Composites Part A 133 (2020) 105895

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Composites Part A
journal homepage: www.elsevier.com/locate/compositesa

Comparative study of fiber reinforced PP composites: Effect of fiber type, T

coupling and failure mechanisms
R. Várdaia,b, T. Lummerstorferc, C. Pretschuhd, M. Jerabekc, M. Gahleitnerc, G. Faludia,b,
J. Móczóa,b, , B. Pukánszkya,b
⁎

a
Institute of Materials and Environmental Chemistry, Research Centre for Natural Sciences, P.O. Box 286, H-1519 Budapest, Hungary
b
Laboratory of Plastics and Rubber Technology, Department of Physical Chemistry and Materials Science, Budapest University of Technology and Economics, P.O. Box 91,
H-1521 Budapest, Hungary
c
Borealis Polyolefine GmbH, St.-Peter-Strasse 25, A-4021 Linz, Austria
d
Competence Centre for Wood Composites and Wood Chemistry (Wood K Plus), Division Biobased Composites and Processes, Altenberger Strasse 69, 4040 Linz, Austria

ARTICLE INFO ABSTRACT

Keywords: A polypropylene (PP) homopolymer was reinforced with carbon fiber, glass fiber and wood flour in order to
A. Fibres compare their advantages and drawbacks. Interfacial adhesion does not influence stiffness, but it affects strongly
B. Impact behavior other properties, i.e. tensile strength and impact resistance. Several local deformation and failure processes take
C. Micro-mechanics place simultaneously or consecutively in the composites during deformation. The fracture of wood fibers is the
D. Acoustic emission
dominating process at good adhesion, while debonding, fiber pullout and fiber fracture occurs in carbon and
glass fiber reinforced composites. Some of the local deformation processes do not result in the failure of the
composites, while others lead to catastrophic failure. A close correlation was found between the characteristic
stress determined by acoustic emission and the mechanical properties of the composites. Composites with ad-
vantageous properties, i.e. large stiffness, acceptable impact resistance and price, can be prepared by the proper
selection of fiber type, composition and interfacial adhesion.

1. Introduction
Polypropylene (PP) is one of the commodity polymers used in the
largest quantities in a wide variety of applications. Besides being rela-
tively cheap, its property profile is excellent, it is light, stiff with good
strength and acceptable deformability. The growth rate of PP produc-
tion is one of the largest among all commodity polymers. Its further
advantage is that it can be modified in various ways to extend its
property profile even further. Blending with elastomers leads to ther-
moplastic elastomers [1], impact modification results in very tough
materials, and fillers as well as fibers can be added to increase its
stiffness, strength and heat deflection temperature [2–8]. Poly-
propylene is extensively used in packaging, for the production of
household utensils and appliances, but also in the automotive industry
[9–11].
Polypropylene is used as structural material in the automotive in-
dustry, which requires sufficient stiffness and dimensional stability
[11]. These properties can be improved by the addition of reinforcing
fibers [4,12]. Glass fiber reinforced grades are commercially available
on the market for a long time and carbon fiber modified PP is also
produced for advanced applications in spite of its higher price [4,13]. In
the last few decades, the reinforcement of PP with wood and natural
fibers came into the focus of attention in both industry and academia
[14–23]. Wood fibers have numerous advantages; they are derived from
natural and renewable resources, they are light, cheap and they im-
prove stiffness, and under appropriate conditions also strength con-
siderably [17–19,24,25]. Environmental considerations are very im-
portant in the application of wood and natural fibers, but the technical
parameters and price of their composites are also quite good [25].
Nevertheless, wood has several drawbacks as well; its properties de-
pend on its source and on the season of harvest, it is sensitive to water
and heat during processing, and its transverse strength is quite small
[26].
Structural applications, especially in the automotive industry, often
require large stiffness and impact resistance simultaneously. The impact
strength of polypropylene homopolymers at the levels of melt flow rate
(MFR) required for complex injection molding (i.e. MFR > 10 g/
10 min at 230 °C/2.16 kg) is usually small, around 2 kJ/m2; the re-
quirement is often 10–15 kJ/m2 or larger. Impact resistance can be
increased by blending, by the introduction of elastomers; often

⁎
Corresponding author at: Institute of Materials and Environmental Chemistry, Research Centre for Natural Sciences, P.O. Box 286, H-1519 Budapest, Hungary.
E-mail address: jmoczo@mail.bme.hu (J. Móczó).

https://doi.org/10.1016/j.compositesa.2020.105895
Received 18 September 2019; Received in revised form 28 March 2020; Accepted 31 March 2020
Available online 02 April 2020
1359-835X/ © 2020 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY license
(http://creativecommons.org/licenses/BY/4.0/).
R. Várdai, et al.
ethylene-propylene (EPR) or ethylene-propylene-diene (EPDM) copo-
lymers are used in the case of PP [27]. However, the addition of such
elastomers decreases the stiffness of the material to below 1 GPa at
large elastomer content, which is not accepted in many applications
[27–29]. The answer of the industry to the problem is the simultaneous
use of an elastomer to increase impact resistance and a filler or fiber to
improve stiffness [28,30–37]. The combination of the three materials
may result in complicated structures, and properties can vary in a wide
range depending on component properties and structure [33–35,38].
Optimization resulted in several commercial grades with acceptable
properties, which contain fillers or fibers to improve stiffness [30–32].
Unfortunately attempts to use wood in such multicomponent materials
proved unsuccessful, although the stiffness of the material reached the
desired level, its impact resistance remained invariably small
[37,39–43].
Although the use of wood flour and natural fibers for the re-
inforcement of PP is widely recommended and numerous studies have
been published on such materials [17–19,44–48], to our greatest sur-
prise hardly any publication is available in the open literature which
compares wood to traditional fibers, i.e. to glass or carbon [49,50].
Consequently, the goal of our study was to compare various fibers as
reinforcements for PP used in structural applications. Carbon fiber,
glass fiber and wood flour were used as reinforcement and attention
was mainly focused on the stiffness and impact resistance of the com-
posites. Besides the identification of the most important factors de-
termining these properties as well as the study of the effect of coupling
on them, special attention was paid to local deformation processes and
their relationship to macroscopic properties. We used acoustic emission
testing and scanning electron microscopy to identify these local de-
formation and failure processes, determined characteristic stresses in-
itiating them and related the obtained values to tensile strength and
impact resistance. The advantages and drawbacks of the various fibers
as well as practical consequences are also discussed briefly at the end of
the paper.
2. Experimental
2.1. Materials
The experiments were carried out with a PP homopolymer as ma-
trix. The polymer was the Daplen HJ 325 MO grade produced and
supplied by Borealis. The melt flow rate (MFR) of the polymer was
50 g/10 min at 2.16 kg and 230 °C, while its density was 0.91 g/cm3.
Interfacial adhesion was modified, improved by the application of a
maleated polypropylene (MAPP) coupling agent. The functionalized
polymer, the Scona 2112 grade, was supplied by Byk-Chemie GmbH.
The polymer contained 0.9–1.2% maleic anhydride (MA) and it had an
MFR of 3.5 g/10 min at 2.16 kg and 190 °C. The functionalized polymer
was used at 10 wt% related to the amount of the reinforcing fiber.
The reinforcing effect of three fibers was compared to each other in
the study. The Panex PX35 grade carbon fiber was obtained from Zoltek
Zrt, Hungary. The diameter of the fiber was 7.2 µm and its stiffness and
strength were 242 and 4.1 GPa according to the data sheet of the
producer. The fiber is recommended for thermoset matrices; it was
sized with an epoxy/polyurethane blend over-coated with a polyester
resin. The amount of carbon fiber changed in the composites from 0 to
50 wt% in eight steps. The producer of the glass fiber used was Johns
Manville, USA. The diameter of the fibers was 13 µm, while their ori-
ginal length was 4 mm. The ThermoFlow 636 grade used in the study
had a silane coating recommended for thermoplastics, including PP,
poly(vinyl chloride) (PVC) and polyethylene (PE). Wood flour was used
as natural reinforcement in the study. The Filtracel EFC 1000 grade
selected for the purpose was obtained from Rettenmeier and Söhne
GmbH, Germany. The particle dimensions of wood was determined by
particle analysis as well as electron microscopy. According to the result
they were 363 µm long in the average, while their average diameter
2
Composites Part A 133 (2020) 105895
was 64 µm. The amount of wood fiber changed from 0 to 40 wt% in
seven steps.
2.2. Sample preparation
The components, the fibers and the matrix polymer, were homo-
genized in a Brabender DSK 42/7 twin-screw compounder. Processing
parameters were 180–190-200–210 °C set temperatures and 40 rpm
screw speed. The wood flour was dried in an oven at 105 °C for 4 h
before extrusion. The material was run through the extruder twice in
order to increase homogeneity. The granules obtained after the second
processing step were injection molded into standard tensile specimens
of 4 mm thickness (ISO 527 1A). Injection molding was done using a
Demag IntElect 50/330-100 machine. Processing temperatures were
40–170-180–190-200 °C in the barrel, while mold temperature was
40 °C. Depending on fiber type and content injection pressure changed
between 300 and 800 bar. Other processing parameters were 50 bar
backpressure, 50 mm/s injection speed as well as 25 and 30 s holding
and cooling time, respectively. Before further testing the specimens
were stored under controlled conditions (23 °C, 50% RH) for a week to
allow for post crystallization.
2.3. Characterization, measurements
The specimens produced by injection molding were characterized
by tensile and fracture testing. An Instron 5566 universal machine was
used for tensile testing. The measurements were done at 115 mm gauge
length and 5 mm/min crosshead speed. Deformation was measured by
an extensometer. Young's modulus was determined in the strain range
of 0.05–0.25% by fitting a straight line to the measured data. The
characteristic values of yield stress and strain, as well as tensile strength
and elongation-at-break were taken from stress vs. strain traces re-
corded during the test. Local deformation and failure processes, which
occur around the fibers and emit sound, were detected by acoustic
emission (AE) testing. The signals were recorded by a Sensophone AED
404 equipment using a single, all resonance detector attached to the
center of the specimen. The resonance frequency of the detector was
150 kHz; the threshold level of detection was adjusted to 23 dB.
Notched Charpy impact tests were done to characterize the fracture
resistance of the samples. Impact strength was determined under con-
ditions defined by the ISO 179 standard. The measurements were car-
ried out at 23 °C and 2 mm notch depth. In order to follow the fracture
process as well, instrumented impact testing was also carried out by
using a Ceast Resil 5.5 equipment (Ceast Spa, Pianezza, Italy). A
hammer of 4 J capacity was used and the recorded traces were analyzed
to determine fracture initiation and propagation energies. The mor-
phology of the samples as well as the mechanism of fracture were
analyzed with the help of scanning electron microscopy (SEM).
Micrographs were recorded on fracture surfaces created during fracture
and tensile testing using a Jeol JSM 6380 apparatus (Jeol Ltd., Tokyo,
Japan).
3. Results and discussion
The properties of heterogeneous polymer systems are determined by
several factors including their structure. The structure of injection-
molded specimens prepared from fiber-reinforced composites is com-
plicated; the anisotropic fibers have a complex orientation distribution,
which changes in space. Fiber orientation is determined by the flow
pattern in the mold, which is controlled by processing conditions. Since
these latter were the same for all composites, we do not analyze
structure in detail, but assume that fiber orientation and its change with
composition are similar in the three sets of composites. After presenting
tensile and impact properties, we focus our attention on local de-
formation and failure processes as well as the effect of interactions
instead. General correlations and consequences for practice are
R. Várdai, et al. Composites Part A 133 (2020) 105895

Fig. 1. Effect of fiber type and content on the stiffness of fiber reinforced PP Fig. 2. Dependence of the tensile strength of fiber reinforced PP composites on
composites. Symbols: (□,■) CF, (○,●) GF, (△,▴) wood flour. Empty: without fiber type, content and coupling. Symbols are the same as in Fig. 1. (For in-
coupling, poor adhesion; full: with MAPP. (For interpretation of the references terpretation of the references to colour in this figure legend, the reader is re-
to colour in this figure legend, the reader is referred to the web version of this ferred to the web version of this article.)
article.)
existing models [51,52] to the experimental data indicates that chan-
discussed briefly in the final section of the paper. ging fiber length is not the reason for the non-linear correlation, and the
use of shear lag models do not explain the deviation from linearity.
3.1. Tensile properties Changing fiber orientation with composition or large extent of de-
bonding, especially for carbon fibers, might explain it better. Not very
One of the main functions of reinforcing fibers is to increase the surprisingly, coupling has only a minor or negligible effect on compo-
stiffness of the polymer. The Young's modulus of the composites pre- site stiffness; the presence or absence of the coupling agent does not
pared is plotted against fiber content in Fig. 1. The addition of the fibers influence modulus. This finding is in accordance with earlier observa-
resulted in considerable increase of stiffness indeed, Young's modulus tions indicating that interfacial adhesion does not affect stiffness de-
increases from 1.5 GPa to about 13 GPa in the composition range used, termined at small deformations [18–20].
at least for composites prepared with the carbon fibers. Three different The relative effect of the fibers differs considerably in the case of
sets of correlations are obtained depending on the fiber used. Composite tensile strength measured at larger deformation (Fig. 2). The stiffness of
modulus is obviously determined by the stiffness of the fibers, their the fiber plays a much smaller role here, while interfacial interactions
aspect ratio and composition. Carbon fibers had an aspect ratio of are more important. The strongest composites were obtained with the
around 25, glass fibers approximately 12, while the aspect ratio of glass fiber at good adhesion, i.e. in the presence of the coupling agent,
wood fibers was around 7 after processing. Aspect ratio was determined while relatively small values were obtained for the wood reinforced
by digital optical microscopy (DOM) on composites containing 30 wt% composites. It is worth to note that without coupling, the carbon fiber
fibers. Thin (about 200 µm) films were compression molded from the reinforces the polymer only slightly, its effect being very similar to that
composites. The exact values depended also on coupling and they are of wood. Obviously, interfacial adhesion is weak in its composites and
listed in Table 1. We have to note that slight changes in aspect ratio the fiber does not carry much load. Although coupling improves
may occur as a function of fiber content but this effect is not large strength in glass fiber composites, composite strength is acceptable also
enough to influence properties considerably. The nonlinear correlation without MAPP, which indicates a mechanism of interaction different
with decreasing gradient indicates some structural effect, possibly the from the other cases. We must also emphasize here that all fibers, in-
changing orientation of the fibers or their attrition, but the effect is very cluding wood without coupling, increase tensile strength resulting in
similar for all three types of fiber, i.e. CF, GF and wood. The fitting of true reinforcement. On the other hand, coupling leads to a considerable
increase in reinforcement in most cases. We can conclude here that
Table 1 interfacial adhesion plays a very important role in the determination of
Fiber characteristics before and after processing, fiber attrition at 30 wt% fiber the strength of fiber reinforced PP composites.
content. The deformability of composites is extremely important for practical
applications. Reinforcing fibers increase the stiffness of the composites,
Fiber Processing Coupling Fiber dimensions (μm) Aspect ratio
often resulting in very brittle materials with inferior impact properties.
length diameter The elongation-at-break values of the composites studied are plotted
against fiber content in Fig. 3. The largest deformation is measured for
Wood before – 363 64.0 6.8
the composites prepared with wood fiber, which have the smallest
Carbon 8400 7.2 1200
Glass 4000 13.0 307 stiffness. Elongation-at-break might be increased also by the fracture of
Wood after no 225 43.0 7.4 the fibers parallel to their axis [17,53] and the ensuing deformation of
Carbon 197 7.2 27.4 the matrix. The deformability of carbon fiber reinforced composites is
Glass 135 13.0 10.4 very small, both with and without coupling. However, we must point
Wood after MAPP 275 60.0 6.20
Carbon 154 7.2 21.4
out here that the elongation of all composites is very small at all
Glass 180 13.0 14.0 compositions especially if we compare it to that of the neat matrix

3
R. Várdai, et al.
Fig. 3. Correlation between the deformability of PP composites and their fiber
content. Effect of fiber type and coupling. Symbols are the same as in Fig. 1.
(For interpretation of the references to colour in this figure legend, the reader is
referred to the web version of this article.)
polymer (450%). The small deformability may lead to very small
fracture resistance, a frequent weakness of fiber-reinforced composites.
3.2. Impact resistance
The notched Charpy impact resistance of the composites is plotted
as a function of fiber content in Fig. 4. The picture is somewhat similar
to the one presented in Fig. 2 for tensile strength. The best performance
is offered by the glass fiber combined with coupling. Apart from the
wood composites containing small amounts of the fibers, impact re-
sistance increases in each case, which is somewhat surprising since
larger stiffness usually leads to smaller impact resistance. For most PP-
based composites an inverse correlation exists between stiffness and
impact strength [54]. Increased impact strength can be explained only
with fiber related processes, which can be, for example, the plastic
Fig. 4. Effect of fiber type, fiber content and the addition of MAPP on the
notched Charpy impact resistance of fiber reinforced PP composites. Symbols
are the same as in Fig. 1. (For interpretation of the references to colour in this
figure legend, the reader is referred to the web version of this article.)
4
Composites Part A 133 (2020) 105895
Fig. 5. Instrumented impact testing of fiber reinforced PP composites con-
taining 30 wt% of the fibers. The second trace in each pair was recorded on
composites containing the coupling agent (MAPP). (For interpretation of the
references to colour in this figure legend, the reader is referred to the web
version of this article.)
deformation of the matrix in the case of debonding or the fracture of the
fibers. This latter process seems to be especially important for the glass
fiber reinforced composites.
If we analyze the effect of coupling, we can observe several inter-
esting phenomena. Improved interfacial adhesion decreases impact
resistance in the wood composites, and even more in the carbon fiber
reinforced composites. This effect of coupling corresponds to the ex-
pectations, since it had been shown earlier that stronger adhesion
usually results in inferior impact strength [55,56]. On the other hand,
the opposite effect is observed in the case of the composites reinforced
with glass fibers. In all probability, local deformation and failure pro-
cesses, or their relative importance are different in the three sets of
composites resulting in dissimilar energy absorption during fracture
and thus different impact resistance.
More insight about the fracture process and the factors influencing it
might be gained from the results of instrumented impact testing. The
traces obtained during such tests are presented in Fig. 5 for the six
composites, three fibers with or without coupling, at 30 wt% fiber
content. Although the figure does not offer an unambiguous explana-
tion for the different effect of the fibers and the dissimilar influence of
coupling, the traces differ considerably from each other. Apparently, all
composites fail by brittle fracture, but large differences can be observed
in the maximum force related to fracture initiation. Some relationship
seems to exist between the maximum force and impact resistance, but
at least one additional factor also influences this property. Carbon fiber
composites have large maximum force, but smaller impact strength
than the glass fiber composites at good adhesion. In the presented form
the traces do not allow the estimation of fracture energy, but a more
detailed analysis shows that it changes similarly to the correlations
shown in Fig. 4 for standard Charpy impact resistance. These results
clearly indicate that several factors influence the impact resistance of
fiber reinforced composites, one of which is definitely interfacial ad-
hesion, coupling. The analysis of local deformation and failure pro-
cesses may shed more light on these factors.
3.3. Local deformation processes and failure mechanisms
Under the effect of external load, stress concentration develops
around the heterogeneities in blends and composites prepared from
components with dissimilar elastic properties [57]. Larger stresses in-
itiate local deformation and failure processes, which, in the end, de-
termine the macroscopic properties of the material. Numerous pro-
cesses related to the fibers may take place in fiber-reinforced polymers.
Some of these processes can be followed by acoustic emission
R. Várdai, et al.
Fig. 6. Results of the acoustic emission testing of a PP/wood composite con-
taining 20 wt% wood at good adhesion (MAPP). Small circles (○) indicate in-
dividual signals. Solid lines represent the cumulative number of signals (right
axis) and the stress vs. strain correlation (left axis) plotted as reference. (For
interpretation of the references to colour in this figure legend, the reader is
referred to the web version of this article.)
Fig. 7. Acoustic emission results obtained for a PP/CF/MAPP composite at
20 wt% fiber content. Symbols are the same as in Fig. 6. (For interpretation of
the references to colour in this figure legend, the reader is referred to the web
version of this article.)
measurements [17,19]. Individual events initiate elastic waves in the
material, which can be detected by piezoelectric sensors placed on the
specimen. The result of such a measurement done on wood reinforced
PP with coupling is presented in Fig. 6. Individual signals (events) are
indicated by small circles in the figure, the height of which corresponds
to the amplitude of the signal, and the stress vs. strain correlation is also
plotted as reference (left axis). Two groups of signals can be identified
in the figure, one at small deformations and the rest above 2.5%
elongation. Although the two groups can be clearly distinguished, the
cumulative number of signal trace (right axis) summarizing all the
events up to a certain deformation facilitates evaluation and under-
standing. Two steps appear in the correlation clearly indicating two
separate processes taking place during the tensile testing of the spe-
cimen. These processes were identified earlier as debonding, the se-
paration at the interface between the matrix and the fiber, and the
5
Composites Part A 133 (2020) 105895
Fig. 8. Comparison of cumulative number of signal traces obtained for the six
composites studied. Fiber content: 20 wt%. ––––– good adhesion (with MAPP),
———— poor adhesion (no MAPP). (For interpretation of the references to
colour in this figure legend, the reader is referred to the web version of this
article.)
fracture of the fibers, which occur especially frequently at strong ad-
hesion [17,47,48,53]. Both processes are initiated above a certain de-
formation from which characteristic stresses (σAE) can be derived
[17,19,47,48,53]. The determination of these stresses is indicated in
Figs. 6 and 7, and the respective values will be used later for evaluation.
The acoustic emission testing of materials reinforced with tradi-
tional fibers, glass or carbon, yields a somewhat different result. Such
an example is presented in Fig. 7 showing the distribution of signals and
the cumulative number of signal trace. Unlike in the case of wood re-
inforced PP, only one process seems to take place during the tensile
testing of this specimen or at least one dominates during deformation.
This process can be the debonding, pullout or the fracture of the fibers.
Debonding may take place to some extent for fibers oriented perpen-
dicular to the load, but pullout or fiber fracture are also probable me-
chanisms, which may occur in the composite.
The shape of the cumulative number of signal trace and the number
of signals offer information about the possible processes taking place
around the fibers during deformation. The cumulative number of signal
traces are presented in Fig. 8 for composites containing 20 wt% of the
various fibers. Two distinct processes take place in wood composites as
shown in Fig. 6, but the steps are less visible in the figure because of the
relative small number of signals. It is interesting to note that the
number of events decreases considerably upon the addition of MAPP,
since at good adhesion less debonding takes place, although the relative
number of fiber fractures increases somewhat. Carbon fiber reinforced
composites present dissimilar traces from those measured on PP/wood
composites, only one process dominates and coupling does not influ-
ence the number of signals, but decreases the deformability of the
composites. The behavior of the glass-reinforced composites is ob-
viously different and only one process seems to take place in these
composites. The process starts at somewhat larger deformation than in
the other two sets of composites, i.e. for CF and wood. The larger
characteristic deformation, and thus stress, the large number of signals
as well as the shape of the trace indicate good adhesion. This result is in
accordance with the one presented in Fig. 2 showing relatively good
strength for the glass fiber reinforced composites even without cou-
pling. These results indicate that several and different local deformation
and failure processes may take place practically in every composite, but
one dominates the failure behavior in most of them.
The identification of the individual processes is practically
R. Várdai, et al. Composites Part A 133 (2020) 105895

n 1
T = T0 exp(B )
1 + 2.5 (1)

Fig. 9. SEM micrographs recorded on the surface of specimens broken during
tensile testing. Identification of local deformation and failure processes. (a) CF,
(b) CF/MAPP, (c) GF (d) wood/MAPP. Fiber content: 20 wt%.
impossible from the results of acoustic emission testing alone. On the
other hand, scanning electron micrographs recorded on the surface of
specimens broken during tensile testing may help in the identification.
Only a few characteristic micrographs are presented in Fig. 9 in order to
save place, but representative ones reveal the most important processes.
Micrograph taken from a composite reinforced with carbon fiber is
shown in Fig. 9a. Some debonding, extensive pullout and the fracture of
the fibers can be seen in the micrograph. Matrix yielding can be also
observed around fibers pulled out. The introduction of MAPP, i.e.
stronger adhesion decreased the length of pulled out fibers and in-
creased the number of fractured ones (Fig. 9b). Accordingly, the pullout
and fracture of the fibers are the main processes in CF reinforced
composites. A similar picture is offered by the micrographs recorded on
glass fiber reinforced PP. Adhesion is surprisingly good both in the
presence and in the absence of MAPP in composites containing the glass
fiber. Although some debonding and pull out can be also observed in
Fig. 9c recorded on a composite prepared with the glass fiber in the
absence of MAPP, the surface is dominated by short broken fibers.
Apparently, the fracture of fibers consumes considerable energy during
failure. Debonding dominates in wood composites not containing the
coupling agent, while fiber fracture in the presence of MAPP (Fig. 9d).
The SEM study confirmed the observations made during acoustic
emission testing and helped the identification of the main local de-
formation mechanisms. The results clearly prove that adhesion is an
important factor determining the mechanism of local deformation
processes and failure mechanisms and thus the macroscopic properties
of the composites.
3.4. Interactions, coupling
Although the effect of interfacial adhesion and coupling is more or
less clear, its quantitative estimation is difficult. Moreover, coupling
influences properties to a lesser extent in the case of the glass fiber than
in the other cases, which also needs some explanation. A model created
for the description of the composition dependence of tensile strength of
heterogeneous materials offers a way to develop some idea about the
effect of interactions on properties [58]. The model describes the
composition dependence of tensile strength in the following way (Eq.
(1))
where σT and σT0 are the true tensile strength of the composite and the
matrix, respectively, φ is the volume fraction of the reinforcement in
the composite, B expresses the load bearing capacity of the reinforce-
ment and it depends on interfacial adhesion. In the equation true tensile
strength (σT = σλ, λ = L/L0, relative elongation) accounts for the
change in specimen cross-section and λn for strain hardening occurring
with increasing elongation. n characterizes the strain hardening ten-
dency of the polymer and can be determined from matrix properties.
The rearrangement of the equation leads to the reduced tensile strength
and if we plot its natural logarithm against composition, we should
obtain straight lines, the slope of which expresses the reinforcing effect
of the filler quantitatively. The parameter of the model, B, is related to
the load bearing capacity of the heterogeneity, i.e. filler, fiber or a blend
component, and it depends, among others on interfacial adhesion. Al-
though the structure, e.g. the orientation of the fibers in this case, also
plays a role in the determination of strength and thus parameter B,
interfacial interactions also influence it. As mentioned before, we as-
sume that fiber orientation is similar in all cases and does not change
much with increasing fiber content.
Parameter B was calculated for all the composites and it is listed in
Table 2. The load bearing capacity of the fibers increases upon the
addition of the coupling agent in each case. The smallest increase oc-
curs for the glass fiber, indicating that the sizing used results in good
adhesion and the coupling agent does not enhance it much further.
Considerable improvement is observed in the other two cases. The table
also contains the impact resistance of the composites and the number of
acoustic signals detected at 30 wt% fiber content. We can see that both
the number of signals and adhesion are related to impact strength, but
not always in the same way. In the case of the carbon fiber and wood,
coupling results in decreased impact resistance, i.e. stronger adhesion
facilitates the fracture of the composite. It must change the dominating
local deformation and failure processes and/or suppress one, which
absorbed energy in the absence of coupling. Fiber fracture does not
absorb much energy in the case of the wood and CF composites, but the
large number of fiber fractures in the glass fiber reinforced composites
does, which results in relatively large impact resistance.
3.5. Correlations
The results presented above clearly prove that local deformation
processes have a considerable impact on the macroscopic properties of
the composites. To see this relationship better, the tensile strength of
the composites was plotted against the characteristic stress (σAE) of the
dominating process, which was derived from acoustic emission testing
(Fig. 10). Characteristic stresses were determined for all three fibers at
all fiber contents. Two processes were detected in many, but not in all
composites and the corresponding values (σAE1, σAE2) were plotted in
Fig. 10. The figure supports the existence of such a relationship, which
Table 2
Relationship among impact resistance, acoustic activity and reinforcing effect
in fiber reinforced polypropylene.
Reinforcement Coupling Impact No. of signalsa Parameter Bb
resistancea an
(kJ/m2)
Carbon – 4.44 ± 0.11 13700 ± 1210 4.45
+ 3.96 ± 0.18 15100 ± 3040 7.80
Glass – 2.62 ± 0.11 43266 ± 5050 4.64
+ 4.42 ± 0.23 163020 ± 14010 5.93
Wood – 2.62 ± 0.22 16100 ± 8410 3.13
+ 2.27 ± 0.05 6860 ± 5360 5.03
a
At 30 wt% fiber content.
b
Related to the load bearing capacity of the fiber and to adhesion.

6
R. Várdai, et al. Composites Part A 133 (2020) 105895

Fig. 10. Correlation between the tensile strength of the composites and the
characteristic (initiation) stress of the local deformation processes determined
by acoustic emission testing. Symbols are the same as in Fig. 1. Additional
symbols: first process in (∇) PP/wood, (▾) PP/wood/MAPP composites. (For
interpretation of the references to colour in this figure legend, the reader is
referred to the web version of this article.)
Fig. 11. Relationship between the impact resistance of the PP composites stu-
died and the characteristic stress of the local deformation processes. Symbols
are the same as in Figs. 1 and 10. (For interpretation of the references to colour
in this figure legend, the reader is referred to the web version of this article.)

is rather similar for practically all composites. The composites can be

divided into several groups. The first local deformation process in wood
and the dominating one in uncoupled CF as well as in the coupled CF
composites do not result in the failure of the composite, the initiation
stress of the corresponding processes being much smaller than the
tensile strength of the composites (see upper straight line). On the other
hand, the second process in wood reinforced PP, i.e. the fracture of
wood particles, leads to the immediate failure of its composites (lower
straight line, full triangles). Finally, the composites prepared with the
glass fiber fail after the initiation of the dominating process, but not
immediately, and the gap between the theoretical line of immediate
and actual failure increases with increasing fiber content (full red cir-
cles). In the case of proper coupling, glass fibers reinforce PP con-
siderably and offer a very advantageous property profile.
One might object that the characteristics determined under the
conditions of static tensile testing do not give any indication about
impact resistance measured at high rate, and local deformation and
failure processes might not influence impact strength. Impact resistance Fig. 12. Correlation between the impact resistance and stiffness of fiber re-
is therefore plotted against the characteristic stress values in Fig. 11. inforced PP composites. Symbols are the same as in Fig. 1. The broken line
Very strong correlations are obtained again, and more or less the same indicates the general correlation of the two properties determined in a previous
groups can be distinguished in this figure as in the previous one. It is study [54]. (For interpretation of the references to colour in this figure legend,
interesting to note that impact resistance increases in all cases with the the reader is referred to the web version of this article.)
increase of characteristic stress indicating that fiber related processes
absorb energy and improve impact resistance. Although the processes Due to the local deformation processes initiated around the fibers im-
are different, thus their energy absorption is also different, the overall pact resistance increases practically in all cases here, i.e. the use of the
effect is the same. Matrix yielding after debonding or pullout, or the traditional fibers is more beneficial than that of wood if impact re-
fracture of the fibers, all lead to smaller or larger additional energy sistance is important for the intended application. We must emphasize
absorption. The beneficial effect of glass fibers with good adhesion is here that although impact resistance increases upon the addition of the
clear in this case again. traditional fibers; its value is not extremely large. Occasionally impact
An important question for structural materials is the balance of strengths in excess of 15–20 kJ/m2 are required for certain applications.
stiffness and impact resistance. The two characteristics are plotted Nevertheless, the proper selection of fiber type, fiber content and
against each other in Fig. 12 for the composites studied. Usually an coupling can lead to a very advantageous combination of properties.
inverse correlation exists between the two quantities as shown by the
broken line taken from one of our earlier works [54]. The correlation
was obtained as the result of the testing of a very large number of wood, 4. Conclusions
as well as wood and elastomer modified PP composites. Impact re-
sistance could not be increased at any combination of the two compo- A comparative study with three different fibers, wood, glass and
nents because the fracture of wood particles dominated failure [19,53]. carbon, was carried out to determine their advantages in the

7
R. Várdai, et al.
reinforcement of PP. The results proved that all three have advantages
and drawbacks. The stiffness of the composites depends on the modulus
of the fiber, their aspect ratio and on composition, but coupling does
not influence it practically at all. Properties measured at larger de-
formations, on the other hand, are influenced quite strongly by inter-
facial adhesion and local deformation processes related to the fibers.
The effect of adhesion depends on the type of the fiber and the local
deformation and failure processes. Large wood particles debond from
the matrix very easily without coupling, while their fracture is the
dominating process at good adhesion, which leads to immediate failure
in PP/wood composites. Increased interfacial adhesion improves re-
inforcement, but decreases impact resistance in carbon fiber reinforced
composites. The glass fiber used in the study offers good adhesion even
without coupling. The initiation of some local deformation processes
does not result in the immediate failure of the composites, but that of
others lead to catastrophic failure. Characteristic stresses related to the
initiation of local processes correlated well with macroscopic proper-
ties. Due to its natural and renewable character as well as low price,
wood is a good reinforcement when the increase of stiffness is the main
goal of modification, but it cannot be used in applications in which
impact resistance is important. Carbon fibers are rather expensive and
their composites are very stiff, but otherwise they possess intermediate
properties. If adhesion is good, glass fibers offer a good balance of
properties including stiffness, strength and impact resistance.
CRediT authorship contribution statement
R. Várdai: Investigation, Methodology, Data curation,
Visualization, Writing - original draft, Writing - review & editing. T.
Lummerstorfer: Conceptualization, Writing - review & editing,
Resources. C. Pretschuh: Writing - review & editing, Funding acqui-
sition. M. Jerabek: Writing - review & editing. M. Gahleitner: Writing
- review & editing, Resources, Funding acquisition, Supervision. G.
Faludi: Writing - original draft, Project administration. J. Móczó:
Conceptualization, Methodology, Data curation, Writing - original
draft. B. Pukánszky: Conceptualization, Methodology, Writing - ori-
ginal draft, Supervision.
Declaration of Competing Interest
None.
Acknowledgements
The significant help of students (Zsigmond Kiss and László Kovács)
in sample preparation and impact testing is highly appreciated. The
authors acknowledge the financial support of the Comet program of
Austria and the National Scientific Research Fund of Hungary (OTKA
Grant No. K 120039 and FK 129270) for this project on the modifica-
tion of polymeric materials. One of the authors (RV) is grateful also to
the Pro Progression Foundation for its support.
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