Accepted Manuscript

Title: Preparation and characterization of tragacanth-locust

bean gum edible blend films

Author: Fatemeh Sadat Mostafavi Rassoul Kadkhodaee

Bahareh Emadzadeh Arash Koocheki

PII: S0144-8617(15)01159-5
DOI: http://dx.doi.org/doi:10.1016/j.carbpol.2015.11.069
Reference: CARP 10588

To appear in:

Received date: 30-4-2015

Revised date: 3-11-2015
Accepted date: 26-11-2015

Please cite this article as: Mostafavi, F. S., Kadkhodaee, R., Emadzadeh,
B., and Koocheki, A.,Preparation and characterization of tragacanth-
locust bean gum edible blend films, Carbohydrate Polymers (2015),
http://dx.doi.org/10.1016/j.carbpol.2015.11.069

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1 Preparation and characterization of tragacanth-locust bean gum edible blend films
2

3 Fatemeh Sadat Mostafavia*, Rassoul Kadkhodaeeb, Bahareh Emadzadehc, Arash Koochekid

t
ip
a
5 Department of Food Nanotechnology, Research Institute of Food Science and Technology, PO
6 Box: 91735-147, Mashhad, Iran, f.mostafavi@rifst.ac.ir
b
7 Department of Food Nanotechnology, Research Institute of Food Science and Technology, PO

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8 Box: 91735-147, Mashhad, Iran, r.kadkhodaee@rifst.ac.ir
c
9 Department of Food Nanotechnology, Research Institute of Food Science and Technology, PO

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10 Box: 91735-147, Mashhad, Iran, b.emadzadeh@rifst.ac.ir
d
11 Department of Food Science and Technology, Ferdowsi University of Mashhad (FUM), PO
12 Box: 91775-1163, Mashhad, Iran, koocheki@um.ac.ir
13
14 *. Tel: +989151194101; fax: 985135425422 an
15
M
16 Abstract
17 The present work introduces the structure and physicomechanical properties of a novel blend
18 film made from binary solutions of gum tragacanth (GT) and locust bean gum (LBG) at different
d

19 mixing ratios. Apparent viscosities and surface tensions of individual and blend gum solutions
e

20 were also investigated. The viscosity data indicated that there was a distinct synergism between
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21 the two gums at all mixing ratios. FTIR spectra showed the existence of noncovalent
22 intermolecular interactions between gums. The surface tensions of binary solutions were
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23 significantly lower than those of individual gums which is advantageous for coating applications.
24 All films had homogenous and smooth surface morphology and their transparency, water vapour
Ac

25 barrier and mechanical properties were improved by incorporating LBG in blend. The results of
26 this study suggest that GT-LBG blend film, owing to its desirable properties, has the potential to
27 be used as a new degradable food packaging material.
28
29 Keywords
30 Edible films, Synergism, Blend film, Gum tragacanth, Locust bean gum.
31
32 1. Introduction

Page 1 of 26
33 The increased production and wide application of synthetic petroleum based films and
34 coatings have grown rapidly over the past few decades which has caused serious
35 environmental pollution due to the fact that they are non-biodegradable (Muscat, Adhikari,
36 Adhikari & Chaudhary, 2012). In order to solve this problem, researchers have focused on
37 using biodegradable materials for food packaging purposes (Khwaldia, Arab Tehrany &

t
38 Desobry, 2010; Persin, Stana-Kleinschek, Foster, Van Dam, Boeriu & Navard, 2011).

ip
39 Edible films and coatings are natural and biodegradable compounds that can potentially

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40 be used for packaging of various food products to extend their shelf life and prevent their
41 quality loss by preventing the transfer of moisture, lipids, flavors or gases across the

us
42 package. Moreover, they can minimize mechanical damage during handling by forming a
43 continuous solid layer around the food surface. Also, they can be used as a carrier of
44
45
an
desirable additives such as flavors, nutrients, colorings and antimicrobials (Pavlath & Orts,
2009).
M
46 Materials used for production of edible films are usually proteins, polysaccharides or lipids. The
47 potential of polysaccharides as edible films and coatings has long been recognized (Nieto, 2009).
48 They usually have the ability to create a continuous network which is responsible for the film
49 functional properties (Falguera, Quintero, Jiménez, Muñoz & Ibarz, 2011; Giancone, Torrieri,
d

50 Masi & Michon, 2009). Increasing shelf life of fruit and vegetables, reducing oil uptake during
51 frying and retarding the loss of flavors and vitamins in the course of processing and storage of
e

52 food products are some of the various applications of polysaccharide films and coatings (Albert
53 & Mittal, 2002; Chien, Sheu & Yang, 2007; Garcıa, Ferrero, Bertola, Martino & Zaritzky, 2002;
pt

54 Kim, Lim, Bae, Lee & Lee, 2011; Maftoonazad & Ramaswamy, 2005; Marcuzzo, Sensidoni,
55 Debeaufort & Voilley, 2010; Teng, Luo & Wang, 2013).
56
ce

57 Over the few past decades, various polysaccharides have been evaluated and introduced as novel
58 film-forming materials for food packaging purposes. However, there is still a considerable
59 requirement for the development of new edible packaging materials to fulfil the increasing
Ac

60 consumer demands for more natural foods which need to be packed and also to meet the
61 environmental concerns (Jouki, Tabatabaei Yazdi, Mortazavi & Koocheki, 2013). Previous
62 works have shown that a number of biopolymers which are currently known as food thickeners
63 or stabilizers could also be used for film formation or coating applications (Phan The,
64 Debeaufort, Voilley & Luu, 2009). In our preliminary studies, capabilities of gum tragacanth
65 (GT) were investigated as a new film forming agent and it was found to have appropriate
66 properties to be considered for this purpose.
67
68 GT, also known as katira, is a dried exudate obtained from trunks and branches of different
69 species of Astragalus and grows wildly in South West Asia, particularly in Iran and Turkey.
70 Chemically, GT is a complex, highly branched and anionic polysaccharide consisting of small

Page 2 of 26
 71 proportions of protein. It is comprised of two main fractions termed as tragacanthin which is
72 soluble in water and bassorin which represents 60–70% of the total gum and has the capacity to
73 swell and form a gel (Weiping, Phillips & Williams, 2000). Since 1961 GT has been accepted as
74 GRAS at the level of 0.2- 1.3% (Balaghi, Mohammadifar, Zargaraan, Gavlighi & Mohammadi,
75 2011). This gum has been employed as a stabiliser, thickener, emulsifier and suspending agent in
76 food products such as sauces, drinks, jellies and frozen desserts due to its high water binding
77 ability, efficient suspending action and effective surface-active and emulsifying properties

t
78 (Nussinovitch, 2009; Weiping, Phillips & Williams, 2000). However a few studies have

ip
79 investigated the properties of GT as a coating or film forming material (Shrestha, Arcot &
80 Paterson, 2003; Şükran & BAYRAKTAR—ALPMEN).
81

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82 Locust bean gum (LBG) is also a suitable candidate for food packaging material among natural
83 polysaccharides. This gum which is a non-ionic hydrocolloid, naturally exists in the endosperm
84 of Ceretonia siliqua seeds (Martins, Cerqueira, Bourbon, Pinheiro, Souza & Vicente, 2012;

us
85 Mikkonen, Heikkilä, Helén, Hyvönen & Tenkanen, 2010). It consists of a β-(1-4)-D-
86 mannopyranosyl backbone with α-D-galactopyranosyl substituted on C6 of mannose and hence
87 they are known as galactomanan. The ratio of mannose to galactose in this gum is approximately
88 3.5:1. LBG is only slightly soluble in cold water and requires heating to become fully hydrated
89
90
an
and achieve maximum viscosity. It has the ability to form viscous solutions at relatively low
concentrations and produce compact and dense films and coatings with good mechanical and
91 water vapour barrier properties. LBG has been extensively studied for film formation and coating
M
92 applications (Aloui et al., 2014; Bozdemir & Tutas, 2003; Cerqueira, Lima, Teixeira, Moreira &
93 Vicente, 2009; Chen & Nussinovitch, 2000, 2001; Mikkonen, Heikkilä, Helén, Hyvönen &
94 Tenkanen, 2010).
95
d

96 The blending of two or more biopolymers could effectively change the rheological properties of
97 hydrocolloids solutions and improve physic-mechanical properties of corresponding film or
e

98 coating (Phan The, Debeaufort, Voilley & Luu, 2009). Martins, Cerqueira, Bourbon, Pinheiro,
99 Souza and Vicente (2012) reported that synergistic interactions between LBG and ĸ-carrageenan
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100 could effectively improve the visual, structural, mechanical and barrier properties of the obtained
101 blend films. Moreover, a number of other studies have been carried out to investigate the
102 properties of blend films made from Konjac glucomannan and curdlan, cassava starch and
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103 arabinoxylan, Konjac glucomannan and gellan gum and also chitosan and aloe vera gel
104 (Khoshgozaran-Abras, Azizi, Hamidy & Bagheripoor-Fallah, 2012; Phan The, Debeaufort,
105 Voilley & Luu, 2009; Wu et al., 2012; Xu, Li, Kennedy, Xie & Huang, 2007).
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106
107 However, no attempt has yet been made to study the characteristics and applications of LBG/GT
108 blend as an edible film forming agent. The objective of the present study was, therefore, to
109 evaluate the interactions between LBG and GT at different ratios and to develop films made
110 from blending these two biopolymers with potential applications as edible films and coatings.
111 Furthermore, the viscosity of film forming solution and also the miscibility, structural and
112 mechanical properties of blend films were investigated by viscometer, FT-IR, SEM and tensile
113 analyzer.
114
115

Page 3 of 26
116 2. Materials and Methods

117 2.1. Materials

118 GT exudates and carob seeds were purchased from local markets in Isfahan, Iran and
119 Kazeroon, Iran, respectively. Ethanol and acetone reagents used for extraction and

t
120 purification of gums were of analytical grade from Mojallal, Mashhad, Iran. Diethyl ether

ip
121 reagent was purchased from Merck, Darmstadt, Germany.

cr
122 2.2. Gum preparation
123 LBG was extracted and purified based on the procedures described by Dakia, Blecker,

us
124 Robert, Wathelet and Paquot (2008) and da Silva and Gonçalves (1990), respectively with
125 some modifications. Briefly carob seeds were immersed in distilled water at 100 for 1 h.
126
127
an
The seeds were then removed from water and the endosperms were separated, dried and
powdered. A 2% (w/w) dispersion of the endosperm powder in distilled water was made
M
128 and after stirring moderately for 1 hour, it was heated at 80℃ for 2 hours with continuous

129 stirring. The resulting solution was allowed to cool, centrifuged for 15 min at 20000 g
d

130 (25℃) and the supernatant was recovered. The solubilized galactomannan was precipitated
e
pt
ce

131 from the crude LBG solution by pouring into a two volume excess of ethanol. The white
132 precipitate was collected by filtration and washed with isopropanol, acetone and diethyl
133 ether. LBG was freeze-dried after purification and kept in desiccator until further use. GT
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134 exudates were prepared according to the method described by Azarikia and Abbasi (2010)
135 and Balaghi, Mohammadifar, Zargaraan, Gavlighi and Mohammadi (2011). They were
136 powdered by an electric mill and sieved using a laboratory screen (mesh No: 45) to obtain
137 particles of the same size.
138
139 2.3. Film preparation

Page 4 of 26
140 All edible films were prepared by using the casting method. Individual film-forming
141 solutions were prepared by dissolving 1% (w/w) of each gum powder in deionized water.

142 LBG required heating for complete solubilisation. Therefore it was heated at 80℃ for 1

143 hour using magnetic stirrer. After dissolution the gum solutions were left to stand

t
144 overnight at 4℃. Binary solutions of gums were prepared according to the formulations

ip
145 presented in Table 1 followed by stirring for 10 minutes at room temperature. Film-
146 forming solutions were centrifuged at 1500 rpm for 5 minutes to remove air bubbles before

cr
147 casting into plates. 40 ml of each gum solution was casted into Teflon plates of 10 cm in

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148 diameter and dried using air oven at 30℃ for 24 hours. They were then carefully peeled

149 off the plates and kept in a conditioning desiccator containing saturated Mg(NO3)2 to

150

151
an
create 52.80 ± 0.20% relative humidity (RH) at 23℃ to reach a constant weight.
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152
153 2.4. Determination of physical properties of film-forming solutions
154 2.4.1. Apparent viscosity
d

155 Apparent viscosities of individual gum solutions at different concentrations (0.25, 0.5,
e

156 0.75 and 1% w/w) were investigated. Also the apparent viscosities of blend gum solutions
157 having 1% w/w gum concentrations at different GT/LBG ratios (25/75, 50/50 and 75/25)
pt

158 were measured by a rotational viscometer (DV III ULTRA, Brookfield Engineering

Laboratories, USA) using spindle No SC4-18 at constant temperature of 25±0.5 ℃ and

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159

160 shear rate of 11s-1. All measurements were carried out in duplicate.
161
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162 2.4.2. Synergism

163 Apparent viscosities of GT/LBG binary solutions were investigated as a function of
164 their blending ratio. Synergism determination was carried out by comparing the measured
165 apparent viscosities of blends with their expected ones. The latter were calculated by
166 concentration addition method (CAM) and viscosity addition method (VAM) using
167 Equations 1 and 2, respectively.
168

Page 5 of 26
169 µCAM = x1.µ LBG + x2 .µ GT (1)
170
171 µVAM = µ x LBG + µ x GT (2)
1 2

172
173 µCAM in Equation (1) refers to the expected viscosity calculated by CAM method, x1

t
ip
174 and x2 are the fractions of LBG and GT and µ LBG and µ GT are the apparent viscosities of
175 1% (w/w) LBG and 1% (w/w) GT solutions, respectively. 1% w/w is the gum

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176 concentration in film forming solution.
177 µVAM in Equation (2) is the expected viscosity calculated by VAM method, µ x LBG and

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1

178 µ x TG are the apparent viscosities of each gum fraction in the final blend solution (Liang et
2

179 al., 2011).

180
an
181 2.4.3. Fourier transform infrared (FTIR) spectroscopy
M
182 In order to study the possible interactions between gums in their binary solutions FTIR
183 spectra of films were recorded on a FTIR spectrophotometer (AVATAR 370 FTIR
184 Thermo Nicolet, USA) with a resolution of 2 cm−1 within the spectral range of 4000–400
d

185 cm−1.
e

186
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187 2.4.4. Surface tension

188 Surface tensions of film-forming solutions were measured using a Krüss K100
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189 tensiometer (Germany) with a jacket linked to a water circulating system (25 ± 0.1 ℃).
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190 The Wilhelmy plate method was used with a roughened platinum plate. Deionized water
191 was used to calibrate the tensiometer before measurements and surface tension data were
192 taken 5 minutes after placing the plate on the dispersion surface. Three replicates were
193 carried out for each sample.
194

Page 6 of 26
195 2.5. Physical properties of films
196 2.5.1. Film thickness and density
197 The thickness of the films was measured using a digital micrometer (Mitutoyo,
198 Manufacturing Co. Ltd., Japan) with an accuracy of 0.001 mm. At least ten measurements
199 were made at random locations on each film and the data averaged. Two films of each

t
200 blend were used for measurements.

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201 Films were cut in circle shapes with t diameter of 6.50 cm. The film density (ρ) was
202 calculated from its weight and dimensions (Seyedi, Koocheki, Mohebbi & Zahedi, 2014)

cr
203 according to the following Equation:

us
m
204 ρ= (3)
A. h
205 where A is the film area (33.17 cm2), h is the film thickness (cm), m is the film dry mass
206
207
an
(g) and ρ is the dry matter density of film (g.cm-3).

208 2.5.2. Retraction ratio

M
209 Retraction ratios of the films were calculated using Equation (4):
h1 − h2
210 R= (4)
d

h1
211 where R is the retraction ratio, h1 is the initial film thickness before drying and h2 is the
e

212 final film thickness after drying in oven at 30℃ (Phan The, Debeaufort, Voilley & Luu,
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213 2009). Retraction ratios were measured in triplicate.

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214
215 2.5.3. Moisture content (MC)
216 The moisture contents of film specimens (2cm×2cm) were analyzed gravimetrically by
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217 oven drying method at 103 ± 2℃ for 24 hours (Seyedi, Koocheki, Mohebbi & Zahedi,

218 2014). The moisture content was calculated using the following Equation:
Mi − M f
219 MC = ×100(5)
Mi
220 where Mi and Mf are the initial and final weights of film samples, respectively.
221

Page 7 of 26
222 2.5.4. Moisture absorption (MA)
223 Moisture absorptions of films were determined according to the method described by
224 Seyedi, Koocheki, Mohebbi and Zahedi (2014). Film samples (2cm×2cm) were first
225 placed in a desiccator containing silicagel (0%RH) to reach a constant weight. After initial
226 weighing they were conditioned in a desiccator containing saturated potassium sulfate

t
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227 solution (97±1% RH) at 25℃ for 48 hours. The moisture absorption was calculated using

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us
228 the following Equation:
Wt − W0
229 MA = ×100(6)

230
W0 an
where W0 and Wt are the initial and final weights of samples at t=0 and t=48 hours,
231 respectively.
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232
233 2.5.5. Water vapour permeability (WVP) and water vapour transmission rate (WVTR)
d

234 WVP and WVTR of films were measured gravimetrically according to the ASTM E96-
e
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235 00 method with a 100% moisture gradient at 25℃ (ASTM, 2000). Before measurements,
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236 film specimens were conditioned in a desiccator containing saturated magnesium nitrate to
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237 reach the relative humidity of 52% at 25℃. Preconditioned films were fixed hermetically

238 on circular permeation cups with a diameter of 6.5cm containing deionized water leaving
239 an air gap of 2 cm between film and water. Test cups were then placed at a desiccator
240 containing silicagel to maintain 0% relative humidity inside the desiccator chamber and

241 stored in 25℃. Water vapour transmission was determined by weighing the cups

242 periodically to the nearest 0.0001g. Weight changes were recorded to provide eight data

Page 8 of 26
243 points and were then plotted as a function of time. WVTR was calculated from the slope of
244 the straight line fitted on these data (R2> 0.99) using equation (8). WVP was obtained
245 using equation (7).
slope ∆m
246 WVTR = = (7)
A ∆tA

t
247

ip
WVTR × X
248 WVP = (8)
∆P

cr
249
∆m

us
250 where is the rate of weight of moisture increase per time (g/s), A is the effective
∆t
251 surface area of film (m2) in test cup, X is the film thickness (m) and ∆P is the difference
252
253
an
between water vapour pressure across the film surface (Pa). All measurements were
carried out in triplicate.
254
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255 2.5.6. Transparency
256 Film transparency was determined using a UV-visible spectrophotometer (Shimadzu
d

257 UV-160) according to the method described by Prakash Maran, Sivakumar,

258 Thirugnanasambandham and Sridhar (2013). Briefly, film specimens were cut into 4cm ×
e

259 1cm rectangular pieces and their transparency were recorded at 560nm against an empty
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260 spectrophotometer cell as blank. The film transmittance was calculated according to the
261 following Equation:
ce

Tf
262 %T = ×100 (9)
TB
Ac

263 where Tf is the transmittance of film sample fixed on an empty cell and TB is the
264 transmittance of empty cell. The transmittance measurements were carried out in triplicate.
265
266 2.5.7. Scanning electron microscopy (SEM)
267 Scanning electron microscopy (LEO 1450 VP) was used to study the surface
268 morphology and cross section structure of films. For cross section studies film strips were
269 first vitrified in liquid nitrogen and then broken into half by hand. Film specimens were
270 fixed on sample holder with aluminum tapes followed by sputtering them with a layer of

Page 9 of 26
271 gold-palladium using a sputter coater (SC- 1620). SEM micrographs were obtained under
272 high vacuum condition at 20kV using back scattering technique. Cross section
273 micrographs were prepared at tilt angles of 60-90 degrees relative to the electrons beam.
274
275 2.5.8. Mechanical properties

t
276 Mechanical properties of film specimens including their tensile strength (TS) and

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277 elongation at break (EB%) were evaluated using a texture analyzer (SMS TA-XT2, UK)
278 according to the method described by ASTM D882-02 standard method (2002). Briefly,

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279 film samples were cut into 10 mm× 90 mm rectangular shapes and stored at 25℃ and 50 ±

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280 2% RH to reach constant weight. After conditioning, film strips were fixed tightly between
281 the device grips, with initial separation distance set at 8 cm, and were pulled apart with a
282

283 %TS =
f
×100 (10)
an
speed of 12.5 mm/min. TS was calculated according to the following equation:

x.w
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284 Were f is the maximum force (N), x is the film thickness (mm) and w is the width (mm)
285 of the film strip.
286 EB (%) was determined according to the following Equation:
d

dr
% EB = ×100 (11)
e

287
d0
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288 where dr is the distance of rupture (cm) and d0 is the initial grip separation distance
289 (cm). All measurements were performed with at least three replications.
ce

290
291 2.6. Statistical analysis
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292 The experiments were factorial with a completely randomized design. MSTAT-C
293 software (version 2.10, 1989) was used to analyze the resulting data. Significant
294 differences among the means were initially evaluated by analysis of variance (one-way
295 ANOVA), and then a Duncan’s multiple range test was employed to detect significant
296 differences at p<0.05.
297
298 3. Results and Discussion
299 3.1. Physical properties of film-forming solutions

10

Page 10 of 26
300 3.1.1. Apparent viscosity
301 The curves in Fig. 1 demonstrate that the measured blend viscosities at all blending
302 ratios were largely greater than the expected values calculated based on CA and VA
303 methods. According to Liang et al. (2011) method, a synergistic effect is observed if the
304 measured blend viscosity is greater than both the CAM and VAM calculated viscosity

t
305 values. This means that a synergism exists between the two biopolymers in this research

ip
306 which could be attributed to their extensive intermolecular interactions. The difference
307 between the measured blend viscosity and the calculated ones (CAM and VAM) differs

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308 among the blending ratios. Maximum synergistic effect was observed at the GT/LBG

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309 blending ratio of 75/25. This could be related to the changes in the intensity of the
310 intermolecular interactions occur between the two biopolymers at different blending ratios.
311 In previous studies synergistic interactions have been observed between LBG and some
312
313
an
other biopolymers such as xanthan and ĸ-carrageenan (Martins, Cerqueira, Bourbon,
Pinheiro, Souza & Vicente, 2012). It has been assumed to be the result of strong
M
314 interactions between unsubstituted portions of LBG backbone with the second biopolymer
315 molecules (Fernandez, Palazolo, Bosisio, Martínez & Wagner, 2012; Mathur, 2011). This
316 could also be true for LBG and GT blend solutions in this study. However, more studies
d

317 are yet required to fully understand the phenomenon and clearly explain the possible
e

318 interactions. Synergistic biopolymer interactions are attractive in the food industry because
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319 they impart novel sensory, textural and rheological characteristics to food products and
320 also reduce polymers costs. Furthermore, these interactions could improve the properties
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321 of edible films made thereof (Martins, Cerqueira, Bourbon, Pinheiro, Souza & Vicente,
322 2012; Moghaddam, Razavi & Emadzadeh, 2011).
323
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324
325
326 3.1.2. FTIR spectroscopy
327 Fig. 2 shows the FTIR spectra of individual GT and LBG as well as their blends at
328 different ratios over the wave number range of 400-4000 cm-1. A comparison of these
329 spectra explicitly indicates two strong absorption bands for the blends centered at 2800-
330 3000 cm-1 and 3700-3100 cm-1. The former is attributed to CH stretching of methyl groups
331 that shows increased absorption with the increase of LBG ratio in the blend as a sign of

11

Page 11 of 26
332 intermolecular hydrogen bonding (Cerqueira, Lima, Teixeira, Moreira & Vicente, 2009;
333 Singh & Sharma, 2014). The latter, on the other hand, is assigned to the stretching of OH
334 groups which denotes to the formation of hydrogen bonds between hydroxyl groups of
335 polysaccharides and water. In the spectra of blend films it is possible to observe changes in
336 the intensity and position of the peaks. The strong absorption bands centered at 3700–3000

t
337 cm−1 attributed to the stretching of intermolecular hydrogen bonds showed significant

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338 changes. They broadened and shifted to a lower wave number as the LBG content
339 increased. This suggests the increase of intermolecular hydrogen bonds between GT and

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340 LBG which is a good evidence for their miscibility and the main reason for the occurrence

us
341 of synergistic viscosity as seen in section 3.1.1. The hydrogen bonds mainly result from
342 the interactions between carboxyl groups (–COO−) and –OH or –COCH3 groups as
343 previously reported for LBG and ĸ-carrageenan, carboxymethylcellulose and
344
345
an
hydroxyethylcellulose, Konjac glucomannan and Curdlan and Konjac glucomannan and
gelan gum binary systems (Martins, Cerqueira, Bourbon, Pinheiro, Souza & Vicente,
M
346 2012; Wu et al., 2012; Xu, Li, Kennedy, Xie & Huang, 2007; Zhang, 1999).
347
348
d

349 3.1.3. Surface tension

e

350 The surface tension results are reported in Table 2. It was found that the surface
351 tensions of GT/LBG solutions at all mixing ratios were significantly (p<0.05) lower
pt

352 compared to that of the individual gum solutions. The decrease in surface tension of gum
353 solutions has previously been reported by using blending technique. García, Pinotti,
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354 Martino and Zaritzky (2009) reported that chitosan and methylcellulose blend gum
355 solutions had lower surface tensions in comparison with their individual gum solutions.
Ac

356 This could be due to the interactions between polysaccharides which changes the gum
357 structure and functional properties and could be extended to the results in the current
358 research. A comparison between the surface tension values in this study and Garcia et al.,
359 2009 research shows that the GT and LBG gum solutions and their blends have all lower
360 surface tensions. This could be due to the difference in their chemical structure and shows
361 that GT/LBG blends could be used as alternatives to chitosan and methylcellulose gums.

12

Page 12 of 26
362 Surface tension is an important property for food coating solutions. It critically affects
363 the suspension spreadability (the ability of a coating solution to spread over a solid surface
364 and adhere to it) and integrity of coating layer on food surfaces after drying. Fresh food
365 products such as vegetables naturally have low surface tensions (eg. Strawberry: 28.94
366 mN/m, tomato: 28.71 mN/m, carrot: 26.48) which interferes with complete coating of

t
367 surfaces by aqueous solutions (Pavlath & Orts, 2009). It has been reported that higher

ip
368 surface tension of coating solution than that of substrate, usually generates beads on the
369 surface leading to a thin, poor and disintegrated layer. Conversely, the coating solution

cr
370 will flow out smoothly on the product surface if it has a surface activity lower than the

us
371 food substrate. Therefore, modification of coating formulation is required for better
372 adhesion. Usually surfactants, plasticizers or lipids are added to the formulation to
373 decrease its surface tension (Carneiro-da-Cunha, Cerqueira, Souza, Souza, Teixeira &
374
375
an
Vicente, 2009; Casariego, Souza, Vicente, Teixeira, Cruz & Díaz, 2008; Ribeiro, Vicente,
Teixeira & Miranda, 2007).
M
376
377
378 3.2. Physical properties of films
d

379 3.2.1. Thickness and density

e

380 The results of films thickness and density measurements are summarized in Table 3.
381 Film thickness varied from 44.50 to 46.97 µm. However, no significant difference
pt

382 (p<0.05) was observed between the thickness of film samples at all mixing ratios. This
383 could be the result of restricted control of dry mass of film solution per unit area of plates
ce

384 during casting process which was also reported by Pelissari, Andrade-Mahecha, do Amaral
385 Sobral and Menegalli (2013). Changing the blending ratio had also no significant effect
Ac

386 (p<0.05) on films density. In previous studies similar thickness and density values were
387 observed for films made from blending agar and cassava starch, LBG and Lipidium
388 perfoliatum seed gum (Kurt & Kahyaoglu, 2014; Phan The, Debeaufort, Voilley & Luu,
389 2009; Seyedi, Koocheki, Mohebbi & Zahedi, 2014).
390
391

392

13

Page 13 of 26
393

394

395

t
396

ip
397

cr
398

us
399

400
401
402
3.2.2. Retraction ratio
an
The retraction ratio of individual and blend films varied from 99.15 to 99.20% and did
M
403 not differ significantly (p<0.05) between samples [Table 3]. This means that all film
404 samples retracted at almost the same rate during drying and the interactions between
405 hydrocolloids did not distinctly affect this phenomenon. The retraction ratios observed in
d

406 this study were higher than those previously reported by Phan The, Debeaufort, Voilley
e

407 and Luu (2009) on the films made from agar gum/cassava starch blends (95.90- 95.19%).
pt

408 This difference could be due to the different chemical structure of film-forming agents
409 which affects the organization of polymer chains in the film matrix and also dissimilar
ce

410 drying conditions.

411
412 3.2.3. Moisture content
Ac

413 Owing to its remarkable plasticizing effect, measuring the moisture content of film is
414 important. It also helps to find out how the interactions between hydrocolloids could affect
415 the films affinity to water. The data in Table 4 show that the moisture content of films
416 varied from 12.02 to 16.20%. It was found that the moisture content of GT film was
417 significantly higher (p<0.05) than that of LBG film. In previous studies also similar values
418 of moisture content have been reported for other polysaccharide-based films (Ahmadi,
419 Kalbasi-Ashtari, Oromiehie, Yarmand & Jahandideh, 2012; Khazaei, Esmaiili, Djomeh,

14

Page 14 of 26
420 Ghasemlou & Jouki, 2014; Kurt & Kahyaoglu, 2014; Martins, Cerqueira, Bourbon,
421 Pinheiro, Souza & Vicente, 2012). The higher moisture content of GT film could be due to
422 its different chemical structure. Kurt and Kahyaoglu (2014) also observed that the moisture
423 content of LBG film was significantly lower than that of the films made from guar gum
424 and salep glucomannan. Results also demonstrate that the moisture contents of blend films

t
425 did not depend on the mixing ratio of hydrocolloids. They were all significantly higher

ip
426 than those of LBG film but lower than those of GT film. This means that incorporation of
427 LBG to GT film formulation modified the film structure at all blending ratios in a way that

cr
428 the moisture content decreased. This could be due to the lower moisture content of LBG

us
429 film in comparison with GT film.
430
431
432
433
3.2.4. Moisture absorption an
Measuring the amount of water absorbed by film matrix helps to predict the stability
434 and quality changes during storage of food products under humid conditions (Kurt &
M
435 Kahyaoglu, 2014). The amount of moisture absorbed by polymeric films also affects
436 molecular mobility and thus alters their thermal, mechanical and barrier properties
d

437 (Martins, Cerqueira, Bourbon, Pinheiro, Souza & Vicente, 2012). The experimental data
438 revealed that the moisture absorption of LBG film was significantly higher than GT film at
e

439 RH 98% (Table 4). On the other hand, it was found that the moisture absorption of blend
pt

440 films was independent of GT/LBG mixing ratio, although they showed higher and lower
441 tendency toward moisture absorption than GT and LBG films, respectively. It has been
ce

442 reported that the amount of water absorbed by polysaccharide films directly depends on
443 the number of available sorption sites which are mainly free hydroxyl and carboxyl groups
Ac

444 indicating their hydrophilic character (Kurt & Kahyaoglu, 2014). Accordingly the
445 difference between the moisture absorption of GT, LBG and their blend films can be
446 explained based on their chemical structure, namely the availability of free –OH and –
447 COOH groups and also the organization of polymeric chains in film matrix.
448 Different results have been reported on the effect of intermolecular interactions on
449 blend films moisture absorption. Martins, Cerqueira, Bourbon, Pinheiro, Souza and
450 Vicente (2012) demonstrated that the interactions between LBG and ĸ-carrageenan led to a
451 higher susceptibility of their blend films to water which was attributed to more exposure of
15

Page 15 of 26
452 hydroxyl groups in the blend. In contrast, Wu et al. (2012) noticed no significant
453 difference between water sorption tendency of konjac glucomannan/curdlan blend films
454 and those of their constituents.
455
456 3.2.5. Water vapour permeability (WVP)

t
457 Water vapour permeability is an indicator of how easily moisture passes across a film

ip
458 (Hernandez, 1994). This phenomenon implies solubility and diffusion of water vapour
459 molecules through film matrix. Since one of the most important requirements for edible

cr
460 films is to block the transformation of moisture between food and its surrounding

us
461 atmosphere, their WVP should be as low as possible (Kurt & Kahyaoglu, 2014). Similarly,
462 WVTR is another characteristic which is directly relevant to the hydrophilic nature of a
463 film, i.e. more hydrophilic films will have higher WVTR (Seyedi, Koocheki, Mohebbi &
464
465
Zahedi, 2014).
an
WVP and WVTR of GT, LBG and their blend films are given in Table 4. As the data
show WVP of film samples varied from 0.27 to 0.38 (g.m/m2.h.kPa). WVP and WVTR of
M
466
467 LBG film were found to be significantly lower than those of GT film. For blend films,
468 WVP seemed to have no dependency on mixing ratio of polymers. However, incorporation
d

469 of LBG regardless of its ratio decreased WVP and WVTR of GT film. Poor water vapour
e

470 barrier of films is due to their hydrophilic character which lets water vapour molecules
pt

471 dissolve and pass through the film matrix. Previous studies have also reported similar
472 results on WVP and WVTR of hydrophilic films (Ahmadi, Kalbasi-Ashtari, Oromiehie,
ce

473 Yarmand & Jahandideh, 2012; Jouki, Tabatabaei Yazdi, Mortazavi & Koocheki, 2013;
474 Khazaei, Esmaiili, Djomeh, Ghasemlou & Jouki, 2014; Seyedi, Koocheki, Mohebbi &
475 Zahedi, 2014). The difference between WVP of GT and LBG films could be explained
Ac

476 based on their chemical structure, i.e., type of building blocks and spatial conformation,
477 size and molecular weight which affect final moisture content and mobility of molecules in
478 the film matrix. Kurt and Kahyaoglu (2014) reported that WVP of LBG film was
479 significantly lower than guar gum film and they related it to lower molecular mobility of
480 LBG in comparison with guar gum. Gaudin, Lourdin, Le Botlan, Ilari and Colonna (1999)
481 also related higher WVP of films to their higher moisture content or higher number of
482 hydroxyl groups in the structure of their constituents. Moreover, the integrity of film is

16

Page 16 of 26
483 another important factor that influences WVP as demonstrated by Seyedi, Koocheki,
484 Mohebbi and Zahedi (2014). The findings of this study also showed that higher integrity of
485 LBG film led to more compact structure as shown in the film SEM cross section photos
486 (Fig. 3:bottom row A-E) and consequently lower WVP. In the case of blend films
487 decreasing WVP of GT film as a result of LBG incorporation could be due to the

t
488 interactions occurred between them (p<0.05). Similar observations have also been reported

ip
489 by others. Khoshgozaran-Abras, Azizi, Hamidy and Bagheripoor-Fallah (2012) noticed
490 that WVP of chitosan film decreased when blended with aloe vera gel. They attributed this

cr
491 to a decrease in the availability of total hydrophilic groups in the blend which resulted in

us
492 diminished interactions with water. Martins, Cerqueira, Bourbon, Pinheiro, Souza and
493 Vicente (2012) also found out that WVP of LBG film decreased in the presence of ĸ-
494 carrageenan which was known to be the consequence of intermolecular interactions
495
496
an
between the two polymers which led to more compact film matrix.
M
497 3.2.6. Transparency
498 Transparency is a critical property for edible films which affects their general
499 appearance and determines their applications. The data in Table (4) show that the
d

500 transparency of LBG film was significantly higher than that of GT film while the
e

501 transparency of their blends laid in between. There was, However, no significant
pt

502 difference (p<0.05) between the transparency of the blend films at different gum ratios.
503 These results were in agreement with films visual observations. Previous studies have
ce

504 reported controversial results on the effect of hydrocolloids interactions on the film
505 transparency. Xu, Li, Kennedy, Xie and Huang (2007) found that the transparency of
506 Konjac glucomannan/gelan gum blend film was higher than that of each film individually
Ac

507 and linked it to their intermolecular interactions. In contrast, Martins, Cerqueira, Bourbon,
508 Pinheiro, Souza and Vicente (2012) observed no significant difference between
509 transparencies of films made from various ratios of LBG and ĸ-carrageenan despite the
510 fact that they showed considerable intermolecular interactions.
511 The results of this study suggest that LBG alone can potentially be used for coating
512 surfaces where higher transparency is desirable. However, for some other applications
513 where the product is required to be protected against light and related deteriorative

17

Page 17 of 26
514 reactions, lower transparency would be needed and hence GT/LBG blend could be
515 employed.
516
517 3.2.7. Film microstructure
518 Scanning electron microscopy (SEM) was carried out to study the microstructure and

t
519 surface characteristics of film samples in order to establish a relationship between

ip
520 molecular orientation in the matrix and physicomechanical properties of films. Fig. 3
521 shows SEM micrographs of surface morphology and cross section of GT, LBG and

cr
522 GT/LBG films. As can be seen all films had a partially smooth and homogeneous surface

us
523 without pores and cracks. Comparing the micrographs of individual LBG and GT films it
524 was found that the surface and cross section of the LBG was smoother, compacted and
525 denser whilst the GT showed more open and porous structure. This could be due to the
526
527
an
difference between their chemical structures. In the case of blend films, it was observed
that all films had a partially smooth and homogeneous surface suggesting high miscibility
M
528 and blend homogeneity, although incorporation of LBG to GT films resulted in denser and
529 more compacted structure. These observations again confirm the miscibility of LBG and
530 GT together in their binary solutions and also in film matrix which is in good agreement
d

531 with the results of apparent viscosity and FTIR spectroscopy.

e

532
pt

533
534
ce

535 3.2.8. Mechanical properties

536 Edible films and coatings are often subjected to different external stresses and impacts during
537 food packaging and handling. Therefore, their strength and mechanical properties are of
Ac

538 paramount important practical and technological characteristics compared to others (Li, Peng,
539 Yie & Xie, 2006; Lu, Wang & Xiao, 2008; Xiao, Lu, Gao & Zhang, 2001). In this study
540 mechanical properties were evaluated on the basis of tensile strength (TS) and elongation at
541 break (EB%). TS and EB% are defined as the maximum force and relative increase in sample
542 length at break point, respectively. They are considered to be appropriate measures for film
543 strength and its flexibility assessment (Kurt & Kahyaoglu, 2014). As the data in Table 5 show
544 the EB (%) of LBG film was higher than that of GT film and the EB (%) of the blend films laid

18

Page 18 of 26
545 in between. TS of LBG film was higher than that of GT film and increased with incorporation of
546 LBG in film formulation in a way that TS of the blend films with the GT/LBG ration of 50/50
547 and 25/75 did not differ significantly (P<0.05) with the LBG film. This indicates that
548 incorporation of LBG into GT film led to an increase in intermolecular interactions and thus
549 cohesive strength of films. Phan The, Debeaufort, Voilley and Luu (2009) also reported the same

t
550 effect on cassava starch/agar blend films. It has been demonstrated that the films, either synthetic

ip
551 or natural, with higher TS usually show lower EB(%) due to their structural characteristics
552 (Seyedi, Koocheki, Mohebbi & Zahedi, 2014). This rule, however, was not applicable to

cr
553 GT/LBG blend films which could be the result of different type and intensity of interactions that

us
554 took place between these polysaccharides.
555
556
557
558
4. Conclusions
an
The results of this study provided useful information on the functional properties of GT,
M
559 LBG and their binary solutions as well as their corresponding films. A synergistic effect
560 was observed between these two biopolymers at all mixing ratios that were explained
561 based on their tendency to form intermolecular hydrogen bonds as clearly revealed by
d

562 FTIR spectra. Scanning electron micrographs also confirmed the existence of miscibility
e

563 between the two hydrocolloids by demonstrating homogeneity and smoothness in their
pt

564 surfaces and cross sections. Blending the two polysaccharides together led to a decrease in
565 their surface tension which could enhance their spreadability and coating integrity when
ce

566 applied on food product. Physical observations showed that although the thickness, density
567 and retraction ratio of films was not affected by gum blending ratio, their transparency,
568 water barrier and mechanical properties were improved by incorporating LBG to the film.
Ac

569 These findings are quite promising suggesting that LBG and GT blend have a good
570 potential to be considered as a new source of biodegradable packaging material for food
571 applications.
572
573
574
575 Fig. 1 Changes in the viscosity of GT/LBG binary solution as a function their blending
576 ratio.

19

Page 19 of 26
577 Fig. 2 FTIR spectra of GT/LBG blend films at different ratios (0/100, 25/75, 50/50, 75/25 and
578 100/0)
579 Fig. 3 Scanning electron micrographs (×10000) of surface (top row) and cross sections (bottom
580 row) of GT/LBG blend films at 100/0 (A), 75/25(B), 50/50 (C), 25/75 (D), 0/100 (E) ratios
581
582 Table 1 Combination ratios of GT and LBG in the binary blends for 100 ml of solvent
GT/LBG ratio GT (g) LBG (g)

t
100/0 1.00 0.00

ip
75/25 0.75 0.25
50/50 0.50 0.50
25/75 0.25 0.75

cr
0/100 0.00 1.00
583
584

us
585 Table 2 Surface tension of GT/LBG blend solutions
GT/LBG Surface tension (mN/m)
ratio
100/0 60.47 a ± 0.24
75/25
50/50
an
51.79 b ± 2.18
53.97 b ± 0.28
25/75 54.32 b ± 2.54
59.83 a ± 1.25
M
0/100
a–b
586 Means (n = 2) with different superscripts are significantly different (p < 0.05).
587
588 Table 3 Thickness, density and retraction ratio of GT/LBG blend films.
Density (g/cm3)
d

GT/ LBG ratio Thickness (µm) Retraction ratio (%)

a
100/0 46.98 ± 1.85 a
1.04 ± 0.03 99.15a ±0.00019
e

75/25 45.88a ± 2.31 0.91a ±0.07 99.16a ±0.00052

pt

50/50 47.03a ± 1.16 1.04a ± 0.15 99.20a ±0.00117

ce

25/75 46.20a ± 2.51 0.93a ±0.09 99.16a ±0.00054

0/100 44.50a ± 3.07 1.04a ±0.15 99.19a ±0.00125

Ac

a
589 Means (n = 3) with same superscripts are significantly the same (p < 0.05).
590
591 Table 4 Moisture content, moisture absorption, WVP, WVTR and transparency of GT/LBG
592 blend films
GT/ LBG ratio Moisture Moisture WVP WVTR Transparency
content (%) absorption (%) (g.mm/m2.h.kpa) (g/m2.h)

100/0 16.20 a ± 1.20 43.80 c ± 1.46 0.38 a ± 0.03 25.92 a ± 2.76 76.65 c ± 1.85
75/25 15.52 b ±1.06 74.70 b ± 2.73 0.30 b ± 0.02 20.75 b ± 0.24 81.65 b ± 1.36
50/50 13.07 b ±0.36 76.83 b ± 5.48 0.30 b ± 0.02 21.92 b ± 0.51 80.81 b ± 0.67

20

Page 20 of 26
 25/75 13.17 b ±0.80 76.68 b ± 3.04 0.29 b ± 0.02 20.19 b ± 0.56 81.25 b ± 0.36
0/100 12.02 c ±2.80 95.84 a ± 0.27 0.27 b ± 0.05 19.28 b ± 1.13 84.91 a ± 0.41
a–c
593 Means (n = 2) in the same column with different superscripts are significantly different (p < 0.05).
594
595 Table 5 Mechanical properties of GT/LBG blend films
GT/ LBG ratio TS (MPa) EB (%)

100/0 11.60 c ± 2.41 0.72 c ± 0.11

t
75/25 16.77 b ± 3.47 1.12 b ± 0.27

ip
50/50 20.28 ab ± 2.07 1.10 b ± 0.22
22.82 a ± 1.44 1.01 b ± 0.08

cr
25/75
0/100 24.29 a ± 3.21 1.73 a ± 0.09
a–c
596 Means (n = 3) in the same column with different superscripts are significantly different (p < 0.05).

us
597
598
599
600
601
602
an
603
M
604
605
606
607
d

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770 Highlights
771 1. A new blend film has been made from binary solutions of GT and LBG.
772 2. A distinct synergism between GT and LBG was observed.
773 3. The surface tensions of gum solutions were lowered significantly (p<0.05) after blending
774 together.

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775 4. The transparency, water vapour barrier and mechanical properties of films were improved by

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776 incorporating LBG in blend.
777 5. GT-LBG blend film has the potential to be used as a new packaging material.

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