Model Prediction Fractre
Model Prediction Fractre
a r t i c l e i n f o a b s t r a c t
Article history: This study presents a methodology to evaluate the performance of different models used in predicting
Received 27 August 2015 the fracture toughness of polymeric particles nanocomposites. Three analytical models are considered:
Received in revised form the model of Huang and Kinloch, the model of Williams, and the model of Quaresimin et al. The purpose
18 January 2016
behind this study is not to recommend which of the three models to be adopted, but to evaluate their
Accepted 8 February 2016
Available online 15 February 2016
performance with respect to experimental data. The Bayesian method is exploited for this purpose based
on different reference measurements gained from the literature. The models' performance is compared
and evaluated comprehensively accounting for the parameter and model uncertainties. Based on the
Keywords:
Nano particles
approximated optimal parameter sets, the coefficients of variation of the model predictions to the
Fracture toughness measurements are compared for the three models. Finally, the model selection probability is obtained
Modelling with respect to the different reference data.
© 2016 Elsevier Ltd. All rights reserved.
1. Introduction have been carried out in order to study the fracture behavior of
polymer/particle nanocomposites ([3e12] among others). On the
Polymeric nanocomposites (PNCs) are commonly formed by an other hand, researchers developed numerical and analytical
epoxy matrix reinforced with a nanosized filler. Due to its inherent methods to get a better understanding of nanocomposite material
characteristic of high crosslink density, an epoxy polymer is known behavior. A close form formula of energy dissipation due to the
to be a relatively brittle material [1]. Nanofillers have shown great interfacial debonding between the particles and matrix was given
improvements in the physical and mechanical properties of epoxy- by Chen et al. [13] considering the effect of particle sizes. Although,
reinforced PNCs. Specifically, they have increased the fracture the increased fracture energy of rubber-toughened epoxy polymers
toughness compared to pristine epoxy. PNCs have numerous ap- was calculated by Huang and Kinloch [14], the model has been
plications in nanotechnology such as: nano-biotechnology, nano- modified for PNCs by Refs. [7,8,10]. The improvement in the fracture
systems, nanoelectronics, and nano-structured materials. Gener- toughness was attributed to two major mechanisms: localized
ally, there are three categories of fillers: nanoparticles, nanoplatelet plastic shear banding and debonding of silica nanoparticles. Further
(layered), and nanofibrous materials. For this scale, the surface area experimental studies also have implied this supposition [15e17].
- to - volume ratio is significantly large. Therefore, the composite According to the assumption of Williams [18], the energy dissipa-
properties are highly modified due to the extreme interfacial area tion is induced by the growth of plastic voids around debonded
between the nanofiller and the matrix [2]. Several experiments particles. The author concluded a large toughness increase for
nanosize particles. Later, his work has been extended to cylindrical
rods and fibres [19,20]. Quaresimin et al. [21] proposed a multiscale
* Corresponding author. approach to predict the overall increase in the fracture toughness
** Corresponding author. Division of Computational Mechanics, Ton Duc Thang taking into account three different damage mechanisms: particle
University, Ho Chi Minh City, Viet Nam
debonding, plastic yielding of nanovoids, and shear banding of the
E-mail addresses: [email protected] (K.M. Hamdia), timon.
[email protected] (T. Rabczuk). polymer. Based on experimental data gathered from the literature,
http://dx.doi.org/10.1016/j.compscitech.2016.02.012
0266-3538/© 2016 Elsevier Ltd. All rights reserved.
K.M. Hamdia et al. / Composites Science and Technology 126 (2016) 122e129 123
a stochastic approach has been presented to predict the fracture to their popularity and their applicability to different experimental
energy of PNCs by Ref. [22]. studies. Moreover, they produce explicit predictions of the
In general, all models inherently underlie an amount of un- enhanced fracture energy of PNCs. Regarding the different theory
certainties which can be related to the model itself and/or its input and mechanism assumed, each of them has its own input param-
parameters. The former might be caused by the simplifications of eters in addition to the joint parameters. Table 1 includes the def-
the physical behavior, while the latter can be related to the number initions of the parameters and their stochastic variation. The
and the stochastic variance of the input parameters. Better pre- uniform distribution was assumed for the parameters uncertainty.
dictions and the subsequent decrease in the model uncertainty are The upper and the lower limits of distributions were mostly pro-
expected by introducing more factors in the model (increasing the posed according to our previous studies [22,28].
model complexity). However, the parameters uncertainties become
more dominant in this case. In light of this, the model with mini-
mum total uncertainty is the most appropriate model, see Fig. 1
[23].
2.1. Huang and Kinloch
In recent years, Bayesian method has been introduced as an
effective tool for evaluating models considering the model and
The model according to Huang and Kinloch [14] was first
parameters uncertainties based on measurements as reference data
developed for the toughening mechanisms of rubber-modified
[24e27].
epoxy polymers and more recently it has been modified for PNCs
This paper is the first attempt to consider the model and pa-
[7,8,10]. The localized plastic shear banding and debonding of
rameters uncertainties in the assessment of the models used for the
nanoparticles which enable plastic void growth of the epoxy matrix
prediction of the fracture energy of PNCs. It aims at presenting a
are the two terms that taking part in the overall enhancement in
methodology to evaluate three different analytical models by using
the fracture toughness of PNCs, while rubber-bridging mechanism
the Bayesian method. In particular, Huang and Kinloch model [14], was disregarded. These two mechanisms are demonstrated in
Williams model [18], and the model according Quaresimin et al.
Fig. 2.
[21] are examined. The purpose of the study is not to give a general The improved fracture energy of PNCs, GIc, is expressed as
recommendation which of the three model to use, but to evaluate
their performance with respect to experimentally tested data se-
GIc ¼ GIm þ DGs þ DGv (1)
ries. The assessment is carried out based on different reference data
(experimental measurements) gathered from the literature [3e12]. where GIm is the fracture energy of the matrix, and DGs and DGv are
Nevertheless, the same methodology can be applied to evaluate the the contribution from the localized shear banding and the plastic
three models based on other measurements. The prior probabilities void growth, respectively.
are first estimated considering the uncertainties in the parameters. The term DGs is given by
Then we find the optimum parameter set which results in best fit of
models prognoses and in consequence the coefficient of variation of
1
the models predictions to the measurements are estimated. Even- DGs ¼ V syc gf F 0 ry (2)
2 f
tually, the model selection probability is calculated.
The remainder of this paper is organized as follows. In Section 2, where Vf is the volume fraction of the nano-filler, gfm is the matrix
the considered models are briefly described. Section 3 presents the shear fracture strain, and syc is the yield stress of the epoxy matrix
method for evaluating the models. Finally, the conclusion of this under compression, which related to the tensile yield stress, sym, by
research is presented in Section 4. Ref. [5].
pffiffiffi !
2. Models for predicting the fracture properties of PNCs
3 þ mm
syc ¼ sym pffiffiffi (3)
Three existing models were chosen to be evaluated; the model 3 mm
of Huang and Kinloch [14], the model of Williams [18], and the
model of Quaresimin et al. [21]. Hereafter, they are abbreviated by mm is a material constant (pressure coefficient).
M1, M2, and M3, respectively. These models have been selected due The parameter F'(ry) is a geometric term given by Ref. [15].
2 !1=3 3 5=2
4p 8 rn rn rn
F ry ¼ ry 4
0
1 1
3Vf 5 ry ry ry
3
16 rn 7=2 rn 2 165
2 1 þ (4)
35 ry ry 35
2
m
ry ¼ 1 þ pmffiffiffi rym Kvm
2
(5)
3
In Eq. (5), rym is radius of the plastic zone of the unmodified
epoxy matrix estimated by Irwin's model [29] and Kvm is the
maximum stress concentration factor of the von Mises stress in the
Fig. 1. Variation in model, parameter, and total uncertainties with respect to the matrix.
number of parameters according to [23]. The term DGv is calculated by
124 K.M. Hamdia et al. / Composites Science and Technology 126 (2016) 122e129
Table 1
The definitions of models' parameters.
2.2. Williams
v
2.3. Quaresimin et al.
v
Vf v Vfp ¼ 1 Vfp (7)
vp
A multiscale methodology has been adopted by Quaresimin
As reported in the studies of [7,17], not all of the nanoparticles et al. [21] to describe the toughening mechanism of PNCs. The
have been observed to be debonded. Finite element simulations authors have considered the interphase zone surrounding the
suggest that around 14% of the particles are debonded [17]. On this nanoparticle to account for the interactions between the nano-
basis, we include a new factor to quantify the percentage of particles and the matrix. The adjacent polymer chains are disor-
debonded particles (Vdp). It has been assumed to vary from 10% to dered due the addition of the nanofiller, leading to the formation of
18%. The volume fraction of debonded particles, Vfp in Eq. (7), is interphase zones surrounding the nanoparticles with properties
substituted by (Vdp)(Vf) different from that of the bulk matrix. The extent of the impact of
particle/polymer interface is principally influenced by the
v manufacturing techniques and the curing processes. The influence
v
Vf v Vfp ¼ 1 Vdp Vf (8) of the interphase was studied experimentally by Refs. [30e33] and
vp
numerically by Refs. [34e37]. Other advanced computational
multiscale methods for crack propagation and material failure were
K.M. Hamdia et al. / Composites Science and Technology 126 (2016) 122e129 125
PðDjMi ÞPðMi Þ
PðMi jDÞ ¼ P (16)
i PðDjMi ÞPðMi Þ
Z [3e12] have been utilized as reference data. For each, Table 2 shows
PðDjMi Þ ¼ PðDjXi ; Mi ÞPðXi jMi ÞdXi (17) the values of the calculated optimal parameter set.
Interestingly, the incorporation of the parameter Vdp in M1 has
enhanced the model predictions to fit the measurements. By the
where PðDjXi ; Mi Þ is the likelihood function and PðXi jMi Þ is the prior finite-element analysis of [45], the value of the maximum stress
probability of the input parameters. concentration for the von Mises stresses around a void, Kvm, was
The likelihood is the joint conditional probability of the refer- estimated to be 2.22 for a matrix of elastic modulus equal 3.2 GPa
ence data, D, given the input parameters, Xi. It measures how the which agrees well with the optimal values obtained in this study.
model fit the data. A higher likelihood factor corresponds to better The interfacial debonding energy, Ga increases as the diameter of
fit of Mi to D. The prior probability of the input parameters char- the nanofiller increases. Its optimal values were in the range of
acterizes what is known about the parameters before any actual [0.184,1.360] and [0.010,0.046] for M2 and M3, respectively. Similar
observation or modelling being considered. In the presence of values of Ga for M2 were reported in Refs. [18] and [20]. The high
measurements and model predictions, the prior probability is value of these results may be explained by assuming that the
updated to posterior probability [43]. optimal values of Ga were reduplicated since the total energy
Assuming that the posterior probability of the parameters is dissipation in M2 was attributed only to one mechanism. Based on
approximated by a Gaussian distribution, the Laplace's method for this, the probability distribution of Ga can be updated to a uniform
asymptotic approximation can be applied to estimate the evidence distribution in the range of [0.1,1.5] for M2 and [0.01,0.1] for M3. The
as [44]. elastic property of the interphase was softer than that of the matrix
h i1 in the measurements; D10 and D11 (c¼1.162 and 1.231, respectively),
P ðDjMi Þ ¼ P D X^i ; Mi P X^i Mi H X^i 2p
2
(18) whereas the matrix showed stiffer elasticity in the remaining
measurements.
where Xbi is the optimal parameter set that maximize the posterior Exploiting the optimal parameter sets, the models predictions
probability and Hð Xbi Þ is the Hessian matrix of versus the nanofiller volume fraction are depicted in Fig. 4. Obvi-
ln½PðDjXi ; Mi ÞPðXi jMi Þ with respect to Xi calculated at Xbi . The ously, M2 and M3 mostly have a similar ascending trend but it dif-
models are compared according to their model selection proba- fers slightly from M1.
bility calculated in Eq. (16). The model with the largest probability The model uncertainty can be demonstrated by the differences
is the optimum one. between the predictions and the measurements. This uncertainty is
In the present work, the models of predicting the fracture en- measured by the coefficient of variation (CV).
ergy of PNCs were evaluated. We considered the model of Huang
vffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
and Kinloch [14] (M1), the model of Williams [18] (M2), and the u
1u X Nj
1
model of Quaresimin et al. [21] (M3), which were described in CVij ¼ t ðDm Yim Þ2 (19)
Section 2. The prior probabilities of these models were assumed to Dj Nj 1 m¼1
be equal, i.e. P(M1) ¼ P(M2) ¼ P(M3) ¼ 1/3.
Thanks to the uniform distribution assumed for the input pa- where Dj and Nj are the mean value and the number of the indi-
rameters, the prior probabilities of the model parameters, PðXi jMi Þ, vidual experiments of the j reference data, Dm is the measured
are constant disregarding the value of the parameter. The input value, and Yim is the corresponding predicted value of the model Mi.
parameters Vf ; dn ; Em ; and GIm were fixed as deterministic param- The CV values for M1, M2, and M3 are shown in Fig. 5. Except of
eters, while we calculated the most probable value (optimal the measurements: D8, D11, D12, and D13, M1 shows better perfor-
parameter value), which realized the best fit of the model pre- mance compared to M2 and M3, where its CV values are the least.
dictions to the measurements, for the remaining parameters. The predictions of M2 have the lowest discrepancies from the
Different experimental measurements gathered from the literature measurements of D11, D12, and D13. M3 produces the best fit
Table 2
The values of the input parameters used in the assessment of the models.
D1 [3] 20 3.20 71.6 0.35 0.732 0.194 2.227 37.7 14.1 72.3 0.36 0.287 85.1 0.36 0.015 0.722 0.184 66.0 3.00 0.882
D2 [3] 20 3.20 115.8 0.36 0.740 0.203 2.216 43.5 11.4 80.0 0.36 0.309 77.6 0.35 0.011 0.746 0.197 52.9 2.26 0.788
D3 [4] 12 3.53 80.5 0.33 0.728 0.206 2.236 25.5 10.4 76.9 0.36 0.184 81.4 0.34 0.013 0.730 0.204 67.3 2.24 0.644
D4 [4] 20 3.53 107.1 0.34 0.730 0.192 2.180 25.5 10.3 86.5 0.36 0.289 110.4 0.34 0.016 0.747 0.184 69.6 1.95 0.670
D5 [4] 40 3.53 118.4 0.34 0.704 0.177 2.108 45.0 13.2 82.7 0.36 0.473 97.0 0.36 0.015 0.727 0.214 59.0 2.90 0.375
D6 [5] 23 3.50 71.6 0.34 0.715 0.210 2.244 25.1 10.8 75.8 0.36 0.250 117.5 0.36 0.010 0.727 0.189 65.1 2.7 0.742
D7 [5] 74 3.50 71.6 0.37 0.745 0.222 2.236 91.2 15.2 75.8 0.35 0.914 110.1 0.34 0.046 0.727 0.188 63.4 2.18 0.447
D8 [6] 20 2.86 118.6 0.34 0.704 0.191 2.110 47.4 16.4 81.7 0.35 0.374 87.2 0.33 0.018 0.713 0.184 68.5 2.97 0.710
D9 [7] 20 2.96 70.5 0.36 0.737 0.205 2.190 25.7 12.5 80.2 0.35 0.310 112.5 0.36 0.011 0.745 0.192 62.6 1.08 0.758
D10 [8] 20 2.41 70.3 0.35 0.747 0.208 2.224 42.2 14.1 73.5 0.36 0.363 94.8 0.35 0.011 0.710 0.187 67.3 1.32 1.162
D11 [8] 80 2.41 70.7 0.36 0.730 0.223 2.239 118.8 17.9 71.5 0.37 1.360 88.5 0.34 0.046 0.716 0.184 63.8 1.20 1.231
D12 [9] 25 3.02 118.4 0.34 0.704 0.177 2.108 29.8 13.3 81.8 0.34 0.340 109.6 0.34 0.012 0.734 0.203 48.3 3.91 0.676
D13 [9] 25 2.78 116.7 0.36 0.704 0.181 2.112 56.6 16.7 72.7 0.34 0.383 87.2 0.34 0.010 0.709 0.220 60.2 3.78 0.656
D14 [10] 20 2.96 71.5 0.37 0.741 0.222 2.229 42.0 13.7 77.4 0.33 0.385 79.0 0.36 0.011 0.708 0.185 50.8 3.43 0.649
D15 [11] 13 2.60 80.6 0.36 0.705 0.181 2.221 35.3 11.1 71.1 0.35 0.224 97.1 0.36 0.010 0.749 0.176 67.4 2.83 0.770
D16 [12] 25 3.27 117.1 0.33 0.708 0.185 2.204 36.4 14.9 83.5 0.36 0.322 110.0 0.36 0.011 0.731 0.215 46.4 3.89 0.830
a
The values of dn and Em are obtained from the corresponding references.
b
These are the optimal values approximated in the current study.
K.M. Hamdia et al. / Composites Science and Technology 126 (2016) 122e129 127
Fig. 4. Predictions of the models using the optimal parameter set for the different reference data.
predictions in the measurements of D8 only. of M2 and M3 have steeper posterior probabilities. Significant
When considering both the model and parameters uncertainties changes in their prognoses are expected due to slight variations in
in the evaluation, M1 outperforms M2 and M3 for all the different the parameters values. One possible explanation is that the natural
measurements. It has significantly higher model selection proba- exponential relation in M2 and in M3 results in high values of the
bility, PðMi jDÞ (See Table 3). It can be concluded that the parameters determinant of their Hessian matrices.
128 K.M. Hamdia et al. / Composites Science and Technology 126 (2016) 122e129
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