Algal Research 56 (2021) 102321

Contents lists available at ScienceDirect

Algal Research
journal homepage: www.elsevier.com/locate/algal

Effect of filler and sonication time on the performance of brown alga

(Sargassum plagiophyllum) filled cassava starch biocomposites
Supichchayapak Jantasrirad a, Jaruwan Mayakun b, c, Apon Numnuam a, d, Kaewta Kaewtatip a, d, *
a
Division of Physical Science, Faculty of Science, Prince of Songkla University, Hat Yai, Songkhla, 90112, Thailand
b
Division of Biological Science, Faculty of Science, Prince of Songkla University, Hat Yai, Songkhla, 90112, Thailand
c
Molecular Evolution and Computational Biology Research Unit, Faculty of Science, Prince of Songkla University, Hat Yai, Songkhla, 90112, Thailand
d
Center of Excellence for Trace Analysis and Biosensor, Prince of Songkla University, Hat Yai, Songkhla, 90112, Thailand

A R T I C L E I N F O A B S T R A C T

Keywords: A biocomposite was prepared from a mixture of pre-gelatinized cassava starch and a brown alga (Sargassum
Cassava starch plagiophyllum) as a potential alternative material to synthetic plastic. The brown alga was ground using a
Biocomposites planetary ball mill and its morphology was characterized and particle size determined. Mixtures of starch and
Sonication
milled brown algae were sonicated to improve dispersion of the algae in the starch matrix. Biocomposites of
Sargassum
starch and milled brown algae were prepared using compression molding. The effects of milled brown algae
content and sonication time on the properties of the obtained starch-based biocomposites were investigated. The
biocomposite with the highest tensile strength (2.22 MPa) and the lowest weight loss after accelerated weath­
ering for 24 h (20.65%) was from a mixture of starch and 10 wt% milled brown algae sonicated for 120 s. These
results were consistent with the good dispersion and adhesion of the milled brown algae in the starch matrix as
revealed by scanning electron microscopy (SEM) images. Stress transfer in this biocomposite was more effective
and photo-degradation and hydrolytic degradation were inhibited. Thermogravimetric analysis (TGA) results
showed that the addition of 10 wt% of milled brown algae and sonication for 120 s also improved the thermal
stability of the obtained biocomposite.

1. Introduction
Synthetic plastic waste causes worldwide environmental problems
since it is resistant to chemicals, weather and biodegradation. It will
continue to accumulate in the environment if it is not suitably managed
and controlled [1–3]. One approach to the management of synthetic
plastic waste for sustainable development is the replacement of syn­
thetic plastics with bioplastics. Starch can be a perfect candidate ma­
terial in the development of bioplastics. It offers several advantages. It is
inexpensive, abundant, renewable and biodegradable [3–5]. Moreover,
standard techniques used for producing petrochemical-based plastics,
such as extrusion, injection and compression molding, can also be used
to process starch-based bioplastics. However, some properties of starch-
based bioplastics must be improved to position them as competitors to
synthetic plastics. In particular, starch exhibits poor mechanical and
thermal properties [6,7]. The fabrication of starch-based composites
using filler materials is an effective modification of starch-based bio­
plastics that improves some properties at low cost and without the need
of special equipment and techniques. Some of the more interesting fillers
are lignocellulosic materials derived from plant sources. Flax, cotton and
sisal fibers, bagasse, rice and coffee husk are widely available with good
biodegradability properties, inexpensive, non-toxic and of low density
[8–12]. Moreover, starch and lignocellulosic materials are poly­
saccharides with similar chemical structures that can have highly
effective performances resulting from good interactions between the
filler and the starch matrix.
The lignocellulosic materials above are all obtained from plants
grown in soil. Lignocellulosic materials can also be obtained from a
marine biomass such as Sargassum. It is one of the largest of the brown
algae commonly found in intertidal and subtidal zones and is widely
distributed in temperate and tropical regions [13–15]. Brown algae
commonly produce a variety of polysaccharides such as sulfated poly­
saccharides and fucoidans. These materials have been widely commer­
cialized as metabolites in cosmetics, medicines, foodstuffs and industry
[16–19]. In Thailand, Sargassum is one of the most dominant and
abundant species growing on wave exposed rocky shores and is widely

* Corresponding author at: Division of Physical Science, Faculty of Science, Prince of Songkla University, Hat Yai, Songkhla, 90112, Thailand.
E-mail address: kaewta.k@psu.ac.th (K. Kaewtatip).

https://doi.org/10.1016/j.algal.2021.102321
Received 21 December 2020; Received in revised form 6 April 2021; Accepted 17 April 2021
Available online 4 May 2021
2211-9264/© 2021 Elsevier B.V. All rights reserved.
S. Jantasrirad et al. Algal Research 56 (2021) 102321

Fig. 1. The processing procedure of milled brown algae powder (BA and MBA were denoted brown alga powder before milling and after milling, respectively).

distributed along the coastal areas of the Thai Peninsula. Seventeen

Table 1
Sargassum species have been reported in Thai waters. Sargassum plagio­
Details of composite constituents.
phyllum C. Agardh from the Andaman Coast was chosen for the present
study because it has a high density. It is an abundant raw material that Samples MBA (wt%) Sonication time (seconds)
can produce chemical compounds such as sulfated fucoidans, poly­ 0%MBA 0 0
phenols, antioxidant compounds, and other polysaccharides useful in 10%MBA 10 0
pharmaceutical, medical, and other commercial applications [20,21]. 20%MBA 20 0
10%MBA/60S 10 60
Moreover, the bioactive compounds present in brown seaweeds have 10%MBA/90S 10 90
been reported to possess strong antibacterial, anti-viral and anti-cancer 10%MBA/120S 10 120
properties [21]. A few studies have focused on the use of marine biomass
MBA and S denoted milled brown algae powder and sonication time,
(e.g., Eucheuma cottonii, Nanochloropsis gaditana, Spirulina, Scendescmus,
respectively.
Heterochlorella luteoviridis BE002 and Dunaliella tertiolecta BE003) as a
filler for starch-based biocomposites [22–24]. They reported that marine
scanning electron microscopy (SEM), thermogravimetric analysis (TGA)
biomass was capable of increasing the mechanical and barrier properties
and accelerated weathering.
of starch-based biocomposites that did not release toxic components
after degradation. However, to the best of our knowledge, there are no
2. Materials and methods
reports on the use of Sargassum as a filler in a starch-based biocomposite.
Sargassum crude extract has potential to be used as a biopolymer
2.1. Materials
nanocomposite films because this algae is rich in carbohydrates such as
cellulose and alginate in its cell walls, which can improve the mechan­
Pre-gelatinized cassava starch (PD 10370) was kindly supplied by
ical, thermal, and biodegradation properties of biopolymer film. It has
Siam Modified Starch Co., Ltd. (Pathum Thani, Thailand). The starch
been reported that the tensile strength of biocomposites was increased
was dried at 105 ◦ C for 24 h in an oven and kept in a desiccator prior to
14.10% and 56.30% when 5% and 25% cellulose nanocrystals were
use. Glycerol was from Ajax Finechem (Auckland, New Zealand).
added, respectively [25]. Thus, Sargassum can be a good candidate as a
S. plagiophyllum was collected from Lanta Island, Krabi Province,
filler for biodegradable biopolymer films. Therefore, this work aims to
Andaman Sea, Thailand. It was washed with tap water to remove any
improve the properties of a starch-based biocomposite by using
impurities, dried in a hot air oven at 70 ◦ C for 24 and cut using a Pol­
S. plagiophyllum as a filler.
ymix, PX-MFC 90 D (Switzerland). The prepared S. plagiophyllum was
Ball milling and high-intensity ultrasonication are well-known
denoted BA (brown algae powder). Ten grams of BA were placed in the
methods of reducing filler particle size and breaking down filler ag­
grinding jar of a planetary ball mill (Model No. PM 100, Retsch Co.,
glomerations to obtain a better dispersion of filler in a polymer matrix.
Germany) with 10 grinding balls. The mill was operated for 1 h at 400
The more compact and homogeneous structures produced improved
rpm. The milled BA was denoted MBA, dried in a hot air oven and kept in
water resistance and mechanical, thermal and barrier properties of
a desiccator until application. The processing procedure of BA and MBA
composites, and the techniques used were environmentally friendly and
is shown in Fig. 1.
economical since toxic and expensive chemical regents were not needed
[26–28]. The particle size of lignocellulosic materials has also been
reduced by novel approaches that involved high-intensity ultra­ 2.2. Preparation of the sonicated milled brown algae powder (MBA)
sonication combined with chemical pretreatments [29] and ball milling
combined with chemical treatment [30]. However, there are few reports MBA (10 wt% of starch) and glycerol (45 wt% of starch) were mixed
of ball milling combined with high-intensity ultrasonication to reduce in a glass beaker. A probe sonicator (VCX-130, Vibra-cells Ultrasonic
the size and improve the dispersion of lignocellulosic materials in a Processor, USA) was immersed in the center of the glass beaker at a
polymer matrix. The combination of ball milling and high-intensity depth of 1 cm. The ultrasonic amplitudes were set at 100% (actual power
ultrasonication is interesting since it constitutes a widely applicable was 35 W) for 60, 90 and 120 s and operated at 130 W at 20 KHz.
method that is completely non-toxic [31].
The focus of this work is the reduction of the particle size of 2.3. Preparation of composites
S. plagiophyllum and the improvement of its dispersion in the starch
matrix using ball milling combined with high-intensity ultrasonication. Pre-gelatinized cassava starch, glycerol (45 wt% of starch) and either
Firstly, the particle size of S. plagiophyllum was reduced using planetary MBA (0, 10 and 20 wt% of starch) or sonicated MBA (10 wt% of starch)
ball milling at 400 rpm for 1 h. The effects of ball milling on the were pre-mixed in polyethylene bags. Each mixture was then further
morphology and median particle size (d50) of S. plagiophyllum were mixed in a two-roll mill at room temperature for 2 min. Sample sheets
investigated. After that, the effects of S. plagiophyllum content (0, 10 and (13 cm × 13 cm × 1.5 mm) were produced by compression molding (KT-
20 wt%) and sonication time (60, 90 and 120 s) were determined on the 7014, Kao Tieh Ltd., Taiwan). The mold was preheated at 150 ◦ C for 5
properties of the prepared starch-based biocomposite. The experimental min. Compression at 150 ◦ C took place in 3 steps: first at 0.70 mPa for 3
approaches used in the characterization of the biocomposite included min, then at 1.70 mPa for 3 min, and lastly at 2.40 mPa for 5 min before
mechanical testing, Fourier transform infrared spectroscopy (FT-IR), cooling at 150 ◦ C for 5 min. The details of composite constituents are
presented in Table 1.

2
S. Jantasrirad et al.
Fig. 2. Appearance, median particle size (d50) (average ± standard errors, n = 3) and SEM micrographs of BA (a) and MBA (b) (BA and MBA denoted brown algae
powder before milling and after milling, respectively.).
2.4. Characterization of composites
The median particle size (d50) of BA and MBA was determined using
a laser particle size analyzer (ANALYSETTE 22 NanoTec, FRITSCH,
Germany). Each sample was tested in three replicates sampled from the
middle of the container. The median particle size was expressed as the
average of the three replicates.
A scanning electron microscope (SEM-Quanta 400, Netherlands) was
used to study the morphology of BA and MBA and fractured surfaces of
neat starch biopolymer and the composites. All samples were mounted
on stubs with double-sided sticky tape. The samples were coated with a
thin layer of evaporated gold.
Tensile tests were performed following the ASTM D412 Type C
protocol [32]. A universal testing machine (Instron model 3365, USA)
was used at a crosshead speed of 20 mm/min with a 100 N load cell.
Tensile testing was conducted at 25 ± 3 ◦ C and 58 ± 2% relative hu­
midity (RH) after equilibrating the samples for 7 days. The data for the
mechanical properties of neat starch biopolymer and the composite
samples were the average values from ten independently tested
specimens.
The accelerated weathering test followed the ASTM G154 CYCLE 2
protocol [33]. Dogbone shaped samples were mounted on aluminum
fixtures and placed in a QUV weatherometer (Q-LAB, LU-8047-TM,
USA) for 24 h. The samples were collected and dried in an oven at
105 ◦ C for 24 h. Their weight loss was calculated using Eq. (1):
Weight loss (%) = [(s1 − s2 )/s1 ] × 100
where s1 was initial weight and s2 was final weight after exposure in the
QUV weatherometer and drying in the oven. The weight loss of neat
starch biopolymer and the composite samples was obtained by
Algal Research 56 (2021) 102321
averaging the loss from six independently tested specimens.
The chemical structures of samples before and after accelerated
weathering were determined using Fourier transform infrared spec­
troscopy (FTIR) (BRUKER EQUINOX 55, Germany) in attenuated total
reflection (ATR) mode. The thin films were applied directly onto the
diamond ATR cell. The samples were then scanned in a frequency range
of 4000–600 cm− 1 with 512 consecutive scans at a 4 cm− 1 resolution.
The thermal decomposition temperatures of samples were obtained
using a thermogravimetric analyzer (TGA 7, Perkin Elmer, USA) oper­
ated at a heating rate of 10 ◦ C/min from 50 to 600 ◦ C using a nitrogen
atmosphere.
The data in this work were evaluated using Microsoft Excel statistics.
3. Results and discussion
3.1. Characterization of brown algae powder before milling (BA) and
after milling (MBA)
BA was dark brown (Fig.2(a)), which is the natural color of brown
algae due to the presence of xanthophyll, the major pigment. MBA was
light brown (Fig.2(b)). The change in the color of the particles after
milling is a known effect due to changes in the size and morphology of
particles [34,35]. The morphology and d50 of BA and MBA were then
investigated using SEM and laser particle size analysis, respectively.
SEM micrographs (Fig.2(c) and (d)) showed that there was a clear dif­
ference in the morphologies of the samples. BA particles were flat, with
(1)
smooth surfaces and a dense structure (Fig.2(c)). This morphology was a
result of the envelopment of cellulose-based fibrils in non-cellulosic
components such as hemicellulose, lignin and waxes [36]. In contrast,
MBA particles were angular with rough surfaces (Fig.2(d)) and the d50 of
3
S. Jantasrirad et al.
Fig. 3. Effect of MBA content and sonication time on the tensile strength (a) and elongation at break (b) of starch-based biocomposite (average ± standard errors, n
= 10) (MBA and S denoted milled brown algae powder and sonication time, respectively.).
Fig. 4. SEM micrographs at low (a) and high magnification (b) of biocomposite obtained from cassava starch mixed with 10 wt% of MBA and sonicated for 120 s
(MBA denoted milled brown algae powder.).
MBA (≈118.0 μm) was about 6 times smaller than the d50 of BA (≈808.6
μm). The changes in morphology and reduction in particle size produced
by planetary ball milling were correlated with the frictional and impact
forces, which broke cell walls into fragments [28,30]. The cellulose-
hemicellulose-lignin network, which is the main component of the cell
walls, was destroyed, resulting in particle defibrillation and opening of
fiber bundles. This morphological change exposed more hydroxyl
groups on the cellulose surface, which increased interaction between
MBA and the starch matrix [30,31]. The effects of MBA content (0, 10
and 20 wt%) and sonication time (60, 90 and 120 s) on the properties of
the starch/brown algae biocomposites were investigated.
3.2. Effect of milled brown algae powder (MBA) content and sonication
periods on the properties of starch-based biocomposite
The tensile strength of the neat starch biopolymer was 0.36 MPa
(Fig. 3(a)). The tensile strength of the starch-based biocomposite
increased to 0.67 MPa with the addition of 10 wt% of MBA. This result
was due to both the good dispersion of MBA particles in the starch
matrix and the strong hydrogen bonds between MBA particles and the
starch matrix, which transferred stress effectively from the starch matrix
4
Algal Research 56 (2021) 102321
to the MBA. However, tensile strength decreased to 0.40 MPa when the
MBA content was increased to 20 wt%. The reduction in tensile strength
can be explained by the occurrence of agglomerations, which impaired
the dispersion and adhesion of MBA in the composite, resulting in poor
transfer of stress from the starch matrix to the filler. In this work, 10 wt%
was the MBA loading that most improved tensile strength and so the
effect of sonication time on mechanical properties was studied using a
starch-based biocomposite with this filler content. Changes in the tensile
strength of this starch-based biocomposite were observed after soni­
cation for different times. The tensile strength of a biocomposite pro­
duced from a mixture sonicated for 60s was 1.30 MPa. Tensile strength
increased to 1.64 and 2.22 MPa, respectively, for biocomposites pro­
duced from mixtures sonicated for 90 and 120 s (Fig. 3(a)). These values
are about 1.94, 2.45 and 3.31 times greater than the tensile strength of a
biocomposite produced from the same formulation that was not soni­
cated (0.67 MPa). Sonication improved the homogeneity of the disper­
sion of MBA particles in the starch matrix and increased the
defibrillation of MBA. The subsequent closer proximity between MBA
particles and the starch matrix produced a large quantity of strong
hydrogen bonds. This conclusion is supported by the morphological
evidence of the SEM micrographs, at low (Fig. 4(a)) and high (Fig. 4(b))
S. Jantasrirad et al.
Fig. 5. Effect of MBA content and sonication periods on the weight loss of
starch-based biocomposite after accelerated weathering for 24 h (average ±
standard errors, n = 6) (MBA and S denoted milled brown algae powder and
sonication time, respectively.).
magnification, of the starch-based biocomposite with 10 wt% of MBA
produced after sonicating the mixture for 120 s. MBA particles were well
dispersed and embedded in the starch matrix and no pullout of MBA
particles was apparent in the fracture surface. Therefore, the adhesion
between MBA particles and starch matrix was good.
The elongation at break of the neat starch biopolymer was 158%
(Fig. 3(b)). Elongation at break was considerably lower at an MBA
loading of 10 wt% and lower again at 20 wt%. The rigidity of the MBA
filler restrained the flexibility of the starch molecular chains, a behavior
widely reported in the literature [37]. The effect of sonication time on
the elongation at break was then investigated using the starch-based
biocomposite with 10 wt% of MBA. The % elongation at break
decreased with increments of sonication time, but the differences were
not significant (Fig. 3(b)).
The 24 h accelerated weathering test subjected the starch-based
biocomposite to electronically controlled cycles of simulated condi­
tions, which included certain levels of UV irradiation, temperature and
moisture. The repeated weathering cycles caused the scission of starch
molecular chains. The weight loss of the starch-based biocomposite
varied considerably depending on the loading of MBA and the sonication
time (Fig. 5). Among all samples, the neat starch biopolymer presented
the greatest weight loss, which was 51.40%. This sample was considered
extremely degraded. The weight loss of the biocomposite of starch
mixed with 10 wt% MBA was 38.70%. These results confirmed that 10
wt% was the optimum content that produced good adhesion between
MBA and the starch matrix. Good adhesion between MBA particles and
the starch matrix can slow down deterioration of polymer composites
caused by photo-degradation and hydrolytic degradation during
weathering [38]. At a loading of 20 wt% MBA, weight loss slightly
increased to 45.00% but was still lower than the weight loss of the neat
starch biopolymer. This suggests that MBA was able to act as an anti­
oxidant to protect the starch matrix from degradation during the
weathering process. This phenomenon was proposed by Ganapathi et al.
[21], who reported that Sargassum presented good antioxidant capac­
ities and could be a rich source of natural antioxidants. Mixture soni­
cation time had a clear effect on the resistance to degradation of the
obtained biocomposites. Weight loss decreased markedly with in­
crements of sonication time. At the MBA content of 10 wt%, the weight
loss of biocomposites obtained from mixtures sonicated for 60, 90 and
120 s was 37.76%, 32.18% and 20.65%, respectively. It has been
5
Algal Research 56 (2021) 102321
Fig. 6. FTIR spectra of neat starch biopolymer (0% MBA) and biocomposite
from starch mixed with 10 wt% of MBA and sonicated for 120 s (10%MBA/
120S) before ( ) and after ( ) accelerated weathering testing for 24 h (MBA
and S denoted milled brown algae powder and sonication time, respectively.)
reported that sonication encourages the dispersion and adhesion of MBA
particles in the starch matrix and this claim was supported by the SEM
micrographs (Fig. 4), that revealed a compact structure and absence of
defects such as micro- and nano-sized cracks [27]. This morphology
could effectively delay photo-degradation and hydrolytic degradation
during weathering.
After the 24 h accelerated weathering test, samples were analyzed by
FTIR spectroscopy to investigate changes in the chemical structure of the
neat starch biopolymer and the various biocomposites and to assess the
interaction between MBA particles and the starch matrix. The FTIR
spectrum of the neat starch biopolymer (0% MBA), before the acceler­
ated weathering test, exhibited main peak positions in the ranges of
3300–3200 cm− 1, 2900–2800 cm− 1 and 1190–950 cm− 1, that repre­
sented O–H stretching, C–H stretching and C–O stretching, respec­
tively (Fig. 6). Since the main component of MBA is cellulose, which has
similar chemical structures to starch [21,29], the spectrum of 10%MBA/
120S showed the same features in nearly the same positions as the
spectrum of the neat starch biopolymer. There were, however, two new
peaks in the FTIR spectrum of 10%MBA/120S, at 1730 cm− 1 and 1252
cm− 1. These peaks were respectively attributed to the C– – O stretching
vibration of the carbonyl and acetyl groups in the xylan component of
hemicelluloses and lignin and to – – C–O–, which is present in ether,
ester, and phenol groups [29,36,39,40]. Importantly, the peak at the
O–H stretching band in the FTIR spectrum of 10%MBA/120S appeared
at a lower wavenumber (3281 cm− 1) than it appeared at in the spectrum
of neat starch biopolymer (3297 cm− 1). This result is good evidence for
the formation of hydrogen bonds between MBA particles and the starch
matrix [22]. After accelerated weathering, the peak at the O–H
stretching band in the FTIR spectrum of neat starch biopolymer
exhibited increased intensity and a strong, new peak appeared at around
1662 cm− 1, which was attributed to OH bending of absorbed water
during the degradation process [38]. In the FTIR spectrum of 10%MBA/
120S, the intensity of the peak at 1252 cm− 1 was greatly reduced after
the accelerated weathering test. This result confirmed that hemicellu­
lose and other small molecules in the MBA structure were partially
degraded [38]. Peng et al. [36] reported that some products of the
degradation of lignocellulosic materials had antioxidant effects.
S. Jantasrirad et al.
Fig. 7. TGA curves of neat starch biopolymer (0% MBA), 10%MBA and 10%
MBA/120S (MBA and S denoted milled brown algae powder and sonication
time, respectively.)
The thermal properties of 0% MBA, 10%MBA and 10%MBA/120S
were investigated from the onset of the decomposition temperature and
the percentage weight loss was evaluated using TGA. TGA curves (Fig.7)
showed that degradation of 0% MBA, 10%MBA and 10%MBA/120S
occurred in two steps of weight loss. The first step occurred from 100 ◦ C
to 250 ◦ C and was attributed to water and glycerol evaporation. In this
step, the onset of the decomposition temperature and the percentage
weight loss of 0% MBA and 10%MBA/120S were similar but the per­
centage weight loss of 10%MBA was higher due to the free hydroxyl
groups in its structure, which could react easily with water molecules. A
more significant change in the percentage weight loss occurred in the
second step, which involved the decomposition of the starch matrix and
polysaccharides in the MBA structure [22,36]. In the second step, there
are differences in the onset of decomposition temperature and per­
centage weight loss between 0% MBA and the biocomposites. The onset
temperature of decomposition of 0% MBA in the second step was about
270 ◦ C, while the onset temperature of decomposition for 10%MBA and
10%MBA/120S occurred at around 230 ◦ C and 240 ◦ C, respectively.
These lower onset temperatures resulted from the decomposition not
only of cellulose and the starch matrix but also of hemicellulose and
other organic components of MBA. The decomposition of the neat starch
biopolymer (0% MBA) involved only the decomposition of the starch
matrix [22]. Moreover, the percentage weight loss of 10%MBA (75%)
and 10%MBA/120S (70%) in this second step were lower than the
percentage weight loss of 0% MBA (80%). The thermal stability of 10%
MBA/120S was highest due to the sonication producing a more compact
microstructure and improved thermal resistance due to the better
dispersion of filler and better interfacial bonding between filler and
polymer matrix [41].
4. Conclusions
The mechanical and thermal properties of a starch-based bio­
composite were successfully improved by the addition 10 wt% of milled
brown algae powder to the mixture and sonication of the mixture for
120 s. Moreover, milled brown algae powder could delay the degrada­
tion process of the starch-based biocomposite. The optimum loading of
milled brown algae powder was 10 wt% of starch. This loading dispersed
well in the starch matrix and sonication for 120 s brought about a ho­
mogeneous dispersion of filler particles in the starch matrix and greater
6
Algal Research 56 (2021) 102321
defibrillation of the milled brown algae particles. A developed bio­
composite prepared from a mixture of starch and 10 wt% milled brown
algae powder that was sonicated for 120 s had promising properties and
could prove to be an alternative material to traditional synthetic plastic.
Statement of informed contest, human/animal rights
No conflicts, informed consent, or human or animal rights are
applicable to this study.
CRediT authorship contribution statement
Supichchayapak Jantasrirad: Conceptualization, Methodology,
Validation, Formal analysis, Investigation. Jaruwan Mayakun: Meth­
odology, Writing – review & editing. Apon Numnuam: Methodology,
Investigation. Kaewta Kaewtatip: Conceptualization, Methodology,
Validation, Formal analysis, Resources, Writing – review & editing,
Visualization, Supervision.
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.
Acknowledgements
The authors would like to thank the Faculty of Science and Prince of
Songkla University, Thailand for financial support (SCI6405078S) and
Siam Modified Starch Co. Ltd., Thailand, for supplying their pre-
gelatinized cassava starch. Thanks also to Mr. Thomas Duncan Coyne
for assistance with the English text.
References
[1] Y. Fang, J. Fu, C. Tao, P. Liu, B. Cui, Mechanical properties and antibacterial
activities of novel starch-based composite films incorporated with salicylic acid,
Int. J. Biol. Macromol. 155 (2020) 1350–1358.
[2] W. Cheng, Preparation and properties of lignocellulosic fiber/CaCO3/thermoplastic
starch composites, Carbohydr. Polym. 211 (2019) 204–208.
[3] C. Chiarathanakrit, J. Mayakun, A. Prathep, K. Kaewtatip, Comparison of the
effects of calcified green macroalga (Halimeda macroloba Decaisne) and
commercial CaCO3 on the properties of composite starch foam trays, Int. J. Biol.
Macromol. 121 (2019) 71–76.
[4] S.A. Riyajan, K. Chantawee, Cassava starch composite based films for encapsulated
neem: effect of carboxylated styrene-butadiene rubber coating, Food Packag. Shelf
Life 23 (2020), 100438.
[5] K. Wilpiszewska, A.K. Antosik, T. Spychaj, Novel hydrophilic carboxymethyl
starch/montmorillonite nanocomposite films, Carbohydr. Polym. 128 (2015)
82–89.
[6] K. González, L. Iturriaga, A. González, A. Eceiza, N. Gabilondo, Improving
mechanical and barrier properties of thermoplastic starch and
polysaccharidenanocrystals nanocomposites, Eur. Polym. J. 123 (2020), 109415.
[7] K. Hanieh, J. Nurain, A. Ishak, Starch biocomposite film reinforced by multiscale
rice husk fiber, Compos. Sci. Technol. 151 (2017) 147–155.
[8] M. Prabhakar, J. Song, Fabrication and characterisation of starch/chitosan/flax
fabric green flame-retardant composites, Int. J. Biol. Macromol. 119 (2018)
1335–13343.
[9] S.A. de Oliveira, J.R. de Macedo, D.S. Rosa, Eco-efficiency of poly (lactic acid)-
starch-cotton composite with high natural cotton fiber content: environmental and
functional value, J. Clean. Prod. 217 (2019) 32–41.
[10] K. Kaewtatip, J. Thongmee, Preparation of thermoplastic starch/treated bagasse
fiber composites, Starch - Stärke 66 (2014) 724–728.
[11] S. Collazo-Bigliardi, R. Ortega-Toro, A. Chiralt, Improving properties of
thermoplastic starch films by incorporating active extracts and cellulose fibres
isolated from rice or coffee husk, Food Packag. Shelf Life 22 (2019), 100383.
[12] C. Zhang, F. Li, J. Li, L. Wang, Q. Xie, J. Xu, S. Chen, A new biodegradable
composite with open cell by combining modified starch and plant fibers, Mater.
Des. 120 (2017) 222–229.
[13] V. Stiger, T. Horiguchi, T. Yoshida, A. Coleman, M. Masuda, Phylogenetic
relationships of Sargassum (Sargassaceae, Phaeophyceae) with reference to a
taxonomic revision of the section Phyllocystae based on ITS-2 nrDNA sequences,
Phycol. Res. 48 (2000) 251–260.
[14] T. Noiraksa, T. Ajisaka, C. Kaewsuralikhit, Species of Sargassum in the East Coast of
the Gulf of Thailand, ScienceAsia. 32 (2006) 99–106.
S. Jantasrirad et al.
[15] J. Praiboon, S. Palakas, T. Noiraksa, K. Miyashita, Seasonal variation in nutritional
composition and anti-proliferative activity of brown seaweed, Sargassum
oligocystum, J. Appl. Phycol. 30 (2018) 101–111.
[16] M. Asker, E. El-Sheikh, Chemical structure and antiviral activity of water-soluble
sulfated polysaccharides from Surgassum latifolium, J. Appl. Sci. Res. 3 (2007)
1178–1185.
[17] A. Tanniou, L. Vandanjon, M. Incera, E. Leon, V. Husa, J. Le, J. Nicolas, N. Poupart,
N. Kervarec, A. Engelen, R. Walsh, F. Guerard, N. Bourgougnon, V. Pouvreau,
Assessment of the spatial variability of phenolic contents and associated
bioactivities in the invasive alga Sargassum muticum sampled along its European
range from Norway to Portugal, J. Appl. Phycol. 26 (2013) 1215–1230.
[18] C. Okumura, O. Miki, Y. Sakamoto, T. Fukami, Toxicological study for phenol using
germling growth of the brown macroalga Sargassum horneri, J. Appl. Phycol. 30
(2018) 2083–2090.
[19] Y. Li, X. Fu, D. Duan, J. Xu, X. Gao, Comparison study of bioactive substances and
nutritional components of brown algae Sargassum fusiforme strains with different
vesicle shapes, J. Appl. Phycol. 30 (2018) 3271–3283.
[20] W. Chotigeat, S. Tongsupa, K. Supamataya, A. Phongdara, Effect of Fucoidan on
disease resistance of black tiger shrimp, Aquaculture 233 (2004) 23–30.
[21] K. Ganapathi, V. Subramanian, S. Mathan, Bioactive potentials of brown sea weeds,
Sargassummyriocystum J. Agardh S. Plagiophyllum C. Agardh and S.Ilicfolium
(Turner), J. Agardh, Int. Res. J. Pharm. App. Sci. 3 (2013) 105–111.
[22] R. Jumaidin, S.M. Sapuan, M. Jawaid, M.R. Ishak, J. Sahari, Thermal, mechanical,
and physical properties of seaweed/sugar palm fibre reinforced thermoplastic
sugar palm starch/agar hybrid composites, Int. J. Biol. Macromol. 97 (2017)
606–615.
[23] M. Fabra, M. Martinez-Sanz, L. Gomez-Mascaraque, R. Gavara, A. Lopez-Rubio,
Structural and physicochemical characterization of thermoplastic corn starch films
containing microalgae, Carbohydr. Polym. 186 (2018) 184–191.
[24] M. Carissimi, S. Flôres, R. Rech, Effect of microalgae addition on active
biodegradable starch film, Algal Res. 32 (2018) 201–209.
[25] H. Doh, K. Dunno, W. Whiteside, Cellulose nanocrystal effects on the
biodegradability with alginate and crude seaweed extract nanocomposite films,
Food Biosci. 38 (2020), 100795.
[26] Z. Davarpanah, J. Keramat, N. Hamdami, M. Shahedi, T. Behzad, Dispersion of
silicate layers in Zein/Montmorillonite composite films using two sonication
methods, J. Agric. Sci. Technol. 18 (2016) 1523–15230.
[27] S. Tuntachon, A. Sukolrat, A. Numnuam, K. Kaewtatip, Effect of kaolin content and
sonication on the properties of wheat gluten composites, Powder Technol. 351
(2019) 66–70.
Algal Research 56 (2021) 102321
[28] T. Sundum, K.M. Szecsenyi, K. Kaewtatip, Preparation and characterization of
thermoplastic starch composites with fly ash modified by planetary ball milling,
Carbohydr. Polym. 191 (2018) 198–204.
[29] W. Chen, H. Yu, Y. Liu, P. Chen, M. Zhang, Y. Hai, Individualization of cellulose
nanofibers from wood using high-intensity ultrasonication combined with
chemical pretreatments, Carbohydr. Polym. 83 (2011) 1804–1811.
[30] M. Nuruddin, M. Hosur, M. Uddin, D. Baah, S. Jeelani, A novel approach for
extracting cellulose nanofibers from lignocellulosic biomass by ball milling
combined with chemical treatment, J. Appl. Polym. Sci. 133 (2016) 42990.
[31] R.R. Ferreira, A.G. Souza, L.L. Nunes, N. Shahi, V.K. Rangari, D. Rosa, Use of ball
mill to prepare nanocellulose from eucalyptus biomass: challenges and process
optimization by combined method, Mater. Today Commun. 22 (2020), 100755.
[32] ASTM D412-98a, Standard Test Methods for Vulcanized Rubber and Thermoplastic
Elastomers-Tension, ASTM International, West, Conshohocken, PA, 2003.
[33] ASTM G154, Standard Practice for Operating Fluorescent Ultraviolet (UV) Lamp
Apparatus for Exposure of Nonmetallic Materials, ASTM International, West
Conshohocken, PA, 2016.
[34] K. Ramachandraiah, K.B. Chin, Evaluation of ball-milling time on the
physicochemical and antioxidant properties of persimmon by-products powder,
Innov. Food Sci. Emerg. 37 (2016) 115–124.
[35] K. Liu, Effects of particle size distribution, compositional and color properties of
ground corn on quality of distillers dried grains with solubles (DDGS), Bioresour.
Technol. 100 (2009) 4433–4440.
[36] Y.W. Chen, H.V. Lee, J.C. Juan, S.M. Phang, Production of new cellulose
nanomaterial from red algae marine biomass Gelidium elegans, Carbohydr. Polym.
151 (2016) 1210–1219.
[37] L. Dai, C. Qiu, L. Xiong, Q. Sun, Characterisation of corn starch-based films
reinforced with taro starch nanoparticles, Food Chem. 174 (2015) 82–88.
[38] Y. Peng, R. Liu, J. Cao, Characterization of surface chemistry and crystallization
behavior of polypropylene composites reinforced with wood flour, cellulose, and
lignin during accelerated weathering, Appl. Surf. Sci. 332 (2015) 253–259.
[39] S. Kannan, FT-IR and EDS analysis of the seaweeds Sargassum wightii (brown algae)
and Gracilaria corticata (red algae), Int. J. Curr. Microbiol. App. Sci. 3 (2014)
341–351.
[40] D. Martins, A. de Souza, M. Henrique, H. Silvério, W. Flauzino, D. Pasquini, The
influence of the cellulose hydrolysis process on the structure of cellulose
nanocrystals extracted from Capim mombaça (Panicum maximum), Ind. Crop.
Prod. 65 (2015) 496–505.
[41] M. Asrofi, H. Abral, Y.K. Putra, S.M. Sapuan, H.J. Kim, Effect of duration of
sonication during gelatinization on properties of tapioca starch water hyacinth
fiber biocomposite, Int. J. Biol. Macromol. 108 (2018) 167–176.