Accepted Manuscript

Active hydroxypropyl methylcellulose-based composite coating powder to maintain

the quality of fresh mango

Ploy Klangmuang, Rungsinee Sothornvit

PII: S0023-6438(18)30127-0
DOI: 10.1016/j.lwt.2018.01.089
Reference: YFSTL 6853

To appear in: LWT - Food Science and Technology

Received Date: 31 October 2017

Revised Date: 30 January 2018
Accepted Date: 31 January 2018

Please cite this article as: Klangmuang, P., Sothornvit, R., Active hydroxypropyl methylcellulose-based
composite coating powder to maintain the quality of fresh mango, LWT - Food Science and Technology
(2018), doi: 10.1016/j.lwt.2018.01.089.

This is a PDF file of an unedited manuscript that has been accepted for publication. As a service to
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4 Active hydroxypropyl methylcellulose-based composite coating powder to maintain the

5 quality of fresh mango

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8 Ploy Klangmuanga and Rungsinee Sothornvita, b *

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13 Department of Food Engineering, Faculty of Engineering at Kamphaengsaen, Kasetsart

14 University, Kamphaengsaen Campus, Nakhonpathom, 73140 Thailand

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16 Center for Advanced Studies of Industrial Technology, Kasetsart University, Thailand

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20 * Corresponding author.

21 E-mail address: fengrns@ku.ac.th

22 Tel. +66 34281 098; fax: +66 3435 1404.

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25 Abstract

26 Edible composite coating powder based on hydroxypropyl methylcellulose (HPMC),

27 beeswax (BW), nanoclay and ginger oil was developed using spray-drying and freeze-drying

28 methods. The antifungal activity of the freeze-dried HPMC-based composite powder was

29 better than from spray drying. The Arrhenius equation used to accelerate shelf-life testing

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30 based on antifungal performance indicated that the shelf-life of the active coating powder was

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31 160 days at 25 °C. The active coating powder was applied on mangoes cv. Namdokmai

32 Sithong to verify its effectiveness. It is proved that the coating powder maintained the quality

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33 of the coated mangoes by reducing the weight loss, firmness loss, changes in flesh color,

34 soluble solids content and disease severity. The shelf-life of coated mangoes was extended to

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18 days at 13 °C. Therefore, coating powder of HPMC-based composite incorporated with
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36 ginger oil will reduce the loss of agricultural produce due to its antifungal activity,
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37 convenience and ease of use.

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39 Key words: Hydroxypropyl methylcellulose; mango; powder; essential oil; shelf-life

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41 1. Introduction

42 Mango is highly perishable and susceptible to various postharvest diseases which

43 limit its quality and shelf-life. In particular, anthracnose caused by Colletotrichum

44 gloeosporioides is a devastating disease that often results in massive economic losses during

45 the transportation of mango. Therefore, there is a need to explore the application of a natural

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46 antifungal edible coating to control anthracnose.

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47 Edible films and coatings based on hydroxypropyl methylcellulose (HPMC) have

48 benefited to maintain quality of fruits by reducing fruit weight loss and improving

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49 mechanical integrity. However, HPMC films and coatings constituted a poor moisture barrier

50 due to their hydrophilic biopolymers. Incorporation of lipids such as beeswax (BW) is needed

51
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to reduce water vapor permeability (WVP) of HPMC-based nanocomposite film
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52 (Klangmuang & Sothornvit, 2016b) and also lowered the weight loss of chitosan-BW coated
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53 strawberries (Velickova, Winkelhausen, Kuzmanova, Alves, & Moldão-Martins, 2013).

54 Moreover, montmorillonite (MMT), a natural reinforced nanoclay, showed good water

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55 barrier and improved mechanical properties of whey protein isolate/nanoclay composite films
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56 (Sothornvit, Rhim, & Hong, 2009). The tortuosity introduced by the dispersed nanoclay

57 (MMT) is probably the cause of a variation of the diffusion of water vapor pathway and the
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58 reduction of film water vapor permeability (Sothornvit, Hong, An, & Rhim, 2010). In

59 particular, MMT Cloisite 30B has shown antimicrobial properties against Gram-positive
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60 bacteria in chitosan films (Rhim, Hong, Park, & Ng, 2006) and it was an effective inhibitor

61 against Listeria monocytogenes in whey protein films (Sothornvit et al., 2009).

62 Ginger (Zingiber officinale) is widely used as a food additive due to the active volatile

63 oils and pungent phenol compounds known as gingerols, sesquiterpenoids and shogaols

64 (Malu, Obochi, Tawo, & Nyong, 2009). Moreover, ginger oil has proven to be effective

65 against C. gloeosporioides (Klangmuang & Sothornvit, 2012) as an alternative disease

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66 control. Therefore, HPMC-based composite coating incorporated with ginger oil might be

67 used as a natural antifungal agent to control postharvest decay and finally maintain the shelf-

68 life of fruits. However, the functional properties of active compounds and the stability of the

69 coating solution might be altered after preparation and during storage in the colloidal form.

70 Thus, a transformation of an active emulsion coating into a coating powder could offer a

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71 convenient way of use by improving stability and providing ease of storage and

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72 transportation due to the weight and volume reduction. The later application of this coating

73 powder as an emulsion coating upon dissolving the powder in distilled water might improve

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74 fruit quality and extend the shelf-life of fruits.

75 Drying methods, (spray and freeze dryings) are often used to convert colloidal

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suspensions to dried food powders. Nonetheless, different drying methods might affect the
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77 functional properties of coating powders. No studies have yet been evaluated the effect of
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78 drying methods on properties of active coating powder. Therefore, the objective of this study

79 was to determine the effect of two drying methods on the physical and antifungal properties
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80 of HPMC-based composite powder. Moreover, aqueous solution of the active coating powder
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81 was verified on the physicochemical parameters and microbial quality of fresh mango.

82
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83 2. Materials and methods

84 2.1. Materials
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85 HPMC type K4M supplied by Dow Chemical (Midland, MI, USA) was purchased

86 from Vicchi Enterprise Co. Ltd. (Bangkok, Thailand). A montmorillonite nanoclay (Cloisite

87 30B) was obtained from Southern Clay Co., Ltd. (Gonzales, TX, USA). Beeswax (BW),

88 stearic acid (SA) and glycerol (Gly) were obtained from Fluka Co. Ltd. (Buchs, Germany),

89 Ajax Fine Chemicals Co. Ltd. (Sydney, NSW, Australia) and Ajax Fine Chemicals Co. Ltd.
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90 (Auckland, New Zealand), respectively. Ginger essential oil (G) was obtained from Thai-

91 China Flavors and Fragrances Industry Co. Ltd. (Ayutthaya, Thailand).

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93 2.2 Coating preparation for drying

94 HPMC-based composite emulsions were prepared by combining hydrophilic phase

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95 and hydrophobic phase suspended in water. Gly and SA were used as the plasticizer and

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96 emulsifier, respectively. The formulations were made using the following proportions of

97 components: HPMC-BW (4:1), HPMC-Gly (3:1) and BW-SA (5:1). Emulsions were

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98 prepared as previously described (Klangmuang & Sothornvit, 2016a). The G was added into

99 coating emulsions to reach the final concentrations of G at 15 g/L. The coating emulsion was

100
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named HPMC+G. The mixture solutions were homogenized using a homogenizer (Polytron
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101 model PT 3100, Littau, Switzerland) at 20,000 rpm for 5 min.
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103 2.3 Drying methods

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104 Two drying methods (spray and freeze dryings) were studied to produce the HPMC
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105 and HPMC+G powders. First, the emulsions were dried using a spray drier (Lab-Plant SD-04

106 spray dryer, West Yorkshire, UK). The drying temperatures were 180 ± 5 °C at the air inlet
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107 and 70 ± 5 °C at the air outlet with a flow rate of 15 mL/min. These spray-dried samples were

108 named HPMC(S) and HPMC+G(S). Second, HPMC(F) and HPMC+G(F) samples were
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109 frozen at -40 °C for 48 h prior to drying in a freeze dryer (Scanvac Coolsafe 100-4 Pro,

110 Lynge, Denmark). All dried samples were ground using a blender (Waring, 8010BU,

111 Stamford, CT, USA).

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113 2.4 Analysis of powders

114 2.4.1 Color

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115 Color measurements of the powders were made using a spectrophotometer (Spectro-

116 guide sphere gloss, model CD-6834, BYK-Gardner GmbH, Geretsried, Germany). The

117 results were expressed using the CIE LAB color parameters (L*, a* and b*).

118

119 2.4.2 Moisture content and water activity

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120 The moisture contents of the powders were determined using a Sartorius MA40

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121 moisture meter (Sartorius, Inc., Goettingen, Germany). The water activity was determined

122 using the AquaLab Model CX3TE water activity meter (Decagon Devices, Inc., Pullman,

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123 WA, USA).

124

125 2.4.3 Bulk density

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126 The bulk density of the powders was determined according to the method of Shittu
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127 & Lawel (2007) and calculated by dividing mass by volume of the powders.

128 .
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129 2.4.4 Solubility

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130 Solubility was determined as described by Shittu & Lawel (2007). The solubility was

131 calculated as following Eq. (1).

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132

wt. of initial dry matter - wt. of dry matter not solubilize d

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133 Solubility (%) = x100 (1)

wt. of initial dry matter
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134

135 2.4.5 Moisture sorption isotherms

136 The equilibrium moisture contents of the powders were determined at 25 °C using

137 the static gravimetric method. This method is based on the use of nine saturated salt

138 solutions—LiCl, CH3COOK, MgCl2•6H2O, K2CO3, Mg(NO3)2•6H2O, NaNO2, NaCl, KCl

139 and K2SO4— representing 0.12, 0.22, 0.33, 0.43, 0.53, 0.65, 0.75, 0.85 and 0.97 aw,
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140 respectively. The experiment was run in triplicate and the experimental moisture sorption

141 isotherm values were averaged and fitted using a Guggenhein- Anderson-DeBoer (GAB)

142 model (Eq. (2)). The standard error of the estimate (SEE) and the coefficient of determination

143 (R2) between the experimental moisture content (Mi, exp) and the predicted moisture content

144 (Mi, pre) were determined (Eq. (3)). All calculations were performed using Microsoft Office

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145 Excel 2007 Solver and the Analysis Toolpak.

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m o cka w
146 X= (2)
(1 - ka w )(1 - ka w + cka w )

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147

n (M − M i,pre )
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148 SEE = ∑i =1
i,exp

n
(3)
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149 where x = moisture content (g of water/g of dried film), aw = water activity, mo = monolayer
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150 moisture content (g of water/g of dried film), c and k = GAB constants.

151
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152 2.4.6 Evaluation of in vivo antifungal activity

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153 The small pieces of anthracnose symptomatic tissue obtained from infected mango

154 fruit peels approximately 3x3 mm2 were surface sterilized and placed on Petri dishes with
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155 potato dextrose agar (PDA). The pathogen was isolated after an incubation period of 7-11

156 days at ambient temperature (29-33°C) under alternative 12 h of darkness and 12 h of light
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157 exposure. Five millimeter diameter discs of mycelia were cut from the margins of actively

158 growing pure cultures of isolated C. gloeosporioides from the representative samples. The

159 discs of mycelia were then transferred onto PDA media and incubated at 25 °C for 5 days.

160 These actively growing pure cultures were used for the inoculations.

161 Unripe mangoes (Mangifera indica L.) cv. Namdokmai Sithong (110 days old) of

162 similar size were washed in 0.05% sodium hypochlorite solution and then washed with
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163 distilled water. A disc (5 mm depth and 5 mm diameter) of mango tissue was removed from

164 the center of two directly opposite sides of each mango to be inoculated. Mycelial plugs of C.

165 gloeosporioides isolates were cut using a 5 mm diameter sterile cork borer. The mycelia were

166 placed onto the mango tissue on both sides of each mango (one plug per hole) and incubated

167 at 25 °C for 12 h. Mangoes were then coated by dipping in either the HPMC+G(S) or the

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168 HPMC+G(F) emulsion (20 °C, 2 min), then drained and allowed to air-dry at room

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169 temperature (30 °C). Inoculated mangoes without coating were used as a control. Each

170 treatment was applied to 3 replicates of 20 mangoes each. All incubated mangoes were stored

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171 at 25 °C for 5 days. The mangoes were examined for disease severity every day. The

172 antifungal activity was determined in terms of the percentage of inhibition severity (Eq. (4)).

% Inhibition severity =
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(A - B ) x 100
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173 (4)
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174 where A is the diameter of mycelial growth in the uncoated mango and B is the diameter
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175 mycelial growth in the coated mango.

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176
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177 2.5 Accelerated shelf-life testing and shelf-life prediction of powder

178 HPMC+G(F) powder (5 g) was packed into polyethylene zip lock bags (6 × 7 cm
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179 and 0.05 mm thickness). Then, the packages were maintained at 3 different temperatures:

180 45±2 °C (31% RH), 55±2 °C (22% RH) and 65±2 °C (17% RH). The storage period was 60
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181 days and during this period three packages of powder were removed every 15 days to
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182 evaluate the antifungal activity. The analyses carried out at day 0 were considered as the

183 standard condition.

184 The antifungal assay of HPMC+G(F) powder was measured in vitro as the inhibition

185 in radial mycelial growth of C. gloeosporioides on potato dextrose agar (PDA) using the

186 poison food technique. Each PDA dish contained 20% HPMC+G(F) coating emulsion. PDA

187 without coating served as a control. The center of each plate was inoculated with a 5 mm
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188 diameter plug of 7–9 day-old cultures of C. gloeosporioides and incubated at 25 °C for 6

189 days. Radial mycelia growth was determined in each plate after 6 days of incubation by

190 calculating the mean of two perpendicular diameters of the fungal colony. Five replicates

191 were used in each treatment. The results were expressed as a percentage of inhibition

192 according to the formula (Eq. (4)): ((A – B) / A) x 100, where A is the average diameter of

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193 the fungal colony on the control plates and B is the average diameter of the fungal colony on

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194 the coatings emulsion-amended plates.

195 To determine the reaction order, the values of percentage of inhibition were plotted

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196 as a function of storage time. Linear regression was carried out using a first order equation to

197 obtain the reaction velocity values (k) as shown in Eq. (5) for each temperature. Temperature

198
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dependence of % inhibition reactions was simulated by an Arrhenius equation (Eq. (6)) and
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199 used to determine the shelf-life estimation (Eq. (5)).

ln A = − kt + ln A0
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200 (5)

 − Ea 
 RT 
k = Ae 
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201 (6)
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202 where Ao is the % inhibition at the beginning of storage, A is the retention of % inhibition at

203 50% of the initial content, Ea is the activation energy (J/mol), R is the universal gas constant
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204 (8.314 J/mol.K), T is the absolute temperature (K) and t is the shelf-life (days).

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206 2.6 Application of coating powder

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207 2.6.1 Sample preparation and coating application

208 The coating was prepared by dissolving 4% (w/w) of HPMC+G(F) powder in

209 distilled water using a hot/cold technique. The mangoes were prepared into 3 groups: (1)

210 uncoated or control, (2) HPMC+G emulsion and (3) HPMC+G(F) powder. Coated mangoes

211 were dipped in the coating solutions at 20 °C for 2 min and drained of any excess coating

212 solution. Coated and uncoated mangoes were dried in the hot-air oven at 40 oC for 30 min
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213 without surface damage or Maillard reaction taking place. After drying, the mangoes were

214 stored at 13±2 °C and 70±5% RH. Quality assessment was done at 3 day intervals until the

215 mangoes had ripened and they were then graded based on a disease severity scale of 4 (black

216 spot area more than 60 mm2).

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218 2.6.2 Weight loss

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219 Lots of 30 numbered mangoes per group were used to measure the weight loss.

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221 2.6.3 Soluble solids content

222 The soluble solids content was measured in the juice of mango using a hand

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refractometer (Atago model N32, Tokyo, Japan).
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225 2.6.4 Firmness measurements

226 Firmness was determined by measuring the force required to penetrate the center of
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227 the mango cheek at a depth of 5 mm using a 2 mm diameter probe (Universal Testing
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228 machine, with a 500 N load cell, Lloyd, model LR 5K, Hampshire, UK). The probe was held

229 perpendicular to the mango using a compression speed of 10 mm/min.

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230

231 2.6.5 Color

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232 Color measurement was made on the pulp of mangoes using the CIELAB color

233 parameters (L*, a* and b*).

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235 2.6.6 Scale of disease severity caused by natural infection

236 Observation of disease severity of mangoes was recorded every 3 days during

237 storage. The surface disease severity was calculated as the total area of decay using a 1-4
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238 scale; 1 = perfect and no disease, 2 = black spots area < 40 mm2, 3 = black spots area 40-60

239 mm2 and 4 = black spots area > 60 mm2.

240

241 2.7 Statistical analyses

242 Three replications of a completely randomized experimental design were used to

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243 determine each property. The SPSS 11.0 for Windows software (SPSS Inc., Chicago, IL,

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244 USA) was used for the analysis of variance test and Duncan’s multiple range tests were used

245 to determine significant differences between treatments at the 95% confidence level.

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246

247 3. Results and discussion

248 3.1 Properties of powder

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249 The drying methods and coating composition significantly affected the color
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250 attributes. The freeze-dried powder (HPMC(F) and HPMC+G(F)) had the highest L* values

251 (Table 1), while the spray-dried powder (HPMC(S) and HPMC+G(S)) had the lowest L*
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252 values (p < 0.05). The darker color of HPMC(S) powder can be attributed to a high drying
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253 temperature resulting in a Maillard reaction, Similar results were observed by Caliskan &

254 Dirim (2016), where the L* values of spray-dried sumac extract powder were lower than for
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255 freeze-dried powder. The addition of G in the spray-dried powder significantly decreased the

256 L* value. The a* values of spray-dried powder were significantly higher but their b* values
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257 were lower than for freeze-dried samples. The color parameters reflect the visual appearance

258 of coating powders which might affect food applications.

259 Moisture content (MC) is an essential property to determine the powder stability

260 during storage. The MC of spray-dried coating powders was lower than that of freeze-dried

261 powders (Table 1). This may have been due to the temperature effect of spray drying. A

262 higher inlet temperature results in a greater heat transfer rate as a driving force to evaporate
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263 moisture from the coatings similar to what was reported for sumac extract powders (Caliskan

264 & Dirim, 2016). The addition of G reduced MC of the HPMC+G(F) and HPMC+G(S)

265 powders compared to the HPMC(F) and HPMC(S) powders. This was attributed to an

266 increase in the hydrophobicity of powder. Furthermore, aw values of spray-dried powders

267 were lower than those from freeze dried, no matter whether the G was included in the

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268 powder. This showed that drying technique much influenced aw value of the powder. All

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269 powders had aw values in the range 0.4-0.5 depending on the powder formula. The low values

270 of aw and MC correlated with the ability of active powders to prolong shelf-life, lowering the

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271 Maillard reaction, lipid oxidation, microbial growth and hydrological and enzymatic

272 reactions.

273
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Bulk density is the density of a material when packed or stacked in bulk. The bulk
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274 density of freeze-dried powder was significantly higher than for spray-dried powder (Table
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275 1). Ginger oil did not significantly affect the bulk density of the HPMC+G(S) coating powder

276 whereas it significantly affected HPMC+G(F). Powders with higher moisture contents tend to
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277 have a higher bulking weight due to the presence of water, which is considerably denser than
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278 the dried solid (Chegini & Ghobadian, 2005). This behavior can be associated with the higher

279 moisture content and bulk density of the freeze-dried powders observed in our study.
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280 The solubility of a powder indicates its integrity in an aqueous solution. A high

281 solubility of powders would be advantageous during the preparation of the coating solution.
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282 There was no significant difference in the solubility between spray-dried and freeze-dried

283 coating powders (Table 1). Moreover, the addition of G did not affect their solubility.

284

285 3.2 Moisture sorption isotherms

286 The sorption isotherm can predict stability and quality changes during storage of the

287 powder. HPMC(S) and HPMC+G(S) coating powders had lower MC values than HPMC(F)
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288 and HPMC+G(F) powders at similar aw values (Fig. 1). This might have resulted from the

289 ability of spray drying to bind less water than freeze drying thereby providing a lower MC.

290 The powder had increased moisture sorption at higher aw values. All curves were sigmoidal in

291 shape (Fig. 1), characteristic of type II isotherms, which are typical isotherms for most

292 biopolymer materials such as freeze-dried rice powder (Oikonomopoulou, Krokida, &

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293 Karathanos, 2011). All data had a good fit using logarithmic non-linear regression with high

values of the coefficient of determination (R2 > 0.900) as shown in Table 2 suggesting that

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294

295 the adsorption process obeys the Guggenheim-Anderson-de Boer (GAB) model. Generally,

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296 the value of a monolayer (Mo) indicates the amount of water that is strongly adsorbed to

297 specific sites of powder at optimum stability (Klangmuang & Sothornvit, 2016b). The

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powder had lower Mo values, while the incorporation of G increased this response.
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299
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300 3.3 Antifungal activity

301 The in vivo antifungal activity of freeze-dried and spray-dried HPMC+G powders was
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302 evaluated the inhibition of disease severity on coated mangoes inoculated with C.
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303 gloeosporioides. The diameters of C. gloeosporioides colonies in all groups increased

304 throughout storage and reached an asymptotic value after 5 days of storage. During storage at
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305 25 oC, HPMC+G(F) and HPMC+G(S) powders significantly reduced disease severity

306 compared with uncoated mango (Table 3). Previously, HPMC+G nanocomposite film had
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307 shown activity against C. gloeosporioides, Staphylococcus aureus and Escherichia coli

308 (Klangmuang & Sothornvit, 2016a). In particular, ginger oil compounds, such as gingerols,

309 sesquiterpenoids and shogaols derivatives, were responsible for antimicrobial activity (Malu

310 et al., 2009). In our study, the drying method significantly affected antifungal activity on

311 inoculated mangoes. HPMC+G(F) powder was more effective than HPMC+G(S) powder in

312 the reduction of disease severity of C. gloeosporioides on mango. This result was in
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313 agreement with the highest encapsulating efficiency, phenolic content, solubility, porosity

314 and flow ability with the lowest hygroscopicity of freeze-dried phenolic compounds extracted

315 from Averrhoa carambola pomace and microencapsulated with maltodextrin (Saikia,

316 Mahnot, & Mahanta, 2015). Drying methods induced changes in the powder structures

317 leading to the differences in antifungal properties. Freeze drying can protect the sensitive

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318 compounds such as phenolic compounds and maintain the appearance, color and aroma of

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319 ginger oil (Zea, Yusof, Aziz, Ling, & Amin, 2013). Therefore, HPMC+G(F) was selected to

320 evaluate the shelf-life and used as a coating for fresh mango.

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321

322 3.4 Accelerated shelf-life testing and shelf-life prediction of powder

323
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The antifungal activity was selected as an important factor to determine the shelf-life
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324 of HPMC+G(F) powder. First-order kinetics produced a good fit with the change of
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325 antifungal inhibitory activity having a linear regression relationship with the logarithm of the

326 inhibition value and time. The reaction rate constant (k) of HPMC+G(F) powder increased
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327 with higher storage temperature (Table 4). After 60 days of storage at different temperatures
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328 of 45, 55 and 65 oC, the antifungal activity on HPMC+G(F) powder decreased with all

329 storage temperatures (Fig. 2). As expected, a lower storage temperature maintained better
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330 antifungal activity of HPMC+G(F) coating powder than that at a higher storage temperature.

331 A higher k value reflects a lower effectiveness of inhibition. Breda, Sanjinez-Argandona, &
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332 Correia (2012) found that increasing the temperature influenced vitamin C degradation in

333 powdered guavira pulp. We considered that a loss of 50% of its initial antifungal activity

334 represented the end of the usable shelf-life of powder. Hence, the shelf-life of HPMC+G(F)

335 powder at 45, 55 and 65 oC was 113.95, 88.24 and 82.42 days, respectively. The difference in

336 shelf-life between 55 and 65 oC was less than between these temperatures and 45 ºC. This

337 might be because the high temperature exposure over 55 oC triggered the rapid microbial
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338 growth, lowered the antifungal activity and finally shortened the shelf-life of the powder.

339 From the Arrhenius equation, the shelf-life of the powder stored at 25 oC was 160 days. This

340 is shorter than the shelf-life of many commercial powdered products (6-12 months).

341 Generally, packaging is an important factor to be considered in terms of its permeability

342 properties for oxygen and moisture and as a light barrier to maintain good quality powder. In

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343 our experiments, polyethylene zip lock packaging which has higher oxygen and water vapor

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344 permeability properties than the laminating packaging was used to contain HPMC+G(F)

345 powder.

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346

347 3.5 Application of powder on mango

348
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All coatings were thin, transparent and adhered well on the mango surfaces. In fact,
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349 Namdokmai Sithong mangoes had a light yellow skin color at the unripe stage that evolved
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350 into a golden yellow color when ripe. The visual quality of the coated mangoes did not

351 change in any treatment during the first 12 days of storage at 13 °C. Disease on uncoated
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352 mango appeared after 3 days of storage and the severity increased thereafter. The HPMC+G
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353 and HPMC+G(F) coatings extended the shelf-life of fresh mangoes to 18 days compared to

354 15 days for uncoated mangoes at 13 oC.

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355 As expected, weight loss increased with storage time (Fig. A.3). Uncoated mangoes

356 had a higher weight loss than coated mangoes, which indicated the effectiveness of the
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357 emulsion and powder coating as moisture barriers. Coatings containing hydrophobic

358 compounds such as BW and EO, deposited as an additional layer over the natural wax,

359 improve the fruit moisture resistance. No significant differences in weight loss were observed

360 between the powder and emulsion coating. This meant that HPMC+G(F) powder coating had

361 the same properties as the original emulsion coating. Thus, freeze drying did not affect the

362 functional properties of the powder.

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363 The coated mangoes had significantly lower SSC at the end of storage. The emulsion

364 coating had a beneficial effect on maintaining the SSC accumulation at a slower rate

365 compared to the powder. The SSC increased with time (Fig. B.3) indicating the change of

366 starch to sugar (Sothornvit & Rodsamran, 2010). The slow increase in SSC in coated mango

367 could have been due to the slow rate of respiration and metabolic activity that retarded fruit

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368 ripening (Jafarizadeh, Osman, Tan, & Abdul Rahman, 2011). Ali, Zahid, Manickam,

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369 Siddiqui, Alderson, & Maqbool (2013) found that coated dragon fruit with chitosan formed a

370 semi-permeable film around the fruit which suppressed ethylene production and maintained

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371 SSC content in the fruit. Similar results were reported for mango fruit coated with a mango-

372 based film (Sothornvit & Rodsamran, 2008).

373
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As expected, the firmness of the mango significantly decreased during storage (Fig.
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374 4). Both coatings significantly delayed the loss of firmness compared to uncoated mango

during storage at 13 oC. Moreover, there was no significant difference between HPMC+G
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376 and HPMC+G(F) at day 15. The ripening of mango fruits is characterized by a loss of
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377 firmness due to cell wall digestion by pectinesterase, polygalacturonase and other enzymes
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378 (Abbasi, Anjum, Sammi, Masud, & Ali, 2011). Coating may also inhibit the activity of

379 pectin-degrading enzymes by reducing the rate of metabolic processes during senescence
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380 (Zhou et al., 2008), resulting in the maintenance of fruit firmness. Edible coatings

381 incorporated with essential oil delayed textural changes, as reported with gum arabic/ginger
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382 oil on papaya (Ali, Hei, & Keat, 2016) and HPMC/bergamot oil on grape (Sánchez-Gonzalez

383 et al., 2011). The decrease in mango firmness with ripening was related to weight loss as

384 found in guava (Sothornvit, 2013).

385 The pulp color changes in mango fruits were progressively from green to yellow

386 during storage. The L* of mangoes decreased as storage time increased, whereas a* and b*

387 values increased (Fig. 5). At day 15, the coating significantly helped maintain L*, a* and b*
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388 values of coated mango. Coated mangoes presented higher L* and lower a* and b* values

389 than uncoated mangoes. The b* value was used as the main indicator for pulp color change

390 (Sothornvit & Rodsamran, 2008). The b* value of all mangoes also significantly increased

391 during storage. No differences were observed in the L* and b* values among coating

392 treatments. All coatings delayed the color changes in mangoes during storage at 13 oC.

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393 Fagundes, Palou, Monteiro, & Pérez-Gago (2015) reported that a HPMC-BW coating on

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394 tomato significantly reduced the changes in L* and b* values compared to the control.

395 Anthracnose is the most important postharvest disease of mango and causes decay

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396 during storage and transportation. The symptoms are black spots and streaks on the mango

397 skin (Sothornvit & Klangmuang, 2015). In this work, the maximum shelf-life was defined as

398
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the time between the application of the coating and the visualization of fungal injury. The
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399 HPMC+G emulsion and HPMC+G(F) coating powder significantly reduced the disease
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400 severity score of coated mango, compared with uncoated mangoes during storage (Fig. C.3).

401 The first symptoms of decay occurred after day 9 for uncoated and after day 15 for coated
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402 mangoes. Uncoated mango was spoiled after 15 days of storage. Furthermore, the coated
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403 mango with HPMC+G(F) coating powder had a higher disease severity score than the

404 HPMC+G emulsion treatment at day 12. However, at the end of storage (day 18), the disease
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405 severity scores were similar for both. Senescence makes the fruit more vulnerable to

406 pathogenic infection as a result of loss of cellular or tissue integrity (Tanada-Palmu &
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407 Grossso, 2005). The early decrease in decay was probably due to the active ingredients in G.

408 Likewise, G showed inhibitory activities against C. gloeosporioides in HPMC-BW-clay films

409 (Klangmuang & Sothornvit, 2012).

410

411 4. Conclusions
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412 The drying methods affected the powder properties. A GAB model was used to

413 explain the moisture sorption isotherm of coating powder and the incorporation of ginger oil

414 decreased the monolayer moisture content parameter. HPMC-based composite powder

415 effectively reduced C. gloeosporioides growth on coated mango and freeze-dried HPMC+G

416 powder was the most effective inhibition. This study indicated the potential to transform

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417 coating solution to edible powder. Hence, the active coating powder could be a good

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418 alternative edible coating to maintain the quality attributes and extend the shelf-life of mango

419 and other tropical fruits such as banana and papaya to inhibit the growth of C.

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420 gloeosporioides during storage and transportation.

421

422 Acknowledgements
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423 The authors thank the Kasetsart University Research Development Institute (KURDI)
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424 and the Thailand Research Fund through the Royal Golden Jubilee Ph.D. Program joint with

425 Kasetsart University (Grant No. PHD/0179/2553) for financial support throughout this
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426 research.
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427

428 References
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429 Abbasi, K.S., Anjum, N., Sammi, S., Masud, T., & Ali, S. (2011). Effect of coatings and

430 packaging material on the keeping quality of mangoes (Mangifera indica L.) stored
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431 at low temperature. Pakistan Journal of Nutrition, 10, 129-138.

432 Ali, A., Maqbool, M., Ramachandran, S., & Alderson, P.G. (2010). Gum arabic as a novel

433 edible coating for enhancing shelf-life and improving postharvest quality of tomato

434 (Solanum lycopersicum L.) fruit. Postharvest Biology and Technology, 58, 42–47.
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435 Ali, A., Hei, G.K., & Keat, Y.W. (2016). Efficacy of ginger oil and extract combined with

436 gum arabic on anthracnose and quality of papaya fruit during cold storage. Journal

437 of Food Science and Technology, 53, 1435-1444.

438 Ali, A., Zahid, N., Manickam, S., Siddiqui, Y., Alderson, P.G., & Maqbool, M. (2013).

439 Effectiveness of submicron chitosan dispersions in controlling anthracnose and

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440 maintaining quality of dragon fruit. Postharvest Biology and Technology, 86, 147-

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441 153.

442 Breda, C.A., Sanjinez-Argandona, E.J., & Correia, C.d.A.C. (2012). Shelf life of powdered

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443 Campomanesia adamantium pulp in controlled environments. Food Chemistry,

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446 of maltodextrin addition on the powder properties of sumac extract powders. Powder
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447 Technology, 287, 308-314

448 Chegini, G.R., & Ghobadian, B. (2005). Effect of spray-drying conditions on physical
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449 properties of orange juice powder. Drying Technology, 23, 656-668.

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450 Fagundes, C., Palou, L., Monteiro, A.R., & Pérez-Gago, M.B. (2015). Hydroxypropyl

451 methylcellulose-beeswax edible coatings formulated with antifungal food additives

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452 to reduce alternaria black spot and maintain postharvest quality of cold-stored cherry

453 tomatoes. Scientia Horticulturae, 193, 249–257.

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454 Jafarizadeh M.H., Osman, A., Tan, C.P., & Abdul Rahman, R. (2011). Development of an

455 edible coating based on chitosan-glycerol to delay ‘Berangan’ banana (Musa

456 sapientum cv. Berangan) ripening process. International Food Research Journal, 18,

457 989-997.
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458 Klangmuang, P., & Sothornvit, R. (2012). Antifungal performance of hydroxypropyl

459 methylcellulose film incorporated with essential oil against Colletotrichum

460 gloeosporioides. Journal of Agricultural Science, 43, 625-628.

461 Klangmuang, P., & Sothornvit, R. (2016a). Barrier properties, mechanical properties and

462 antimicrobial activity of hydroxypropyl methylcellulose-based nanocomposite films

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463 incorporated with Thai essential oils. Food Hydrocolloids, 61, 609-616.

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464 Klangmuang, P., & Sothornvit, R. (2016b). Combination of beeswax and nanoclay on

465 barriers, sorption isotherm and mechanical properties of hydroxypropyl

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466 methylcellulose based composite films. LWT - Food Science and Technology, 65,

467 222-227.

468
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469 medicinal properties of (Zingiber officinale). Global Journal of Pure and
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470 Applied Sciences, 15, 365-368.

471 Oikonomopoulou, V.P., Krokida, M.K., & Karathanos, V.T. (2011). Structural properties of
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472 freeze-dried rice. Journal of Food Engineering, 107, 326-333.

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473 Rhim, J.W., Hong, S.I., Park, H.M., & Ng, P.K.W. (2006). Preparation and characterization

474 of chitosan-based nanocomposite films with antimicrobial activity. Journal of

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475 Agricultural and Food Chemistry, 54, 5814-5822.

476 Saikia, S., Mahnot, N.K., & Mahanta, C.L. (2015). Optimisation of phenolic extraction from
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477 Averrhoa carambola pomace by response surface methodology and its

478 microencapsulation by spray and freeze drying. Food Chemistry, 171, 144-152.
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479 Sánchez-González, L., Pastor, C., Vargas, M., Chiralt, A., González-Martínez, C., & Cháfer,

480 M. (2011). Effect of hydroxypropylmethylcellulose and chitosan coatings with and

481 without bergamot essential oil on quality and safety of cold-stored grapes.

482 Postharvest Biology and Technology, 60, 57-63.

483 Shittu, T.A., & Lawal, M.O. (2007). Factors affecting instant properties of powdered cocoa

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484 beverages. Food Chemistry, 100, 91-98.

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485 Sothornvit, R. (2013). Effect of edible coating on the qualities of fresh guava. Acta

486 Horticulturae, 1012, 453-460.

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487 Sothornvit, R., & Rodsamran, P. (2008). Effect of a mango film on quality of whole and

488 minimally processed mangoes. Postharvest Biology and Technology, 47, 407-415.

489
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Sothornvit, R., & Rodsamran, P. (2010). Mango film coated for fresh-cut mango in modified
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490 atmosphere. International Journal of Food Science and Technology, 45, 1689-1695.
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491 Sothornvit, R., Hong, S.I., An, D.J. & Rhim, J.W. (2010). Effect of clay content on the

492 physical and antimicrobial properties of whey protein isolate/organo-clay composite

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493 films. LWT-Food Science and Technology, 43, 279-284.

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494 Sothornvit, R., Rhim, J.W., & Hong, S.I. (2009). Effect of nano-clay type on the physical and

495 antimicrobial properties of whey protein isolate/clay composite films. Journal of

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496 Food Engineering, 91, 468-473.

497
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498 Tanada-Palmu, P.S., & Grosso, C.R.F. (2005). Effect of edible wheat gluten-based coating

499 and coatings on refrigerated strawberry (Fragaria ananassa) quality. Postharvest

500 Biology and Technology, 36, 199-208.

501 Velickova, E., Winkelhausen, E., Kuzmanova, S., Alves, V.D., & Moldão-Martins, M.

502 (2013). Impact of chitosan-beeswax edible coatings on the quality of fresh

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503 strawberries (Fragaria ananassa cv Camarosa) under commercial storage

504 conditions. LWT - Food Science and Technology, 52, 80-92.

505 Zea, L.P., Yusof, Y.A., Aziz, M.G., Ling, C.N., & Amin, N.A.M. (2013). Compressibility

506 and dissolution characteristics of mixed fruit tablets made from guava and pitaya

507 fruit powders. Powder Technology, 247, 112-119.

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508

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1 Table Legends

2 Table 1 Physical properties of HPMC-based composite coating powder incorporated with or

3 without ginger oil using freeze drying or spray drying.

4 Means in the same row with different letters indicate significant differences (p < 0.05).

5 Table 2 Effect of freeze drying or spray drying method on the GAB parameters of

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6 HPMC-based composite coating powder.

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7 Table 3 Effect of freeze drying or spray drying method on the diameters of anthracnose in

8 vivo test, visual appearance and the percent inhibition of disease severity on

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9 mango fruits inoculated with Colletotrichum gloeosporioides after 5 days at 25
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10 C.

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Means in the same column with different letters indicate significant differences (p < 0.05)
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12 Table 4 Reaction rate constant (k) (1/days) and shelf-life (days) evaluation of HPMC-
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13 based composite incorporated with ginger oil coating powder.

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15 Table 1

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Parameter HPMC(F)* HPMC(S) HPMC+G(F) HPMC+G(S)

Moisture content (%) 27.35±2.15a 23.90±0.58b 25.90 ±1.96ab 21.73 ± 0.81b

Water activity 0.44±0.01a 0.41±0.01b 0.44 ± 0.02ab 0.41 ± 0.01b

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Bulk density (g/cm3)) 0.08±0.002b 0.03±0.003c 0.09±0.001a 0.03±0.001c

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Solubility (%) 92.98±2.18a 95.05±0.26a 92.53±1.85a 94.42±1.63a

Color

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L* 88.66±1.56a 80.02±1.87b 87.52 ± 1.75a 76.19 ± 4.07c

a* -1.01±0.55b 0.30±0.07a -1.00 ± 0.21b 0.29 ± 0.07a

b* 6.39±0.90b
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3.28±0.48c 9.33 ± 1.14a 3.56 ± 0.43c
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17 *HPMC(F) = HPMC-based composite coating powder using freeze drying, HPMC(S) = HPMC-based

18 composite coating powder using spray drying, HPMC+G(F) = HPMC-based composite coating powder
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19 incorporated with ginger oil using freeze drying, and HPMC+G(S) = HPMC-based composite coating powder
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20 incorporated with ginger oil using spray drying.

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22 Table 2

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Treatment* Mo c k SEE R2

HPMC(F) 1.39 0.566 1.106 1.49 0.974

HPMC(S) 1.24 0.468 1.016 1.23 0.986

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HPMC+G(F) 2.40 0.429 1.103 1.67 0.978

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HPMC+G(S) 2.01 0.458 1.109 1.44 0.989

24 *HPMC(F) = HPMC-based composite coating powder using freeze drying, HPMC(S) = HPMC-based

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25 composite coating powder using spray drying, HPMC+G(F) = HPMC-based composite coating powder

26 incorporated with ginger oil using freeze drying, and HPMC+G(S) = HPMC-based composite coating powder

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27 incorporated with ginger oil using spray drying.
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28 Mo = monolayer moisture content (g of water/g of dried powder), c and k = constants, SEE = standard error of

29 estimate and R2 = coefficient of determination

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31 Table 3

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Treatment* Colony diameter (cm) Visual appearance Inhibition (%)

Control 2.89±0.34a 0

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HPMC 2.69±0.20a 6.92c

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HPMC+G(F) 1.94±0.10c 32.87a
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HPMC+G(S) 2.16±0.10b 25.26b

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33 *HPMC(F) = HPMC-based composite coating powder using freeze drying, HPMC(S) = HPMC-based
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34 composite coating powder using spray drying, HPMC+G(F) = HPMC-based composite coating powder

35 incorporated with ginger oil using freeze drying, and HPMC+G(S) = HPMC-based composite coating powder
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36 incorporated with ginger oil using spray drying.

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39 Table 4

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Kinetic model (first-order) 45 oC 55 oC 65 oC

Reaction rate constant (k) 0.0067 0.0086 0.0090

Shelf-life (days) 113.95 88.24 82.42

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1 Figure Legends

2 Fig. 1. Moisture sorption isotherm of HPMC-based composite coating powder incorporated

3 without ginger oil (HPMC) and with ginger oil (HPMC+G) using freeze drying (F) or

4 spray drying (S). Error bars represent the standard deviation. Different letters indicate the

5 significant differences among treatments at the same water activity.

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6

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7 Fig. 2. Percentage of inhibition of HPMC-based composite powder incorporated with ginger oil

8 coating against C. gloeosporioides during storage at 45, 55 and 65 oC. Different letters

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9 indicate the significant differences among treatments in each day of storage.

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11 Fig. 3. Effect of HPMC-based composite incorporated with ginger oil coating emulsion

12 (HPMC+G) and powder (HPMC+G(F)) and storage time on weight loss (A), soluble
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13 solids content (SSC) (B) and disease severity (C) of whole mangoes during storage at 13
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14 C (1 = perfect to 4 = severe symptoms). Error bars represent the standard deviation.
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15 Different letters indicate the significant differences among treatments in each day of
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16 storage.
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18 Fig. 4. Effect of HPMC-based composite incorporated with ginger oil coating emulsion
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19 (HPMC+G) and powder (HPMC+G(F)) and storage time on firmness of whole mangoes
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20 during storage at 13 oC. Error bars represent the standard deviation. Different letters

21 indicate the significant differences among treatments in each day of storage.

22

23 Fig. 5. Effect of HPMC-based composite incorporated with ginger oil coating emulsion

24 (HPMC+G) and powder (HPMC+G(F)) and storage time on pulp color (A) L*, (B) a* and
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25 (C) b* of whole mangoes during storage at 13 oC. Error bars represent the standard

26 deviation. Different letters indicate the significant differences among treatments in each

27 day of storage.

28

29

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30

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33 Figure 1
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38 Figure 2

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46 (A)

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52 Figure 5

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Highlights

• Ginger oil was used to form HPMC-based nanocomposite coating and powder.

• Antifungal activity of freeze-dried coating powder was better than spray-dried

one.

• Freeze drying and spray drying maintained antifungal properties of coating

powder.

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• The accelerate shelf-life of the active coating powder was 160 days at 25 °C.

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The active coating maintained the quality of coated mangoes up to 18 days at 13
°C.

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