic Feasibility and Benefits of Edible Packaging One of the most important parameters to take into account (if not the most important) during development and commercialization of any product is the economic feasibility, because no matter if the product or in this particular case edible films are excellent alternatives to traditional packaging if it is not economically profitable and technically possible. For that, the challenge to overcome for edible coatings is the low cost of fossil materials, from which traditional plastics are made; during the last year’s plastic from fossil sources has been the cheap way to package food, not only for FCM, but also the bags where food is transported from store to consumer houses. Nevertheless, in recent years economic sources of biopolymers have been explored to make edible films economically competitive with traditional packaging, which has resulted actually in really viable options. Van Beilen and Poirier (2007) attributes the increase of investigation of biopolymers for consumer and industrial purposes to three causes: (1) economics, (2) public acceptance, and (3) regulations. In the case of “economics,” biopolymers used in edible film formulation can be obtained from traditional agricultural wastes and commodities (Arvanitoyannis, 2010), representing a cheap

38  Chapter 1 source of raw materials, such as polysaccharides, lipids, and proteins (Espitia et al., 2014a,b). In the case of polysaccharides, the main used are alginate, carrageenan, pectin, gums, and starch. Proteins are obtained from animal origins, such as fish, pig, and bovine gelatin and also whey protein (Milani and Maleki, 2012). Lipids that are used as edible film ingredients include essential oils (Slavutsky and Bertuzzi, 2016), candelilla wax (Kowalczyk, 2016), and beeswax (Velickova et al., 2015). In the second point, “public acceptance,” we can affirm that consumer demand of healthier and/or functionalized food has been covered by the use of edible packaging, meaning that it is an acceptance by the public, of course, with their previous knowledge about edible films, including ingredients, benefits, and intention of the ingredients in the food. Linked to this part, the “regulations” are intimately related and as it is described later, edible film legislation establishes the obligation to inform consumers about composition and function of the film and establishes the need that the ingredients must be edible and biodegradable. This last has a positive impact on the public acceptance, too. Plastic waste represents a huge problem around the world. Recycling is not a single solution, as actually less than 5% of plastic waste is recycled (Espintia et al., 2014) and the other 95% remains as waste in the environment. Consumers accept that edible films can help to decrease this problem. Among the benefits of edible packagings, they are biodegradable, without toxicity, they can reduce moisture loss, and unfavorable chemical reaction in the food, such as enzymatic browning (Osorio et al., 2011), spoilage, and microbial development (Arvanitoyannis, 2010) by adding bioactive compounds. Valero et al. (2013) report that edible coatings are also effective at preserving the quality of fruits at postharvest level. They can also prolong the shelf life of foods mainly by preventing dehydration, oxidative rancidity, and gas permeation (Dhanapal et al., 2012). Viebke et al. (2014) refers nutritious characteristics at the hydrocolloids used in edible films (pectin, alginate, carrageenan, etc.), so they are acting like food ingredients with the following benefits: lowering the risk factors for cardiovascular disease, immune function, weight management, and intestinal problems. Edible films could be used also to enhance organoleptic attributes of the food, such as visual appearance and tactile sensation and to haul active substances, such as antioxidants, antimicrobial, nutraceuticals, colors, and flavors (Han and Scanlon, 2014) because they can be considered as active packaging and a food component (Salgado et al., 2015).

6.3  Commercialization Aspects of This Type of Packaging One of the first commercial interests related to edible films is a patent submitted by the FMC Corporation, with the intention to use a wax coating in fresh fruit (De Ore, 1933). Another formulation was presented in the same year by Griffin Laboratories, using gelatin coating

Basic and Applied Concepts of Edible Packaging for Foods  39 for food preservation; foods that can be covered with this film include meat, fruits, packaged food, and vegetables (Griffith and Hall, 1933). Since then, but especially in the last 35 years, commercialization of edible films and coatings has expanded as pointed out by Attila E. Pavlath (Bernstein and Woods, 2013) who says that in the middle of 1980s only 10 companies were in the business of edible packaging, compared with more than 1000 that actually are now and that have an annual income for almost $100 million (USD). Current applications of edible films and coatings are expected to continue to grow, for example, in the use of ready-to-eat products that actually represent 10% of the total produce sales. In actuality, patent requests for inventions as edible films and coatings for food applications included an ultrathin edible coating made from gold or silver in an edible substrate, claimed by Ds Group (Kumar and Kumar, 2015), the use of seaweed, paper fibers, and starch (Santos, 2013), and a film from polysaccharide gum as pullulan replacement (Nieto, 2012). Table 1.16 summarizes some companies as examples of the current commercially available edible food packages. One of the most important considerations to take into account to commercialize edible, natural, biodegradable, or active packaging for food application is the current legislation of the country where the product is to be sold. With the aim to have a legal product, all of the ingredients contained in the edible package shall be approved for use in food, as ingredients, additives, or as FCM, depending of the country. The great number of applications of the edible packages, such as inhibit spoilage, microbial contamination, prevention of loss of water, prolonged storage and shelf life, increased nutritional value of food, added bioactivities for the human health, serves as transportation units for the food, being healthier edible packages and biodegradables, where most of them are made of renewable raw materials in sustainable processes, make them promising technologies for the assurance of food quality for consumers. Investigation, development, and commercialization of edible packaging for food applications will still grow in the next years, due to the almost unlimited applications, the research of new sources of raw materials, specific activities by demands of consumers, and by the need to change the actual tendency in traditional plastics uses.

7  Properties, Production, and Processing of Edible Packaging There is a wide variety of material used to make edible packaging and, as a result, various film-forming behaviors may come about. Proteins and polysaccharides normally form films with good mechanical properties but are poor moisture barriers due to their hydrophilic nature. Lipid’s functional properties depend on their chemical structure (Rhim and

40  Chapter 1 Table 1.16: Some companies with examples of commercially available edible food packaging. Company

Product

Bioingenio lifetech S.A de C.V.

Coatings for Made with candelilla wax, fruits (berries natural polymers, and and pineapple) natural antioxidants

Agricoat natureseal ltd.

Semperfresh

Natureseal WikiFoods

Wiki Pearl

Characteristics

Made of sugar esters, vegetable oils, and cellulose Does not impregnate in the fruit odor or flavor Edible-protective electrostatic gel (with and without flavor)

Uses

Form of Application

Postharvest protection against fruit oxidation spoilage and improvement of brightness For pre- and postharvest protection. Prolongs storage and shelf life Shelf life prolongation

Dipping or spraying

Dipping, drenching, or spraying N/M

Transportation, storage N/M of diverse types of food, as liquids and solids. Wraps the food into a protective pearl BASF FreshSeal Extends storage, shipping Postharvest in: N/M distance, and shelf life. cantaloupes, Is made with ingredients honeydews, pineapples, approved by the FDA mangos, avocadoes Improveat BioCheeseCoat Prolongs shelf life, inhibits Cheese N/M bacteria, yeast and, fungi contamination, and prevents water loss BioNutriCoat Increases nutritional Cheese, meat, bread N/M capacities of food by adding vitamins, antioxidants, pre- and probiotics BioFruitCoat Prolongs shelf life by Fruits and vegetables N/M inhibiting enzymatic degradation and oxidation Caragum Fibrecoat spray A natural filmogenic Fried breaded products Spraying international barrier; permits reducing the lipids absorption Fibrecoat Helps reduce fat in fried By adding the tempura tempura foods product at the tempura mixture MantroseCrystalac A natural glaze to enhance Confectionary products N/M Haeuser Co., shelf life, moisture Inc. resistance, and fat barriers Certicoat Coating made of oil and Molded and extruded Immersion and natural wax, for moisture confectionary products spraying retention, a custom finish Fruitsymbiose Pürbloom Colorless and tasteless Fresh cut vegetables and N/M Inc. edible microcoating fruits containing algae extract for shelf life extension N/M, Not mentioned.

Basic and Applied Concepts of Edible Packaging for Foods  41 Shellhammer, 2005) and their polarity, which further depends on the distribution of chemical groups, the length of aliphatic chains, and degree of saturation. Hence, saturated fatty acids are very efficient at controlling moisture transfer due to their lower polarity when compared with unsaturated ones (Morillon et al., 2002). Usually, vegetable oils and other liquid lipid substances form layers on the hydrocolloid surface as a bilayer or multilayer and are not capable of forming a separate film; , waxes form solid but brittle and fragile films. A way to obtain films with certain mechanical properties is by using the emulsification process. Ultimate research describing inclusion of lipid substances in film-forming solutions is focused on upgrading moisture efficiency of composite films due to the fact that emulsified films that form as coatings of food surfaces do not need the mechanical properties of stand-alone films used as wraps, pouches, or casings. Commonly, the mechanical properties of emulsified films are analogous to those made of a hydrocolloid matrix and are modified by lipid concentration or type (Galus and Kadzińska, 2015). Hence, the stability or structure of an emulsion is an important parameter affecting mechanical properties of emulsified films. Another major parameter of edible films and coatings is transparency, which is meaningful for the consumer’s acceptance of the product coated based on the appearance. Commonly, emulsified films possess high lightness values with a small decreasing tendency correlated with the increasing concentration of lipid (Monedero et al., 2010; Pereda et al., 2010). A high transparency of the emulsion-based films is related to a good homogeneity in the film structure (Ortega-Toro et al., 2014). It’s important to point out that the presence of a lipid phase provokes opacity as a function of the differences in the refractive index of the phases, concentration, and particle size distributions. The barrier properties of emulsion-based and hydrocolloid films depend on relative humidity and temperature. Oxygen permeability increases at lower relative humidity and decreases at high humidity conditions. Whereas, carbon dioxide permeability of emulsion-based films depend mostly on the chemical composition of lipids. This is due to the shorter hydrocarbon chain length of the fatty acid that makes attraction forces between the fatty acid molecules weaker. Water vapor permeability of the films has a remarkable effect on deteriorative reactions of foods; that is why it is the most important property of the films studied (Rao et al., 2010). Usually, most investigations establish a decrease in water vapor permeability due to the hydrophobic character of lipids and waxes that are the best moisture barriers (Bourtoom, 2008).

7.1  Technological Applications of Edible Packaging and Their Behavior During Storage, Transportation, and Packaging An important characteristic of packaging is to act as a barrier that separates the product from the environment. Several studies stated that edible films have been commercially used to

42  Chapter 1 protect various food products, such as fruits, vegetables, meat, and cheese from pathogenic microbial contamination. Among other functions, it is used as a barrier to moisture, oxygen, and other gases, fats, and oils. These barriers can be applied to fresh produce, such as fruits, vegetables, and ready-to-eat food (Rossman, 2009). Mainly, the chemical, environmental conditions, and the stress handled by consumers can influence the barrier performance of the edible packaging (Krochta et al., 1994). Several active compounds can be added to blends of edible coating or films. These active ingredients can be antimicrobial agents, flavoring, pigment, nutrients, and antioxidants. During the blending process, the functional groups from the edible material could be bonded to the compounds within the matrix. As an example, pigment additives carried by edible materials could improve the appearance of some products during storage. Another is the addition of nisin to alginate-edible films showed antimicrobial activity against Staphylococcus when applied to beef. Edible films made with xanthan gum, calcium lactate, and α-tocopherol can increase the orange color and decrease the white discoloration during 3 weeks of the storage period (Mei et al., 2002). In Mei et al. (2002), it seems that the edible film helped maintained the β-carotene content, and increased vitamin E and calcium in carrots (Han et al., 2005; Mei et al., 2002). There are fragile products that can improve its mechanical properties with the use of edible coatings. Some examples are the use of chitosan coating applied on strawberries to decrease the mechanical damage during storage, processing, and transportation of the fruit (Han et al., 2005; Pascall and Lin, 2013). Nonetheless, carbohydrate and protein-based edible packaging have less tensile strength due to their strong cohesive energy density. This characteristic could be used to supply a hard shell-like protective outer layer to some products. As an example, the use of plasticizers that could be used in these films include sorbitol, xylitol, mannitol, and glycerol. Edible coatings might also increase the flavor and appearance of the product, for example, the waxes are used to add a glossy appearance on lemons, oranges, and apples, and at the same time, they reduce wilting of the product due to a moisture barrier (Han et al., 2005; Mei et al., 2002; Pascall and Lin, 2013).

7.2  Examples of Wet (Casting, Roll Drying) and Dry Processes (Extrusion, Coextrusion) for Edible Film Production The wet and dry processes are two groups of methods for edible film production. The wet process requires solvents for the solution and dispersion of the polymer onto a flat surface, continuing with drying under controlled conditions in order to remove the solvent and allowing the formation of the film. This method is adequate for laboratories but not for industrial scale-up due to high-energyconsuming. The production of edible films by drying methods includes the most commonly used: extrusion, injection, blow-molding, and heatpressing processes (Han and Aristippos, 2005; Silva-Weiss et al., 2013). Both the efficiency

Basic and Applied Concepts of Edible Packaging for Foods  43 and high productivity provided by these processes increased the application for active edible film production (Lopez et al., 2014). On the other hand, the high temperatures used in the drying process might alter the quality, presence, and amount of an active compound on the films (Silva-Weiss et al., 2013), when in fact the addition of plasticizers is sometimes necessary to decrease the glass-transition temperature for polymer matrices. Hence, it is very important that the method selected to obtain the edible films might change the final characteristics of the material. Casting, as a wet process, is a simple method to obtain edible films, but it is a batch procedure used on a very small scale. However, a continuous casting method can be used on the industrial scale (Espitia et al., 2014a) because the film-forming suspension is prepared on continuous carrier tapes with thickness controlled. The film is dried by heat conduction, convection, or radiation in short times. The tape casting is an appropriate technology for cassava-starch edible films (De Moraes et al., 2013). Mainly, the wet process is divided into four steps: dispersion, homogenization, casting, and drying. Various factors, such as a plasticizer, granule disruption, the temperature, and the time, influence and should be optimized depending on the polymer matrix, solvent, plasticizer, and/or other additive contents (Jimenez et al., 2012). In order to obtain stable emulsions and homogeneous films, several mixing steps must be applied. Homogenization is done right away by homogenizer devices (Bahram et al., 2014; Maniglia et al., 2014; Matsakidou et al., 2013; Razavi et al., 2015; Salarbashi et al., 2014; Shen and Kamdem, 2015; Shojaee-Aliabadi et al., 2014). Since the final product should be edible and biodegradable, only ethanol and water or a combination of both are adequate solvents (Campos et al., 2011; Han and Aristippos, 2005). All the ingredients of the film’s solutions should be homogeneously combined in the solvent in order to produce the film without separation of phases. There are other components that can be added to the formulation so that separation of phases does not occur; they are called emulsifiers (Albertos et al., 2015; Bahram et al., 2014; Salarbashi et al., 2014; Shen and Kamdem, 2015). These emulsifiers are food-grade plasticizers rich in hydroxyl groups, such as glycerol, sorbitol, or poly (ethylene glycol, PEG). The components mentioned reduce the polymer rigidity and glass transition temperature and enhance the homogeneity of the formulation. Recently, the use of essential oils extracted from plants has gained importance as ingredients of edible films formulating. These extracts have bioactive compounds that give the films specific characteristics. There are different techniques that facilitate the addition of active compounds in water-soluble polymers, such as casting method (Bahram et al., 2014; Li et al., 2014; Liakos et al., 2014; Perazzo et al., 2014; Salgado et al., 2013; Souza et al., 2013; Teixeira et al., 2014), nanoemulsions by ultrasonication (Otoni et al., 2014b) and encapsulation through nanoliposomes by sonication of aqueous dispersions (Jiménez et al., 2014; Wu et al., 2015).

44  Chapter 1 There are some studies related to this issue. Otoni et al. (2014a) prepared coarse emulsions and nanoemulsions with clove oil through low-speed mixing and ultrasonication, respectively, using emulsifiers for homogenization in water. The results for these emulsions into methylcellulose matrices plasticized with polyethylene glycol showed that the droplets size reduction provided higher antimicrobial properties. Nevertheless, there are some negative effects on the mechanical properties observed with the addition of EO emulsions. On gelatin films with nanoliposomes an increase in the antimicrobial stability with a decrease in the cinnamon, EO release rate was observed. A widely used method for the incorporation of EOs into the film solutions with low temperatures is casting. As an example, cinnamon O increased the antimicrobial activity of whey-protein concentrate, as well as the water permeability and water solubility (Bahram et al., 2014). Other authors added lignin to gelatin matrices by casting; the films produced had excellent antioxidant and light barrier properties that prevent the lipid oxidation in certain food applications (Nuñez-Flores et al., 2013), unfortunately, they did not use any emulsifiers, having a microphase separation. Maniglia et al. (2014) developed turmeric flour films with antioxidant properties by casting. Despite this, the air bubbles frequently form due to the homogenization step, and vacuum (Badr et al., 2014; Hosseini et al., 2013; Pan et al., 2014) or ultrasound (Albertos et al., 2015; Li et al., 2014) devices are used to eliminate them. After homogenization, the film solution is cast on leveled dishes and allowed to dry under controlled conditions. An important issue to mention is that depending on the polymer, different materials, such as polystyrene (Salarbashi et al., 2014; Salgado et al., 2013) polyethylene (Razavi et al., 2015), polycarbonate (Perazzo et al., 2014), methacrylate (Li et al., 2014; Otoni et al., 2014a), and glass (Badr et al., 2014; Bahram et al., 2014; ShojaeeAliabadi et al., 2014) have been used to obtain films by casting. Other surfaces, such as stainless steel, silicone (De Moraes et al., 2013), and polytetrafluoroethylene (Abdollahi et al., 2012; Pastor et al., 2013) have also been considered for their high inertness. The temperature used for film forming varies between 20 and 50°C and the time varies from 5 to 75 h. Blending is another method used to obtain edible films; it consists of mixing different macromolecules and applying a codrying process. Recent studies on blending various matrices to produce edible films have focused on the combination of polysaccharides with proteins, due to their synergetic effect (Arancibia et al., 2015; Hosseini et al., 2013; Jiménez et al., 2014; Jridi et al., 2014; Pan et al., 2014). This method consists of an initial preparation stage of individual polymer solutions followed by homogenization and casting. The codrying method requires strict conditions, such as a narrow concentration range and good compatibility (Pan et al., 2014). One of the most used biopolymers in production of edible films (Van den Broek et al., 2015) is chitosan. The mixing of protein concentrate solutions with chitosan considerably changes

Basic and Applied Concepts of Edible Packaging for Foods  45 the structure and leads to the reinforcement of the chitosan matrices. All this supplies their barrier, antimicrobial, and antioxidant properties (Arancibia et al., 2015). Edible films of chitosan and gelatin (Hosseini et al., 2013; Jridi et al., 2014) or methylcellulose (Pastor et al., 2013) have been developed to enhance the barrier, mechanical properties, and to obtain antimicrobial activity against Gram-negative bacteria. The chitosan-gelatin films have presented antioxidant activity as monitored by β-carotene bleaching and 2,2-diphenyl-1picrylhydrazyl (DPPH) radical scavenging (Jridi et al., 2014). Recently, different polysaccharides (Pastor et al., 2013; Paula et al., 2015; Zhu et al., 2014) or proteins (Song et al., 2014), blendings formed composite edible films (Table 1.1). As an example, the resveratrol, an active compound, was efficiently added into methylcellulose and chitosan blends. This active compound provided antioxidant activity with physical changes that did not affect negatively the handling and appearance of the films (Pastor et al., 2013). Another good application is the incorporation of clove EO into gelatin-chicken feather protein blended films improved the antimicrobial and antioxidant properties without affecting its mechanical characteristics (Song et al., 2014). A wet-processing method used for coating production is spraying. The film-forming solution is sprayed onto the surface where it will be applied. The solvent evaporates after it passed the nozzle of the sprayer, and then it is allowed to dry for a certain time (Espitia et al., 2014a). Dry processing is known as a process where materials with thermoplastic behavior can be processed into films by applying various thermal–mechanical processing techniques. So, it is important to study the rheological properties and the effect of additives on the thermoplastic behavior of film-forming materials to choose the best processing conditions. There are other dry-processing methods that are frequently used to obtain edible films and these are extrusion, injection, blow molding, and heat pressing. Some advantages can be mentioned regarding to this technique, which include the absence of solvents, the easy handling of high viscocity polymers, a broad range of processing conditions, and multiple injections, where a pair of rotating screws produce pressure and high temperature to break the granules of polymer and homogenized the mixture of ingredients (Liu et al., 2009). A mixture of sodium caseinate (NaCas) containing lysozyme was obtained and prepared as pellets with extrusion using glycerol as plasticizer. The pellets were blown by an industrial blown film extruder in order to produce thermoplastic antimicrobial films (Colak et al., 2015), further processed into transparent films with a classical film-blowing machine. The films obtained showed mechanical properties similar to the ones obtained by casting methods. A method to improve film efficiency is lamination. This method consists on the formulation of multilayered structures and the combination of characteristics of various ingredients into a sheet. An advantage of these multilayered films compared to a single layered film is a higher

46  Chapter 1 toughness and tensile strength. Despite this advantage, this method is complex and solvent consuming at high temperatures and time, so it increases the production costs (Martucci and Ruseckaite, 2010; Pan et al., 2014). An example of a three-layer film produced by the heat compression of dialdehyde crosslinked starch and plasticized gelatin films as outer layers and plasticized gelatin sodium composite films as an inner layer provided a multilayer biodegradable film with a compact structure and reinforced properties (Martucci and Ruseckaite, 2010). Other bioactive three-layer films were produced with poly(e-caprolactone) as an external layer and methylcellulose with essential oil encapsulated as the internal layer (Takala et al., 2013). Another method to improve the properties in active edible films of chitosan is by the use of electric fields (Perazzo et al., 2014; Souza et al., 2013).

7.3 Conclusions Edible films and coatings have been considered to be important due to their properties and good performance in food packaging, biomedical, and other applications as carriers for active compounds. Research in this area has greatly increased in the last few years, but some issues are still to be solved in order to be used in upscaling in the packaging of food, especially difficulties in processing because most of the recent research has been applied with wet methods. However, even the difficulties in up-scaling the laboratory research to the industrial applications, which is still under various studies, the use of edible films or coatings are sustainable alternatives in active food packaging or biomedical systems instead of conventional plastic packages. Hopefully, in a few years they could be in potential use.

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Further Reading Rojas Marzo, 2010. Efecto del tipo de aceites esenciales sobre las propiedades mecánicas y barrera de películas comestibles basadas en zeína. Escuela Técnica Superior de Ingenieros Agrónomos, Universidad Pública de Navarra, Junio. Suput, D.Z., Lazic, V.L., Popovic, S.Z., Hromis, N.M., 2015. Edible films and coatings: sources, properties and application. Food Feed Res. 42, 11–22. Volpe, M.G., Siano, F., Paolucci, M., Sacco, A., Sorrentino, A., Malinconico, M., Varricchio, E., 2015. Active edible coating effectiveness in shelf-life enhancement of trout (Oncorhynchusmykiss) fillets. LWT—Food Sci. Technol. 60, 615–622. Wan, J., et al., 2015. Optimization of instant edible films based on dietary fiber processed with dynamic high pressure microfluidization for barrier properties and water solubility. LWT—Food Sci. Technol. 60 (1), 603–608, Available from: http://www.sciencedirect.com/science/article/pii/S0023643814004630. Zaritzky, N., 2007. Películas biodegradables y recubrimientos comestibles a base de hidrocoloides: caracterización y aplicaciones. Centro de Investigaciones y Desarrollo en Criotecnología de Alimentos (CIDCA). UNLP– CONICET.