Polymer Testing 116 (2022) 107812

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Polymer Testing
journal homepage: www.elsevier.com/locate/polytest

Comprehensive analysis of mechanical properties of microcellular

polypropylene: Experiment and simulation
Yichong Chen a, c, Jiabao Yu a, b, Yijie Ling a, Shun Yao a, Xiulei Jiang b, Dongdong Hu a,
Huifeng Wang c, Ling Zhao a, *
a
State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai, 200237, PR China
b
Shincell New Material Co., Ltd., Suzhou, 215000, PR China
c
School of Information Science and Engineering, East China University of Science and Technology, Shanghai, 200237, PR China

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

Keywords: A series of microcellular polypropylene (PP) with different bubble size and expansion ratio were prepared by
Microcellular polypropylene supercritical CO2 moulding compression foaming, and their compressive, flexural and tensile properties were
Mechanical property measured. A comprehensive calculation model for the mechanical properties of polymer foam based on tetra­
Bubble structure
decahedron structure was further established, and the error between the simulation results and the experimental
Finite element calculation
results is less than 25%. Based on the model, the contributions of the elastic stress of polymer matrix and counter-
Counter-acting force of gas
acting force of gas to the elastic modulus were quantitatively analyzed for the first time. The results show that the
smaller bubble size can improve the compressive elastic modulus and flexural elastic modulus but has little effect
on the tensile elastic modulus. At the same time, the counter-acting force of gas has a positive effect on the
compressive elastic modulus, but has a weakening effect on the tensile elastic modulus, and has almost no effect
on the flexural elastic modulus. Finally, the generality of the above model is verified by the prediction for elastic
modulus of different polymer foams.

1. Introduction which contribute to the mechanical properties. When the gas pressure is
atmospheric pressure, the contribution caused by the gas compression is
Due to its unique versatility, polymer foams have been used in many negligible. The Gibson-Ashby model describes the relationship between
fields such as thermal insulation [1], sound insulation [2], cushioning the relative properties and the relative density of foams, where the
[3], electromagnetic shielding [4,5], sensing [6,7], smart response [8, volume fraction of the polymer that makes up the edges was used as a
9], mechanical energy harvesting [10], etc. As the demand for light­ fitting parameter, and for open-cell foams, the value is 1. According to
weight materials increases, low-density polymer foams with excellent the performance prediction model of Gibson-Ashby, the mechanical
properties are gaining attention. However, the mechanical properties of properties of foams mainly depend on the properties of polymer matrix
polymer foams will also decrease due to the decrease of their density and the material density after foaming. When the density after foaming
[11], which greatly limits their application fields. Therefore, the me­ is consistent, the mechanical properties of foams depend only on the
chanical properties of polymer foams have always been the focus of inherent properties of the polymer matrix. However, in this model, Ф is
researchers. considered to be a fixed value, and the effect of bubble connectivity is
Many scholars have done a lot of research on the relationship be­ not considered. Saint-Michel et al. [20] studied the mechanical prop­
tween mechanical properties and material structure through theoretical erties of high-density polyurethane foams. The results show that for
models and experimental studies [12–18]. Gibson and Ashby [19] pro­ high-density foams, the calculation results of the Gibson-Ashby model
posed a quantitative prediction model for the mechanical properties of cannot predict the actual situation. Wang et al. [21] also found in­
foams based on the bubble structure. In this model, the bubble is consistencies in the model predictions on high-density ethyl­
assumed to be composed of edges, walls and internal gas, all three of ene-propylene-diene rubber foams. In order to solve the deviation of the

Abbreviations: CO2, Carbon Dioxide; N2, Nitrogen; PP, Polypropylene; PS, Polystyrene; PVC, Polyvinyl Chloride; TPU, Thermoplastic Polyurethane; SEM, Scanning
Electron Microscopy.
* Corresponding author.
E-mail address: [email protected] (L. Zhao).

https://doi.org/10.1016/j.polymertesting.2022.107812
Received 7 July 2022; Received in revised form 2 September 2022; Accepted 29 September 2022
Available online 4 October 2022
0142-9418/© 2022 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/).
Y. Chen et al. Polymer Testing 116 (2022) 107812

Gibson-Ashby model in predicting the mechanical properties of through the measurement of compressive, flexural and tensile proper­
high-density foams, Naguib [22] and Chen [23] proposed new models ties. At the same time, a comprehensive mechanical property calculation
for predicting the mechanical properties of cubic bubble structures for model based on tetradecahedron structure was established, the stress
open-cell and closed-cell foams, respectively. The new cube model analysis of bubble wall in different processes was studied, and the elastic
correlates the relative density of the foams with the thickness and modulus was calculated. For the first time, the effects of the polymer
length, and the results show that the model is more accurate during the matrix and the counter-acting force generated by the air in bubbles on
relative density of 0.2–0.5. the elastic modulus of foams were comprehensively analyzed. And then,
However, none of the above models clearly indicate the structure- the elastic modulus of foams in the literature was predicted by the model
performance relationship between the mechanical properties of foams to verify the generality of the above model.
and the bubble structure. At the same time, for foams prepared by
different polymer matrix, there are differences in the dependence of 2. Experimental and simulation
their mechanical properties on the bubble structure. For example, for
rigid materials, larger bubble size causes the foams to be more easily 2.1. Materials
crushed [24]. Alvarez et al. [25] has studied the relationship between
the structure and properties of foams by finite element simulation. The Commercial random PP (E02ES) with a melt mass flow rate of 1.5 g/
results show that the Young’s modulus of foams has a linear relationship 10 min was supplied by the Sinopec Zhenhai Refining&Chemical Com­
with the relative density, and the effect of bubble size on Young’s pany. The crystallization temperature (Tc) and melting temperature (Tm)
modulus is almost negligible. Weller and Kumar [26] studied the effect of the PP were 109 οC and 155 οC, respectively, as measured by differ­
of bubble size on the tensile properties of polycarbonate foams when the ential scanning calorimetry (NETZSCH DSC 204 HP, Germany) under
relative density was below 0.5, and the results show that the bubble size atmospheric Nitrogen. CO2 (purity: 99.99% w/w) and N2 (purity:
has little effect on the tensile properties. However, Doroudiani [27] 99.99% w/w) were obtained from Air Products (Shanghai) Co., Ltd.
found that under the same relative density, the bubble structure would
affect the impact strength of polystyrene (PS) foams. Saha et al. [28] also 2.2. Supercritical CO2 moulding compression foaming processes
found that smaller bubble size can provide higher Young’s modulus and
yield stress when the bubble density is the same in their study of poly­ Supercritical CO2 moulding compression foaming PP was carried out
vinyl chloride (PVC) foams. Bai et al. [29] found that the bubble density in a rectangular cavity with an inner diameter of 300mm × 200mm ×
of the silicone rubber foams can be increased while the bubble size can 20 mm. The PP sample was formed by hot pressing to 150mm × 100mm
be reduced by adding nano-graphite, so that the compressive strength × 12 mm at 170 ◦ C for 5 min, and then vented to ensure that there was
can be greatly improved. Wang et al. [30] established a finite element no gas in the sample for 5 min. Firstly, the cavity was heated to the
analysis model with a representative tetradecahedron as the basic foaming temperature, and then the PP sample was placed into the cavity.
structural unit to study the property-structure relationship of polyamine The cavity was closed by the hydraulic system and the pressure was
methacrylate foams. It is found that the larger the bubble size and the maintained. CO2 was added into the cavity to purge air, repeat three
thinner the bubble wall, the lower the Young’s and shear modulus of the times. The cavity was pressurized by CO2 to a certain value afterward.
material. After the sample was kept for 240 min to allow CO2 to reach dissolution
In addition, the pressure inside the bubble also has an effect on the equilibrium in the PP matrix, the pressure was quickly relieved by a
mechanical properties. Ramsteiner et al. [31] studied the compressive solenoid valve with a diameter of 10 mm, and the depressurization rate
properties of open-cell melamine foam and closed-cell polystyrene foam, is about 80 MPa/s. Finally, the cavity was opened quickly and the
and it is found that polystyrene foam with a closed-cell structure has a foamed sample is taken out.
higher compressive elastic modulus due to the counter-acting force
generated by air compression. Roberts et al. [32] evaluated the Young’s 2.3. Characterization
modulus of foams with different open-cell ratios by finite element
method, and the results show that the content of polymer matrix in the 2.3.1. Scanning electron microscopy (SEM)
model did not have a linear relationship with the Young’s modulus, The cellmorphology of the foamed samples was observed by a JSM-
confirming the effect of gas pressure on the Young’s modulus. Ge et al. 6360LV (JEOL Ltd., Tokyo, Japan) scanning electron microscopy (SEM).
[33] studied the mechanical properties of thermoplastic polyurethane The samples were immersed in liquid nitrogen for 10 min and then
(TPU) foam and found that TPU with open-cell structure has a higher fractured. The average bubble size was obtained through the analysis of
tensile elastic modulus due to the communication of gas. However, the the SEM photographs using Image-Pro Plus. The relevant calculations
existing literatures have only carried out qualitative experimental have been detailed in our previous work [35].
studies on the effect of bubble pressure on mechanical properties, and
there is no report on quantitative analysis of its mechanism of action. 2.3.2. Compressive performance test
The mechanical properties of polymer foams depend not only on the Compressive performance test was conducted by Instron 5865 uni­
intrinsic properties of the polymer and the relative density of the foam versal tester. The foam was cut into a standard spline of 100 × 100mm
but also on the bubble structure, such as bubble size [26], bubble density × 20 mm by special-shaped cutting machine (iECHO, TK3S3521), and
[34], open-cell ratio [31] and so on. In addition, the air inside bubbles the spline was compressed at a speed of 1.0 mm/min after loading,
also affects the mechanical properties. However, most of the current which was repeated for at least 5 times. The compressive elastic modulus
researches focus on experimental studies or modeling the relationship was calculated according to:
between relative density and mechanical properties, and lack of
FC /AC
in-depth study on the effect of cell structure on mechanical properties. CM = (1)
xC /tC
At the same time, the influence of the pressure inside the bubble on the
mechanical properties is only in the qualitative research. Therefore, it is
Where CM is the compressive elastic modulus (MPa), FC is the
necessary to develop a method to comprehensively evaluate the influ­
compressive force within the proportional limit (N), AC is the area of
ence factors on the mechanical properties of foams.
foams (mm2), xC is the deformation corresponding to FC (mm), tC is the
In this work, polypropylene (PP) was used as the matrix, a series of
thickness of foams (mm).
PP foams with different expansion ratio and bubble size were prepared
by supercritical CO2 moulding compression foaming. The effects of
bubble size and expansion ratio on mechanical properties were studied

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2.3.3. Flexural performance test

Flexural performance test was conducted by Instron 5865 universal
tester. The foam was cut into a standard spline of 350 × 100mm × 25
mm by special-shaped cutting machine, and the spline was loaded on the
flexural module with the span between the two supports of 300 mm. The
stress was applied by a loading indenter perpendicular to the longitu­
dinal axis of the spline with a speed of 20 mm/min. The entire test was
repeated for at least 5 times. The flexural elastic modulus was calculated
according to:

L3F FF
FM = × (2)
4wF tF3 xF

Where FM is the flexural elastic modulus (MPa), LF is the span between

the two supports (mm), wF is the width of foams (mm), tF is the thickness
of foams (mm), FF is the flexural force within the proportional limit (N),
xF is the deformation corresponding to FF (mm).

2.3.4. Uniaxial tensile test

Fig. 1. Schematic diagram of the modeling process. Uniaxial tensile test was conducted by Instron 5865 universal tester.
The foam was cut into a standard spline of 150 × 40mm × 10 mm by
special-shaped cutting machine (the distance between gauges is 50 mm),
Table 1 and the spline was loaded on the tensile module with the distance be­
Material properties of PP used in the simulation. tween fixtures of 100 mm. A prestress of 0.1 kPa was applied to the
Value spline after loading, and then the tensile test was carried out at a speed
Density (kg/m3) 920 [37] of 5 mm/min. The entire test was repeated for at least 5 times. The
Flexural elastic modulus (MPa) 1160 [37] tensile elastic modulus was calculated according to:
Tensile elastic modulus (MPa) 1070 [37]
Poisson ratio 0.42 [38] FT /AT
TM = (3)
xT /tT

Fig. 2. Bubble morphology of different PP foams.

Table 2
Parameters of PP foams with different foaming conditions.
Sample Foaming temperature (◦ C) Foaming pressure (MPa) Expansion ratio Average bubble diameter (μm) Cell density (cells/cm3) Thickness of bubble wall (μm)

I 146 14 26.06 12.26 9.98 × 108 0.078

II 149 10 27.43 34.30 4.97 × 107 0.206
III 152 8 26.01 60.68 8.23 × 106 0.386
IV 147 11 21.22 33.80 4.72 × 107 0.267
V 144 12 16.67 34.02 4.57 × 107 0.347

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Y. Chen et al. Polymer Testing 116 (2022) 107812

Fig. 3. Bubble diameter distribution of PP foams with different expansion ratio and bubble size.

Where TM is the tensile elastic modulus (kPa), FT is the tensile force method to simulate the mechanical properties of PP foams with different
within the proportional limit (N), AT is the area of foams (mm2), xT is the bubble structures. The schematic diagram of modeling is shown in
deformation corresponding to FF (mm), tT is the thickness of foams Fig. 1, a single tetrakaidecahedron unit has spatial defects and cannot be
(mm). directly applied to the calculation of structural mechanics. Therefore, it
is necessary to establish a spatially repeatable unit bubble structure
based on tetrakaidecahedron unit for simulation.
2.4. Finite element simulation of mechanical properties However, since the bubble size is very small compared to the actual
measured size, it is not realistic to completely construct the actual
In order to more intuitively understand the contribution of gas measured size by the finite element method. During all subsequent
counter-acting force and material elastic stress to elastic modulus, a simulations, with the repeatable unit bubble structure as the basic
finite element model for the simulation calculation of polymer me­ structure, the actual size was scaled down for finite element simulation.
chanical properties was established based on Comsol Multiphysics At the same time, the inside of the cell was set to compressible air, thus
software. Structural stress analysis was performed by the finite element simulating the counter-acting force of air. It is worth noting that the

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Y. Chen et al. Polymer Testing 116 (2022) 107812

Fig. 4. (a) Compressive curves and (b) compressive elastic modulus of different PP foams.

Fig. 5. (a) Flexural curves and (b) flexural elastic modulus of different PP foams.

Fig. 6. (a) Tensile curves and (b) tensile elastic modulus of different PP foams.

original sample size is scaled down in the compressive process and in the flexural process simulation) to prevent foams from moving under
flexural process, and the effective section (the section between gauges) the simulation, and the other side (the upper indenter in the flexural
is selected in the tensile process to be scaled down. process simulation) was loaded with displacement to 5% strain. The
The transient research was used. During the simulation, a fixed elastic modulus was calculated by counting the counter-acting force in
boundary condition was used on one side of the foam (the lower support the force direction. At the same time, the air in the model was removed

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Y. Chen et al. Polymer Testing 116 (2022) 107812

Fig. 7. Force analysis of single bubble. Mises stress distribution for (a) compressive process and (b) tensile process under 5% strain; variation of (c) stress and (d) ΔP
with strain.

mainly undergo bending deformation during the compressive process

Table 3 [36], in the simulation of the compressive and flexural processes, the
Parameters obtained from compressive curves of PP foams. flexural elastic modulus of PP was used, while in the simulation of the
Sample ES (MPa) EP (MPa) εA εB β (10− 3) EC (MPa) tensile process, The tensile elastic modulus of PP was used.
I 5.7224 0.1891 0.02129 0.1145 3.985 7.4812
II 5.3775 0.1929 0.01997 0.1212 4.055 6.8918 3. Results and discussion
III 5.0520 0.1984 0.01749 0.1259 4.506 6.4974
IV 6.9768 0.2004 0.02324 0.1042 4.363 9.9335 3.1. Preparation of microcellular PP foams
V 8.3149 0.2292 0.02559 0.0802 4.031 11.6579

In order to explore the structure-activity relationship between the

and the model was re-simulated to calculate the contribution of the bubble structure and mechanical properties, microcellular PP foams
elastic stress of polymer matrix to the elastic modulus. Finally, the dif­ with different bubble morphologies were prepared by supercritical CO2
ference between elastic modulus of foams and elastic stress of polymer moulding compression foaming process. The plasticization of CO2 can
matrix was taken as the contribution of the counter-acting force change the melting behavior of the polymer, so with the increase of CO2
generated by air to the elastic modulus. The elastic modulus (τe ), the pressure, the melting range of the polymer moves to the low tempera­
contribution of polymer matrix to the elastic modulus (τP ), and the ture region. Since the moulding compression foaming process is semi-
contribution of air to the elastic modulus (ΔP) satisfy the following solid foaming, in the high-pressure CO2 environment, the polymer is
relationship: saturated in the second half of the melting range and then foamed.
Therefore, the melting degree of the crystal region in polymer matrix
τe = τP + ΔP (4) can be regulated by adjusting the foaming temperature and foaming
The material properties parameters of air are from material library of pressure, so as to realize the regulation of expansion ratio and bubble
Comsol, while the material parameters of PP used for simulations are size. As shown in Fig. S1, according to our previous work [39], foaming
listed in Table 1, where the flexural modulus and tensile modulus of PP experiment was carried out under the conditions of foaming tempera­
are from the manufacturer. It should be noted that since the bubble walls ture of 144 ◦ C–152 ◦ C and foaming pressure of 8 MPa–14 MPa. The

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Y. Chen et al. Polymer Testing 116 (2022) 107812

Fig. 8. Force analysis of compressive process. Mises stress distribution for different PP foams (a)–(e) under 5% strain, (f) is the comparison of compressive
elastic modulus.

hollow circles in Fig. S1 correspond to the foaming conditions in this size can be prepared. Finally, two series of PP foams were prepared:
work, which are all between the melting point and the ending melting similar in expansion ratio and different in bubble size (Sample (I), (II)
temperature. The larger the deviation of the foaming temperature from and (III)), similar in bubble size and different in expansion ratio (sample
the ending melting temperature at the foaming pressure, the more (II), (IV) and (V)).
crystalline regions in the polymer matrix. Microcellular PP foams were prepared under semi-solid conditions,
The bubble morphology of PP foam is shown in Fig. 2, and the therefore, there were still some crystalline regions in the polymer ma­
foaming process conditions and cell morphology parameters are listed in trix, and the growth of cells was restricted by the crystalline regions.
Table 2. The results show that under high foaming temperature and low Although the average bubble size dose not vary much, there is still dif­
foaming pressure, PP foams with low cell density and large bubble size ferences in bubble size, which can affect the mechanical properties, so it
can be prepared due to the low dissolved CO2 and the low driving force is necessary to investigate the bubble size distribution of PP foams. As
for cell nucleation. Conversely, under low foaming temperature and shown in Fig. 3, there are differences in the bubble size distribution of
high foaming pressure, due to the high dissolved CO2 and the driving sample (I), (II) and (III), and the bubble size of a single sample is less
force of cell nucleation, PP foams with high cell density and small bubble distributed among the characteristic sizes of other samples. Therefore, it

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Y. Chen et al. Polymer Testing 116 (2022) 107812

Fig. 9. (a) Stress of PP matrix and (b) ΔP of air as a function of strain under compressive process of microcellular PP foams.

is believed that the effect of bubble size on mechanical properties can be 3.2.2. Flexural properties of microcellular PP foams
researched through this group of samples. However, sample (II), (IV) Fig. 5 shows the flexural curves and flexural elastic modulus of
and (V) show similar bubble size distribution, which means that their different PP foams. Similar to the law of compressive properties, under
mechanical properties are not greatly affected by bubble size. Therefore, the same expansion ratio, the smaller the bubble size, the higher the
it is believed that the effect of expansion ratio on mechanical properties flexural elastic modulus, and under the same bubble size, the smaller the
can be researched through this group of samples. expansion ratio, the higher the flexural elastic modulus. Although the
laws are similar, the gas in the bubble is hardly compressed during the
flexural measurement, the improvement of the flexural elastic modulus
3.2. Mechanical properties of microcellular PP foams
mainly depends on the properties of PP matrix. Furthermore, since there
is no incomplete contact in the flexural measurement, the flexural elastic
The crystallinity of the polymer matrix significantly affects its me­
modulus is higher than the uncorrected compressive elastic modulus,
chanical properties [40], so before all measurements, the foams were
although the bubble walls are all undergo bending deformation.
annealed in a vacuum oven at 60 ◦ C for 24 h to eliminate the crystallinity
differences caused during the foaming process. As shown in Fig. S2 and
3.2.3. Tensile properties of microcellular PP foams
Table S1, the melting point difference of all samples is less than 1 ◦ C, and
Fig. 6 shows the tensile curves and tensile elastic modulus of
the melting enthalpy difference is less than 0.25 J/g, so it can be
different PP foams. Different from the laws of compressive properties
considered that crystallization has no effect on the measurement of
and flexural properties, the tensile elastic modulus is almost unchanged
mechanical property. At the same time, the melting point and melting
under the same expansion ratio. The reason is that the bubble walls are
enthalpy of the annealed samples are higher than those of the original PP
broken during stretching. Under the similar expansion ratio, smaller
[39], which is due to the more regular crystal arrangement by annealing.
bubble size means thinner bubble walls, which are more prone to break,
resulting in a decrease in its tensile elastic modulus [41]. With the
3.2.1. Compressive properties of microcellular PP foams
decrease of the expansion ratio, the solid content of PP increases, which
Firstly, the compressive properties of PP foams were measured. Fig. 4
leads to the increase of tensile elastic modulus under the same volume. It
(a) shows the compressive curves of five PP foamed samples. It can be
is worth noting that the tensile elastic modulus is always lower than the
intuitively observed from the curves that under similar expansion ratio,
flexural elastic modulus under the same expansion ratio. On the one
the smaller the bubble size, the higher the compressive elastic modulus.
hand, the tensile elastic modulus of the PP matrix is smaller than the
The reason is that during the compressive process, the foam mainly
flexural elastic modulus, and on the other hand, it may be related to the
undergoes bending deformation, and smaller bubble size means thinner
gas pressure inside the bubble, which is discussed in detail in the sub­
bubble wall, which provide more elastic stress [36]. At the same time,
sequent simulation section. Of course, since there is also no incomplete
under the same bubble size, the lower the expansion ratio, the higher the
contact in the tensile measurement, the tensile elastic modulus is higher
compressive elastic modulus. The reason is that the lower expansion
than the compressive elastic modulus, which is consistent with the law
ratio means that the gas content in the foam is lower under the same
in the literature [43].
volume. At this time, the counter-acting force of air generated by
Therefore, for PP foams, under the same expansion ratio, the
compression is weak, and the main contribution of the compressive
reduction of bubble size can improve the compressive elastic modulus
elastic modulus comes from the PP matrix. It is worth noting that at the
and flexural elastic modulus, but has little effect on the tensile elastic
beginning of the compression, the force does not increase linearly with
modulus; under the same bubble size, the reduction of expansion ratio
the deformation. The reason is that it is difficult to ensure the absolute
can simultaneously increase the compressive elastic modulus, flexural
flatness of the sample surface during the compressive measurement of
elastic modulus and tensile elastic modulus.
the foam material, so there is an incomplete contact phenomenon [41].
At the same time, this phenomenon also leads to a low compressive
elastic modulus in the measurement [42], which is corrected in the 3.3. Finite element simulation of mechanical properties
following sections. Fig. 4(b) shows the comparison of the compressive
elastic modulus. It can be found that although the compressive elastic During the measurement of mechanical properties, the elastic
modulus of the sample with smaller bubble size is higher, it is always modulus mainly comes from two aspects: the elastic stress of the poly­
lower than that of the sample with low expansion ratio, which means mer matrix and the counter-acting force generated by the air in the
that the compressive elastic modulus is more significantly affected by bubbles. Therefore, it is necessary to explore the influence of the elastic
the expansion ratio. stress and the counter-acting force of air on the elastic modulus through

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Y. Chen et al. Polymer Testing 116 (2022) 107812

Fig. 10. Force analysis of flexural process. Mises stress distribution for different PP foams (a)–(e) under 5% strain, (f) is the comparison of flexural elastic modulus.

finite element simulation. Since the bubble structure used in simulation is not simulated here.
process was tetradecahedron, and the statistical bubble structure was Fig. 7(a)-(b) shows the stress distribution of the bubble wall for
circle, the bubble size was first converted by the equal volume rule. The compressive and tensile process under 5% strain, respectively. Since the
conversion results are shown in Table S2, where the height refers to the flexural elastic modulus of the PP matrix is higher than the tensile elastic
distance between its lower bottom surface and its upper top surface. modulus, under the same strain, the stress under compressive process is
higher than that of tensile process. However, this phenomenon is
3.3.1. Force analysis of single bubble inconsistent with the actual results, and the main reason is incomplete
In order to understand the stress and gas pressure changes of bubbles contact. Fig. 7(c)–(d) show the variation of total stress, PP matrix stress,
during compressive and tensile process, the bubble parameter of sample and ΔP in the bubble with strain during compressive and tensile process.
(I) was used to simulate the compressive and tensile process of single The total stress was calculated by the counter-acting force of the top
bubble. During the simulation, a fixed boundary condition was applied surface on the z-axis, and the PP matrix stress was calculated by the
to the lower bottom surface, and a displacement was applied to the difference between the total stress and ΔP in the bubble. The results
upper top surface. It should be noted that since bubbles are hardly show that since there is no bubble-to-bubble interaction during the
compressed or stretched during the flexural process, the flexural process simulation of a single cell, the contribution of the bubble pressure to the

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Y. Chen et al. Polymer Testing 116 (2022) 107812

Fig. 11. (a) Counter-acting force on the indenter in the z-axis direction and (b) ΔP of air as a function of strain under flexural process of microcellular PP foams.

total stress is small, only about 1%. Interestingly, during compressive compressive process well. At the same time, the simulated value is al­
process, the pressure inside the bubble keeps increasing, while during ways higher than the experimental value. The main reason is that during
tensile process, the pressure inside the bubble keeps decreasing. The the simulation process, all bubbles are regular and completely closed-
reason is that the gas volume is continuously reduced during the cell structure, while in the actual foams, the difference in bubble size
compressive process and continuously increased during the tensile and existence of open-cell structure is unavoidable, especially open-cell
process, thus resulting in the difference in gas pressure under different structure leads to a decrease in compressive elastic modulus.
stress modes. Fig. 9 shows the stress of PP matrix and ΔP of air as a function of
strain under compressive process, respectively. It can be found that the
3.3.2. Simulation of compressive elastic modulus for microcellular PP law of PP matrix stress is basically consistent with the above discussion.
foams It is worth noting that ΔP changes little under the same expansion ratio,
Before simulating the compressive properties of PP foams, the the reason is that the air volume in the foams is similar, and the counter-
compressive elastic modulus needs to be corrected to eliminate the in­ acting force during compressive process is also similar. The counter-
fluence of incomplete contact. Liu et al. [42] proposed a correction acting force of sample (II) is slightly higher, which is caused by the
method for linear hardening materials, which corrected the compressive larger expansion ratio. At the same time, since the counter-acting force
elastic modulus of solid materials to obtain the corrected modulus close of the gas is almost constant, and the elastic stress of PP decreases with
to the intrinsic modulus. The research object in this work is the foam, the increase of the bubble size, the contribution of the counter-acting
and only the PP matrix has incomplete contact during the compressive force to the compressive elastic modulus increases with the increase of
process. Therefore, the correction method needs to be improved by the the bubble size, which is up to about 13.3%. However, with the decrease
expansion ratio: of the expansion ratio, the counter-acting force generated by air
compression gradually decreases, and its contribution to the compres­
εB + εA /2
β= (5) sive elastic modulus also gradually decreases, which is only less than 5%
Expansion ratio
when the expansion ratio is 16.67. In addition, it can be predicted from
the results that with the increase of expansion ratio, the elastic stress of
(1 − 2β)ES EP
EC = (6) PP matrix will be decreased, and the counter-acting force of air
EP − 2βES
compression will be increased. Therefore, the effect of bubble size on the
Where, β is the volume fraction of incomplete contact, εA is the strain compressive elastic modulus will be decreased.
value at the beginning of the elastic, εB is the strain value of the yield
point, EC is the corrected modulus, ES is the slope of elastic Section, EP is 3.3.3. Simulation of flexural elastic modulus for microcellular PP foams
the slope of hardened section. Fig. 10(a)-(e) show the stress distribution of the bubble wall for
The parameters used in the calculation and the corrected compres­ different PP foams under 5% strain at flexural process, which is similar
sive elastic modulus are shown in Table 3. After the correction, the to the compressive process. The difference is that the stress is only
compressive elastic modulus is increased by 28–42%, which is consistent concentrated near the indenter and the support during the flexural
with the conclusion of Liu et al. [42]. Therefore, the above improvement process. Fig. 10(f) shows the comparison of the flexural elastic modulus
method for the correction model is reasonable. obtained by simulation and experiment, and the flexural elastic modulus
Fig. 8(a)-(e) show the stress distribution of the bubble wall for was calculated by counting the counter-acting force on the indenter in
different PP foams under 5% strain at compressive process. Comparing the z-axis direction. It can be found from the results that the deviation
(I)-(III), it can be found that under the similar expansion ratio, the between the simulated value and the experimental value is not more
smaller the bubble size, the larger the stress on the bubble wall, and than 25% and the model can also simulate the actual flexural process
comparing (II), (IV), (V), it can be found that under the similar bubble well. The difference between the simulated value and the experimental
size, with the increase of the expansion ratio, the air volume in foams value also comes from the incomplete uniformity of the cell structure
increases, so the stress on the bubble wall decreases. Fig. 8(f) shows the and the open-cell structure. At the same time, compared to the
comparison of compressive elastic modulus obtained in different ways. compressive elastic modulus, the flexural elastic modulus is consistently
Since there is no incomplete contact during the simulation, the lower. The reason is that there is almost no counter-acting force of air
compressive elastic modulus obtained from the simulation is closer to during flexural process.
the corrected data. The deviation between the simulated value and the Fig. 11 shows the counter-acting force experienced on the indenter
experimental value is not more than 22%, so the model can simulate the and ΔP of air as a function of strain under flexural process, respectively.

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Y. Chen et al. Polymer Testing 116 (2022) 107812

Fig. 12. Force analysis of tensile process. Mises stress distribution for different PP foams (a)–(e) under 5% strain, (f) is the comparison of tensile elastic modulus.

It is worth noting that due to the different sizes of different samples about 5 Pa at the highest. Therefore, it is difficult for the bubble to
during the simulation process, it is impossible to visually observe the change in volume during the flexural initial stage, which is similar to the
difference through the counter-acting force. For an intuitive compari­ above discussion. However, ΔP increases exponentially with the in­
son, the counter-acting force was corrected to remove the effect of crease of strain. Therefore, when the strain is large to a certain extent,
sample size by: the counter-acting force generated by the bubble compression cannot be
ignored, which may have a certain influence on the flexural strength.
L3Fx L3FA
FFx = 3
× 3
(7)
4wFx tFx dFx 4wFA tFA dFA
3.3.4. Simulation of tensile elastic modulus for microcellular PP foams
Fig. 12(a)–(e) show the stress distribution of the bubble wall for
Where FF is the flexural force, dF is the maximum deformation in
different PP foams under 5% strain at tensile process, and Fig. 12(f)
simulation, subscript x represents sample (II)-(V), subscript A represents
shows the comparison of the flexural elastic modulus obtained by
sample (I).
simulation and experiment. Due to the difference of the elastic modulus
The results show that at the initial stage of bending, ΔP under all
of polymer matrix, the stress of bubble wall in the tensile process is
simulation conditions is almost the same, and at 5% strain, ΔP is only
lower than that in the compressive process. At the same time, as

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Y. Chen et al. Polymer Testing 116 (2022) 107812

Fig. 13. (a) Stress of PP matrix and (b) ΔP of air as a function of strain under tensile process of microcellular PP foams.

Table 4
Elastic modulus prediction of different polymer foams.
Process Density (kg/m3) Bubble size (μm) Elastic modulus (MPa) Contribution of gasa Errora

Experimental value Simulated valuea

Compressive process [44] (PU foams) 35 490 4.15 4.68 21.27% 12.77%
50 412 6.15 6.84 10.59% 11.22%
73 354 13.45 13.90 3.55% 3.35%
Flexural process [45] (Phenolic foams) 140 140 71 77.94 – 9.77%
210 120 190 205.06 – 7.93%
250 115 200 212.98 – 6.49%
290 110 260 267.49 – 2.88%
360 100 270 274.49 – 1.66%
Tensile process [46] (PP foams) 36 40.34 23 25.45 − 3.98% 10.65%
557 2.12 1338 1383.52 − 0.0046% 3.40%
638 1.55 1668 1715.70 − 0.0028% 2.86%
701 1.32 2069 2144.38 − 0.0020% 3.64%
a
Means the data in this work.

discussed in 3.3.1, the tensile elastic modulus obtained from the simu­ modulus of PP microcellular foams in different processes. In order to
lation is lower than the compressive elastic modulus and flexural elastic verify the universality of the model, the elastic modulus of foams with
modulus due to the decrease of gas pressure inside the bubble. It is worth different bubble structures and matrix materials in the literature was
noting that, at the similar expansion ratio, the simulated tensile elastic simulated, and the contribution of the gas in bubbles to elastic modulus
modulus decreases with the increase of bubble size, instead of remaining was also analyzed. The foams during compressive, flexural and tensile
almost constant as in the experimental results. The reason is that there is are polyurethane (PU) foams, PP foams and phenolic foams (PF),
no rupture of the bubble wall during the simulation, and all bubble walls respectively, and the material parameters in the simulation process are
play a role. Although there are differences between the simulated results listed in Table S3. The prediction results are shown in Table 4, and
and the experimental values, the general rule is consistent, and the error detailed calculation results can be seen in Figs. S3–S5. The density and
does not exceed 25%. bubble size of simulated foams are 35–701 kg/m3 and 1.32–490 μm,
Fig. 13 shows the stress of PP matrix and ΔP of air as a function of respectively, which covers common foams. The error between the
strain under tensile process, respectively. The results show that the stress simulated value and the experimental value is less than 13%, and the
of PP matrix and the counter-acting force generated by air during the model can accurately predict the elastic modulus of different foams. At
tensile process are weaker than those during the compressive process the same time, the model is more accurate in predicting high-density
due to the difference in the elastic modulus of polymer matrix and the foams due to the more uniform bubble size and higher closed-cell ratio.
change of the bubble volume. At the same time, due to the decrease of Further analyzing the contribution of the counter-acting force of gas
the gas pressure inside the bubble during the tensile process, its effect on to the elastic modulus, it can be found that during the compressive
the elastic modulus is completely opposite to that during the compres­ process, compared with the microcellular PP foams, although the elastic
sive process. Under the similar expansion ratio, with the increase of modulus of PU matrix is higher, the stress of PU matrix during
bubble size, the weakening of the tensile elastic modulus by the gas compressive process is lower due to the larger bubble size of PU foams,
pressure is greater, which is up to about 12.9%; under the similar bubble and finally, the gas in bubbles contributes more to the elastic modulus,
size, with the decrease of expansion ratio, the weakening of the tensile up to 21.27%. During the flexural process, the gas in PF produces a
elastic modulus by the gas pressure is smaller, which is only 5.3% when smaller counter-acting force due to the higher density. During the tensile
the expansion ratio is 16.67. process, due to the higher elastic modulus of PP matrix in the literature,
the counter-acting force of gas has a weaker weakening effect on the
3.3.5. Prediction for elastic modulus of foams tensile elastic modulus, and at higher density, the weakening effect of
The above calculation model of elastic modulus was used to the gas is less than 0.005%, which is almost negligible.
comprehensively analyze the influence mechanism for the elastic

12
Y. Chen et al. Polymer Testing 116 (2022) 107812

4. Conclusion org/10.1016/j.polymertesting.2022.107812.

In this work, a series of microcellular PP with bubble diameter of References

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