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Critical Reviews in Food Science and Nutrition

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Recent Advances in Edible Coatings for Fresh and Minimally Processed Fruits

Maria Vargas a; Clara Pastor a; Amparo Chiralt a; D. Julian McClements b; Chelo Gonzlez-Martnez a a Department of Food Technology-Institute of Food Engineering for Development, Universidad Politcnica de Valencia, Valencia, Spain b Biopolymers and Colloids Research Laboratory, Department of Food Science, University of Massachusetts, Amherst, MA, USA

To cite this Article Vargas, Maria, Pastor, Clara, Chiralt, Amparo, McClements, D. Julian and Gonzlez-Martnez,

Chelo(2008) 'Recent Advances in Edible Coatings for Fresh and Minimally Processed Fruits', Critical Reviews in Food Science and Nutrition, 48: 6, 496 511 To link to this Article: DOI: 10.1080/10408390701537344 URL: http://dx.doi.org/10.1080/10408390701537344

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Critical Reviews in Food Science and Nutrition, 48:496511 (2008) Copyright C Taylor and Francis Group, LLC ISSN: 1040-8398 DOI: 10.1080/10408390701537344

Recent Advances in Edible Coatings for Fresh and Minimally Processed Fruits
MARIA VARGAS,1 CLARA PASTOR,1 AMPARO CHIRALT,1 D. JULIAN McCLEMENTS,2 and CHELO GONZALEZ-MARTINEZ1
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Department of Food TechnologyInstitute of Food Engineering for Development, Universidad Polit cnica de Valencia, e Camino de Vera s/n, 46022, Valencia, Spain 2 Biopolymers and Colloids Research Laboratory, Department of Food Science, University of Massachusetts, Amherst, MA 01003, USA

The development of new edible coatings with improved functionality and performance for fresh and minimally processed fruits is one of the challenges of the post harvest industry. In the past few years, research efforts have focused on the design of new eco-friendly coatings based on biodegradable polymers, which not only reduce the requirements of packaging but also lead to the conversion of by-products of the food industry into value added lm-forming components. This work reviews the different coating formulations and applications available at present, as well as the main results of the most recent investigations carried out on the topic. Traditionally, edible coatings have been used as a barrier to minimize water loss and delay the natural senescence of coated fruits through selective permeability to gases. However, the new generation of edible coatings is being especially designed to allow the incorporation and/or controlled release of antioxidants, vitamins, nutraceuticals, and natural antimicrobial agents by means of the application of promising technologies such as nanoencapsulation and the layer-by-layer assembly. Keywords Edible coatings, fruits, biopolymers, composites, micro- and nanoencapsulation, multilayered structures

INTRODUCTION The application of edible coatings is one of the most innovative methods to extend the commercial shelf-life of fruits by, among other mechanisms, acting as a barrier against gas transport and having a similar effect on the storage under controlled or modied atmospheres (Park, 1999). Two of the most important advantages of this technology are the reduction of synthetic packaging waste and the incorporation of preservatives and other functional ingredients into biodegradable raw materials obtained from natural sources. The latter is in response to the growing demand for safe, healthy foods as well as to the increasing concerns over the environment. When developing edible coatings, the classical approach has been to characterize their properties when they are cast and then peeled off from a plate. This approach can be very useful to
Address correspondence to Chelo Gonz lez-Mart a inez, Department of Food Technology, Institute of Food Engineering for Development, Universidad Polit cnica de Valencia, Camino de Vera s/n, 46022, Valencia, Spain. Telephone: e 0034 96 387 93 62 Fax: 0034 96 387 73 69. E-mail: cgonza@tal.upv.es

compare coatings, but an important weakness is that it does not take into account the interaction between a coating and a fruit surface and its subsequent inuence on coating properties. Thus, it is of interest to gather some of the available methodologies that are used to characterize coated fruits and to discuss their limitations and signicance. This paper reviews some of the most recent advances in the application and development of edible coatings for fresh and minimally processed fruits, focusing on the main methodologies available to characterize coated commodities, in order to set the basis to obtain new and highly functional edible coatings by introducing some of the techniques that have not yet been used in food science. EDIBLE COATINGS: DEFINITIONS AND REGULATORY STATUS Edible coatings may be dened as a thin layer of material that covers the surface of the food and can be eaten as part of the whole product. The composition of edible coatings must

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therefore conform to the regulations that apply to the food product concerned (Guilbert et al., 1995). According to the European Directive (ED, 1995; 1998) and the USA Code of Federal Regulations (FDA, 2006) edible coatings are those coatings that are formulated with food-grade additives. According to what the USA Code of Federal Regulations states about their application to fresh citrus fruits, the amount of edible coating ingredients used must be only that which is necessary to accomplish the intended effect, and the ingredients have to be GRAS and be listed in the above-mentioned Code. Among the ingredients that can be incorporated into the formulation of edible coatings, the European Directive (1995; 1998) includes the following: arabic and karaya gum, pectins, shellac, beeswax, candelilla wax, and carnauba wax. This Directive was modied in 1998 by introducing new ingredients such as lecithin, polysorbates, fatty acids, and fatty acid salts. On the other hand, the Food and Drug Administration mentions other additives used as components of protective coatings applied to fresh fruits and vegetables like morpholine, polydextrose, sorbitan monostearate, sucrose fatty acid esters, cocoa butter, and castor oil. As stated by Kester and Fennema (1986), edible coatings have to follow some functional requirements, which depend on the kind of coated product and its metabolic pathways, such as:

Sensory properties: Edible coatings must be transparent, tasteless and odourless Barrier properties: Coatings must have an adequate water vapor and solutes permeability and selective permeability to gases and volatile compounds.

Moreover, the edible coating formulations have to contain safe, food-grade substances and the cost of the technology and raw materials from which coatings are produced has to be relatively low.

COMPOSITION OF EDIBLE COATINGS FOR FRESH AND MINIMALLY PROCESSED FRUITS There is a very wide range of compounds that can be used in the formulation of edible coatings and their choice depends mainly on the target application. The major components are polysaccharides, proteins and lipids and their properties are discussed below. The minor components usually include polyols acting as plasticizers (such as glycerol) or acid/base compounds used to regulate pH (such as acetic or lactic acid). Polysaccharides Polysaccharides are the most widely used components found in edible coatings for fruits (Kester and Fernema, 1986; Krochta and de-Mulder-Johnston, 1997), as they are present in most com-

mercially available formulations. Polysaccharides show effective gas barrier properties although they are highly hydrophilic and show high water vapor permeability in comparison with commercial plastic lms. The main polysaccharides that can be included in edible coating formulations are starch and starch derivates, cellulose derivates, alginate, carrageenan, chitosan, pectin, and several gums. Table 1 shows the most relevant properties of polysaccharide-based lms, together with the permeability values of common synthetic materials used for food packaging. On the molecular level, polysaccharides vary according to their molecular weight, degree of branching, conformation, electrical charge, and hydrophobicity. Variations in these molecular characteristics will lead to variations in the ability of different polysaccharides to form coatings, as well as to variations in the physicochemical properties and performance of the coatings formed. Almost all of them are highly water soluble, so they cannot be used for coating samples that will remain immersed in a solution (for example dipped in juices) or in a high relative humidity environment. In some cases, cross-linking treatments in the presence of monovalent and divalent ions can be used to make the coatings insoluble. Starch is the natural polysaccharide most commonly used in the formulation of edible coatings because it is inexpensive, abundant, biodegradable, and easy to use. Native granular starch is converted into a thermoplastic material by conventional methods in the presence of plasticizers, such as water and glycerol (Thir et al., 2003). Coatings made from starch become brittle e in dry atmospheres and lose strength and barrier properties in high humidity (Peterson and Stading, 2005). The addition of plasticizers overcomes their exibility and extensibility (Mali et al., 2002). In addition, during storage at high relative humidity or high plasticizer content starch-based materials are in a rubbery state, which allows the development of crystallinity by increasing macromolecular mobility (Delville et al., 2003). In these conditions, retrogradation, which involves amylose and amylopectin recrystallization, does occur (Rindlav et al., 1997). Crystallites may be acting as physical crosslinking points, which generate internal stresses or cracks which in turn lead to the damage of the coatings (Delville et al., 2003), thus modifying the physicochemical properties of the starch-based material (Fama et al., 2007). Another polysaccharide that is of high interest is chitosan, obtained from the deacetylation of chitin (poly--(14)-N-acetylD-glucosamine), which is mainly obtained from crab and shrimp shells (Hirano, 1999). Films and coatings based on chitosan have selective permeability to gases (CO2 and O2 ) and good mechanical properties. However, their uses are limited mainly because of their high water vapor permeability (Butler et al., 1996; Caner et al., 1998). Moreover, chitosan shows antifungal and antibacterial properties, which are believed to be originated from its polycationic nature (Cuero, 1999; Tharanathan and Kittur, 2003), although the precise mechanism of its antimicrobial activity is still unknown (Srinivasa and Tharanathan, 2007). In addition,

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Water vapor permeability (WVP)a Others GRAS Flexible GRAS 11 1.01 62.03 0 30 7.55 0/75 25 1.12 64.19 0 30 WVP x 1011 PO2 PCO2 References Park, 1999; Kester and Fennema, 1986; Garcia et al., 2004, Pinotti, 2007 Park, 1999; Kester and Fennema, 1986; Guilbert, 2000; Hagenmaier and Shaw, 1991 Krochta, and De-Mulder-Johnston, 1997; Hagenmaier and Shaw, 1991 Peterson and Stading, 2005; Greener and Fennema, 1994; Garcia et al., 2000; Glicksman, 1983 25 Guilbert, 2000; Glicksman, 1983 Park et al., 2001; Meheriuk and Lau, 1988; Meheriuk, 1990 40.78 96 25 Gontard et al., 1996; Liu et al., 2006 Park et al., 2001; Ribeiro et al., 2007 Kester and Fennema, 1986; Greener and Fennema, 1994 RH gradient (%/%) T ( C) RH (%) T ( C) O2 /CO2 permeability (P)b Thermoplastic GRAS 10.5 217 390 360 100/50 25 0.90 15.33 93 100/50 20 74/50 23 137.5 2523.7 63.8 20 0/85 27 0.01-0.1 50 25 Brittle Fragile GRAS Antimicrobial GRAS 190 100/50 25 0.362 2.55 Fragile Good adhesion Firming agent Good adhesion 0.07-0.097 0.024 0/90 0/90 38 38 1.92 0.642 10.36 1.875 90 90 25 25 Faber et al., 2003 Faber et al., 2003

Table 1

Polysaccharides used in the formulation of edible coatings for fruits, properties of polysaccharide-based lms, and permeability of synthetic packaging materials.

Polysaccharide

Source

1 MC

(E461)

Cellulose

2 HPC

(E463)

Cellulose

3 HPMC

(E464)

Cellulose

Starch

Potato Corn

Alginate

Brown seaweeds

(E401-405) Chitosan

Crustacean shells

Pectin (E440)

Fruit Peel

Carrageenan (E407)

Red seaweeds

Gum Arabic (E414)

Acacia senegal

Guar gum (E412) Xanthan gum (E415)

Cyamopsis tetragonolobus Xanthomonas campestris Low Density Polyethylene

High Density Polyethylene

1 Methylcellulose; 2 Hydroxypropyl

cellulose; 3 Hydroxypropyl methylcellulose; a (g m1 s1 Pa1 ); b (mL.m/(m2 .d.Pa)

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the cationic nature of chitosan offers the possibility to take advantage of the electrostatic interactions with anionic polyelectrolytes, such as pectin to develop laminate coatings (Hoagland and Parris, 1996) and multilayered structures (Marudova et al., 2005; Krzemisk, 2006). Cellulose (poly--(14)-D-glucopyranose) derivatives such as methylcellulose (MC), hydroxypropylmethylcellulose and the ionic carboxymethylcellulose are also commonly found in the formulation of edible coatings, especially in commercial products. MC is formed by the alkali treatment of cellulose, followed by a reaction with methylchloride. MC is stable at a wide range of pH (211), compatible with other water-soluble polysaccharides, and being the least hydrophilic of the cellulose ethers, it would be expected to be more resistant to water transmission (Kester and Fennaema, 1986; Nisperos-Carriedo, 1994). MC is a non-ionic ether, exhibits thermal gelation, high solubility, and efcient oxygen and lipid barrier properties (Turhan and Sahboz, 2004; Bravin et al., 2004). Alginates and carrageenans can also be used to prepare edible coatings. Alginates are the salts of alginic acid, which is a linear copolymer of D-mannuronic and L-guluronic acid monomers. Alginate coating formation is based on the ability of alginates to react with di-valent and tri-valent cations such as calcium, ferrum or magnesium, which are added as gelling agents (Cha and Chinnan, 2004). Carrageenan is a complex mixture of at least ve different water-soluble galactose polymers designated as , , , and -carrageenan. Gelation of and -carrageenan occurs in the presence of monovalents or divalent cations. Carrageenan lm formation includes this gelation mechanism during moderate drying, leading to a three-dimensional network formed by polysaccharide double-helices and to a solid lm after solvent evaporation (Karbowiak et al., 2007).

Proteins Proteins that can be used in the formulation of edible coatings for fruits include those derived from animal sources, such as casein and whey protein, or obtained from plant sources like corn-zein, wheat gluten, soy protein, peanut protein, and cottonseed protein (Gennadios, 2002). Table 2 shows examples of these proteins used for coating purposes together with their main functional characteristics. Proteins exhibit a wide variety of different molecular characteristics depending on their biological origin and function. For example, proteins may vary in their molecular weights, conformations (globular, random coil, helix), electrical characteristics (charge versus pH), exibilities (rigid versus exible), and thermal stabilities. Differences in these molecular characteristics will again ultimately determine the ability of particular proteins to form coatings and the characteristics of the coatings formed. Casein based edible coatings are attractive for food applications due to their high nutritional quality, excellent sensory properties, and good potential for providing food products with adequate protection against their surrounding environment. Whey proteins have been the subject of intense investigation over the past decade or so. With the addition of plasticizer, heat-denatured whey proteins produce transparent and exible water-based edible coatings with excellent oxygen, aroma, and oil barrier properties at low relative humidity. However, the hydrophilic nature of whey protein coatings causes them to be less effective as moisture barriers. Proteins that are insoluble in water, such as corn zein and wheat gluten, produce insoluble coatings, whereas proteins that are soluble in water produce coatings of varying solubility, depending on the protein and the conditions of coating formation and treatment (Krochta, 2002). For example, whey protein

Table 2

Proteins used in the formulation of edible coatings for fruits and properties of protein-based lms. Water vapor permeability (WVP)a O2 /CO2 permeability (P)b PO2 0.25 1.88 RH T PCO2 (%) ( C) References 1.13 46.88 60 91 20 25 Park, 1999; Gennadios and Weller, 1990; McHugh and Krochta, 1994; Bai et al., 2003 Gontard et al., 1996; Gontard et al., 1992; Guilbert et al., 1996; Hern ndez-Mu oz et a n al., 2004 Gennadios and Weller, 1991; Cho and Rhee, 2004; Cho et al., 2007 Krochta, and De-Mulder-Johnston, 1997; McHugh and Krochta, 1994; McHugh and Krochta, 1994; McHugh and Krochta, 1994, Mei and Zhao, 2003; Mat et al., 1996 e Guilbert et al., 1996; Dangaran et al., 2006; Khwaldia et al., 2004

Protein Zein Gluten

Source Corn Wheat

Others GRAS Fragile

WVP 1011 8.913.2 4.3

RH gradient (%/%) 0/85 0/50

T ( C) 21 23

Soy Whey proteins

Soybean Flexible Milk Flexible

354 417

100/50 100/55

25 25

0.067 0.001- 0.01

50 50

25 25

Sodium caseinate Milk

Brittle

42.5

0/81

25

0.76

4.56

77

25

a (g

m1 s1 Pa1 );b (mL.m/(m2 .d.Pa); *with plasticizer

500
Table 3

M. VARGAS ET AL.
Lipids used in the formulation of edible coatings for fruits and properties of lipid-based lms. Water vapor permeability (WVP)a O2 /CO2 permeability (P)b

Lipid Shellac (E904) Beeswax (E901) Insects

Source

Others

WVP 1011

RH gradient (%/%) 0/100 0/100 0/100 0/100 12/56

T ( C) 30 25 25 25 23

PO2 0.083 0.092 0.537 0.016

RH T PCO2 (%) ( C) References 0.29 2.04 60 0 60 0 20 25 30 25 Bai et al., 2003; Hagenmaier and Baker, 1995; Hagenmaier, 2000 Hagenmaier and Baker, 1997 Guilbert, 2000; Hagenmaier and Baker, 1997; Bai et al., 2003 Guilbert, 2000; Martin-Polo et al., 1992 116; 151; Martin-Polo et al., 1992; Martin-Polo et al., 1992

GRAS 0.4620.66 GRAS GRAS GRAS 0.058 0.017 0.033 0.223.47

Beeswax

Candelilla wax (E902) Plant exudates Carnauba wax (E903) Fatty acids (E471) Plant exudates

Plant or animal material GRAS

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a (g

m1 s1 Pa1 ); b (mL.m/(m2 .d.Pa).

isolate produces totally water-soluble coatings but heatdenatured solutions of whey protein isolate produce coatings in which the protein is insoluble (Perez- Gago et al., 1999). Moreover, protein solubility is considered to be dependent on the pH, so this parameter should be taken into account during the formulation and application of coatings. Only if the proteins have been denatured, does solubility becomes unimportant. Lipids Edible lipids used to develop edible coatings are shown in Table 3 and include beeswax, candelilla wax, carnauba wax, triglycerides, acetylated monoglycerides, fatty acids, fatty alcohols, and sucrose fatty acid esters. Edible resins include shellac and terpene resin. Lipid-based edible coatings have a low afnity for water, which explains why they have low water vapor permeability. The latter is extremely important, as a great number of studies deal with the use of coatings on fresh fruits and vegetables to control their desiccation (Morillon et al., 2002). Due to the fact that each hydrophobic substance has its own physicochemical properties, each lipid-based edible coating behaves in a different way as regards moisture transfer. The polarity of lipid constituents has to be considered, that is to say, the distribution of electrostatic potentials on the molecules that depends on the chemical group, aliphatic chain length, and on the presence of unsaturation. As the carbon number of fatty alcohols and fatty acids increases (from 14 to 18), so does their effectiveness to act as moisture barriers, because the non-polar part of the molecule increases and therefore favors neither water solubility in the lm nor, as a consequence, moisture transfer across the lm (Morillon et al., 2002). Composites The main disadvantage of lipid based coatings is their poor mechanical properties, and thus, at present, research efforts are

focused on the design of composite coatings that are based on both lipids and hydrocolloids (proteins or polysaccharides) to take advantage of the special functional characteristics of each group, thereby diminishing their drawbacks (Greener and Fennema, 1994). Generally, lipids contribute to the improvement of the water vapor resistance whereas hydrocolloids confer selective permeability to O2 and CO2 , as well as durability, structural cohesion, and integrity (Krochta, 1997). Composite coatings can be created by the subsequent deposition of different layers (multilayered coatings) or can be made by the deposition of a single layer of material. Bilayer coatings are formed in two stages: In the rst stage the layer of polysaccharide or protein is cast and dried and in the second one, the lipid layer is applied (Krochta, 1997). As an example, Debeaufort et al. (2000), developed bilayers by adding a mixture of lipids (parafn oil, parafn wax, or a mixture of hydrogenated palm oil and triolein) onto a methylcellulose layer. Wong et al. (1994), coated apple cubes with double layers of polysaccharides (cellulose, carrageenan, pectin, or alginate) and acetylated monoglyceride. Nevertheless, in monolayer composite edible coatings, the lipid is dispersed in the hydrophilic phase of an emulsion (Shellhammer and Krochta, 1997). Bertan et al. (2005), used stearic and palmitic acid to allow the incorporation of a hydrophobic exudate into a gelatine-based coating. This mixture was emulsied using triacetin as plasticizer. Bosquez-Molina et al. (2003), obtained emulsied coatings by mixing mesquite gum (structural matrix) and a combination of some lipids (candelilla wax, mineral oil, oleic acid, or beeswax). Emulsied coatings are less efcient than bilayers due to the non-homogeneous distribution of lipids but they have received more interest because they need only one drying step instead of the two necessary for the bilayer lms, and they can be applied on food at room temperature. Moreover, being both, hydrophilic and lipophilic, allows them to adhere to any support, whatever its polarity, and to exhibit good mechanical resistance (QuezadaGallo et al., 2000).

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CHARACTERIZATION OF COATED FRUITS The use of edible coatings to extend the shelf-life and improve the quality of fresh and minimally processed fruits has come under examination during the past few years due to their ecofriendly and biodegradable nature. Moreover, these outer layers can provide a supplementary and sometimes essential means of controlling physiological, morphological, and physicochemical changes in fruits. The effectiveness and functionality of each coating depends on their physicochemical and barrier properties, which are very often closely related with the molecular arrangement of the different components of the coating, that is, its microstructure. The coating is usually characterized and afterwards, the properties are correlated with those observed in the coated fruit, however, sometimes, these coating properties are affected by the fruit surface during its application. On the other hand, after the coating has been applied, the fruit response has to be analyzed and therefore, the characterization of the coated fruit becomes an important task. The most important properties to be measured when characterizing coated fruits are the following. Thickness and Microstructure The thickness of the edible coatings is directly related with other important properties such as permeability to gases. The coatings that are obtained by casting and drying on levelled plates can be pealed off and their thickness can be easily measured by using a hand-held micrometer. However, it is difcult to measure the thickness of coatings accurately once they have been applied to the fruit surface. In these cases, an estimation of the coating thickness can be obtained by means of the quantication of the surface solid density, SSD (Villalobos et al., 2004; Vargas et al., 2006; 2006b) (Eq. 1). SS D = M Fa X s As (1)

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skin of most fruits covered with a natural wax layer (Choi et al., 2002). One of the most promising, recent techniques that could be potentially used to determine the thickness of coatings is spectroscopic ellipsometry. This technique has been used for the characterization of lms and multilayered structures (Schram et al., 2000), although, to the best of our knowledge, it has not yet been used in edible coatings. An ellipsometer shines linearly polarized light on the sample surface and then the ellipticity of the light reected off the sample surface is analyzed. The principle of the method is based on the determination of the complex reectance ratio of the reection coefcient of light, polarized both parallel and perpendicular to the plane of incidence. The spectroscopic ellipsometry data are interpreted by tting the calculated ellipsometric response of an optical model of the presumed surface structure to the experimental data by means of a least-squares regression analysis (Zuber et al., 1995; Jellison, 1996). The data are measured over the entire wavelength range and compared to the mathematically generated model to obtain the lm thickness and the refractive index of the coating. On the other hand, different kinds of microscopy techniques (e.g. confocal, Scanning Electron Microscopy, Atomic Force Microscopy, etc.) can be used not only to measure the thickness of the coating but also to characterize the surface roughness and topography of coated fruits (Hershko and Nussinovitch, 1998). Moreover, the analysis of coating microstructure plays an important role in reaching a better understanding of the important coating properties like permeability to gases and resistance to water vapor transmission. Water vapor resistance The direct measurement of the products permeability to water vapor exchange under controlled environmental conditions would make it possible to determine in situ if the coating shows the required properties for a specic combination of storage conditions (Amarante and Banks, 2001). Thus, the water vapor resistance (WVR) of coated fruits can be obtained by monitoring the weight loss of samples both at a controlled temperature and under controlled relative humidity conditions and expressed by using Equation 2 (Wong et al., 1994; Vargas et al., 2006; 2006b; Avena- Bustillos et al., 1994; 1997; Pastor et al., 2005). WV R = aw
%R H 100

The mass fraction of solids (Xs ) of each lm-forming solution has to be considered to calculate SSD as well as the mass of the coating solution adhered to the fruit surface (M Fa ), which can be calculated by weighing the fruits before and after coating application. The estimation of the average sample area (As ) sometimes requires the use of image analysis techniques or volumetric and surface area measurements; the more irregular the shape of the fruit, the more complicated these measurements become. Films thickness can be also dened in terms of coating solution properties such as viscosity, density, draining time, and the solid concentration of the original solution. In addition, as stated by Cisneros-Zevallos and Krochta (2003), surface tension effects can play a major role in the nal thickness, especially when considering a high or medium hydrophobic surface (low or medium surface energy), like the

Pwv

RT

As J

(2)

where J , is the slope of the weight loss curve in stationary conditions, As , is the sample area, aw , the water activity of samples, Pwv , the saturated vapor pressure, T , the absolute temperature, and R, the universal constant of gases. One of the problems that arises when using this methodology is how to measure the sample area accurately. This area can be tailored and easily determined in fresh-cut fruits but can be particularly difcult to measure in irregular-shaped whole fruits.

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An indirect method of determining the water vapor permeability of coated fruits is to form a coating by casting and drying on a plate and measure its water vapor permeability by standard methods based on gravimetric techniques (ASTM, 1995). Numerous studies have used this technique to characterize the permeability properties of a wide variety of edible coatings (Gennadios et al., 1994; McHugh and Krochta, 1994; 1994b; 1994c; Avena-Bustillos et al., 2006; Clasen et al., 1996; Villalobos et al., 2006). However, it must be pointed out that these values are useful for comparing different formulations, but that the permeability properties of coatings could be altered when they are applied to a real fruit surface. For instance, they can be modied because of a partial absorption of the barrier layer by the fruit surface or, in the case of emulsied coatings, by a heterogeneous lipid distribution due to surface irregularities (Morillon et al., 2002). Thus, it is always recommended that measurements be taken on the coated fruit. Gas Permeability The gas permeability of coatings can be evaluated by measuring the internal composition of coated fruits, generally in terms of O2 and CO2 concentration, as well as some important volatile compounds such as ethanol and acetaldehyde, which play an important role in the metabolism of coated fruits. The internal atmosphere of the coated fruits is typically measured by withdrawing samples from the core of the fruit with a syringe and injecting them in a gas chromatograph (Chen and Nussinovitch, 2001). Salveit (1982) used a partial vacuum procedure for extracting internal gas samples from fruits and vegetables, previously submerged in a saturated salt solution. As the pressure is reduced, internal gases expand, and there is a mass ow of gas out of the fruit through the lenticels, stomata, pores, and other regions of low resistance. Gasses dissolved within the tissue will come out of solution as the vacuum is applied. Appropriated gas samples can be removed after the pressure is returned to normal and injected into the gas chromatograph. This methodology has been applied to coated fruits and vegetables by several authors (CisnerosZeballos and Krochta, 2003; Avena Bustillos et al., 1994). Alternatively, changes in the internal composition of coated fruits can be determined by measuring their respiration rate. To this end, fruits are stored in a tightly-sealed glass container, and the headspace is sampled at different time intervals in order to analyze CO2 and O2 content by using gas chromatography (Wong et al., 1994; Vargas et al., 2006; 2006b; Pastor et al., 2005; Jiang and Li, 2001; Maftoonazad and Ramaswamy, 2005; Lee et al., 2003). Appearance: Color and Gloss Many studies have focused on the study of color, opacity and gloss of edible coatings (Nussinovitch et al., 1996; Ward and Nussinovitch, 1996; Trezza and Krochta, 2000; 2000b; 2001). The changes in fruit color caused by coating application can be measured by means of colorimeters, which calculate chro-

matic parameters such as luminosity, chroma, and hue, from the reection spectra of samples, considering a standard observer/illuminant system (Hutchings, 1999). The differences in luminosity differences can be related with changes in the reectance properties of samples after coating is applied. On the other hand, the gloss of the coated fruits can be measured using a at surface glossmeter. The results are reported in gloss units (from 0 to 100) relative to a highly polished planar surface of black glass, which serves as a standard and is usually arbitrarily assigned with a gloss value of 100. The use of this technique is limited to planar samples obtained from the coated fruit peel. Following this procedure, Chen and Nussinovitch (2001) measured gloss in strips of mandarin peel that were coated with hydrocolloids (xanthan or locust bean gum) and wax.

Other Properties In terms of coating application, it is essential to know properties related with wettability, such as surface free energy, the interfacial tension between the coating solution and the surface of the coated fruit, as well as the contact angle (Choi et al., 2002; Hershko and Nussinovitch, 1998; 1998; Wong et al., 1992). These parameters are mainly determining the amount of liquid that adheres to the surface and so, the nal thickness of the lm on the fruit. In this sense, Cisneros-Zevallos and Krochta (2003) found that the average liquid lm thickness on coated apples was a function of viscosity, draining time, density of the biopolymer solutions, surface tension of fruit, surface tension of liquid, and the surface roughness. In order to perform contact angle measurements, specimens must be planar in nature (e.g. fresh-cut fruit slices). Thus, when performing the measurements on whole fruits, the coated-peel has to be cut into small pieces and if possible, xed on a planar surface. On the other hand, it is important to ensure that the coatings have as little impact as possible on the sensory quality of coated fruits in terms of color, gloss, basic tastes (bitterness, sourness, and sweetness), aroma, and rmness. The evaluation of the sensory attributes of coated fruits is usually performed by means of descriptive analysis (Eswaranandam et al., 2006) or consumer and free-choice proling panels (Han et al., 2005). In some cases, especially when incorporating lipids into coatings, consumers reject the samples because of their articial color and waxy appearance (Han et al., 2005; Tanada-Palmu and Grosso, 2005). Finally, it should be mentioned that the changes in the internal atmosphere of coated fruits and the subsequent delay in their metabolism are also reected in their mechanical properties. The latter are generally evaluated via compression assays carried out using an Instron Universal Testing Machine or a Texture Analyzer. Firmness or resistance to fracture are the most commonly reported parameters when evaluating the quality of stored coated fruits (Vargas et al., 2006; Tanada- Palmu and Grosso, 2005; Del-Valle et al., 2005).

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APPLICATION OF EDIBLE COATINGS TO FRESH AND MINIMALLY PROCESSED FRUITS Edible coating technology is a promising method to preserve the quality of fresh and minimally processed fruits. Research and development efforts are leading to an improvement of the functional characteristics of the coatings, which depends on the properties of the fruit to be preserved or enhanced. These can be achieved by a precise optimum control of gas permeability, texture, and color changes by means of quantitative or qualitative changes in coating formulation. Table 4 shows some of the formulations that have already been applied to fresh fruits. It should be mentioned that cellulose derivatives are incorporated in most commercial products such as Semperfresh (AgriCoat Industries Ltd., Berkshire, UK), Pro-long (Courtaulds Group, London), Nature-Seal (Ecoscience Product System Divison, Orlando, FL), and Natural Shine 9000 (Pace Internacional, Seattle, USA) among others. Edible coatings can affect the quality of coated fruits in several different ways, since there are many mechanisms involved. These mechanisms include controlled moisture transfer between the fruit and the surrounding environment, the controlled release of chemical agents like antimicrobial substances, avor compounds, and antioxidants; the reduction of the internal oxygen partial pressure with a decrease in fruit metabolism, as well as some kind of structural reinforcement (Shaidi et al., 1999). Therefore, some of the effects that can be observed in coated fruits during storage are a reduction in respiration rate (Wong et al., 1994; El Gaouth et al., 1991), a decrease in weight loss (Baldwin et al., 1999), a delay in the occurrence of enzymatic browning (Baldwin et al., 1999; McHugh and Senesi, 2000; La Tien et al., 2001) and, in general, a signicant extension of fruit shelf-life. Nowadays, there is a new generation of edible coatings that is being applied to minimally processed (MP) fruits, which are those fruits that have been cut, peeled and/or slightly processed to be ready to eat but show a quality and freshness similar to the fresh product, still having living tissues (Perez, 2003). Some examples of the application of these coatings to MP fruits are shown in Table 5. The main problem when applying the coatings to MP fruits is the low adherence presented by the highly hydrophilic cut surface of the fruit, as it remains wet for a long time and also because of the possible presence of liquid exudates. As a consequence, the drying process of the coating on the fruit surface slows down (if drying is possible) and a partial loss of coating integrity could occur. As regards the commercial coatings tested on MP fruits, the use of Nutrisave (Nova Chem, Halifax, NS, Canad ) should be a mentioned. This is a chitosan derivative that has been applied to MP pears and apples, subsequently reducing the respiration rate and weight loss signicantly, and delaying microbial decay (Baldwin et al., 1995). It is also interesting to point out the application of edible coatings as a pre-treatment in osmotic processes carried out to

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obtain minimally processed fruits. In osmotic dehydration a cellular tissue is immersed in a concentrated solution of sugars or salts to promote water loss in the cells due to differences in water chemical potential established between the external solution and the internal liquid phase of the cells. Nevertheless, a diffusion of external solutes and hydrodynamic gain of the external solution also occur (Chiralt and Fito, 2003; Chiralt and Talens, 2005). Edible coatings can be used in order to control extensive solute uptake while having no serious negative effect in water removal (Lenart and Piotrowski, 2001). In this sense, Lenart and Dabrowska (1999) coated apple slices with pectin based coatings prior to osmotic dehydration, thus obtaining a better dehydration efciency with the lowest solute gain by using low methoxyl pectin coatings. Similar results were obtained by Matuska et al. (2006) in strawberries coated with different concentrations of sodium alginate, carrageenan, or guar gum solutions before osmotic dehydration.

IMPROVEMENT OF FUNCTIONAL PROPERTIES OF EDIBLE COATINGS The functionality of edible coatings can be improved by incorporating antimicrobial agents (chemical preservatives or antimicrobial compounds obtained from a natural source), antioxidants, and functional ingredients such as minerals and vitamins. Antioxidants are added to edible coatings to protect fruits against oxidative rancidity, degradation, and discoloration (Baldwin et al., 1995). For example, the antioxidants citric and ascorbic acid were incorporated into methylcellulose-based edible coatings in order to control oxygen permeability and reduce Vitamin C losses in apricots during storage (Ayranci and Tunc, 2004). On the other hand, the addition of chemical preservatives is of great interest for MP fruits, which have an extremely short shelf-life because of microbiological limits as well as sensory and nutritional losses that occur during their distribution and storage. Thus, the most recent investigations in the edible coating technology deal with the addition of antimicrobial agents to coating formulations. Eswaranandam et al. (2006), incorporated malic and lactic acid into soy protein coatings to extend the shelf life of fresh-cut cantaloupe melon. In the same way, edible coatings for MP fruits can contain antibrowning agents (Lee et al., 2003; McHugh and Senesi, 2000; Baldwin et al., 1996; Perez- Gago et al., 2006), and texture enhancers like CaCl2 (Wong et al., 1994; Le Tien et al., 2001). With reference to the use of natural antimicrobials, the development of coatings which use inherently antimicrobial polymers as a support matrix is very promising. For example, chitosan, which is mainly obtained from the deacetylation of crustacean chitin, is one of the most effective antimicrobial lmforming biopolymers. Chitosan is a cationic polysaccharide, which, among other antimicrobial mechanisms, promotes cell adhesion by the interaction of the positive-charged amines with

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Table 4 Coating

Application of edible coatings to fresh fruits Composition Maltodextrin, propylene glycol, fatty acid esters, sodium benzoate MC, 2 PEG, stearic acid, citric acid, ascorbic acid Parafn wax, beeswax, soybean oil; CMC from sugar beet pulp; emulgin PE, oleic acid and sodium oleate. HPMC, beeswax, shellac, estearic acid and glycerol Chitosan and Tween 80 CMC,1 Mango Apricot Peach, pear mandarin Application References Daz-Sobac et al., 1996 Ayranci and Tunc, 2004 Togrul and Arslan, 2004; Togrul and Arslan, 2004b

Polysaccharide-lipid

Plum Strawberry, grape, cherry, litchi, peach, Japanese Pear, kiwi P rez-Gago et al., 2003; Vargas e et al., 2006; Vargas et al., 2006b; El Gaouth et al., 1991; Zhang and Quantick, 1998; Devlieghere et al., 2004; Park et al., 2005; Han et al., 2004; Park and Zhou, 2004; Ribeiro et al., 2007; Du, 1997; Zhang and Quantick, 1997; Li and Yu, 2000; Romanazzi et al., 2002; Romanazzi et al., 2003 Ribeiro et al., 2007 Vachon et al., 2003 Maftoonazad and Ramaswamy, 2005 Garca et al., 1998; Garca et al., 1998 Eswaranandam et al., 2006 Bai et al., 2003 Krochta et al., 1996; Nisperos-Carriedo and Baldwin, 1994 Baldwin, 1994 Baldwin, 1994 Faber et al., 2003; Nisperos-Carriedo and Baldwin, 1993; Nisperos-Carriedo and Baldwin, 1994 Dhalla and Hanson, 1988 Faber et al., 2003; Worrell et al., 2002; Lau and Meheriuk, 1990; Lau and Yastremski, 1991; Meheriuk et al., 1991 Ribeiro et al., 2007 Faber et al., 2003; Posey et al., 2005 Faber et al., 2003 Faber et al., 2003 Alonso and Alique, 2004

Chitosan

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Carrageenan Protein-Polysaccharide Cellulose Starch Soy protein Zein SemperfreshTM

Carrageenan, glycerol and Tween 80 CMC, 3 WPI, caseinates and glycerol MC and glycerol Starch and glycerol Soy protein, glycerol, malic acid, lactic acid Zein and propylene glycol Sucrose esters of fatty acids and sodium salts of CMC Sucrose esters of fatty acids and sodium salts of CMC Sucrose esters and wax (shine) Blend of sucrose esters of fatty acids and sodium salts of CMC

Strawberry Strawberry Strawberry, avocado Strawberry Apple Apple Most fruits

Nu-Coat Flo, Ban-seel, Brilloshine TAL Pro-Long

Apple, banana, cherry, cucumber, guava, mango, melon, pear, plum Most fruits Pear

Pro-Long Nutri-Save

Sucrose polyesters of fatty acids and sodium salts of CMC N,O-carboxymethyl chitosan

Mango Apple, breadfruit, cherry, pear

Crisp Coat 868 FreshSealTM Nature-SealTM AgriCoat Food Coat

Starch Polyvinyl alcohol, starch and surfactant Composite polysaccharides Composite polysaccharides Fatty acids and polysaccharides glycol;3 Whey protein isolate.

Strawberry Fruits Pome fruit Avocado, pear, pome fruit Sweet cherry

1 Carboxymethylcellulose; 2 Polyethilene

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the negative charges in the cell membranes, causing leakage of intracellular constituents (Helander et al., 2001). Chitosan based coatings were shown to protect highly perishable fruits like strawberries, raspberries, and grapes from fungal decay (Vargas et al., 2006; El Gaouth et al., 1991; Zhang and Quantick, 1998; Romanazzi et al., 2002; Devligehere et al., 2004; Park et al., 2005). Moreover, chitosan-based edible coatings can be also used to carry other antimicrobials compounds such as organic acids (Outtara et al., 2000), essential oils (Zivanovich et al., 2005), spice extracts (Pranoto et al., 2005), lysozyme (Park et al., 2004) and nisin (Pranoto et al., 2005; Cha et al., 2003). On the other hand, some authors have incorporated natural antimicrobial compounds into protein or polysaccharide-based matrices, thereby obtaining a great variety of multicomponent antimicrobial coatings. In this sense, Seydim and Sarykus (2006) developed whey protein based antimicrobial coatings by adding oregano, rosemary, and garlic essential oils; Rojas-Grau et al. (2006), used apple puree and high methoxyl pectin combined with oregano, lemon grass, or cinnamon oil at different concentrations. However, these coatings showed their efcacy in vitro against a wide spectrum of microorganisms but they were not tested in real food systems and, as a result, there is a lack of available information about their possible impact on the aroma and avor of the coated products, which becomes more signicant when plant and herb essential oils/extracts or phenolic avors are added (Han, 2002). Thus, it is recommended to study the inuence of the incorporation of antimicrobial compounds into edible lms and coatings on sensory properties of coated commodities (Min and Krochta, 2005). Moreover, the most commonly chosen model systems when testing these kinds of coatings are sh (Min et al., 2005) or meat-based products (Janes et al., 2002; Langu and Johnson, 2005; Theivendran et al., 2006) and limited examples of fresh or MP coated fruits are available. Therefore, the direct application of natural antimicrobial coatings to whole and MP fruits is still an interesting and innovative research eld.

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Antimicrobial and antioxidant coatings have advantages over direct applications of the antimicrobial or antioxidant agents because they can be designed to slow down the diffusion of the active compounds from the surface of the coated commodity. By slowing their diffusion into coated foods, the preservative activity at the surface of the food is maintained. Thus, a smaller amount of antimicrobials/antioxidants would come into contact with the food to achieve a target shelf-life, compared to dipping, dusting or spraying the preservatives onto the surface of the food (Min and Krochta, 2005). Finally, nutraceuticals can be incorporated into the formulation of edible coatings, providing an alternative way to fortify unprocessed foods, such as fresh fruits, and encouraging their consumption. Following this approach, Han et al. (2004), improved the nutritional and physicochemical quality of strawberries and raspberries by means of chitosan-based coatings enriched with calcium and Vitamin E. In the same way, Park and Zhao (2004) incorporated high concentrations of minerals (calcium and zinc) and Vitamin E into a chitosan matrix.

FUTURE TRENDS IN THE EDIBLE COATINGS TECHNOLOGY Recent studies in this eld have focused on the development of new technologies that allow for a more efcient control of coating properties and functionality. To this end, new methodologies have been developed, most of them based on composite or multilayered systems. Nevertheless, applications to food products are still scarce. One of these new methodologies consists of the development of multilayered coatings by means of the layer-by-layer (LbL) electrodeposition (Weiss et al., 2006). LbL assembly, which is performed by alternating the immersion of substrates

Table 5 Coating

Application of edible coatings to minimally processed (MP) fruits Composition Carregeenan, pectin, cellulose, alginate, monoglycerides Fatty acids and wax WPI or HPMC, stearic acid, beeswax or carnauba wax Carrageenan glycerol, PEG 200 WPC, glycerol, CMC, CaCl2 Apple puree, ascorbic acid, citric acid, soy oil Soy protein, glycerol, malic acid, lactic acid Chitosan Composite polysaccharide Composite polysaccharide
1 WPC,

Application Fresh-cut apple cylinders Whole peeled grapefruit Fresh-cut apple pieces Fresh-cut apple cubes Fresh-cut apple Pieces. Cantaloupe melon cubes Sliced mango fuit Sliced apple Sliced banana Sliced apple Sliced banana

References Wong et al., 1994 Hagenmaier and Baker, 1997 P rez-Gago et al., 2005 e Lee et al., 2003 McHugh and Senesi, 2000 Eswaranandam et al., 2006 Chien et al., 2007 Faber et al., 2003 Faber et al., 2003

Double layer: Polysaccharide/ Lipid Microemulsion Emulsion Carrageenan Protein/ Polysaccharide Apple puree Soy protein Chitosan Nature-SealTM AgriCoat
1 Whey

protein concentrate.

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Figure 1 (a) Components that could be used to develop multilayered edible coatings for fruits and (b) example of a possible laminated coating assembled over a fruit surface.

in solutions of oppositely charged polyelectrolytes with rinsing steps, produces ultrathin polyelectrolyte multilayers on charged surfaces. A requirement for multilayer formation is that the addition of an opposite charged polyelectrolyte to a charged surface results in a charge reversal, which permits the successive deposition of oppositely charge polyelectrolytes (Krzemiski et al., 2006). Chitosan, poly-L-lysine, pectin, and alginate are the most common biopolymers that can be used in the formation of these multilayered structures (Marudova et al., 2005; Krzemiski et al., 2006; Bernab et al., 2005). It is also possible to utilize other e charged species to assemble the multilayered structures, including charged lipid droplets, solid particles, micelles, or surfactants. Examples of adsorbing substances that can be used in LbL assembly, together with a possible multilayered structure, are shown in Fig. 1. As mentioned above, the application of edible coatings to MP fruits has to face some technical problems related to the difcult adhesion of materials to the hydrophilic surface of the cut fruit. The LbL electrodeposition technique could eventually solve these problems, because even if LbL assembly has normally been applied to solid substrates, it has the potential to be applied on hydrogel surfaces (Serizawa et al., 2005). Thus, the LbL technique could be used to coat highly hydrophilic food systems such as fresh-cut fruits and vegetables. Figure 2 shows an example of how the LbL electrodeposition technique could

be used to coat a MP fruit (e.g. a fresh-cut apple slice) with a multilayered edible coating. In the near future, multilayered edible coatings will receive more attention (than single layer coatings) as they could be specially engineered to incorporate and allow the controlled release of vitamins and other functional or antimicrobial agents. A possible multilayered structure could include three layers: a matrix layer (e.g. biopolymer based) that contains the functional substance; an inner control layer to govern the rate of diffusion of the functional substance by allowing its controlled release; and a barrier layer that prevents the migration of the active agent from the coated food as well as controlling the permeability to gases. This mass transfer control can be employed, for example, to incorporate antimicrobials into edible coatings, which require a high concentration together with a very slow diffusion rate to be preserved to maintain the efciency of the antimicrobial functions against spoilage and pathogenic microorganisms (Han et al., 2002). Another promising technique that can be potentially used to incorporate functional ingredients and antimicrobials into edible coatings for fruits is micro- and nanoencapsulation. Microand nanoencapsulation is dened as a technology for packaging solids, liquids, or gaseous substances in miniature (micro and nanoscale), sealed capsules that can release their contents at controlled rates under specic conditions. Release can be solvent activated or signalled by changes in pH, temperature, irradiation, or osmotic shock. This technique is being applied more and more in the food industry since encapsulated materials can be protected from moisture, heat, or other extreme conditions, thus enhancing their stability and maintaining viability. This technique is especially suitable for incorporating ingredients that add value to the food product like enzymes and pro- and prebiotics, as well as functional ingredients that are very susceptible to lipid oxidation such as omega-3-fatty acids or to mask odors or tastes (Lopez- Rubio, 2006). Moreover, micro and nanoscale encapsulation systems seem to allow for better encapsulation and release efciency than traditional encapsulation systems. Finally, the most recent approach to improve coating properties is to make nanocomposites by incorporating nanosized clay materials such as layered silicates into biopolymer based

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Figure 2

Schematic representation of coating a MP fruit with a multilayered edible coating by using the LbL assembly with three dipping and washing steps.

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matrices. Rhim et al. (2006), incorporated different types of nanoparticles (montmorillonites, nano-silver, and silver-zeolite) into a chitosan matrix, obtaining composites with better mechanical, water vapor barrier, and antimicrobial properties than the traditional chitosan coating. Cellulose nanobers have also shown good possibilities as reinforcements in composite coatings for food packaging. However, even if these studies seem to be promising, the major concern of the scientic community when incorporating these nanomaterials into edible coatings or food is still unsolved: the lack of studies into their possible toxicity. CONCLUDING REMARKS Both, fresh and minimally processed fruits are highly perishable products and new technologies designed to extend their shelf life and ensure their safety are in demand both, in the food industry and by consumers. Edible coating technology seems to be very promising as long as consumers accept this technique as safe and friendly. Limitations mainly arise from the relatively low capability to control lm properties (since good water barrier properties are mainly provided by lipids and waxes) and the poor sensory acceptance of these lipid compounds (especially regarding their impact on color, taste, and avor rejection). New trends have focused on highly functional micro- or nanostructured, multilayered composite coatings, which are developed by using techniques that, at present, have hardly ever been applied in food systems. Future studies are expected into the development of tailormade coatings. These coatings would be designed to provide highly specic functional performances based on the selection of the most appropriate lm forming and active ingredients and assembling them in the most effective arrangement. ACKNOWLEDGEMENTS The authors acknowledge nancial support from the Spanish Ministerio de Educaci n y Ciencia by the Project AGL2004o 01009. Author M. Vargas is grateful to the Research, Development, and Innovation Ofce of the Universidad Polit cnica de e Valencia (Spain) for the concession of a grant (PAID-00-06). REFERENCES
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