Composites: Part A 35 (2004) 423429

www.elsevier.com/locate/compositesa

Thermal conductivity, thermal diffusivity, and specific heat capacity

of particle filled polypropylene
Bernd Weidenfellera,b,*, Michael Hoferc, Frank R. Schillingc
a
Institute of Polymer Science and Plastics Processing, Technical University of Clausthal, Agricolastrasse 6, D-38678 Clausthal-Zellerfeld, Germany
b
Institute of Metallurgy, Robert-Koch-Str. 42, D-38678 Clausthal-Zellerfeld, Germany
c
GeoForschungsZentrum Potsdam, Section 4.1 Experimental Geochemistry and Mineral Physics, Telegrafenberg, D-14473 Potsdam, Germany
Received 22 July 2003; revised 19 November 2003; accepted 20 November 2003

Abstract
By the addition of metal and oxide particles to plastics, thermal transport properties, heat capacity, and density of polymers can be varied
systematically. Composites samples of polypropylene (PP) with various fillers in different fractions (up to 50 vol%) were prepared with an
injection moulding process to study the evolution of the properties as a function of filler content. Standard filler materials like magnetite,
barite, talc, copper, strontium ferrite and glass fibres were used. Thermal diffusivities, specific heat capacities and densities of the prepared
composite samples were measured, and thermal conductivities were derived. Thermal conductivity of the polypropylene is increased from
0.27 up to 2.5 W/(m K) with 30 vol% talc in the polypropylene matrix. Thermal conductivities of the filled polypropylene samples are
compared with the modelled values according to Hashin and Shtrikman. The interconnectivity of the particles in the polypropylene matrix is
derived from a comparison between modelled and measured thermal conductivity values. For higher talc and glass fibre content in PP
plastics, a complete interconnectivity is achieved, while copper particles in PP show a very poor interconnectivity. Specific heat capacities
and thermal diffusivities of magnetite and barite filled polypropylene were measured in the temperature range from 300 to 395 K.
q 2004 Elsevier Ltd. All rights reserved.
Keywords: A. Polymer-matric Composites (PMCs); B. Thermal Properities; D. Physical Methods of testing; E. Injection Moulding

1. Introduction graphite [4], aluminum nitrides [3,5] or magnetite particles

Commonly used plastics, such as polypropylene (PP) or
polyamide are electrical insulators with a low thermal
conductivity. New applications, like heat sinks in electronic
packaging, require new composites with higher thermal
conductivity. By the addition of fillers to plastics the thermal
behaviour of polymers can be increased significantly. Such
filled polymers with higher thermal conductivities than
unfilled ones become more and more an important area of
study because of the wide range of applications, e.g. in
electronic packaging in applications with decreasing
geometric dimensions and increasing output of power, like
in computer chips or in electronic packaging [1 3]. The
higher thermal conductivity can be achieved by the use of a
suitable filler such as aluminum [1], carbon fibres and
* Corresponding author. Present address: Institute of Metallurgy, Robert-
Koch-Str. 42, D-38678 Clausthal-Zellerfeld, Germany. Tel.: 49-5323-
723708; fax: 49-5323-723184.
E-mail address: bernd.weidenfeller@tu-clausthal.de (B. Weidenfeller).
1359-835X/$ - see front matter q 2004 Elsevier Ltd. All rights reserved.
doi:10.1016/j.compositesa.2003.11.005
[6]. Furthermore, the cooling behaviour in the mould of the
injection moulding machine is influenced by the thermal
properties of the used filler, where a high thermal diffusivity
is responsible for a high efficiency of the moulding process.
A high thermal diffusivity is achieved for samples with a
high thermal conductivity and low density and low heat
capacity.
Published values of thermal conductivities of the same
filler materials in different polymer matrices vary drastically
and a comparison of different materials is difficult [6], as
most of these studies do not vary systematically the filler
content and do not describe detailed enough the filler and
the microstructure of the composite samples. Therefore,
polypropylene samples with different commercially avail-
able fillers were prepared by extrusion and injection
moulding using various volume fractions of filler content
to systematically vary density and thermal transport
properties of these composites. The thermal properties,
heat capacity and density of these samples were investigated
424 B. Weidenfeller et al. / Composites: Part A 35 (2004) 423429
and correlated to the amount and the kind of the filler
material.
2. Theoretical considerations
The thermal conductivity of a homogeneous compo-
site can be derived according to the model of Hashin
Shtrikman (HS). The thermal conductivity of a composite
consisting of a homogenous matrix M with a thermal
conductivity lM ; spherical particles P with a thermal con-
ductivity of lP ; and a volume fraction of spheres xP relates
to [6]
2lM lP 2 2xP lM 2 lP
lComp;l lHS2 lM
2lM lP xP lM 2 lP
with sHS2 the HS lower boundary [7] for a matrix with a
low thermal conductivity lM , lP :
If the matrix consists of a highly thermally conducting
phase surrounding particles of low thermal conductivity, the
HS upper boundary sHS would describe the conductivity
behaviour lM . lP ; i.e. a high conducting talc matrix
would surround polymer particles
2ltalc lPP 2 2xPP ltalc 2 lPP
lComp;l lHS ltalc 2
2ltalc lPP xPP ltalc 2 lPP
Eqs. (1) and (2) only depend on the volume fraction of
the materials and do not take into account the micro-
geometry and morphology of filler and matrix, while using a
spherical approximation for particle shape. For a compari-
son of measurements of particle filled polymer composites
with Eqs. (1) and (2) the particles have to be randomly
distributed in the matrix.
Using the model conductivities after Hashin and Shtrik-
man [7], lHS and lHS2 ; the interconnectivity of the
conducting phase Xinterconnected can be revealed according to
Schilling and Partzsch [12]
lmeasured 2 lHS2
Xinterconnected
lHS 2 lHS2
The as determined interconnectivity is a relative measure
to an ideally interconnected network of the high thermally
conducting phase. As the conductivity is dominated by the
smallest junctions of the path of high conductivity, the
resultant interconnectivity is dominated by these junctions.
If, for example, the high conducting phase is interconnected
by point contacts, most of the high conducting phase will
not directly contribute to the overall conductivitynot
ideally interconnectedand the determined interconnectiv-
ity is dominated by point contacts. This especially holds
true, if the difference between the conductivities of the
different phases is huge.
In an homogenous body, thermal diffusivity a and
thermal conductivity l are inter-related by specific density
r and specific heat capacity cp according to
l acp r 4
while thermal diffusivity a quantifies the thermal equili-
bration process and the thermal conductivity l describes the
ability of a body to transport heat.
3. Experimental
3.1. Materials and sample preparation
Test materials were supplied by Minelco B.V. (The
Netherlands). Minelco B.V. prepared in cooperation with
1 RTP s.a.r.l (France) several polypropylene (PP) compounds
with various fillers (Fe3O4, BaSO4, Cu, glass fibres, talc,
SrFe12O19, cf. Table 1) in an extrusion process similar to
that one described in Ref. [6]. The filler fraction was varied
from 0 to 50 vol%.
With an injection moulding machine (Allrounder 320C
600-250, Arburg, Germany) standard samples for measuring
tensile properties together with a rod for thermal measure-
ments of 10 mm diameter and 130 mm length were
prepared in one mould. Selected injection moulding
parameters are listed in Table 2. For thermal diffusivity
measurements, small cylinders of 10 mm diameter and
5 6 mm height were cut out of the injection-moulded rods.
3.2. Experimental methods
3.2.1. Specific density
The specific density rC of the composite materials was
determined using Archimedes principle, where the volume
is measured by the buoyancy in a fluid with known density.
The weight and buoyancy measurements were performed
with an electromagnetic balance (LA203S, Sartorius,
Germany). Isopropyl was chosen as fluid. The measurement
conditions as proposed in standard DIN 53479 [13] were
applied. The accuracy of density measurements is # 0.5%.
3 3.2.2. Specific heat measurements
Specific heat capacity measurements were performed
using a modulated differential scanning calorimeter (DSC
2920 modulated, TA Instruments). Measurements were
carried out in the temperature range from 2 10 to 50 8C with
a heating rate of 5 K/min. The DSC was calibrated in the
same temperature region before each experiment, using a
sapphire sample as standard, with a well-known specific
heat capacity. This leads to an accuracy of # 2% for the
presented data. Heat capacity values at 23 8C are presented.
3.2.3. Thermal diffusivity measurements
The thermal diffusivity of the polymers is measured by a
transient method, closely related to laser-flash experiments
[14]. The used transient technique is especially optimised
for measurements of polyphase aggregates. A temperature
 B. Weidenfeller et al. / Composites: Part A 35 (2004) 423429 425

Table 1
Selected properties of filler materials

Magnetite Barite Talc Strontium ferrite Copper Glass fibres

(Fe3O4) (BaSO4) (Mg3[Si4O10][OH]2) (SrFe12O19) (Cu)

Thermal conductivity (W/(m K)) a: 4.61 ^ 0.42 : 2.07 ^ 0.02 : 1.76 ^ 0.00 .3 401 1.21.5
a: 5.10 k: 2.92 ^ 0.07 k: 10.69 ^ 1.35
l11 : 9.7 a: 1.72 ^ 0.04 a: 2.97
a: 3.00 ^ 0.10
a: 6.10 ^ 0.90
Ref. [8] [8] [8] [9] [10] [11]
Mean particle diameter (mm) 9 1.5 2.0 1.5 15 11
Particle shape Irregular Irregular Platelet Irregular Fibre
Density (g/cm3) 5.1 4.48 2.78 5.11 8.94 2.58

a denotes measurements on monomineralic aggregates. Directions of anisotropy are specified by the thermal conductivity tensor l11 ; l22 ; l33 ; where l33
is parallel to the crystals optical c-axis; and the optical c-axis lies within the plane defined by l11 and l22 or by the thermal conductivity components normal or
parallel to the direction of maximum thermal conductivity ( , k).

signal is transferred to the upper side of the sample and
registered by a thermocouple. The transferred temperature
signal starts a thermal equilibration process in the specimen,
which is recorded by a difference thermocouple on the rear
surface and used for the evaluation of thermal diffusivity.
The thermal diffusivity of the sample is evaluated from the
temperature time evolution recorded at the two thermo-
couples using a one-dimensional finite difference scheme,
which allows consideration of heat losses from the sample
surfaces [15]. The finite difference scheme is based on a
discrete formulation of diffusivity equation

 ! has an apparent lower thermal conductivity (lbarite <
T 2 T
a 5
t x 2
where t is time, a thermal diffusivity, x distance, and T
temperature.
The temperature time curve recorded by difference
thermocouple is sensitive to the thermal diffusivity of the
sample. Similarly to laser-flash experiments, the evaluation
procedure does not require the absolute heat transfer. A least
square algorithm is utilized to determine the thermal
diffusivity, while varying systematically the thermal
diffusivity value in the finite difference scheme. A detailed
description of the apparatus is given by Schilling [15]. The
accuracy of the measurements of the polyphase aggregates
is 3 5%.
glass fibre and barite filled polypropylene composites is
relative poor, whereas magnetite and strontium ferrite
increases the thermal conductivity of the PP significantly.
The enhancement of thermal conductivity of polymers by
the use of magnetite or strontium ferrite is in the same range
as if standard fillers like aluminum oxide (Al2O3) or
aluminum nitride (AlN) are used to increase thermal
conductivity of polymers [6].
To enhance the density of polymers, both barite and
magnetite are used. However, the competing material to
magnetite for the increase of density of polymersbarite
2 W/(m K)) than magnetite (lmagnetite < 5 W/(m K)) and
strontium ferrite (lstrontium ferrite . 3 W/(m K) approximated
from its structure and chemical composition according to
Slack [9]) (Table 1).
Copper (lcopper < 400 W/(m K)) has a much higher
thermal conductivity than talc (ltalc < 10:6 W/(m K)) and
the other used filler materials. Surprisingly, the thermal

4. Results

The thermal conductivities of the investigated samples

are plotted in Fig. 1. The increase in thermal conductivity of

Table 2
Selected injection moulding parameters during preparation of sample rods
for measurements of thermal diffusivity

Mass temperature 200 8C

Mould temperature 20 8C
Cycle time 70.8 s
Injection pressure 6 107 Pa Fig. 1. Thermal conductivity of injection-moulded polypropylene-particle-
composites with different fillers and various filler fractions.
426 B. Weidenfeller et al. / Composites: Part A 35 (2004) 423429

Fig. 2. Comparison of specific heat capacities at room temperature of several injection-moulded particle filled polypropylene samples for several filler
fractions.

conductivity of talc filled PP are comparably high polypropylene samples are very low. For filler fractions
(< 2.5 W/(m K) for 30 vol% filler) and the copper filled higher than 30 vol% the specific heat capacities of barite
PP shows much lower conductivity values (< 1.25 W/(m K) and copper filled PP is significant lower than the specific
for 30 vol% filler) compared to the values of the other heat capacities of the other investigated materials. While the
composite materials (Fig. 1). specific heat capacity of talc and magnetite filled PP are
about the same for 15 and 30 vol% filler fraction, the
5. Discussion thermal diffusivity of talc filled PP is considerably higher
(cf. Fig. 3) than the diffusivity of the magnetite filled PP and
The high thermal conductivity of the talc filled PP can be the other investigated composites. As expected from the
explained by the relative high thermal conductivity of talc high thermal conductivity of copper, the thermal diffusivity
ltalc 10:69 W/(m K) parallel to the direction of maximum of copper filled PP at 30 vol% filler fraction is clearly higher
thermal conductivity (cf. Table 1). As the thermal than the diffusivities of the other investigated composites
conductivity of copper is approximately 40 times higher except talc filled PP.
than the thermal conductivity of talc one might expect that
the thermal conductivity of copper filled polymers is much
higher than the thermal conductivity of the talc filled PP.
However, the opposite is observed. The talc filled PP shows
a higher thermal conductivity ltalc;PP < 2:5 W/(m K) that is
twice as high as the copper filled PP with a thermal
conductivity of approximately lCu;PP < 1:25 W/(m K) at a
filler fraction of 30 vol% for both composites. One might
regard that the density of copper is approximately three
times higher than the density of talc, and relates the large
difference in the thermal conductivity between the different
composites as a result of the differences of heat capacities
and density (Eq. (4)). However, the difference in density
(3 ) and heat capacity (, 2 ) (Fig. 2) of the copper and
talc filled PP cannot explain the high discrepancy in the
observed thermal conductivity and thermal diffusivity
behaviour.
Figs. 2 and 3 show the specific heat capacities and the
thermal diffusivities of the investigated materials. It can be Fig. 3. Comparison of thermal diffusivity at room temperature of injection-
seen, that the heat capacities of the copper filled moulded particle filled polypropylene samples for different filler fractions.
 B. Weidenfeller et al. / Composites: Part A 35 (2004) 423429
Fig. 4. Interconnectivity of filler particles in polypropylene at a filler
fraction of 30 vol% at room temperature (for details see text).
The thermal transport properties cannot be explained
solely by the differences in the properties of the filler
materials. Therefore, the microstructure and texture has to
be taken into account. As described by Eqs. (1) and (2), the
thermal conductivity of composites strongly depends on the
thermal conductivity of the matrix and the interconnectivity
of the higher conducting phase (Eq. (3)). The observed
different values of thermal conductivities in talc and copper
filled PP can be related to the interconnectivity of the
particles using Eq. (3).
Fig. 4 shows the interconnectivity of the investigated
materials for a filler fraction of 30 vol%. For the
calculations of the upper and lower HS boundary the bold-
faced values of thermal conductivity of Table 1 are used.
The high interconnectivity around Xinterconnect < 1 of the
glass fibre and talc filled polypropylene is conspicuous. For
interconnectivity close to 1 the measured values reach the
upper HS boundary (Eq. (2)). This means that the glass
Fig. 5. (a) SEM micrograph of a fracture of the glass fibre filled PP sample with glass fibres aligned parallel to the flow direction of the polypropylene in the
mould of the injection moulding machine, and (b) SEM micrograph of a fracture of the talc filled PP with talc plates aligned parallel to the flow direction in the
mould.
427
fibres and talc form a complete interconnected network.
This high value of interconnectivity might be due to an
alignment of the glass fibres and the talc particles in the
polypropylene matrix (cf. Fig. 5) into the flow direction
during the injection moulding process of the sample rods.
This behaviour simulates quite well polypropylene particles
in a glass matrix or polypropylene particles in a talc matrix,
respectively. However, the model conductivities after
Hashin and Shtrikman require spherical particles. This
condition is not fulfilled for the talc and glass fibre fillers.
However, the isotropic approach by HS gives a first
approximation for the interconnectivity behaviour of these
composites, as the upper and lower HS boundaries describe
maximum and minimum estimates for macroscopic iso-
tropic two phase compositesregardless of the detailed
microstructure.
In Fig. 4 the very low interconnectivity of the copper
filled polypropylene is remarkable. This interconnectivity is
the result of poor contacts between the copper particles and
indicates that the copper particles are well wetted by the PP
matrix. The differences may be the result of a different
wetting behaviour of filler and matrix or due to a clustering
of barite and magnetite particles. Therefore, the clear
differences in the interconnectivity between magnetite or
barite filled PP and copper filled PP cannot be explained by
the differences in particle sizes alone and therefore further
research is required to clarify the experimental results.
As can be seen in Figs. 1 3 the thermal conductivity, the
specific heat capacity and the thermal diffusivity of
magnetite filled polypropylene samples are higher than the
corresponding values of polypropylene with the competing
filler material barite. This also holds true at temperatures
higher than room temperature. Fig. 6 shows the dependence
of the specific heat capacity of magnetite and barite in the
temperature range from 295 to 385 K. The heat capacities
428 B. Weidenfeller et al. / Composites: Part A 35 (2004) 423429
Fig. 6. Temperature dependence of the specific heat capacity of PP filled
with 45 vol% magnetite and barite. The symbols are measured values, the
lines represent linear fits.
of magnetite and barite increase in the measured temp-
erature range from cp Fe3 O4 ; 300 K 1:20 J/(g K) and
cp BaSO4 ; 300 K 0:77 J/(g K) up to cp Fe3 O4 ; 392 K
1:87 J/(g K) and cp BaSO4 ; 395 K 1:29 J/(g K). In the
same temperature range the thermal diffusivity (Fig. 7)
decreases from aFe3 O4 ; 300 K 0:443 mm2 /s and
aBaSO4 ; 300K 0:353 mm2/s down to aFe3 O4 ; 392 K
0:322 mm2/s and aBaSO4 ; 395 K 0:244 mm2/s.
Analogous to the differences in the measured values
between magnetite and barite filled polypropylene it was
proven in our injection moulding experiments that the
cooling time in injection moulding process for magnetite
filled PP is shorter than for barite filled PP, this is a direct
consequence of the higher thermal diffusivity of the
magnetite filled composite.
Fig. 7. Temperature dependence of the thermal diffusivity of PP filled with
45 vol% magnetite and barite. The symbols are measured values, the lines
represent linear fits.
If a material with a high thermal conductivity but
considerable low density is requested, talc filled PP will be a
good candidate. Similarly to the reduced cooling time for
magnetite filled PP, the talc filled PPwhich has the highest
thermal diffusivity of the examined sampleswill have the
lowest cooling time and therefore enhance the productivity
in the moulding process.
6. Conclusions
Thermal properties of injection-moulded polypropylene
samples with various fillers and filler fractions were
prepared and investigated. As filler materials copper, talc,
magnetite, strontium ferrite, barite and glass fibres were
selected to vary over a broad range of different filler
properties, ranging from 2.58 (glass fibres) to 8.94 g/cm3
(copper) in density, and from nearly 1.5 (glass fibres)
to approximately 400 W/(m K) (copper) in thermal
conductivity.
Surprisingly, the highest thermal conductivity of a
composite was achieved with talc which has a moderate
thermal conductivity (ltalc < 10:6 W/(m K)) compared to
the high thermal conductivity of copper ( lcopper <
400 W/(m K)). The thermal conductivity of the talc filled
polymer was increased from 0.27 up to 2.50 W/(m K) with
30 vol% talc filler. This behaviour is a consequence of the
microstructure of talc filled PP showing a high intercon-
nectivity of the talc crystals. On the other hand, the thermal
conductivity of copper filled polypropylene is in spite of
the very high conductivity of pure copper lower than talc
filled PP composites due to a poor interconnectivity of the
Cu-particles.
The talc platelets and the glass fibres were aligned in the
test samples by the injection moulding process. This leads to
a thermal conductivity close to the HS upper boundary
and simulates a talc matrix and a glass matrix, respectively,
which surrounds polypropylene particles. Also the specific
heat capacities and thermal diffusivities of talc filled
polypropylene are much higher than that of copper filled
polypropylene.
A comparison of the two competing materials, barite and
magnetite, for increasing the weight of polymers, shows for
magnetite filled PP a higher thermal conductivity than for
barite filled PP. This results not only from small differences
in specific density but also from lower specific heat capacity
and thermal diffusivity of barite filled PP compared with
magnetite filled PP. The significant lower thermal conduc-
tivity of the barite filled PP compared to the magnetite filled
one can be directly related to the substantially lower thermal
conductivity of barite < 2 W/(m K) compared to the higher
conductivity of magnetite < 5 W/(m K). Furthermore, the
higher interconnectivity of magnetite filled PP increases
the thermal conductivity of the composite compared to the
barite filled one.
In the temperature range from 300 to 385 K the specific
heat capacity of the composites is increased for PP with
 B. Weidenfeller et al. / Composites: Part A 35 (2004) 423429
magnetite (from 1.20 up to 1.87 J/(g K)) and for PP with
barite fillers (from 0.77 up to 1.29 J/(g K)). In the same
temperature region the thermal diffusivity decreases.
This study indicates that for injection moulding pro-
cesses of heavy plastic composites magnetite might be a
good choice, as it allows higher production cycles than the
barite filled composites. To increase the thermal conduc-
tivity significantly without increasing the density very
much, talc filled composites seem to be a good candidate
and can help to save cooling time during the injection
moulding process.
Acknowledgements
The authors would like to thank P. Duifhuis and
R. Mangnus, Minelco B.V. (Rotterdam, The Netherlands)
for the support and providing materials.
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