j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 1 ; 1 5 : 1 3 4 2 e1 3 5 5

Available online at www.sciencedirect.com

journal homepage: www.elsevier.com/locate/jmrt

Original Article

Preparation and characterization of starch-based

biocomposite films reinforced by Dioscorea hispida
fibers

K.Z. Hazrati a,b, S.M. Sapuan a,c,*, M.Y.M. Zuhri a,c, R. Jumaidin d
a
Advanced Engineering Materials and Composites Research Centre, Department of Mechanical and Manufacturing
Engineering, Universiti Putra Malaysia, 43400, UPM Serdang, Selangor, Malaysia
b
German Malaysian Institute, Jalan Ilmiah, Taman Universiti, 43000, Kajang, Selangor, Malaysia
c
Laboratory of Biocomposite Technology, Institute of Tropical Forestry and Forest Products (INTROP), Universiti
Putra Malaysia, 43400, UPM Serdang, Selangor, Malaysia
d
Fakulti Teknologi Kejuruteraan Mekanikal dan Pembuatan, Universiti Teknikal Malaysia Melaka, Hang Tuah Jaya,
76100, Durian Tunggal, Melaka, Malaysia

article info abstract

Article history: In this paper, Dioscorea hispida starch (DHS) biocomposites films were successfully prepared
Received 15 May 2021 via combining D. hispida starch with sorbitol at different sizes (F1, F2) and concentrations
Accepted 1 September 2021 (3, 6, and 9 wt%) D. hispida fiber (DHF) using a film-forming casting technique. Character-
Available online 3 September 2021 ization via physical, morphological, mechanical, thermal, and biodegradability was con-
ducted on the films. A significant increment in tensile strength (TS) of the D. hispida starch
Keywords: based films was found with rising fiber content 3e6% and a 9% decrement in concentration.
Dioscorea hispida fiber The different sizes and concentrations of D. hispida fiber which were used with 6% small-
Starch sized fibers displayed the highest capabilities of increasing the tensile strength and
Biodegradable film decreasing elongation at break and possessing high value of Young's modulus. The findings
Biocomposites demonstrated that tensile strength and Young modulus of the biocomposite films were
Tensile properties increased after reinforcement with D. hispida fibers, and the optimal biofiller content was
Thermal properties 6%. The biocomposites film revealed a novel waste material, D. hispida fiber, that is eco-
friendly and easy to process. It also generates new information on the interactions of
different fiber sizes and their effect on the film abilities, which can aid in development of
biodegradable materials.
© 2021 The Author(s). Published by Elsevier B.V. This is an open access article under the CC
BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).

* Corresponding author.
E-mail address: sapuan@upm.edu.my (S.M. Sapuan).
https://doi.org/10.1016/j.jmrt.2021.09.003
2238-7854/© 2021 The Author(s). Published by Elsevier B.V. This is an open access article under the CC BY-NC-ND license (http://
creativecommons.org/licenses/by-nc-nd/4.0/).
 j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 1 ; 1 5 : 1 3 4 2 e1 3 5 5
1. Introduction
Petroleum-derived plastics are among the main materials
used in the packaging industry, which have been raising
global environmental issues for decades. The increasing
growth of environmental-threatening plastic waste has
stimulated the evolution of nature-based, renewable, as well
as biodegradable materials. The desirable characteristics of
the potential materials include environmental sustainability
and no polluting carbon emissions generation during pro-
cessing, and even after destruction [1e4]. An essential alter-
native to conventional plastic materials is biodegradable films
and coatings. Hence, many biopolymer composites have been
used to produce materials for environmentally-safe food
packaging applications [5e7]. The field of packaging materials
is becoming extremely valuable as a response to customer
demand and industry trends. Active packaging is a creative
term that can be described as a mode of packaging whereby
the interaction between the packaging, product, and envi-
ronment takes place to prolong the shelf life of a product or to
enhance safety or sensory characteristics while maintaining
its quality [8]. It is predicted that this excessive quantity of
packaging material will be quickly disposed of as waste after a
single use [9].
Furthermore, due to difficulties in differentiating polymer
and additional costs in recycling, the excess amount of plastic
waste is too much for the recycling program to accommodate
[10]. The pollution of synthetic plastic packaging has been
contributing to the environmental destruction problem,
which has resulted in the urgency to produce eco-friendly
packaging products at a comparable cost in order to
conserve our world [11]. Therefore, natural biopolymers, e.g.
PLA, PHAs, protein, and starch based plastics are being
explored as possible replacements for conventional plastics in
overcoming this ongoing problem caused by non-
biodegradable plastics [12,13].
Starch films have been used widely for both food and non-
food purposes. Enhancing starch-based materials' properties
is a significant challenge because of their poor mechanical
efficiency, especially tensile strength [14]. Numerous blending
and compositing methodologies have been developed to
enhance these mechanical characteristics, e.g. blending with
various polymers or reinforcing natural fillers [15]. Different
types of additive agents have been used to strengthen the
interaction between starch and other elements. However,
because of safety concerns or toxicity issues, any additive is
vulnerable to the development of edible packaging films [16].
Among the main factors in fixing these crucial matters is to
understand the physicochemical properties of starch, thermal
characteristics, and the development of starch formulation
[17].
More attention has recently been directed to the addition of
filler reinforcement to starch-based polymers to create bio-
composites, along with the development of polymer bio-
composites [18,19]. This natural filler reinforcement method
has been verified as a successful approach for simultaneously
enhancing these properties and introducing new features to
starch-based material [20]. Recently, cellulosic fibers and
polymers from plants have played important roles as
1343
feedstock in various applications due to their unique envi-
ronmental benefits [21]. The strong correlation between
starch matrix and cellulose fiber and is significant for me-
chanical efficiency and hydrous sensitivity enhancement [22].
An effective way of developing the functional characteristics
of composite films is using natural fibers as reinforcing agents
in the starch-based composite's development. Therefore, re-
searchers have performed many studies to enhance the water
barrier and mechanical performance characteristics of ther-
moplastic starch based materials without compromising their
biodegradability [23,24].
In the context of biopolymers, a variety of fiber re-
inforcements have recently been used, including potato peel
waste [25], cassava bagasse [26], and sugar palm [27]. Rein-
forcing starch matrix and natural fibers has proven due to
their great compatibility resulting from the creation of the 3D
hydrogen bonding structure between starch and fiber com-
ponents, resulting in improved biocomposite's performance
(e.g. water permeability and mechanical properties), thus
improving their characteristic as a food packaging material
[28,29]. According to the findings of Dioscorea hispida fiber [30],
the fiber has a considerable amount of cellulose, thereby
serving as a source of cellulose fiber. Besides, D. hispida tubers
have rich starch and green fiber content obtained from
bagasse fibers to develop biodegradable composite materials,
respectively. The characterization findings of native starch
films by authors for active food packaging uses indicated that
improving both the water vapor barrier and the films' me-
chanical properties would further improve their performance
[31].
However, to the best of our knowledge, no information is
available on the preparation and characterization of D. hispida
starch composite films reinforced with D. hispida fibers using
sorbitol as a plasticizer. This research's main objective is to
evaluate the effect of different D. hispida fiber loadings with
two particle sizes of the fiber used on the biocomposite's
physical, morphological, tensile, and thermal properties. It
should be noted that the fiber used in this work was not either
chemically treated or modified, resulting in more environ-
mentally sustainable and cheaper materials being produced.
2. Materials and methods
2.1. Materials
D. hispida starch was derived from fresh tubers purchased
from local farm M Abd Halim Enterprise, Kuala Terengganu,
Malaysia by following the procedure in the published study
[30]. D. hispida fiber was washed, dehydrated, grounded, and
screened with mesh sieve (F1 ˂ 300 mm and 300 mm˂ F2 ˂600 mm)
and transformed into powder form. Sorbitol plasticizer was
supplied by Evergreen Sdn. Bhd., Selangor, Malaysia.
2.2. Preparation of biocomposite films
The casting technique was applied in the preparation of the
starch films composite using a film-forming solution
comprising 5 g and 100 mL of D. hispida starch and distilled
water, respectively. The concentration of sorbitol used was
1344 j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 1 ; 1 5 : 1 3 4 2 e1 3 5 5

0.30 g/g of dry starch. D. hispida fiber was used as filler at
various concentrations (3, 6, and 9% w/w dry starch). Two
particle size ranges denoted by F1< 300 mm and 300 mm < F2 <
600 mm were used. F1-3, F1-6, and F1-9 were allocated
respectively for films comprising 3, 6, and 9% w/w dry starch
of small size fiber. F2-3, F2-6, and F2-9 films were labeled with
3, 6, and 9% w/w dry starch of a large fiber scale. In a thermal
bath, the mixture was heated to 85
C and was let and
continuously stirred for 20 min in this state. After that, a
vacuum desiccator was used to store the mixture to prevent
the air bubbles formation. The solution (45 g) was then cast
equally onto thermal plates with a diameter of 140 mm and
placed in an air circulation oven at 50
C for 24 h for drying.
The dried films were then peeled off the Petri-dish plates and
kept at ambient temperature for one week in individual plastic
bags before characterization.
2.3. Film thickness of biocomposites
The films’ thickness was calculated using a digital micrometer
(Mitutoyo Co., Japan) with an accuracy of ±0.001 mm. For each
film sample, five random measurements were taken and an
average value was calculated.
2.4. Density of biocomposite films
The film density was calculated from its volume (V) and
weight (m). Based on the dimensions proposed
(10 mm  30 mm), the size of each film was determined by the
thickness obtained from the film thickness analysis. The
calculation of the film density (r), was achieved by means of
the Eq. (1).
m
r¼
V
where, m ¼ mass (g), V ¼ volume (cm3).
2.5. Moisture content of biocomposite films
determination of each film sample's moisture content. The
experiment was performed in triplicate, and the mean result
for each film was calculated to be the final moisture content.
MC ð%Þ ¼ ððwi  wf Þ=wiÞ  100 (2)
2.6. Water solubility
Vacuum oven drying for the film samples (30 mm  10 mm)
was carried out at 105
C for 24 h with the various bio-
composite film concentrations. The initial dry matter of each
specimen was fixed by examining the sample's weight and
described as (Wi). This was supported by immersing each
specimen in a beaker containing distilled water (100 mL). The
beaker was then affixed, and the beaker was continuously
stirred under constant stirring for a period of 6 h at a tem-
perature of 23 ± 2
C. Finally, the sample fraction that did not
dissolve was isolated and allowed to dry for 24 h in an oven at
105
C temperature and subsequently weighed (Wo). Using Eq.
(3), each sample's water solubility was determined.
Wi  Wo
Solubility ð%Þ ¼ ½   100 (3)
Wi
2.7. Water absorption
Investigation of water absorption was conducted with the
implementation of the ASTM D 570-98 (1998) approach. The
film samples were oven dried at 50
C for 24 h and then cooled
in a desiccator to ensure consistent weight. Then, the speci-
mens were weighed at room temperature, immersed in
distilled water. The soaked film samples were cleaned and
reweighed with a clean piece of cloth. Using the recorded
initial and final masses, the mass difference was calculated
(1) using Eq. (4).
Mfinal  Minitial
Water absorptionð%Þ ¼  100 (4)
Minitial
2.8. Soil burial test

The film samples' moisture content was calculated by

The tests for biodegradation were performed for all samples
weighing each sample initially (wi) using a digital weighing
using the method defined by Ibrahim et al. [23], respectively.
scale. Drying of the film samples was performed in an oven for
Each film sample with equal volume with the known weight
24 h at a temperature of 105
C (wf). Eq. (2) was applied for the
(Wi) was placed in a control condition and buried 5 cm deep in

Fig. 1 e (a) Thickness and (b) density of Dioscorea hispida biocomposite films.
 j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 1 ; 1 5 : 1 3 4 2 e1 3 5 5
Fig. 2 e (a) Moisture content, (b) water solubility and (c) water absorption of Dioscorea hispida biocomposite films.
moist soil. The weight loss (WL) assessment was carried out in
triplicate by getting the samples from the soil at various pe-
riods followed by rubbing them gently with a brush. The
samples were then dehydrated at 105
C for 6 h and reweighed
(Wf). The analysis of degradation was performed on the
collected samples every couple of days and determined using
the Eq. (5):
Wo  Wt
Weight lossð%Þ ¼  100
Wo
2.9. Microstructure of films
The samples' morphological surface properties were investi-
gated by an SEM instrument (Hitachi S-3400 N, Nara, Japan). A
thin gold layer was applied to the film samples to supply
electricity before scanning. A high vacuum voltage of 20 kV
was applied to generate a pack of electrons that convey sig-
nals to visualize the surface topography and generate images
of high resolution.
2.10. Fourier transforms infrared (FTIR) spectroscopy
The samples’ FT-IR spectrum was tracked by a spectrometer
type (Bruker Vector 22, Lancashire, UK) to examine functional
1345
groups' existence in the film samples. The analysis was con-
ducted with 16 scans of 4000e400 cm1 in each sample, with a
4 cm1 spectral resolution.
2.11. Thermogravimetric analysis (TGA)
The thermal analyzer (Q500 V20.13 Build 39, Bellingham, USA)
was applied to investigate the specimens' thermal behavior.
(5) The film specimens were placed under a vacuum of nitrogen
in a platinum vessel and heated from room temperature to


500
C at a fixed heating rate of 10 C/min. TGA generates data
weight loss as a function of temperature as TGA (thermogra-
vimetric) and DTG (derivative of thermogravimetric) curves.
2.12. Tensile properties
The tensile properties of biocomposite films were tested using
5 kN INSTRON tensile machines of compliance with the D882
(ASTM, 2002) standard in ambient conditions. Both ends of the
film strips (10  70 mm) were tightly connected to tensile
clamps. The initial measurement length and crosshead speed
was fixed to 30 mm, and 2 mm/min, respectively. Each sample
underwent five repetitions to determine elastic modulus,
tensile strength, and break elongation.
1346 j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 1 ; 1 5 : 1 3 4 2 e1 3 5 5
2.13. Statistical analysis
SPSS software was applied to conduct variance analysis
(ANOVA) on the obtained experimental results. Duncan's test
was employed to perform a means comparison with a signif-
icance level of 0.05 (p  0.05).
3. Results and discussion
3.1. Thickness and density of the biocomposite starch
films
There were no obvious significant differences in film densities
and thicknesses among the various D. hispida starch-based
composite films. However, when fiber was added, the thick-
ness was observed to increase while the density was
decreased with minimal variations, as shown in Fig. 1. During
the casting process, the content of dry mass per unit area of
the film-forming solutions was strictly controlled, resulting in
different thickness values for control films D. hispida starch
and D. hispida biocomposite films. The slight variation in film
density had resulted between control and D. hispida composite
films (Fig. 1(a)). It might be caused by the filler that was much
more concentrated in the film matrix, where it was stated that
the density of the D. hispida fiber was 1.47 g/cm3 [30]. Edhirej
et al. [26] revealed that cassava starch-based composite film
density was respectively affected by the reinforcement of
bagasse fiber with different concentrations and sizes.
The fiber size affected the thickness as well, and when
comparing films with small size fiber and films with the large-
sized fiber of the same concentration, the films' thickness with
small size fiber was lower. The higher fiber content and a
larger filler size resulted in thicker and rougher films [32]. The
phenomenon might have been explained by the fiber's
chemical properties, which related an abundance of hydroxyl
groups in a large surface area of fiber, whereby strong in-
teractions between fibers were partially destroyed and a new
strong interfacial adhesion was created between the fibers
and starch matrix after the film processing [33]. The free vol-
ume within the starch biopolymer was reduced as a result of
creating a strong adhesion matrix/fiber, making it more
compact than neat starch. A substance's density, or more
precisely, its density of volumetric mass, is its mass per unit
volume. The lower the volume of the biofilms, the higher the
density of the biofilms. Furthermore, these results were
aligned with findings by Ibrahim et al. [15] and Sanyang et al.
[34].
3.2. Moisture content
D. hispida starch film composites with different sizes and
concentrations of fiber had moisture contents of 5.70%e
10.46% that were lower than that of the control Dioscorea his-
pida biopolymer film (10.46%) (Fig. 2(a)). Increasing the con-
centrations of size fiber (F1eF2) from 3 to 9% (w/w) resulted in
a substantial increase in the films' moisture content due to the
D. hispida starch film's hydrophilic behavior that includes a
multi-hydroxyl polymer with three hydroxyl groups per
monomer. Reinforcement of D. hispida fiber had raised the
hydrophilic content. This might be due to the tight hydrogen
bonds that exist between the filler and the matrix, influencing
water from coming into contact with the starch molecules
[35].
3.3. Water solubility
Fig. 2(b) shows the biocomposites' water solubility, which
emphasized continuous stirring on the composite films during
their water immersion. One of the most critical properties to
understand in biodegradable packaging is the water solubility
of films. Due to its high water solubility, starch's applications
are usually limited [36]. Water insolubility can be required for
various applications, including improving product quality and
providing water barriers to securely store food products.
Starch usually has restricted applications because of its high
water solubility. As a result, D. hispida starch reinforced with
D. hispida fiber should be able to resolve this limitation.
Fig. 2(b) shows the film solubility of D. hispida biocomposite
films. When biofilms were immersed in water, it was discov-
ered that they did not stay undamaged. Even though the films
had the highest moisture stability, the solubility was found to
decrease with an increased concentration of fiber. The addi-
tion of D. hispida fiber reduced films' solubility from 47.0% to
36.0% for the smaller fiber size (F1) and 40.60%e33.23% for the
bigger fiber size (F2).
The F2-9 demonstrated the lowest film solubility of 33.23%,
which revealed that the films had good water stability. The
interactions between filler-D. hispida fiber and D. hispida starch
chains in the film matrix were also strong. The existence of
interaction of hydrogen bonds in starch with the hydroxyl
groups present in the D. hispida fiber was responsible for the
fiber's ability to interact with starch chains. The stability and
water-resistance of D. hispida biocomposite films were
improved as a result of these interactions. These interfaces
improved the biopolymer matrix's cohesiveness and reduced
water sensitivity because water molecules failed to separate
these strong bonds properly. Furthermore, Edhirej et al. [37]
discovered that when the fiber was added to the biopolymer,
the film's water solubility decreased. They reported that there
was a relationship between the strong hydrogen bonds
formed between the biopolymer's hydroxyl groups and the
filler hydroxyl groups. The F2-9 demonstrated the lowest D.
hispida film's solubility value of 33.23%, which revealed that
the film samples possessed excellent water stability. Within
the film matrix, there were also indications of strong con-
nections between the individual D. hispida fiber and D. hispida
starch chains.
The interaction between the hydrogen bonds in starch
with the hydroxyl groups of D. hispida fiber was responsible for
D. hispida fiber's ability to bind with starch chains. These in-
teractions had improved the stability and water resistance of
the plasticized D. hispida starch/D. hispida fiber films. Ilyas
et al. [38] reported that these interfaces resulted in biopolymer
matrix increased cohesiveness and decreased water sensi-
tivity, as water molecules were incapable of cleaving the
strong bonds. Furthermore, Rhim and Ng [39] discovered that
when the starch film was combined with the fillers, its water
solubility decreased, which might be associated with the
strong hydrogen bond formation between the biopolymer's
 j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 1 ; 1 5 : 1 3 4 2 e1 3 5 5 1347

hydroxyl groups and the biofiller's hydroxyl groups. These
findings were also verified by Dularia et al. [40] in their bio-
composite film research study. Moreover, Jha [41] determined
that the structure of matrix and the resulting interaction be-
tween matrix/filler and filler/filler were important factors to
consider when determining the reinforcing impact of natural
fillers. It can be concluded that adding biofiller to the films
improved their water resistance, which was an important
feature for food packaging materials for the purpose of
extending the food products' shelf life.
3.4. Water absorption
Fig. 2(c) shows the findings of the water absorption test for D.
hispida biocomposite films. Based on a Fickian diffusion pro-
cess, weight gain due to water absorption experienced by all

Fig. 3 e Cross-sectional morphology (500£ magnification) of the biocomposite films.

1348 j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 1 ; 1 5 : 1 3 4 2 e1 3 5 5
biocomposite films increases linearly with longer immersion
time and becomes more stable after 1 h. Vilay et al. [42]
revealed that the fiber content, temperature, permeability,
orientation, surface protection, and exposed surface area
affected water absorption analysis. Temperature and fiber
size content was controlled in this study. Due to the same
processing parameters, the D. hispida fiber orientation in the D.
hispida starch biofilm was assumed to be similar. The hydro-
philicity of films reinforced with D. hispida fiber was higher
due to the hydroxyl groups existence in the films' molecules,
and the biocomposite films had the highest potential for water
absorption. From Fig. 3, all D. hispida films absorbed high water
amount after 60 min of immersion in water at ambient tem-
perature because of the hydrophilicity of starch and fiber. The
water absorption of the D. hispida films was increased with
rising fiber content due to the fiber's properties, e.g. water
solubility and naturally hygroscopic.
Furthermore, the control film had absorbed about 81.23% of
water within an hour while the 3, 6, and 9% small size fiber-
containing films absorbed about 80.37, 81.77, and 83.47%, of
water, respectively. Similarly, films comprising 3, 6, and 9%
big size fiber absorbed 86.33, 87.07, and 88.27%, respectively.
3% fiber film absorbed less water than other films. For the film
containing 9% big size fiber, the highest water uptake
observed was 96.80% at 180 min, while at the same duration,
the lowest value was 84.80% for 3% small size fiber film. A
similar pattern was demonstrated by Salaberria et al. [43] who
utilized chitin as a filler in thermoplastic starch-based com-
posites and revealed that the biocomposites’ rate of water
absorption was proportional to the filler percentage in the
thermoplastic starch matrix. Biocomposites having low and
high filler contents were more and less resistant to water ab-
sorption than the thermoplastic starch matrix, respectively.
According to Edhirej et al. [44], the higher filler content
contributed to the increment in water absorption of cassava
starch-based composite films that was ascribed to the hy-
groscopic nature of cassava peel fiber. However, the high hy-
drophilicity of D. hispida starch and D. hispida fiber is most
likely to contribute to this hygroscopic nature.
Fig. 4 e Weight loss of Dioscorea hispida starch films
composite.
Stimulation of the starch structure's hydrophilicity takes
place with fiber incorporation of fiber by raising porosity
within the starch matrix which led to higher water diffusion.
The control film demonstrated a higher water absorption than
F1˂ 300 mm film samples because of their high hydrophilic
existence. Despite this, the addition of the large D. hispida fiber
resulted in a substantial decrease in the water absorption
value and reduced hydrophilicity by increasing the concen-
tration of fiber. For F2-9, the presence of D. hispida fiber and its
increased concentration to 9 wt % had decreased the control
film's water absorption by 8%. It was revealed that the control
film of D. hispida starch exhibited the highest water absorp-
tion. In contrast, the biocomposite films were reasonably
resistant to water uptake due to their less hydrophilicity
caused by the strong interaction between filler and matrix
adhesion. Furthermore, when the starch matrix is exposed to
a moist environment, the biocomposite films' strong hydrogen
bonding interactions help to stabilize it [18].
3.5. Morphological properties
Fig. 3 shows the SEM image of the cross-sectional surface of
the D. hispida starch-based film samples with and without D.
hispida fiber addition. The control film's surface displayed a
smooth and even surface without traces of starch granules or
cracks. Similar SEM image observation was reported in a work
completed by Aydogdu et al. [45] for the lentil flour films. In
addition, it was observable from the cross-sections of all films
that the control film surface was smooth, while the D. hispida
starch biocomposite film was very rough. This phenomenon
was due to the rising D. hispida fiber concentration and
apparent aggregation of fiber within the D. hispida starch
matrix that resulted in the irregularities on the D. hispida
starch composite film's surface. Multiple macromolecules had
caused these irregularities in the polymer matrix, such as
starch, lipids, protein, and fibers. The interactions between
these polymers had resulted in the formation of stable com-
plexes. The amylose-lipid and protein-lipid complexes might
Fig. 5 e FTIR spectra of Dioscorea hispida starch
biocomposite films.
 j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 1 ; 1 5 : 1 3 4 2 e1 3 5 5 1349

have disrupted the starch matrix's continuity, resulting in a
less dense and nonhomogeneous structure [45].
The rough structures indicated the interfacial adhesion
between D. hispida fiber and D. hispida starch polymer that was
comparatively low. The observed cross-sections of the D. his-
pida starch biocomposites (Fig. 3) were also coarser than the D.
hispida starch films due to the D. hispida fiber incorporation as
filler. However, it appeared to be much smoother than the F2-9
biocomposite film. This implied that low-concentration D.
hispida fiber had a stronger interaction with D. hispida starch
and distributed more uniformly within the D. hispida starch
matrix than high-concentration D. hispida fiber. The film with
3% fiber has a compacted structure and smooth poreless
surfaces. D. hispida starch film microstructure with 6% small
fiber size (F1-6) demonstrated a smooth surface and uniform
texture. For the film with 9% fiber, a less compact structure
and a rough texture with large pores were observed. It might
be due to the fiber joining that was not desired, resulted in
reduced stress transfer from the matrix to the fiber, conse-
quently reduced the mechanical strength of biocomposites
[26]. It was found that the thermoplastic starch matrix was
separated with a crack, and gaps were left in the matrix film
with 9% fiber.
In starch-based films, the matrix's homogeneity is a sig-
nificant indicator of its structural reliability, and it can be
predicted the 6% fiber had considerably enhanced the films'
mechanical performance. The improved compatibility be-
tween D. hispida fiber and D. hispida starch was ascribed to the
comparable chemical compositions in fiber and starch, effect
of matrix size due to the D. hispida fiber, as well as hydrogen
bond linkages between filler and matrix [30]. The natural
filler's even dispersion and strong adhesion in the matrix
might have played a significant part in improving the me-
chanical efficiency of the subsequent biocomposite films (high
elasticity). Furthermore, these findings were parallel with
other studies performed by Podshivalov et al. [46], and Alves
et al. [47].
3.6. Biodegradation of the biocomposite starch films
The researches on the properties of biodegradation are
essential for the implementation of biocomposite films in the
environment. In this study, soil burial tests were performed
for the unreinforced D. hispida starch film, as well as the bio-
composite film sample. In short, biodegradation is defined as
the material decomposition by fungi, bacteria, or other bio-
logical decomposers [48]. The interaction of microbial organ-
isms generally starts polymer decomposition with
biodegradable polymer. Via an enzymatic or metabolic pro-
cess, these microbial organisms break down the polymer into
smaller compounds with a lower average molecular weight.
This aided the decomposition of wastes in the environment.
The process is called mineralization when the biodegradation
was completed [46]. The weight loss of control film, F1-3, F1-6,
F1-9, F2-3, F2-6, and F2-9 biocomposite films as a function of
biodegradation time showed the degradation of 56.30, 58.5,
64.5, 69.5, 62.0, 66.2, and 74.5%, at the end of 10 days, as pre-
sented in Fig. 4. The average rate of degradation was 5.63%/
day and 7.45%/day for the control film and F2-9, respectively.
The weight loss of D. hispida starch biocomposites was
observed to be higher than the control at any time points. The
control film was found to completely degrade after 12 days.
In the meantime, biocomposite films took 10 days to fully
degrade. In terms of weight loss, the control matrix exhibited
smaller loss compared to the biocomposite films. The water
absorption and crystallinity degree of D. hispida starch in
biocomposite films were two factors that might have

Table 1 e Thermal degradation for control and Dioscorea

hispida starch biocomposite films in different sizes and
concentrations.
Film Degradation DTG Peak Mass
Temperature (oC) Temperature Residue
(oC) (%)
T10% T25% T50%
Control 178.5 286.5 308.3 311.5 16.38
F1-3 235.5 295.2 322.0 323.3 19.69
F1-6 229.2 294.3 321.7 327.2 19.16
F1-9 245.3 295.3 322.7 326.5 19.60
F2-3 229.3 295.2 322.2 326.2 19.20
F2-6 171.8 293.8 321.7 320.7 18.84
Fig. 6 e TGA and DTG of control and Dioscorea hispida F2-9 249.7 298.0 324.8 329.2 18.87

starch biocomposite films in different concentrations.

1350 j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 1 ; 1 5 : 1 3 4 2 e1 3 5 5
contributed to this situation. For all of the successive degra-
dation tests, weight loss for the D. hispida starch control film
was lower than the D. hispida starch biocomposites. Due to D.
hispida starch biocomposites' physical properties, more water
was absorbed by them than the control films that resulted in
their higher susceptibility to microbial attack [14]. When in a
water medium, these microbial organisms infected the starch
composite films that can be described by the properties of
water absorption of starch-based film composites, which were
about 89.47% for the control film and 96.8% for the F2-9 bio-
composite film. The fiber size also influenced the film degra-
dation, whereby films with larger fiber size degraded more
quickly, especially when the fiber content was high. This was
most likely due to the large fiber that possessed a higher ratio
of surface area. The findings suggested that films with a larger
size or higher fiber content had a great tendency for biodeg-
radation, making them more vulnerable to microorganisms
attack [26]. Indeed, the findings revealed that the D. hispida
starch biocomposite films would not have an environmental
effect, implying that the D. hispida starch biocomposites film
was fully biodegradable.
3.7. FTIR of D. hispida biocomposite films
The functional groups that exist in the chemical structure of
crystalline starch and cellulose can be interpreted using FT-IR
spectroscopy, a good characterization approach [49]. The FT-
Fig. 7 e Effect of Dioscorea hispida fiber size and concentration on the (a) tensile strength, (b)Young modulus, (c) elongation at
break (%) Dioscorea hispida starch biocomposite films.
IR spectra of the control film and D. hispida starch bio-
composite films with different concentrations of D. hispida
fiber were presented in Fig. 5. In the 3600e3020 cm1 wave-
length range, the D. hispida starch film showed a wide peak
that might be associated with the hydroxyl (OH) group. At
2950 cm1, the peak might be attributed to the stretching of
CeH, even though a small peak that appeared at 1680 cm1
might be associated with the stretching of CO (carbonyl). Hy-
droxyl (OH) group of water was detected at 1305 cm1
wavelength, which was aligned with findings from Aloui et al.
[50] and Edhirej et al. [44] with gallnut and cassava starch
films, respectively. The carbonyl functionality (C) that existed
in COC groups might be correlated to the sharp peak at
1004 cm1.
In contrast to the D. hispida starch biocomposite films, the
IR spectrum of the control D. hispida starch control film was
similar. The absence of new peaks resulted in a negligible ef-
fect of the incorporation of D. hispida fiber on the IR spectrum
of the control film. Since D. hispida fiber and D. hispida starch
matrices are both derived from a single source (D. hispida tu-
bers), a potential agreement between the two components
was demonstrated. Furthermore, this circumstance indicated
inter-and/or intramolecular interaction(s) between fibers and
starch, possibly caused by the van der Waals force or
hydrogen bonding. This interaction(s) had increased as the
concentration of fiber was increased. For biocomposites film
containing 3% D. hispida fiber, the resulting band positioned at
 j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 1 ; 1 5 : 1 3 4 2 e1 3 5 5
Table 2 e Summary of the analysis of variance (ANOVA) of mechanical properties.
Variables df Tensile strength
Mixture 4 0.00a
a
Values with different letters in the figures are significantly different (p < 0.05).
3260 cm1 was observed to shift to 3275 cm1. The shift was
farther when the concentration of D. hispida fiber was
increased that led to interactions of hydrogen bonding be-
tween hydroxyl groups of D. hispida starch and D. hispida fiber.
These findings broadly support other researches’ studies in
this field, linking corn fiber and corn starch [15].
3.8. Thermal analysis (TGA)
The thermal behavior in terms of stability and degradation of
D. hispida starch based-films with and without D. hispida fibers
are presented by the curves of TGA and DTG, as displayed in
Fig. 6. In the TGA curve, the plot of film samples’ weight loss
(mg) was against temperature (ºC), and in the DTG curve, the
derivative of weight loss (mg) was plotted as a function of
temperature (ºC). The occurrence of multi-step thermal
degradation events was found in both curves of the control D.
hispida starch film. Comparable findings were also revealed in
the previous work [46].
The initial degradation stage below 100
C was the result of
the elimination of the films’ molecules of water. Furthermore,
the weight loss at this stage could be linked with the dehy-
dration or vaporization of compounds of low molecular
weight and loosely bound water in biocomposite films. This
weight loss was observed in all other film samples, including
the control D. hispida starch film. Further heating resulted in a
sharp peak in the DTG of control film at 311.5
C, leading to
approximately 73.0% weight loss, which was likely due to
saccharide ring degradation in control D. hispida starch film. At
temperatures lower than 100
C, the control D. hispida starch
film displayed a higher weight loss than the D. hispida starch
biocomposite films. These results can be ascribed to the
higher moisture content of the control film D. hispida starch
than the D. hispida starch biocomposite films.
The plasticizer compounds evaporation (e.g. sorbitol) and
chemisorbed water molecules were correlated with the sec-
ond stage of thermal degradation, which occurred at a tem-
perature range of 125e290
C. The degradation temperature at
which sorbitol-plasticized D. hispida starch and D. hispida
starch biocomposite films agreed with the results obtained by
Podshivalov et al. [46] and Edhirej et al. [44] from their works
on potato and cassava starch. Furthermore, Ilyas et al. [18]
indicated that the thermal degradation of sugar palm starch-
based films using glycerol plasticizers was between 150 and
280
C. The highest thermal degradation rate was attained at
temperatures above 290
C, as shown by the significant weight
decrease by both the control film and D. hispida starch bio-
composite films.
According to Fig. 6, the thermal degradation onset of D.
hispida starch films was observed at around 300
C. This might
associate with hydrogen group removal, depolymerization,
and degradation of the carbon chains polymer of starch. The
1351
Young modulus Elongation at break
0.00a 0.00a
maximum thermal decomposition of D. hispida starch and D.
hispida starch biocomposites were 311.5
C and 329.2
C, which
showed that D. hispida starch biocomposite films (F2-9)
possessed higher thermal stability than control D. hispida
starch. The heat stability of starch biocomposite was
improved by the fiber reinforcement addition as similarly
demonstrated in past studies, reinforcing cellulose nanofibril
into chitosan/oregano essential oil and starch [12,51]. It was
found that no significant influence of different fiber sizes on
the thermal stability of fiber in D. hispida starch biocomposites
film. The degradation temperatures at the same concentration
of the D. hispida starch films composite with large-sized fiber
were a little higher than small-sized ones and resulted in
minimal variations, as shown in Table 1.
However, Fig. 6 showed that increasing the concentration
of D. hispida fiber has reduced the biocomposites' weight loss
at over 300
C, observing improved thermal stability of the
biocomposites. By definition, char is the residual material
succeeding pyrolysis of all volatile parts in the material. The D.
hispida starch biocomposites char residue was observed to
increase with D. hispida fiber reinforcement. The concentra-
tion of 3% (F1-3/F2-3) D. hispida fiber into the control D. hispida
starch displayed an increment of 19.69% or 19.20% from
16.38% (control). The improvement in the thermal stability of
D. hispida starch biocomposite films might result from the
composition of large carbonate in the D. hispida fiber that
corresponded to the thermal degradation outcome of the
biocomposites. This result was in agreement with past works,
which revealed that the combination of natural fiber within
the starch had enhanced the starch matrix polymer's thermal
stability [40,52].
3.9. Tensile properties
The Young modulus, tensile strength, as well as elongation at
break of D. hispida starch biocomposite films and their indi-
vidual concentration, are presented in Fig. 7. The incorpora-
tion of natural filler into the polymer matrix could possibly
influence the biocomposites film's mechanical properties [53].
There were three main aspects in the determination of the
mechanical properties of biocomposite materials, as stated by
Pickering et al. [54]: (1) morphology and dimensions, (2) pro-
cessing methods, and (3) the microstructure of the matrix/
filler and matrix interface. According to Fitch-Vargas et al. [55],
these natural fibers were reliable for the creation of net
adhesion among the matrix composite during the
manufacturing process' dehydrating procedure. Raising the
specific surface area of natural fiber using a rough surface and
reducing the fiber's diameter could enhance natural fiber/
matrix composite mechanical properties. Table 2 displays
analysis of variance (ANOVA) of the mechanical properties D.
hispida starch biocomposite films. Since the P-value is below
1352 j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 1 ; 1 5 : 1 3 4 2 e1 3 5 5
0.05 (p < 0.05), a statistically significant difference between the
mean of tensile strength, elongation and Young modulus from
one level of biocomposite films to another. The tensile anal-
ysis was conducted at room temperature, and the mechanical
properties of the well-structured D. hispida starch film and the
D. hispida starch biocomposites film were tested, varying the
size and concentration of biocomposite composition. For D.
hispida starch-based films, the tensile strength had signifi-
cantly increased (p < 0.05) with increasing fiber composition
from 3 to 6% and declined at 9% fiber. This decrement in the
film's tensile strength with 9% D. hispida fiber in the thermo-
plastic starch matrix might ascribe to the larger fiber content,
leading to less material homogeneity and might develop
structural defects [15]. The biocomposites displayed
improvement in the tensile strength for D. hispida starch bio-
composites film concentration up to 6%. The tensile strength
was raised to the highest of 9.29 MPa for small-sized fiber and
7.81 MPa for large-sized fiber at 6% fiber loading of D. hispida
starch biocomposites film. In comparing the tensile strength
of the D. hispida starch biocomposites films (Fig. 5), it was clear
that adding D. hispida fiber had enhanced the tensile strength
of the film.
As stated, the morphological observation result revealed
that D. hispida fiber was microscale in size and distributed
homogeneously for small-sized fiber within D. hispida starch.
As a result of the close interaction between D. hispida fibers
biofiller and D. hispida starch particle formation during the
film-making process, the mechanical properties of the
resulting biocomposite films were noticeably improved. The
increase in the tensile and modulus can be linked to the
physical interaction between D. hispida starch polymer
matrices and D. hispida fiber because their chemical similarity
facilitated enough interfacial adhesion. Furthermore, it was
also reported by the findings of reinforcement from the even
distribution high-performance biofiller within D. hispida
starch matrix arrangement and the strong hydrogen bonding
between D. hispida fiber and D. hispida starch molecules. The
reinforcement of D. hispida fiber and D. hispida starch
demonstrated comparable influence with the previously
conducted studies of corn husk [15], sugar palm [18], and
cassava peel [44] towards the starch-based biocomposites’
mechanical properties.
However, adding 3 and 6% D. hispida fibers had led to higher
tensile strength and modulus of the film except for concen-
tration of 9% biocomposites film. This might be attributed to
the favorable interaction between the fibers and starch poly-
mer matrices, which resulting adequate interfacial adhesion
because of their chemical similarities [56]. These results are
considerable with data obtained in moisture content film as
shown in Fig. 2(a). When the incorporation of D. hispida fibers
at 3%e9%, the moisture content of the film has reduced, which
might be associated with the lower moisture content of the D.
hispida fibers than D. hispida starch [30]. Similar results were
observed about the effect of fiber loading on the biocomposite
film thickness and mechanical strength when D. hispida
starch-based film was filled with D. hispida fibers. The bio-
composites film thickness has increased with the addition of
3%e9% D. hispida fiber, resulting in the reduction of elongation
at break, tensile strength and modulus at 9% of fiber. This
might be ascribed to the presence of higher concentration
fiber within the polymer matrix, leading to a less homogenous
material and likely to cause structural defects [26]. This
improvement results from the structural similarity and
compatibility of fiber and starch since it is from the same
biological origin. The strong hydrogen bonding interaction
between the fiber and starch molecules during the film-
making process and drying of the biocomposites restricted
the chain motion of the starch matrix [57]. Therefore, the
biocomposites film demonstrated improvements in Young
modulus and tensile strength simultaneously. These findings
were supported by other works done by Chen et al. [58], and
Ilyas et al. [18].
Nevertheless, raising the D. hispida fiber composition from
6 to 9% produced films having lower young modulus and
tensile stress for both fibers. It might be attributed to the
accumulation and imbalanced dispersion of the D. hispida fi-
bers within the D. hispida starch, whereby the D. hispida fibers
failed to function as a reinforcement in the D. hispida
starch matrix. In addition, it was also sourced from the excess
of D. hispida fibers concentration that probably caused phase
separation, poor particle distribution, as well as significant
agglomerates creation, resulting in poor mechanical charac-
teristics [59]. However, in D. hispida starch composite films
with large-sized fiber at similar concentration, the mechanical
performance was decreased than films with small fiber size. It
could be due to the matrix being incapable to wholly transfer
the load at large fiber size and high concentration. Neverthe-
less, the small-sized fiber exhibited better mechanical prop-
erties due to the easiness of smaller fiber to interact with the
compounding matrix compared to the larger ones. The finding
was parallel with the previous studies [26,54]. Moreover, in
contrast to the increments in young modulus and tensile
strength, the elongation at break for the D. hispida starch
biocomposites film was decreased from 25.44 to 19.57% and
11.97 to 7.98%, respectively as the concentrations of D. hispida
fiber were increased from F1-6 to F1-9 and F2-6 to F2-9 in the
starch-based composite films.
Meanwhile, 3% of small-sized D. hispida fibers had consid-
erably influenced the elongation at break of the biocomposite
films that was increased from 14.78 to 24.447%. This might be
attributed to the distribution of the D. hispida fiber on the
thermoplastic starch matrix, enhancing the ability of the
material to deform up to fracture. The increasing thermo-
plastic starch film's ductility with the fiber composition is
positively impacting the mechanical properties to suit indus-
trial applications [60]. The different sizes and concentrations
of D. hispida fibers, which were used with 6% small-sized fi-
bers, displayed maximum tensile strength increment and
elongation at break decrement as well as a high Young's
modulus. The addition of D. hispida fiber concentration had
resulted in reduced molecule mobility in the D. hispida starch
matrix that consequently made the composite film materials
stiffer. Therefore, the large-sized fiber of D. hispida starch
biocomposite films was more break-resistant besides less
stretchable than the small-sized fiber films. In brief, the
reduced elongation at break was due to the rigid filler struc-
ture, as demonstrated in a past published work in the litera-
ture [55]. The tensile strength of biofiller was optimum with
small-sized fiber at a concentration of 6% D. hispida fiber
loading followed by tensile strength reduction at 9% fiber due
 j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 1 ; 1 5 : 1 3 4 2 e1 3 5 5
to D. hispida fibers agglomeration, progressively decreasing
the filler dispersion effectiveness.
4. Conclusions
D. hispida fiber was used to reinforce the D. hispida starch
matrix from 3 to 9 wt % concentration with two sizes of fiber
for the preparation of biocomposites via casting method. The
SEM images demonstrated that the cross-sections of the D.
hispida starch biocomposites were rougher than the D. hispida
starch film as a result of the incorporation of D. hispida fiber.
Improvements in the properties of thermal, mechanical, as
well as water barrier were exhibited by the D. hispida starch-
based films. The D. hispida starch-based films had recorded
significant improvement in tensile strength with greater fiber
content from 3 to 6% and decreased at 9% of concentration.
The different sizes and concentrations of D. hispida fiber,
which was used with 6% small-sized fiber displayed the
highest increment in the tensile strength and decrement in
elongation at break and demonstrated a high Young's
modulus value. The maximum thermal decomposition of D.
hispida starch and D. hispida starch biocomposites were
311.5
C and 329.2
C, which showed that D. hispida starch
biocomposite films (F2-9) had better thermal stability
compared to the control D. hispida starch. The starch-based
biocomposites film also exhibited a greater water resistance.
The performance enhancement of these films might result
from the excellent intermolecular interaction compatibility
between the two components, consequently of the good fiber
dispersion, chemical similarities, and adhesion of D. hispida
fiber within the D. hispida starch matrix. The biocomposites
film revealed a novel waste material D. hispida fiber that is eco-
friendly and easy to be processed. It also generates new in-
formation on the interactions of different fiber sizes and their
effect on the film capabilities, which can aid in development
of biodegradable materials.
Declaration of Competing Interest
The authors declare that they have no known competing
financial interests or personal relationships that could have
appeared to influence the work reported in this paper.
Acknowledgments
The authors would like to thank the Universiti Putra Malaysia
for the financial support provided through the Universiti Putra
Malaysia Grant Inisiatif Putra Siswazah (GP-IPS/2021/9697100),
as well as the German Malaysian Institute (GMI), Malaysia for
providing the award to the principal author in this project.
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