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Food Hydrocolloids
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Article history:
Received 21 December 2013
Accepted 30 May 2014
Available online 14 June 2014
The present work dealt with investigating physicochemical, barrier, mechanical and surface properties of
sage seed gum (SSG) edible lms as a function of plasticiser type (glycerol and sorbitol) and concentration (20, 40, 60, 80 & 100, w/w%). Based on the results, it was revealed that glycerol and sorbitol
effectively plasticise the lms of SSG while glycerol efciency was higher than sorbitol. Although the
lms plasticised by glycerol were of high moisture content (27e49%), moisture uptake (110e140%) and
solubility in water (~80%), but they exhibited low permeability to water vapour, acceptable mechanical
properties, surface hydrophilicity, and transparency. In contrast, the lms plasticised by different concentrations of sorbitol exhibited a low moisture content (~14%), water vapour permeability (lower than
4 1011 g/m.s.Pa), and moisture uptake (below 90%) with high surface hydrophobicity but less desirable
mechanical properties. The probable mechanisms of plasticising are discussed in details regarding the
observed characteristics of SSG edible lms. Concluding, the lms of SSG in present work showed a
substantial potential to be incorporated in food packaging applications.
2014 Elsevier Ltd. All rights reserved.
Keywords:
Edible lm
Glycerol
Mechanical properties
Permeability
Sage seed gum
Sorbitol
1. Introduction
Nowadays, due to the non-degradability of synthetic packaging
materials, there have been increasing research interests toward
natural resources to produce biodegradable edible lms. These
studies mainly focused on developing edible lms and improving
their characteristics to exert the main desired features of conventional synthetic materials, such as high mechanical strength, softness, lightness, transparency, water resistance, and so on.
The major potential alternatives to plastics, which have been
studied extensively, are biopolymers including polysaccharides,
proteins, and lipids. Based on the diversity, availability, and unique
characteristics, most effort has been put on studying the lm
forming and characterisation of edible lms from hydrocolloids of
different sources with diverse chemical structures, e.g. keran,
Opuntia nopal mucilage, psyllium mucilage, starches of different
sources, gellan, cress seed gum, guar, locust bean gum (LBG),
hydroxypropyl methylcellulose (HPMC), alginate, chitosan, agar,
and gelatin (Ahmadi, Kalbasi-Ashtari, Oromiehie, Yarmand, &
Jahandideh, 2012; Bergo et al., 2008; Dias, Muller, Larotonda, &
291
Moisture uptake%
m2 m1
m1
100
(1)
292
S%
m1 1 u m3
m1 1 u
(2)
WVP g Pa1 s1 m1
WVTR
SR1 R2 $d
(3)
gL 1 cos q 2
q
q
D
P P
gD
L gS 2 gL gS
(4)
293
Table 1
The dependence of density, colour parameters, and water vapour permeability (WVP) of SSG lms to plasticisers.
Plasticiser (%)
Density (g/cm3)
L*
Glycerol
40
60
80
100
Sorbitol
40
60
80
100
Colour parameters
a*
b*
1.40
1.39
1.35
1.32
0.06
0.04
0.03
0.05
73.09
74.04
75.57
75.22
1.45
0.84
2.23
1.18
0.00
0.02
0.03
0.02
0.01
0.02
0.00
0.01
1.38
1.28
1.17
1.40
0.05
0.78
0.48
0.67
4.23
4.80
5.44
5.71
0.57a
0.32a
0.25a
1.00a
1.41
1.38
1.35
1.27
0.11
0.01
0.04
0.05
73.23
73.95
74.08
73.79
2.37
1.72
1.08
0.93
0.05
0.07
0.05
0.05
0.02
0.02
0.00
0.01
1.36
1.48
1.58
1.39
0.22
0.60
0.01
0.68
2.98
3.68
3.73
4.09
0.08b
0.17ab
0.16ab
0.77a
294
Fig. 2. The dependence of moisture uptake and solubility in water (Sw) of SSG lms as
a function of plasticiser concentration (error bars represent standard deviation and
different letters on error bars indicate the statistical signicance).
the assumption that the more expanded the polymer network inside lms by restructuring the interactions to a disordered state,
the higher the opportunity to bind water, observed as a signicant
rise in moisture uptake.
3.5. Solubility in water
Generally, it is believed that Sw increases by adding and raising
concentration of plasticiser in lm matrix due to the hydrophilic
nature of both the base material and polyol plasticisers used in
edible hydrocolloid lms (Ahmadi et al., 2012; Ghasemlou,
Khodaiyan, & Oromiehie, 2011; Jouki et al., 2013; Laohakunjit &
Noomhorm, 2004; Piermaria et al., 2009; da Silva et al., 2009).
The Sw of SSG lms almost remained constant (~82%) by
increasing proportion of glycerol in lm formulation and it was
barely affected (p > 0.05). Although scant variations in Sw observed
for sorbitol plasticised samples (65e84%), but still the inuence of
sorbitol concentration was insignicant (Fig. 2). Both samples, i.e.
glycerol and sorbitol plasticised, can be considered as highly
soluble.
The values of Sw determined for SSG lms are close to solubility
of cassava starch lms (Phan et al., 2005), but higher than the Sw of
lms from psyllium gum (Ahmadi et al., 2012), keran (Ghasemlou,
Khodaiyan, & Oromiehie, 2011), cress seed gum (Jouki et al., 2013),
rice starch (Laohakunjit & Noomhorm, 2004), and agar, normal and
waxy rice starch (Phan et al., 2005).
The higher afnity of SSG lms in relation to the presence of
plasticisers could be probably attributed to the hygroscopic nature
of plasticisers along with the weakened swollen structure of the
lm network induced by structure disordering inuence of plasticiser which resulted in less stability in aqueous medium.
3.6. Colour
The results of SSG lm colour parameters are tabulated in
Table 1. The high lightness, L*, values observed in presence of both
glycerol and sorbitol at all investigated concentrations indicates the
high transparency of samples, which is a desirable characteristic in
edible lm packaging and coatings. The L* of SSG lms was
observed to be independent of plasticiser concentration (p > 0.05).
This is consistent with the results of Thakhiew et al. (2010) and
Seyedi et al. (2014), although it is generally believed that plasticisers increase the L* value of hydrocolloid lms (Ahmadi et al.,
normal and waxy rice starch (Phan et al., 2005), gelatin (Rivero
et al., 2010), LPSG (Seyedi et al., 2014) and arabinoxylan (Zhang &
Whistler, 2004); while higher than LDPE (Phan et al., 2005) and
gellan (Yang & Paulson, 2000) lms. This clearly indicates that SSG
lms are good barriers against water vapour.
3.8. Contact angle and surface free energy
The surface properties of SSG lms was characterised through
contact angle measurements against three types of liquids, i.e.
water, ethylene glycol (EG), and glycerol. The results of contact
angle measurements for lm samples plasticised by different concentrations of glycerol and sorbitol are presented in Table 2. It can
be seen that the water contact angle increases from 32 to 56 and
42 to 103 in glycerol and sorbitol plasticised lms, respectively. It
could be inferred that although the surface hydrophobicity of
glycerol plasticised samples increase by elevating plasticiser concentration, still it has a hydrophilic surface which could be wetted
by water. In contrast, the lms plasticised by sorbitol showed an
abrupt increase in hydrophobicity in which the samples containing
80% w/w or more are completely hydrophobic indicated by contact
angles greater than 90 . Contrary to the results of the present work,
it has been reported that water contact angle of hydrocolloid lms
decreases by plasticisers (Ahmadi et al., 2012; Ghasemlou,
Khodaiyan, Oromiehie, et al., 2011; Jouki et al., 2013; Seyedi et al.,
2014; Suyatma, Tighzert, & Copinet, 2005). The contact angle of
SSG lms plasticised by glycerol are lower than the lms prepared
by psyllium gum (Ahmadi et al., 2012), keran (Ghasemlou,
Khodaiyan, Oromiehie, et al., 2011), cress seed gum (Jouki et al.,
2013) and LPSG (Seyedi et al., 2014).
In order to further characterise the surface properties of SSG
lms, estimation of critical surface energy, the maximum surface
tension a liquid may have to ensure complete wetting of a given
material, and polar and dispersive energy components of lm
surface were performed. The lower the critical surface energy (gC),
the lower the ability of surface to be wetted by most liquids, i.e. the
lower hydrophilicity. As shown in Table 2, gC was diminished in
case of both glycerol and sorbitol plasticised samples by an increase
in concentration, indicating an increase in surface hydrophobicity.
It is also conrmed by the values of surface free energy (gS), in
which its decreasing trend indicate the more hydrophobic surface
exhibited by SSG lms in relation to a rise in the proportion of
plasticisers. By increasing the concentration of plasticisers, the
polar contribution to surface energy (gPS ) of SSG lms declined
while at the same time, the dispersive contribution (gD
S ) increased.
At all concentrations investigated, the surface hydrophobicity was
295
Table 2
Surface properties of SSG edible lms as affected by different proportions of glycerol
and sorbitol.
Plasticiser (%)
Glycerol
40
60
80
100
Sorbitol
40
60
80
100
Contact angle ( )
gC
gS
gPS
gD
S
32.26
36.91
42.34
55.98
9.18b
6.80b
5.16b
15.18a
39.86
37.67
37.91
30.74
15.07
14.68
14.17
12.64
10.39
9.67
8.81
6.95
4.68
5.01
5.36
5.68
41.56
72.26
90.96
103.10
5.14c
27.40b
30.55ab
15.86a
32.33
24.67
23.32
22.36
14.30
10.50
7.76
7.03
9.50
4.82
1.49
0.53
4.80
5.68
6.27
6.50
Different letters in the same column indicate signicant differences (p < 0.05).
Abbreviations: gC critical surface tension, gS overall surface free energy, and
superscripts P and D denote polar and dispersive components, respectively.
Fig. 3. Tensile strength (TS) and percentage elongation (E) of SSG lms with different
concentrations of glycerol and sorbitol; standard deviations are indicated by error bars,
different letters on error bars represent statistical signicances.
296
Table 3
Thermal properties of SSG lms without plasticiser (control) and containing 100%
(w/w) plasticisers based on DSC and TGA characterisations.
Control
T1*
T2
T3
T4
DSC
TGA
DSC
TGA
DSC
TGA
DSC
TGA
59.70
262.86
277.68
426.51
e
e
e
e
Glycerol
2.13
3.22
0.94
5.92
52.24
53.53
179.10
178.96
286.43
280.41
340.82
454.24
Sorbitol
0.01
3.46
7.13
3.14
2.18
2.72
2.58
1.63
47.19
76.86
245.31
261.68
e
440.99
e
e
1.78
2.74
7.05
2.68
8.38
curve, with an initial small peak with Td of 53.5 C revealing the free
water loss; followed by a major peak at 179.0 C most likely associated with the loss of glycerol compounds and chemisorbed
structurally bound water (Cerqueira et al., 2012; Martins et al.,
2012; Mu et al., 2012); ending with two peaks at 280.4 and
454.2 C related to SSG macromolecular chain scission. Similarly,
there was a slight weight loss in sorbitol plasticised SSG lm
starting from 76.9 C followed by two peaks with Td of 261.7 and
441.0 C with about 70% decomposition.
By considering the Td values of SSG lms with and without
plasticiser, it could be concluded that the presence of plasticiser
shifted the degradation temperatures more or less toward higher
values, showing an increase in heat stability which is consistent
with the results reported by Cerqueira et al. (2012) and Mu et al.
(2012).
4. Conclusions
The inuence of incorporating different concentrations of glycerol and sorbitol as plasticiser in formulation of edible lms fabricated from SSG was investigated through physicochemical,
mechanical, barrier, and surface properties. Based on the visual and
preliminary characterisations, it was observed that PEG is not an
appropriate plasticiser for SSG lms, therefore, its application could
not be recommended. The results indicated that glycerol has a great
efciency in plasticising SSG lms in terms of increased thickness,
moisture content, moisture uptake, and percentage of elongation
with declining the tensile strength and surface hydrophilicity.
Surprisingly, the values of WVP were low enough to be regarded as
less permeable in comparison with other hydrocolloid lms. In
addition, acceptable mechanical properties and high heat stability
were achieved by the lms plasticised by glycerol. In sorbitol
plasticised lms, it was observed that raising the concentration
leads to highly soluble low moisture content lms with low afnity
to uptake moisture and high surface hydrophobicity. The mechanical characteristics of lms containing sorbitol were not
notable. Based on the characterised properties of lms it was
revealed that glycerol has a greater plasticisation efciency
compared with sorbitol, although the lms containing sorbitol are
still of reasonable and acceptable characteristics. Overall, the results of the present study indicated that SSG could be regarded as
an appropriate source of edible lms for common food applications.
It should be noted that the results of ongoing study which deals
with the incorporation of different fatty acids in SSG edible lms
will be presented in forthcoming paper.
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