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Procedia Manufacturing 12 (2017) 221 – 229

International Conference on Sustainable and Intelligent Manufacturing, RESIM 2016, 14-17


December 2016, Leiria, Portugal

Study of Wood-Plastic Composites with reused High Density


Polyethylene and Wood Sawdust
J.F.Hortaª*, F.J.Simõesª, A.Mateusª
ªCDRsp-Center for Rapiud and Sustainable Product Development,2430-028 Marinha Grande, Portugal

Abstract

In recent years, concerns about environmental preservation have motivated industries to adapt towards more environmentally
friendly materials, resorting for this to recycled and waste materials. This has been the center for a growing number of research
studies to enable less and less virgin materials waste [1], [2]. The use of recycled thermoplastics has been considered for the
production of wood and plastic composites in recent years [3]. New materials have been developed with a view to developing
eco-composites, materials with several advantages, both at an environmental level and an ecological level, including natural
polymers[4]. Solid plastic waste from polymers such as high density polyethylene is creating new challenges for an industry that
is seeking greater waste utilization to ensure products that are efficient ecologically and environmentally friendly [5][6]. The cost
and quality of these composites depends on the waste type incorporated, on the material and the processing route used [4]. The
sawdust waste produced by the sawdust industry is about 5% per tree log, which makes this an important renewable raw material
[2]. The objective of this study was to investigate composite material properties developed from reused HDPE thermoplastic
material from the thermoplastics injection industry and pine sawdust from the lumber industry. The materials were developed
with three different volume fractions of pine sawdust and two different particle sizes, mixed in a double screw extruder. A
validation of a processing route – injection molding – was also performed.
© 2017 Published
© 2017 by Elsevier
The Authors. B.V. This
Published by is an openB.V.
Elsevier access article under the CC BY-NC-ND license
(http://creativecommons.org/licenses/by-nc-nd/4.0/).
Peer-review under responsibility of the scientific committee of the International Conference on Sustainable and Intelligent
Peer-review under responsibility of the scientific committee of the International Conference on Sustainable and Intelligent
Manufacturing.
Manufacturing

Keywords: Materials; Sawdust; HDPE; Recycled.

* J.F.Horta Tel.:+351244569441.
E-mail address: joao.f.horta@ipleiria.pt

2351-9789 © 2017 Published by Elsevier B.V. This is an open access article under the CC BY-NC-ND license
(http://creativecommons.org/licenses/by-nc-nd/4.0/).
Peer-review under responsibility of the scientific committee of the International Conference on Sustainable and Intelligent Manufacturing
doi:10.1016/j.promfg.2017.08.026
222 J.F. Horta et al. / Procedia Manufacturing 12 (2017) 221 – 229

1. Introduction

Technology has contributed to a major development of mankind, but many times at the expense of the
environment and natural resources. Toxic, non-degradable materials were, for many years, the basis on which this
development was carried out. Increasing awareness for sustainability issues led governments and companies to
derive towards using ecologically appropriate materials. To reduce, reuse and recycle have been increasingly applied
principles in practice, when dealing with materials, processing and product design and development. Incorporating
recycled materials back into the product lifecycle enables a visible reduction in virgin raw materials usage, thus
lowering the impact on natural resources[7], [8].
Composite materials, being defined as the combination of two different types of materials, have high potential for
contributing for this reduction in virgin materials usage. This is because they can consist on a combination of
materials, that otherwise would be wasted, into a single, different material, which can be used in a new application.
Classic composite mechanics has already addressed the main issues of the matrix / reinforcement system, and how
the type, size and distribution of reinforcements affect the composite material properties. Traditionally, particle-
reinforced composites are manufactured towards cost optimization of parts, whereas fibre and especially continuous
fibre composites are designed towards increased mechanical performance. In this work, the incorporation of natural
particles - sawdust - into a synthetic matrix - high density polyethylene - is studied. The composite material that
emerges is called a Wood-Plastic Composite, or WPC. The base materials were chosen because they both are waste
materials from local industries. This means that the re usage of these materials may have an impact on local
economy [9]–[11].
The study focused on obtaining mixtures of high-density polyethylene (HDPE) and sawdust having different
particle sizes and several mass percentages. These materials were then characterized mechanically, after being
processed by injection moulding.

2. Composite Materials

Nowadays, materials are usually classified into five main groups: metals, ceramics, polymers, semiconductors
and composites [8]. Composite materials are composed of 2 or more materials: a matrix material that transmits the
mechanical stresses; and a reinforcement material that supports the stresses in the composite. The major evolution of
this type of materials occurred in the second half of the twentieth century. In the 1980s and 1990s its use became
common in space vehicles and military aircraft because they were materials with better performance than the
materials used until then. Concerns about the environment and reduction of manufacturing costs led to a
reintegration of the use of natural fibres in reinforced composite technologies [10], [12], [13].
The Wood-Plastic Composite sector has been a steadily growing within the plastics industry. WPCs are usually
obtained from wood waste such as bamboo, pine, straw, and other cellulose based fibres, mixed with synthetic
plastics such as polyethylene, polypropylene and polyvinyl chloride. Coupling agents, lubricants and stabilizers are
usually added to enable good adhesion and processability to these composites [11], [14], [15].
High-density polyethylene has been used since the 1950’s. Nowadays, it remains as one of the most used
thermoplastics. It has a good impact resistance, as well as a good chemical resistance. It can achieve crystallinity
levels up to 90%, meaning increased mechanical properties. It is also easily processed by extrusion, blow moulding
and injection moulding [16].
Wood is a very important natural resource, especially in Portugal. Woodworking is a strong industry, and has
been evolving successfully towards incorporating new designs and technologies into their products. Pine wood
(Pinus Pinaster) is one of the main wood types used in Portugal, and hence one of the main sources of wood
residues (sawdust)[17].

3. Experimental procedure

The flowchart on Fig. 1 shows the general procedure undertaken to develop and characterize the composite
materials. Pine sawdust was dried and controlled for granulometry prior to the mixing stage. Then, HDPE is added
J.F. Horta et al. / Procedia Manufacturing 12 (2017) 221 – 229 223

to pine sawdust in a dual screw extruder, along with an additional compatibilizer agent – Dupont Fusabond® E265,
thus producing the composite material. Each individual step is described below.

Fig. 1. Materials Processing Route Used

3.1. Sawdust Processing

Sawdust drying: The drying step is relevant for wood since it enables a better dimensional stability and
uniformity within the batch. It also improves the sawdust adhesion to the polymeric material. Drying of the sawed
pine was accomplished using a furnace. When all the water in the material evaporated, the mass stabilized.
Sawdust granulometry: for granulometry assessment, a screening procedure was undertaken. Screening is a
method of particle separation in which solid particles are placed on a sieve with a certain aperture size. The finer or
smaller particles pass through the sieve and the larger ones do not. This separation is done to split the granular solid
into homogeneous fractions and obtaining fractions with particles of the same size.

3.2. Composite Processing:Extrusion

In the extrusion process, the sifted material of pine sawdust and recycled HDPE (granulated) were mixed. The
adjustment of the mixture ratio is accomplished by changing the rotation speed of the feeding screws from each
hopper, as well as each one of the main screws. Preliminary tests were performed to gain awareness on this
procedure. It was then found that the largest mass percentage of sawdust possible to process using the existing
extruder was 12.5%. This corresponds to setting the spindle speed of the secondary hopper (sawdust) to the
maximum, and the spindle speed for the primary hopper containing HDPE to the minimum. A percentage higher
than 12.5% in mass would be possible only by performing additional re-processing steps by extrusion, using
composite and sawdust as initial materials. This option was discarded because the material would be subjected to
224 J.F. Horta et al. / Procedia Manufacturing 12 (2017) 221 – 229

melting more than one time, causing its degradation. Instead, the material was pre-mixed outside the extruder, and
extruded in only one step. Several mass ratios of sawdust/HDPE were considered, based on an initial value of
11.25% (set to be lower than the limit of the extruder). From this baseline, values of 22.5% and 45% were obtained
by combining mixtures. For the ratios considered, sawdust was sieved between 300 to 500 Pm (Mixture Table 1)
and 500 to 700 mm (Mixture 2 Table 1).

Table 1. Metodology to do Mixtures for Material Characterization


% of Sawdust 11,25 22,5 45
Kind of Mixture Mixture 1 Mixture 2 Mixture 1 Mixture 2 Mixture 1 Mixture 2
Hopper 1 HDPE+fus HDPE+fus HDPE+fus+11,25 HDPE+fus+11,25 HDPE+fus+33,75 HDPE+fus+33,75
Hopper 2 11,25 11,25 11,25 11,25 11,25 11,25

3.3. Materials Characterization

A thermal characterization was carried out initially through a simultaneous thermal analysis (STA) of the pine
sawdust this enabled to access the processing temperature limits for this material. The composite material
characterization was performed on specimens obtained by injection moulding. Tensile tests were then carried out on
composite materials developed. Thermogravimetric analysis (TGA) was afterwards used to verify the real
composition on manufactured specimens.

3.3.1. Simultaneous Thermal Analysis(STA) and Thermogravimetric Analysis(TGA)

The simultaneous thermal analysis (STA) test is a technique that combines the benefits of thermal analysis and
differential scanning calorimetry in which the energy flow is measured to or from a sample, quantifying the changes
as exothermic or endothermic in an experience. The STA is thus a hybrid material characterization process in which
samples can be analysed through differential temperature differential analysis (DTA or DSC) with proven
thermogravimetric technology (TG or TGA).
For the current analyses, an Perkin Elmer STA 6000® equipment was used. It allows to perform a simultaneous
thermal analysis and to return data of a series of phenomena that take place during the heating of material until its
decomposition.
Thermogravimetric analysis is a method of thermal analysis in which changes in physical and chemical properties
of materials are measured as a function of increasing temperature and as a function of time. The STA 6000 machine
was also used for this analysis.

3.3.2. Injection moulding

Tensile specimens were manufactured by injection moulding from mixtures obtained in the extrusion process -
Table 2. A micro injection machine Boy® 22A and a standard two-cavity mould were used. The Boy® 22A
injection machine is a machine designed for the automatic processing of thermoplastic materials, elastomers,
silicones among other thermoplastic materials. This machine has 220KN of maximum closing force. The screw used
in the injections was 18mm in diameter. The mould used was a standard structure of Bru & Rubio, having
dimensions 196mmX156mm and two halves, composed of: injection plate, cavity plate, bushing plate, wedges,
extraction plates and extraction tightening plate. The cavity of the mould was then machined to obtain 2 test
specimens, as per EN ISO 527-4.
J.F. Horta et al. / Procedia Manufacturing 12 (2017) 221 – 229 225

Table 2. Mixtures Injected for Material Characterization

Reused Sawdust % Compatible Fusabond


% Reused HDPE
Percentage Granulometry E365

11,25% 300 to 500µm 78,75% 10%


11,25% 500 to 700µm 78,75% 10%
22,50% 300 to 500µm 67,50% 10%
22,50% 500 to 700µm 67,50% 10%
45% 300 to 500µm 45% 10%
45% 500 to 700µm 45% 10%

3.3.3. Tensile Tests

An Instron® model 4505 universal test machine was used for tensile tests. The EN ISO 527 standard, that
specifies the general principles to determine the traction properties of plastics and plastic composites through several
conditions, was employed. Specimens used in the tests are of the Type 1B.

4. Results and Discussion

4.1. Sawdust drying

The container used for the drying test had dimensions of 214.5mm in diameter and height of 114mm,
corresponding to a volume of approximately 4,12dm3. At the start of the process the mass of the container was
measured by using a precision scale. A mass of 1517g was obtained. Then, 500g of pine sawdust were placed inside
the container, totalizing a mass of 2017g.The container was then placed in the furnace at 80ºC. Every 2 hours, the
container was removed, and its mass measured, to verify the loss of mass (Table 3) that would ultimately give the
moisture content of the sawdust.
After 16 hours in the furnace, it was observed that the mass of the material stagnated. This means that most the
existing moisture had evaporated. This observation was confirmed after 18 hours. The moisture content of the pine
sawdust was found to be 34.6%.

Table 3. Measurements of mass loss in drying Process

Material Drying - Pine Sawdust

Hours Total Mass(gr) Pine Mass(gr) % Pine Mass % Evaporated Mass


0 2017 500 100 0
2 1970 453 90,6 9,4
4 1937 420 84 16
6 1910 393 78,6 21,4
8 1880 363 72,6 27,4
10 1859 342 68,4 31,6
12 1850 333 66,6 33,4
14 1845 328 65,6 34,4
16 1844 327 65,4 34,6
18 1844 327 65,4 34,6

4.2. Sawdust Granulometry

Initially, and to verify the best sieve to start the granulometry process, 100g of material were filtered
through a 1mm aperture sieve. From those, 95.34g passed through, leaving only a few residues in the upper part of
226 J.F. Horta et al. / Procedia Manufacturing 12 (2017) 221 – 229

the sieve. Testing proceeded until WKH ȝP VLHYH UHVXOWHG LQ PDVV of selected particles of 80.4g, leaving little
PDWHULDOLQWKHXSSHUSDUWRIWKHVLHYH6RLWZDVGHFLGHGWRVWDUWZLWKWKHȝPDSHUWXUHVLHYHDQGSURFHHGGRZQ
WRDVLHYHRIȝPDSHUWXUHVL]HZKLFKZDVIRXQGWROHDYHRXWDERXWJSHUJRILQSXWPDWHULDOAfter the
measurements, it was verified that in the ȝPVLHYHallowed more than 80% of the material to pass, the ȝP
sieve allowed more than 50% of the material, DQGDWȝP sieve allowed less than 20%. This was the reason why
the reference intervals, 300ȝP WR ȝP DQG 500ȝP to 700ȝP were chosen. Table 4 shows the results for
granulometry of the sawdust.

Table 4. Material that passes on the sieves in 100grams

Sieve Material in 100grams


1mm 95,3gr
700µm 80,4gr
500µm 53,36gr
300µm 17,39gr

4.3. Definition of processing temperatures

For the extrusion process, it was necessary to check the temperature values allowed by the pine sawdust. For this
purpose, analyses were carried out by the STA process, to verify the degradation temperature of the sawdust. Fig. 2
shows the STA analysis for 500ȝP to 700ȝP granulometry. The Trigger X point on the plot indicates the beginning
of degradation, corresponding to a temperature of 277.59°C. The temperature of 320.44°C represents the point
where degradation is at 50%. The melting temperature for the HDPE matrix, defined as the processing temperature
in the extrusion spindle, was 198ºC, well below those values.

Fig. 2. Graph of STA analysis done to the 500 to 700 ȝP Sawdust


J.F. Horta et al. / Procedia Manufacturing 12 (2017) 221 – 229 227

4.4. Analysis of homogeneity of Mixtures

To verify the homogeneity and consistency of the composite materials, thermogravimetric analyses were
performed on all mixtures. In this test, a small amount of material is subjected to a temperature increase between 0
and 500ºC, until total loss of mass occurs. The variation of mass is then plot against temperature. The initial mass
loss corresponds to residual water in the material. The second stage mass loss refers to the pine sawdust degradation,
and the third and final step refers to the degradation of the polymer. Three analyses were performed for each one of
the mixtures processed in the extruder. Fig. 3 shows the thermogravimetric results for the three mixtures, and
compares the mass percentage values with the theoretical values.
From the analysis of the plot, it is possible to state that the differences in water, sawdust and HDPE content
observed between theoretical and real mixtures increase as the percentage of sawdust increases. Moreover, there
seems to be no significant differences when comparing different granulometries. Water content increases with
increasing sawdust mass percentage, which is expected due to the tendency of this material to absorb water. The
influence of the compatibilizer (Fusabond®) is included on the polymer degradation stage.

TGA results comparison

Expected Water Residual Water Expected Sawdust Real Sawdust Expected Polymer(Reused HDPE+Fusabond E265) Real Polymer

100
88,75 88,75
90
77,5 77,5
80
68,19
70 63,67
61,08
57,27
55 55
% in mixture

60 52,84
51,46
50 45 45

40
26,96 25,92
30 22,5 22,5
21,6
17,75 15,85
20
11,25 11,25
11,17
10 3,08 4,33 2,59 3,07
0 1,1 0 0 0 1,77 0 0
0
0%/11,25%/88,75% 300 to 500um 0%/22,5%/77,5% 300 to 500um 0%/45%/55% 300 to 500um 0%/11,25%/88,75% 500 to 700um 0%/22,5%/77,5% 500 to 700um 0%/45%/55% 500 to 700um

Fig. 1. TGA analyses performed in all mixtures. Comparison with theoretical values of components mass percentage.

4.5. Mechanical Properties

Fig. 4 presents tensile test results for all materials studied. As particle mass increases, maximum strain decreases
and elastic modulus increases. Ultimate tensile strength becomes higher for all composite materials, when compared
to HDPE only. These results are in agreement with the classical particle-reinforced composite theory[18].
Nevertheless, for the polymeric material (HDPE) sample, while maximum stress is lower than the composite
materials, maximum strain is also lower, which is an unexpected result. For 11.25% and 22.5% samples, the
maximum strain is higher than HDPE. Lower strain can only be observed for 45% sawdust. Granulometry seems to
have little effect on the above observations. Still, for 11.25% and 22.5% sawdust, larger granulometry displays
higher strength. For 45% sawdust, differences are almost non-existent.
Strain results for HDPE are lower than some of the composite materials. Some works report a high dependence of
HDPE properties on processing route. Kalay et al [19] report a clear difference in several properties of HDPE when
using shear controlled orientation (SCORIM) injection moulding over conventional injection moulding. In the latter,
maximum strain (at peak stress) was 0.031, which is in accordance to the current results. However, maximum strain
228 J.F. Horta et al. / Procedia Manufacturing 12 (2017) 221 – 229

at break is much higher (1.554). Using SCORIM, maximum strain (at peak stress) more than doubled, but the
material showed little additional plastic strain. Other authors don't indicate strain while comparing results of virgin
materials and recycled/reused materials. Adhikary et al [20] mixed HDPE and different percentages of wood. They
do not give information about strain for the 100% recycled/reused HDPE and for the virgin HDPE. The above
observations seem to indicate that not only the composition of the HDPE / sawdust mixture is relevant to take into
account, but also the processing route.

Average Values of 10 Tested Samples


25

20
Stress(MPa)

15

10

0
0 0,01 0,02 0,03 0,04 0,05 0,06 0,07 0,08 0,09 0,1

Strain

11,25%Sawdust 300to500um 11,25%Sawdust 500to700um 22,5%Sawdust 300to500um


22,5%Sawdust 500to700um 45%Sawdust 300to500um 45%Sawdust 500to700um
Reused HDPE

Fig. 2. Tensile test average results for 10 samples. Granulometries of 300Pm – 500Pm and 500Pm - 700Pm. Sawdust percentages of 11,25%,
22,5% and 45%.

5. Conclusions

The present work was carried out to investigate composite material properties developed from reused HDPE
thermoplastic material from the thermoplastics injection industry and pine sawdust from the lumber industry.
Sawdust was previously dried and filtered to obtain specific particle sizes. Processing temperatures were accessed
by thermal analysis, allowing to carry out extrusion and injection moulding without degradation of any of the
materials in mixtures. Sawdust was added to HDPE in a dual screw extruder, along with a compatibilizing agent. It
was possible to observe that the materials obtained follow the expected trends in mechanical response of particle
reinforced composites, but the base polymeric material displayed low plastic strain, which was unexpected, even for
a re-used thermoplastic material. This may be due to processing conditions. Nevertheless, adding sawdust to the
base recycled HDPE together with a compatibilizing agent has shown to improve mechanical response especially in
terms of modulus and, in minor extent, to maximum stress.
Processing conditions, especially the injection moulding process, are of great importance for accessing the
potential of these materials to be a competitive advantage for industries, and should be further studied.

Acknowledgements

This research work was supported by the Portuguese Foundation for Science and Technology (FCT) through the
Project reference UID/Multi/04044/2013.
J.F. Horta et al. / Procedia Manufacturing 12 (2017) 221 – 229 229

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