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Predicting The Stress Relaxation Behavior of Glass-Fiber Reinforced
Predicting The Stress Relaxation Behavior of Glass-Fiber Reinforced
A R T I C LE I N FO A B S T R A C T
Keywords: It is well established that the addition of short elastic fibers slows the relaxation process in composites, but this
Polymer-matrix composites (PMCs) phenomenon is not well-understood. Our recent study explained changes in the stress relaxation constant by
Short-fiber composites accounting for the time-dependent interfacial shear stress transfer at the fiber-matrix interface. An analytical
Stress relaxation model was developed and was successfully compared to finite-element experiments. This approach represents a
Modelling
significant departure from the previously published literature, where the effect of fibers on viscoelasticity was
Stress transfer
typically attributed to changes in the covalent bonds at the fiber-matrix interface. In the present study, the stress
relaxation behavior of glass fiber-reinforced polypropylene composites was experimentally measured and
compared to analytical model predictions. Further, the effect of additional covalent bonding at the fiber-matrix
interface was studied experimentally by introducing an interfacial coupling agent. Good agreement was obtained
between the experimental data and the analytical model and it was concluded that most of the stress relaxation
behavior of a composite can be predicted using a model that only accounts for the time-dependent matrix
modulus and a time-dependent shear stress transfer efficiency.
1. Introduction observed to slow the rate of stress relaxation of a composite [3–7]. This
has been a subject of interest because elastic fibers do not exhibit time-
Short, elastic fibers are routinely incorporated in polymers to im- dependent behavior, but nevertheless appear to do so when embedded
prove mechanical properties such as modulus and strength. The static in a viscoelastic matrix. The explanation for this observation remains
properties of polymers and their composites are relatively simple to elusive and previous studies in literature have focused on attributing
understand: the addition of a stiff, elastic reinforcing phase into a softer the effect of fibers on stress relaxation to chemical bonding at the fiber/
polymer matrix typically increases both stiffness and strength. There is matrix interface [8–12]. These studies have proposed that covalent
a substantial body of theory to predict these mechanical properties interfacial bonds between the two phases inhibit polymer mobility and
based on the size, shape, and orientation of the reinforcing phase [1,2]. thus slow stress relaxation.
The viscoelastic properties of composites are significantly more In a previous paper, we proposed a novel explanation for the effect
complex. The time-dependent properties of the matrix makes polymer- of elastic fibers on the stress relaxation of polymer matrix composites
based composites prone to creep and stress relaxation, which is a [13]. We proposed that the time-dependent shear stress transfer at the
challenge when considering composites for long-term applications. A fiber-matrix interface, and not increased covalent bonding at the in-
better understanding of composite viscoelasticity is needed in order to terface, was primarily responsible for altering the non-linear viscoe-
provide guidance for optimizing composite structure, and for predicting lasticity of the composite. In that study, a quantitative model was de-
long-term properties. veloped based on composite micromechanics, and was used to predict
Stress relaxation is a straightforward way of characterising polymer the stress relaxation of composites without postulating changes in
viscoelasticity. Since all viscoelastic properties stem from the same structure near the fiber interface.
basic mechanisms, a model for composite stress relaxation would also There have been other attempts to model the behavior of viscoe-
provide insight into composite creep and dynamic mechanical beha- lastic and viscoplastic matrices reinforced with elastic fibers. Several
vior. studies have used a tensor approach to model the full stress field around
The addition of short fibers in a composite has been repeatedly elastic inclusions in viscoelastic matrices [14–16]. This approach,
∗
Corresponding author.
E-mail address: mark.kortschot@utoronto.ca (M.T. Kortschot).
https://doi.org/10.1016/j.compscitech.2018.04.004
Received 18 November 2017; Received in revised form 1 April 2018; Accepted 4 April 2018
Available online 05 April 2018
0266-3538/ © 2018 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY license (http://creativecommons.org/licenses/BY/4.0/).
N. Obaid et al. Composites Science and Technology 161 (2018) 85–91
though accurate, does not provide a simple analytical model useful for Table 2
predicting stress relaxation in a short fiber reinforced polymer as a Experimental design for this study.
function of fiber loading and aspect ratio. Sample PP GF MAPP Replicates
There is also an extensive body of literature for high volume fraction
continuous fiber composites, where at high stress, fiber breakage results Set 1: Samples without MAPP S1 100% – – 5
S2 90% 10% – 5
in concentrated matrix shear stresses near the end of the broken fibre,
S3 80% 20% – 3
and the decay of these stresses with time has been modelled [17–19]. S4 70% 30% – 4
Solutions to such problems tend to be quite specific for the particulars
of the geometry chosen [20,21], although the conceptual underpinning Set 2: Samples with MAPP S5 95% – 5% 5
is the same. Fibre fracture can be modelled with a Weibull approach S6 85% 10% 5% 5
S7 75% 20% 5% 5
[22–25], and understanding the causes and evolution of fibre fractures
S8 65% 30% 5% 5
is often the focus of these studies.
The purpose of the present study was to compare the experimental
stress relaxation behavior of glass fiber-reinforced polypropylene 2.3. Fiber characterization
composites to predictions from a simplified analytical model.
Additionally, the hypothesis that there is additional covalent bonding at The fiber orientation in the samples was examined via x-ray tomo-
the fiber-matrix interface on the stress relaxation behavior of compo- graphy. The post-processing aspect ratio of the fibers was measured by
sites was examined experimentally. examining 100 fibers for each fiber content after a matrix burnout at
600 °C for 6 h. The post-processing fiber aspect ratio was not observed
to vary with fiber content significantly.
2. Experimental
2.4. Stress relaxation tests
2.1. Sample preparation
The stress relaxation samples were milled from a region near the
Two batches of glass fiber reinforced polypropylene composites edge of the injection molded flexural modulus samples where the fibers
were prepared: one without any compatibilizer or coupling agent and were well oriented. The final samples had an approximate dimension of
another containing maleic anhydride-grafted polypropylene (MAPP, 3.5 mm (W), 1.3 mm (T) and 26 mm (L). The stress relaxation behavior
5% by weight) to improve interfacial bonding. Polypropylene (with and was evaluated using a TA Q800 Dynamic Mechanical Analyser (DMA)
without MAPP) was first melted in a C.W. Brabender Compounder with a tensile clamp. The tests were conducted at 30 °C with a soaking
(Type R.E.E.6) at 185 °C and 20 RPM for 10 min. Glass fibers were time of 150 min to ensure that the entire thickness of the sample had
added to the mixer and the mixing speed was increased to 60 RPM, and reached the target temperature, followed by the application of a con-
the compound was mixed for five additional minutes. The details of all stant strain of 0.05% for 90 min.
the chemical components used in this study are summarized in Table 1.
The compounded mixture was granulated using a C.W. Brabender
3. Analytical model
Granulator (Model S9-10). The samples were prepared via an Engel ES-
28 injection molder with an injection temperature of 210 °C, an injec-
The analytical model proposed previously was based on the shear-
tion time of 8 s, a cooling time of 38 s, and a mold opening time of 2 s.
lag theory, as defined by Cox [26]. Although the theory has been ex-
The injection mold produced ASTM tensile, flexural and impact test
tensively used to understand and predict the elastic properties of
specimens.
composites, it had not been used to predict their stress relaxation be-
havior before our work [13]. The previously developed analytical
model can be best understood by first examining the elastic case pre-
2.2. Experimental design
sented in Cox's shear-lag theory.
The composites examined in this study consisted of 10%, 20%, and
30% mass fraction of fibers (5%, 10%, and 15% by volume). Table 2 3.1. Elastic properties
summarizes all the samples that were prepared for this study and the
number of replicates conducted for each sample. The stress-relaxation In short-fiber composites, the fiber end faces are assumed to carry
behavior of the composites without MAPP was compared to that of neat no load, and the stress-transfer between the fiber and matrix occurs
polypropylene without MAPP (S1). Similarly, the stress relaxation be- through shear stresses stemming from the significant mismatch in the
havior of composites with MAPP was compared to neat polypropylene modulus of the matrix and fiber. Upon tensile loading the matrix re-
containing MAPP (S5). A comparison between samples S1 and S5 (see mote from the fiber is assumed to experience the global strain applied
Table 2) was also conducted to determine whether or not the presence to the composite. However, the matrix adjacent to the fiber is assumed
of MAPP resulted in any changes to the properties of the base matrix to be bonded to the fiber and thus constrained, creating a gradient of
itself. stress within the matrix, and shear stresses at the interface (Fig. 1).
Based on the ratio of the matrix and fiber moduli, a fraction of the fiber
will experience maximum tensile strain while a fraction near the ends
will experience both shear strain and tensile strain; the tensile strain
Table 1
increases inwards from the fiber ends. Accordingly, only a fraction of
Details of the chemical components used in the study.
the fiber length will experience maximum tensile stresses, while a
Component Company Product Name fraction near the ends of the fiber will experience tensile stresses less
Polypropylene Total Petrochemicals PP3622
than the maximum. The total contribution of a fiber to the composite
Inc. modulus depends on the average tensile stress over its entire length.
E-Glass Fibers Johns Manville StarStrain EC14
738
3.2. Stress relaxation behavior
Maleic anhydride grafted Eastman G-3003 Polymer
polypropylene (MAPP)
In the case of a viscoelastic matrix, where the Young's modulus of
86
N. Obaid et al. Composites Science and Technology 161 (2018) 85–91
tanh (n (t ) s ) ⎞
Ec (t ) = Vm Em (t ) + Vf Ef ⎛1 −
⎜ ⎟
⎝ n (t ) s ⎠ (1)
1
2
⎡ ⎤
⎢ 4 ⎥ 1
n (t ) = ⎢ ⎥ [Gm (t )] 2
⎢ Ef ln
⎣
() Pf
Vf ⎥
⎦ (2)
Fig. 2. In a stress relaxation test, stresses in the fiber decrease over time due to the decay in the matrix modulus during stress relaxation.
87
N. Obaid et al. Composites Science and Technology 161 (2018) 85–91
Fig. 3. The glass fibers were well-oriented within the matrix in the direction of loading (Vf = 5%)
Fig. 4. Post-processing fiber aspect ratios were measured via matrix burnout; approximately 100 fibers were measured at each fiber content.
88
N. Obaid et al. Composites Science and Technology 161 (2018) 85–91
Fig. 7. The effect of MAPP addition on the stress relaxation behavior of the base
polymer was evaluated by comparing the behavior of polypropylene without
MAPP [S1 (○)] to polypropylene with MAPP [S5 (●)].
89
N. Obaid et al. Composites Science and Technology 161 (2018) 85–91
4. Conclusions
90
N. Obaid et al. Composites Science and Technology 161 (2018) 85–91
Acknowledgements 437–445.
[13] N. Obaid, M.T. Kortschot, M. Sain, Understanding the stress relaxation behavior of
polymers reinforced with short elastic fibers, Materials 10 (2017) 472.
The authors gratefully acknowledge the National Science and [14] I. Sevostianov, V. Levin, E. Radi, Effective viscoelastic properties of short-fiber re-
Engineering Research Council of Canada (NSERC) for financial support. inforced composites, Int. J. Eng. Sci. 100 (2016) 61–73.
[15] N. Smith, G.A. Medvedev, R.B. Pipes, Viscoelastic shear lag analysis of the dis-
continuous fiber composite, Proceedings of the 19th International Conference on
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