You are on page 1of 18

Journal of Natural Fibers

ISSN: (Print) (Online) Journal homepage: https://www.tandfonline.com/loi/wjnf20

Development and Characterization of Sustainable


Bioplastic Films Using Cellulose Extracted from
Prosopis juliflora

Marichelvam M K, Manimaran P, Anish Khan, Geetha M, Kandakodeeswaran


K, Ahmed H. Abduljabbar, Edi Syafri, Mohammad A. Wazzan, Huda Wazzan &
Waseem Khan

To cite this article: Marichelvam M K, Manimaran P, Anish Khan, Geetha M, Kandakodeeswaran


K, Ahmed H. Abduljabbar, Edi Syafri, Mohammad A. Wazzan, Huda Wazzan & Waseem
Khan (2023) Development and Characterization of Sustainable Bioplastic Films Using
Cellulose Extracted from Prosopis juliflora, Journal of Natural Fibers, 20:2, 2231271, DOI:
10.1080/15440478.2023.2231271

To link to this article: https://doi.org/10.1080/15440478.2023.2231271

© 2023 The Author(s). Published with


license by Taylor & Francis Group, LLC.

Published online: 07 Jul 2023.

Submit your article to this journal

View related articles

View Crossmark data

Full Terms & Conditions of access and use can be found at


https://www.tandfonline.com/action/journalInformation?journalCode=wjnf20
JOURNAL OF NATURAL FIBERS
2023, VOL. 20, NO. 2, 2231271
https://doi.org/10.1080/15440478.2023.2231271

Development and Characterization of Sustainable Bioplastic Films


Using Cellulose Extracted from Prosopis juliflora
Marichelvam M Ka, Manimaran Pb, Anish Khanc, Geetha Md, Kandakodeeswaran Ka,
Ahmed H. Abduljabbare, Edi Syafri f, Mohammad A. Wazzane, Huda Wazzang,
and Waseem Khane
a
Department of Mechanical Engineering, Mepco Schlenk Engineering College, Sivakasi, India; bDepartment of
Mechanical Engineering, Karpagam Institute of Technology, Coimbatore, India; cCenter of Excellence for Advanced
Materials Research, King Abdulaziz University, Jeddah, Saudi Arabia; dDepartment of Mathematics, Kamaraj College of
Engineering and Technology, Virudhunagar, India; eDepartment of Radiology, Faculty of Medicine, King Abdulaziz
University, Jeddah, Saudi Arabia; fDepartment of Agricultural Technology, Politeknik Pertanian Negeri Payakumbuh,
West Sumatra, Indonesia; gSchool of Human Science and Design Food and Nutrition, King Abdulaziz University,
Jeddah, Saudi Arabia

ABSTRACT KEYWORDS
To diminish the environmental impacts instigated by plastics, investigators Plastics; bioplastics; starch;
recommended bioplastics. In the current work, an attempt is made to cellulose; biodegradability;
develop sustainable bioplastics from waste plants. Cellulose was extracted Prosopis juliflora
from the wood of Prosopis juliflora. The Prosopis juliflora wood was cut and 关键词
ground into powder. The powder was washed with water and subjected to 塑料; 生物塑料; 淀粉; 纤维
several chemical treatments to extract the cellulose. The bioplastic film 素; 生物降解性
samples were produced using it. Six different samples were prepared by
varying the composition of cellulose, gelatin, citric acid, and glycerol. Several
tests were carried out on samples developed as per ASTM standards, and the
results were compared with the existing bioplastics. The test results indicated
that sample 1 has a maximum tensile strength of 7.73 MPa. The average
bursting strength of the bioplastic film is 12.44 kg/cm2, which is better than
the other bioplastics reported in the literature. The average biodegradability
of developed bioplastic films is approximately 59.43%. The results revealed
that the Prosopis juliflora cellulose-based bioplastics would be a better sub­
stitute for conventional plastics.
摘要
为了减少塑料对环境的影响,研究人员推荐使用生物塑料. 在目前的工作
中,试图从废物工厂中开发可持续的生物塑料. 从胡罗卜的木材中提取纤
维素. 普罗索匹斯的juliflora木材被切割并研磨成粉末. 用水洗涤该粉末并
进行若干化学处理以提取纤维素. 使用它生产生物塑料薄膜样品. 通过改变
纤维素、明胶、柠檬酸和甘油的组成制备了六种不同的样品. 对根据ASTM
标准开发的样品进行了几项测试,并将结果与现有的生物塑料进行了比
较. 试验结果表明,样品1的最大抗拉强度为7.73MPa. 生物塑料薄膜的平均
爆裂强度为12.44 kg/cm2,比文献中报道的其他生物塑料要好. 已开发的
生物塑料薄膜的平均生物降性约为59.43%. 研究结果表明,基于Prosopis
juliflora纤维素的生物塑料将是传统塑料的更好替代品

CONTACT Edi Syafri edisyafri11@gmail.com Department of Agricultural Technology, Politeknik Pertanian Negeri
Payakumbuh, West Sumatra, Indonesia
© 2023 The Author(s). Published with license by Taylor & Francis Group, LLC.
This is an Open Access article distributed under the terms of the Creative Commons Attribution-NonCommercial License (http://creativecommons.org/
licenses/by-nc/4.0/), which permits unrestricted non-commercial use, distribution, and reproduction in any medium, provided the original work is
properly cited. The terms on which this article has been published allow the posting of the Accepted Manuscript in a repository by the author(s) or with
their consent.
2 M. M K ET AL.

1. Introduction
The usage of plastics is inevitable in the modern era. A wide variety of plastics are used for
diverse applications. During the year 2020, nearly 367 million metric tons of plastics were
produced worldwide. Though this is 0.3% less than the previous year’s production, plastics
cause severe environmental impacts. To solve this issue, researchers have developed various
bioplastics. Due to its simplicity and better tensile and other properties, most of the research­
ers developed bioplastics from starch (Abidin et al. 2015; Marichelvam, Jawaid, and Asim
2019). Researchers developed bioplastics by using cassava starch (Edhirej et al. 2017a, 2017b;
Luchese et al. 2018), sugar palm starch (Ceseracciu et al. 2015), corn starch (Ghanbarzadeh,
Almasi, and Entezami 2011; Kim, Jane, and Lamsal 2017; Yang et al. 2022), potato starch
(Podshivalov et al. 2017; Zakaria et al. 2018; Zhang, Wang, and Cheng 2018), rice starch
(Woggum, Sirivongpaisal, and Wittaya 2014), Prosopis juliflora starch (Marichelvam et al.
2022) and wheat starch (Song, Zuo, and Chen 2018). Rodrigues et al. (2020) developed
bioplastics films using the starch derived from babassu mesocarp. The other starches used
for bioplastics and the additives added with the starch materials to enhance the properties can
be found in (Jabeen et al. 2015; Siracusa et al. 2008). The starches described above are food
grains, and reports indicated that 957 million people from 93 countries do not have sufficient
food because of poverty. Hence, it is the responsibility of researchers to develop new
bioplastics from other bioresources.
Prosopis juliflora is one of the plants that was introduced to stabilize the ecosystem in several parts of the
world. Unfortunately, this plant has created some environmental problems (Edrisi, El-Keblawy, and
Abhilash 2020). The Prosopis juliflora consists of 40–45 wt. % of cellulose, 25–30 wt. % of hemicellulose,
11–28 wt. % of lignin, and the remaining 3–15 wt.% of extractives (Prabha, Dahms, and Malliga 2014).
Researchers attempted to extract the cellulose from Prosopis juliflora because it contains more amount of
cellulose. Peelman et al. (2015) substantiated that cellulose could be used for packaging applications.
Mostafa et al. (2018) developed cellulose acetate bioplastics from agricultural waste and concluded that
cellulose acetate bioplastics could be used in food industries and medical applications. Cifriadi et al. (2017)
manufactured cellulose-based bioplastics from the oil palm empty fruit bunch and mixed plasticizer and
compatibilizer with the cellulose. They mixed cassava starch and glycerol with the cellulose solution to
produce the bioplastics and investigated their properties. Asgher, Bilal, and Iqbal (2020) addressed the
importance of biomaterials in food packaging applications. They pointed out that researchers should
concentrate their work to increase the properties of the biomaterial. Batista Meneses et al. (2022) reported
the various agro-industrial waste materials available worldwide. They discussed the biochemical composi­
tion of many agro-industrial wastes like rice straw, rice husk, wheat stalk, corn bagasse, etc. Chopra (2022)
has explained the cellulose extraction techniques in detail.
Harini, Ramya, and Sukumar (2018) utilized banana peel and bract to extract the micro and nano
cellulose fibers and concluded that the cellulose-based fibers would substitute the synthetic polymers
and reduce the environmental impacts. Rohmawati et al. (2018) produced bioplastics from cellulose
that were extracted from teak wood. They synthesized cellulose acetate from the extracted cellulose.
They mixed this cellulose acetate with various chemicals and plasticizers to produce the bioplastics.
Tang et al. (2018) developed nanocomposite films using nanocrystalline cellulose, chitosan, and guar
gum and investigated the rheological and mechanical properties by varying the nanocrystalline
cellulose percentage and determining the optimal value. Tedeschi et al. (2018) examined the barrier
and ductile properties of thermoplastic cellulose acetate oleate films. Madhu et al. (2019) investigated
the mechanical, morphological, Physico-chemical, and thermal properties of alkali-treated Prosopis
juliflora fibers and concluded that the fibers can be used as an effective reinforcement material in
composite manufacturing. Ravindran, Sreekala, and Thomas (2019) extracted cellulose nanofibers
from the pineapple leaves and reported that the cellulose fiber could be used for different applications.
A biodegradable bioplastics film was developed by Azmin and Nor (2020) using the cellulose extracted
from cocoa pod husk and the sugarcane bagasse fiber. The ratio of the cellulose and fiber was varied
JOURNAL OF NATURAL FIBERS 3

and several samples were prepared. They reported that the bioplastics film with 75% cellulose and 25%
fiber provided better physicochemical properties.
Debiagi, Faria-Tischer, and Mali (2020) recommended a simple and low-cost method to develop
nano-fibrillated cellulose from the soybean hull. Yaradoddi et al. (2020) developed carboxymethyl
cellulose that was resulting from agricultural waste materials like sugar cane bagasse. They mixed the
carboxymethyl cellulose with agar, gelatin, and varied concentrations of glycerol to manufacture film
for packaging applications. Debiagi, Faria-Tischer, and Mali (2021) used a reactive extrusion process
in an oat hull to produce nano-fibrillated cellulose. Hu et al. (2021) discussed various mechanical
methods to produce cellulose nanofibrils to increase the mechanical properties of recycled paper. Liu
et al. (2021) addressed a detailed literature review on biopolymers resulting from cellulose for food
packing applications. Menezes et al. (2021) prepared membranes using cellulose nanofibers attained
from orange peel. The cellulose nanofibers were treated with the aid of 1-methylimidazolium. To
improve the mechanical strength, the cellulose nanofibers were incorporated with the starch.
Suryanto, Pahlevi, and Yanuhar (2021) focussed on the impact of bacterial cellulose addition to the
biocomposites derived from cassava starch. They considered the mechanical properties and the
morphological properties. Wang et al. (2021) applied a multilayer surface construction technique to
improve cellulose-based packaging materials’ barrier properties.
From the above literature review, it is concluded that not much work has been done on the
extraction of cellulose from Prosopis juliflora. Hence, it is proposed to extract the cellulose from
Prosopis juliflora and the pull-out cellulose was mixed with the plasticizers to prepare the biofilms. The
performance of the biofilms was analyzed by conducting several tests like biodegradability test, tensile
test, water absorption test, water contact angle test, and water solubility test.

2. Materials and methods


The Prosopis juliflora plant was obtainable at Sethur village, Virudhunagar district of Tamilnadu,
India, and the plant and the stem of the plant are shown in Figure 1a–b respectively. The analytical
grades of chemicals used for the extraction of cellulose were supplied by Ranabai Chemicals and
Housekeeping, Bangalore, India. The cellulose pull-out from Prosopis juliflora is depicted in Figure 1c.
Citric acid, the gelatine powder, the glycerol, and purified water required for the manufacture of
bioplastics film were procured from Punitha Enterprises, Madurai, Tamilnadu, India.

2.1. Extraction process


In this work, an attempt was made to extract cellulose from Prosopis juliflora in the test center on an
experimental scale using the methods described by Valencia et al. (2019). Prosopis juliflora wood was
cut and then ground into powder. The powder was washed with water. Then, it was treated with
NaOH solution. A mixture of NaOH, CH3COOH, and NaCl solution was used to bleach the powder.
The bleaching process was repeated several times. The powder was again washed and treated with C2
H2O4. Then, a mechanical and acid hydrolysis process was carried out and the cellulose was extracted.

2.2. Preparation of bioplastics film samples


The bioplastics films are produced by different methods such as compression molding, casting, and
extrusion are some of the important methods used to prepare the bioplastics film samples. In this work, the
bioplastics film samples were prepared by the method described by Muscat et al. (2012). Prosopis juliflora
cellulose, citric acid, purified water, gelatine, and glycerol are used to manufacture the bioplastics film. 100
mL of purified water was taken. The required quantities of cellulose gelatin, glycerol, and citric acid are
added to the purified water. The mixture was rigorously stirred continuously for 10 min at about 180 rpm.
The mixture was kept on a hot plate and heated at 100°C. The mixture was stirred manually for 70 min.
The mixture was poured onto a Teflon-coated glass plate and spread uniformly. The mixture was dried out
4 M. M K ET AL.

Figure 1. (a) Prosopis juliflora Plant (b) Stem of Prosopis juliflora (c) Cellulose pull-out.

Table 1. Composition of different bioplastics film.


Cellulose Gelatin Glycerol Citric acid Purified water
Sample (g) (g) (g) (g) (ml)
S1 10 2 3 1 100
S2 10 2 3 2 100
S3 10 3 3 2 100
S4 10 3 4 2 100
S5 10 3 4 3 100
S6 10 3 5 3 100

for 3 to 4 days and then the cast film was removed (Muscat et al. 2012). The other samples were prepared
by varying the composition of the materials. The composition of different bioplastics is shown in Table 1.

3. Characterization
3.1. Biodegradability test of bioplastics films
The biodegradable nature of the bioplastics film was determined using the soil kept in a container. The
square-sized samples of bioplastics film were suppressed into a biodegradability test. The square pieces
of dimension 2 cm x 2 cm are prepared from the bioplastics film and their initial weight is recorded.
The soil of weight of about 500 g close to the plant roots which contains a good amount of bacteria and
JOURNAL OF NATURAL FIBERS 5

moisture content was considered for the test. The depth of 3 cm for 15 days under the atmospheric
environment. The samples were taken out of the container after 15 days and their final weight is noted
(Marichelvam et al. 2022).
The biodegradability was determined by using Equation (1).
Wi Wf
Biodegradabilityð%Þ ¼ � 100 (1)
Wi
Where
Wi – initial weight of the bioplastics (g)
Wf – final weight of the bioplastics (g)

3.2. Bursting test of bioplastics films


The resistance of a bioplastics film to a sudden rupture especially due to internal pressure is known as
bursting strength. The bursting strength of the films is measured as per the ASTM D774 standards
using a Bursting strength tester (Vertex BST – S2, India).

3.3. Fourier transform infrared spectroscopy analysis of bioplastics films


Fourier Transform Infrared (FT-IR) Spectroscopy is an analytical method used to identify the
chemical functional groups present in the bioplastics films by producing an infrared absorption
spectrum. The wave number of the spectrum was collected between the ranges 400 cm−1 and 4000
cm−1 using a Shimadzu spectrometer (FTIR-8400S, Japan). The number of scans used was 64 and the
resolution was 4 cm−1.

3.4. Moisture content test of bioplastics films


The square pieces of dimension 2 cm x 2 cm are prepared from the bioplastics film and the weight of
each film was noted. The film was kept in the oven maintaining the temperature of 110°C till the fixed
dry weight of the film was obtained and the mass of the dry film was recorded (Salarbashi et al. 2013).
Five numbers of each film sample were considered for determining the moisture content of the films.
The moisture content is measured using Equation (2).
W1 W2
Moisturecontent ð%Þ ¼ � 100 (2)
W1
Where
W1 – initial weight of the bioplastics (g)
W2 – final weight of the bioplastics (g)

3.5. Scanning electron microscopy analysis of bioplastics films


Scanning electron microscopy (SEM) machine model HITACHIS-3400 N was used to analyze the
morphology of the biodegraded bioplastics films. This analysis was performed with the current intensity
of 58 μA for operating the instrument. The voltage potential was maintained at 10 kV with a preset
working distance of 7.4 mm. For conducting SEM analysis, the bioplastics film samples were gold coated.

3.6. Tensile test of bioplastics films


The tensile strength of the bioplastics films was measured by conducting the tensile test as per ASTM
D882 standard using Testometric Machine M350 10CT. The distance between the grips was
6 M. M K ET AL.

maintained at 50 mm with a cross-head speed of 50 mm/min. The film samples were prepared with
dimensions of a length of 110 mm, a width of 30 mm, and a thickness of 0.36 mm. The film samples
were prepared in the Dumbbell shape for tensile testing. This test was performed with ten replications
for each film. The tensile strength of the film was measured in the period of stretching and the mean
value was recorded.

3.7. Thickness measurement of bioplastics films


The thickness of the bioplastics film plays a significant role when using the film for packaging
applications. The thickness of bioplastics films was measured as per ASTM D6988 standards.
A digital Vernier Caliper (Mitutoyo, Japan) was adopted to determine the thickness of the bioplastics
film. The readings were taken at five different places and the average value is considered.

3.8. Measurement of water contact angle of bioplastics films


The hydrophobicity nature of the bioplastic films was measured by examining their wettability through
the water contact angle by using a goniometer. The sample was positioned during light and the camera
was at a similar angle. This allowed the flat baseline to be attained for the measurement of the contact
angle measurement. The contact angle varies between 0 and 180°, according to the wettability of solid
material. The nature of the material is extreme hydrophilic if the contact angle value is 0º and extreme
hydrophobic if the value is 180º. The bioplastic sample films are cut into small pieces so that a small drop
of about 0.005 mL water could be poured over the piece (Marichelvam et al. 2022). If the water contact
angle is around 60º then the better solubility of bioplastics film was obtained.

3.9. Thermal studies of bioplastics films


To study the thermal degradation behavior, the samples were assessed by thermogravimetric analyses
(TGA) using Jupiter simultaneous analyzer (model: STA449 F3TGA). The mass transformation was
analyzed as a function of temperature in an interval of 25–1000°C at a heating rate of 5°C/min. The
sample was exposed to nitrogen gas at a flow rate of 20 mL/min.

4. Results and discussions


4.1. Biodegradability of bioplastics films
The biodegradability values of different samples are represented in Figure 2. The biodegradability of
the first sample was 52.6%. The biodegradability of bioplastic films increases when the amount of citric
acid, gelatin, and glycerol increases. This may be due to the presence of the O-H and C-O functional
groups present in the films. The average biodegradability of bioplastic films was approximately
59.43%. As the biodegradability of the bioplastics films is greater than 50%, the cellulose-based
bioplastics films could be used for packaging applications and also minimized the environmental
impacts. The results indicated that the biodegradability of the cellulose-based bioplastics films is
superior to starch-based bioplastics films (48.73%) addressed in the literature (Marichelvam, Jawaid,
and Asim 2019).

4.2. Bursting strength of bioplastics films


The bursting strength of the bioplastics films produced is provided in Table 2. The average bursting
strength of the six bioplastics film is 12.44 kg/cm2 which is greater than the plastic films made by the
linear low-density polyethylene (LLDPE), low-density polyethylene (LDPE), medium-density poly­
ethylene (MDPE) and high-density polyethylene (HDPE) (Kumar et al. 2007). The bioplastics sample
JOURNAL OF NATURAL FIBERS 7

80
70

Biodegradeability (in %)
60
50
40
30
20
10
0
S1 S2 S3 S4 S5 S6
Samples

Figure 2. Biodegradability comparison of different bioplastics film samples.

Table 2. Bursting strength of different bioplastics


film.
Sample Bursting strength (kg/cm2)
S1 16.08 ± 0.22
S2 14.67 ± 0.16
S3 12.96 ± 0.32
S4 11.42 ± 0.26
S5 10.27 ± 0.18
S6 9.22 ± 0.24

6 has a minimum bursting strength of 9.22 ± 0.24 kg/cm2. However, it is very much greater than the
bursting strength of LLDPE (0.5 kg/cm2), LDPE (1.2 kg/cm2), MDPE (2.0 kg/cm2), and HDPE (4.5 kg/
cm2). Hence, the proposed cellulose-based bioplastics films can be used for packaging applications.

4.3. Fourier transform infrared spectroscopy analysis of bioplastics films


FTIR results of cellulose-based bioplastics film samples are presented in Figure 3. The FTIR result of
sample S1 is shown in Figure 3 (a). The results of sample S1 indicated that wave number 3733.93 cm−1
represents the stretching of hydroxyl groups because of water as well as carbohydrates, 3610.49 cm−1
indicates O-H stretching due to primary alcohol and secondary alcohol, 3307.69 cm−1 shows the
strong C-O stretching due to primary alcohol present in the cellulose. The wave numbers 3722.36
cm−1, 3722.36 cm−1, 3734.90 cm−1, 3722.36 cm−1, and 3724.29 cm−1 represent the stretching of hydro­
xyl groups, 3634.60 cm−1, 3634.60 cm−1, 3613.39 cm−1, 3634.60 cm−1, and 3632.67 cm−1 indicates to
O-H stretching due to primary alcohol and secondary alcohol, 3196.79 cm−1, 3118.60 cm−1, 3122.54
cm−1, 3179.43 cm−1, and 3119.65 cm−1 shows the strong C-O stretching due to primary alcohol present
in the cellulose for samples 2–6 respectively.

4.4. Moisture content of bioplastics films


The moisture content values of the cellulose-based bioplastics films are shown in Figure 4. Sample S1
has a moisture content of 10.5%. The moisture content of the bioplastics films increases with the raise
in the percentage of the amount of citric acid, gelatin, and glycerol. The average moisture content of
cellulose-based bioplastics films is 12.95% which is almost equal to the moisture content of starch-
based bioplastics films (12.88%) (Marichelvam, Jawaid, and Asim 2019). The bioplastic films with less
moisture content are desirable as the bioplastics are to be used for packaging applications. More
8 M. M K ET AL.

(a) Sample S1 (b) Sample S2

(c) Sample S3 (d) Sample S4

(e) Sample S5 (f) Sample S6


Figure 3. FTIR results of cellulose- based bioplastics films samples.
JOURNAL OF NATURAL FIBERS 9

18
16
14

Moisture Content (%)


12
10
8
6
4
2
0
Samples

S1 S2 S3 S4 S5 S6

Figure 4. Moisture content of different bioplastics film samples.

moisture content in the bioplastics would affect the quality of packed materials. Hence, the bioplastics
developed in the present work could be used for packaging applications.

4.5. Scanning electron microscopy images of bioplastics films


The SEM images of the biodegraded cellulose-based bioplastics films are illustrated in Figure 5. The
SEM images of bioplastic samples indicated that the surface structure has changed the degradation in
the bioplastic samples due to microbial action. The uneven film surface and the flaws present on the
surface also prove that the developed bioplastics are biodegradable. The SEM image of sample S1
which has a smaller amount of citric acid, gelatin, and glycerol is depicted in Figure 5 (a). The surface
integrity (i.e., the surface condition of the samples after the biodegradability test) was poor for sample
S1. Sample S1 also has a greater number of defects, rough grains, and irregularities. Many cellulose
granules were witnessed as a result of the presence of a reduced amount of concentration of
plasticizers. For sample S6 which has more amount of plasticizers, the surface integrity was better.
The number of flaws is relatively less in sample S6. The other samples represent a medium amount of
plasticizers and therefore a modest level of surface integrity and flaws were observed.

4.6. Tensile strength of bioplastics films


The comparison of tensile strength of different cellulose-based bioplastics films is described in Figure 6. The
result indicated that sample S1 has a maximum tensile strength of 7.73 MPa. When the percentage of citric
acid, gelatin and glycerol added with cellulose increases the tensile strength decreases. Sample 2 has a tensile
strength of 6.67 MPa. Sample 6 has the least tensile strength of 4.54 MPa and results indicated the average
tensile strength as 5.84 MPa. However, this tensile strength is greater than the bioplastics films made of
Amylomaize starch 5.47 MPa (Qin et al. 2019), Banana starch 5.00 MPa (Sapei et al. 2015), Cassava starch
5.20 MPa (Wahyuningtiyas and Suryanto 2018), Corn Starch 4.81 MPa (Jiugao, Ning, and Xiaofei 2005),
Potato starch 2.66 MPa (Oleyaei et al. 2016), Taro starch 2.15 MPa (Shanmathy, Mohanta, and
Thirugnanam 2021), and yam starch 4.075 MPa (Behera, Mohanta, and Thirugnanam 2022). The results
revealed that the tensile strength of the developed cellulose-based bioplastic samples is much better than
many other bioplastics addressed in the literature. The tensile properties of the bioplastics films revealed
that cellulose-based bioplastics can be used for packaging applications. The elongation at break values of the
samples is depicted in Figure 7. Sample 1 has 120.8% of elongation at break. The percentage elongation at
10 M. M K ET AL.

(a) Sample S1 (b) Sample S2

(c) Sample S3 (d) Sample S4

(e) Sample S5 (f) Sample S6


Figure 5. (a-f). SEM images of bioplastics film after the biodegradability test.

break values changes with the change in the percentage of citric acid, gelatin, and glycerol added with
cellulose. The stress-strain curves of the films are depicted in Figure 8. Since there are no appreciable
changes in the slope of the curves, it can be inferred from the figure that the samples exhibited plastic
behavior.
JOURNAL OF NATURAL FIBERS 11

9
8
7

Tensile Strength (MPa)


6
5
4
3
2
1
0
Samples

S1 S2 S3 S4 S5 S6

Figure 6. Tensile strength of different bioplastics film samples.

160
140
Elongation at break (%)

120
100
80
60
40
20
0
1
Samples

S1 S2 S3 S4 S5 S6

Figure 7. The elongation at break values of the samples.

4.7. Film thickness of bioplastics films


The film thickness values of the different bioplastics film samples are depicted in Figure 9.
From the results, it is concluded that the mean thickness of all the prepared samples is greater
than 50 microns. This indicates that the prepared samples satisfy the requirements of the
Plastic Waste Management Amendment Rules, 2021 in India. The bioplastics with more than
50 microns are stronger, and more durable and they could be recycled. Hence, film thickness
values of the different bioplastics film samples indicated that cellulose-based bioplastics can be
used for packaging applications.

4.8. Water contact angle of bioplastics films


The water contact angle of various bioplastics samples is depicted in Figure 10. The sample’s water
contact angles are greater than 60º for the first five samples. Sample S6 has a water contact angle of
about 70º. This proves that the cellulose-based bioplastics films are hydrophilic when compared with
12 M. M K ET AL.

Figure 8. Stress-strain curves of bioplastics film samples.

normal LDPE plastic (almost hydrophobic). The hydrophilic films are used as suitable materials for
some medical applications. Hence, the developed samples could be used for the manufacturing of
glucose test strip covers. The water contact angle of the cellulose-based bioplastics films is better than
the water contact angles of bioplastics film prepared from Corn starch (47.25º) (Amin, Chowdhury,
and Kowser 2019) and Potato starch (Abdullah et al. 2018).

4.9. Thermogravimetric analysis of bioplastics films


The Thermogravimetric analysis (TGA) result of sample 1 is shown in Figure 11. One can easily observe
the three different regimes of degradation from the TGA thermograms. It is observed that a small weight
loss of nearly 5 to 8% was found in the first regime of degradation in the range of 70–130°C. A significant
weight loss occurred in the range of 230°C −320°C. This weight loss would be the degradation of the
additives. From the TGA curve, it may be concluded that the bioplastics could be used for high-
temperature packaging applications.

140

120

100
Thickness (in µm)

80

60

40

20

0
S1 S2 S3 S4 S5 S6
Samples
Figure 9. Film thickness for different bioplastics film samples.
JOURNAL OF NATURAL FIBERS 13

(a) Sample S1 (b) Sample S2

(c) Sample S3 (d) Sample S4

(e) Sample S5 (f) Sample S6

(g) LDPE
Figure 10. Water contact angle of the different bioplastics film samples and LDPE.
14 M. M K ET AL.

Figure 11. TGA curve for sample 1.

5. Conclusion
Prosopis juliflora creates severe environmental impacts. In this work, cellulose is extracted from Prosopis
juliflora, and six bioplastics films were made by adding citric acid, gelatin, and glycerol. Different tests
were performed to validate the performance of the cellulose-based bioplastics films. The average tensile
strength of the cellulose-based bioplastics films was 5.84 MPa which is greater than other bioplastics
films. The bursting strength, water contact angle, and biodegradability properties were superior to other
bioplastics available in the literature. The film thickness was more than 50 microns, and the water
contact angle of the bioplastics was greater than 60º. The thermogravimetric analysis results proved the
thermal stability of the samples. The results revealed that the developed cellulose-based bioplastics film
could be used for packaging applications. The usage of cellulose-based bioplastics not only reduces the
impact of Prosopis juliflora but also reduces the effect of petroleum-based plastics. However, appropriate
manufacturing techniques would be developed for the commercialization of cellulose-based bioplastics.

Acknowledgements
This research work was funded by Institutional Fund Projects under grant no. (IFPIP:1009-140-1443). The authors
gratefully acknowledge the technical and financial support provided by the Ministry of Education and King Abdulaziz
University, DSR, Jeddah, Saudi Arabia.

Disclosure statement
No potential conflict of interest was reported by the author(s).

ORCID
Edi Syafri http://orcid.org/0000-0002-5784-6694

Availability of data and materials


Yes
JOURNAL OF NATURAL FIBERS 15

Author Contribution
Marichelvam, M.K, and Manimaran P designed the experiment and did experimental analysis while Anish Khan, Edi
Syafri, Geetha, M, repeat the results and verify after that Kandakodeeswaran, K and Abdullah M. Asiri write the final
draft of the manuscript.

Consent for publication


Yes

Highlights of this Investigation


● This research focuses on developing environmentally friendly bioplastics derived from cellulose extracted from the
Prosopis juliflora plant.
● Cellulose-based bioplastics from Prosopis juliflora would be a better substitute for conventional plastics as the average
biodegradability of the developed bioplastic films is about 59.43%.
● The average tensile strength of the cellulose- based bioplastics films was 5.84 MPa which is greater than other
bioplastics films.

References
Abdullah, A. H. D., P. Sri, K. Myrtha, D. P. Oceu, and H. F. Rani. 2018. Fabrication and characterization of sweet potato
starch-based bioplastics plasticized with glycerol. Journal of Biological Sciences 19 (1):57–64. doi:10.3923/jbs.2019.57.64.
Abidin, M. Z. A. Z., N. M. Julkapli, H. Juahir, F. Azaman, N. H. Sulaiman, and I. Z. Abidin. 2015. Fabrication and
properties of chitosan with starch for packaging application. Malaysian Journal of Analytical Sciences 19:1032–42.
Amin, M. R. M. A. C., M. A. Chowdhury, and M. A. Kowser. 2019. Characterization and performance analysis of
composite bioplastics synthesized using titanium dioxide nanoparticles with corn starch. Heliyon 5 (8):e02009. doi:10.
1016/j.heliyon.2019.e02009.
Asgher, M. S. A. Q., M. Bilal, and H. M. N. Iqbal. 2020. Bio-based active food packaging materials: Sustainable alternative
to conventional petrochemical-based packaging materials. Food Research International 137:109625. doi:10.1016/j.
foodres.2020.109625.
Azmin, S. N. H. M., and M. S. M. Nor. 2020. Development and characterization of food packaging bioplastic film from
cocoa pod husk cellulose incorporated with sugarcane bagasse fibre. Journal of Bioresources and Bioproducts
5 (4):248–55. doi:10.1016/j.jobab.2020.10.003.
Batista Meneses, D., G. Montes de Oca-Vásquez, J. R. Vega-Baudrit, M. Rojas-Álvarez, J. Corrales-Castillo, and
L. C. Murillo-Araya. 2022. Pretreatment methods of lignocellulosic wastes into value-added products: Recent
advances and possibilities. Biomass Conversion and Biorefinery 12:547–64. doi:10.1007/s13399-020-00722-0.
Behera, L., M. Mohanta, and A. Thirugnanam. 2022. Intensification of yam-starch based biodegradable bioplastic film
with bentonite for food packaging application. Environmental Technology & Innovation 25:102180. doi:10.1016/j.eti.
2021.102180.
Ceseracciu, L., J. A. Heredia-Guerrero, S. Dante, A. Athanassiou, and I. S. Bayer. 2015. Robust and biodegradable
elastomers based on corn starch and polydimethylsiloxane (PDMS). ACS Applied Materials & Interfaces
7 (6):3742–53. doi:10.1021/am508515z.
Chopra, L. 2022. Extraction of cellulosic fibers from the natural resources: A short review. Materials Today: Proceedings
48:1265–70. doi:10.1016/j.matpr.2021.08.267.
Cifriadi, A., T. Panji, N. A. Wibowo, and K. Syamsu. 2017. Bioplastic production from cellulose of oil palm empty fruit
bunch. IOP Conference Series: Earth and Environmental Sciences 65 (1):012011. doi:10.1088/1755-1315/65/1/012011.
Debiagi, F., P. C. S. Faria-Tischer, and S. Mali. 2020. Nanofibrillated cellulose obtained from soybean hull using simple
and eco-friendly processes based on reactive extrusion. Cellulose 27 (4):1975–88. doi:10.1007/s10570-019-02893-0.
Debiagi, F., P. C. S. Faria-Tischer, and S. Mali. 2021. A green approach based on reactive extrusion to produce
nanofibrillated cellulose from Oat Hull. Waste and Biomass Valorization 12 (2):1051–60. doi:10.1007/s12649-020-
01025-1.
Edhirej, A., S. M. Sapuan, M. Jawaid, and N. I. Zahari. 2017a. Cassava/Sugar palm fiber reinforced cassava starch hybrid
composites: Physical, thermal and structural properties. International Journal of Biological Macromolecules
101:75–83. doi:10.1016/j.ijbiomac.2017.03.045.
Edhirej, A., S. M. Sapuan, M. Jawaid, and N. I. Zahari. 2017b. Preparation and characterization of cassava bagasse
reinforced thermoplastic cassava starch. Fibers and Polymers 18 (1):162–71. doi:10.1007/s12221-017-6251-7.
Edrisi, S. A., A. El-Keblawy, and P. C. Abhilash. 2020. Sustainability analysis of Prosopis juliflora (Sw.) DC based
restoration of degraded land in North India. Land 9 (2):59. doi:10.3390/land9020059.
16 M. M K ET AL.

Ghanbarzadeh, B., H. Almasi, and A. A. Entezami. 2011. Improving the barrier and mechanical properties of corn
starch-based edible films: Effect of citric acid and carboxymethyl cellulose. Industrial Crops and Products
33 (1):229–35. doi:10.1016/j.indcrop.2010.10.016.
Harini, K., K. Ramya, and M. Sukumar. 2018. Extraction of nano cellulose fibers from the banana peel and bract for
production of acetyl and lauroyl cellulose. Carbohydrate Polymers 201:329–39. doi:10.1016/j.carbpol.2018.08.081.
Hu, F., J. Zeng, Z. Cheng, X. Wang, B. Wang, Z. Zeng, and K. Chen. 2021. Cellulose nanofibrils (CNFs) produced by
different mechanical methods to improve mechanical properties of recycled paper. Carbohydrate Polymers
254:117474. doi:10.1016/j.carbpol.2020.117474.
Jabeen, N., I. Majid, G. A. Nayik, and F. Yildiz. 2015. Bioplastics and food packaging: A review. Cogent Food &
Agriculture 1 (1):1117749. doi:10.1080/23311932.2015.1117749.
Jiugao, Y., W. Ning, and M. Xiaofei. 2005. The Effects of citric acid on the properties of thermoplastic starch plasticized
by glycerol. Starch - Stärke 57 (10):494–504. doi:10.1002/star.200500423.
Kim, H. Y., J. Jane, and B. Lamsal. 2017. Hydroxypropylation improves film properties of high amylose corn starch.
Industrial Crops and Products 95:175–83. doi:10.1016/j.indcrop.2016.10.025.
Kumar, B., S. Patel, N. K. Mishra, and R. K. Naik. 2007. Assessment of some physical and mechanical properties of
different flexible packaging films for packaging of tamarind (Tamarindus indica L.) Pulp Briquettes. Trends in
Biosciences 10 (21):4180–83.
Liu, Y., S. Ahmed, D. E. Sameen, Y. Wang, R. Lu, J. Dai, S. Li, and W. Qin. 2021. A review of cellulose and its derivatives
in biopolymer-based for food packaging application. Trends in Food Science & Technology 112:532–46. doi:10.1016/j.
tifs.2021.04.016.
Luchese, C. L., T. Garrido, J. C. Spada, I. C. Tessaro, and K. de la Caba. 2018. Development and characterization of
cassava starch films incorporated with blueberry pomace. International Journal of Biological Macromolecules
106:834–39. doi:10.1016/j.ijbiomac.2017.08.083.
Madhu, P., S. Pradeep, M. R. Sanjay, and S. Siengchin. 2019. Characterization of raw and alkali treated Prosopis juliflora
fibers for potential polymer composite reinforcement. IOP Conference Series: Materials Science & Engineering
653 (1):012016. doi:10.1088/1757-899X/653/1/012016.
Marichelvam, M. K., M. Jawaid, and M. Asim. 2019. Corn and rice starch-based bio-plastics as alternative packaging
materials. Fibers 7 (4):32. doi:10.3390/fib7040032.
Marichelvam, M. K., P. Manimaran, M. R. Sanjay, S. Siengchin, M. Geetha, K. Kandakodeeswaran, P. Boonyasopon, and
S. Gorbatyuk. 2022. Extraction and development of starch-based bioplastics from Prosopis Juliflora Plant:
Eco-friendly and sustainability aspects. Current Research in Green and Sustainable Chemistry 5:100296. doi:10.
1016/j.crgsc.2022.100296.
Menezes, D. B., F. M. Diz, L. F. Romanholo Ferreira, Y. Corrales, J. R. Baudrit, L. P. Costa, and M. L. Hernández-
Macedo. 2021. Starch-based biocomposite membrane reinforced by orange bagasse cellulose nanofibers extracted
from ionic liquid treatment. Cellulose 28 (7):4137–49. doi:10.1007/s10570-021-03814-w.
Mostafa, N. A., A. A. Farag, H. M. Abo-Dief, and A. M. Tayeb. 2018. Production of biodegradable plastic from
agricultural wastes. Arabian Journal Chemistry 11 (4):546–53. doi:10.1016/j.arabjc.2015.04.008.
Muscat, D., B. Adhikari, R. Adhikari, and D. S. Chaudhary. 2012. Comparative study of film forming behaviour of low
and high amylose starches using glycerol and xylitol as plasticizers. Journal of Food Engineering 109 (2):189–201.
doi:10.1016/j.jfoodeng.2011.10.019.
Oleyaei, S. A., Y. Zahedi, B. Ghanbarzadeh, and A. A. Moayedi. 2016. Modification of physicochemical and thermal
properties of starch films by incorporation of TiO2 nanoparticles. International Journal of Biological Macromolecules
89:256–64. doi:10.1016/j.ijbiomac.2016.04.078.
Peelman, N., P. Ragaert, K. Ragaert, B. de Meulenaer, F. Devlieghere, and L. Cardon. 2015. Heat resistance of new
biobased polymeric materials, focusing on starch, cellulose, PLA, and PHA. Journal of Applied Polymer Science
132:42305. doi:10.1002/app.42305.
Podshivalov, A., M. Zakharova, E. Glazacheva, and M. Uspenskaya. 2017. Gelatin/Potato starch edible biocomposite
films: Correlation between morphology and physical properties. Carbohydrate Polymers 157:1162–72. doi:10.1016/j.
carbpol.2016.10.079.
Prabha, D. S., H. U. Dahms, and P. Malliga. 2014. Pharmacological potentials of phenolic compounds from Prosopis
spp.–a review. Journal of Coastal Life Medicine 2 (11):918–24.
Qin, Y., W. Wang, H. Zhang, Y. Dai, H. Hou, and H. Dong. 2019. Effects of citric acid on structures and properties of
thermoplastic hydroxypropyl amylomaize starch films. Materials 12 (9):1565. doi:10.3390/ma12091565.
Ravindran, L., M. S. Sreekala, and S. Thomas. 2019. Novel processing parameters for the extraction of cellulose
nanofibres (CNF) from environmentally benign pineapple leaf fibres (PALF): Structure-property relationships.
International Journal of Biological Macromolecules 131:858–70. doi:10.1016/j.ijbiomac.2019.03.134.
Rodrigues, S. C. S., A. D. da Silva, L. H. de Carvalho, T. S. Alves, and R. Barbosa. 2020. Morphological, structural, thermal
properties of a native starch obtained from babassu mesocarp for food packaging application. Journal of Materials
Research and Technology 9 (6):15670–78. doi:10.1016/j.jmrt.2020.11.030.
JOURNAL OF NATURAL FIBERS 17

Rohmawati, B., F. Atikah Nata Sya’idah, R. Rhismayanti, D. Alighiri, and W. Tirza Eden. 2018. Synthesis of
bioplastic-based renewable cellulose acetate from teak wood (tectona grandis) biowaste using glycerol-chitosan
plasticizer. Oriental Journal of Chemistry 34 (4):1810–16. doi:10.13005/ojc/3404014.
Salarbashi, D., S. Tajik, M. Ghasemlou, S. Shojaee-Aliabadi, M. Shahidi Noghabi, and R. Khaksar. 2013. Characterization
of soluble soybean polysaccharide film incorporated essential oil intended for food packaging. Carbohydrate Polymers
98 (1):1127–36. doi:10.1016/j.carbpol.2013.07.031.
Sapei, L., K. S. Padmawijaya, O. Sijayanti, and P. J. Wardhana. 2015. The effect of banana starch concentration on the
properties of chitosan-starch bioplastics. Journal of Chemical and Pharmaceutical Research 7 (9S):101–05.
Shanmathy, M., M. Mohanta, and A. Thirugnanam. 2021. Development of biodegradable bioplastic films from Taro
starch reinforced with bentonite. Carbohydrate Polymer Technologies and Applications 2:100173. doi:10.1016/j.carpta.
2021.100173.
Siracusa, V., P. Rocculi, S. Romani, and M. D. Rosa. 2008. Biodegradable polymers for food packaging: A review. Trends
in Food Science & Technology 19 (12):634–43. doi:10.1016/j.tifs.2008.07.003.
Song, X., G. Zuo, and F. Chen. 2018. Effect of essential oil and surfactant on the physical and antimicrobial properties of
corn and wheat starch films. International Journal of Biological Macromolecules 107:1302–09. doi:10.1016/j.ijbiomac.
2017.09.114.
Suryanto, H., A. S. Pahlevi, and U. Yanuhar. 2021. Effect of bacterial cellulose reinforcement on morphology and tensile
properties of starch-based biocomposite. IOP Conference Series: Materials Science & Engineering 1034 (1):012167.
doi:10.1088/1757-899X/1034/1/012167.
Tang, Y., X. Zhang, R. Zhao, D. Guo, and J. Zhang. 2018. Preparation and properties of chitosan/guar gum/nanocrystal­
line cellulose nanocomposite films. Carbohydrate Polymers 197:128–36. doi:10.1016/j.carbpol.2018.05.073.
Tedeschi, G., S. Guzman-Puyol, U. C. Paul, M. J. Barthel, L. Goldoni, G. Caputo, L. Ceseracciu, A. Athanassiou, and
J. A. Heredia-Guerrero. 2018. Thermoplastic cellulose acetate oleate films with high barrier properties and ductile
behaviour. Chemical Engineering Journal 348:840–49. doi:10.1016/j.cej.2018.05.031.
Valencia, L., V. Arumughan, B. Jalvo, H. J. Maria, S. Thomas, and A. P. Mathew. 2019. Nanolignocellulose extracted
from environmentally undesired Prosopis juliflora. ACS Omega 4 (2):4330–38. doi:10.1021/acsomega.8b02685.
Wahyuningtiyas, N. E., and H. Suryanto. 2018. Properties of cassava starch based bioplastic reinforced by nanoclay.
Journal of Mechanical Engineering Science and Technology 2 (1):20–26. doi:10.17977/um016v2i12018p020.
Wang, W., F. Gu, Z. Deng, Y. Zhu, J. Zhu, T. Guo, J. Song, and H. Xiao. 2021. Multilayer surface construction for
enhancing barrier properties of cellulose-based packaging. Carbohydrate Polymers 255:117431. doi:10.1016/j.carbpol.
2020.117431.
Woggum, T., P. Sirivongpaisal, and T. Wittaya. 2014. Properties and characteristics of dual-modified rice starch based
biodegradable films. International Journal of Biological Macromolecules 67:490–502. doi:10.1016/j.ijbiomac.2014.03.029.
Yang, J., X. Dong, J. Wang, Y. C. Ching, J. Liu, C. Li, Y. Baikeli, Z. Li, N. Mohammed Al-Hada, and S. Xu. 2022. Synthesis
and properties of bioplastics from corn starch and citric acid-epoxidized soybean oil oligomers. Journal of Materials
Research and Technology 20:373–80. doi:10.1016/j.jmrt.2022.07.119.
Yaradoddi, J. S., N. R. Banapurmath, S. V. Ganachari, M. E. M. Soudagar, N. M. Mubarak, S. Hallad, S. Hugar, and
H. Fayaz. 2020. Biodegradable carboxymethyl cellulose based material for sustainable packaging application. Scientific
Reports 10 (1):21960. doi:10.1038/s41598-020-78912-z.
Zakaria, N. H., N. Muhammad, A. V. Sandu, and M. M. A. B. Abdullah. 2018. Effect of mixing temperature on
characteristics of thermoplastic potato starch film. IOP Conference Series: Materials Science & Engineering
374 (1):012083. doi:10.1088/1757-899X/374/1/012083.
Zhang, R., X. Wang, and M. Cheng. 2018. Preparation and characterization of potato starch film with various size of
nano-SiO2. Polymers 10 (10):1172. doi:10.3390/polym10101172.

You might also like