DOI: 10.5604/01.3001.0014.

7195 Volume 103 • Issue 2 • December 2020

International Scientific Journal

published monthly by the

of Achievements in Materials World Academy of Materials

and Manufacturing Engineering and Manufacturing Engineering

Polypropylene matrix composite

with charcoal filler

M. Polok-Rubiniec *, A. Włodarczyk-Fligier
Department of Materials Engineering and Biomaterials, Faculty of Mechanical Engineering,
Silesian University of Technology, ul. Konarskiego 18a, 44-100 Gliwice, Poland
* Corresponding e-mail address: [email protected]
ORCID identifier: https://orcid.org/0000-0001-8940-0147 (M.P.-R.); https://orcid.
org/0000-0002-6907-1451 (A.W.-F.)

ABSTRACT

Purpose: The aim of the article is to present the thermal, electrical and mechanical
properties of the produced polymer composites with a filler in the form of charcoal powder.
Design/methodology/approach: The tests were carried out on samples of pure
polypropylene (PP) and polymer composites, the matrix of which is polypropylene (PP), and
the filler was charcoal powder with a volume fraction of 10%, 20%, 30%, 40% and 50%.
The tested polymer composites in the form of granules were produced by extrusion, and
then standardised test profiles were made by injection moulding.
Findings: The hardness of the tested composites was determined by the Shore D method,
the grain size distribution of the filler used was determined using the laser method and its
thermal stability was tested using the TGA thermogravimetric analysis. The volume and
surface resistivity were also determined and the density was determined. It was found that
the charcoal powder used as a filler is characterised by high thermal stability – up to 600°C
– and with an increase in its volume share in the polymer matrix, the hardness and density
of the produced composites increases.
Practical implications: The tested composites can be used as structural composites for
complex elements requiring high hardness and strength.
Originality/value: The research results indicate the possibility of using charcoal as a filler
in polymer matrix, which, due to its low production cost, may be an alternative to expensive
carbon fillers.
Keywords: Composite, Polymer composites, Charcoal filler, Thermogravimetric analysis,
Resistivity
Reference to this paper should be given in the following way:
M. Polok-Rubiniec, A. Włodarczyk-Fligier, Polypropylene matrix composite with charcoal
filler, Journal of Achievements in Materials and Manufacturing Engineering 103/2 (2020)
60-66. DOI: https://doi.org/10.5604/01.3001.0014.7195

PROPERTIES

60 Research paper © Copyright by International OCSCO World Press. All rights reserved. 2020
 Volume 103 • Issue 2 • December 2020

1. Introduction
1. Introduction properties, are of significant importance in the modification
of polymeric materials. For several years, among
Specific processing and functional properties of polymer construction materials, interest has been gained in
materials have contributed to their wide application in many composites based on polymeric materials with the addition
branches of industry such as: automotive and aviation, of fillers in the form of powders and dusts, fibres and nano-
pharmaceutical, packaging, textile, construction, chemical additives. Carbon fillers, which include various types of
and cable industries. The most commonly employed carbon black and graphite, as well as hard coal, shungite,
thermoplastics include polyethylene, polypropylene and anthracite, are very popular, they are an alternative to
poly(vinyl chloride). Polymer composites, defined as expensive fillers made of carbon nanotubes [7-10]. Carbon
multifunctional and versatile materials, are becoming fillers are an important component of polymer composites,
increasingly important among construction materials and are due to their favourable properties and the possibility of
now applied in nearly all areas of life [1-3]. modification, which – in combination with appropriate
Composites are heterogeneous materials consisting of a polymer matrices – have a positive effect on the
polymer phase-matrix and dispergated types of other improvement of electrical properties, resistance of polymers
auxiliary substances-fillers, among which active fillers such to environmental factors and UV radiation. Particularly good
as diffirent coal particles deserve special attention. The results were obtained in the case of carbon fillers in
phase of a continuous character is represented by a polyolefin matrices, and materials of this type can be used
composite matrix, while the filler is the dispergated or as: shields against the effects of electric and magnetic fields,
reinforcing phase, which usually has greater rigidity and sensors for measuring various physical quantities,
mechanical strength than the polymer phase. The polymer thermistors, protective coatings against the accumulation of
matrix is designed to combine all the components of a electrostatic charges and heating elements emitting infrared
composite as a whole and is responsible for transferring radiation. It was found that the use of carbon black evenly
stresses between fillers and determines the method of distributed in the polypropylene matrix significantly
processing the composite. A filler is a solid particle with a increases the value of the longitudinal stiffness modulus and
proportion of more than 10% by weight in a polymer matrix. causes a slight increase in the mechanical strength of the
In the case of materials processed by injection or extrusion, material. Literature data confirms that composites with a
the filler content can reach up to 60%, and in the case of polypropylene matrix with a carbon black content of up to
resins up to 90%; it has been found that at such a filling level, 9% can be used as materials for the production of multiple
macromolecular material becomes more a filler binder chemical sensors. The materials with the best electrical
characteristics were obtained from PP and PE composites, in
[2-6].The use of fillers does not guarantee that we will
which the carbon black content was close to the percolation
achieve an improvement in all properties, there is no filler
threshold [8-18]. The use of carbon fillers also increases the
with a comprehensive effect, the improvement of some
hardness and abrasion resistance of polymer composites, as
properties causes deterioration of others. The filler, which
well as the strength properties. The addition of shungite and
is to fulfil specific tasks, should indicate: low absorption and
anthracite in polypropylene matrices increased the hardness
water content, low specific weight, chemical inertness to the
and stiffness of the tested composites. The addition of
polymer and hardener in the case of hardenable materials,
shungite improves electrostatic properties, and the
good wettability and thermal resistance, allowing it to be
processed with the plastic. The most common undesirable composites are hydrophobic [14-19].
side effects of using fillers are: sedimentation (may cause
heterogeneity of the material), agglomeration – reduces
the value of mechanical properties, deterioration of 2. Experimentalprocedure
2. Experimental procedure
processing properties, increase in density, increase in
moisture absorption, which affects the deterioration of Prepared for the tests was a polymer composite with
dielectric properties. The effects of the interaction of fillers a polypropylene matrix with the addition of a filler in the
with a polymer matrix should be determined individually form of a charcoal powder with a percentage share of 10%
for each type of composite and tested using experimental (G2), 20% (G3), 30% (G4), 40% (G5) and 50% (G6).
methods [6-11]. A sample containing 100% polypropylene was designated
Active fillers, which improve mechanical, tribological, G1. The matrix is made of MOPLEN H548R polypropylene
rheological, thermal, dielectric, chemical and processing (PP), it is a homopolymer with high fluidity, which is

Polypropylene matrix composite with charcoal filler 61

 Journal of Achievements in Materials and Manufacturing Engineering

characterised by good stiffness and low viscosity. The filler On a Keithley Instruments Inc., Model 8009 electro-
used in the form of charcoal was created as a result of meter, the surface and volume resistivity of the PP/charcoal
pyrolysis of wood from deciduous beech trees. The charcoal composites tested were determined using a test voltage of
before extrusion was ground twice to the smallest grain on a 300 V. The tests were carried out in accordance with the
finger mill called MUT at the New Chemical Synthesis research methodology according to ASTM D257-14 and
Institute, Inorganic Chemistry Division “IChN” in Gliwice, IEC 60093:1980.
Poland, and then sieved through screens with different mesh The image of microstructure of the filler powders,
sizes. The obtained charcoal powder was dried for several sputtered with gold, were made using an electron scanning
hours at 100°C and mixed with polypropylene granules. The microscope, ZEISS Supra 35, using the accelerating voltage
PP/charcoal blends obtained in this way were homogenised of 15 kV.
using a Göetffert counter-rotating twin-screw extruder, with
an L/D25 ratio, equipped with a bar extrusion head with an
exit diameter of ø 3 mm. The following extrusion parameters 3. Results
Results and
3.  discussion
and discussion
were used: 1st zone temp. 200°C; 2nd zone temp. 220°C; 3rd
zone temp. 230°C; head temp. 240°C; turnover: 6-8 rpm.
The study of the thermal properties of fillers used in
A granulate was obtained by grinding the extruded rod with
polymer composites is necessary to determine the effect of
a laboratory “Metalchem” granulator, and then by injection,
materials reinforcing polymer matrix on the thermal stability
samples were prepared for testing in the form of standard A1
of composites. The thermal stability of charcoal was
type “paddles” in accordance with PN-EN ISO 527-2:2012.
investigated by TGA thermogravimetric analysis in nitrogen
The injection process was performed on a Battenfeld Plus
and pure oxygen atmosphere. The distribution curve of the
35/75 injection moulding machine with the Unilog B2
tested charcoal powder is shown in Figure 1. Charcoal is
control system, with an L/D17 ratio.
characterised by a single-stage decomposition process that
The analyses of measurement of the charcoal powder
takes place above 600°C, a phenomenon typical of carbon
grain size were performed by laser diffraction on a Beckman
fillers. In the temperature range of 25°C-600°C, the charcoal
Coulter LS 13320 apparatus, according to ISO 13320:2009.
powder filler is very stable. One can observe (Fig. 1) a slight
The decomposition temperature of the charcoal powder
loss of mass at the temperature of approx. 80°C, this
was determined using the TGA thermogravimetric analysis.
phenomenon is related to the evaporation of moisture and
The investigations were carried out with the following
volatile organic compounds that occur as components
parameters: Mettler-Toledo XS 105 thermobalance, heating
of charcoal. As a result of the thermogravimetric analysis,
rate: 20°C/min., the flow rate of gases through the measuring
it was found that the charcoal powder is characterised
cell: 60 ml/min. The samples were heated to 600°C under
by good thermal properties and a low content of volatile
a pure nitrogen atmosphere, and to remove the carbon black
compounds.
in an atmosphere of pure oxygen in the temperature range of
600-900°C. The parameter that also affects the mechanical properties
Density was examined using the immersion method in of the produced PP/charcoal composites is the grain
accordance with PN-EN ISO 1183. The following size distribution of the charcoal powder, which determines
measurement conditions and parameters were used: test the size of the contact surface of the filler-matrix
method: A (immersion method), test liquid: distilled water; components.
the material cut out from the injected test pieces was Based on the laser analysis (Fig. 2) and the grain size
examined, the determination was carried out using the distribution of the ground charcoal powder, it was calculated
analytical balance Mettler-Toledo XS 105 with an that more than 75% of the filler particles used have
attachment for density testing. dimensions in the range of 0-20 µm. Based on the analysis
The Shore D scale method according to PN-EN ISO of the SEM images, it was noticed that the charcoal powder
868:2005 was used to determine the hardness of the tested is uniformly distributed in the polypropylene matrix (Fig. 3).
composites. The samples were conditioned at a temperature No agglomerates of the tested filler were found in any of the
of 22°C before the hardness measurement. The test was tested samples, which could adversely affect the strength of
performed on an electronic hardness tester (durometer) by the produced composites. Moreover, it was found that the
Zwick, at a temperature of 22°C. Measurement readings individual filler grains showed a heterogeneous and well-
were taken after 15 s. developed outer surface with a preserved partial structure of

62 Research paper M. Polok-Rubiniec, A. Włodarczyk-Fligier

 Volume 103 • Issue 2 • December 2020

the wood cell walls (Fig. 4). The heterogeneous and especially with a low viscosity at the processing
discontinuous grain morphology of the charcoal powder has temperature, fills the voids in the grains of the charcoal
a positive effect on the adhesion and better combination of powder, thanks to which it adheres better to it, creating
components in the polymer composite. Polypropylene, a kind of mechanical bond.

Fig. 1. Thermogram of the charcoal powder

Fig. 2. Particle size distribution

Polypropylene matrix composite with charcoal filler 63

 Journal of Achievements in Materials and Manufacturing Engineering

An important property of the produced polymer

composites is the hardness, which was determined by the
Shore D method. With the increase of the percentage content
of the filler in the polymer matrix, the hardness of the
produced composite increases. The hardness of the polymer
matrix is 69.5°ShD, along with an increase in the volume
fraction of charcoal powder to 50% (G6), the hardness
increases to 76.7°ShD (Tab. 1).

Table 1.
Density and hardness of matrix PP and PP/charcoal
composite
Marking of the Density, Hardness,
samples g/cm3 °ShD

Fig. 3. Microstructure of charcoal powder G1 0.8642 69.5

G2 0.8822 72.1
G3 0.9328 72.7
G4 1.0160 74.0
G5 1.0736 75.0
G6 1.3500 76.7

Such a large increase in hardness with a maximum filler

percentage of 50% may indicate that this is the optimal
content in the case of improving the hardness of the
produced composites. The 50% filler content will not affect
the permanent deformation of the sample. A slight change in
hardness was noticed in the case of samples with the content
of G2 10% (72.1°ShD) and G3 20% (72.7°ShD), which is
probably related to a slight influence of this content on the
hardness of the PP/charcoal composite produced.
The volume and surface resistivity of the produced
Fig. 4. Surface morphology of a single gran of charcoal PP/charcoal composites were also tested, due to the filler
powder used in the form of charcoal powder, which is to improve the
electrical properties of the polymer composite. Charcoal has
The higher the filler content in the composite material, a three times higher energy value than wood and shows
the higher its density (Tab. 1), similar trends have been strong absorption, due to its highly developed surface, and
found in many scientific publications [6-19]. The composite is characterised by a low tar content. The introduction of
with 50% charcoal powder has a density of 1.35 g/cm3, while charcoal powder into the polypropylene matrix resulted in a
pure PP has a density of 0.8642 g/cm3. decrease in volume and surface resistivity (Tab. 2), which
A significant increase in density is related to a higher decreased the electrical insulating properties of the produced
density of the filler, approx. 1 g/cm3. The density test results composites. The produced PP/charcoal composites can be
obtained for the described samples correspond to the used wherever an increase in anti-electrostatic properties is
theoretical calculations, which confirms the lack of gas needed – e.g. in electronics or components working in
inclusions in the material, which could indicate degradation potentially explosive areas. It is worth noting that the tests
of the material or its porosity caused by the emission of showed a much greater impact of the filler introduction on
volatile compounds from the filler. the volume resistance value than on the surface resistance.

64 Research paper M. Polok-Rubiniec, A. Włodarczyk-Fligier

 Volume 103 • Issue 2 • December 2020

Table 2.
Effects of charcoal content on surface and volume resistance
Surface resistance Volume resistance
Marking of the samples (ASTM D257/IEC 60093) (ASTM D257/IEC 60093)
U=300 V, Ω U=300 V, Ωcm
G1 1.17E+17 1.12E+15
G2 6.64E+14 4.06E+15
G3 6.41E+14 1.89E+08
G4 1.01E+15 5.00E+07
G5 1.61E+15 5.12E+07
G6 1.69E+15 3.77E+08

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