| |

Received: 7 February 2018    Revised: 28 May 2018    Accepted: 30 May 2018

DOI: 10.1111/jfpp.13715

ORIGINAL ARTICLE

The physicochemical and structural properties of psyllium

gum/modified starch composite edible film

Fatemeh Askari1 | Ehsan Sadeghi1  | Reza Mohammadi1 | Milad Rouhi1 | Masoumeh

Taghizadeh1 | Mohammad Hosein Shirgardoun2 | Mohaddeseh Kariminejad1

1
Research Center for Environmental
Determinants of Health
(RCEDH), Kermanshah University of Medical
Sciences, Kermanshah, Iran
2
School of Agriculture and natural
resource, Islamic Azad University, Yazd, Iran
Correspondence
Ehsan Sadeghi, Research Center for
Environmental Determinants of Health
(RCEDH), Kermanshah University of
Medical Sciences, P.O. Box: 6719851351,
Kermanshah, Iran.
Email: e.sadeghi@kums.ac.ir
Funding information
Kermanshah University of Medical Sciences
Abstract
The current study investigated the physicochemical and structural properties of dif‐
ferent ratios of psyllium gum (PG) and modified starch (MS) (100:0, 50:50, 75:25,
0:100) composite films. The results indicated that the moisture content, water solu‐
bility, water vapor permeability (WVP), and tensile strength (TS) of films decreased
with increasing proportions of PG. However, the films’ elongation at break (EB) in‐
creased with gum content >50%. Cross‐sectional scanning electron microscopy
(SEM) of composite films showed homogeneity, integrity, and a smooth structure.
The results of differential scanning calorimetry (DSC) indicated a reduction of ther‐
mal stability with increasing proportions of PG. The films’ Fourier transform infrared
spectroscopy (FTIR) spectra indicated miscibility and good interactions between MS
and PG. These findings were in agreement with the results of physicochemical, me‐
chanical, morphological, and thermal analyses. The PG/MS composite films with im‐
proved properties have potential for use in food packaging.
Practical applications
The film forming is a technique that polymer(s) combine with together and may be
created cross‐linked between them. The combination of polymers for film forming
was used for reinforcement and stability the films networks. In this study, the com‐
posite edible films of psyllium gum/modified starch made and the physicochemical,
mechanical, and structural properties of films was measured.

1 |  I NTRO D U C TI O N
Increased consumer demand for fresh and high‐quality foods has
increased the need for packaging that can more effectively pro‐
tect food and extend its shelf life (Lago‐Vanzela, Do Nascimento,
Fontes, Mauro, & Kimura, 2013; Parra, Tadini, Ponce, & Lugão,
2004). Because of edible films made from biopolymers offer advan‐
tages such as renewability, low‐cost, accessibility, and the mainte‐
nance of food quality, they can replace packaging produced from
petroleum‐based plastics (Ahmadi, Kalbasi‐Ashtari, Oromiehie,
Yarmand, & Jahandideh, 2012; Rao, Warrier, Gaikwad, & Shevate,
2016; Thakur & Thakur, 2014). The main ingredients of biopolymer‐
based edible films and coatings are proteins, polysaccharide, and
lipids, which can be used alone or combined (Gennadios, 2002; Jung,
2006; Lago‐Vanzela et al., 2013; Ustunol, 2009). Commonly, films
based on single biopolymers have poor mechanical properties and
are sensitive to environmental conditions. Blending biopolymers in
the manufacture of films could be an effective method to overcome
these disadvantages.
In recent years, many studies have investigated films based on
natural biopolymers such as gums. Psyllium seed (Plantago ovate
Forsk) is an annual plant grown in many moderate climate areas of the
world, particularly India and Iran (Ahmadi et al., 2012), and is consid‐
ered a source of natural biopolymers. The main functional properties
of psyllium are derived from the polysaccharides in its husk: 74.65%
xylose, 22.6% arabinose and some other sugars (Rao et al., 2016).

J Food Process Preserv. 2018;42:e13715. wileyonlinelibrary.com/journal/jfpp © 2018 Wiley Periodicals, Inc.  |  1 of 9
https://doi.org/10.1111/jfpp.13715
 |
2 of 9       ASKARI et al.
Psyllium husk has many benefits in medicine (for example, it is used
to treat constipation, colon cancer, diarrhea, high cholesterol, and
diabetes), pharmaceutics (such as serving as a carrier and bioactive
polysaccharide), and food manufacture (such as serving as a thick‐
ener, stabilizer, and gel‐forming ingredient) (Ahmadi et al., 2012; Rao
et al., 2016; Thakur & Thakur, 2014). It can also be used as a hydro‐
gel in food manufacture due to its high water‐binding capacity and
intense viscosity. Ahmadi et al. have studied the characteristics of
psyllium gum film and shown that these films have poor mechanical
properties (Rao et al., 2016). However, psyllium gum could be com‐
bined with another biopolymer such as modified starch to improve
the properties of its film.
Starch is a polymer widely used in the food industry, especially in
the production of edible film and coatings because of the variety of its
sources and amenability to physical or chemical modification, low cost,
and biodegradability (López, García, & Zaritzky, 2008). Starch can be
obtained from wheat, rice, corn, cassava, and potato (López et al., 2008).
The methods of modification of starch include of chemical (cross‐link‐
ing, acetylation, phosphorylation), enzymatic, physical (pregelatiniza‐
tion), and combined modification (López et al., 2008). Starch films have
a poor mechanical properties and high sensitivity to moisture, so that to
improve the properties of film it could combine with another polymers
such as chitosan, gelatin, or gums (Santacruz, Rivadeneira, & Castro,
2015; Woggum, Sirivongpaisal, & Wittaya, 2014). Also, modified starch
has higher water solubility than neat starch, which enhances its compat‐
ibility with water soluble polysaccharides. So that, modified starch has a
good potential for film and coating formation.
Psyllium gum has a good potential for use in food packaging, but
has a poor mechanical properties. Blending of psyllium gum with
modified starch can reinforce the properties of its films. The goal
of this research was to investigate the physicochemical, structural,
mechanical, and thermal properties of psyllium gum films. Also, it
were analyzed the effect of modified starch concentration on the
properties of psyllium gum films.
2 |  M ATE R I A L S A N D M E TH O DS
2.1 | Materials
Psyllium seed was purchased from a local market (Kermanshah, Iran).
Modified starch (wheat acylation starch, degree of acylation = 20%–
25%), and ethanol (96%) were obtained from Pouya Kabak (Tehran,
Iran) and Razi Corporation (Tehran, Iran), respectively. Glycerol, so‐
dium chloride, saturated magnesium nitrate, and calcium chloride
were obtained from Merck Chemicals Co. (Darmstadt, Germany).
2.2 | Methods
2.2.1 | Extraction of polysaccharide
Psyllium gum (PG) was extracted and purified according to the
procedure of Ahmadi et al. (Ahmadi et al., 2012). First, about
10 g of psyllium seeds were cleaned to eliminate foreign parti‐
cles, then washed with 30 g of ethanol (96% w/v) three times
to remove all foreign particles such as dust and chaff. Next, the
seeds were placed in an oven (Heraew W.C. Heraeus Hanau,
Germany) 45 ± 2°C for 2 hr to remove the ethanol. To extract the
PG, 500‐ml distilled water was added to the seeds (70°C) and
stirred continuously with an electronic stirrer (RW 20 DZM‐ IKA
WERK, Germany) at 70 ± 5°C for 1 hr and 300 rpm. The seeds
were separated by filter (mesh 18). The polysaccharide fraction
precipitated with addition ethanol and then dried at 45 ± 2°C in
an oven. The gum was sieved and stored at room temperature
25 ± 3°C and 50% RH.
2.2.2 | Preparation of solutions
To produce the film, PG (1.5% w/v) was dissolved in distilled water
for 30 min and allowed to hydrate for 24 hr at 45°C. Modified
starch (MS) solution (3% W/V) was produced using the same
procedure (dissolved in distilled water and hydration for 24 hr at
45°C). The PG and MS solutions were mixed in different ratios
(100:0, 50:50, 75:25, and 0:100), blended, and stirred at 300 rpm
and 50°C for 15 min. Thereafter, 50 ml of each PG/MS solution
was spread on 15‐cm‐diameter petri dishes. The films were dried
in an air convection oven, and the films were peeled off and placed
in a desiccator containing saturated magnesium nitrate (25 ± 3°C
& 53% RH) for 72 hr before analysis. All tests were conducted in
triplicate.
2.2.3 | Thickness of films
The films’ thickness was measured with a digital micrometer
(Mitutoyo, Japan) to the nearest 0.001 mm. Measurements were
done at six random points on each film, and the six measurements
were used to calculate an average value.
2.2.4 | Moisture content
The film samples (2 × 2 cm2) were dried at 105 ± 1°C in a laboratory
oven until they reached constant weight. Moisture content (MC) was
determined using Equation (1):
m1 − m2
MC =
m1
× 100 (1)
where m1 and m2 are the initial and the dried sample weight, respec‐
tively. Three replicates were analyzed per film formulation.
2.2.5 | Water solubility
Water solubility (WS) is defined as the percentage of dried matter
that is soluble in water. Samples were placed in 50‐ml distilled water
(25 ± 3°C, 2 hr) under constant stirring (30 rpm) using a magnetic stirrer
(RW 20 DZM‐IKA WERK, Germany). The resulting solution was filtered
ASKARI et al.
using Whatman paper and then dried in an oven (105°C for 1 h) until
reaching to constant weight. WS was determined using Equation (2).
w1 − w2
WS = × 100
w1
where w1 and w2 are the weight of samples before and after soaking
in distilled water, respectively.
2.2.6 | Water vapor permeability
Water vapor permeability (WVP) measures film resistance to water
vapor. WVP was measured using ASTM E96‐00 Method (ASTM
E96‐00 Method (2000)). Film without flaws was fixed on a cell (ex‐
posed area = 23.7462 cm2) containing CaCl2 as a desiccant. The cell
was placed in a desiccator containing saturated NaCl solution (75%
RH). The weight of the cell measured to the nearest 0.0001 g every
24 hr for 5 days, and changes in weight were plotted as a function
of time; the slope of this plot was the water vapor transmission rate
(WVTR). These values were calculated using Equations (3) and (4):
WVTR =
Δm
A×t
WVTR × x
WVP =
ΔP
where ∆m is the change in weight over time (t), A is the surface area
of the exposed film, x is film thickness, and ∆P is difference in partial
pressure.
2.2.7 | Mechanical properties
The samples (1 × 10 cm) such as were preconditioned at room tem‐
perature (25 ± 3°C) and 55% ± 3% RH in a desiccator for 72 hr.
Tensile strength (TS) and elongation at break (EB) of films were meas‐
ured using a texture analyzer (Testometric M350‐10CT, England) ac‐
cording to ASTM 882‐02 Standard Method (ASTM 882-02 Standard
Method (2002)). The samples were fixed in the grips of the device
with a gap of 50 mm. The change of length and force were recorded
during tension of the specimens at 50 mm/min up to the break. TS
and EB were calculated using the following equations:
F the thickest of films was neat MS film (about 130 µm). The heat‐
TS =
x×w
Δl
EB = × 100
li
where F is maximum force, w is film width, x is film thickness, ∆l is
the change of film length, and li is initial film length. Three repetitions
were carried out for each film sample.
2.2.8 | Microstructure of films
Microstructural analysis of films was carried out using scan‐
ning electron microscopy (SEM; EM3200, KXKY, China). Samples
were immersed in liquid nitrogen and then dried in a vacuum and
|
      3 of 9
immediately fractioned. Finally, the films were fixed on aluminum
stubs and coated with gold. The samples were examined at an ac‐
celerating voltage of 25.0 kV. The cross section of the samples was
(2) observed at magnification 1,000×.
2.2.9 | FTIR
Analysis of the films’ structure was carried out using Fourier
Transform Infrared Spectroscopy (FTIR). The FTIR spectrum was
recorded in attenuated total reflectance (ATR) mode using a FTIR
spectrometer (Shimadzu Irprestige‐21, Japan). The range of absorb‐
ance was from 700 to 4,000 cm−1 with 16 scans and resolution of
4 cm−1.
2.2.10 | Thermal properties of films
A differential scanning calorimeter (DSC; Model‐1, Mettler Toledo,
Switzerland) was used to characterize the thermal properties of the
film samples. Samples were conditioned at 54% RH and 25°C, previ‐
ously. About 10 mg of film was cut into small pieces and placed in the
(3)
sample pan of the DSC. An empty aluminum pan was used as a refer‐
ence. The range of heating was −20°C to 150°C at rate of 10°C/min.
(4)
2.2.11 | Statistical analysis
SPSS software (Version 23.0, SPSS Inc., Chicago, USA) was used to
analyze the data. All the experiments were conducted in triplicate.
Data were initially evaluated by analysis of variance (ANOVA), and
then a Duncan’s multiple range test was employed to detect signifi‐
cant (p < 0.05) differences.
3 | R E S U LT S A N D D I S CU S S I O N
3.1 | Thickness and moisture content
Thickness is an effective parameter on permeability and mechani‐
cal properties. Table 1 shows the thickness of films. The neat PG
film was the thinnest films with thickness about 80 µm, while
(5)
ing leads to gelatinization of starch and swelling of granules and
therefore increasing film thickness (Wang, Wang, Xiao, Liu, et al.,
(6)
2017). As can be seen, the thickness of samples was decreased
with reduction of starch concentration. The different ratios of MS/
PG film had a significant difference (p < 0.05). Reduction in thick‐
ness of films with different concentration of PG can be caused by
less dry matter in these films. The thickness of these films were
significantly higher than cress seed gum, quince seed mucilage, le‐
pidium perfoliatum seed gum, and basil seed gum (Farhan & Hani,
2017; Jouki, Khazaei, Khazaei, Ghasemlou, & HadiNezhad, 2013;
Jouki, Yazdi, Yazdi, Mortazavi, & Koocheki, 2013; Khazaei, Esmaiili,
Djomeh, Ghasemlou, & Jouki, 2014; Seyedi, Koocheki, Mohebbi,
& Zahedi, 2014; Sukhija, Singh, & Riar, 2016). It may be duo the
 |
4 of 9       ASKARI et al.
TA B L E 1   Moisture content, water solubility, water vapor permeability, tensile strength, and elongation at break of PG/MS composite
films
Moisture
PG/MS ratios Thickness (mm) content (%)
100:0 0.080 ± 0.03d 4.54 ± 0.16d
c c
25:75 0.090 ± 0.03 7.06 ± 0.15
50:50 0.110 ± 0.02b 10.87 ± 0.18b
a a
0:100 0.130 ± 0.01 12.58 ± 0.19
Note. Means within each column with same letters are not significantly different (p < 0.05). Data are mean ± SD.
differences of polysaccharide source, the type of extraction, and
the structure of polysaccharide.
Table 1 shows the moisture values of treatments. The mois‐
ture content of samples ranged from 4.54% to 12.58%. The
lowest moisture content was observed in the neat PG film, prob‐
ably because of the lower dry matter content (1.5%). The MC of
films increased significantly (p < 0.05) with increasing moisture
content. Formation of cross‐linkages between polymer chains
results in a reduction of accessibility to hydroxyl groups and hy‐
drogen bonds between polymers and water molecules (Kanmani
& Lim, 2013; Martins et al., 2012). However, modified starch
can create hydrogen bonds with water and swell the granules
(12.58%). This finding was contrast with Kanmani and Lim found
that the moisture content of films decreased with the addition
of starch to pullulan, due to pullulan’s greater hydrophilicity
(Kanmani & Lim, 2013). Also, Marvdashti et al, expressed the
moisture content of Alyssum homolocarpum seed gum/polyvinyl
alcohol composite film enhanced with increasing of PVA ratio
from 23.17% to 54.07% duo to many hydroxyl groups of PVA
which it can give higher hydrophilicity to the film (Marvdashti,
Koocheki, & Yavarmanesh, 2017). Generally, The structure and
functional groups of polysaccharide resulted to increase the
moisture content of Alyssum homolocarpum seed gum/polyvinyl
alcohol composite film (Marvdashti et al., 2017), psyllium gum
(Ahmadi et al., 2012), whey protein concentrate/psyllium husk/
lotus starch (Sukhija et al., 2016), basil seed gum (Khazaei et al.,
2014), and cress seed gum (Jouki, Khazaei, et al., 2013) from the
samples of this research.
3.2 | Water solubility
Water solubility is an important factor in food packaging. Higher
water solubility indicates the higher biodegradability and lower
resistance to water (Marvdashti et al., 2017; Sukhija et al.,
2016). The water solubility of the films in this study is shown in
Table 1. The lowest solubility in water was observed in neat PG
films (41.63%). The neat MS films showed the highest solubil‐
ity in water (95.04%), probably because of interactions between
water molecules and the functional groups of the modified starch.
However, the solubility of films were higher than that found for
waxy/native corn starch (31%), waxy/phosphate corn starch (32%;
WVP (×10 −10 g m−1 s−1
Solubility (%) Pa −1) TS (MPa) EB (%)
41.63 ± 0.22d 1.45 ± 0.38b 20.83 ± 0.33c 59.06 ± 0.35d
c b b
69.76 ± 0.23 1.15 ± 0.36 40.37 ± 0.26 18.21 ± 0.42c
84.06 ± 0.27b 1.56 ± 0.36b 40.69 ± 0.28b 6.08 ± 0.27b
a a a
95.04 ± 0.25 2.18 ± 0.46 42.53 ± 0.28 12.79 ± 0.27a
Gutiérrez, Morales, Tapia, Morales, Tapia, Pérez, & Famá, 2015),
thermoplastic native cush‐cush yam starch (32%) and native cas‐
sava starch (24%; Gutiérrez, Morales, Pérez, Morales, Pérez,
Tapia, & Famá, 2015). It is duo to the type of starch source and the
method of modification that can change the functional proper‐
ties. PG/MS blend films (75:25 and 50:50) showed higher solubil‐
ity than neat PG film. This may be due to the reaction of MS with
PG and reduction in the compact structure of PG polymer chains
(Figure 1), with more spaces in the polymer matrix leading to pen‐
etration of more water molecules (Wang, Wang, Ye, Liu, Xiao, et
al., 2017). In contrast to these findings, Wang et al. reported a
decrease in water solubility with the addition of starch to colla‐
gen or gelatin films because of cross‐linkages between starch and
collagen or gelatin molecules, which reinforced the film structure
(Wang, Wang, Xiao, Liu, et al., 2017; Wang, Wang, Ye, Liu, Xiao, et
al., 2017). Also, Basiak et al. showed that wheat starch films had
the lowest water solubility and increased with increasing the ratio
of whey protein isolate (Basiak, Galus, & Lenart, 2015). The water
solubility of these were less than the films of psyllium seed gum
(50.71%; Ahmadi et al., 2012), chia seed mucilage (52.74%; Dick
et al., 2015), Sega seed gum (82%; Razavi, Amini, & Zahedi, 2015),
quince seed mucilage (45.45%; Jouki, Yazdi, et al., 2013), and basil
seed gum (49.65%; Khazaei et al., 2014).
3.3 | Water vapor permeability (WVP)
The most important role of edible films in food packaging is to pre‐
vent or reduce moisture loss (Krochta, Baldwin, & Nisperos‐Carriedo,
1994). Water vapor permeability is influenced by different factors
such as the nature and extraction method of the biopolymers, film
thickness, moisture level, the ratio of the hydrophilic to hydropho‐
bic portions, and the reaction between the functional groups of
polymers (Garavand, Rouhi, Razavi, Cacciotti, & Mohammadi, 2017;
Krochta et al., 1994; Mohammadi et al., 2018). The films’ WVP is
shown in Table 1. The WVP of the films examined in this study was
higher than that found for rice starch/ι‐carrageenan (Thakur et al.,
2016), probiotic‐residing pullulan/starch (Kanmani & Lim, 2013),
lotus starch/whey protein concentrate/psyllium husk (Sukhija et al.,
2016), corn starch/chitosan (Garcia, Pinotti, & Zaritzky, 2006), and
modified starch/carboxy methyl cellulose (Ghanbarzadeh, Almasi,
& Entezami, 2010). The neat MS film had the highest WVP value
ASKARI et al.
F I G U R E 1   The main possible interactions between psyllium gum (PG) and modified starch (MS) in PG/MS edible films
(2.18 × 10 ‐10 g m−1 s−1 Pa−1). This could be due to the hydrophilic na‐
ture of modified starch molecules, which absorb water molecules
from their surroundings. Seyedi et al. reported that the higher mois‐
ture content of lepidium perfoliatum seed gum films resulted higher
values for WVP (Seyedi et al., 2014). The WVP of PG/MS blend films
(50:50 and 75:25) was significantly (p < 0.05) lower than the neat
MS films and 75:25 PG/MS ratio had the lowest WVP (1.15 × 10 ‐10
g m−1 s−1 Pa−1). This may be due to interactions between the two bi‐
opolymers leading to fewer free spaces in the film matrix (Dick et
al., 2015). Also, psyllium hydrocolloid has a branched and compact
structure that prevents the permeability and transition of water
molecules (Yu, Perret, Parker, & Allen, 2003). However, the neat PG
films and composite films indicated insignificant (p > 0.05) changes
in WVP value. This study was contrast with Basiak et al, which found
the WVP of wheat starch increased with increasing the ratio of whey
protein isolate to these films (Basiak et al., 2015). Galus et al, ex‐
pressed the WVP of oxidized potato starch/soy protein isolate based
edible films was enhanced with increasing of the ratio of oxidized
potato starch from 0% to 20% (Galus, Lenart, Voilley, & Debeaufort,
2013). The WVP of these films was lower than of oxidized potato
starch/soy protein isolate (Galus et al., 2013), sega seed gum (Razavi
et al., 2015), and basil seed gum (Khazaei et al., 2014) and closed
to chia seed mucilage (Dick et al., 2015), psyllium gum (Ahmadi et
al., 2012), cress seed gum (Jouki, Khazaei, et al., 2013), and whey
protein concentrate/psyllium husk/lotus rhizome starch (Sukhija et
al., 2016).
3.4 | Mechanical properties
The mechanical properties of films, including tensile strength (TS)
and elongation at break (EB), are shown in Table 1. Tensile strength
shows the mechanical resistance of films to stretching and elonga‐
tion at break shows the flexibility of films before breaking (Qiu,
Hu, & Peng, 2013; Thakur et al., 2016). As shown in Table 1, neat
|
      5 of 9
PG films had the lowest (20.83 MPa) TS. Tensile strength signifi‐
cantly increased (by about twice) when the MS ratio was increased
to 25%, as the PG molecules could create cross‐linkages with MS
functional groups in the blended films. However, an increase in the
proportion of MS from 25% to 50% showed insignificant (p > 0.05)
changes in the films’ TS. The highest tensile strength (42.53 MPa)
was observed in neat MS films, which may be due to the ordered
and crystalline structure of modified starch. Vu and Lumdubwong
found that the TS and crystallinity of films increased with increased
amylose content in the starch used in the films (Vu & Lumdubwong,
2016). The TS of psyllium gum/modified starch composite edible
films was higher than Chaing rice starch (Woggum et al., 2014),
whey protein (Ramos et al., 2013), pea starch/peanut protein iso‐
late (Sun, Sun, & Xiong, 2013), potato starch (da Rosa Zavareze
et al., 2012), whey protein isolate‫‏‬/gelatin/sodium alginate (Wang,
Auty, & Kerry, 2010), and whey protein concentrate/psyllium husk/
lotus rhizome starch (Sukhija et al., 2016).
The highest EB (59.06%) was observed in neat PG films (Table 1).
The amorphous structure of PG films increases their extensibility.
Increases in MS concentration led to decreases in the films’ EB. These
results were in agreement with those of Thakur et al., who reported
a decrease in the EB of rice starch films with decreasing the ɩ‐carra‐
geenan concentration (Thakur et al., 2016). According to Table 1, neat
MS film showed the lowest EB (6.08%). Ahmadi et al, demonstrated
the TS of psyllium gum films diminished and EB of them rose up with
increasing of glycerol ratio (Ahmadi et al., 2012). Also, Seyedi et al,
have mentioned that the resistance reduced and extensibility of films
augmented with the glycerol ratio (Seyedi et al., 2014).
3.5 | Microstructure of films
The study of films’ microstructure shows their homogeneity and mi‐
croscopic structure. The SEM micrographs of the films are shown in
Figure 2. Cross‐sectional images of neat PG films indicated a rough
 |
6 of 9       ASKARI et al.
100:0 PG
50:50 PG/MS
F I G U R E 2   Scanning Electron Micrographs for the cross section of PG/MS blend films
structure. This result may be explained by the gumminess and ge‐
latinous structure of PG solutions, which resulted in the compact
structure of neat PG films. Moreover, MS films showed a brittle
structure. However, a compact and homogenous structure was ob‐
served in composite films. This could be due to compatibility and in‐
teraction between the two polymers, creating a uniform and integral
structure. The results of films’ micrographs confirmed the findings
of water solubility, WVP, and mechanical properties. These results
are similar to the findings of other studies that found a smooth and
compaction surface in starch/hydrocolloid composite films indicat‐
ing the miscibility of the two polymers (Bonilla, Atarés, Vargas, &
Chiralt, 2013; Kanmani & Lim, 2013; Lozano‐Navarro et al., 2018;
Sukhija et al., 2016; Wang, Wang, Ye, Xiao, et al., 2017).
3.6 | FTIR spectroscopy
FTIR spectroscopy is considered one of the most powerful and
widely applicable spectroscopic techniques (Sun, 2009). The FTIR
spectrum shows some interactions between polymers that could
lead to changes in the location, width and/or intensity of peaks
(Bourbon et al., 2011; Marvdashti et al., 2017; Thakur et al., 2016).
Figure 3 shows the FTIR spectrum of the films examined in this
75:25 PG/MS
100:0 MS
study. The characteristic peaks of starch were at 3,000–3,600 cm−1
(O–H stretching), 2,924 cm−1 (C–H stretching), 1,593 cm−1 (O–H
bending of water absorbed), and 860–1,250 cm−1 (C–O stretching of
the anhydroglucose ring and C–H stretching) (Fang, Fowler, Sayers,
& Williams, 2004; Woggum et al., 2014; Zullo & Iannace, 2009).
The intensity of the broad band at ~3,300 cm−1 (O–H stretch‐
ing of starch) increased with increases in the proportion of PG. This
could be due to the presence of more hydroxyl groups in PG, which
could form more hydrogen bonds. An absorption peak at 2,924 cm‐1
in neat starch films corresponds to the C–H stretching vibration of
the polysaccharide matrix. The presence of gum in films resulted in
an increase of this peak’s intensity and a shift to a lower wavenum‐
ber. The intensity of the peak in the 1,018 cm−1 band in neat MS film
dramatically increased with an increase in the proportion of PG. A
peak at 1,593 cm−1 shifted to a higher wavenumber (1,608 cm−1) in
neat PG film. In contrast to the other peaks, those in the range of
1,200–1,650 cm‐1 showed higher intensity in composite films than
in neat PG film. Moreover, the highest intensity in this range was
observed in 75:25 PG/MS film. This might be due to the formation
of new interactions between the two polymers in composite films.
These interactions could lead to improved film integrity, as observed
in the results for solubility, SEM and mechanical properties.
ASKARI et al. |
      7 of 9

Absorbance PG 100:0

MS/PG 25:75

MS/PG 50:50

MS 100:0

3700 3200 2700 2200 1700 1200 700

Wavenumber (cm-1)

F I G U R E 3   The FTIR spectra for PG/MS blend films with different ratios

Generally, the incorporation of PG with MS could form more
hydrogen bonds between the two polymers and reinforce the net‐
work of composite films; this has been reported in previous studies
(Martins et al., 2012; Sukhija et al., 2016; Thakur et al., 2016).
3.7 | Differential scanning calorimetry (DSC)
Thermal analysis includes of melting temperature (Tm) and Glass
transition temperature (Tg). Tg usually measured for crystalline poly‐
mers, which not discussed in this study. DSC thermograms of the
MS 100:0
MS/PG 50:50
Heat Flow ( W/g)
films showed a range for Tm between 101.1 and 121.7°C (Figure 4).
The Tm of neat MS film was significantly (p < 0.05) higher than that of
neat PG film. The crystalline structure of MS could result in low mo‐
bility of the polymer chains and high Tm. The lowest Tm was related
to neat PG film (101.1°C). This can be attributed to the branched
structure of PG, which creates amorphous regions. Therefore, the
Tm of composite films decreased with increasing proportions of PG.
Moreover, the increase of interactions between two polymers could
reduce the crystallinity and Tm of the MS films. These results were in
accordance with those of Jaramillo et al., who reported a decrease
in Tm with the addition of yerba mate extract to cassava starch films
due to interaction between the yerba mate extract and the starch
polymeric chains, which limits the growth of crystals and recrystal‐
lization (Jaramillo, Gutiérrez, Goyanes, Bernal, & Famá, 2016). In
contrast to these results, Sukhija et al. found that the Tm of lotus‐
starch films decreased with decreasing proportions of psyllium husk
(Sukhija et al., 2016). However, Almasi et al. reported an increase in

the Tm of starch–CMC–montmorillonite films with increases in the

MS/PG 25:75 proportion of starch (Almasi, Ghanbarzadeh, & Entezami, 2010).
Galus et al, observed the Tm of oxidized potato starch/soy protein
isolate‐based edible films intensified with increasing of starch con‐
PG 100:0
centration (Galus et al., 2013). This increasing of Tm was resulted
from the crystallinity and ordered structure of starch.

-30 0 30 60 90 120 150 4 | CO N C LU S I O N

Temperature (°C)
The results showed that the physicochemical properties of films,
such as moisture content, solubility, and WVP, were different in
blend films from neat modified starch and psyllium gum films.
F I G U R E 4   DSC thermoghrams of PG/MS blend films Higher proportions of psyllium gum resulted in the films’ higher
 |
8 of 9       ASKARI et al.
flexibility and lower TS. The films’ thermal stability declined with
increased proportions of psyllium gum. SEM results showed com‐
patibility and interactions between the two biopolymers and
the integrity of the resulting composite films. The FTIR spectra
confirmed these findings. Therefore, 75:25 PG/MS blend films
showed suitable physicochemical and mechanical properties for
use in food packaging. It can be concluded that the addition of
psyllium gum could be considered to improve the physicochemical
properties of starch films.
AC K N OW L E D G M E N T S
We are thankful to the Department of Food Science and Technology,
Kermanshah University of Medical Sciences, for support of this
study or their assistance for this research [Grant number: 95392].
ORCID
Ehsan Sadeghi  http://orcid.org/0000-0001-8209-2217
REFERENCES
Ahmadi, R., Kalbasi‐Ashtari, A., Oromiehie, A., Yarmand, M.‐S., &
Jahandideh, F. (2012). Development and characterization of a novel
biodegradable edible film obtained from psyllium seed (Plantago
ovata Forsk). Journal of Food Engineering., 109, 745–751.
Almasi, H., Ghanbarzadeh, B., & Entezami, A. A. (2010). Physicochemical
properties of starch–CMC–nanoclay biodegradable films.
International Journal of Biological Macromolecules., 46, 1–5.
ASTM, Designation E96‐00, (2000). Standard method for water vapor
transmission of materials. In Annual book of ASTM standards.
American Society for Testing and Materials.
ASTM, Designation D882‐02, (2002). Standard method for tensile prop‐
erties of thin plastic sheeting. In Annual book of ASTM standards.
American Society for testing and Materials.
Basiak, E., Galus, S., & Lenart, A. (2015). Characterisation of compos‐
ite edible films based on wheat starch and whey‐protein isolate.
International Journal of Food Science & Technology., 50, 372–380.
Bonilla, J., Atarés, L., Vargas, M., & Chiralt, A. (2013). Properties of wheat
starch film‐forming dispersions and films as affected by chitosan
addition. Journal of Food Engineering, 114, 303–312.
Bourbon, A. I., Pinheiro, A. C., Cerqueira, M. A., Rocha, C. M., Avides,
M. C., Quintas, M. A., & Vicente, A. A. (2011). Physico‐chemical
characterization of chitosan‐based edible films incorporating bio‐
active compounds of different molecular weight. Journal of Food
Engineering, 106, 111–118.
da Rosa Zavareze, E., Pinto, V. Z., Klein, B., El Halal, S. L. M., Elias, M.
C., Prentice‐Hernández, C., & Dias, A. R. G. (2012). Development
of oxidised and heat–moisture treated potato starch film. Food
Chemistry, 132, 344–350.
Dick, M., Costa, T. M. H., Gomaa, A., Subirade, M., de Oliveira Rios, A.,
& Flôres, S. H. (2015). Edible film production from chia seed muci‐
lage: Effect of glycerol concentration on its physicochemical and
mechanical properties. Carbohydrate Polymers, 130, 198–205.
Fang, J., Fowler, P., Sayers, C., & Williams, P. (2004). The chemical mod‐
ification of a range of starches under aqueous reaction conditions.
Carbohydrate Polymers, 55, 283–289.
Farhan, A., & Hani, N. M. (2017). Characterization of edible packaging
films based on semi‐refined kappa‐carrageenan plasticized with
glycerol and sorbitol. Food Hydrocolloids, 64, 48–58.
Galus, S., Lenart, A., Voilley, A., & Debeaufort, F. (2013). Effect of oxi‐
dized potato starch on the physicochemical properties of soy pro‐
tein isolate‐based edible films. Food Technology and Biotechnology,
51, 403–409.
Garavand, F., Rouhi, M., Razavi, S. H., Cacciotti, I., & Mohammadi, R.
(2017). Improving the integrity of natural biopolymer films used in
food packaging by crosslinking approach: A review. International
Journal of Biological Macromolecules, 104, 687–707. https://doi.
org/10.1016/j.ijbiomac.2017.06.093
Garcia, M. A., Pinotti, A., & Zaritzky, N. E. (2006). Physicochemical, water
vapor barrier and mechanical properties of corn starch and chitosan
composite films. Starch‐Stärke., 58, 453–463.
Gennadios, A. (2002). Protein‐based films and coatings. Boca Raton, FL:
CRC Press.
Ghanbarzadeh, B., Almasi, H., & Entezami, A. A. (2010). Physical prop‐
erties of edible modified starch/carboxymethyl cellulose films.
Innovative Food Science & Emerging Technologies, 11, 697–702.
Gutiérrez, T. J., Morales, N. J., Pérez, E., Tapia, M. S., & Famá, L. (2015).
Physico‐chemical properties of edible films derived from native and
phosphated cush‐cush yam and cassava starches. Food Packaging
and Shelf Life, 3, 1–8.
Gutiérrez, T. J., Morales, N. J., Tapia, M. S., Pérez, E., & Famá, L. (2015).
Corn starch 80: 20 “waxy”: Regular, “native” and phosphated,
as bio‐matrixes for edible films. Procedia Materials Science., 8,
304–310.
Jaramillo, C. M., Gutiérrez, T. J., Goyanes, S., Bernal, C., & Famá, L. (2016).
Biodegradability and plasticizing effect of yerba mate extract on
cassava starch edible films. Carbohydrate Polymers, 151, 150–159.
Jouki, M., Khazaei, N., Ghasemlou, M., & HadiNezhad, M. (2013). Effect
of glycerol concentration on edible film production from cress seed
carbohydrate gum. Carbohydrate Polymers, 96, 39–46.
Jouki, M., Yazdi, F. T., Mortazavi, S. A., & Koocheki, A. (2013). Physical,
barrier and antioxidant properties of a novel plasticized edible
film from quince seed mucilage. International Journal of Biological
Macromolecules, 62, 500–507.
Jung, H. G. A. (2006). Innovations in food packaging (pp. 57–86). New York,
NY: CRC Press, USA.
Kanmani, P., & Lim, S. T. (2013). Development and characterization of
novel probiotic‐residing pullulan/starch edible films. Food Chemistry,
141, 1041–1049.
Khazaei, N., Esmaiili, M., Djomeh, Z. E., Ghasemlou, M., & Jouki, M.
(2014). Characterization of new biodegradable edible film made
from basil seed (Ocimum basilicum L.) gum. Carbohydrate Polymers,
102, 199–206.
Krochta, J. M., Baldwin, E. A., & Nisperos‐Carriedo, M. O. (1994). Edible
coatings and films to improve food quality. Lancaster, PA: Technomic
Publ Co.
Lago‐Vanzela, E., Do Nascimento, P., Fontes, E., Mauro, M., & Kimura,
M. (2013). Edible coatings from native and modified starches re‐
tain carotenoids in pumpkin during drying. LWT‐Food Science and
Technology, 50, 420–425.
López, O. V., García, M. A., & Zaritzky, N. E. (2008). Film forming capac‐
ity of chemically modified corn starches. Carbohydrate Polymers, 73,
573–581.
Lozano‐Navarro, J. I., Díaz‐Zavala, N. P., Velasco‐Santos, C., Melo‐
Banda, J. A., Páramo‐García, U., Paraguay‐Delgado, F., …
Zapién‐Castillo, S. (2018). Chitosan‐starch films with natural ex‐
tracts: Physical, chemical. Morphological and Thermal Properties.
Materials, 11, 120.
Martins, J. T., Cerqueira, M. A., Bourbon, A. I., Pinheiro, A. C., Souza,
B. W., & Vicente, A. A. (2012). Synergistic effects between κ‐car‐
rageenan and locust bean gum on physicochemical properties of
edible films made thereof. Food Hydrocolloids, 29, 280–289.
Marvdashti, L. M., Koocheki, A., & Yavarmanesh, M. (2017). Alyssum ho‐
molocarpum seed gum‐polyvinyl alcohol biodegradable composite
ASKARI et al.
film: Physicochemical, mechanical, thermal and barrier properties.
Carbohydrate Polymers, 155, 280–293.
Mohammadi, R., Mohammadifar, M. A., Rouhi, M., Kariminejad, M.,
Mortazavian, A. M., Sadeghi, E., & Hasanvand, S. (2018). Physico‐
mechanical and structural properties of eggshell membrane gela‐
tin‐chitosan blend edible films. International Journal of Biological
Macromolecules, 107, 406–412.
Parra, D., Tadini, C., Ponce, P., & Lugão, A. (2004). Mechanical properties
and water vapor transmission in some blends of cassava starch edi‐
ble films. Carbohydrate Polymers, 58, 475–481.
Qiu, L., Hu, F., & Peng, Y. (2013). Structural and mechanical character‐
istics of film using modified corn starch by the same two chemical
processes used in different sequences. Carbohydrate Polymers, 91,
590–596.
Ramos, Ó. L., Reinas, I., Silva, S. I., Fernandes, J. C., Cerqueira, M. A.,
Pereira, R. N., … Malcata, F. X. (2013). Effect of whey protein purity
and glycerol content upon physical properties of edible films manu‐
factured therefrom. Food Hydrocolloids, 30, 110–122.
Rao, M. R., Warrier, D. U., Gaikwad, S. R., & Shevate, P. M. (2016).
Phosphorylation of psyllium seed polysaccharide and its charac‐
terization. International Journal of Biological Macromolecules, 85,
317–326.
Razavi, S. M. A., Amini, A. M., & Zahedi, Y. (2015). Characterisation of a
new biodegradable edible film based on sage seed gum: Influence of
plasticiser type and concentration. Food Hydrocolloids, 43, 290–298.
Santacruz, S., Rivadeneira, C., & Castro, M. (2015). Edible films based
on starch and chitosan. Effect of starch source and concentration,
plasticizer, surfactant’s hydrophobic tail and mechanical treatment.
Food Hydrocolloids, 49, 89–94.
Seyedi, S., Koocheki, A., Mohebbi, M., & Zahedi, Y. (2014). Lepidium per‐
foliatum seed gum: A new source of carbohydrate to make a biode‐
gradable film. Carbohydrate Polymers, 101, 349–358.
Sukhija, S., Singh, S., & Riar, C. S. (2016). Analyzing the effect of whey
protein concentrate and psyllium husk on various characteristics
of biodegradable film from lotus (Nelumbo nucifera) rhizome starch.
Food Hydrocolloids, 60, 128–137.
Sun, D.‐W. (2009). Infrared spectroscopy for food quality analysis and con‐
trol. Cambridge, MA: Academic Press.
Sun, Q., Sun, C., & Xiong, L. (2013). Mechanical, barrier and morphologi‐
cal properties of pea starch and peanut protein isolate blend films.
Carbohydrate Polymers, 98, 630–637.
Thakur, R., Saberi, B., Pristijono, P., Golding, J., Stathopoulos, C., Scarlett,
C., … Vuong, Q. (2016). Characterization of rice starch‐ι‐carra‐
geenan biodegradable edible film. Effect of stearic acid on the film
properties. International Journal of Biological Macromolecules, 93,
952–960.
|
      9 of 9
Thakur, V. K., & Thakur, M. K. (2014). Recent trends in hydrogels based
on psyllium polysaccharide: A review. Journal of Cleaner Production,
82, 1–15.
Ustunol, Z. (2009). Edible films and coatings for food applications (pp. 245–
268). New York, NY: Springer.
Vu, H. P. N., & Lumdubwong, N. (2016). Starch behaviors and mechan‐
ical properties of starch blend films with different plasticizers.
Carbohydrate Polymers, 154, 112–120.
Wang, L., Auty, M. A., & Kerry, J. P. (2010). Physical assessment of com‐
posite biodegradable films manufactured using whey protein iso‐
late, gelatin and sodium alginate. Journal of Food Engineering, 96,
199–207.
Wang, W., Wang, K., Xiao, J., Liu, Y., Zhao, Y., & Liu, A. (2017). Performance
of high amylose starch‐composited gelatin films influenced by ge‐
latinization and concentration. International Journal of Biological
Macromolecules, 94, 258–265.
Wang, K., Wang, W., Ye, R., Liu, A., Xiao, J., Liu, Y., & Zhao, Y. (2017).
Mechanical properties and solubility in water of corn starch‐colla‐
gen composite films: Effect of starch type and concentrations. Food
Chemistry, 216, 209–216.
Wang, K., Wang, W., Ye, R., Xiao, J., Liu, Y., Ding, J., … Liu, A. (2017).
Mechanical and barrier properties of maize starch–gelatin compos‐
ite films: Effects of amylose content. Journal of the Science of Food
and Agriculture, 97, 3613–3622.
Woggum, T., Sirivongpaisal, P., & Wittaya, T. (2014). Properties and char‐
acteristics of dual‐modified rice starch based biodegradable films.
International Journal of Biological Macromolecules, 67, 490–502.
Yu, L., Perret, J., Parker, T., & Allen, K. G. (2003). Enzymatic modification
to improve the water‐absorbing and gelling properties of psyllium.
Food Chemistry, 82, 243–248.
Zullo, R., & Iannace, S. (2009). The effects of different starch sources
and plasticizers on film blowing of thermoplastic starch: Correlation
among process, elongational properties and macromolecular struc‐
ture. Carbohydrate Polymers, 77, 376–383.
How to cite this article: Askari F, Sadeghi E, Mohammadi R,
et al. The physicochemical and structural properties of
psyllium gum/modified starch composite edible film. J Food
Process Preserv. 2018;42:e13715. https://doi.org/10.1111/
jfpp.13715