Polymer Degradation and Stability 183 (2021) 109410

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Polymer Degradation and Stability

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

Constitutive modeling of γ -irradiated silicone rubber foams under

compression and shear loading
Dong Jia a,b, Shunping Yan a,b,∗, Yunqiang Peng a, Liming Wei a, Luobin Wang a, Yang Gao a,
Zhiming Hao a, Yong Qiu c, Qiang Wan a
a
Institute of Systems Engineering, China Academy of Engineering Physics, Mianyang, Sichuan 621999, PR China
b
Shock and Vibration of Engineering Materials and Structures Key Laboratory of Sichuan Province, Mianyang, Sichuan 621999, P.R China
c
China Academy of Engineering Physics, Mianyang, Sichuan 621999, P.R China

a r t i c l e i n f o a b s t r a c t

Article history: Under the service conditions of nuclear engineering applications, silicone rubber foams should endure
Received 15 June 2020 radiation of γ rays accompanied by compression and shear loading. In this paper, the Hyperfoam model
Revised 26 September 2020
is extended to characterize the mechanical behaviors of silicone rubber foams under γ -irradiation. After
Accepted 22 October 2020
exposing silicone rubber foams to a wide radiation dose range from 0 to 500 kGy at room temperature,
Available online 23 October 2020
uniaxial compression and simple shear tests were carried out to establish the relationships between the
Keywords: model parameters of Hyperfoam model and radiation dose, and indentation tests were performed to ver-
Silicone rubber foams ify the extended Hyperfoam model. The linear radiation dose-related hardening properties of the material
γ -irradiation are derived using the testing results, including the linear increases of the initial shear modulus, and the
Hyperfoam model compression stress and the shear stress for a given strain condition, which result in the linear radiation
Uniaxial compression dose-dependent relationships for the initial shear modulus-related model parameters and the radiation
Simple shear
dose-independent hardening exponent-related model parameters of Hyperfoam model. The performances
Indentation test
of the extended Hyperfoam model are demonstrated by comparing the fitted material responses with
uniaxial compression and simple shear data. And the prediction ability is verified by comparing the sim-
ulated results of indentation using the finite element method with the test data. The extended model is
capable of characterizing the coupling stress state of compression and shear in the investigated irradia-
tion dose range, which is expected to aid in evaluating the safety of nuclear engineering structures.
© 2020 Elsevier Ltd. All rights reserved.

1. Introduction
Silicone rubber foams are commonly foamed from silicone rub-
ber matrix, including the main components of polysiloxane, voids,
fillers and other additives [1]. They are widely used in aerospace,
weapon systems and nuclear plants as typical sandwich structures
or cushion structures, owing to their high weight-to-volume ratio,
preferred thermal and chemical stability, and excellent mechani-
cal properties [2–4]. In the service environments, the mechanical
properties of silicone rubber foam structures deteriorate over time
as a result of the extremely harsh conditions, including the γ -
irradiation [4]. For example, the cushion structure made of silicone
rubber foams in nuclear power plants requires to bear thousands
of kGy of γ -irradiation dose [5]. Because γ -irradiation changes the
microstructure of rubber matrix by the crosslinking and scission
reactions of polymer chains, the mechanical properties of silicone
∗
Corresponding author.
E-mail address: 402yansp@caep.cn (S. Yan).
rubber foams change with γ -irradiation dose [4,6,7]. Prior to the
formation of products in engineering and manufacture, the me-
chanical behaviors of silicone rubber foam structures strongly de-
pend on the result of numerical analyses by computer simulation
[8]. To describe the mechanical behaviors of silicone rubber foams
under the service condition accurately, it is necessary to establish
a constitutive model to consider the γ -irradiation effect.
In particular, there are two kinds of modeling methods to char-
acterize the mechanical responses for rubber foams. The first kind
is based on the mesoscopic structures of the material, including
the rubber matrix and the distribution of voids [9–13]. After ac-
quiring the distribution of voids using a scanning reconstruction
tool (such as micro X-ray CT [13]), a representative volume includ-
ing the solid mesh structure and several voids is constructed. Ap-
plying the finite element method to simulate the mechanical be-
haviors of the representative volume, the macroscopic response of
the rubber foam is obtained by averaging the values of the rep-
resentative volume. Although different rubber foam materials can
be characterized by changing the constitutive model of the matrix

https://doi.org/10.1016/j.polymdegradstab.2020.109410
0141-3910/© 2020 Elsevier Ltd. All rights reserved.
D. Jia, S. Yan, Y. Peng et al.
from the representative volume, such as the γ -irradiation dose-
related constitutive model for silicone rubber [14,15], this method
is not efficient for engineering application, and convergence prob-
lems caused by the instability of the void deformation appears
occasionally. Furthermore, the equivalence for the mechanical re-
sponse of mesoscopic structure with that of macroscopic struc-
ture is still in doubt, and the scale effect of the representative vol-
ume cannot be ignored [11–13]. The second kind is based on the
phenomenological constitutive model of rubber foams, which con-
tains the contributions from shape deformation of rubber matrix
and compressible deformation of voids [16]. To characterize the ef-
fects of material properties and environmental variables using the
phenomenological model, model parameters have been associated
with density, strain rate and temperature [17]. One of the most
successful models to describe the stress–strain response of rub-
ber foams is Hyperfoam model, which has been widely used in the
commercial finite element software (such as ABAQUS), owing to its
flexibility for modeling static as well as time-dependent responses
of rubber foams [18,19]. With the help of Hyperfoam model, the
macroscopic mechanical response of rubber foams is simulated di-
rectly by the homogenized finite element model [20,21]. The Hy-
perfoam model is efficient and can avoid the disadvantages of the
first kind of modeling method. However, few works have been
done to correlate the model parameters of Hyperfoam model with
irradiation dose [22]. In this paper, we extended the Hyperfoam
model based on the experimental results to include the effect of
γ -irradiation on mechanical behaviors of silicone rubber foams.
Studies have shown that the prediction accuracy of the Hyper-
foam model is directly proportional to the number of test data
used in parameter fitting procedure [2,23–25]. Many experimental
results have been used to construct the constitutive models of sil-
icone rubber foams, including uniaxial compression, uniaxial ten-
sion, creep, and stress relaxation [17,26–28], but the coupling ef-
fects of several stress states are lacking [24]. It has been demon-
strated that the Hyperfoam model fitted from a single stress–strain
state can only characterize the corresponding deformation behav-
ior, and cannot correctly predict the responses of the complex de-
formation states [23,24]. The reason is attributed to the nonlinear
mechanical properties induced by the hyper-elasticity and com-
pressibility of silicone rubber foams [29,30]. Owing to the diversity
of loading conditions for engineering structures, rubber foams bear
not only compression stress but also shear stress, especially when
it is used on inclined or curved surfaces [31]. The slipping phe-
nomenon occurs occasionally between the upper and lower sur-
faces of the foamed structure, which inevitably leads to shear de-
formation of rubber foams. Therefore, uniaxial compression and
simple shear test data are commonly used for model parameters
fitting [32]. For irradiated silicone rubber foams, a set of model pa-
rameters can be fitted using the experimental data under a given
radiation dose condition. Different groups of model parameters can
be obtained by fitting test data for samples irradiated with differ-
ent irradiation doses. A phenomenological approach to establish
the relationships between model parameters and radiation dose
is adopting a phenomenological function to fit model parameters
with radiation dose. In this way, it is difficult to give a clear phys-
ical explanation for model parameters, and the parameters cannot
be generalized to other engineering applications. Hence, further
study is required to establish the physical relationships between
model parameters of Hyperfoam model and γ -irradiation dose, es-
pecially to describe the coupling state of compression and shear.
This paper aims to get an accurate constitutive model to char-
acterize the mechanical behaviors of silicone rubber foams irra-
diated by γ -irradiation. First, uniaxial compression, simple shear
and indentation tests were carried out in Section 2. Next, analy-
ses and discussion about the effect of γ -irradiation on mechani-
cal behaviors of unirradiated and irradiated silicone rubber foams
2
Polymer Degradation and Stability 183 (2021) 109410
Fig. 1. Illustrations of (a) the macroscopic samples and (b) the mesoscopic cells of
silicone rubber foam achieved by micro X-ray CT.
were given in Section 3. Based on the experimental findings, the
Hyperfoam model was extended to characterize the mechanical
behaviors of unirradiated and irradiated silicone rubber foams in
Section 4, by establishing the relationships between model param-
eters and radiation dose. Section 5 provides the model parameters
fitted using uniaxial compression and simple shear data, and gives
the comparisons of indentation test data with simulated results
to verify the model prediction ability about the coupling stress
state of compression and shear. Finally, the concluding remarks are
given in Section 6.
2. Materials and experimental setups
2.1. Materials and samples
The silicone rubber foams used in this paper were synthesized
from silica-reinforced silicone rubber gum stock which contained
100 phr silicone rubber, 12.5 phr hydroxyl silicone oil, 38 phr
fumed silica (5 phr silazane has been used to reduce the density
of hydroxyl radical on the surface), 5 phr ZnO Whisker and 3 phr
Fe2 O3 . The spherical urea particles were mixed into silicone rubber
gum stock as the pore-forming agent. The average diameter of the
spherical urea particle is approximately 300 μm. Then the mix-
ture was poured into two kinds of synthesized molds. One mold
was used to form the cylindrical specimens for uniaxial compres-
sion test. Another mold was used to form the cuboidal samples for
simple shear test. The molds were placed in the plate vulcanizing
machine for vulcanization at a constant temperature (100 ◦ C) for
12 h. After vulcanizing, the urea particles were washed off with
sufficient distilled water. Then, the washed samples were placed in
the oven for drying and post-curing at a constant temperature (200
◦ C) for 4 h. Finally, the samples of silicone rubber foam were ob-
tained. The density of the samples was approximately 0.52 g/cm3
and the porosity was approximately 55%. The diameter and height
of the cylindrical sample were 28 mm and 12 mm, respectively.
The length, width and thickness of the cuboidal sample were 19
mm, 14.5 mm and 10 mm, respectively. The pictures of the macro-
scopic samples are shown in Fig. 1 (a), and the mesoscopic cell
morphology achieved by micro X-ray CT is shown in Fig. 1 (b). As
shown in Fig. 1 (b), the shape of the voids is nearly circle and no
residual urea has been found.
2.2. Irradiation
Each kind of sample was divided into six groups, one of which
was not irradiated, and the other five groups were irradiated in
air at room temperature by γ rays from a 60 Co source provided by
Institute of Nuclear Physics and Chemistry, China Academy of Engi-
neering Physics, with the cumulative irradiation doses 50 kGy, 150
kGy, 300 kGy, 400 kGy and 500 kGy, respectively. The irradiation
dose rate was selected as 60 Gy/min.
D. Jia, S. Yan, Y. Peng et al. Polymer Degradation and Stability 183 (2021) 109410

Fig. 2. The experimental setups for (a) uniaxial compression and (b) simple shear
tests.

2.3. Uniaxial compression and simple shear tests

To investigate the compression and shear mechanical behav-

iors of silicone rubber foams, the uniaxial compression and sim-
Fig. 3. The experimental setup of indentation test.
ple shear tests were carried out on the material testing machine
with a calibrated 1 kN load cell. Tests were implemented with
the displacement control mode at room temperature. As shown in
Fig. 2(a), the uniaxial compression tests were carried out directly
by compressing the cylindrical sample between two parallel steel
plates. For the simple shear tests shown in Fig. 2(b), the sample
was pasted on two parallel steel plates and sheared by the tension
force applied on the plates. To stick the sample on two parallel
steel plates, we first spread the epoxy glue evenly on the inner
surfaces of two parallel steel plates, and then pasted the sample
on the steel plate to ensure that the sample does not slip during
the simple shear test. To obtain the stable stress–strain response of
silicone rubber foams, four cycles of loading–unloading were car-
ried out in uniaxial compression and simple shear tests. The first
three cycles were applied to ensure that the mechanical proper-
ties of the silicone rubber foams had reached a stable state and
the Mullins effect could be ignored [33]. In this way, the radiation
dose effect on the silica-rubber interface has been ignored, owning
to the Mullins effect-related interface interaction has been reduced
by cyclic loading and unloading. A low loading rate 5 mm/min was
Fig. 4. Relationship between initial shear modulus and irradiation dose.
selected to avoid the viscoelastic effect. The time interval between
every cycle was set as 1 min for deformation recovery. The maxi-
mum compression strain is 50% and the maximum shear strain is
load–displacement responses of silicone rubber foams, four cycles
40%. For uniaxial compression and simple shear tests, three sam-
of loading–unloading were performed for each sample. Also, three
ples were tested for each irradiation dose condition. The averaged
samples for every radiation dose condition were tested to ensure
loading force and displacement data of the fourth loading cycle for
the repetition of the test. The average load–displacement values of
the three samples were used to calculate the nominal compres-
the last cycle for the three samples were used to represent the in-
sion stress Tc , nominal compression strain ε , nominal shear stress
dentation responses of silicone rubber foams.
Ts and nominal shear strain γ based on the initial thickness and
initial cross-section area of the sample.
3. Test results and discussion

2.4. Indentation test

3.1. Effect of radiation dose on initial shear modulus

The indentation tests were performed to verify the proposed

The initial shear modulus G was defined as the secant modu-
model in the following section of this paper. To obtain the non-
lus of nominal shear stress–strain curves for shear strain ranging
uniform compression and shear stress state, a hemispherical in-
from γ = 0 to γ = 0.05, where the linearity in this range can
denter was selected to perform the indentation tests on silicone
be guaranteed. The relationship between G and radiation dose is
rubber foams as done by the previous studies [24,34]. The in-
given in Fig. 4. It is shown that G increases linearly with irradi-
denter is made of stainless steel with a diameter of 20 mm. The
ation dose, namely, the radiation dose-related hardening effect as
samples used in the indentation tests were the cylindrical sam-
found by Fang et al. for tension tests of unirradiated and irradiated
ples which had been tested in the uniaxial compression tests.
silicone rubber foams [7]. The values of initial shear modulus are
The experimental setup is shown in Fig. 3. During the indenta-
so small that only 0.6 MPa is obtained for the radiation dose con-
tion, the bottom surface of the cylindrical sample was bonded to
dition of 500 kGy. Based on Fig. 4, a linear function can be used to
a plate, and the top surface was indented vertically in the center
fit the initial shear modulus G as
by the indenter. The loading rate was 5 mm/min, and the max-
imum indentation displacement was 5 mm. To obtain the stable G = 0.297 + 0.311D/Dr , (1)

3
D. Jia, S. Yan, Y. Peng et al.
Fig. 5. Comparisons of the nominal stress–strain curves of silicone rubber foams
under (a) uniaxial compression and (b) simple shear with theoretical model for dif-
ferent irradiation dose conditions. The error bars represent the corresponding stan-
dard deviation values.
where the unit for G is “MPa”, D is the radiation dose and Dr is the
reference dose which is selected as 500 kGy in this paper. In fact,
the initial shear modulus is mainly related to mechanical proper-
ties of silicone rubber matrix. The deformation of silicone rubber
matrix is dominated by the entropy variation of polymer chains,
which is proportional to the cross-link density of the silicone rub-
ber matrix [35]. Under γ radiation, the cross-link density of sili-
cone rubber increases linearly with radiation dose up to 1600 kGy
[36]. Therefore, the linear function of Eq. (1) defines the evolution
of cross-link density for the irradiated silicone rubber matrix. In
the following section, Eq. (1) was used to establish the radiation
dose-related constitutive model for silicone rubber foams.
3.2. Effects of radiation dose on uniaxial compression and simple
shear
According to the experimental methods presented in
Section 2.3, the nominal compression stresses and nominal
shear stresses of silicone rubber foams irradiated at different
irradiation dose conditions were given in Fig. 5. Also, the corre-
sponding standard deviation values were depicted as error bars.
Fig. 5(a) shows that the nominal compression stresses increase
slowly when the strain is less than 0.1, and increase rapidly
4
Polymer Degradation and Stability 183 (2021) 109410
Fig. 6. Relationships between nominal stresses for the given strain conditions and
irradiation doses under (a) uniaxial compression and (b) simple shear tests.
when the strain is more than 0.4. The reason is attributed to the
nonlinear deformation modes of cell structures [29,30]. Because
the maximum compression strain (50%) is lower than the porosity
(55%) of the material, the bending and elastic buckling of cell
walls are the main mesoscopic deformation modes, which only
require a small increment of stress [37]. However, owing to the
inhomogeneity of cell distribution as shown in Fig. 1 (b), after cell
walls collapsing under large strain, large forces are required to
deform the crushed structures than the uncrushed ones. Fig. 5(b)
shows that the shear stress increases approximately linearly with
the increase of shear strain. It is owing to the combined effects of
compression and tension on the mesoscopic deformation of cells
under the simple shear loading. The cell walls bend, rotate and
align in tension loading direction, so the platform of stress–strain
curve caused by the buckling of cell walls does not appear in
nominal shear stress–strain curves of Fig. 5(b) [38]. In Fig. 5, both
compression stiffness and shear stiffness for a given strain are
increase with radiation dose, namely, the radiation dose-related
hardening effect. To highlight the hardening behaviors induced by
γ -irradiation, Fig. 6(a) shows the relationships between nominal
compression stresses and radiation dose for the given nominal
compression strains ε = 0.1, 0.2, 0.3, 0.4 and 0.5, and Fig. 6(b)
shows the relationships between nominal shear stresses and
D. Jia, S. Yan, Y. Peng et al. Polymer Degradation and Stability 183 (2021) 109410

Fig. 8. Load–irradiation dose curves for the given displacements of 1 mm, 2 mm, 3
Fig. 7. Comparisons of the predicted load–displacement curves with experimental
mm, 4 mm and 5 mm for indentation tests.
data in indentation tests. The error bars represent the standard deviation values.

sion of the compressible function was refined by Hill and Storak-

radiation dose for the given nominal shear strains γ = 0.1, 0.2,
ers [44,45]. The compressible hyperelastic model was further in-
0.3 and 0.4. The linear relationships between the stresses and
troduced into ABAQUS software and named as ‘Hyperfoam model’.
radiation dose in Fig. 6 indicate the linear hardening mechanical
The Hyperfoam model is widely used for describing mechanical
behaviors induced by γ -irradiation for silicone rubber foams. The
behaviors of rubber foam materials. It is based on the strain en-
mechanical properties of silicone rubber foams are mainly affected
ergy function U, which is expressed as
by the mechanical properties of silicone rubber matrix and the
 
deformation modes of cell structures. Therefore, the reasons for   −α β 
2 μi 
N 3
αi 1
the hardening of the irradiated silicone rubber foams include two U= λj − 3 + J i i
−1 , (2)
factors. First, γ -irradiation causes the predominated crosslinking i=1
αi 2 j=1
βi
reactions of the molecular chains in rubber matrix, so the rubber
matrix hardens [39]. Second, although the cell structures are where N is the order of the model, μi , αi and βi are the model
not significantly affected by γ -irradiation even under 500 kGy parameters, and λ j (j = 1, 2, 3) is the principal stretch. In ad-
condition, which is consistent with the previous work [40], the dition, βi is related to the Poisson’s ratio νi by the expression
hardening of rubber matrix leads to the change of deformation βi = νi /(1 − 2νi ). And J is the volume ratio which is defined as
resistance ability of cell walls [41,42]. J = λ1 λ2 λ3 .
To describe the mechanical responses of silicone rubber foams,
the second-order Hyperfoam model has been chosen in the previ-
3.3. Effect of radiation dose on indentation
ous studies [37,38,46], owing to its well prediction property and
stability with a few model parameters. In this paper, the compar-
Fig. 7 gave the load–displacement curves for the unirradiated
isons of the fitted results from the Hyperfoam model of order 1
and irradiated cylindrical samples under indentation, including
and order 2 with uniaxial compression data showed that the first-
the error bars about the standard deviation values of the loads.
order Hyperfoam model had a great deviation from experimental
It is shown that the loads increase nonlinearly with displace-
data and the second-order Hyperfoam model had a good perfor-
ments. The secant stiffness increases with displacement, namely,
mance. Hence, the second-order Hyperfoam model was adopted to
the indentation-related hardening effect. The reason is attributed
characterize the mechanical behaviors of unirradiated and irradi-
to the dramatic changes of cell structures induced by the cou-
ated silicone rubber foams. Therefore, we have N = 2. For uniax-
pling effects of compression stresses and shear stresses. The col-
ial compression test, the principal stretches in the loading direc-
lapsed cells require a larger load to deform than the complete
tion and the other two transverse directions can be redefined as
ones. Furthermore, Fig. 7 shows that γ -irradiation enhances the
λ1 = λ and λ2 = λ3 = λT , respectively. Therefore, the volume ratio
indentation-related hardening effect. The indentation loads for a
is J = λ1 λ2 λ3 = λλT . The nominal stresses (T1 , T2 and T3 ) in the
2
given indentation displacement increase with radiation dose. To
three corresponding principal directions are
highlight the enhancement of γ -irradiation on the indentation-
related hardening effect, Fig. 8 gave the indentation load–radiation ∂U 2 2
μi  αi  2 −αi βi 
dose curves for the given indentation displacements of 1 mm, 2 T1 = = λ − λλT , (3)
∂λ λ i=1 αi
mm, 3 mm, 4 mm and 5 mm. It is shown that the indentation
loads increase linearly with radiation dose, indicating that the ra-
diation dose-related linear hardening effect is also true for the cou- ∂U 2  μi
2   −αi βi 
T2 = T3 = = λT αi − λλT 2 = 0. (4)
pling state of compression and shear under indentation. ∂λT λT i=1 αi

4. Constitutive modeling and numerical simulation
4.1. Hyperfoam constitutive model
In 1972, Ogden proposed a
ible materials [43], by adding a
hyperelastic constitutive model
tion of compressible materials.
Because the porosity of silicone rubber foams studied in this
paper is high (55%), the transverse deformation of the sample dur-
ing uniaxial compression is so small that can be ignored, and we
have βi = νi = 0, λT = 1 and Eq. (4) is satisfied automatically. The
constitutive model for compress- nominal compression stress can be redefined as
compressible term on the basis of
to describe the volume deforma- ∂U 2 2
μi αi
Tc = T1 = = (λ − 1 ). (5)
Subsequently, the specific expres- ∂λ λ i=1 αi

5
D. Jia, S. Yan, Y. Peng et al. Polymer Degradation and Stability 183 (2021) 109410

For simple shear test, the thickness and volume of the sam- which indicates that the hardening exponent-related model pa-
ple remain unchanged during the loading process, so we have rameters αi are independent of radiation dose. Introducing
λ3 = 1 and J = λ1 λ2 λ3 = λ1 λ2 = 1. Therefore, the in-plane princi- Eq. (9) and (13) into Eq. (5) and (7), we extended Hyperfoam
pal stretches λ1 and λ2 can be derived as functions of the shear model to describe the effect of radiation dose on mechanical be-
strain γ , which are haviors of silicone rubber foams with the functions
μ D + μ D μ Dr + μ2D D α2 

2
Tc =
10 r 1D
(λα1 − 1 ) + 20 (λ − 1 ) ,
γ 2 γ 2
λ α1 Dr α2 Dr
λ1,2 = 1+ ±γ 1+ . (6)
2 4 (14)

The nominal shear stress can be expressed as 
2
2γ
μ D + μ D 
  Ts =   10 r 1D
λαj 1 − 1
∂U  2
2γ 
2
μi  αi  2 λj − 1 − γ
2 2 α1 Dr
Ts = =  2  λj − 1 . (7) j=1

∂γ 2 λ j − 1 − γ i=1 αi

2
j=1
μ20 Dr + μ2D D  α2
+ λj − 1 . (15)
α2 Dr
4.2. Effect of γ -irradiation on model parameters

The Hyperfoam model is a phenomenological constitutive 4.3. Fitting procedure of model parameters
model, which contains the macroscopic shape deformation of sili-
cone rubber matrix and compression deformation of voids. Micro- For the extended Hyperfoam model of Eq. (14) and (15), there
scopic properties, such as the changes of cross-link density induced are 6 model parameters required to be determined, including μ10 ,
by γ -irradiation, are difficult to be included in Hyperfoam model. μ1D , α1 , μ20 , μ2D and α2 . Based on Eq. (10), we have μ10 =
In this paper, the effect of γ -irradiation on mechanical properties (0.297 − μ20 )MPa and μ1D = (0.311 − μ2D )MPa, so the number of
of silicone rubber foams is introduced indirectly by establishing re- model parameters is reduced to 4. All the data of uniaxial com-
lationships between the model parameters and irradiation dose D. pression and simple shear for unirradiated and irradiated silicone
In general, the parameters μi and αi can be defined as μi = fi (D ) rubber foams were used to fit model parameters of the extended
and αi = gi (D ). In this way, the extended Hyperfoam model can Hyperfoam model. And the optimization method of minimizing the
be applied conveniently in the finite element models to investigate comprehensive relative error was used to determine the model pa-
mechanical behaviors of irradiated silicone rubber foams. To ob- rameters [48]. The relative error function is defined as
tain expressions of fi (D ) and gi (D ), the relationships between ex-  2 2 
perimental data and model parameters were further analyzed. The 
R 
6
Tc th (λi , Dk ) Ts th (λi , Dk )
ED = 1− + 1− ,
comparison of Hyperfoam model with small-strain elastic theory
i=1 k=1
Tc test (λi , Dk ) Ts test (λi , Dk )
provides the relationship [47]
(16)
G = μ1 + μ2 . (8)
in which Tc (λi , Dk ) and Tc (λi , Dk ) are the nominal compres-
th test

Furthermore, the linear relationship between G and D is given sion stresses for the condition of stretch λi and radiation dose
in Eq. (1). So the simplified radiation dose-related definitions about Dk obtained from theoretical model and test, Ts th (λi , Dk ) and
μ1 and μ2 are Ts test (λi , Dk ) are the nominal shear stresses for the condition of
μ1 = μ10 + μ1D D/Dr , stretch λi and radiation dose Dk obtained from theoretical model
(9) and test, R represents the number of fitted test points, and Dk
μ2 = μ20 + μ2D D/Dr ,
(k = 1, 2, · · · 6) denotes the radiation doses of 0 kGy, 50 kGy, 150
where μ10 , μ20 , μ1D and μ1D are model parameters. For the ma- kGy, 300 kGy, 400 kGy and 500 kGy, respectively. The build-in op-
terial studied in this paper, the comparison between Eq. (9) and timization function “fmincon” in MATLAB software was adopted
(1) gives that to minimize ED with nonlinear least square method. Setting five
groups of the initial parameters in advance, the model parameters
μ10 + μ20 = 0.297 MPa,
(10) can be derived numerically. After obtained the model parameters,
μ1D + μ2D = 0.311MPa.
the stable condition that the initial shear modulus G is positive has
To get values of gi (D ), the radiation dose-related hardening be- been checked. And the parameters satisfying the stable condition
haviors of the nominal compression stress Tc in Eq. (5) and the have been adopted.
nominal shear stress Ts in Eq. (7) were investigated. In Fig. 6, the
linear hardening behaviors induced by radiation dose for the given 4.4. Numerical simulation
strain conditions denote that
   The indentation tests of unirradiated and irradiated silicone
∂ Tc  2  ∂ μi λαi − 1
2
∂ λαi − 1
= + μi = const, (11) rubber foams were simulated using ABAQUS/Standard software
∂ D λ λ i=1 ∂ D αi ∂D αi [23]. The prediction accuracy of the extended Hyperfoam model
   α was verified by comparing the simulation results with experimen-
∂ Ts  2
2γ 2
∂μi λ j i − 1
=   tal data. In the numerical simulation, the axisymmetric finite el-
∂ D γ j=1 2 λ j − 1 − γ 2 i=1 ∂ D
2 αi ement model was adopted according to the symmetrical property
αi  of indentation test, as shown in Fig. 9. The indenter and sample
∂ λj − 1
+ μi = const. (12) were meshed using four-node linear reduced integration elements
∂D αi (CAX4R), and the dimensions were consistent with the experimen-
tal conditions. The bottom surface of the cylindrical sample was
Because Eq. (11) is true for all values of λ, Eq. (12) is true for
completely constrained, and a compression displacement ranging
all values of γ and λj , and μi is a linear function about radiation
from 0 to 5 mm was applied by the steel indenter. The contact
dose D, we have
type between the hemispherical surface and the upper surface of
αi ≡ const, (13) the sample was surface to surface without friction as done by Li

6
D. Jia, S. Yan, Y. Peng et al.
Fig. 9. Finite element model for indentation test.
Table 1
Model parameters estimated using data of uniaxial compression and simple shear.
μ10 [MPa] μ20 [MPa] μ1D [MPa] μ2D [MPa] α 1 [-]
0.2969 6.0029E-5 0.3109 1.2446E-4 2.3679
et. al. [49]. The elastic modulus of steel indenter was set as 210
GPa and Poisson’s ratio was 0.3. The material property of silicone
rubber foams in finite element model was defined by the extended
Hyperfoam model defined in Section 4.2.
5. Characterization results and discussion
Firstly, the model parameters of the extended Hyperfoam model
were estimated based on the parameter fitting procedure proposed
in Section 4.3. The discrete experimental data of uniaxial com-
pression and simple shear for the parameter fitting procedure are
listed in Tables A.1 and A.2 of the supplementary material. Nu-
merical calculation for the parameter fitting procedure was im-
plemented in MATLAB. The fitted model parameters are listed in
Table 1, where the number of significant digits for the fitted model
parameters is selected as more than four to improve the numeri-
cal accuracy of the model. In addition, the values of R-square for
Tc and Ts about each radiation dose condition are listed in Table 2.
Fig. 10. Illustrations of (a) the deformation state from indentation test, and (b) displacement contours, (c) compression stress contours, (d) shear stress contours from
numerical simulation for the sample irradiated with 150 kGy.
Polymer Degradation and Stability 183 (2021) 109410
Table 2
Values of R2 for Tc , Ts , and indentation loads.
Dose [kGy] R2 [%]
Tc Ts Indentation loads
0 99.61 99.45 99.66
50 99.82 99.60 99.85
150 99.90 99.70 99.94
300 99.82 99.55 99.81
400 99.88 99.44 99.80
500 99.77 99.46 99.77
The larger the R-square value is, the better fitting quality is ob-
tained by the fitted model. It is evident that all the values of R-
square are more than 99%. The high values of R-square indicate
that the extended Hyperfoam model fits test data well, which is
demonstrated in Fig 5 for the comparisons of Tc and Ts with test
data. Based on Fig. 5(b), there is still some noticeable departure
of the fitted shear stresses from the experimental data, especially
when the shear strain γ > 25%. Two reasons can be used to ex-
plain this derivation. On the one hand, the local debonding phe-
nomenon may occur at the sample-steel plate interface under a
α 2 [-] great shear strain condition. The shear stress-strain data may have
-14.3983
a certain deviation under large shear strain condition. On the other
hand, the second-order Hyperfoam model has a poor prediction
about the nonlinear responses of silicone rubber foams under the
large shear strain condition [32].
According to the numerical simulation method in Section 4.4,
the extended Hyperfoam model with fitted model parameters of
Table 1 were used to simulate the indentation test. The predicted
load–displacement curves of the numerical model were compared
with experimental data for different irradiation dose conditions in
Fig. 7, where the discrete experimental data are listed in Table
A.3 of the supplementary material. It shows that the indentation
load increases nonlinearly with the increase of indentation dis-
placement. The R-square values of indentation loads between the
numerical results and test data are listed in Table 3. All the val-
ues of R-square are more than 99%, indicating that the extended
Hyperfoam model can reproduce the mechanical responses of the
cylindrical samples under indentation. To further illustrate the dis-
tributions of displacement and stresses for the indentation test,
taking the sample irradiated with 150 kGy as an example, the de-
formation state and stress distributions of the cylindrical sample
at the maximum compression displacement (5 mm) are shown in
7
D. Jia, S. Yan, Y. Peng et al.
Fig. 10. Fig. 10(a) showed that a dimple-shaped deformation ap-
peared on the upper surface of the sample when the steel indenter
was loaded downward, and the circumferential bulging deforma-
tion occurred, which were consistent with the numerical results il-
lustrated in Fig. 10(b). Figs. 10 (c) and 10 (d) gave the compression
stress and shear stress distributions of the sample when indenter
reaching the end of indentation. The maximum compression stress
was approximately 0.84 MPa, which was located at the center of
the upper surface. The maximum shear stress was approximately
0.20 MPa, which was located on the slope of the dimple with a
ring distribution. Hence, the stress state of the indented sample is
a coupling state with compression and shear stresses, which can
be captured by the extended Hyperfoam model. In conclusion, the
extended Hyperfoam model can be used to analyze the mechanical
behaviors of the silicone rubber foams under the coupling stress
state of compression and shear in nuclear engineering applications.
6. Conclusions
In this paper, the effect of γ -irradiation on the mechanical be-
haviors of silicone rubber foams was investigated by uniaxial com-
pression, simple shear and indentation tests. Within the studied ir-
radiation dose range from 0 to 500 kGy, γ -irradiation leads to the
linear hardening mechanical behaviors for the material, where the
initial shear modulus, the compression stress and shear stress for
a given strain condition, and the indentation force for a given in-
dentation displacement increase linearly with irradiation dose. The
reasons are attributed to the radiation dose-related linear hard-
ening of the silicone rubber matrix and the changes of deforma-
tion resistance ability for cell walls induced by γ -irradiation. The
Hyperfoam model was extended to describe the radiation dose-
related mechanical behaviors of the silicone rubber foams. For
the extended Hyperfoam model, the initial shear modulus-related
model parameters showed explicitly the linear correlation with ir-
radiation dose, the hardening exponent-related model parameters
were independent of irradiation dose, and the effective Poisson’s
ratio-related parameters were approximated to zero. The extended
second-order Ogden Hyperfoam model was used to fit the uni-
axial compression and simple shear test data. The performances
of the extended Hyperfoam model were demonstrated by compar-
ing the fitted material responses with experimental data. The pre-
diction ability of the extended Hyperfoam model was verified by
comparing the simulated results of indentation using the finite ele-
ment method with test data. The results indicate that the extended
model is capable of characterizing the coupling compression-shear
stress state of silicone rubber foams in the investigated irradiation
dose range. The model is expected to aid in predicting mechanical
responses of silicone rubber foams under γ -irradiation and evalu-
ating the safety of nuclear engineering structures.
Declaration of Competing Interest
The authors declare that they have no known competing finan-
cial interests or personal relationships that could have appeared to
influence the work reported in this paper.
CRediT authorship contribution statement
Dong Jia: Investigation, Software, Validation, Formal analysis,
Writing - original draft. Shunping Yan: Conceptualization, Method-
ology, Formal analysis, Writing - review & editing, Visualization.
Yunqiang Peng: Validation, Data curation. Liming Wei: Investi-
gation, Data curation. Luobin Wang: Investigation, Data curation.
Yang Gao: Investigation, Resources. Zhiming Hao: Supervision,
Project administration. Yong Qiu: Supervision, Project administra-
tion. Qiang Wan: Supervision, Project administration.
8
Polymer Degradation and Stability 183 (2021) 109410
Acknowledgments
We acknowledge the financial supports from NSAF (Grant No.
U1530259), Science Challenge Project (Grant No. TZ2018007) and
National Natural Science Foundation of China (Grant No. 11602254
and 11632001).
Supplementary materials
Supplementary material associated with this article can be
found, in the online version, at doi:10.1016/j.polymdegradstab.
2020.109410.
References
[1] A.H. Landrock, Handbook of Plastic Foams: Types, Properties, Manufacture and
Applications, Noes Publications, Park Ridge, 1995.
[2] B. Sanborn, B. Song, S. Smith, Pre-strain effect on frequency-based impact en-
ergy dissipation through a silicone foam pad for shock mitigation, J. Dynam.
Behav. Mater. 2 (2016) 138–145.
[3] T. Métivier, P. Cassagnau, Foaming behavior of silicone/fluorosilicone blends,
Polymer 146 (2018) 21–30.
[4] A. Maiti, T. Weisgraber, R. Gee, Modeling the Mechanical and Aging Properties
of Silicone Rubber and Foam-Stockpile-Historical & Additively Manufactured
Materials, Lawrence Livermore National Lab., Livermore, United States, 2014.
[5] Y. Gong, S. Hu, X. Yang, J. Fei, Z. Yang, X. Shi, Y. Xie, A. Guo, J. Xu, Compar-
ative study on degradation of ethylene-propylene rubber for nuclear cables
from gamma and beta irradiation, Polym. Test. 60 (2017) 102–109.
[6] B. Liu, P. Wang, Y. Ao, Y. Zhao, Y. An, H. Chen, W. Huang, Effects of combined
neutron and gamma irradiation upon silicone foam, Radiat. Phys. Chem. 133
(2017) 31–36.
[7] H. Fang, J. Li, H. Chen, B. Liu, W. Huang, Y. Liu, T. Wang, Radiation induced
degradation of silica reinforced silicone foam: experiments and modeling,
Mech. Mater. 105 (2017) 148–156.
[8] J.D. Hoffman, S. Frankel, Numerical Methods for Engineers and Scientists, 2 ed.,
CRC Press, Boca Raton, 2018.
[9] H. Wang, W. Hu, F. Zhao, Numerical simulation of quasi-static compression on
a complex rubber foam, Acta Mech. Solida Sin. 30 (2017) 285–290.
[10] T.M. Gebhart, D. Jehnichen, R. Koschichow, M. Müller, M. Göbel, V. Geske,
M. Stegelmann, M. Gude, Multi-scale modelling approach to homogenise the
mechanical properties of polymeric closed-cell bead foams, Int. J. Eng. Sci. 145
(2019) 103168.
[11] A. Roberts, E.J. Garboczi, Elastic properties of model random three-dimensional
open-cell solids, J. Mech. Phys. Solids 50 (2002) 33–55.
[12] C. Tekog, L. Gibson, T. Pardoen, P. Onck, Size effects in foams: experiments and
modeling, Prog. Mater Sci. 56 (2011) 109–138.
[13] K. Natesaiyer, C. Chan, S. Sinha-Ray, D. Song, C. Lin, J. Miller, E. Garboczi,
A. Forster, X-ray CT imaging and finite element computations of the elastic
properties of a rigid organic foam compared to experimental measurements:
insights into foam variability, J. Mater. Sci. 50 (2015) 4012–4024.
[14] A. Maiti, R.H. Gee, T. Weisgraber, S.C. Chinn, R.S. Maxwell, Constitutive mod-
eling of radiation effects on the permanent set in a silicone elastomer, Polym.
Degrad. Stab. 93 (2008) 2226–2229.
[15] A. Maiti, T. Weisgraber, L.N. Dinh, R.H. Gee, T. Wilson, S.C. Chinn, R.S. Maxwell,
Controlled manipulation of elastomers with radiation: Insights from mul-
tiquantum nuclear-magnetic-resonance data and mechanical measurements,
Phys. Rev. E 83 (2011) 031802.
[16] G.A. Holzapfel, Nonlinear Solid Mechanics, John Wiley and Sons, New York,
2001.
[17] L.J. Gibson, M.F. Ashby, Cellular Solids: Structure and Properties, 2 ed., Cam-
bridge University Press, Cambridge, 1997.
[18] N.J. Mills, Finite element models for the viscoelasticity of open-cell
polyurethane foam, Cell. Polym. 25 (2006) 293–316.
[19] A. Kossa, S. Berezvai, Visco-hyperelastic characterization of polymeric foam
materials, Mater. Today-Proc. 3 (2016) 1003–1008.
[20] C. Briody, B. Duignan, S. Jerrams, J. Tiernan, The implementation of a visco-hy-
perelastic numerical material model for simulating the behaviour of polymer
foam materials, Comp. Mater. Sci. 64 (2012) 47–51.
[21] M. Rubin, L. Dorfmann, A hyperelastic model for soft polymer foam including
micromechanics of porosity, J. Elasticity (2019) 1–16.
[22] B. Fazekas, T.J. Goda, Determination of the hyper-viscoelastic model parame-
ters of open-cell polymer foams and rubber-like materials with high accuracy,
Mater. Des. 156 (2018) 596–608.
[23] A. Donnard, S. Guerard, L. Maheo, P. Viot, G. Rio, Multiaxial experiments with
radial loading paths on a polymeric foam, Polym. Test. 67 (2018) 441–449.
[24] M. Petre, A. Erdemir, P. Cavanagh, Determination of elastomeric foam param-
eters for simulations of complex loading, Comput. Methods Biomech. Biomed.
Eng. 9 (2006) 231–242.
[25] A. Kossa, A new biaxial compression fixture for polymeric foams, Polym. Test.
45 (2015) 47–51.
[26] C. Wei, A. Lu, S. Sun, X. Wei, X. Zhou, J. Sun, Establishment of constitutive
model of silicone rubber foams based on statistical theory of rubber elasticity,
Chin. J. Polym. Sci. 36 (2018) 1077–1083.
D. Jia, S. Yan, Y. Peng et al.
[27] R.B. Malla, M.R. Shrestha, M.T. Shaw, S.B. Brijmohan, Temperature aging, com-
pression recovery, creep, and weathering of a foam silicone sealant for bridge
expansion joints, J. Mater. Civ. Eng. 23 (2011) 287–297.
[28] M. Patel, M. Soames, A.R. Skinner, T.S. Stephens, Stress relaxation and ther-
mogravimetric studies on room temperature vulcanised polysiloxane rubbers,
Polym. Degrad. Stab. 83 (2004) 111–116.
[29] H. Iba, Y. Nishikawa, K. Urayama, Nonlinear stress-strain behavior of elas-
tomer foams investigated by various types of deformation, Polymer 83 (2016)
190–198.
[30] W. Tang, X. Liao, Y. Zhang, J. Li, G. Wang, G. Li, Mechanical–microstructure
relationship and cellular failure mechanism of silicone rubber foam by the
cell microstructure designed in supercritical CO2 , J. Phys. Chem. C 123 (2019)
26947–26956.
[31] U.E. Ozturk, G. Anlas, Finite element analysis of expanded polystyrene foam
under multiple compressive loading and unloading, Mater. Des. 32 (2011)
773–780.
[32] M.R. Shariatmadari, R. English, G. Rothwell, Effects of temperature on the
material characteristics of midsole and insole footwear foams subject to
quasi-static compressive and shear force loading, Mater. Des. 37 (2012)
543–559.
[33] L. Mullins, Softening of rubber by deformation, Rubber Chem. Technol. 42
(1969) 339–362.
[34] S. Kim, H. Shin, S. Rhim, K.Y. Rhee, Calibration of hyperelastic and hyperfoam
constitutive models for an indentation event of rigid polyurethane foam, Com-
pos. Part B-Eng. 163 (2019) 297–302.
[35] T. Rey, G. Chagnon, J.-B.L. Cam, D. Favier, Influence of the temperature on the
mechanical behaviour of filled and unfilled silicone rubbers, Polym. Test. 32
(2013) 492–501.
[36] C.G. Delides, I.W. Shepherd, Dose effects in the crosslinking of irradiated
polysiloxane, Radiat. Phys. Chem. 10 (1977) 379–385.
[37] A. Maiti, W. Small, J.P. Lewicki, S.C. chinn, T.S. Wilson, A.P. Saab, Age-aware
constitutive materials model for a 3D printed polymeric foam, Sci. Rep. 9
(2019) 15923.
Polymer Degradation and Stability 183 (2021) 109410
[38] A.A. Siranosian, R.R. Stevens, in: Developing an Abaqus Hyperfoam Model for
M9747 (4003047) Cellular Silicone Foam, Los Alamos National Laboratory Re-
port, 2012, pp. 1–21.
[39] A. Labouriau, C. Cady, J. Gill, J. Stull, D. Ortiz-Acosta, K. Henderson, V. Hartung,
A. Quintana, M. Celina, Gamma irradiation and oxidative degradation of a sili-
ca-filled silicone elastomer, Polym. Degrad. Stab. 116 (2015) 62–74.
[40] H. Chen, B. Liu, W. Huang, W. Wu, Gamma radiation induced effects of com-
pressed silicone foam, Polym. Degrad. Stab. 114 (2015) 89–93.
[41] A. Labouriau, C. Cady, J. Gill, D. Taylor, A. Zocco, J. Stull, K. Henderson, D. Wrob-
leski, The effects of gamma irradiation on RTV polysiloxane foams, Polym. De-
grad.Stabil. 117 (2015) 75–83.
[42] L.A. Lubbers, M. van Hecke, C. Coulais, A nonlinear beam model to describe
the postbuckling of wide neo-Hookean beams, J. Mech. Phys. Solids 106 (2017)
191–206.
[43] R.W. Ogden, Large deformation isotropic elasticity–on the correlation of theory
and experiment for incompressible rubberlike solids, P. Roy. Soc. Lond A Mat.
326 (1972) 565–584.
[44] R. Hill, Aspects of invariance in solid mechanics, Adv. Appl. Mech. 18 (1978)
1–75.
[45] B. Storakers, On material representation and constitutive branching in finite
compressible elasticity, J. Mech. Phys. Solids 34 (1986) 125–145.
[46] A. Kossa, S. Berezvai, Novel strategy for the hyperelastic parameter fitting pro-
cedure of polymer foam materials, Polym. Test. 53 (2016) 149–155.
[47] R.W. Ogden, Non-Linear Elastic Deformations, Dover Publications, New York,
1984.
[48] M.Y. Ali, W. Lai, J. Pan, Computational models for simulation of a lithium-ion
battery module specimen under punch indentation, J. Power Sources 273
(2015) 448–459.
[49] B. Li, Y.D. Gu, R. English, G. Rothwell, X.J. Ren, Characterisation of nonlinear
material parameters of foams based on indentation tests, Mater. Des. 30 (2009)
2708–2714.