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WOOD PLASTICS COMPOSITES PRODUCED BY ROTOMOLDING

Alexandre Raymond, Denis Rodrigue


Université Laval, Department of Chemical Engineering, Quebec City, Quebec, Canada, G1V 0A6.

Abstract
Materials
This study reports on the properties of wood plastic
composites produced by rotomolding. As a special case, Linear low density polyethylene (LLDPE),
wood flour (maple) was dry-blended with linear low- EXXONMOBIL LL 8460, having a melt flow index of 3.3
density polyethylene (LLDPE) to produce composites up g/10 min (2.16 kg, 190oC) and a density of 938 kg/m3, was
to 25%wt. From the samples produced, a complete supplied by ExxonMobil Chemical Canada. Maple wood
characterization was performed including density, flour was purchased from PWI Industries (St-Hyacinthe,
morphology, and mechanical properties (tensile and Quebec, Canada). The material received was only sieved
flexural). As expected, tensile and flexural moduli (no surface treatment) to keep particles between 125 and
increased with wood content, while tensile strength and 250 microns which correspond to the average particle size
elongation at break decreased. The optimum wood content of the LLDPE powder. Similar particle size will limit
was found to be around 20%wt. for the range of conditions powder segregation in the dry-blending step of the process
tested. as presented next.

Introduction Experimental
In the last few years, several developments have been Sample Production
done in the production of wood plastic composites (WPC) First, the wood flour and LLDPE powder were dry-
for applications in automotive, building and construction, blended using an anchor-type mixer for 3 to 4 minutes. To
packaging and furniture [1,2]. As generally known, WPC simplify the process, the wood flour was not dried before
have several advantages over inorganic reinforced processing as most of the volatiles inside the wood
composites like glass fibres in terms of reduced weight, particles are believed to be removed in the first minutes of
cost and processing conditions. They also have good the rotational molding cycle as shown in a previous study
aesthetic properties (wood-like) without having the [5].
limitations of wood products (water absorption, mold The samples were produced by rotomolding at WES
degradation, etc.). WPC also have a favorable incentive Industries (Princeville, Quebec, Canada) using a
related to their “bio” or “green” origin making them a conventional shuttle-type rotomolding machine with two-
logical choice of materials in terms of life cycle analysis arms. The mold used was made of aluminum and has the
due to good recyclability and degradability. shape of a two-level rectangular box having total
dimensions of 35 x 21 x 12 cm3. The optimum conditions
Most of the time, standard processing techniques like were found to be: a 4:1 speed ratio, heating for 21 minutes
extrusion, injection and compression molding are used to with an oven (natural gas heated) at a temperature of 270oC
produce WPC. Unfortunately, very few works have been and a cooling period of 24 minutes with forced air
published on the production of these materials using (blowing fans) during summer time (May-August 2012). A
rotomolding, but this work represents a second step demolding agent was applied to prevent the parts from
towards our understanding of this process based on a adhering to the inside of the mold. Finally, to minimize
previous study on the subject [3]. A recent review of the shrinkage and warpage, the parts were air-blown from the
published literature can be found elsewhere [4]. inside after being removed from the mold. To perform all
the characterization, samples were cut directly inside the
So the main objective of this study is to show that molded parts.
polyethylene parts reinforced with natural fibers can be
easily produced by rotomolding. As a special case, linear Density
low density polyethylene will be reinforced by wood Density of LLDPE powder, maple flour and molded
(maple) flour. In particular, mixing all the component will composites was determined using an Ultrapyc 1200e
be performed using the simple dry-blending technique (Quantachrome Instruments, USA) gas (nitrogen)
described in our previous work [3,4]. The effect of wood pycnometer. The results are the average and standard
content between 0 and 25%wt. is reported in terms of deviation of a minimum of 5 samples.
density, morphology and mechanical properties (tensile
and flexural) of the final parts.
Morphology
Images of the rotomolded parts were taken by a HDR-
SR12 Sony Handycam to get an overall view, while
micrographs of the cross-section were obtained by a JEOL
JSM-840a scanning electron microscope (SEM). The
samples were first broken in liquid nitrogen to expose the
surface which was covered by a conductive layer (Au/Pd).
Micrographs of the raw materials were also taken to
compare particle size, geometry and surface state.

Tensile Properties
Young’s modulus, tensile strength and elongation at
break were determined using a model 5565 (Instron, USA)
universal tester with a 500 N load cell. Type V dog bone
samples were cut from the molded parts according to
ASTM D638. The tests were performed at room Figure 1. Micrographs of the wood flour (left) and LLDPE
temperature and the travel speed was set at 10 mm/min. A powder (right) at different magnifications.
minimum of five samples were tested to report on the
average and standard deviation. Figure 2 presents typical pictures of the composites
produced. In general, the images show that good part
Flexural Properties quality (smooth, uniform and homogeneous surfaces) was
Flexural modulus was determined with a model 5565 obtained up to 20%wt. wood. Above this value, there is a
(Instron, USA) universal tester in the three-point bending lack of polymer to cover all the wood particles present and
geometry (ASTM D790) using a 50 N load cell. Five surface defects can be seen in relation with the simple dry-
samples having cross-sections of about 14 x 5 mm2 were blending technique used. This is more clearly seen at
tested. The span (distance between supports) was set at 100 25%wt. wood where the corners of the part show some
mm to limit internal shear in the samples and the travel discoloration and surface porosity associated with low
speed was set at 10 mm/min. polymer content.
To explain the density results reported in Table 1,
Figure 3 presents typical SEM of the cross-sections under
Results and Discussion
different magnifications. Although high amounts of holes
can be seen in some micrographs, especially at low wood
Density
content (0-15%), not all of them can be related to porosity.
As expected, Table 1 shows that density of the
Actually, some of the holes observed on these micrographs
composites increases with wood content because the wood
are the results of fibre pull-out related to sample
flour has a higher density (1408±8 kg/m3) than the LLDPE
preparation for SEM observation. Nevertheless, there are
matrix (938 kg/m3). But some of the samples, especially at
more holes at lower wood concentration which explains the
low wood contents (5-10%), have densities lower than the
density results observed in Table 1 (higher porosity).
neat matrix. This indicates that porosity in the composite
Nevertheless, micrographs taken at higher magnification
was formed and not completely eliminated. Based on the
show that good adhesion seems to occur between the wood
theoretical density of each component, an estimation of
particles and the polyethylene matrix in our case; i.e. no
porosity can be made and the results are presented in Table
clear void or space can be seen at the interface. This
1. The effect of porosity on part’s properties is discussed
indicates that wettability conditions (processing time, melt
next.
viscosity and surface tension) are good for the polymer
melt to enclose the wood particles. But as wood content
Morphology
increases, there is a clear segregation across thickness that
First, Figure 1 presents typical micrographs of the raw
is driven by the density difference between polyethylene
materials. It is clear that the wood flour has a more
and wood particles and accelerated by the biaxial rotation
elongated shape (fibre-like) compared to the more cubic
of the mold since most of the wood particles are
(particle-shape) polyethylene. It is expected that
accumulating near the inside of the part as seen at 25%wt.
differences in geometry will have an effect on particle
wood with 10X magnification. All these morphological
stacking inside the rotating mold which might improve or
parameters will have an effect on the mechanical properties
not the mixing between both components depending on the
of the rotomolded parts as described next.
time before the polymer start sticking to the mold walls
[6].
Tensile Properties
Tensile modulus (E), tensile strength (σy) and
elongation at break (εb) values for the rotomolded samples
are presented in Table 1. First, Young’s modulus was
found to decrease at low wood content (5%wt.), then
increase to a maximum value around 20%wt. wood. This
behavior can be explained by a competition between
porosity present at low wood content which tends to
decrease the mechanical properties (presence of defects),
and the reinforcing effect of wood particle addition. At
higher wood content (25%wt.), there is probably not
enough polymer matrix to recover all the wood particles as
discussed earlier (see Figure 2) and lower modulus is
observed as possible particle-particle contact can produce
local defects inside the composite.
For tensile strength, the values are decreasing slightly
with wood content. This is expected as the adhesion
between the hydrophilic wood is not good with the
hydrophobic polyolefin matrix [7]. Nevertheless, the
decrease is mostly noticeable (more than 25% reduction)
for wood contents of 20%wt. and higher.
Finally, the elongations at break were found to
decrease substantially with wood content. As expected in a
wood polymer composite [7], the elongations at break
varied between 83 and 25%, compared to 748% for the
neat polymer matrix. This indicates that the composites
may not be able to sustain high deformation and will
probably be very brittle, especially at high deformation
rates like impact tests. Nevertheless, the properties can
probably be improved by adding impact modifiers in the
initial blend and work is already being done in this
direction.

Table 1: Density and tensile properties of the samples.

Wood Tensile properties


Density Porosity
content
(kg/m3) (%) E σy εb
(%wt.)
(MPa) (MPa) (%)
0 932 0.6 202 16.0 748
5 908 5.6 186 13.4 83
10 926 6.0 202 12.9 57
15 963 4.5 229 12.7 41
20 992 3.9 237 11.8 29
25 1014 3.9 203 9.2 25

Figure 2. Typical images of the rotomolded samples


produced. The left column presents the overall surface of
the part, while the right column presents magnifications to
show the quality of the corners. Each line represents 0, 5,
10, 15, 20 and 25%wt. wood content, respectively.
increased the flexural modulus by 35% (from 612 to 827
MPa), while the tensile modulus only increased by 17%
(from 202 to 237 MPa). Also, adding more wood leads to
lower moduli (tensile and flexural) due to a lack of
polymer matrix to recover all the wood particles thus
creating local defects inside the composites. Nevertheless,
the optimum wood content here (20%wt.) is higher than
the one obtained in our previous studies (10-15%wt.) using
different wood species (agave or pine) and polymer matrix
(linear medium density polyethylene, LMDPE) [3,4]. This
indicates that further optimization can be made for a
specific combination of polymer-reinforcement and more
work is already being done on the subject. There is also the
possibility of improving the mechanical properties by a
surface treatment of the wood particles to increase
adhesion with the polymer matrix like any hydrophilic
natural fibre inside a hydrophobic polymer [8], and/or a
careful control of the wood particle size distribution to
produce hybrid of self-hybrid materials [3,9].

Table 2: Flexural modulus of the rotomolded samples.


Wood Flexion
content Modulus
(%wt.) (MPa)
0 612
5 620
10 692
15 784
20 827
25 794

Conclusions
Based on the results of this work, it is clear that wood
plastic composites (WPC) can be produced by rotomolding
using linear low density polyethylene and wood (maple)
flour. It was also shown that simple dry-blending of the
material in a powder form is an economic and technical
alternative to standard melt blending (compounding in a
twin-screw extruder) to introduce wood particles in a
polymer matrix.
The main parameter studied was wood content
between 0 and 25%wt. for wood particle size between 125
and 250 microns.
From the materials produced, a complete
Figure 3. Typical images of the cross-section of the characterization in terms of density, morphology and
rotomolded samples produced. Each line represents 0, 5, mechanical properties in tension and flexion was
10, 15, 20 and 25%wt. wood content, respectively. performed. From the results obtained, the following
conclusions can be drawn:
Flexural Properties
The results of flexural modulus are presented in Table • Tensile modulus increased by up to 17%, while
2. In this case, it is clear that porosity and defects inside the flexural modulus increased by up to 35% with
molded parts is not as important as in the case of tensile increasing wood flour content,
modulus since the modulus increases monotonically with • Increasing the wood flour content decreased both
wood content up to 20%wt. Furthermore, the increases are tensile strength and tensile elongation at break,
more important here. For example, adding 20%wt. wood
• The optimum wood content was around 20%wt.
for the conditions tested.

Although the mechanical properties are not as high as


expected, for some applications where mechanical strength
is not a priority, good samples can be produced, especially
for more aesthetics applications because of their natural
(green) or wood-like texture/appearance.

Acknowledgements
Financial support from the National Science and
Engineering Research Council of Canada (NSERC) was
appreciated. Technical support from the Research Centre
on Advanced Materials (CERMA) was also highly useful.
LLDPE samples from ExxonMobil Chemical Canada (Ron
Cooke) are highly appreciated. Finally, WES industries
inc. is highly thanked for the time allowed to perform the
experimental work related to the preparation and the
molding of the rotomolded samples.

References
1. K. Oksman, M. Sain, Wood-polymers composites,
CRC Press, Boca Raton, 366 p. (2008).
2. A.A. Klyosov, Wood-plastic composites, Wiley-
Interscience, Hoboken, 698 p. (2007).
3. N. Ward-Perron, D. Rodrigue, Proc. of SPE ANTEC,
paper 00467 (2012).
4. R.H. López-Bañuelos, F.J. Moscoso, P. Ortega-Gudiño,
E. Mendizabal, D. Rodrigue, R. González-Núñez,
Polym. Eng. Sci. 52, 2489 (2012).
5. N. Ward-Perron, D. Rodrigue, Proc. of SPE ANTEC,
paper 00443 (2012).
6. A. Aït Aissa, C. Duchesne, D. Rodrigue, Polym. Eng.
Sci., 52, 953 (2012).
7. A. Mechraoui, B. Riedl, D. Rodrigue, Compos. Interf.,
14, 837 (2007).
8. O. Faruk, A.K. Bledzki, H.P. Fink, M. Sain, Prog.
Polym. Sci., 37, 1552 (2012).
9. A. Ramezani Kakroodi, S. Leduc, D. Rodrigue, J. Appl.
Polym. Sci., 124, 2494 (2012).

Key Words: Maple flour, LLDPE, composite, rotomolding.

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