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Composites: Part A
journal homepage: www.elsevier.com/locate/compositesa
Effects of processing method and fiber size on the structure and properties
of wood–plastic composites
Sebastien Migneault a, Ahmed Koubaa b,*, Fouad Erchiqui b, Abdelkader Chaala c,
Karl Englund d, Michael P. Wolcott d
a
Centre de recherche sur le bois, Université Laval, Que., Canada G1V 0A6
b
Chaire de recherche du Canada en valorisation, caractérisation et transformation du bois, Université du Québec en Abitibi-Témiscamingue, 445 boul. de l’Université,
Rouyn-Noranda, Que., Canada J9X 5E4
c
Service de recherche et d’expertise en transformation des produits forestiers, 25 rue Armand-Sinclair, Amqui Que., Canada G5J 1K3
d
Wood Materials and Engineering Laboratory, Washington State University, Pullman, WA 99164-1806, USA
a r t i c l e i n f o a b s t r a c t
Article history: The aim of this study was to understand the roles of processing method and fiber size on the properties of
Received 22 June 2008 wood–plastic composites (WPC). Composites were manufactured using extrusion or injection molding
Received in revised form 9 October 2008 (IM) and fibers of different fiber length-to-diameter (L/D) ratio. IM resulted in better mechanical proper-
Accepted 13 October 2008
ties and lower water absorption and swelling than extrusion. These differences can be explained by the
structure and surface quality of the composites. Fiber L/D ratio had a beneficial effect on mechanical
properties but resulted in decreased water absorption characteristics. These results allow identifying a
Keywords:
suitable forming process and/or fiber size according to application needs. This study provides a better
A. Fibers
A. Wood
understanding of the relationships between processing method, fiber characteristics, and composite
E. Extrusion behavior.
E. Injection molding Ó 2008 Elsevier Ltd. All rights reserved.
1. Introduction tural parameters such as orientation and boundary layers are less
distinct.
The ability of thermoplastics to melt and re-harden has been In wood–plastic composites (WPC), Stark et al. [5] compared IM
exploited in many different processing methods. The most com- and extruded samples made with 50% by weight of ponderosa pine
monly used methods to produce plastics and wood-fiber filled flour and high-density polyethylene (HDPE) matrix. The flexural
plastic parts are extrusion and injection molding (IM) [1–3]. The modulus of elasticity (MOE) of composites using both processes
extrusion process produces continuous linear profiles by forcing was similar. However, IM resulted in higher modulus of rupture
a melted thermoplastic through a die. The IM process produces (MOR) than extrusion. The authors suggest that the higher density
three-dimensional items with minimal post-manufacturing stages. of IM samples resulted in more intimate contact between the HDPE
Although different, both processes follow the same basic steps: matrix and wood flour, and consequently higher mechanical proper-
melting, shaping, and cooling [4]. Both processes also use screws ties. Improved interfacial contact resulted in more efficient stress
to convey, pump, and blend the heterogeneous components [2]. transfer between matrix and wood particles, resulting in increased
Michaeli and Menges [4] compared extrusion and IM using de- strength. Stark et al. 2004 [5] observed that IM sample surfaces were
fined process parameters such as residence time, temperature, polymer-rich, whereas wood fibers were apparent at extruded sam-
pressure, shear rate, shear stress, and cooling rate. Regardless of ple surfaces. In a further study, Stark [1] observed polymer flow over
the processing data used, pressure and shearing in IM are signifi- wood particles at the surface of IM composites, whereas polymer
cantly higher than in extrusion. Conditions that vary with process- failed to encapsulate wood particles on many areas of the surface
ing method result in different final plastic product properties. of extruded composites. Bledzki and Faruk [6] also compared IM
Other investigators [4] found highly oriented layers in IM inorganic and extruded WPC made with 30% by weight of hardwood particles
short fiber-reinforced thermoplastics. When forming, these layers with a polyethylene matrix. IM produced higher specific tensile
align fibers with a specific orientation: in outer layers, fibers are strength, but specific bending MOEs were similar. In this study, how-
oriented in the main flow direction, while in the core layer they ever, composite density was similar for both processes.
are oriented perpendicular to flow. With extrusion, however, struc- Clemons and Ibach [7] compared sorption behavior in compos-
ites made with 50% by weight of 40-mesh pine flour and HDPE
* Corresponding author. Tel.: +1 819 762 0971; fax: +1 819 797 4727.
manufactured by extrusion and IM. Water-soaked extruded sam-
E-mail address: ahmed.koubaa@uqat.ca (A. Koubaa). ples absorbed more water and swelled more than IM samples.
1359-835X/$ - see front matter Ó 2008 Elsevier Ltd. All rights reserved.
doi:10.1016/j.compositesa.2008.10.004
S. Migneault et al. / Composites: Part A 40 (2009) 80–85 81
The opposite trend was expected, because the IM composite had Duncan multiple comparison tests (5% significance level) were
higher density. For conventional wood-based composites, higher conducted using Statistical Analysis System (SAS).
density generally yields greater swelling. The authors attributed Processing conditions are presented in Table 1. All composites
this result to the polymer-rich surface layer and lower void content were prepared in two stages: compounding for pelletizing fol-
of the IM composites. The literature contains no other studies com- lowed by either extrusion or IM. A Cincinnati Milacron 55-mm
paring sorption behavior between IM and extruded WPC. counter-rotating conical twin-screw extruder having a L/D ratio
Fiber L/D ratio and size play important roles in the strength of 22:1 was used to compound the dry CTMP fibers at a proportion
development of non-natural fiber-reinforced polymers [8] and of 40 wt% and HDPE at 60 wt%. The obtained compound was then
wood-fiber-based products such as paper and fiberboard [9]. Com- air cooled and ground with a Nelmor rotary knife grinder equipped
mercial WPC are generally produced from wood flour particles with a screen having 9.6-mm diameter openings to form WPC pel-
with a low L/D ratio. Although these small-sized particles integrate lets. The die was removed in a first step to reduce pressure, shear
well into the processing equipment, low L/D ratios cause stress stress, and residence time of the wood fibers in the extruder, and
concentrations leading to decreased strength compared to neat consequently to reduce fiber degradation. Temperature and RPM
polymer [10,11]. Few reports have shown that using long fibers in- speed were adjusted according to fiber length to obtain a homog-
creases the mechanical strength of WPC when formed with IM enous extrudate with no apparent thermal degradation. The ex-
[12,13]. One study reported beneficial effects of fiber length on truded material was air cooled and ground to form pellets.
mechanical properties using extrusion [14], whereas other studies Composites were formed (final stage) using either extrusion or
have reported limited or no effects [15,16]. Thus, the effect of fiber IM. A Cincinnati Milacron 35 mm conical counter-rotating twin-
size on the strength development of WPC appears to vary with the screw extruder was used to form extruded samples. The length-to-
forming process. No studies are found in the literature on interac- front diameter ratio of the screws was 23:1. The extruder die was
tions between processing method, fiber size, and their effects on 9.53 mm in height by 38.1 mm in width. A vacuum of approximately
the physicomechanical properties of WPC. 300 kPa was used. Low RPM was set to limit fiber breakage. After
The effects of processing parameters and raw material character- exiting the die, the extruded composite material was cooled by
istics on the final material properties of extruded WPC have been water jets. A Sumitomo 55-US ton SE-DU Series injection molding
extensively investigated [10]. However, few studies have compared machine was used to form injection-molded samples. The injection
the characteristics of extruded and injection-molded WPC. Further molding machine had a single screw plasticizing unit and a mold
research is needed to understand the relationships between process- forming one tensile test sample and one bending test sample.
ing method, fiber characteristics, and material behavior. The objec- Composite sample surfaces were analyzed using scanning elec-
tive of this study was therefore to understand how processing tron microscopy (SEM) using an S-3500N variable pressure vac-
method and fiber size affect WPC structure and properties. uum scanning electron microscope (Hitachi) combined with a
Link ISIS Series 300 EDS analytical system (Oxford Instruments).
2. Experimental Physical and mechanical properties of the obtained composites
were measured according to standard procedures: ASTM D 1037-
Three chemi-thermo-mechanical pulp (CTMP) fiber length-to- 99 for moisture tests, ASTM D 2395-93 for specific gravity tests,
diameter ratio (L/D) classes were obtained through mechanical ASTM D 790-03 for three-point bending tests, and ASTM D 638-
refining and characterized with a fiber quality analyzer (FQA) 03 for tensile tests. A span-to-depth ratio of 22 was used for
according to the procedure described in Migneault et al. [14]. Fiber three-point bending. Specimen type number I was used for tensile
characteristics for the different classes are presented in Table 1. tests at a testing speed of 5 mm/min. Unmodified IM samples were
HDPE LB 0100-00 (Equistar) having a melt index of 0.5 g/10 min, used for all tests, and extruded samples were cut to specific size
solid density of 953 kg/m3, tensile strength at break of 27.3 MPa, requirements (machined for mechanical tests and SEM analysis
and flexural modulus of elasticity (MOE) of 1.276 GPa was used and sandpapered for physical tests) according to the procedure de-
as the matrix. Maleated polyethylene (MAPE) AC575A (Honeywell) scribed in Migneault et al. [14]. Six replicates were run for mechan-
was used as the coupling agent and OptiPak OP-100 (Honeywell) ical testing and three replicates were run for physical testing.
was used as lubricant.
Composite formulations were produced according to a factorial 3. Results and discussion
design. Factors were processing method (2 levels, extrusion, and
injection molding) and fiber L/D ratio classes (3 levels, Table 1). 3.1. Composite structure
This experimental design allows an evaluation of the effects of pro-
cessing method and fiber size on the physical and mechanical Electronic micrographs taken at the surface of the WPC sam-
properties of WPC. Analysis of variance (ANOVA) and Waller- ples showed major differences in fiber organization within the
Table 1
Fiber characteristics, WPC formulations, and processing conditions.
composites (Fig. 1). Fibers were clearly aligned in the main flow ical water absorption and volumetric swell curves with immersion
direction at the surface of IM samples (Fig. 1a and b). Frequent sur- time for the two processes are shown in Fig. 2 and Fig. 3, respec-
face defects were observed along with non-oriented long fibers on tively. Water absorption and volumetric swell are on average 13%
the surface of extruded and non-machined WPC samples (Fig. 1c and 42% lower for injected-molded WPC samples than for extruded
and d). Fibers at the surface of extruded and machined WPC sam- samples (averages for the three fiber size classes, Fig. 4). A similar
ples were more randomly oriented (Fig. 1e and f) compared to IM trend between the two processes is found in the literature for
samples. The literature contains reports of oriented fibers at the wood-flour filled thermoplastics [7]. These differences in sorption
surface of injection-molded parts made with short inorganic fi- behavior could be explained by the surface quality of the compos-
ber-reinforced thermoplastics [4]. Micrographs enlarged 450 times ites: exposed fiber ends at the surface of extruded composites may
show smooth, polymer-rich surfaces in IM samples, whereas sur- help water to diffuse from the surface to the core of extruded sam-
face defects (exposed fiber ends and voids) are seen at the ma- ples, whereas the hydrophobic polymer-rich surface of IM compos-
chined surface of extruded samples (Fig. 1). This result concurs ites may prevent water diffusion. Fiber orientation may also have
with a previous report [5]. As shown in Fig. 1, fibers at the surface contributed to the difference in water immersion behavior with
of machined and non-machined extruded samples are twisted, processing method: fibers aligned lengthwise in IM samples could
damaged, and intermeshed, whereas fibers at the surface of IM not diffuse water from the surface to the sample centers, resulting
samples are straight. These structural differences suggest that the in lower volumetric swell in IM than in extruded samples. The
mechanical and physical behavior of WPC differ. presence of hydrophobic lubricant on the surface of IM composites
Adding wood fibers to HDPE slightly increased its density. This could also explain their lower water absorption compared to ex-
was expected, because cell density (about 1500 kg/m3) is much truded composites.
higher than HDPE density (about 950 kg/m3), and this result is in The effect of fiber size on water absorption and volumetric swell
good agreement with previous findings [17]. A significant effect in WPC was highly significant for both processes studied (Table 2).
of L/D on density of extruded composites was found, but no signif- Increasing fiber L/D ratio resulted in increasing water absorption
icant effect of L/D was found on the density of IM composites and volumetric swell (Fig. 2 and Fig. 3), and a similar trend was ob-
(Table 3). served for both processes (no significant interaction, Table 2).
Volumetric swell and water absorption of immersed samples Increasing water absorption with increasing sieved wood flour par-
were significantly influenced by processing method (Table 2). Typ- ticle size has been reported in the literature [17]. Water absorption
Fig. 1. Electronic micrographs at 100 and 450 enlargement of (a and b) aligned fibers and smooth surface on injection-moulded sample, (c and d) surface defect and non-
oriented fibres on extruded sample (original surface), and (e and f) surface defects (exposed fiber ends and voids) on extruded machined sample.
S. Migneault et al. / Composites: Part A 40 (2009) 80–85 83
Table 2
Results of the analysis of variance (ANOVA) for the physical and mechanical properties of WPC.
(L/D = 8.3) (averages for the two processes and all immersion
10
times). Shorter fibers might be coated with thin hydrophobic poly-
Water absorption (%)
Extrusion,
8 L/D = 21.3 mer film. The use of longer fibers may increase the probability of
voids within the composite, which represent water sites, resulting
Injection,
6 L/D = 21.3 in higher water content in the composite after several hours of
Injection,
water immersion. The variation in the adhesion in the fiber/poly-
4 L/D = 13.0 mer interface is among other factors that could explain the impact
Injection, of L/D ratio on water absorption. However, further investigations
2 L/D = 8.3 are needed to verify this hypothesis. Results of the immersion tests
suggest that short fibers and the IM process are more suitable for
0 composites to be used in moist environments.
0 500 1000 1500 2000 2500
Another explanation for the lower volumetric swell of IM sam-
Immersion time (hours) ples is their higher stiffness (Fig. 4), because the energy required
for dimensional change increases with stiffness. However, compos-
Fig. 2. Water absorption with immersion time for extruded and injection-molded
WPC made with HDPE and CTMP fibers of different L/D ratio. ites having longer fibers are stiffer (Fig. 6) and have higher volu-
metric swell (Fig. 3). The difference in composite density could
also influence volumetric swell, although the difference in density
10 is minimal (Table 3). Thus, structural differences, as mentioned
Extrusion,
above, appear to be the dominant factors affecting sorption
Volumetric swell (%)
L/D = 21.3
8 behavior.
Extrusion,
L/D = 13.0
6 Extrusion,
3.2. Mechanical properties
L/D = 8.3
4 Injection, All mechanical properties tested varied significantly with pro-
L/D = 8.3 cessing method and fiber size (Table 2). Typical stress–strain
2 curves in flexure for the two processes with increasing fiber size
are presented in Fig. 5. For the same L/D fiber size, IM composites
0 have higher stiffness, resistance, strain to maximum load, and
0 500 1000 1500 2000 2500
toughness than extruded composites. Compared to extruded com-
Immersion time (hours) posites, IM composites have 17% higher tensile MOE and 31% high-
er flexure MOE (averages for the three fiber size classes, Fig. 4).
Fig. 3. Volumetric swell with immersion time for extruded and injection-molded
WPC made with HDPE and CTMP fibers of different L/D ratio.
Compared to extruded composites, IM composites have 43% higher
tensile MOR and 33% higher flexure MOR, respectively. Toughness,
measured as tensile strain energy, is 170% higher for IM than for
160 extrusion. Toughness is much higher for IM composites because
143 Extrusion
they have higher MOE, MOR, and strain to maximum load (Table
Relative properties
Table 3
Average and standard deviation (between parentheses) of the physical and mechanical properties of WPC made with different processes and CTMP fibers of different L/D ratio.
60
direction. Accordingly, in this study, oriented fibers in IM composites
50 resulted in better mechanical performance than randomly oriented
fibers in extruded composites. SEM micrographs showed surface de-
40 fects on extruded samples, whereas the IM surface was smooth and
Stress (MPa)
3.0
differences in structure and fiber size, as explained above, appear
30
2.5 to be the dominant factors affecting mechanical behavior in this
25 study. Other factors could have influenced the properties of the
formed WPC.
2.0
20 According to the literature, the extrusion process is generally
accompanied by fiber breakage when slender fibers are used
1.5
15 [15,16,18]. It is possible that the compounding and injection-mold-
ing processes resulted in less fiber breakage than the extrusion
1.0 10 process. Moreover, the use of lubricant in IM formulations (Table
HDPE 8.3 13.0 21.3
1) may have reduced shear forces, thereby reducing fiber breakage.
Fiber L/D ratio Further investigation is needed to better understand this phenom-
enon and to accurately assess the effects of the three processes
Fig. 6. Variation in modulus of rupture (MOR) and modulus of elasticity (MOE) with
increasing fiber L/D ratio for extruded and injection-molded WPC and pure HDPE. (compounding, injection, and extrusion) on fiber length.
Previous reports suggest that water absorption increases when
The differences in mechanical behavior with processing method a lubricant additive is used [14] and that mechanical properties are
could be explained in part by the fiber orientation in the composite negatively affected by lubricant additive [14,19]. Thus, differences
structure. According to the classical theory of mechanics, load ap- in physicomechanical properties between the two processes could
plied to a fiber-reinforced composite material is transferred from be greater with the use of lubricant in extruded formulations.
the matrix to the fibers by shear stresses along the fiber–matrix Finally, the processing conditions such as temperature (Table 1),
interface [8,11]. Transfer efficiency increases with increasing fiber residence time, pressure, cooling rate, shear rate, and shear stress
L/D ratio and reaches a maximum when fibers are aligned in the load varied with the processing method and could have affected the
S. Migneault et al. / Composites: Part A 40 (2009) 80–85 85
mechanical properties of the finished fiber-filled thermoplastic Québec (MDEIE), NSERC, Caisse Populaire DesJardins, Tembec and
composites [4]. the UQAT foundation for financial support. Authors are also grate-
ful to Margaret McKyes for the editorial revision of this
3.3. Practical implications manuscript.