Carbohydrate Polymer Technologies and Applications 2 (2021) 100167

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Carbohydrate Polymer Technologies and Applications

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carbohydrate-polymer-technologies-and-applications

Effects of the addition of cotton fibers and cotton microfibers on the

structure and mechanical properties of starch foams made from
potato starch
Bruno Felipe Bergel *, Ludmila Leite Araujo, Ruth Marlene Campomanes Santana
Polymeric Materials Lab, Materials Engineering Department, Federal University of Rio Grande do Sul, Av. Bento Gonçalves, 9500, P.O. Box 15090, ZC, Porto Alegre, RS
91501-970, Brazil

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

Keywords: Foams from thermoplastic starch (TPS) are interesting options to replace single-use packaging made with non-
TPS foam biodegradable polymers derived from fossil fuels. These foams are made with materials from renewable and
Starch biodegradable sources, which do not harm the environment. However, this material has poor mechanical
Cotton
properties and breaks easily when handled. Adding natural fibers, such as cotton, is an easy option that can
Cotton microfiber
Chemical treatment
generate foams that are more resistant to impact and handling. In this work, the incorporation of cotton fibers
into starch foams was studied. Two types of fiber were used: cotton fiber and cotton microfiber. In addition, three
fiber contents were evaluated: 0.67%, 2.00% and 3.33%. The results showed that both cotton types showed great
compatibility and homogeneity with starch and both significantly improved the mechanical properties of the
foams. Foams with a greater amount of cotton fibers (2.00% and 3.33%) showed the best results for impact and
tensile tests.

1. Introduction Tucker & Parker, 2019; Soykeabkaew, Thanomsilp & Suwantong,

Recently, several organizations have concentrated their efforts on
replacing packaging based on non-biodegradable polymers derived from
petroleum with packaging based on biodegradable polymers derived
from renewable sources. These efforts are in line with a policy of caring
for the environment, a policy that has grown in recent years. As plastic
packages derived from petroleum-based polymers negatively affect the
environment, replacement is required (Clemente, Paresque & Santos,
2018; Compa et al., 2019; Dikareva & Simon, 2019; Jepsen & de Bruyn,
2019; Menicagli, Balestri, Vallerini, Castelli & Lardicci, 2019). Among
the materials that can be used in disposable biodegradable packaging,
thermoplastic starch foams (TPS) stand out. These foams are easily
produced and processed by extrusion, compression and injection using
only water as the blowing agent. Foams made by compression can easily
form products such as cups and trays, as the foam is shaped like the
mold. Despite these great advantages, TPS foams also present serious
problems. These foams are generally fragile and have poor mechanical
properties. They also have high water absorption, which causes the
material to collapse and disintegrate when in contact with water (Glenn,
Orts & Nobes, 2001; Hassan, Tucker & Le Guen, 2020; Hassan, Le Guen,
2015).
The water absorption of the foams can be improved by hydrophobic
coatings or by chemical modification of the starch (Bergel, Dias Osorio,
da Luz & Santana, 2018; Bergel, da Luz & Santana, 2017, 2018; Bergel,
Araujo, dos Santos da Silva, & Santana, 2020). The mechanical prop­
erties can be greatly improved by the incorporation of hydrophilic fi­
bers. The mixture of starch with other more flexible and resistant
biodegradable polymers leads to the improvement of the mechanical
properties of TPS foams and does not alter the biodegradability of the
material, providing environmentally compatible solutions for waste
disposal (Bergeret & Benezet, 2011; Lopez-Gil, Silva-Bellucci, Velasco,
Ardanuy & Rodriguez-Perez, 2015; Machado, Benelli & Tessaro, 2017,
2020; Xie et al., 2018). Bénézet, Stanojlovic-Davidovic, Bergeret, Ferry
& Crespy (2012) produced starch foams with several natural fibers
(wheat straw, cellulose and hemp) by extrusion and the products ob­
tained showed improvements in the mechanical properties (flexural
test) compared to the foams without reinforcement. Among the fibers
that can be used, cotton has several advantages such as wide availability,
low cost, renewable, abundant, strong, resistant, durable and biode­
gradable. In addition, it has great compatibility with starch in composite

* Corresponding author.
E-mail address: bruno-bergel@hotmail.com (B.F. Bergel).

https://doi.org/10.1016/j.carpta.2021.100167
Received 28 April 2021; Received in revised form 7 September 2021; Accepted 24 September 2021
Available online 25 September 2021
2666-8939/© 2021 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND license
(http://creativecommons.org/licenses/by-nc-nd/4.0/).
B.F. Bergel et al.
materials. Sanhawong, Banhalee, Boonsang & Kaewpirom (2017)
incorporated cotton fibers into foams containing starch and reported
that the addition of cotton improved the mechanical properties of the
foams and also slightly decreased their moisture absorption.
Cotton has long fibers and can present low dispersion in starch pastes
and consequently form foams with more concentrated areas of cotton
(Sanhawong et al., 2017). This problem can be solved through a
chemical treatment on cotton with the objective of forming cellulose
microfibers. Acid hydrolysis is the most common method used for the
production of cellulose microfibers. First, the cotton undergoes a basic
hydrolysis, in order to purify the cellulose present, eliminating impu­
rities (mainly proteins). After this process, the product is placed in
contact with a strong acid (usually sulfuric acid) to occur the acid hy­
drolysis (Morais et al., 2013; Theivasanthi, Anne Christma, Toyin,
Gopinath & Ravichandran, 2018). The use of cellulose microfibers in
several types of materials has been gaining interest in recent years. They
can be used as reinforcements for adhesives, electronic device compo­
nents, biomaterials, foams, airgel and in the textile industry. These
microfibers have also been used in polymeric composites because they
have interesting mechanical properties, such as low gas permeability
and ability to increase stiffness, in addition to having good dispersion
through the matrix (Capadona et al., 2009; Eichhorn et al., 2010; Stelte
& Sanadi, 2009). Capadona et al. (2009) used cellulose microfibers to
reinforce composites and reported that the addition of cellulose micro­
fibers from cotton increased the mechanical strength of the composites.
The main hypothesis of the work is, taking into account the great
compatibility between cotton and starch, that cotton can significantly
improve the mechanical properties of starch foams. So these foams can
be used as packaging. Although starch foams with cotton fibers have
already been studied (mainly when compared to other fibers or as a basis
for incorporating another component), mainly made with natural fiber
or physically modified (fiber cutting) (Kaisangsri, Kerdchoechuen &
Laohakunjit, 2012; Sanhawong et al., 2017), this study is relevant and
unprecedented for presenting a comparison between foams with natural
fiber and with microfibers obtained by chemical treatment. This topic,
the comparison between long and short cotton fibers in starch foams, is
relevant to advancing research on starch foams.
In this way, the objective of this work was to evaluate the incorpo­
ration of cotton fibers and microfibers in the structure and properties of
TPS foams; and identifying the type and fiber content that most
improved the mechanical properties of TPS foams. All foams were pro­
duced using the compression method.
2. Materials and methods
2.1. Materials
Potato starch (Giro Verde ®) and cotton (Apolo ®) (99% of cellulose
and 73% of crystallinity) were purchased at a local market in Porto
Alegre, Brazil. Sodium hydroxide (Neon ®) and sulfuric acid (Neon ®)
were used to produce the cotton microfibers. Polyvinyl alcohol (PVOH)
(Neon ®) was used as a plasticizer in the preparation of the starch paste.
2.2. Preparation of cellulose microfibers
Acid hydrolysis is the most used method to break down cellulose
fibers and form microfibers. 20 g of cotton were added in a beaker of
250 mL. Afterwards, a solution of 1 mol/L of NaOH was added to the
beaker until the cotton was completely submerged. After 4 h, the cotton
was removed from the solution, washed several times (until the pH was
between 6 and 7) and placed in an oven at 60 ◦ C for 24 h. The cotton was
then placed in a 6.22 mol/L solution of H2SO4. The solution was heated
to 40◦ C and stirred constantly for about 4 h. After this period, the cotton
was removed and washed several times until the pH was neutral. The
final product was dried in an oven for 24 h at 100 ◦ C. The methodology
was based on the work of Theivasanthi et al. (2018).
2
Carbohydrate Polymer Technologies and Applications 2 (2021) 100167
2.3. Preparation of TPS foams with cotton
Starch pastes were prepared from a mixture of PVOH, water, starch
and cotton. A portion of the starch was gelatinized beforehand as a way
to assist in the dispersion of all components in the paste, keeping the
solid components homogeneous and with adequate viscosity. The
gelatinized starch was made with 20 g of starch and 100 ml of water at
70 ◦ C. Starch gelatinized in approximately 3 min. Afterwards, dry starch
and PVOH plasticizer diluted in water were added. After a first ho­
mogenization, cotton was added little by little. After adding the cotton,
the pastes were mixed and homogenized with the aid of a mechanical
stirrer. Then, the obtained pastes were placed in a mold preheated to
180 ◦ C and compressed in a 2.5 ton hydraulic press for 240 s. The mold
used has the following dimensions: 15 cm × 15 cm × 0.3 cm. All foams
used for the following experiments filled the mold completely. Foams
that did not fill the mold completely were discarded. The analyzed foams
were kept at room temperature in a desiccator. Table 1 shows the
formulation of the analyzed foams. The parameters used for this work
were previously evaluated in previous works and the proportions used of
starch, water and PVA were those that formed foams with the most
adequate properties (Bergel et al., 2017, 2018).
2.4. Characterization of TPS foams with cotton
2.4.1. Scanning electron microscopy
The morphology of natural cotton, cotton microfibers and TPS foams
was studied through SEM analysis of the foams cross section using a
JEOL microscope, model JSM 6060 operating at an acceleration voltage
of 5 kV. The samples were metallized with a thin layer of gold. The
average cell size of the analyzed TPS foams and cell density (number of
cells per volume unit) were obtained using the ImageJ software. Cell
density was calculated using Eq. (1):
( 2 )3/2 ( )
nM 1
Nf = . (1)
A 1 − Vf
Where Vf is the empty content, Nf is the cell density (cells/cm3), n is the
number of cells in the micrograph, A is the area of the micrograph (cm2)
and M is the magnification of the image. This method was based on the
work developed by Zimmermann, Da Silva, Zattera & Santana, (2017).
2.4.2. Density
The apparent density of the foams was calculated by dividing the
masses by the volumes of the foams, in triplicate for each sample
(Shogren, Lawton, Doane & Tiefenbacher, 1998). The dimensions of the
length, width and thickness of the test bodies were made in triplicate for
each foam.
2.4.3. Water absorption
Samples of TPS foam with cotton fibers measuring 4 cm × 2 cm were
weighed and placed in distilled water for 5 min. After the passage of
time, the samples were removed from the water (the excess water was
removed) and weighed again. The amount of water absorbed was
calculated gravimetrically. This method was based on the work devel­
oped by Vercelheze et al., (2012).
2.4.4. Mechanical properties
The mechanical tests used in this step were tensile test, flexural test
and IZOD impact test. The tensile test was carried out according to
ASTM D638 method with a test speed of 3 mm/min in an INSTRON
universal testing machine, model 3382. The dimensions of the samples
tested (TPS foams) were 100 mm × 25 mm × 3 mm. From the stress
versus strain curves, the parameters of maximum stress at break (σ),
Young’s modulus (E) and deformation at break (Ԑb) were determined.
The results obtained are the test average of at least 5 independent
specimens for each formulation.
B.F. Bergel et al. Carbohydrate Polymer Technologies and Applications 2 (2021) 100167

Table 1
Formulation of the evaluated foams.
Sample Dry Starch (g) Gel. Starch (g) PVOH (g) Water (mL) Cotton Fibers (g) Cotton Microfibers (g) Proportion of cotton fibers in paste (%)

TPS 47 47 6 50 0 0 0
TPS-1C 46 47 6 50 1 0 0.67
TPS-3C 44 47 6 50 3 0 2.00
TPS-5C 42 47 6 50 5 0 3.33
TPS-1MC 46 47 6 50 0 1 0.67
TPS-3MC 44 47 6 50 0 3 2.00
TPS-5MC 42 47 6 50 0 5 3.33

The flexural test was also performed on an INSTRON ® universal
testing machine, model 3382 (USA). The test was performed according
to ASTM D790 method with a test speed of 1 mm/min. The dimensions
of the samples were 100 mm × 25 mm × 3 mm. The results obtained are
the test average of at least five independent specimens for each
formulation.
The IZOD impact resistance test was performed following the ASTM
D256 method on an CEAST ® machine, model IMPACTOR II (USA),
using a 0.5 J hammer. The sample dimensions were 60 mm × 12 mm ×
3 mm and the results obtained were the test average of nine independent
samples.
For a better understanding of the properties of the foams analyzed in
this work, the same tests were carried out for samples of commercial
expanded polystyrene (EPS) trays. The comparison between TPS and
EPS foams was made to assess whether TPS foams have the necessary
requirements to be used as packaging.
2.5. Statistical analysis
Analysis of Variance (ANOVA) were performed using commercial
software. Single-factor ANOVA and Tukey’s test were used to verify
statistical differences between groups with 95% confidence in the results
of density, water absorption, tensile, flexure and impact tests.
3. Results and discussions
3.1. Morphology of TPS foams with cotton
Fig. 1 shows the SEM images of normal cotton fibers and cotton fibers
after chemical treatment (cotton microfibers). It can be seen that the
chemical treatment has considerably modified the cotton fibers, making
them smaller and shorter. Natural cotton fibers are much longer (above
500 µm) compared to cotton microfibers (below 200 µm). These shorter
fibers can assist in the formation of more homogeneous composites. The
shape of the treated cotton fibers also indicates an increase in their
specific area. This increase favors the interaction of these fibers with the
polymeric starch matrix. It can also favor chemical reactions in cotton
fibers.
Fig. 2 shows SEM images of TPS-1C, TPS-3C and TPS-5C foams
(containing natural cotton) and TPS-1MCF, TPS-3MCF and TPS-5MCF
foams (containing chemically treated cotton). As can be seen, the
foams maintained a sandwich-like structure, with a thicker outer layer
and a more expanded internal structure (Matsuda, Verceheze, Carvalho,
Yamashita & Mali, 2013; Sanhawong et al., 2017; Vercelheze et al.,
2012). Foams with a greater amount of cotton fibers (TPS-3C and
TPS-5C) showed denser structures and less porosity. The TPS-5C foam
has the densest structure among the analyzed foams, showing little
expanded and small cells. It is also possible to notice the great presence
of fibers in the polymeric matrix of this foam. This more compact
structure is due to the increase in viscosity of the starch paste when
greater amounts of cotton are added to this paste. Cotton fibers decrease
the mobility of starch chains via hydrogen bonding, resulting in high
viscosity and consequently low expansion.
Separations between the cotton fibers and the polymeric matrix were
not observed, confirming the good compatibility and the strong inter­
action between starch and cotton (Bénézet et al., 2012; Bergeret &
Benezet, 2011; Pornsuksomboon, Holló, Szécsényi & Kaewtatip, 2016;
Prachayawarakorn, Sangnitidej & Boonpasith, 2010; Sanhawong et al.,
2017). Foams containing cotton microfibers also showed sandwich-like
structures, but exhibited greater expansion compared to foams with
cotton fibers. Although microfibers also increase the viscosity of starch
pastes (for the same reasons mentioned previously), the viscosity is not
as high as foams with normal cotton because these fibers are smaller and
shorter and consequently do not decrease the mobility of the chains as
much as normal cotton fibers (longer). Microfibers can also act as
nucleating agents, favoring the creation of vapor bubbles during the
foaming process (Capadona et al., 2009; Matsuda et al., 2013; Soy­
keabkaew et al., 2015; Theivasanthi et al., 2018). Bénézet et al., (2012)
explains that fibers can act as nucleating agents, providing surfaces for
cell growth and, therefore, increasing expansion and porosity.
Table 2 shows the average cell area and the cell density of the
analyzed foams. The results show that the addition of cotton decreased

Fig. 1. SEM images of cotton fibers (A) and cotton microfibers (B), after the cotton undergoes chemical treatment.

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B.F. Bergel et al. Carbohydrate Polymer Technologies and Applications 2 (2021) 100167

Fig. 2. SEM images of TPS foams with cotton (TPS-C) and cotton microfibers (TPS-MC).

the average cell area and increased the cell density of the starch foams.
This is an indication that foams containing cotton have smaller cells and
more cells scattered through the foams. The TPS foam without cotton,
due to the lower viscosity of the paste, has larger cells and these during
processing tend to swallow the smaller cells, consequently decreasing
the cell density. Foams containing cotton, on the other hand, due to their
higher viscosity, tend to form smaller cells and they are unable to
swallow nearby cells. Consequently, the cell density is higher. These
results confirm the visual analysis made previously. It can be noted that
the average area of TPS-MC foams is larger compared to the average area

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B.F. Bergel et al. Carbohydrate Polymer Technologies and Applications 2 (2021) 100167

Table 2 formulation. Thus, the cells formed during this process tend to be more
Density, cell area and cell density of the evaluated foams. irregular and with different sizes. TPS foams made by the compression
Samples Density (g/cm3) Average cell area Cell density(cell/cm3 method usually have cells of different sizes, because an outer layer with
(mm2) x108) small cells and an inner layer with large cells are formed (Soykeabkaew
TPS 0.1428 ± 0.2687 4.19 et al., 2015).
0.0051a
TPS-1C 0.1503 ± 0.2195 6.34
0.0067ab 3.2. Density of TPS foams with cotton
TPS-3C 0.2026 ± 0.1237 8.19
0.0117c Table 2 also shows the densities of TPS foams with cotton fibers and
TPS-5C 0.2309 ± 0.1125 18.52 TPS foams with cotton microfibers. It can be noted that with the addition
0.0031d
of the fibers, the density of the foams increased. The increase in density
TPS- 0.1493 ± 0.2390 6.84
1MC 0.0009a is a trend when adding fillers in TPS foams (Glenn et al., 2001; Lopez-Gil
TPS- 0.1522 ± 0.2580 6.71 et al., 2015; Machado et al., 2017; Mello & Mali, 2014; Sanhawong et al.,
3MC 0.0091ab 2017; Shey et al., 2006). Foams with normal cotton showed higher
TPS- 0.1679 ± 0.2435 6.41
densities compared to foams with cotton microfibers, with the highest
5MC 0.0121b
density being achieved by TPS-5C foam (0.23 g/cm3).
Different letters in the same column indicate significant differences (p ≤ 0.05) Starch pastes containing 3 g and 5 g of cotton fibers showed high
between means (Tukey’s test). viscosity, and therefore during processing they did not expand as much
as foam with cotton microfibers. Consequently, the resulting foams
of TPS-C foams. This is explained by the lower viscosity of pastes con­ became more dense. Cotton fibers tend to make the starch paste more
taining microfibers and the fact that these microfibers can act as viscous, as these fibers are long and have great compatibility with
nucleating agents, which help to form larger cells. starch. Microfibers, on the other hand, are short, do not increase the
Fig. 3 shows the EPS structure of a commercial food tray. It can be viscosity of the starch paste so much, and so during processing tend to
seen that the structure of these foams has uniform cells well distributed expand more (Lawton, Shogren & Tiefenbacher, 2004; Mello & Mali,
throughout the material (Cronin & Ouellet, 2016; Zhang, Zhu, Li & Lee, 2014; Pornsuksomboon et al., 2016; Pornsuksomboon, Szécsényi, Holló
2012). Unlike TPS foams that have an outer layer (smaller cells) and a & Kaewtatip, 2014; Sanhawong et al., 2017; Shogren, Lawton & Tie­
distinct inner layer (larger cells), EPS is uniform throughout its structure fenbacher, 2002). EPS has a density of 0.06 g/cm3, which makes this
and has only a thin outer layer. EPS presented cells with an average area material extremely desirable for packaging such as trays (Glenn et al.,
of 0.15 mm2 and cell density of 1.57 × 109 cells/cm3. This result shows 2001; Glenn & Orts, 2001). Although TPS foams have a higher density
that the EPS cells are smaller than the cells of the TPS foams analyzed in compared to EPS (between 0.23 to 0.14 g/cm3), they are also relatively
this work, except for the foams with a higher amount of cotton fibers light to be used as packaging (Soykeabkaew et al., 2015).
(TPS-3CF and TPS-5CF), which presented similar cellular area (Glenn
et al., 2001). However, as the SEM images prove, TPS foam cells are
3.3. Water absorption of TPS foams with cotton
more irregular compared to EPS cells. The way to obtain these foams
(TPS and EPS) presents significant differences (Cronin & Ouellet, 2016;
The water absorption results of TPS foams with cotton are shown in
Soykeabkaew et al., 2015) that influence the final formation of cells. TPS
Fig. 4. The TPS-1C, TPS-3C and TPS-5C foams showed absorption of 80,
foams are obtained through the rapid expansion of a starch paste. Cells
72 and 68 g of water/100 g of solids, respectively. TPS-1C and TPS-3C
are formed by the violent expulsion of water vapor present in the
foams showed absorption similar to that found for normal TPS foam,

Fig. 3. SEM image of EPS used in commercial packaging.

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B.F. Bergel et al. Carbohydrate Polymer Technologies and Applications 2 (2021) 100167

Fig. 4. Water absorption of TPS foams with cotton. Different letters in the same column indicate significant differences (p ≤ 0.05) between means (Tukey’s test).

although a tendency to decrease absorption can be seen with the in­

Table 3
crease in the amount of cotton.
Results of the tensile test of the analyzed foams.
The addition of cotton makes the foams denser, more compact, and
therefore less porous. The porosity of foams strongly influences the Sample Young Modulus Tensile Stress Elongation at break
(MPa) (MPa) (%)
initial water absorption, the more porous a foam is, the faster it tends to
absorb water. TPS-5C foams showed less absorption in 5 min of contact TPS 42.55 ± 2.52a 1.10 ± 0.13a 1.64 ± 0.25c
TPS-1C 41.32 ± 4.68a 1.21 ± 0.16a 1.06 ± 0.17ab
with water due to their lower porosity and more compact structure
TPS-3C 65.87 ± 3.96b 1.57 ± 0.09b 1.09 ± 0.08ab
(Sanhawong et al., 2017; Vercelheze et al., 2012, 2013). Foams with TPS-5C 77.18 ± 2.47c 1.84 ± 0.11c 1.16 ± 0.17b
cotton microfibers TPS-1MC, TPS-3MC and TPS-5MC showed absorption TPS- 49.04 ± 4.67a 1.17 ± 0.13a 1.01 ± 0.21ab
of 80, 92 and 89 g of water/100 g of solids, respectively. It can be noted 1MC
that the TPS-3MC and TPS-5MC foams exhibited higher water absorp­ TPS- 72.88 ± 4.02bc 1.31 ± 0.15ab 0.77 ± 0.26a
3MC
tion compared to normal TPS foam.
TPS- 70.11 ± 3.39b 1.59 ± 0.07b 0.98 ± 0.12a
Foams with cotton microfibers have a less compact (more expanded) 5MC
structure, as shown by the SEM images. Due to this more expanded
Different letters in the same column indicate significant differences (p ≤ 0.05)
structure, these foams have cells with a cellular area similar to normal
between means (Tukey’s test).
TPS cells, but with a higher cell density. While the cell density of the TPS
foam is 4.19 × 108 cells/cm3 the cell density of the TPS-1MC, TPS-3MC
and TPS-5MC foams are 6.84 × 108, 6.71 × 108 and 7.12 × 108 cells/ The best result (greater tensile strength) was obtained by the TPS-5C
cm3, respectively. These two factors combined form foams relatively foam, an expected result due to its more compact and denser structure.
more porous than normal TPS and consequently absorb water more Foams containing microfibers showed mechanical properties slightly
quickly in early times (Kaewtatip, Tanrattanakul & Phetrat, 2013, below those found for foams with normal cotton, probably due to the
2018). Sjoqvist, Boldizar & Rigdahl (2010) reported that the increase in structure of these foams (more expanded structure) (Cruz-tirado, Siche,
the amount of water absorbed in early times is strongly related to the Cabanillas, Díaz-sánchez & Vejarano, 2017; Pornsuksomboon et al.,
foam porosity. Vercelheze et al. (2012) found similar results in foams 2016; Sanhawong et al., 2017). Sanhawong et al. (2017) achieved re­
sults similar to those of this study.
reinforced with sugar cane fibers.
Table 4 presents the results of the flexion test of the analyzed TPS
foams. Starch foams often exhibit anisotropic structure and brittleness,
3.4. Mechanical properties of TPS foams with cotton
as the foam’s surface stiffness is significantly greater than that of the
center. When the foam is flexed, the surface is subjected to the highest
Table 3 presents the results of the tensile test of the analyzed foams.
stress values. The results presented in the Table 4 show that the flexural
The results of the tensile test show that foams with added cotton (normal
modulus, flexural strength and elongation at break of foam starch
cotton fibers and cotton microfibers) obtained greater modulus, greater
increased significantly with the addition of cotton. These results are
tensile strength and less elongation at break compared to foams without
related to the adequate transfer of stress between the phases, caused by
cotton. This mechanical reinforcement is attributed to the strong inter­
the good adhesion via hydrogen bonds between the cotton fibers and the
facial interaction between the cotton fibers and the starch matrix. As
starch molecules (Bénézet et al., 2012; Mali, Debiagi, Grossmann &
both components (cotton and starch) have hydroxyl groups in their
Yamashita, 2010; Matsuda et al., 2013; Mello & Mali, 2014; Sanhawong
compositions, the interaction by hydrogen bonds tends to be strong,
et al., 2017; Vercelheze et al., 2012, 2013).
which increases the compatibility between the fiber and the matrix
In addition, the cotton fiber contents used in this study (mainly the
(Bénézet et al., 2012; Mello & Mali, 2014; Vercelheze et al., 2012).

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B.F. Bergel et al. Carbohydrate Polymer Technologies and Applications 2 (2021) 100167

Table 4 Table 5
Flexure test results of the analyzed foams. Impact resistance of TPS-C and TPS-MC foams.
Sample Flexure Modulus Flexure Stress Elongation at break Sample Impact Strenght (J/m)
(MPa) (MPa) (%)
TPS 12.33 ± 0.52a
TPS 127.62 ± 15.22a 0.51 ± 0.10a 1.68 ± 0.26a TPS-1C 12.69 ± 0.61a
TPS-1C 125.87 ± 20.34a 0.77 ± 0.21ab 2.85 ± 0.23c TPS-3C 57.86 ± 3.98d
TPS-3C 187.07 ± 11.09bc 1.38 ± 0.17c 3.41 ± 0.31d TPS-5C 66.52 ± 3.48e
TPS-5C 191.85 ± 12.65bc 1.54 ± 0.12c 3.51 ± 0.33d TPS-1MC 11.95 ± 1.13a
TPS- 138.66 ± 14.35a 0.99 ± 0.08b 2.32 ± 0.18b TPS-3MC 34.35 ± 3.39b
1MC TPS-5MC 47.97 ± 3.11c
TPS- 173.37 ± 10.78b 1.70 ± 0.15cd 2.93 ± 0.12c
3MC Different letters in the same column indicate significant
TPS- 205.70 ± 10.25c 1.77 ± 0.11d 2.88 ± 0.20c differences (p ≤ 0.05) between means (Tukey’s test).
5MC

Different letters in the same column indicate significant differences (p ≤ 0.05)
between means (Tukey’s test).
TPS-3C, TPS-5C, TPS 3MC and TPS 5MC foams) were high enough to
form an adequate structure with good fiber dispersion, leading to a
better modulus and elongation in the rupture for the foams.
Foams containing cotton microfibers showed greater flexural
strength results compared to foams with normal cotton, possibly due to
the greater dispersion of the (smaller) cotton fibers in the starch matrix.
Santos et al., (2014) state that the good dispersion of cellulose nano­
crystals leads to a significant improvement in the module and the tensile
strength of gelatin films.
The impact test is important in the search for materials that are
intended to be used as packaging. The main disadvantage of TPS foams
(in addition to water absorption) is their high fragility, as they tend to
break easily when handled. Table 5 shows the impact results of TPS
foams containing cotton fibers. The results for the analyzed starch foams
show that the addition of cotton to the foams significantly increased
their impact resistance. Highlight for TPS-5C foam, which showed a
large increase in impact resistance compared to normal TPS foam.
Machado et al., (2017) and Salgado, Schmidt, Molina Ortiz, Mauri &
Laurindo (2008) reported that the resistance and rigidity of foams are
correlated to their density. High density foams exhibit high resistance to
external forces.
Foams with treated cotton also showed an increase in strength
compared to normal foam, but less compared to foams with normal
cotton. These results are probably due to the longer length of the cotton
fibers (they are bigger and longer than the microfibers), which help
more in impact resistance than the short fibers. There may also have
been an increase and an intensification of the fragility of microfibers due
to chemical treatment. As the treatment consists of the contact of the
fibers with sodium hydroxide and sulfuric acid, the damage that caused
the fiber breaks also weakened these fibers and consequently decreased
the impact resistance. (Kargarzadeh et al., 2017; Sanhawong et al.,
2017; Soykeabkaew et al., 2015).
The mechanical properties of EPS packaging were also tested. EPS
presented maximum tensile stress of 1.08 ± 0.15 MPa, Young’s modulus
of 26.29 ± 3.54 MPa, flexure stress of 2.50 ± 0.12 MPa and flexure
modulus of 220.05 ± 7.98 MPa. The elongation at break of the tensile
test was 3.01 ± 0.26% and that of the flexure test was considered greater
than 5%, as the EPS specimens did not break during the test (5% is the
limit of elongation, according to the method described in ASTM D790).
The results found in this work are similar to those found by Glenn et al.,
(2001) and Machado et al., (2017). It can be noted that TPS foam
without added fibers has a tensile strength similar to EPS. Young’s
modulus of TPS was higher than that of EPS, which indicates greater
rigidity of starch foams. The TPS-3CF, TPS-5CF and TPS-5MCF foams
showed greater tensile strength compared to EPS, which is a good
indication for the replacement of EPS by these foams. It can be noted
that EPS showed higher bending stress (2.5 MPa) compared to TPS
foams. The addition of cotton fibers and microfibers increased the
flexural strength and flexibility (greater elongation at break) of the TPS
foams, making them less brittle, but the results remained below EPS.
Although Machado et al. (2017) have found similar values in the flexure
test, Glenn et al. (2001) found slightly lower values in this same test
(flexure strength of 1.3 MPa and modulus of 105 MPa). which possibly
indicates that there are differences in the specifications of EPS packaging
made by different manufacturers. Glenn et al., (2001) explain that TPS
foams with flexural properties within the EPS range can be considered
promising for use in food packaging. It is important to note that TPS
foams with silylated starch (with more than 13.34% m/m of silylated
starch) presented in the previous step (Bergel et al., 2020) had higher
flexural strength than EPS (between 3.21–2.01 MPa).
EPS presented an impact strength of 15.87 ± 0.92 J/m. This result is
slightly higher than that found for TPS foams without fibers (12.33 J/
m). With the addition of cotton fibers, impact resistance increased
considerably, surpassing the result found for EPS. The foams TPS-3CF,
TPS-5CF, TPS-3MCF and TPS-5MCF showed superior results than EPS,
which indicates the formation of resistant packaging with these
formulations.
4. Conclusion
This present work proposes to use cotton as reinforcement of TPS
foams, evaluating the amount of cotton and the type of cotton (normal
and chemically treated). The incorporation of cotton fibers in TPS foams
was satisfactory. With the aid of a mechanical stirrer in the mixture of
starch pastes, there were no homogenization problems. The reinforced
foams showed better results in the tensile, flexure and impact tests. In
addition, foams with a greater amount of cotton fibers showed a
decrease in water absorption in 5 min of contact with water. In general,
TPS-C foams showed better mechanical properties and less water ab­
sorption than TPS-MC foams. TPS-C foams also showed higher densities
and a more compact structure (which explains the other results). The
TPS-5C foam showed the most satisfactory results, as it absorbed less
water than the normal TPS foam, in addition to presenting greater
resistance to impact and traction. Comparison with the EPS used in
commercial trays shows that TPS foams with cotton fibers (mainly TPS
5CF and TPS 5MCF foams) can be used as packaging. These foams can be
used as single-use packaging for foods such as fruit and sandwiches.
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
This work was supported by the National Council of Scientific and
Technological Development of Brazil (CNPQ) and authors greatly thank
the assistance. The authors would also like to thank the Laboratory of
Polymeric Materials (LAPOL), the post-graduate program in Materials
Engineering (PPGE3M) and the SENAI Institute of Innovation in Poly­
mer Engineering for the necessary assistance.

7
B.F. Bergel et al. Carbohydrate Polymer Technologies and Applications 2 (2021) 100167

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