10.2417/spepro.

005393

Characterization of glass
fiber-reinforced high-density
polyethylene
Usman Saeed, Kashif Hussain, and Ghaus Rizvi

Glass fiber-reinforced high-density polyethylene composite increases

in strength as the fiber orientation increases in anisotropy, which could
lead to stronger composite materials.

For thermosetting composites, it has been standard practice to use var-

ious coupling agents to strengthen the adhesion between fibers and
matrix.1, 2 However, the known coupling agents for glass fibers typi-
cally do not work well with common thermoplastic polymers, so they
do not increase the chemical compatibility between the fibers and the
matrix. This is a major concern when manufacturing thermoplastic
composites.3 Glass fibers have been used for decades to improve the
mechanical, thermal, and insulation properties of polymers, especially
within high-density polyethylene (HDPE) for structural and automo-
tive applications.4 These property improvements are highly dependent
on the orientation and distribution of the glass fiber. Thus, it is desirable
to be able to predict not only the rheological behavior of the composite
melt but also how processing will orient the fibers.
Figure 1. Complex viscosities of neat high density polyethylene
We compounded HDPE polyethylene resin (melt flow index of
(HDPE) and composites at investigated temperatures (a), and (b) com-
17g/10min) with glass fibers using a twin screw extruder (TSE). We
plex viscosities of composites with 9% glass fiber, with and without
added Fusabond M603 (random ethylene copolymer) and Eastman
Fusabond M603 (FB) and Eastman G-3003 (G-3003). GF: glass fiber.
G-3003 (maleic anhydride grafted polypropylene) as coupling agents
Pa-S: Pascal-seconds.
(see Table 1). The compounded pellets were dried in an oven at
80◦C for 12 hours and were compression molded into a dog-bone
hinder the chain mobility and thus gradually increase  . The com-
shape corresponding to ASTM D638. The section of composite sample
posite samples had higher  than the virgin polymer: see Figure 1(a).
was scanned using high-resolution desktop x-ray microtomography in
The incorporation of fibers in polymer systems generally increased the
order to determine the fiber orientation. We used a torsional rheometer
value of  , which increased continuously with fiber loading and de-
to characterize the viscosity.
creased with higher temperatures. Due to fiber loading, the viscosity is
The complex viscosities of composites at the investigated temper-
expected to increase rapidly as the filler packs move closely together
atures are presented in Figure 1(a). We found that complex viscosity
and collisions between fibers increase. We found the increase in  to
( ) increased with an increase in fiber loading and decreased with an
be predominant at lower frequency as the fiber and polymer molecules
increase in temperature and frequency. This was due to the strong shear
were not completely oriented during the dynamic frequency test. The
thinning behavior of the HDPE in a molten state. In the HDPE/glass
addition of a fiber to a polymer system perturbs the normal flow of
fiber formulations, a greater amount of glass fiber loading will cause
either greater entanglement of the chains, or the solid glass fiber will Continued on next page
 10.2417/spepro.005393 Page 2/3

the polymer and hinders the mobility of chain segments in the flow.
As the fiber loading increases, the phenomenon becomes more pre-
dominant, and the viscosity further increases. The formulations having
9% glass fiber with G3003 have a higher  compared with formu-
lations with Fusabond as well as formulations without any additives:
see Figure 1(b). The observed behavior is due to the formation of a
strong network structure, which causes greater resistance under dy-
namic flow because the rheological behavior is sensitive to the molecu-
lar structure. Similar effects have been observed with 1% and 5% glass
fiber composites.
Shear rate varies from the center of the plate to the outer edge in a
torsional rheometer with parallel plates, resulting in an inhomogeneous
shear field. An inhomogeneous shear field could lead to increased fiber-
fiber interaction. These interactions are higher when the rheometer gap
is small compared to the characteristic length of the filler. If the gap
height is >2Lw (double the height of the weighted average length of
the fibers), then the rheological data is reproducible within a relative
error of ˙5% (see Figure 2). In our study here, the gap height was
1mm, double the weighted average length of 0.407mm.5
The sectioned sample for the x-ray microtomography scanner is
shown in Figure 3a. Due to a rather large density difference be-
tween the fibers and the polymer matrix, individual fibers are clearly
visible in the x-ray microtomography image and can be segmented
three-dimensionally: see Figure 3(b).
Figure 3. (a) A schematic illustration of the compression molded plate
Figure 4 illustrates the glass fiber concentrations in relation to the
and the position of the sample collected for the x-ray microtomogra-
tensor components aij . The a33 component corresponds to the machine
phy experiments, and (b) a three-dimensional and top view of 1% glass
direction (the flow or z-direction) while a11 and a22 are associated with
fiber, 5% glass fiber, and 9% glass fiber composites. ND, TD, MD: Nor-
the transverse and normal directions. In the figure, we see that the a33
mal, transverse and machine flow directions.
component of the tensor is higher compared to the a11 and a22 compo-
nents. This may have been due to higher viscosity and higher stresses
during compression molding that led the fibers to orient in the machin-
ing direction as the fiber content increased. The a11 and a22 compo-
nents of the fiber increased as the concentrations of fiber decreased.
We used the eigenvalues obtained using a 2nd order tensor equation
(see Equation 1) to calculate the degree of anisotropy (DA).6, 7 Isotropy
is a measure of 3D symmetry or the presence or absence of preferential
alignment of structures along a particular directional axis.
 
.Eigenvaluemin /
DA D 1 (1)
.Eigenvaluemax /
Here DA is 0 for total isotropy and 1 for total anisotropy. The degree of
anisotropy was lower in 1% glass fiber as compared to 9% glass fiber
(see Figure 5). We deduced that in 9% glass fiber composite, a higher
degree of fiber alignment along the principal direction (the flow direc-
tion or z-axis, a33 / is achieved, compared to the lower values found in
the 1% glass fiber composite, indicating a higher scatter of fiber orien-
Figure 2. Complex viscosities of 9% glass fiber composites, with
tations.
experimental error.
Continued on next page
 10.2417/spepro.005393 Page 3/3

Table 1. Selected composition of composites.

Neat HDPE
HDPE C 1%glass fiber HDPE C 1%glass fiber C 3% FB HDPE C 1%glass fiber C 3%G3003
HDPE C 5%glass fiber HDPE C 5%glass fiber C 3%FB HDPE C 5%glass fiber C 3%G3003
HDPE C 9%glass fiber HDPE C 9%glass fiber C 3%FB HDPE C 9%glass fiber C 3%G3003

We found that overall, the viscosity of composites with the addi-

tion of G3003 as a coupling agent increased in comparison to the vis-
cosity of composites using Fusabond. The complex viscosity ( ) was
strongly affected by temperature and fiber loading. The orientation of
the fiber was strongly dependent on the amount of fiber loading, which
in turn influenced the likelihood of anisotropy in composites. In the fu-
ture, we would like to improve the composites’ degree of anisotropy,
and we will measure the orientation-based thermomechanical proper-
ties of the glass fiber composites.

Author Information

Usman Saeed
University of Ontario & Institute Of Technology
Oshawa, Canada

Figure 4. Effect of fiber concentration on orientation. aij : Tensor com- Kashif Hussain and Ghaus Rizvi
ponents, where a11 corresponds to the transverse, a22 to the normal Department of Automotive, Mechanical, and
and a33 to the machine directions. Manufacturing Engineering
University of Ontario Institute of Technology
North Oshawa, Canada

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Figure 5. Effect of fiber concentration on degree of anisotropy.

c 2014 Society of Plastics Engineers (SPE)