Compression Behavior of Biodegradable Thermoplastic Plasticizer-Containing Composites
Thermoplastic starch-based composites generate worldwide interest as they are based on green raw materials and undergo complete degradation. The composites were first fabricated from starch and sisal fibers as the major materials via the forming process. The effect of starches with different content...
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Інститут проблем міцності ім. Г.С. Писаренко НАН України
2019
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irk-123456789-1882992023-02-24T01:27:08Z Compression Behavior of Biodegradable Thermoplastic Plasticizer-Containing Composites Guo, A.F. Li, J.F. Li, F.Y. Xu, J. Zhang, C.W. Chen, S. Научно-технический раздел Thermoplastic starch-based composites generate worldwide interest as they are based on green raw materials and undergo complete degradation. The composites were first fabricated from starch and sisal fibers as the major materials via the forming process. The effect of starches with different contents of single- and multicomponent plasticizers on the cushioning properties of the composites was studied. An increase in plasticizer contents within a certain range is shown to enhance materials resistance to pressure and its cushioning performance. With the multicomponent plasticizer content of 15%, the resistance to pressure for four types of composites prepared at different weight ratios of formamide and urea were of the order of 2:1>1:1>1:2, and that of the four types of composites fabricated at different weight ratios of glycerol and ethylene glycol were of the order of 1:2>2:1>1:1. Multicomponent plasticizer-containing starch-based composites are shown to be irregular elastomers and the stress-strain relation to be first defined by a hyperbolic tangent curve function and then by the tangent one. Композиты на основе термопластичного крахмала оказались в центре внимания как отечественных, так и зарубежных ученых, так как они основаны на экологичном сырье и полностью разлагаются. Такие композиты получали формовкой с использованием крахмала и сизалевых волокон в качестве основных материалов. Изучено влияние термопластичного крахмала с различной долей простых и составных пластификаторов на амортизационные свойства композитов. Экспериментальные результаты показали, что в определенных пределах с увеличением содержания пластификаторов повышаются сопротивление материала давлению и его амортизационные характеристики. При содержании составного пластификатора 15% сопротивление давлению четырех типов композитов, полученных с использованием различных массовых соотношений фомамида и мочевины, изменяется в ряду 2:1>1:1>1:2, а с использованием различных массовых соотношений глицерина и этиленгликоля в последовательности 1:2>2:1>1:1. Композиты на основе крахмала, содержащие составной пластификатор, являются нерегулярными эластомерами, и зависимость между напряжением и деформацией описывается в первую очередь функцией гиперболической тангенсоиды и во вторую очередь функцией тангенсоиды. Композити на основі термопластичного крохмалю виявилися в центрі уваги як вітчизняних, так і зарубіжних вчених, так як вони засновані на екологічної сировині і повністю розкладаються. Такі композити отримували формуванням з використанням крохмалю і сизалевих волокон в якості основних матеріалів. Вивчено вплив термопластичного крохмалю з різною часткою простих і складових пластифікаторів на амортизаційні властивості композитів. Експериментальні результати показали, що в певних межах зі збільшенням вмісту пластифікаторів підвищуються опір матеріалу тиску і його амортизаційні властивості. При утриманні складеного пластифікатора 15% опір тиску чотирьох типів композитів, отриманих з використанням різних масових співвідношень фомаміда і сечовини, змінюється в ряду 2: 1> 1: 1> 1: 2, а з використанням різних масових співвідношень гліцерину і етиленгліколю - в послідовності 1 : 2> 2: 1> 1: 1. Композити на основі крохмалю, які містять складовою пластифікатор, є нерегулярними еластомерами, і залежність між напруженням і деформацією описується в першу чергу функцією гіперболічної тангенсоіди і в другу чергу функцією тангенсоіди. 2019 Article Compression Behavior of Biodegradable Thermoplastic Plasticizer-Containing Composites / A.F. Guo, J.F. Li, F.Y. Li, J. Xu, C.W. Zhang, S. Chen // Проблеми міцності. — 2019. — № 1. — С. 24-31. — Бібліогр.: 25 назв. — англ. 0556-171X http://dspace.nbuv.gov.ua/handle/123456789/188299 539.4 en Проблемы прочности Інститут проблем міцності ім. Г.С. Писаренко НАН України |
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Научно-технический раздел Научно-технический раздел Guo, A.F. Li, J.F. Li, F.Y. Xu, J. Zhang, C.W. Chen, S. Compression Behavior of Biodegradable Thermoplastic Plasticizer-Containing Composites Проблемы прочности |
| description |
Thermoplastic starch-based composites generate worldwide interest as they are based on green raw materials and undergo complete degradation. The composites were first fabricated from starch and sisal fibers as the major materials via the forming process. The effect of starches with different contents of single- and multicomponent plasticizers on the cushioning properties of the composites was studied. An increase in plasticizer contents within a certain range is shown to enhance materials resistance to pressure and its cushioning performance. With the multicomponent plasticizer content of 15%, the resistance to pressure for four types of composites prepared at different weight ratios of formamide and urea were of the order of 2:1>1:1>1:2, and that of the four types of composites fabricated at different weight ratios of glycerol and ethylene glycol were of the order of 1:2>2:1>1:1. Multicomponent plasticizer-containing starch-based composites are shown to be irregular elastomers and the stress-strain relation to be first defined by a hyperbolic tangent curve function and then by the tangent one. |
| format |
Article |
| author |
Guo, A.F. Li, J.F. Li, F.Y. Xu, J. Zhang, C.W. Chen, S. |
| author_facet |
Guo, A.F. Li, J.F. Li, F.Y. Xu, J. Zhang, C.W. Chen, S. |
| author_sort |
Guo, A.F. |
| title |
Compression Behavior of Biodegradable Thermoplastic Plasticizer-Containing Composites |
| title_short |
Compression Behavior of Biodegradable Thermoplastic Plasticizer-Containing Composites |
| title_full |
Compression Behavior of Biodegradable Thermoplastic Plasticizer-Containing Composites |
| title_fullStr |
Compression Behavior of Biodegradable Thermoplastic Plasticizer-Containing Composites |
| title_full_unstemmed |
Compression Behavior of Biodegradable Thermoplastic Plasticizer-Containing Composites |
| title_sort |
compression behavior of biodegradable thermoplastic plasticizer-containing composites |
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Інститут проблем міцності ім. Г.С. Писаренко НАН України |
| publishDate |
2019 |
| topic_facet |
Научно-технический раздел |
| url |
http://dspace.nbuv.gov.ua/handle/123456789/188299 |
| citation_txt |
Compression Behavior of Biodegradable Thermoplastic Plasticizer-Containing Composites / A.F. Guo, J.F. Li, F.Y. Li, J. Xu, C.W. Zhang, S. Chen // Проблеми міцності. — 2019. — № 1. — С. 24-31. — Бібліогр.: 25 назв. — англ. |
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Проблемы прочности |
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2025-07-16T10:18:01Z |
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| fulltext |
UDC 539.4
Compression Behavior of Biodegradable Thermoplastic Plasticizer-Containing
Composites
A. F. Guo,
a,1
J. F. Li,
b
F. Y. Li,
b
J. Xu,
b
C. W. Zhang,
b
and S. Chen
b
a School of Mechanical & Automobile Engineering, Liaocheng University, Liaocheng, China
b School of Mechanical Engineering, Shandong University, Jinan, China
1 guoanfu@lcu.edu.cn
Thermoplastic starch-based composites generate worldwide interest as they are based on green raw
materials and undergo complete degradation. The composites were first fabricated from starch and
sisal fibers as the major materials via the forming process. The effect of starches with different
contents of single- and multicomponent plasticizers on the cushioning properties of the composites
was studied. An increase in plasticizer contents within a certain range is shown to enhance materials
resistance to pressure and its cushioning performance. With the multicomponent plasticizer content
of 15%, the resistance to pressure for four types of composites prepared at different weight ratios of
formamide and urea were of the order of 2:1�1:1�1:2, and that of the four types of composites
fabricated at different weight ratios of glycerol and ethylene glycol were of the order of 1:2�
2:1�1:1. Multicomponent plasticizer-containing starch-based composites are shown to be irregular
elastomers and the stress-strain relation to be first defined by a hyperbolic tangent curve function
and then by the tangent one.
Keywords: biodegradation, starch-based composite, single/multicomponent plasticizers,
cushioning package, compression behavior.
Introduction. The application of plastic packing materials has brought considerable
convenience to humansociety, but also leads to “white pollution” and other environmental
problems. To solve these problems, scholars [1–4] have focused on the use of biomass
composites in recent decades. Starch-based composites are a class of new cushion
packaging materials whose principal components are plant fibers and starch. Starch-based
composites using natural resources as raw materials possess excellent biodegradability
[5–8]. These composites can not only mitigate the pollution problem but also avert a
biochemical crisis [9–11]. Therefore, green alternatives such as starch-based composites are
presently a hot topic of research.
Starch is a natural polymer with many intramolecular and intermolecular hydrogen
bonds; hence, its molecules are strongly bonded. When small molecules are added into
starch and mixed, new hydrogen bonds are formed that are capable of replacing the
hydrogen bonds of starch molecules. The new hydrogen bonds can decrease the
intermolecular force of molecules and increase their capacity for action [12, 13]. Thus,
these small molecules impart thermoplasticity to plastic. As an important component of
starch-based composites, thermoplastic starch (TPS) significantly influences the properties
of the compound material.
In recent years, many reports have been published on TPS-based composites. Liu et
al. [14] studied the plasticizing mechanism of plasticized starch by infrared spectroscopy
and X-ray diffraction. Ma and Yu [15, 16] studied the mechanism of interaction between
the hydrogen bonds of starch and the plasticizer in glycerol-plasticized thermoplastic starch
(GPTPS) and formamide-plasticized thermoplastic starch (FPTPS). Aichholzer and Fritz
[17] and Della Valle et al. [18] analyzed the rheological properties of TPS-based
composites. Guo et al. [19] and Canché-Escamilla et al. [20] studied the biodegradability of
TPS composites. Some scholars [21–24] investigated the cushioning performance of
© A. F. GUO, J. F. LI, F. Y. LI, J. XU, C. W. ZHANG, S. CHEN, 2019
24 ISSN 0556-171X. Ïðîáëåìè ì³öíîñò³, 2019, ¹ 1
common cushion packaging materials using static compression tests. Nevertheless, to the
best of the authors’ knowledge, there has been no comprehensive study focusing on the
mechanical properties of TPS-based composites.
In this study, the effect of TPS with different proportions of single and compound
plasticizers on the cushioning properties of their composites was studied by analyzing the
static compression curves of the composites via static compression tests using formamide,
urea, glycerol, and ethylene glycol as plasticizers.
1. Materials and Experiments.
1.1. Materials and Equipment. Materials: Sisal fibers of 100–150 mesh with a length
of 5–10 mm were provided by Yantai Jiulong Co., Ltd. Corn starch with an average
diameter of 70 nm was purchased from Hebei Huachen Starch Sugar Co., Ltd. Analytical
reagent (AR) grade formamide was purchased from Tianjin Damao Chemical Reagent
Factory. AR grade urea was purchased from Tianjin Guangcheng Chemical Reagent Co.,
Ltd. AR grade ethylene glycol and glycerol were purchased from Tianjin Fuyu Fine
Chemical Co., Ltd. Other materials such as talcum powder of 0.038 mm grade, stearic acid,
foaming agent AC, polyvinyl alcohol (99% purity) AR grade sodium hydroxide, and
distilled water were purchased from Tianjin Guangcheng Chemical Reagent Co., Ltd.
Table 1 shows the materials used in the preparation.
Testing equipment included: electronic constant temperature water bath (model
HHS-2), precision electric mixer (model JJ-1), electronic balance (model JM-B),
electrothermal constant temperature dry box (model DHG), double column simplex
mechanical compression machine, and microcomputer-controlled electron universal testing
machine (model WDW-100A).
1.2. Preparation of Starch-Based Composite. The preparation process can be
subdivided into four stages: fiber pre-treatment, TPS preparation, slurry mixture, and
foaming (Fig. 1).
Compression Behavior of Biodegradable Thermoplastic ...
ISSN 0556-171X. Ïðîáëåìè ì³öíîñò³, 2019, ¹ 1 25
T a b l e 1
Materials Used in the Preparation
Material Type Material Type Material Type
Sisal fiber 5–10 mm
length
Urea AR grade Talcum
powder
0.038 mm
grade
Corn starch 70 nm
diameter
Ethylene
glycol
AR grade Polyvinyl
alcohol
99% purity
Formamide AR grade Glycerol AR grade Sodium
hydroxide
AR grade
Fig. 1. Preparation of thermoplastic starch-based composites.
(1) Fiber pretreatment: The sisal fibers were immersed in 5% sodium hydroxide
solution for 4 h. Then, they were washed with distilled water until pH=7 was reached.
Finally, they were dried at 80�C for 8 h in a heat oven.
(2) TPS preparation: Single plasticizer: FPTPS and urea plasticized thermoplastic
starch (UPTPS) were compounded in the proportion of 10, 15, and 20%. GPTPS and
ethylene glycol-plasticized thermoplastic starch (EGPTPS) were compounded in the
proportion of 15%.
Compound plasticizer: The proportion of formamide to urea in formamide-urea
plasticized thermoplastic starch (FUPTPS) was set at 2:1, 1:2, and 1:1. The proportion of
glycerol to ethylene glycol in glycerol-ethylene glycol-plasticized thermoplastic starch
(GGPTPS) was set at 2:1, 1:2, and 1:1.
Starch and water were mixed according to the formula ratio. Then starch was pasted
in 75-85°C water. Subsequently, the plasticizer was stirred and added to the starch.
(3) Slurry mixture: The amount of TPS and sisal fibers used in this process was 500 g.
They were treated by alkali, added to a mixer, and stirred for 20 min at room temperature.
Subsequently, the additives were added to the slurry for 30 min.
(4) Foaming: The mixed slurry was poured into a mold of size 300 300� mm, with the
upper mold temperature set at 180°C, the lower mold temperature set at 195�C, pressure set
at 3 MPa, and the elevate pressure was set of 20 s. Then, the pressure process was
continued for 30 s. Finally, the product was removed from the mold.
1.3. Testing of Mechanical Properties of Starch-Based Composite. According to the
method of GB 8168-2008 [25], standard samples (100 100 25� � mm) were used for the
static compression test. The samples were pressed by increasing load along the width at a
speed of 12 mm/min. The test was performed at a speed of 10 mm/min until the sample was
crushed. The loads were recorded automatically. The compressive stress and strain were
calculated by formulas (1) and (2), respectively:
� �
P
A
, (1)
where � is the compressive stress (MPa), P is compressive load (N), and A is test
sample cross-sectional area (mm2),
��
�T T
T
j
, (2)
where � is the compressive strain (%), T is original thickness of testing sample (mm), and
T j is thickness after testing (mm).
According to the stress–strain curve obtained by analyzing the test data, the volume
deformation energy and cushion coefficient at different stresses were calculated. Then, the
cushion coefficient–stress curve was plotted as follows:
(i) Divide the area under the stress–strain curve into several small areas. The smaller
the area, the higher is the computational accuracy.
(ii) Calculate � i and � i (i� 1 2 3, , , ...).
(iii) Calculate the increment in every stressed section, that is, calculate the proportion
of each area
ui i i i i�
�� �
1
2
1 1( )( ).� � � � (3)
(iv) Calculate the corresponding creep resistance ui ,
u ui k� � ( , , ... , ).k i� 1 2 (4)
A. F. Guo, J. F. Li, F. Y. Li, et al.
26 ISSN 0556-171X. Ïðîáëåìè ì³öíîñò³, 2019, ¹ 1
(v) Calculate the corresponding cushion coefficient Ci ,
C
u
i
i
i
�
�
. (5)
(vi) Draw the cushion coefficient–maximum stress curve, taking C as the ordinate
and � as the abscissa.
2. Results and Discussion.
2.1. Influence of Single Plasticizers on Properties of Composites. Figure 2 shows the
compressive stress–strain curves of the FPTPS- and UPTPS-based composites, respectively.
When the plasticizer content is in the range 10–20% at a fixed strain, the stress decreases
with an increase in the plasticizer content. The higher the resistance to pressure of the
material, the greater its cushioning performance.
Figure 3 shows the compressive stress–strain curves of the GPTPS-, EGPTPS-,
UPTPS-, and FPTPS-based composites with a plasticizer content of 15%. When the
plasticizer content is fixed, the stress of the four materials follows the order FPTPS�
UPTPS�EGPTPS�GPTPS; therefore, the resistance to pressure follows the order
FPTPS�UPTPS�EGPTPS�GPTPS. As stated above, the higher the resistance to
pressure, the better the cushioning performance. Accordingly, the cushioning performance
ISSN 0556-171X. Ïðîáëåìè ì³öíîñò³, 2019, ¹ 1 27
a b
Fig. 2. Compressive stress–strain curves of FPTPS- (a) and UPTPS-based (b) composites.
Fig. 3. Compressive stress–strain curves of four starch-based composites.
Compression Behavior of Biodegradable Thermoplastic ...
of FPTPS and UPTPS is better than that of EGPTPS and GPTPS. The reason for the higher
stress of FPTPS and UPTPS is that formamide and urea have a C�O group and exhibit
strong electronegativity; hence, they easily form hydrogen bonds with the hydrogen atoms
of starch. Besides, the �NH2 group of formamide and urea can form hydrogen bonds with
the ether bonds of starch. Therefore, the plasticizing effect of formamide and urea is better
than that of glycerol and ethylene glycol; thus, better-quality TPS can be obtained when
using formamide and urea as plasticizers.
As shown in Fig. 2, FPTPS and UPTPS are tangent-curve elastomers that show a kind
of tangential relation between stress and strain. Taking the stress–strain curve of UPTPS
with a plasticizer content of 10% as an example, in segment a, strain increases gradually
with increasing stress, the local distortion of stress is larger, and stress does not exhibit a
very large change; hence, the material shows definite cushioning performance. In segment
b, when stress reaches the extreme value of compression, bubbles in the material burst and
gas is expelled, and the material is pressed. Therefore, the stress increases sharply and the
cushioning effect disappears.
Figure 4a shows the static cushion coefficient–stress curves of the FPTPS-based
composites. Figure 4b shows the static cushion coefficient–stress curves of the UPTPS-
based composites. As can be seen from Fig. 4a, the cushion coefficient of the material first
decreases and then stabilizes with an increase in stress; the smallest cushion coefficient
obtained for the FPTPS-based composites is 5. Figure 4b also shows that the cushion
coefficient of the material decreases first and then stabilizes with an increase in stress; the
smallest cushion coefficient obtained for the UPTPS-based composites is in the range 4–6.
2.2. Influence of Compound Plasticizers on Properties of Composites. Figure 5a
shows the compressive stress–strain curves of FUPTPS-based composites. At a plasticizer
content of 15%, the resistance to pressure of the starch-based composites prepared using
different mass ratios of formamide and urea follows the order 2:1�1:1�1:2. Figure 2b
shows that the cushioning performance of the FPTPS-based composites is better than that
of the UPTPS-based composites, with the latter being hard and brittle. If urea is replaced by
formamide, the brittleness of the compound material decreases, increasing its flexibility.
Figure 5b shows the compressive stress–strain curves of the GGPTPS-based
composites. At a plasticizer content of 15%, the resistance to pressure of the starch-based
composites prepared using different mass ratios of glycerol and ethylene glycol follows the
order 2:1�1:1�1:2. Figure 3 shows that the cushioning performance of the EGPTPS-
based composites is better than that of the GPTPS-based composites. Similarly, when
28 ISSN 0556-171X. Ïðîáëåìè ì³öíîñò³, 2019, ¹ 1
A. F. Guo, J. F. Li, F. Y. Li, et al.
a b
Fig. 4. Static cushion coefficient–stress curves of FPTPS- (a) and UPTPS-based (b) composites.
glycerol is partially replaced by ethylene glycol, the cushioning performance of the
compound material is enhanced.
Under conditions of constant compound plasticizer content and stress, the mass ratio
of the compound plasticizer and resistance to pressure are different.
From Fig. 5, we can see that FUPTPS and GGPTPS are irregular elastomers. Their
stress–strain relation first shows a hyperbolic tangent curve function and then a tangent
curve function. Taking compressive stress–strain curves of FUPTPS-based composites in
Fig. 5a as an example, we can see a hyperbolic tangent curve function relationship in
segment c, and at the elastic stage, the material undergoes a small deformation and the
cushioning performance is good. However, there exists a tangent curve function relationship
in segments d and e.
Figure 6a shows the static cushion coefficient–stress curves of the FUPTPS-based
composites. With increasing stress, the cushion coefficient of the material first decreases
and then stabilizes. The smallest cushion coefficient obtained for the FUPTPS-based
composites is between 4.5 and 5.5. With a change in the mass ratio of formamide and urea,
the cushion coefficient of the material changes greatly. When the mass ratio of formamide
and urea in the compound plasticizer is 2:1, the cushion coefficient is the smallest and the
cushioning performance of the material is the best.
ISSN 0556-171X. Ïðîáëåìè ì³öíîñò³, 2019, ¹ 1 29
Compression Behavior of Biodegradable Thermoplastic ...
a b
Fig. 5. Compressive stress–strain curves of FUPTPS- (a) and GGPTPS-based (b) composites.
a b
Fig. 6. Static cushion coefficient–stress curves of FUPTPS- (a) and GGPTPS-based (b) composites.
Figure 6b shows the static cushion coefficient–stress curves of the GGPTPS-based
composites. We can see that with increasing stress, the cushion coefficient of the material
first decreases and then stabilizes. The smallest cushion coefficient for the GGPTPS-based
composites is between 4.5 and 5. With a change in the mass ratio of glycerol and ethylene
glycol, the cushion coefficient of the material changes greatly. When the mass ratio of
glycerol and ethylene glycol in the compound plasticizer is 1:2, the cushion coefficient is
the smallest and the cushioning performance of the material is the best.
C o n c l u s i o n s
1. Plasticizers enhance the flexibility of starch-based composites. Within a certain
range, as the plasticizer content increases, the resistance to pressure of the composite and its
cushioning performance increase.
2. FPTPS and UPTPS are tangent-curve elastomers showing a kind of tangential
relation between stress and strain, while compound plasticizer starch-based composite
materials are irregular elastomers. The stress-strain relation of the latter is first a hyperbolic
tangent curve function and then a tangent curve function.
3. When the single plasticizer content is 15%, the resistance to pressure of the four
types of composites prepared using single plasticizers follows the order FPTPS�UPTPS�
EGPTPS�GPTPS. When the compound plasticizer content is 15%, the resistance to
pressure of the four types of FUPTPS composites prepared using different mass ratios of
formamide and urea follows the order 2:1�1:1�1:2, and that of the four types of GGPTPS
composites prepared using different mass ratios of glycerol and ethylene glycol follows the
order 1:2�2:1�1:1.
Acknowledgments. The authors gratefully appreciate the financial support from the
National Natural Science Foundation of China (Nos. 51775318, 51305239, and 51275278),
and Natural Science Foundation of Shandong Provincial (Nos. ZR2013EEQ010 and
2014ZRB019XH). We also appreciate the assistance of our colleagues from Shandong
University, China.
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Received 15. 03. 2018
Compression Behavior of Biodegradable Thermoplastic ...
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/ENU (Use these settings to create Adobe PDF documents best suited for high-quality prepress printing. Created PDF documents can be opened with Acrobat and Adobe Reader 5.0 and later.)
>>
/Namespace [
(Adobe)
(Common)
(1.0)
]
/OtherNamespaces [
<<
/AsReaderSpreads false
/CropImagesToFrames true
/ErrorControl /WarnAndContinue
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/IncludeNonPrinting false
/IncludeSlug false
/Namespace [
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(InDesign)
(4.0)
]
/OmitPlacedBitmaps false
/OmitPlacedEPS false
/OmitPlacedPDF false
/SimulateOverprint /Legacy
>>
<<
/AddBleedMarks false
/AddColorBars false
/AddCropMarks false
/AddPageInfo false
/AddRegMarks false
/ConvertColors /ConvertToCMYK
/DestinationProfileName ()
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/Downsample16BitImages true
/FlattenerPreset <<
/PresetSelector /MediumResolution
>>
/FormElements false
/GenerateStructure false
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/MultimediaHandling /UseObjectSettings
/Namespace [
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(CreativeSuite)
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]
/PDFXOutputIntentProfileSelector /DocumentCMYK
/PreserveEditing true
/UntaggedCMYKHandling /LeaveUntagged
/UntaggedRGBHandling /UseDocumentProfile
/UseDocumentBleed false
>>
]
>> setdistillerparams
<<
/HWResolution [2400 2400]
/PageSize [612.000 792.000]
>> setpagedevice
|