Composites Part B 266 (2023) 110971

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Composites Part B
journal homepage: www.elsevier.com/locate/compositesb

Mechanical characterization and design of hybrid reinforced polypropylene

composites with talc fillers and cellulose fibers
Taiki Kinoshita a, Tatsuto Yamamoto b, Chao Luo b, Kouta Ide c, Kenji Aoki d, Yasutomo Uetsuji b, *
a
Graduate School, Osaka Institute of Technology, 5-16-1 Omiya, Asahi-ku, Osaka, 5358585, Japan
b
Department of Mechanical Engineering, Osaka Institute of Technology, 5-16-1 Omiya, Asahi-ku, Osaka, 535-8585, Japan
c
Toyo Resin Corporation, 2104-1 Atsuhara, Fuji-shi, Shizuoka, 419-0201, Japan
d
Faculty of Global Interdisciplinary Science and Innovation, Shizuoka University, 836 Ohya, Suruga-ku, Shizuoka, 422-8529, Japan

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

Keywords: Hybrid reinforced polypropylene composites (PPCs) were fabricated via injection molding, and tensile tests were
PP composite conducted. The results showed that the addition of cellulose nano-fibers (CNFs) and maleic-anhydride-modified
Cellulose fiber polypropylene enhanced the PPC elastic constant and tensile strength. The nonlinear properties of the composites
Talc filler
were analyzed via two-step asymptotic homogenization. After confirming that the numerical simulation can
Maleic anhydride modified PP
Filler contribution proportion
predict the experimental results well, a new strain-energy-based indicator was introduced to quantify the filler
Asymptotic homogenization addition effect. The mechanical properties of PPCs can be linearly approximated using the indicator, named filler
contribution proportion, and a simple composite design based on this relationship was proposed. As verification
examples, the elastic constant and maximum tensile stress of unknown PPCs were predicted within a 5% error.

1. Introduction
Polypropylene (PP) is widely used, primarily in the automotive in­
dustry, because of its excellent mechanical properties, moldability, low
cost, thermoplasticity, and high recyclability [1]. Short glass and carbon
fibers, natural fibers such as hemp, and mineral fillers such as talc and
calcium carbonate are generally added to PP as reinforcement materials
to improve its stiffness and strength [2–6]. The mechanical properties of
these PP composites strongly depend on various factors such as their
fiber and filler contents, particle size, aspect ratio, orientation, and
surface treatment. Therefore, a large number of studies can be found on
the mechanical properties of PP composites.
This paper is focused on the use of talc, which is one of the most
commonly used fillers, in PP. Talc is a metamorphic hydrated magne­
sium silicate mineral with the chemical formula Mg3Si4O10(OH)2. In
addition to the fundamental properties of PP/talc composites such as
thermal, elastic, and electrical properties [7], the effects of the filler
morphology [8], effect of talc content on degradation in the case of
re-extrusion [9], effect of chemical modification pathways of synthetic
talc on filler dispersion [10], and the temperature dependence of the
tensile, bending, and impact properties of PP/talc composites have been
studied [11]. In addition, laminated materials of PP and PP/talc
composite layers were fabricated via multi-layered co-extrusion, and the
effects of talc orientation and crystallization on mechanical properties
and thermal stability were analyzed [12]. Furthermore, it was found
that nanofiller-reinforced PP composites with fine talc particles exhibi­
ted no significant difference in tensile modulus and strength compared
to those comprising microfillers; however, the former exhibited signif­
icantly improved impact strength [13].
The use of matrix polymer blends and multi-fillers to further improve
the aforementioned properties was also investigated. In the former
approach, poly (styrene-ethylene-butylene-styrene) block copolymer
was blended with PP, the resulting effects on the mechanical and ther­
mal properties [14] and impact strength [15] of the PP/talc composite
were investigated, and a property improvement due to the elastomer
blend was confirmed. The temperature dependence of the impact
properties and the effects of the use of filler content and recycling were
also elucidated for PP/talc composites in which ethylene octene copol­
ymer was added to PP as a soft-rubber reinforcing agent [16]. In the
latter approach comprising the use of multi-fillers, inorganic fillers such
as mica [17], nanoclay [18], and silica limestone [19] are added to
PP/talc composites to achieve improved mechanical properties, and the
effectiveness of multi-filler reinforcement has attracted attention.
Natural fibers have also attracted attention over the last decade as an

* Corresponding author.
E-mail addresses: m1m21411@st.oit.ac.jp (T. Kinoshita), e1420162@st.oit.ac.jp (T. Yamamoto), cho.ra@oit.ac.jp (C. Luo), kouta-ide@resin.co.jp (K. Ide), aoki.
kenji@shizuoka.ac.jp (K. Aoki), yasutomo.uetsuji@oit.ac.jp (Y. Uetsuji).

https://doi.org/10.1016/j.compositesb.2023.110971
Received 20 April 2023; Received in revised form 3 July 2023; Accepted 28 August 2023
Available online 10 September 2023
1359-8368/© 2023 Elsevier Ltd. All rights reserved.
T. Kinoshita et al.
alternative material to inorganic fillers [5]. Natural fibers such as hemp,
used newspaper, kraft pulp [20,21], and wood flour [22,23] have been
actively used as such alternative materials. Furthermore, cellulose
nanofibers (CNFs)—in the form of cellulose nanovehicles that were
prototyped in Japan and achieved 10% weight reduction compared to
using conventional materials [24]—have recently shown promise as a
new environmental material [25–29]. Although the specific stiffness and
strength of PP composites have been significantly improved with the
application of CNFs, there exist technical issues such as the fragile
PP/cellulose interface and cellulose aggregation that are yet to be
addressed. Therefore, hybrid reinforced PP composites have been
developed with the addition of talc, which has a low cost and is easy to
handle, and wood powder, which can provide an improvement in spe­
cific stiffness and strength, to the PP matrix [30,31]. Similar hybrid
reinforcement was also attempted in polylactic acid (PLA)/talc com­
posites, wherein the addition of wood flours or recycled newspaper
cellulose was confirmed to reduce the weight [32,33]. In hybrid rein­
forced PP composites, wood flours are currently used mainly as a sec­
ondary filler, but CNFs are also expected to be applied in the future.
However, the introduction of mathematical and numerical analyses is
essential for the application of such hybrid reinforced composites
because the number of design parameters for determining the mechan­
ical properties is doubled and the degree of influence of each factor is
more complex compared to the case of single-type filler reinforced PP
composites.
The mixture law is well known as the classical theory at the core of
the mathematical analysis of composite materials. In addition to series
and parallel models, the mixture law has been applied to composite
materials with uniformly dispersed short fibers and fillers [34]. Exper­
imental parameters were also introduced to account for the effects of the
filler anisotropy and orientation in PP/talc composites [35] and the
effects of aggregation in PLA/talc composites [36]. Moreover, multiscale
numerical simulations of composite materials have been performed at
various scales, ranging from atoms, molecules, and particles to continua.
On the atomic scale, first-principles calculations based on density
functional theory were applied to PP composites. The atomistic analysis
of the interfacial strength between the PP matrix and cellulose crystals
revealed the effect of maleic anhydride modified PP (MAPP) as a
coupling material [37]. On the molecular scale, molecular dynamics
(MD) simulations were used to construct composite models of amor­
phous PP comprising 10 chains of 50 monomers as the matrix with 7–14
cellulose molecular chains inherent in it. The effect of the cellulose
molecular content on the elastic modulus was investigated, and the
effectiveness of MAPP on the mechanical properties was clarified [38].
Other active applications of MD simulations include composites of cel­
lulose nanocrystals and carbon nanotubes [39]. Furthermore, in Monte
Carlo simulations, for polyethylene (PE) composites filled with spherical
nanofillers, the deformation of the matrix molecular chains was related
to the filler dispersion and arrangement and was considered as a volume
exclusion effect owing to the filler inclusion [40]. Dissipative particle
dynamics simulations, in which functional groups and molecules are
coarse-grained and scaled up, have also been actively applied to com­
posite materials. For example, the dispersibility of particles and the
decoupling effect of electrical and thermal conduction were revealed for
a polydivinylbenzene composite comprising hybrid nanoparticles of
fullerene and polyaniline [41]. Atomic-, molecular-, and particle-scale
simulations are useful for understanding the effects of interfaces and
fillers on mechanical properties and the mechanism of complexity and
for obtaining qualitative design guidelines, although the analytical re­
gion is localized and it is difficult to characterize the overall composite
material.
Numerical simulations based on the finite element analysis (FEA) are
often used on the continuum scale, which takes a global view of com­
posite materials. FEA simulations have also been applied to various
short-fiber or filler-dispersed polymer composites, thus facilitating the
direct modeling of arbitrary heterogeneous structures. The Monte Carlo
2
Composites Part B 266 (2023) 110971
method [42–44] and random sequential adsorption (RSA) algorithm
[45–51] are frequently used for modeling representative volume ele­
ments (RVEs) of heterogeneous microstructures. For example, in RSA,
the coordinates and orientation angles of the reinforcement are gener­
ated by random numbers, and the reinforcements are added to the RVE
region in succession. If an added reinforcement interferes with the
previously placed reinforcement, it is discarded and a new reinforce­
ment is created or its coordinates or orientation angle are changed to
eliminate the interference. The same procedure is repeated until the
reinforcement content reaches a predetermined value. In addition to
being able to consider any reinforcement morphology in RVE models,
various dispersion and orientation states can be reflected in RVE models
by controlling the coordinates and orientation angles. In general,
asymptotic homogenization theory [52] is commonly used to evaluate
the mechanical properties of macrostructures using microstructural RVE
models. This theory introduces a scale ratio for micro- and
macro-structures, expresses displacement in terms of an asymptotic
expansion equation using microstructural perturbation, and derives
micro- and macro-structural coupled equations. Multiscale FEA based on
homogenization theory was applied to composite materials to clarify the
relationship between the microscopic heterostructure and macroscopic
material properties [53–58]. There exist a wide variety of applications of
this analysis, ranging from glass and carbon short fibers [46,50,53,54,
59] to carbon nanotubes [51,60–64], flax fibers [65,66], and CNFs [67,
68], in the context of reinforcement materials. For examples, in our
previous study, the effects of the fiber orientation angle, fiber aspect
ratio, fiber-to-fiber distance, and fiber/matrix interface on the elastic
properties in unidirectionally oriented CNF reinforced composites were
systematically clarified [69]. The effects of the fiber aspect ratio and
aggregation on nonlinear properties under tensile loading were also
elucidated for randomly oriented CNF-reinforced composites [70]. In
addition, this analysis has been applied to PP composites with halloysite
added as an inorganic filler [71] and polymer composites blended with
PP and high-molecular-weight PE [72]. The multiscale FEA based on
RSA-generated RVE and homogenization theory is useful and reliable for
application to composite materials.
To summarize the trends in multiscale FEA till date, there have been
many applications to glass, carbon short fibers, and carbon nanotubes,
and the effects of fiber morphology on mechanical properties have been
well discussed. However, the evaluation of the mechanical properties of
talc-reinforced PP composites has been limited to experimental ap­
proaches and the classical mixture law, although industrial applications
are flourishing. Therefore, multiscale FEA has been rarely applied, and
furthermore, it has not been applied to hybrid reinforced composites.
There is a strong need for the multiscale FEA of hybrid reinforced PP
composites for coping with the increase in the design parameters and the
complexity of the strengthening mechanism due to use of multi-filler
reinforcement.
In this study, hybrid reinforced PP composites comprising talc filler
and CNF were targeted, and the effect of adding CNF as a secondary filler
was investigated experimentally and computationally. In the experi­
mental approach, MAPP was blended to form a strong interface with
CNF, and the CNF aggregation was reduced by fabricating a high-
concentration master batch (MB) of CNF in the pre-kneading process.
Hybrid PP composites were fabricated via injection molding using CNF
and talc filler MBs, and their elastic constant and tensile strength were
investigated via tensile tests. The addition of MAPP to hybrid reinforced
composites is expected to improve the dispersibility of the re­
inforcements and enhance their interface with the matrix. In the
computational approach, the RVE model was constructed using RSA,
and a multiscale simulation based on homogenization theory was con­
ducted to analyze the nonlinear characteristics associated with tensile
loading. Furthermore, an original indicator based on strain energy was
introduced to quantify the effect of the addition of fillers in hybrid
reinforced PP composites. A simple design procedure for realizing the
desired mechanical properties was proposed using the introduced
T. Kinoshita et al.
Table 1
MB formulation ratios for fabrication of PP composites via injection molding.
Blended mass (g) Volume content ratio (%)
PP Talc MB CNF MB Talc CNF
mTalc mCNF
PP/Talc 100 10 0 2.22 0.0
PP/CNF 100 0 10 0.0 0.90
PP/Talc/CNF 100 10 10 2.20 0.85
indicator, i.e., the filler contribution proportion. The accuracy in pre­
dicting the elastic constant and maximum tensile stress of unknown PP
composites with different filler combinations was verified.
2. Experimental method
In the fabrication of hybrid reinforced composites, block PP (J707G,
Prime Polymer), a thermoplastic polymer, was used as the matrix, and
talc filler and CNF were used as reinforcements. In the flow test of the
PP, the melt flow rate under a load of 21.2 N was 30 g/10 min. The
specimens were prepared via injection molding and using a high con­
centration MB for both the talc filler and CNF. For the former talc MB, a
commercial PP MB mixed with talc fillers at 15 mass% (PEX1470, Tokyo
Printing Ink) was used. The talc fillers comprised thin particles of 4-μm
diameter as representative dimensions, as discussed in Section 2.1. For
the latter, CNFs (BiNFi-s WFo-10010, Sugino Machine) having an
average diameter of 0.03 μm, average length of 1.5 μm, and aspect ratio
of 50 were used to produce the CNF MB in two-step mixing processes. In
the first step, the CNF was blended with MAPP at equal mass contents to
form a strong interface with the PP. The contents of MAPP and CNF in
the first step of fabricating the MB was 50 mass%. In the second step, the
MB comprising CNF and a MAPP content of 50 mass% was then fed from
the hopper, and PP was side-fed to produce the MB with CNF and MAPP
contents of 20 mass% through melt kneading. The CNF MBs were
fabricated using a mixer (TEM-26SX-12/2V, Shibaura Machinery) with a
screw diameter of 26 mm, screw speed of 100 rpm, effective length L/D
of 48, discharge rate of 5 kg/h, and in-barrel temperature of 160 ◦ C. The
talc and CNF MBs were then blended as shown in Table 1, and the in­
jection molding machine (EC100SXIII-2A, Shibaura Machinery) was
used to produce dumbbell-shaped specimens (JIS K7139) with 100-mm
parallel sections and 4-mm thickness. The MAPP content in the MB was
limited to 20 mass%, which is the same as the amount of CNF. If the
MAPP content is too large, excess MAPP may be mixed into the PP
matrix, thus reducing the stiffness of the composite or adversely
affecting the dispersibility of the talc fillers. The optimality of the MAPP
content is discussed in Section 4.2 below, based on a comparison of the
multiscale simulation and experimental results.
The microstructures of the PP composites were observed using the
scanning electron microscope (SEM) (JCM-6000, JEOL Ltd.) at an
Fig. 1. Multiscale modeling of hybrid reinforced composites.
3
Composites Part B 266 (2023) 110971
acceleration voltage of 15 kV after platinum deposition on a vertical
section of the dumbbell-shaped specimen. After cutting a rectangular
section (1 mm × 1 mm × 2 mm) from the center of the dumbbell-shaped
specimen at a depth of 1 mm from the surface, the micro X-ray computed
tomography (CT) (nano 3DX, Rigaku) was used to observe talc filler
dispersion. After ashing the specimens, the size of the talc fillers was
analyzed using the laser diffraction particle size analyzer (MT3000II,
MicrotracBEL). Tensile tests were conducted using the universal testing
machine (Autograph AGS-5kN, Shimadzu) at a test speed of 5 mm/min
until to 5% strain was reached in the elastic range and at 50 mm/min
thereafter.
3. Computational method
3.1. Multiscale FEA
As shown in Fig. 1, a macrostructure, a microstructure with talc filler
dispersion, and a sub-microstructure with CNF dispersion were consid­
ered for the hybrid reinforced polymer composites. Asymptotic ho­
mogenization theory was employed for realizing scale coupling in the
macro- and micro-structures and in the micro- and sub-microstructures.
In homogenization theory, a scale ratio is introduced, and the
displacement is expressed using an asymptotic expansion equation with
the displacement of the global structure and displacement perturbation
of the local structure, thus facilitating the derivation of scale-coupled
equations with mathematical consistency [49].
In the first stage of the homogenization process, the homogenized
material properties of the matrix region of the microstructure with the
talc filler dispersed as the global structure were calculated, with the
CNF-dispersed sub-microstructure as the local.
Structure. In the second stage of the homogenization process, the
microstructure with talc filler dispersion was used as the local structure,
and the homogenized material properties of the macrostructure as the
global structure were obtained. The mechanical response of the
macrostructure to external loading was also analyzed.
The coordinates in the global structure of region Ω and the local
structure of region Y are defined by x and y = x/λ, respectively, where λ
is the scale ratio defined by the representative dimensions of both the
structures. Periodicity was assumed for the local structure, and the
overall structure was considered to be the product space of the global
and local structures. Using the displacement of the global structure
u0i (x, y) and the displacement perturbation of the local structure u1i (x,y),
the displacement of the overall structure is expressed as an asymptotic
expansion. Here, the higher-order terms are neglected, and uλi are given
as
uλi = u0i (x, y) + λu1i (x, y) . (1)
Finally, u0i (x, y)
becomes independent of the local coordinate y and
can be expressed as u0i (x). u1i (x, y) is assumed to be proportional to the
T. Kinoshita et al. Composites Part B 266 (2023) 110971

strain in the global structure, as in the following equation:

∂u0m (x)
u1i (x, y) = − χ mn
i (x, y) , (2)
∂yn

where χ mn i (x, y) is a proportionality constant obtained as the solution of

the following local structure equation under periodic boundary condi­
tions.
∫ ∫
∂χ mn (x, y) ∂δu1i (x, y) ∂δu1 (x, y)
local
Cijkl k dY = local Cijmn i dY . (3)
Y ∂ yl ∂ y j Y ∂yj

local
Cijkl is the elastic constant of the talc filler, CNF, PP matrix, or PP/
CNF composite that constitutes the heterogeneous structure. From
χ mn
i (x, y) obtained using the local equations, the homogenized elastic
constant for the global structure can be calculated as follows:
∫ ( )
1 ∂χ kl (x, y)
global
Cijkl = global
Cijkl − global Cijmn m dY . (4)
|Y| Y ∂yn

when no object forces exist, the mechanical response to external loads is

evaluated using the following global structure equation:
∫ ∫
∂u0 (x) ∂δu0i (x)
global
Cijkl k dΩ = ti δu0i (x)dΓ . (5)
Ω ∂xl ∂xj Γ

From the solution u0i (x) obtained using the global structure equation,
the displacement global ui (x), strain global εij (x), and stress global σij (x) in the
global structure are evaluated according to the following equations:
global
ui (x) = u0i (x), (6)
( )
global
1 ∂global ui (x) ∂ uj (x)
global
εij (x) = + , (7)
2 ∂xj ∂xi

global
σij (x) = global Cijkl εkl (x) . (8)

In contrast, the displacement local

uij (x), strain local
εij (x), and stress
global
σij (x) in the local structure are evaluated as follows:

∂u0i (x)
local
uij (x, y) = yj + u1i (x, y), (9)
∂xj
( )
local local
1 ∂ uij (x, y) ∂ uij (x, y)
local
εij (x, y) = + , (10)
2 ∂yj ∂yi

local
σ ij (x, y) = local Cijkl local εkl (x, y) . (11)

In the analysis of the nonlinear response to external loads, the material

nonlinearities were approximated as interval linear approximations, and
the above was applied to each interval in the incremental form. Multi­
scale. Sim was used for the scale coupled analysis based on the ho­
mogenization theory, and ANSYS was used as the FEA solver.

3.2. Quantification of filler effect Fig. 2. Flowchart of RVE modeling and multiscale FEA process for
PP composites.
The external load performed work on the macrostructure, and strain
energy was stored in the microstructure or sub-microstructure accord­ where Yf and Ym refer to the region occupied by the talc filler or fiber and
ingly. The strain energy Uf and Um accumulated in the talc filler or fiber the matrix in the local structure, respectively. When the reinforcing ef­
inherent in the local structure and in the matrix, respectively, can be fect of the filler in the composite is significant, it is also assumed that the
calculated using the following equations. reinforcing material contributes a large amount of the total strain en­
∫ ergy. Therefore, the effect of the reinforcement on the improvement of
Uf = local σij (x, y)local εij (x, y) dYf (12) the mechanical properties is quantified by defining the contribution
Yf
proportion of Uf to the total strain energy as shown in the following
∫ equation [69,70,73].
Um = local
σij (x, y)local εij (x, y) dYm (13)
Ym

4
T. Kinoshita et al.
Table 2
Material properties of talc filler and CNF used in the multiscale FEA.
Material Elastic modulus Poisson’s ratio
Filler Talc 17.2 GPa 0.27
Cellulose 140 GPa 0.30
Matrix PP 1.07 GPa 0.30
Uf
CPf = × 100
Uf + Um
In our previous study [69], the fiber contribution proportion was
applied to unidirectionally oriented cellulose composites to investigate
the effect of the fiber morphology on the elastic properties. It was found
that the mechanical properties increase monotonically with the fiber
contribution proportion and that the fiber morphology can be broadly
classified according to the primary parameters, which determine the
change rate of the mechanical properties with respect to the fiber
contribution proportion, and the secondary parameters, which cause
changes in the mechanical properties according to the change rate
determined by the primary factors. For CNF-dispersed PLA composites
[73], the primary parameters include the fiber orientation angle and
CNF content, while the secondary parameters include the CNF aspect
ratio, CNF/matrix interface, and fiber-to-fiber distance. Furthermore, in
the case of 3D randomly oriented cellulose composites [70], it was found
that the degree of CNF aggregation was a secondary parameter in
addition to the fiber aspect ratio.
3.3. RVE modeling and multiscale analytical process
The flowchart for generating RVE models for the talc filler and CNF-
dispersed PP composites is presented in Fig. 2 (a). First, the dimensions
of the talc filler and CNF were entered. The talc shape is set as a disk of
diameter 4 μm and thickness 0.3 μm based on the SEM observations, X-
ray CT and the laser diffraction particle size analyses in Section 4.1
below. The CNF is determined to have a diameter of 0.03 μm and length
of 1.5 μm based on the published values of the material manufacturer.
The number of talc fillers and CNFs in the RVE is set as 50, and the di­
mensions of the RVE were determined to satisfy the volume content
presented in Table 1. Next, separate RVE models were developed for
each reinforcement, without mixing the talc fillers and CNFs, and each
reinforcement was inserted in succession into the RVE region based on
the RSA algorithm. The center coordinates and orientation angles of the
reinforcement were generated using random numbers and inserted into
the RVE region. If the reinforcement to be inserted extends beyond the
RVE region, it was inserted from the opposite boundary, while taking
Fig. 3. RVE models of PP composites employed in microstructure.
Composites Part B 266 (2023) 110971
into consideration the periodicity of the microstructure. If the rein­
forcement to be inserted interferes with existing reinforcements, the
center coordinates and orientation angle of the reinforcement to be
inserted were re-generated using random numbers. The above process
was repeated until the number of reinforcements reaches a pre­
determined number, which was when the RVE model generation was
completed.
The flow of the multiscale FEA process for PP/talc, PP/CNF, and PP/
talc/CNF composites is presented in Fig. 2(b). The reinforcements were
(14)
placed in the RVE region using random numbers as shown in Fig. 2(a).
Without a large RVE model, the resulting mechanical properties were
subject to variation, and thus, a statistical evaluation that introduces
multiple models is essential. Therefore, the number of RVE models N
was set as two or more. In our previous study [70], it was confirmed that
the variation in the homogenized mechanical properties of composites
can be reduced to within an error of approximately 1% by adopting the
average of multiple RVE models, even when the number of re­
inforcements n (dimensions of the RVE model) is not sufficiently large.
In.
This computation, based on the results of the above study, n was set
as 50 and N as 3. Next, finite element (FE) mesh models were con­
structed via automatic element partitioning after the RVE models were
generated. Here, tetrahedral quadratic elements were employed to
create FE meshes. For the PP/talc composites, the talc fillers were
assumed to be elastic, and the material properties listed in Table 2 were
entered. The matrix was assumed to be elastoplastic, and the nonlinear
stress–strain relationship for PP obtained from the tensile tests (indi­
cated by the black line in Fig. 6) was entered. For the PP/CNF com­
posites, the RVE models are generated as in the case of the PP/talc
composites, and the FE mesh models are constructed. The CNFs are
assumed to comprise an elastic body having the material properties
listed in Table 2, and the matrix comprised elastoplastic PP. In the case
of the PP/talc/CNF composites, the mechanical properties of the PP/
CNF composites obtained from the first homogenization process for the
CNF dispersion models are input into the matrix, and the mechanical
properties of the hybrid reinforced composites are obtained through the
second homogenization process for the talc filler dispersion models. The
mechanical properties in three physically equivalent directions in the
Cartesian coordinate system are averaged for the three models. Exam­
ples of the RVE and FE mesh models used in the computation are pre­
sented in Figs. 3 and 4, respectively. The number of element divisions
was determined after confirming that the elastic modulus and maximum
tensile stress converge within an error of 1% or less. No.
5
T. Kinoshita et al. Composites Part B 266 (2023) 110971

Fig. 4. FE mesh models of PP composites employed in microstructure interfacial phase was set up between the talc fillers or CNFs and the matrix, and the rein­
forcements–matrix interface was assumed to be in the ideal state of perfect bonding.

Fig. 5. SEM images of injection-molded PP/talc and PP/talc/CNF composites.

Fig. 6. X-ray CT images of injection-molded PP/talc and PP/talc/CNF composites.

4. Results and discussion
4.1. Experiments
Dumbbell-shaped tensile specimens of injection-molded PP/talc and
PP/talc/CNF composites were observed via SEM in the cross-section
perpendicular to the loading direction. Fig. 5 presents the SEM images
of the specimens at 10,000 × magnification. Fig. 5(a) presents the PP/
talc composite without MAPP. Fig. 5(b) presents the PP/talc/CNF
composite that contains MAPP. In the observed images, several talc
fillers were highlighted in a circle with a diameter of 10 μm. Talc fillers
of several microns in.
Size were observed scattered in the images. In the micro X-ray CT
observation, innumerable micron-sized talc fillers were uniformly

6
T. Kinoshita et al. Composites Part B 266 (2023) 110971

talc/CNF composites, but not in PP/talc composite.

A comparison of the elastic constant and maximum tensile stress is
presented in Fig. 8. The mechanical properties of PP and the PP/talc, PP/
CNF, and PP/talc/CNF composites are presented from left to right. In
Fig. 8(a), the elastic constants of the PP/talc, PP/CNF, and PP/talc/CNF
composites increased by 16.8%, 15.4%, and 34.1%, respectively, with
the addition of filler compared to those of PP. The maximum tensile
stress in Fig. 8(b) decreased by 2.64% in the PP/talc composite and
increased by 6.93% and 8.58% in the PP/CNF and PP/talc/CNF com­
posites, respectively. The addition of talc and CNF was effective in
enhancing the elastic constant. CNF was also effective for increasing the
maximum tensile stress. However, the addition of talc was ineffective
and had the opposite effect instead. At a low applied strain, the interface
between talc fillers and PP matrix was sound, but as the applied strain
increased, interface delamination occurred, and the reinforcement effect
of the fillers was lost. In contrast, in the case of CNF, the MAPP formed a
strong interface with the CNF and maintained its strengthening effect
even under increased loading.

4.2. Multiscale FEA

Fig. 7. Comparison of stress–strain relationship of injection molded PP com­

Fig. 9 presents a comparison of the tensile test results obtained from
posites via tensile testing.
the previous section and the multiscale FEA results for the stress–strain
relationship of PP composites. The solid lines indicate the numerical
dispersed in three dimensions, although there were a few large fillers
larger than 10 μm in diameter. Fig. 6 shows the micro X-ray CT images of
the PP/talc and PP/talc/CNF composites. In both these cases, no ag­
gregation of the talc fillers or delamination at the filler interface was
observed; however, good dispersion was observed. In the PP/talc com­
posite comprising the use of the commercial talc MB used industrially, a
good dispersion of the talc fillers was also observed, even though it did
not contain MAPP. In contrast, in the case of the PP/talc/CNF composite,
the addition of CNF resulted in an increase in the viscosity, making the
uniform dispersion of the particles difficult. However, the addition of
MAPP is considered to have achieved a good dispersion state without
causing the aggregation of talc fillers. Next, the filler size in the observed
cross section varied with the talc-filler orientation, the size of which
ranged from 2 to 10 μm. The laser diffraction particle size analysis of the
ashed specimen showed that the talc size distribution had a single peak
near 6 μm and ranged from 0.5 to 30 μm, with an average size of 4–5 μm.
SEM observation of the ashed talc fillers demonstrated that the thickness
of the talc filler ranged from 0.1 to 0.5 μm.
Fig. 7 presents the stress–strain relationship of PP composites as
obtained from tensile tests. All the composites exhibited a linear rela­
tionship at an applied strain of less than 1%, this relationship then
became increasingly nonlinear, and a maximum stress was observed in
the strain range of 5%–15%. Compared to PP, the PP/talc, PP/CNF, and
PP/talc/CNF composites all exhibited an increase in elastic modulus. In Fig. 9. Comparison of stress–strain relationship of PP composites obtained via
contrast, the maximum tensile stress increased in the PP/CNF and PP/ tensile tests and multiscale FEA.

Fig. 8. Comparison of mechanical properties of injection molded PP composites.

7
T. Kinoshita et al.
Fig. 10. Relationship between mechanical properties and contribution proportion of CNFs of PP composites with different CNF content.
results, and the dots indicate the test results. PP and the PP/CNF, PP/
talc, and PP/talc/CNF composites are indicated in black, red, blue, and
green, respectively. As it is inferred that delamination occurs at the talc
interface as the tensile load is increased, a comparison was made under
low loading conditions wherein no damage occurs, i.e., in the applied
strain range of less than 5%. The solid lines match well with the dot
plots, thus confirming the validity of the constructed multiscale FEA
model of the PP composites and the soundness of the injection-molded
composites. In the above multiscale simulation, the following three as­
sumptions were made. (1) The matrix in the composites does not lose its
mechanical properties due to the mixing of the reinforcing particles and
has the same mechanical properties as neat PP. (2) The interface.
Between the talc fillers, CNFs, and PP is not damaged up to a loading
strain of 5% and maintains sufficient stiffness owing to the resulting
strong bond. (3) Talc fillers and CNFs do not aggregate and are uni­
formly dispersed within the composite. Therefore, the results of the
multiscale simulation provided the upper limits of the mechanical
properties in the ideal state, where there was no degradation of the
properties of the matrix and interface and no dispersion defects of the
reinforcing particles. The experimental results were in good agreement
with the upper limits obtained from the multiscale simulation, although
the stresses were slightly lower than those resulting from the multiscale
simulation when the applied strain exceeds 3%, which confirms that the
MB mixing process, MAPP content, and injection molding conditions
were appropriate. Using the filler contribution proportion based on the
strain energy, the effect of the CNF addition was first analyzed. The
relationship between the mechanical properties of the PP/CNF com­
posites and the CNF contribution proportion obtained from the multi­
scale FEA is presented in Fig. 10. Here, the added mass of CNF mCNF to
100 g of the PP matrix was 0, 10, and 20 g. The elastic constant is
Fig. 11. Relationship between mechanical properties and contribution proportion of talc fillers of PP composites with different talc and CNF combinations.
8
Composites Part B 266 (2023) 110971
presented in Fig. 9(a) and the maximum tensile stress up to an applied
strain of 5% is presented in Fig. 9(b). The horizontal axis presents the
strain energy of the CNF, calculated from the strain energy in the elastic
region in Fig. 9(a) and in the nonlinear region wherein the applied strain
reaches 5% in Fig. 9(b), as a percentage of the total strain energy in the
microstructure. In our previous studies on unidirectional and randomly
oriented CNF-dispersed PP composites [69,70], it was found that the
effect of the fiber morphology on mechanical properties can be
approximated linearly based on the CNF contribution. Fiber morphology
parameters can be broadly classified into primary factors that determine
the change rate of the mechanical properties with respect to the CNF
contribution proportion and secondary factors that vary the mechanical
properties according to the change rate determined by the primary
factors. The primary factors include the fiber orientation and content,
and the secondary factors include the fiber aspect ratio, degree of ag­
gregation, and the interfacial properties between the fiber and matrix.
Therefore, both the elastic constant and maximum tensile stress pre­
sented in Fig. 10 can be linearly approximated by the dotted red line,
with the matrix property as the intercept on the vertical axis, i.e., the
mechanical properties increased linearly as the fiber contribution
increased. As the CNF content increased, the fiber contribution
increased and its effect on the mechanical properties became stronger,
which resulted in an increase in the slope of the approximate line.
Compared with the elastic range in Fig. 10(a), the difference in stiffness
between the CNF and matrix increased under the condition of an applied
strain of 5% in Fig. 10(b) owing to the nonlinear characteristics of the PP
matrix. That is, the stiffness of matrix decreased to a greater extent in the
nonlinear range than in the elastic range, and the matrix was more easily
deformed than the CNF.
Therefore, the fiber contribution along the horizontal axis was less
T. Kinoshita et al.
when the applied strain reached 5% in Fig. 10(b) than that in the elastic
range in Fig. 10(a) and was approximately halved.
Considering the contribution proportion of the talc fillers, the effect
of talc addition and the influence of CNF addition to PP were analyzed,
and the results on the relationship thus observed between the mechan­
ical properties of the PP composites and the contribution proportion of
the talc fillers is presented in Fig. 11. The masses of the talc fillers and
CNFs, mTalc and mCNF, added to 100 g of the PP matrix were 0, 10, and
20 g. The elastic constant and maximum tensile stress up to an applied
strain of 5% are presented in Fig. 11(a) and (b), respectively. The hor­
izontal axis presents the strain energy of only the talc fillers as a per­
centage of the total strain energy in the microstructure. As indicated by
the black dotted line in the figure, the mechanical properties of the PP
composites can be approximated linearly by intercepting the.
Properties of the PP matrix or PP/CNF composite on the vertical axis.
Compared to the CNF contribution proportion presented in Fig. 10, the
contribution proportion of the talc fillers was small. Although mTalc is
one of the primary factors, it can be observed that the difference be­
tween the lines is small, which indicates that they can be approximated
by straight lines with an identical slope. The stiffness and aspect ratio of
talc fillers were small, and their effect on the composites was small
compared to that of the CNFs, and the difference in the slope of the
approximate line as a function of the talc filler content was considered to
be negligible.
The effect of reinforcement addition on the mechanical properties is
presented in Fig. 11. The increase in both the elastic modulus and
maximum tensile stress from those of neat PP as indicated by the black
plot in the lower left of the figure increases at a nearly constant rate
depending on the amount of talc fillers and CNFs added, i.e., mTalc and
mCNF, respectively. The elastic modulus of CNF was more than eight
times greater than that of the talc filler, and the percentage increase
from that of the neat PP was greater for the CNF. In the case of mCNF = 0,
the average increase in the elastic modulus and maximum tensile stress
with the addition of 10 g of talc fillers was 8.96% and 7.15%, respec­
tively. However, in the case of mTalc = 0, the average increase in the
elastic modulus and maximum tensile stress with the addition of 10 g of
CNFs was approximately 17.7% and 16.8%, respectively. Next, we
considered the three conditions (indicated by A, B, and C in Fig. 11)
wherein the same amount of reinforcement was added. The mass ratio
mPP/mTalc/mCNF was 100/20/0, 100/10/10, and 100/0/20 for A, B, and
C, respectively. The elastic modulus and maximum tensile stress were
1.24 GPa and 2.74 MPa for the PP/talc composite of A, 1.33 GPa and
3.01 MPa for the hybridized PP/talc/CNF composite of B, and 1.45 GPa
and 3.23 MPa for the PP/CNF composite of C, respectively. Thus, as the
talc fillers were replaced by CNFs, both the mechanical properties
increased. In contrast, in the case of polyhydoxybutyrate-co-valerate
(PHBV) composites comprising talc fillers and wood fibers [30],
although the matrix was different, the mechanical properties of the
60/0/40 PHBV/wood composite were inferior to those of the 60/40/0
PHBV/talc composite because the wood fiber had properties that were
inferior to those of the talc filler. In the hybridized 60/30/10 and
60/20/20 PHBV/talc/wood composites, the elastic modulus did not
change significantly, but the tensile strength was less than that of the
PHBV/talc composite. In the case of the 60/10/30 mass ratio with more
wood fibers, the elastic modulus and tensile strength were less than
those of the PHBV/wood composite owing to the interfacial area in­
crease, poor bonding, and occurrence of damage. Therefore, hybridi­
zation with wood fibers can result in a reduced composite weight, but
the mechanical properties are also adversely affected. In contrast, hy­
bridization with CNFs can result in a simultaneous weight reduction and
improved characteristics, which are a significant advantage.
4.3. Design of mechanical properties
Based on the results presented in Section 4.2, the relationship be­
tween the mechanical properties and filler contribution proportion of
9
Composites Part B 266 (2023) 110971
Fig. 12. Conceptual diagram of the relationship between the mechanical
properties of hybrid reinforced composites and contribution proportion of
talc fillers.
the PP composites reinforced with talc fillers and CNFs can be summa­
rized as shown in the schematic of Fig. 12. The mechanical properties of
the PP composites (y) can be expressed by the following linear equation
depending on the contribution proportion of talc fillers (x).
y=αx+β (15)
The change rate of y with respect to x (α) can be uniquely deter­
mined, independently of the talc content and CNF addition. However,
the longitudinal intercept (β) matches the property values of the PP
matrix and PP/CNF composites in the cases of the PP/talc composites
and hybrid reinforced composites, respectively, and varies with the CNF
content.
We tested the validity of Equation (15) in predicting the mechanical
properties of hybrid reinforced composites under three conditions with
unknown PP composites of different filler contents, i.e., talc filler con­
tent of mTalc = 30 g and CNF content of mCNF = 10, 20, and 30 g. In the
prediction, β, i.e., the mechanical properties of the PP matrix and PP/
CNF composites, were assumed to be known experimentally or via a
numerical simulation. In this paper, we used numerical values obtained
from the relevant RVE model for β, but it was also possible to use ap­
proximations based on linear relationships between the mechanical
properties and CNF contribution proportion, as shown in Fig. 10.
Moreover, the change rate in the mechanical properties observed in
Fig. 11 was adopted for α. Furthermore, x is determined from the rela­
tionship between the talc filler contribution proportion and content
ratio, as presented in Fig. 13. The talc filler contribution proportion can
be approximated by a straight line passing through the origin, depend­
ing on the talc filler content ratio. The slope of the approximate line
varies with the CNF content. As in the case of β, if the numerical analysis
data are available for different CNF contents, the slope corresponding to
mCNF can be applied. If there is insufficient numerical analysis data, the
average value of the slopes for different CNF contents should be used. In
the following, the average values for mCNF = 0, 10, and 20 g presented in
Fig. 13 were used and validated as the stringent condition for prediction
accuracy.
As validation values, several actual RVE models of the PP/talc/CNF
composites were generated, and mechanical properties were obtained
via multiscale FEA. The predicted and numerical values of the me­
chanical properties for the three conditions with different contents are
compared in Table 3. The predicted values were within 5% of the nu­
merical analysis values under all the conditions, thus confirming the
validity of the predictions. In the validation in Table 3, the average value
T. Kinoshita et al. Composites Part B 266 (2023) 110971

Fig. 13. Relationship between talc filler contribution proportion and content from multiscale FEA of PP composites.

Table 3
Verification of the proposed composite design for different filler combinations.
Blended mass (g)

PP Talc MB CNF MB Properties Predicted Computed Error [%]

mTalc mCNF

COND 1 100 30 10 E (GPa) 1.49 1.51 1.2

σmax (MPa) 33.2 33.4 0.6
COND 2 100 30 20 E (GPa) 1.69 1.70 0.6
σmax (MPa) 37.1 36.6 1.4
COND 3 100 30 30 E (GPa) 1.78 1.87 4.8
σmax (MPa) 39.7 40.4 1.7

of the slopes among different CNF contents in Fig. 13 was used, but the
accuracy of the predictions would be improved if the respective slopes
corresponding to mCNF = 0, 10, and 20 g were used. Using the respective
slopes according to CNF content instead of the average, the prediction
errors for the elastic constant for conditions 1, 2, and 3 were 0.8%, 0.6%,
and 0.0%, respectively, and those for the maximum tensile stress
improved to 0.8%, 0.8%, and 0.9%, respectively. The proposed Equation
(15) can be used to find a combination of talc filler and CNF contents
that satisfies the target values of the mechanical properties, and a new
design procedure for hybrid reinforced composites has been established.
5. Conclusion
The improvement of the mechanical properties of injection-molded
PP composite materials via the addition of talc fillers and CNFs was
investigated experimentally and using multiscale FEA. The conducted
tensile experiments showed that the talc filler was effective in improving
the elastic properties, while the CNF and MAPP were effective in
improving the elastic properties and maximum tensile stress.
Two-step homogenization multiscale simulation was applied to
hybrid reinforced PP composites, and RVE models were constructed that
reproduced the experimental results well. The new indicator based on
the strain-energy proportion in the microstructure, i.e., the filler
contribution proportion, was introduced to quantify the effect of the
filler addition, and it was found that the mechanical properties of the PP
composites could be approximated linearly using this indicator. A
composite design procedure was proposed based on this relationship. As
examples of verification, the elastic constant and maximum tensile stress
of the unknown PP composites with different filler contents were pre­
dicted within an error of 5%. This procedure also made it possible to find
a combination of the talc filler and CNF contents that satisfied the target
values of the mechanical properties, thus providing a new composite
design for hybrid reinforced PP composites.
Author statement
Taiki Kinoshita: Software, Formal analysis, Investigation, Validation,
Writing - Review & Editing. Tatsuto Yamamoto: Formal analysis,
Investigation, Validation, Writing - Review & Editing. Luo Chao: Vali­
dation, Writing - Review & Editing. Kouta Ide: Validation, Formal
analysis, Resources, Writing - Review & Editing. Kenji Aoki: Validation,
Formal analysis, Resources, Writing - Review & Editing. Yasutomo
Uetsuji: Conceptualization, Methodology, Formal analysis, Validation,
Writing - Original Draft, Visualization, Supervision, Project adminis­
tration, Funding acquisition.
Declaration of competing interest
The authors declare the following financial interests/personal re­
lationships which may be considered as potential competing interests:
Yasutomo Uetsuji reports financial support was provided by Japan
Science and Technology Agency. Luo Chao reports financial support was
provided by Japan Science and Technology Agency.
Data availability
Data will be made available on request.
Acknowledgements
This research was supported in part by the Japan Science and
Technology Agency via the Core Research for Evolutional Science and
Technology program (Grant no. JPMJCR22L4).
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