Journal Pre-proofs

Development of antioxidant chitosan film with banana peels extract and its
application as coating in maintaining the storage quality of apple

Wanli Zhang, Xiangxin Li, Weibo Jiang

PII: S0141-8130(19)36811-4
DOI: https://doi.org/10.1016/j.ijbiomac.2019.10.275
Reference: BIOMAC 13776

To appear in: International Journal of Biological Macromole-

cules

Received Date: 25 August 2019

Revised Date: 29 October 2019
Accepted Date: 30 October 2019

Please cite this article as: W. Zhang, X. Li, W. Jiang, Development of antioxidant chitosan film with banana peels
extract and its application as coating in maintaining the storage quality of apple, International Journal of
Biological Macromolecules (2019), doi: https://doi.org/10.1016/j.ijbiomac.2019.10.275

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1 Development of antioxidant chitosan film with banana peels extract and

2 its application as coating in maintaining the storage quality of apple

5 Wanli Zhanga, Xiangxin Lia, Weibo Jianga,*

a
6 College of Food Science and Nutritional Engineering, China

7 Agricultural University, Beijing 100083, PR China

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13 *Correspondence to Weibo Jiang. E-mail: jwb@cau.edu.cn (W Jiang). Tel:

14 (86 10) 6273 6565; Fax: (86 10) 6273 6565.

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20

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1
23 Abstract

24 In the present study, the antioxidant chitosan (CS)-banana peels extract (BPE) composite film

25 was developed. The different content of BPE (4%, 8% and 12%) was added to the CS film not

26 only as the antioxidant but also as the cross-linking. The CS, CS-4% BPE, CS-8% BPE and

27 CS-12% BPE films were characterized by scanning electron microscopy (SEM), fourier transform

28 infrared spectroscopy (FTIR), X-ray diffraction analysis (XRD) and thermogravimetric analysis

29 (TGA). The physical and mechanical properties possessed by the CS and CS-BPE films were

30 compared as well, and the CS-4 %BPE composite film exhibited the most excellent properties.

31 The decline in moisture contents, water solubility and water vapor permeability of CS-BPE

32 composite film indicated the reduced hydrophilicity. Moreover, the CS-BPE composite film

33 exhibited excellent antioxidant activity in different food simulants. Finally, the optimal

34 concentration of CS-BPE coating treatment was identified and applied to apple fruit, and the

35 results showed that CS-BPE coating was more capable of improving the postharvest quality of

36 apple fruit than CS coating. This study evidences the promising nature of CS-BPE composite film

37 and coating as a desirable alternative for active packaging and it is believed as conducive to

38 valorization of banana peel by-products for allied applications.

39 Key words: Chitosan antioxidant film; Banana peels extract; Postharvest apple fruit.

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44

2
45 1. Introduction

46 As the most important temperate fruits, apple contains high levels of polyphenolic

47 compounds, vitamins and organic acids. Nevertheless, the relatively rapid process of aging leads

48 to a short shelf life for apple in postharvest storage [1]. One way to maintain the storage quality

49 of fruit is active coatings, which is effective in delaying over-ripening and senescence through

50 the regulation of moisture, solutes and gaseous exchange [2]. In recent years, the material of

51 natural active films and coatings that have been exploited generally derived from edible natural

52 biopolymers including proteins, polysaccharides and lipids [3]. Chitosan (CS), as a positively

53 charged polysaccharide, has been widely applied in the preparation of edible films and coatings

54 due to its high biocompatibility, strong film forming ability and natural antibacterial properties

55 [4].

56 Despite these advantages as mentioned above, the practical applications of pure film

57 composed of pure chitosan and other pure biopolymers as a matrix remain constrained by the

58 insufficient antibacterial and antioxidant capacity [3, 5]. Therefore, the addition of natural active

59 products is considered as a promising approach to improving the performance of active film

60 composed of biopolymers [[3], [6], [7]]. So far, the natural products added into modified chitosan

61 films and coatings, including plant essential oils, bacteriocins, and plant extracts, have already

62 been developed [[2], [8], [9]]. Due to the high content of phenolics substances with excellent

63 antioxidant capacity, the plant extracts (PE), including leaves, seeds, and fruit extracts have been

64 identified as excellent materials for incorporation of chitosan films and coatings [[6], [10], [11]].

65 Compared with a single component of chitosan, the addition of PE improved the mechanical and

66 physical properties of the active film, especially the antioxidant and antibacterial activity, and for

3
67 the application of the coating, the composite chitosan coating incorporated with PE demonstrates

68 a more excellent ability to maintain the quality of postharvest fruits [2, 3].

69 Banana is a sort of fruit that is frequently consumed by people around the world for its good

70 taste [12]. The annual banana production worldwide amounts to approximately 102 million tons,

71 while banana peel accounts for 35% of banana fruit, it is basically discarded as industrial waste

72 [13]. Traditionally, banana peel is claimed to have various medicinal value, including therapeutic

73 and preventive effects on a variety of such diseases as burns, anaemia, inflammation and

74 depression [14]. In addition, banana peel contains a large amount of bioactive ingredients, for

75 instance, carotenoids, phenolics and biogenic amines, which provide a good source of

76 pro-vitamin A and possess a superior antioxidant capacity to other fruit peel like avocado,

77 pineapple, papaya, passion fruit, water melon and melon [15, 16]. Therefore, the extraction and

78 application of active substances contained in banana peel is worthy of further exploration and

79 research. In recent reports, attempt has been made to make use of ripe banana skin powder

80 straightaway for the production of edible coatings [17]. Nevertheless, up to now, rare reports

81 have investigated the effects of the addition of ripe banana peel extract (BPE) on active

82 packaging films.

83 Therefore, this research aims at incorporating ripe banana peel extract into chitosan film and

84 coating for the purpose of developing a modified active packaging film and coating to find a

85 promising recycling method for this by-product. The physical, structural and mechanical

86 properties of chitosan films incorporated different concentrations of BPE were characterized. In

87 addition, the antioxidant capacity of these films developed were evaluated under different food

88 simulation conditions. Finally, the chitosan coating with and without 4% BPE were applied in

4
 89 order to compare the capability of maintaining the quality of apple fruit in the postharvest storage.

90 We hypothesize the incorporation of BPE, acting as the cross-linking and antioxidant, could

91 enhance chitosan film properties.

92 2. Materials and methods

93 2.1. Material

94 Chitosan (degree of deacetylation > 90%, viscosity 100-200 cps) was obtained from Sigma

95 Chemical Co. (St. Louis, MO, USA). Mature bananas, about 12 % of pulp soluble solids content

96 (SSC), were purchased from the market in Haidian District, Beijing, China. All other chemical

97 reagents used were of analytical grade.

98 2.2. Preparation of BPE

99 The banana peel derived from the ripe bananas was removed and frozen with liquid nitrogen

100 immediately after the fruit was washed with distilled water. Then, a pulverizer was employed to

101 prepare the powder. According to the results of previous experiments, 80 % (v/v) ethanol solution

102 has the best extraction effect, and 0.1% (v/v) hydrochloric acid can inhibit browning during the

103 extraction process.100 g of banana peel powder was mixed with 500 mL of 80 % (v/v) ethanol and

104 magnetically stirred for extraction at 500 rpm for 12 hours at 25 °C. The obtained mixture was

105 suction filtered, and the derived filtrate was evaporated in vacuum at 39 °C for one hour to obtain

106 an extract of 20 % volume. The extract was stored at 4 °C for further usage. BPE was

107 characterized by total phenolic content (TP) and SSC. A previous method was used to test TP and

108 SSC contents [18]. To evaluate phenolic compounds in BPE, a HPLC method [19], with a

109 Shimadzu liquid chromatograph, was used. The particle size of BPE was determined by using a

110 combined dynamic light scattering (DLS).

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111 2.4. Preparation of chitosan-BPE composite films

112 Preparation of chitosan-BPE composite films were developed according to [20]. Firstly,

113 2 wt % of chitosan solution was obtained by dissolving chitosan to distilled water containing 1 %

114 (v/v) acetic acid, 30 % (w/w) glycerol was added as a plasticizer. 4 %, 8 % and 12 % (v/v) of BPE

115 were mixed into the film forming solution for preparing CS-4% BPE, CS-8% BPE and CS-12%

116 BPE films respectively, stirred for half an hour to make the BPE distribution uniform, and then the

117 mixed film forming solution was ultrasonicated for 30 min for degassing treatment. The

118 film-forming solutions were poured into polystyrene petri dishes (diameter of 9 cm). Film was

119 obtained by drying the dish in a drying oven at 30 °C for 24 hours. All films were stored at 25 °C,

120 in a desiccator with 60 % relative humidity. The pure chitosan film without BPE was prepared in

121 the same manner as a control.

122 2.5. Physical and mechanical properties

123 2.5.1. Film thickness

124 The film thickness was determined with a digital micrometer (Mitutoyo Absolute, Tester

125 Sangyo Co. Ltd., Japan) with a precision of 0.001 mm.

126 2.5.2. Color and transparency

127 Color parameters L* (lightness), a* (green to red) and b* (yellow to blue) of the films were

128 determined using a reflectance spectrophotometer (Model NF333, Nippon Denshoku Industries,

129 Tokyo, Japan).

130 According to our previous method [20], the transparency of the films was calculated by the

131 following equation.

A
132 Opacity  (1)
x

6
133 where A was the value of absorbance at 600 nm and x was the thickness of the film (mm).

134 2.5.3. Moisture content

135 The film sample was dried at 110 °C until constant weight, moisture content was determined

136 according to the following formula (2).

(initial mass  final dry mass)

137 Moisture contents (%)   100 (2)
initial mass
138 2.5.4. Water solubility

139 The film sample dried to initial constant weight was immersed in distilled water, shaken at

140 25 °C for 24 hours, and then dried again to constant weight. Water solubility was determined

141 according to the following formula (3).

(initial dry mass  final dry mass)

142 Water solubility (%)   100 (3)
initial dry mass

143 2.5.5. Water vapor permeability

144 According to our previous method [20], the film sample was sealed in a weighing cup mouth

145 (4 cm in diameter and 4 cm depth) containing 3 g of cacl2, and then the cup was placed in a

146 desiccator containing saturated potassium iodide (20 °C, 70% relative humidity) and the weight of

147 the cup was weighed every 4 h for 2d. Equation (4) was used to calculate the water vapor

148 permeability.

(Weight difference)  (film thickness)

149 Water vapor permeability  (4)
(Exposed area)  (time)  (presure difference)

150 2.5.6. Mechanical properties

151 The film sample (60 mm×8 mm) was tested by a texture analyzer (CT3, Brookfield Ltd.,

152 USA) at stretching rate of 1.0 mm/s. The following equations were used to calculating tensile

153 strength and elongation at break of film. The tensile attributes-elastic modulus of film was

7
154 determined from the linear slope of the stress versus strains curves.

F
155 Tensile strength (MPa)  (5)
xw
Δx
156 Elongation at break (%)   100 (6)
x0

157 where F was the stress at film break (N), x was film thickness (mm), w was film width (mm),

158 Δx and x0 was the extended distance (mm) the initial length of film, respectively.

159 2.6. Characterization of chitosan-BPE composite film

160 2.6.1. Morphology by scanning electron microscopy (SEM)

161 The film sample (0.5 × 0.5 cm2) was fixed on a copper column with double-sided tape, and

162 then sprayed with gold to observe. For the cross-section analysis, the film was frozen with liquid

163 nitrogen and breaking it with tweezers. The microscopic morphology of the surface and cross

164 section of the film was observed with a scanning electron microscope (JSM-6700F, Jeol Ltd.,

165 Japan) at 3500× and 500× magnifications with the accelerating voltage of 20 kV.

166 2.6.2. Fourier transform infrared (FT-IR) anaysis

167 FT-IR spectrum of every kind of films was recorded on a Perkin Eimer spectrum 1000

168 (Varian Inc., USA) using KBr dispersive method. The film samples were ground to a powder after

169 frozen in liquid nitrogen, and lyophilized under vacuum. FT-IR analysis was conducted in the

170 wavenumber ranging from 4000 to 500 cm−1 with a resolution of 4 cm−1.

171 2.6.3. Thermogravimetric analysis (TGA)

172 The thermal stability of film was conducted by thermogravimetric analyzer (DTG-60 Shim

173 ADZU, Japan). Approximately 4 mg of the lyophilized film sample was placed in a ceramic

174 crucible and heated from 40 °C to 400 °C at a constant rate of 10 °C per minute under a flowing

175 nitrogen atmosphere.

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176 2.6.4. X-ray diffraction analysis

177 Wide-angle X-ray diffraction measurements were performed by a XRD diffractometer

178 (D8-Advance, Bruker, USA) at a voltage of 40 kV and 30 mA. The patterns with Cu Kα radiation

179 were recorded in the region of 2θ from 10 to 80 ° with a step speed of 2 °min-1.

180 2.7. Total phenolics content and antioxidant activity

181 In the present study, 25 mg of film sample were immersed in 5 mL of distilled water. The

182 mixed solution containing the film sample was stirred at 50 °C for 4 hours, and then centrifuged at

183 12,000 ×g for 5 min at 4 °C. The supernatant was taken for following total phenolics content and

184 antioxidant activity determination. The ABTS, DPPH, FRAP, Cu2+ reducing power were used to

185 measure antioxidant activities of the film [21].

186 2.7.1. Total phenolics content

187 Total phenolics content was determined according to Folin-Ciocalteu method [21]. 1mL

188 supernatant extract was added to 2.5 ml Folin Ciocalteu reagent (10 % v/v) followed by 2 ml

189 7.5 % (w/v) sodium carbonate solution. The mixture was incubated at 50 °C for 5 min before the

190 absorption was measured at 760 nm. According to standard curve of gallic acid obtained by the

191 same method, the total phenolics content of film was expressed as μg of gallic acid equivalents

192 (GAE) mg-1.

193 2.7.2. Antioxidant activity

194 The DPPH inhibition assay was determined with some modification from a previous method

195 [22]. The reaction system consisted of 1mL supernatant and 3mL 0.1 mM DPPH ethanol solution.

196 The reaction system was then mixed thoroughly and was incubated in a dark room at 25 °C for 30

197 min before the absorption was measured at 517 nm. The result is expressed as the clearance rate as

9
198 DPPH inhibition (%).

199 The ABTS radical scavenging activity of sample was determined according to method

200 reported by [23]. The ABTS was dissolved in water to reach 7 mM concentration. It was then

201 mixed with 2.45 mM potassium persulfate solution in 1:1 ratio for 16 h. The solution was then

202 diluted with ethanol until it reached the absorbance of 0.70 ± 0.02 at 734 nm. The reaction system

203 consisted of 1mL supernatant and 3mL 7.4 mM ABTS solution. The reaction system was then

204 mixed thoroughly and was incubated in a dark room at 25 °C for 10 min before the absorption was

205 measured at 734 nm. The result is expressed as the clearance rate as ABTS radical scavenging

206 (%).

207 Determination of FRAP was conducted from the method by [24] with some modification.

208 The reaction system prepared by 1 mL supernatant and 3 mL FRAP solution. The FRAP solution

209 consisted of TPTZ (10 mM) - HCl (40 mM ) solution, 20 mM FeCl3·6H2O solution and 0.3 M

210 acetate buffer (PH 3.6) :1:1:10 (v/v/v). The reaction system was then mixed thoroughly and was

211 incubated in a dark room at 25 °C for 30 min before the absorption was measured at 593 nm.

212 According to standard curve of FeSO4. 7H2O obtained by the same method, the FPAP was

213 expressed as mmol Fe( ) kg-1.

214 The Cupric ion (Cu2+) reducing power was determined by a previous method the [25]. The

215 reaction system consisted of 1mL supernatant, 1mL 5 mM copper chloride, 2.75 mM neocuproine

216 hydrate and 1mL 1 mM ammonium acetate. The reaction system was then mixed thoroughly and

217 was incubated at 25 °C for 30 min before the absorption was measured at 450 nm.Aqueous

218 solution of Trolox was used for calibration. Results were expressed as mmol Trolox equivalents

219 (TE) kg-1.

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220 2.8. Coating treatment and quality measurements of apple fruit

221 The preparation of the 1% (w/v) CS coating solution was done as per the method of the film

222 forming solution. According to the results on characterization of CS-4% BPE, CS-8% BPE and

223 CS-12% BPE films, 4% (v/v) of the BPE was used to prepare a CS-BPE coating solution. The

224 varieties of apples “Huangyuanshuai” was all divided into three groups, i.e. CK (Control Check),

225 CS and CS-BPE with each group containing 30 fruits. The treatment application of coatings on

226 apple was conducted according to our previous study [18].

227 The respiration rate, weight loss, firmness, soluble solids content (SSC), titratable acidity (TA)

228 and ascorbic acid (ASA) were used to represent the quality of apple fruit in storage. The quality

229 measurements of apple fruit were done as per our previous study [18]. All assays were carried out

230 in triplicates.

231 2.9. Statistical analysis

232 The Duncan test and one-way analysis of variance (ANOVA) were used for multiple

233 comparisons by SPSS 22.0 window. Results were considered statistically different if p < 0.05.

234 3. Results and discussion

235 The banana peel extract (BPE) had 12.56±0.21° SSC and a TPC of 3.48±0.15 mg/ml. Three

236 phenolic compounds including catechin, ferulic acid and kaempferol were identified and

237 determined in BPE by means of HPLC analysis and the content was 147.66±0.47 μg/ml,

238 18.95±0.63 μg/ml and 94.15±0.3 μg/ml respectively. In addition, the mean particle size of BPE is

239 67.99±0.89 μm.

240 3.1. Color and transparency

241 Fig. 1 suggests that though each film was transparent, the incorporation of different

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242 concentrations of BPE gradually increased the yellow color of the film, and the CS-12 % BPE

243 exhibited the most obvious yellow color, which was attributed to the higher amount of lutein in

244 ripe banana peel. This was also confirmed by the increase of b* as shown in Table 1. Compared

245 with the CS film, the incorporation of different concentrations of BPE significantly up-regulated

246 the b* value of the film, and the CS-12% BPE displayed the highest b* value (Table 1). Likewise,

247 biodegradable films incorporated with mango peel extracts have also been observed to have a

248 higher b* value [26]. Besides, with the rise in the concentration of BPE addition, the L* value of

249 film is in decline on a continued basis, while the a* value continue to increase (Table 1). The

250 increase in a* value remains attributed to the natural pigments contained in ripe banana peels. The

251 increase in L * value could be explained by the scatter light caused by phenolic substances in BEP,

252 thus resulting in the reduced film brightness [6].

253 The light barrier property of bio-based active film represents a critical parameter for food

254 packaging applications [27]. Table 1 shows that the incorporation of different concentrations of

255 BPE contributed to a significant enhancement to the opacity of the CS film, which is considered as

256 an advantage in the inhibition of lipid oxidation and preservation of the organoleptic properties for

257 the packaged food [28].

258 3.2. Thickness

259 As revealed by our results, the thickness of film exhibited an incremental increase with the

260 incorporation of different concentrations of BPE (Table 2). This was in agreement with those

261 reported for chitosan films incorporated with young apple phenol [29], mango peel extract [26],

262 and Nigella sativa seedcake extract [4].

263 3.3. Moisture content and water solubility

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264 The decreasing trends of the moisture content and water solubility were observed when

265 chitosan film was incorporated with BPE (Table 2). Compared with the CS film, the lower

266 moisture content and water solubility of the CS-BPE composite film are associated with the

267 phenolic substance contained in the BPE. The hydroxyl group and carboxyl group of the phenolic

268 substance show a stronger binding ability to the chitosan molecule, thereby reducing the binding

269 of chitosan to water molecules [30]. The low moisture content and water solubility film are

270 conducive to the packaging of moisture sensitive foods [31].

271 3.4. Water vapor permeability

272 In comparison with CS film, the CS-BPE composite film showed a lower water vapor

273 permeability (Table 2). This may be due to the interactions of hydroxyl and carboxyl groups of

274 BPE with the hydroxyl and amino groups in CS. This interaction, in turn, may resulting in more

275 narrow channel of film to inhibit water molecules passing [3]. A similar decline in water vapor

276 permeability was observed as well in chitosan composite films containing green tea extract [32].

277 3.5. Mechanical properties

278 The tensile strength (TS), elongation at break and tensile attributes-elastic modulus (TE) are

279 the most commonly used mechanical parameters for food packaging applications, which suggests

280 the capability to maintain integrity and properties for the packaged products [3]. The CS film

281 presented a TS and elongation at break of 37.76 MPa and 26.08 %, respectively. These results are

282 comparable to the values (TS: 48.72 MPa, elongation at break: 28.59%) of pure chitosan film in a

283 previous research [6]. However, These results are lower than that values (TS: 43.2 MPa, TE:

284 3.1GPa) of a film made from chitosan (CS) and carboxymethyl cellulose (CMC) [33]. This

285 difference is mainly attributed to the strong ion crosslinking of CMC and CS in mixed films.

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286 Compared with the CS film, though the CS-4 % BPE film made no significant difference to TS, it

287 exhibited the higher level of elongation at break and TE (Table 2). It is noteworthy that as the

288 concentration of BPE increased, the opposite occurred, with the significantly lower TS and

289 elongation at break for 8 % BPE and 12 % BPE films relative to CS and CS-4 % BPE films (Table

290 2). The improved mechanical properties of CS-4 % BPE composite film can be attributed to the

291 cross-linking role of BPE, resulting in a stronger binding between phenolic compounds in BPE

292 and chitosan molecules, however, the incorporation of excess BPE disrupted the basic internal

293 structure of the chitosan, resulting in a decrease in mechanical properties [4]. The similar

294 phenomena were also observed in CS films incorporated with Nigella sativa seedcake extracts [4],

295 Lepidium sativum seedcake extracts [5].

296 3.6. Morphology by scanning electron microscopy (SEM)

297 The microstructure and biopolymer compatibility of CS and CS-BPE films are exhibited in

298 Fig. 2. The surface of various films all were smooth indicating the high compatibility of matrix

299 and additives. Despite this, a number of small white spots were observed on the surface of the

300 CS-8 % BPE and CS-12 % BPE films. The similar small white spots appeared on the surface of

301 the CS film incorporated with purple-fleshed sweet potato extracts, which was attributed to

302 excessive aggregation of chitosan molecules with PSPE [27]. Under 1000 × magnification, the

303 cross section of the CS film exhibited a clear wrinkle, while the cross section of the CS-BPE film

304 is uniform and smooth. Under 3000 × magnifications (3000 ×), the cross section of the CS film

305 was roughness and cavitated, while the CS-4 % PBE was smooth and dense. The cross section of

306 CS-8 % BPE and CS-12 % BPE films exhibited a highly heterogeneous and porous structure at

307 3000 × magnifications, which may be due to the excessive content of BPE, resulting in phased

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308 separation (Fig. 2). Therefore, the incorporation of 4 % BPE is capable of making the structure of

309 the film more dense and uniform, whereas the high concentration of BPE (8 % and 12 %) leads to

310 the film being more porous, also demonstrating the more excellent mechanical properties of

311 CS-4 % BPE film than the CS film (Table 2).

312 3.7. Fourier transform infrared (FT-IR) anaysis

313 In the present study, (FT-IR) analysis was conducted to investigate the molecules interaction

314 between chitosan and BPE. As illustrated in Fig. 3, according to the literature [34], the

315 characteristic peaks of the CS films appeared at 1708, 1564 and 1336 cm-1 represented

316 respectively due to C=O stretching of amide group (amide I), N-H bending (amide II), and

317 HN-CO bending (amide III ). The broad peak shown at 3408 cm-1 was due to the overlapping

318 stretching vibration of O-H and N-H, and peaks at 1156 and 1140 cm-1 represent characteristic

319 saccharide structure [27]. Although no new characteristic peaks were observed due to the low

320 contents of BPE, it was worth noting that the incorporation of BPE leaded to some changes in the

321 FT-IR spectrum of CS film (Fig. 3). With the addition of BPE, the peak around 3408 cm-1 was

322 broadened, indicating that the combination of phenolics in the BPE with -OH or -NH2 in the

323 chitosan molecule resulting in a decline in free O-H and N-H stretching [35]. In addition, the peak

324 at 1568 cm-1 gradually shifted toward 1550 cm-1, which further proved the strong interaction

325 between the phenolics in BPE and the -NH2 of chitosan molecule [5]. However, no ester bond (at

326 1715 cm−1) and amide bond (at 1645 cm−1) were observed in the CS-BPE composite film,

327 indicating the molecular interactions was non-covalent bond interaction between BPE and CS

328 [36].

329 3.8. X-ray diffraction analysis (XRD)

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330 As illustrated in Fig. 4, the clear diffraction peak at around 14 ° was assigned to

331 crystallization peak of CS [36]. As BPE was incorporated into the CS film, the crystallization peak

332 at about 14 ° gradually disappeared, suggesting that the incorporation of PBE led to a decline in

333 the crystallinity of the CS film. This might be due to the molecule interaction between the chitosan

334 and the BPE, which changed the original arrangement of the chitosan molecule, resulting in the

335 formation of an amorphous complex [5]. Similarly, the diffraction peak was found to be weaken

336 and disappeared in chitosan composite film combined with apple polyphenol extract [29].

337 3.9. Thermogravimetric analysis (TGA)

338 The TGA and DTG thermograms of the CS and CS-BPE composite films are shown in Fig. 5.

339 And the detailed pyrolysis parameters are listed in Table S1 according to a previous study [37].

340 The first step in thermal degradation at 0-150 °C was mainly attributed to the evaporation of

341 loosely bounded water in the film. As shown in Fig. 5A, the incorporation of BPE reduced the

342 weight loss of CS film at this stage, which was consistent with the lower moisture content of

343 CS-BPE compisite film (Table 2). The second step in thermal degradation was observed at

344 150-500 °C, which was primarily attributed to the degradation of glycerol, decomposition of

345 chitosan molecules and BPE [34]. In comparison with the CS film, as the concentration of BPE

346 was up-regulated, the weight loss of CS-BPE composite films were gradually reduced in the

347 second stage (Fig. 5A). This is speculated to be attributed to the formation of more powerful

348 hydrogen bonds between phenolics substances in BPE and chitosan or interactions between

349 glycerol and BPE [27]. Furthermore, as seen from Table S1, the maximum thermal degradation

350 temperatures corresponding to the first process of CS film appeared at 148.3 °C, while it was

351 between 151.1-161.1 °C for the CS-BPE composite film. In brief, the CS-BPE composite films

16
352 demonstrate a superior thermal stability to the CS film. Additionally, it has been reported as well

353 that the CS film incorporated with purple-fleshed sweet potato extract exhibits a more desirable

354 thermal stability than the gelatin film [27].

355 3.10. Total phenolics content

356 One potential function of active packaging films is that the active compound can be released

357 by migration directly on the surface of the food, while different foods have a significant effect on

358 the release of the active compound of the film. Therefore, different food simulants are often used

359 to investigate the migration and release of active compounds of the film [21]. In this study, pure

360 water, 50 % ethanol, 95 % ethanol solutions were employed to represent aqueous medium,

361 oil-in-water emulsion medium and fatty or oil medium respectively. The total phenolics content of

362 the CS-BPE composite film in different food simulants was indicated in Fig. 6A. Overall, with the

363 concentration of incorporated BPE increased, the total phenolics content of film also increased

364 significantly. Importantly, the CS-BPE composite film showed significant differences in the total

365 phenolics content of different food simulants (Fig. 6A). The total phenolics content of each film in

366 water and 50 % ethanol solutions was discovered to be significantly higher than in the 95 %

367 ethanol solution. In addition to the difference in film water solubility, which is mainly attributed to

368 the hydrophilicity of the film that can be more thoroughly decomposed in pure water, more

369 phenolics substances were released [36]. As revealed by a recent study, the kinetics of migration

370 for phenolics from chitosan films indicated that phenolics have lower diffusivity in 96 % of the

371 environment [38].

372 3.11. Antioxidant activity

373 Despite phenolic substances being a major contributor to the antioxidant capacity of BPE,

17
374 other antioxidant active substances are found to be present in BPE as well, including carotenoids,

375 biogenic amines and ascorbic acid [39]. Therefore, in this study, the ABTS, DPPH, FRAP, Cu2+

376 reducing power were involved to measure antioxidant activities of the film. As shown in Fig.6, the

377 CS film exhibited a weak antioxidant activity, which was due to the capability of chitosan to form

378 stable macromolecule radicals through residual amino (NH2) groups and free radicals [40].In

379 general, the incorporation of BPE could improve the antioxidant capacity of the film significantly

380 when compared to the CS film (Fig. 6). The antioxidant activities increased with the concentration

381 of BPE. In addition, similar to the pattern shown by the total phenolic content, the antioxidant

382 activities of each kind of films in the aqueous solution were significantly enhanced with respect to

383 in the 95 % ethanol solution (Fig.6). From the results obtained from applying various antioxidant

384 methods, the order of increase in magnitude compared to the control film is as follows: FRAP＞

385 Cu2+ reducing power＞ABTS＞DPPH (Fig. 6). Notably, the total phenolics content of the

386 CS-12 % BPE film with the highest total phenolics content was 2.37 times higher in water

387 solution than in 95% ethanol (Fig. 6A), however, the FRAP of the CS-12 % BPE film was 3.44

388 times higher in water solution than in 95 % ethanol (Fig. 6D). This indicated that in addition to

389 phenolics substances in banana peel, it also contains other antioxidant active substances.

390 3.12. Coating treatment of the apple fruit

391 The effects exerted by the coatings on the respiration rate (A), weight loss (B), firmness (C),

392 SSC (D), TA (E) and ASA content (F) of apple fruit during storage at 25 ± 2 °C are demonstrated

393 in Fig. 7. Apple fruit has typical respiration climacteric nature, which makes fruit highly

394 perishable [38]. It is well known that a major way of chitosan coating to improve the quality of

395 postharvest fruits is to inhibit the gas exchange occurring on the fruit surface to reduce the

18
396 respiratory rate, thereby delaying fruit senescence [18]. The weight loss gradually increased with

397 respiration and water transpiration of postharvest fruit during storage.

398 As revealed by the present research, the respiration rate of apple exhibited a single peak in all

399 fruit at week 2 after treatment (Fig. 7A ). Compared with the uncoated group (CK), the application

400 of the CS and CS-BPE coatings invariably significantly reduced the respiration rate and weight

401 loss of fruit throughout the storage period. Importantly, CS-BPE group showed a lower respiratory

402 rate and weight loss of fruit than CS group throughout the storage period, suggesting that the

403 CS-BPE coating has more desirable inhibitory effects on the gas exchange occurring on the fruit

404 surface, which is mainly attributed to the denser structure of CS-BPE than CS in the

405 microstructure of the film, thus contributing to the stronger gas barrier capability. The similar

406 results have been reported in the case of guava coated with chitosan enriched with pomegranate

407 peel extract [41].

408 The main cause of the decreased firmness of harvested fruits lies in the increase in cell wall

409 hydrolase activity [42]. Fig. 7C shows that the values of fruit firmness for all the samples showed

410 a continuous decline during storage. Particular, the fastest decline was spotted as in week 3, which

411 is speculated to be due to the respiratory climacteric of apple fruit [43]. Both the CS and CS-BPE

412 coatings exerted a significant inhibitory effect on the declining firmness of the apple fruit, and the

413 incorporation of BPE created a more beneficial effect on maintaining the firmness than pure CS

414 coating. The results obtained from this research conformed to the findings of [44] where a positive

415 effect was reported on the firmness of coated peach when rhubarb extract was added into alginate

416 coatings. Usually, owing to the the conversion of starch to sugars, the SSC of apple fruit tends to

417 increase in the initial stage of storage and the content of organic acids would gradually decrease as

19
418 a substrate for respiration over storage [45]. The SSC of apple fruits increased first, prior to a

419 constant decline during storage (Fig. 7D). The SSC in the CS and CS-BPE coating group showed

420 a lower level than uncoated fruit in week 3. Both the CS and CS-BPE coatings inhibited the

421 decrease in TA of apple over storage considerably (Fig. 7E), with the CS-BPE group shown to

422 have a higher TA than CS. In addition, The CS and CS-BPE coatings maintained a higher content

423 of ASA than uncoated fruit in the late stage of storage (Fig. 7F), and CS-BPE coating exerts an

424 impressive effect when compared to CS coating.

425 4. Conclusion

426 The incorporation of BPE contributed to the changes to the physical and mechanical

427 properties possessed by chitosan films. The water solubility, moisture content and water vapor

428 permeability of the CS-BPE composite film were discovered to be significantly lower than the CS

429 film, indicating that the incorporation of BPE made difference to the original bond formed

430 between the CS-CS and CS-water. This was further confirmed by the results obtained from FT-IR

431 anaysis, TGA and X-ray diffraction analysis. The mechanical properties exhibited by CS-BPE

432 composite film was closely associated with the concentration of BPE incorporated. Compared

433 with CS film, the incorporation of 8 % and 12 % BPE reduced the TS and elongation at break of

434 the film, while the incorporation of 4 % BPE on the film TS produced only insignificant effect,

435 despite the increase in elongation at break of the film. The smoother surface and denser

436 cross-section of the film as observed by SEM analysis evidenced the improvement to the

437 mechanical properties of CS-4 % BPE film. The CS-BPE composite film showed excellent

438 antioxidant activity in different food simulants. In addition, the results demonstrated that the

439 application of CS-BPE coating led to more positive effects on the preservation of apple fruits

20
440 during room temperature storage when compared with the CS coating and the control, as

441 confirmed by the physiological quality including lower respiration rate, weight loss, and SSC

442 higher firmness, TA and ASA content. Therefore, the incorporation of BPE into chitosan film and

443 coating is believed as an effective strategy to improve the value of banana peel waste. Therefore,

444 the application of BPE on active film and coating prepared from other biopolymers is worthy of a

445 further study so as to maximize the value of banana peel waste.

446 Acknowledgements

447 This research was supported by the National key R & D projects (No. 2018YFD0401302) of

448 china.

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568

26
569 Fig captions:

570 Fig.1. Appearance of BPE modified and unmodified chitosan films.

571 Fig.2. SEM micrographs of the surface (A, B, C and D) and cross-section (E1, E2, F1,F2, G1, G2,

572 H1 and H2) of CS film (A, E1 and E2), CS-4% BPE film (B, F1 and F2), CS-8% BPE film (C, G1

573 and G2), and CS-12% BPE film (D, H1 and H2). Magnification was × 2000 for A, B, C and D,

574 was × 1000 for E1, F1, G1 and H1 and was × 3000 for E2, F2, G2 and H2.

575 Fig.3. FT-IR spectra of CS film (A), CS-4% BPE film (B), CS-8% BPE film (C) and CS-12% BPE

576 film (D).

577 Fig.4. X-ray diffraction pattern of CS film (A), CS-4% BPE film (B), CS-8% BPE film (C) and

578 CS-12% BPE film (D).

579 Fig.5. Thermogravimetric curves (A) and first derivative curves (B) of CS film (a), CS-4% BPE

580 film (b), CS-8% BPE film (c) and CS-12% BPE film (d).

581 Fig.6. The total phenolics content antioxidant assessment of the CS and CS-BPE composite films

582 in different food stimulants. The error bars indicated the standard deviation. Bars with different

583 letters represent statistical differences (P < 0.05).

584 Fig.7. Effect of CS and CS-BPE coatings on respiration rate (A), weight loss (B), firmness (C),

585 SSC (D), TA (E) and ASA content (F) of apple fruit during storage at 25 ± 2 °C for 5 weeks. Each

586 value represents the mean for three replicates, and vertical bars indicate the standard deviations for

587 each treatment (n=3). Bars with different letters represent statistical differences (P < 0.05).

588 Untreated fruits were used as control.

589

27
590

591

592

28
593

594

595

596

597

29
598

599

600

601

602

30
603

604

Table 1. Color and opacity of chitosan films without and with different contents of BPE.

Films L* a* b* Opacity
(A mm−1)
CS
78.91±0.75a 6.03±0.75d 14.72±1.03d 0.81±0.11b

CS-4%BPE
76.87±0.64b 10.63±0.97c 53.33±3.09c 1.06±0.12a

CS-8%BPE
75.45±1.00c 12.98±1.74b 60.19±4.53b 1.05±0.12a

CS-12%BPE
73.31±1.22d 15.75±2.07a 64.77±3.61a 1.13±0.09a

31
 a Values followed by the same letter in the column on the same day were not significantly
different according to Duncan’s Multiple Range Test (P < 0.05). Data are accompanied by
standard errors of the means (n ≥ 3).
605
606
607
608
609

610

611

612

613

614

615

616

Table 2. Thicknesses, moisture contents, water solubility, water vapor permeability and mechanical properties of chitosan fi
of BPE.
Films Thickness Moisture Water Water vapor Tensile
(μm) contents (%) Solubility (%) permeability (10−11 g m−1 strength (MPa)
s−1 Pa−1)
CS
51.09±5.59d 24.29±2.03ab 17.52±0.91a 16.78±1.16a 37.76±3.55a

CS-4%BPE
61.72±5.23c 24.8±3.70a 17.13±0.83a 14.26±1.39b 35.05±3.45a

CS-8%BPE
73.00±5.76b 19.83±2.28bc 13.86±1.05b 13.45±1.66c 23.02±2.00b

CS-12%BPE
80.90±6.36a 18.36±0.76c 13.10±1.05b 10.56±1.82d 21.56±2.29b

a Values followed by the same letter in the column on the same day were not significantly different according to Duncan’
are accompanied by standard errors of the means (n ≥ 3).
617
618
619
620
621

622

32
623

624

625

626

627

628

629 Highlights

630 1. Chitosan (CS) films incorporated with banana peels extract (BPE) were developed.

631 2. BPE affected films’ physical, mechanical and structural properties.

632 3. Films incorporated with 4% BPE showed better functionality.

633 4. Antioxidants could be released from the CS-BPE film in different food simulants.

634 5. CS-BPE coating more effectively improved the quality of apple fruit than CS coating.

635

636

637

638

639

640

33