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 2 ; 2 0 : 3 7 3 e3 8 0

Available online at www.sciencedirect.com

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

Original Article

Synthesis and properties of bioplastics from corn

starch and citric acid-epoxidized soybean oil
oligomers

Jianlei Yang a,*, Xiaotong Dong b, Jiyi Wang c, Yern Chee Ching d, Jing Liu e,
Chunhui li c, Yiliyasi Baikeli c, Zhen li c, Naif Mohammed Al-Hada a,
Shicai Xu a
a
Shandong Key Laboratory of Biophysics, Institute of Biophysics, Dezhou University, Dezhou, 253023, China
b
College of Physics and Electronic Information, Dezhou University, Dezhou, 253023, China
c
College of Chemistry and Chemical Engineering, Dezhou University, Dezhou, 253023, China
d
Department of Chemical Engineering, Faculty of Engineering, University of Malaya, Kuala Lumpur, 50603,
Malaysia
e
College of Medicine and Nursing, Dezhou University, Dezhou, 253023, China

article info abstract

Article history: Citric acid-epoxidized soybean oil oligomers (CESO) were prepared and utilized to improve
Received 8 July 2022 the properties of corn starch-based bioplastics. CESO were synthesized by controlling the
Accepted 18 July 2022 stoichiometric ratio of acid equivalent weight and epoxy equivalent weight at 3:1. Starch-
Available online 31 July 2022 based bioplastics with satisfactory properties were fabricated through solution casting.
Analysis including FTIR, molecular distribution, and polydispersity index validated the ring
Keywords: opening polymerization of ESO and CA. The hydrogen bond and crosslinking interactions
Starch between CESO and starch were evidenced by the FTIR. SEM micrographs suggested that
Bioplastic CESO exhibited better compatibility with starch than ESO. X-ray diffraction patterns of the
Citric acid bioplastics were changed apparently by CESO due to the crosslinking interaction. Swelling
Epoxidized soybean oil degree and opacity of the bioplastics reduced significantly after the introduction of CESO,
Compatibility while tensile strength increased remarkably from 5.62 to 6.93 MPa (p < 0.05). The bioplastic
Packaging with 4 wt% CESO revealed the most comprehensive properties. Higher content of CESO
(16 wt%) displayed poor interaction with starch and led to deteriorated properties of the
bioplastics. The synthesized bioplastics exhibited enormous potential to partially replace
petroleum-based plastics for various applications such as packaging.
© 2022 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: yangjlly1985@outlook.com (J. Yang).
https://doi.org/10.1016/j.jmrt.2022.07.119
2238-7854/© 2022 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/).
374 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 2 ; 2 0 : 3 7 3 e3 8 0
1. Introduction
Currently, more than 99% of packaging plastic, including bags,
tableware, and disposable straws, are produced from
petroleum-based polymers [1]. Packaging plastic pollution has
become one of the most urgent environmental problems all
over the world. Bioplastic from the conversion of biomass is
considered as one of the sustainable methods to address the
issue [2,3].
Up to now, numerous renewable resources, such as cellu-
lose, starch, natural oils, and protein, have been applied as
promising alternatives to develop the bioplastics [4,5]. The
biodegradability, renewability, and resource abundance
endow starch-derived bioplastic an ideal candidate for pack-
aging bioplastic. However, the mechanical properties and
water-stability of starch-based bioplastics are undesirable and
drastically impede their practical application [6]. Although
attempts have been made to prepare starch-derived bio-
plastics with water stability and high strength, the progress is
unsatisfactory [7,8]. Therefore, it is urgent to develop a facile
method to manufacture the starch-based bioplastics featuring
high water resistance and mechanical strength.
Soybean oil is one of the cheapest and most abundant plant
oils in the world and it can be used to prepare epoxidized
soybean oils (ESO) industrially, which have been extensively
investigated to synthesize thermosets [3,4]. Great progress has
been made in the bioplastic development based on starch and
ESO. ESO can effectively enhance the mechanical properties
and hydrolytic stability of starch-based bioplastics based on
the condensation reaction between epoxy groups and hy-
droxyl groups [5,9]. However, ESO have a low compatibility
and reaction efficiency with starch, which leads to low
crosslinking network and hamper their application signifi-
cantly [3,10]. There is a tremendous room to design starch/
ESO-based bioplastics with excellent properties.
Compatibilizers such as polyethylenimine, maleic anhy-
dride, and citric acid have been attempted to enhance the
bonding of starch and epoxy oil [10,11]. Citric acid (CA) is a
natural organic acid and has three carboxyl groups that could
participate in the reaction with epoxy groups of ESO [12] and
hydroxyl groups of starch to form the crosslinked network
[13,14]. In previous work, we proposed citric acid-epoxidized
palm oil oligomers (nCOOH/epoxy ¼ 1) to modify the properties
of starch-based bioplastics. Enhancement efficiency of the
oligomers on the properties of the bioplastic was compro-
mised as all carboxyl groups of CA have formed tight inter-
action with ESO and there were no excess carboxyl groups to
react with starch [15]. Therefore, the formulation for synthe-
sizing the oligomers needs to be adjusted further.
In this study, a facile strategy was operated to convert ESO
into multi-functional oligomers and synthesize starch-based
bioplastics with the oligomers by solution casting. Firstly,
the CESO oligomers were synthesized with acid equivalent
weight and epoxy equivalent weight at 3:1. It was supposed
that only one carboxyl group of CA molecule participated in
the ring opening reaction with ESO, while the other two
carboxyl groups performed esterification reaction with starch.
The effect of CESO contents (4, 8, and 16 wt%) on the struc-
tures and properties of the bioplastics was studied. FTIR, SEM,
XRD, mechanical property, water resistance, and opacity of
the bioplastics were investigated to establish the relationship
between structures and performance.
2. Materials and methods
2.1. Materials
Chitosan (deacetylation degree: 90%; molecular weight:
30,000 g/mol), corn starch (5.30% moisture and 27% amylose),
sodium bromide, and polystyrene standards were supplied by
Macklin biochemical Co., Ltd (Shanghai, China). Commercial
epoxidized soybean oil (minimum 99.00% purity and 356 g/
mol epoxy equivalent weight) was supplied by Qilu petro-
chemical engineering Co., Ltd (Shandong, China). Epoxy
equivalent weight describes the mass (g) of ESO required to
give 1 mol epoxy groups. Citric acid monohydrate (99.5%),
microcrystalline cellulose, sodium chloride, glycerol, tetra-
hydrofuran (HPLC grade), and Tween 80 were provided by
Tianjin kemiou chemical reagent Co., Ltd.
2.2. Synthesis of citric acid-epoxidized soybean oil
oligomers (CESO)
The synthesis of CESO was performed based on our previous
work [15]. A mixture of CA and water was heated at 90  C until
dissolved completely. ESO were added into it with the stoi-
chiometric ratio of acid equivalent weight and epoxy equiva-
lent weight of 3:1. The reaction was performed at 90  C for
45 min. Afterwards, a certain amount of glycerol was intro-
duced into the product to make the mixture homogeneous.
Finally, the synthesized CESO were immediately used to pre-
pare the bioplastics in the next section.
2.3. Preparation of the CESO/corn starch bioplastics
In this study, chitosan and microcrystalline cellulose were
applied to improve the strength of the bioplastics. Instead of
preparing the bioplastic by reactive extrusion, a commonly
used process in the industry [16,17], solution casting was used
for the sake of simplicity in our laboratory. Specifically, an
aqueous solution of corn starch, glycerol, and microcrystalline
cellulose was prepared and heated at 90  C for 30 min. Chi-
tosan solution (2 wt%) in 1% acetic acid was incorporated and
the dry mass ratio of starch to chitosan was 19:1. Next, ESO or
CESO and Tween 80 were added into above solution. The
mixture was homogenized at 10,000 rpm for 60 s. 60 g of the
solution was poured into the glass plate and dried at 60  C in
an oven for 6 h. The films were further cured for 1 h at 120  C to
induce the crosslinking reaction between starch and epoxy oil.
The samples were placed in a desiccator (57% relative hu-
midity, achieved using saturated sodium bromide) for 72 h at
room temperature. The formulations for synthesizing starch-
based bioplastics are shown in Table 1.
2.4. Characterization techniques
2.4.1. Gel permeation chromatography (GPC)
Molecular weight and polydispersity index of ESO and CESO
were tested by a GPC (1515, Waters Corporation, USA) with
 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 2 ; 2 0 : 3 7 3 e3 8 0 375

Table 1 e Composition of starch-based bioplastics based on dry weight.

Samplesa Starch (g) Chitosan (g) Cellulose (g) Glycerol (g) ESO/CESO (g) Tween 80 (g)
ST-ESO-8 5.7000 0.3000 0.3000 2.4000 0.4800 0.0480
ST-CESO-4 5.7000 0.3000 0.3000 2.4000 0.2400 0.0240
ST-CESO-8 5.7000 0.3000 0.3000 2.4000 0.4800 0.0480
ST-CESO-16 5.7000 0.3000 0.3000 2.4000 0.9600 0.0960
a
The number in the code indicates the weight proportion of CESO or ESO to the total weight of starch and chitosan.

2414 refractive index detector. Tetrahydrofuran was the mo- dried at 105  C in an oven. Swelling degree and water solubility
bile phase with 1 mL/min flow rate. The standards were were calculated by Eqs. (1) and (2), respectively:
polystyrene.
Swelling degree ¼ ðM1  Mo Þ = Mo (1)

2.4.2. Fourier transform infrared spectroscopy (FTIR)

FTIR spectra of all the samples were analyzed on the sample
surfaces using ATR-FTIR (Netzsch Sta449 F5 Jupiter, Thermo
Scientific Nicolet iS50, USA) with 32 scans, 4 cm1 resolution,
and wavenumbers of 4000e500 cm1.
Water solubility ð%Þ ¼ ðMo  M2 Þ = Mo  100 (2)
where Mo indicates the initial sample mass, M1 represents the
wet sample mass, and M2 is the dry mass of undissolved
sample after soaked in water.

2.4.3. Field emission scanning electron microscopy (FESEM) 2.4.7. Opacity

The tensile-fractured surfaces of the bioplastics were coated
by a gold layer using a sputter coater (108auto, Cressington)
and then observed by the FESEM (Merlin Compact, ZEISS,
Germany). The sample micrographs were recorded at the
1000 magnification.
2.4.4. X-ray diffraction (XRD)
The X-ray diffractometer (D8 advance, Bruker, Germany) was
utilized to analyze the XRD diffractograms of the samples. The
current and voltage were 40 mA and 40 kV, respectively. The
diffraction patterns were collected from 5 to 60 by a step of
0.02 .
2.4.5. Mechanical property
The Auto Tensile Tester (XLW, Labthink Instruments Co., Ltd.,
Jinan, China) was used to perform the mechanical property of
the bioplastics based on ASTM D882. The sample strips were
15 mm  100 mm. The crosshead speed was 50 mm/min and
the original distance between the grips was 50 mm. Five
determinations were obtained for each sample.
2.4.6. Swelling degree and water solubility
Swelling degree and water solubility were performed by placing
the dry samples (20 mm  20 mm, thickness: 0.14e0.17 mm) in
distilled water for 24 h. Undissolved parts were obtained and
The opacity of the bioplastics was determined by a Spectro-
photometer (UV 1900, Shanghai Youke Instrument Co., Ltd,
China). The light absorbance of specimens (10 mm  35 mm,
thickness: 0.14e0.17 mm) was tested at 600 nm with an empty
cuvette as the control. The opacity was calculated with Eq. (3):


Opacity mm1 ¼ A600 T (3)
where A600 presents the light absorbance at 600 nm and T
indicates the sample thickness (mm).
2.5. Statistical analysis
Statistical analysis was carried out with SPSS version 19.0
(SPSS Inc., Chicago, USA). One-way analysis of variance
(ANOVA) with Tukey’ test was conducted with 5% significance
level.
3. Results and discussion
3.1. Characterization of CESO
FTIR spectra of ESO and CESO are shown in Fig. 1. In the case of
ESO, the band around 823 cm1 is associated with epoxy group
[18]. The band (823 cm1) disappeared for CESO. The carboxyl

Fig. 1 e FTIR spectra of ESO and CESO.

376 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 2 ; 2 0 : 3 7 3 e3 8 0
Fig. 2 e FTIR spectra for starch-based bioplastics.
groups of CA would react with the epoxy groups of ESO to
produce ester bonds and new hydroxyl groups [19]. The band
at 1740 cm1 was associated with carbonyl groups (C]O) of ESO
[9]. The band (1740 cm1) for CESO became broader compared
to that of ESO, which suggested the formation of ester bonds.
Moreover, the band might derive from the excess carboxyl
groups of CA [20]. The formation of new hydroxyl groups for
CESO was evidenced by the broad band around 3470 cm1. The
generated hydroxyl groups could further react with the epoxy
groups of ESO. The reaction of ESO and CA is generally too
complicated to be illustrated by chemical structures and
equations [4,15].
The GPC results displayed that the number-average molec-
ular weight (Mn) and weight-average molecular weight (Mw) of
ESO were 1186 and 1274 g/mol, respectively. The polydispersity
index (PDI) of ESO was 1.07. CESO exhibited higher molecular
weight (Mn and Mw, 1887 and 5550 g/mol, respectively) and PDI
(2.94) than ESO, which demonstrated the reaction of ESO and
CA and the presence of CESO with different molecular weights
[21]. One CA molecule might react with 1e3 ESO molecules as
CA contained three eCOOH groups. This was consistent with
the result of wide molecular weight distribution.
3.2. Characterization of the bioplastics
Starch and CESO were chosen as the materials to fabricate the
bioplastics. CESO with multiple carboxylic groups were
Fig. 3 e XRD diffractograms of starch-based bioplastics.
supposed to provide adequate crosslinking sites with hydroxy
groups of starch, while various amount of CESO might provide
tunable water resistance, stiffness, and toughness to the
bioplastics.
3.2.1. FTIR
FTIR spectra of the bioplastics are illustrated in Fig. 2. The
band for OeH stretching of ST-ESO-8 is observed at 3277 cm1.
It was shifted to lower wavenumbers for the bioplastics with
CESO. These shifts revealed the hydrogen bonding in-
teractions between starch and CESO [15]. The band shift might
also demonstrate the decreased number of free hydroxyl
groups due to the crosslinking interaction. The substitution of
the hydroxyl groups with the ester groups on the starch
molecules prohibited the inter and intra-molecular hydrogen
bonding. The bands at 2923 cm1 and 2854 cm1 are ascribed
to the eCH stretching vibration of eCH2 groups. Both band
intensity reduced as different contents of CESO were intro-
duced. The band at 1741 cm1 for ST-ESO-8 can be attributed
to the stretching vibration of C]O in ESO. The absorption band
(1741 cm1) of the bioplastics diminished after the introduc-
tion of 4 wt% CESO and intensified gradually as higher con-
tents of CESO were added. The band shapes of the bioplastics
were in agreement with that of the introduced oil types. The
increase of the band's height can reflect the increase of the
ester bonds formed by starch and CESO [22]. Besides, it might
be caused by the excess carboxyl groups in CESO also [23].
 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 2 ; 2 0 : 3 7 3 e3 8 0 377

Fig. 4 e Tensile-fractured surfaces of starch-based bioplastics at the magnification of 1000£. (a) ST-ESO-8, (b) ST-CESO-4, (c)
ST-CESO-8, and (d) ST-CESO-16.

3.2.2. XRD 3.2.3. Field emission scanning electron microscopy (FESEM)

Figure 3 displays the XRD diffractograms [24] of starch-based
bioplastics. ST-ESO-8 presented the B-type crystalline struc-
ture, exhibiting two intense peaks at 19.7 and 22.1 , which
were in agreement with previous publications [7,25]. ST-CESO-4
also exhibited a typical B-type pattern with three characteristic
peaks at 2q around 17.0 , 19.7 and 22.1 , respectively [6,26]. The
appearance of peak at 17.0 should be due to amylopectin
retrogradation [25,27]. The peak intensity (17.0 ) reduced grad-
ually after the samples were introduced with higher contents of
CESO, demonstrating the inhibition of amylopectin retrogra-
dation. The crosslinking interaction between CESO and starch
restrained the molecular chain movements and crystallization
process, thus disrupting the ordered array of molecules and
reducing the crystallinity of the matrix [6,15].
Figure 4 exhibits the tensile-fractured surface images of
the bioplastics. Many microvoids appeared on the
cross-section of the samples containing ESO (Fig. 4(a)),
which resulted from ESO droplets [28]. The fracture
surfaces of ST-CESO exhibited fewer holes, suggesting
that CESO showed better compatibility with starch than
ESO (Fig. 4(b)e(d)). The outcome might be ascribed to
strong hydrogen bond and esterification interactions
between starch and CESO [29]. However, there were still a
few holes present in the films containing CESO. The rougher
fractured surface as a result of an increase in the CESO
content in the bioplastic would indicate a tougher material
[30]. This agreed with an increase in EAB with increasing
CESO content.

Fig. 5 e Tensile strength and elongation at break of the bioplastics.

378 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 2 ; 2 0 : 3 7 3 e3 8 0

3.2.4. Mechanical property

Table 2 e Opacity and water resistance of the bioplastics.
Figure 5 presents the mechanical property of the bioplastics.
ST-ESO-8 showed the tensile strength (TS) of 5.62 MPa and Samples Opacity Swelling Water solubility
(mm1) degree (%)
elongation at break (EAB) of 36.30%, respectively. TS of the
bioplastics sharply increased (6.80e6.93 MPa) when 4 wt% or ST-ESO-8 3.04 ± 0.22a 5.12 ± 0.25a 15.93 ± 0.92a
8 wt% CESO was incorporated (p < 0.05). This result might be ST-CESO-4 2.09 ± 0.29b 4.40 ± 0.064b 17.79 ± 1.43a
ST-CESO-8 2.31 ± 0.19b 5.20 ± 0.078a 16.56 ± 0.28a
attributed to the fact that extra carboxylic groups of CESO
ST-CESO-16 2.50 ± 0.34ab 4.07 ± 0.11b 17.88 ± 0.28a
could form stronger crosslinking interactions with starch,
a and b mean that values in the same column with different letters
resulting in more rigid structure [31]. There was no significant
are significantly different (p < 0.05).
impact of 4 wt% and 8 wt% CESO on the tensile strength of the
films. TS reduced remarkably for the bioplastics with 16 wt%
CESO (p < 0.05). Lower TS might emphasize the poor interac-
result can be explained by the fact that CESO had lower
tion between CESO and starch, which agreed with the rough
swelling than starch, thus reducing the swelling degree [6].
and heterogeneous cross-section as revealed by FESEM. Addi-
Water solubility of all the bioplastics varied from 15.93% to
tionally, this might be ascribed to the poor mechanical prop-
17.88%. The incorporation of various contents of CESO into
erty of CESO cured films [2,29]. Xiong, Yang, Feng, Zhang,
the bioplastics improved the water solubility slightly
Zhang, Tang and Zhu [10] also discovered a significant deteri-
(p > 0.05). Although CESO were not soluble in water, they
oration of mechanical property when the concentration of
might cause the acid hydrolysis of starch in the process of
vegetable oil in biopolymer composites increased up to a
curing process [10].
certain value.
It was expected that EAB of the bioplastics showed opposite
3.2.7. Comparison between the bioplastics and petroleum-
trend to TS. EAB reduced drastically (17.18%) (p < 0.05) and then
based plastics
increased slightly with the contents of CESO increasing
In order to evaluate the potential of the bioplastics to replace
(p > 0.05). Regarding the reduction of EAB, this might be
petroleum-based plastics for packaging application. Water
assigned to the high molecular weight of CESO as shown by
solubility and mechanical property of the bioplastics were
GPC results, which cannot play the role of plasticizers for
compared with those of commercial petroleum-based plas-
starch.
tics such as low-density polyethylene (LDPE), high-density
polyethylene (HDPE), polyethylene terephthalate (PET),
3.2.5. Opacity
polyvinyl chloride (PVC), polyamide (PA, nylon), poly-
The opacity of the bioplastic composites is displayed in Table
propylene (PP), polystyrene (PS), and polyvinyl alcohol (PVA)
2. Film opacity is closely associated with the microstructure of
(Table 3).
the film. A higher opacity represents a lower degree of trans-
It was noted that tensile strength of the bioplastics was
parency [7]. The opacity of ST-ESO-8 was 3.04 mm1, which
close to that of LDPE and far below the other plastics. The
might be attributed to the difference in the refractive index of
bioplastics were more brittle compared to other petroleum-
starch and ESO. It obviously decreased to 2.09e2.50 mm1
based plastics except PS. The application of the bioplastics
upon the addition of CESO (p < 0.05). This remarkable decrease
might be restrained in the environment with high humidity
suggested that CESO had better dispersibility in the bioplastics
due to their high solubility. Therefore, the prepared
than ESO, which enhanced light transmittance. The opacity of
bioplastics can be introduced into petroleum-based plastics,
the samples increased as higher contents of CESO was incor-
such as LDPE or PVA, in a certain percentage, thus
porated. This might be related to the heterogeneous structure
reducing the application of petroleum-based plastics.
of the bioplastics, which hindered light transmittance and
Further study is needed to improve the tensile and water
caused light dispersion.
resistance property of starch-based bioplastics to broaden
their applications.
3.2.6. Water resistance
Water resistance exhibits the integrity of the sample in an
aqueous environment. Water resistance of the bioplastics
was assessed by swelling degree and water solubility as
summarized in Table 2. ST-ESO-8 showed a swelling degree of Table 3 e Tensile property and water solubility of the
fabricated bioplastics and some petroleum-based plastics
5.12. It can be seen that swelling degree of the bioplastics
[32e35].
varied as different contents of CESO were incorporated.
Plastics Tensile strength Elongation Water
Swelling degree of the samples decreased remarkably after
(MPa) at break (%) solubility (%)
the addition of 4 wt% CESO (p < 0.05). CESO had stronger
interaction with starch than ESO, which hindered the pene- This study 6.93 17.18 15.93
LDPE 7e25 300e900 0
tration of water into the starch network. However, swelling
HDPE 19e31 30e50 0
degree of the bioplastics increased again when 8 wt% CESO PET 155e177 70 0
was added. This might be associated with the heterogeneous PVC 42e55 20e180 0
structure of the bioplastics, as demonstrated by FESEM, PA 49e69 200e300 0
which reduced the cohesiveness of the starch matrix and PP 27e98 200e1000 0
promoted the water permeation. Interestingly, swelling de- PS 31e49 2e3 0
PVA 58.5 141.7 45.0
gree reduced remarkably for ST-CESO-16 again (p < 0.05). The
 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 2 ; 2 0 : 3 7 3 e3 8 0
4. Conclusions
We designed starch-based bioplastics by chemical modifica-
tion with citric acid-epoxidized soybean oil oligomers (CESO),
both being renewable and biodegradable. The successful
synthesis of CESO was confirmed by FTIR and GPC analysis.
CESO and starch developed hydrogen bonding interaction and
crosslinking reaction as observed by the FTIR. SEM photo-
graphs observed that CESO exhibited higher compatibility
with starch than ESO. The XRD patterns of the bioplastics
were influenced obviously by the CESO contents. Conse-
quently, the resulting bioplastics with CESO showed superior
tensile strength, transparency, and swelling degree than that
with ESO. Comparatively, ST-CESO-4 exhibited the most
favorable properties among all the samples. In addition, 16 wt
% CESO did not contribute to obvious improvement of water
resistance and mechanical property of the samples due to
incompatibility and acid hydrolysis. The developed starch-
based bioplastic was confirmed as an attractive candidate
for developing packaging materials. Future study is needed to
synthesize CESO by removing excess CA, which may over-
come the starch hydrolysis and further increase CESO addi-
tion level in the bioplastics.
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 study was supported by the Talent Introduction Project of
Dezhou University (No. 2022xjrc102).
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