Development of recycled polymer composites

for structural applications

A.-M. Hugo1, L. Scelsi*1, A. Hodzic1, F. R. Jones2 and R. Dwyer-Joyce1
This paper is concerned with the formulation of composite materials for structural or semistructural
applications using thermoplastic polymer waste. The mechanical and thermal properties of a
proprietary blend of recycled polymers with a range of different fillers were investigated. The
effect varied with the aspect ratio of the filler and the mode of loading. Spherical calcium
carbonate gave a marginal improvement in modulus. Plate-like mica produced a significant
increase in modulus without reduction in strength. Glass fibres caused a significant increase in
modulus and strength while decreasing the linear coefficient of thermal expansion. Hybrid
systems containing glass fibre and a lower aspect ratio filler were also investigated to obtain a
material system which combines high properties and reasonably low cost. It was found that
addition of small quantities of mica to glass fibre reinforced blends exhibited a significant synergy
in tensile strength and modulus.
Keywords: Recycled, Thermoplastic, Mica, Glass fibre, Polymer blend, Composites

This paper is part of a special issue on Latest developments in research on composite materials

Introduction polymer formulation and production can be challenging

to overcome the natural variability in feedstock.2
In 2005, the annual consumption of plastic materials was Semicrystalline polyolefins have many desirable proper-
nearly 44 million tonnes for Western Europe alone, and it ties for structural applications: good toughness, high
has been rapidly growing.1 Recycling of plastics has fatigue resistance, chemical resistance, non-toxicity in
therefore become a worldwide environmental priority. the environment, high electrical resistivity, low water
The main barriers to plastics recycling are the high cost of absorption, good corrosion resistance, UV stability,
the recycled products relative to their performance and lifetime of up to 50 years and recyclability. Conven-
the difficulty to identify satisfactory markets for these tional building products have higher stiffness, better
materials.2 In the UK, recycling targets for plastics of creep resistance and lower coefficient of thermal ex-
26% for 2008 have been set by legislation.3 Any post-use pansion (CTE). This study investigates the use of fillers
plastic packaging contributes to this target, which has led to improve the properties of a proprietary blend of
to a focus on the most cost effective and easily plastics.
recoverable streams, such as industrial and commercial, The polymer blend examined in this work consists
rather than domestic, packaging. mainly of post-industrial plastic waste. Post-industrial
Traditionally, recovered plastics are separated into waste is the scrap from industrial processes, e.g. yarn
polymer types and used to produce ‘second grade’ bobbins, jerry cans, end of runs, misprinted pots, etc. It
pellets. However, the range of applications for these is usually clean and segregated by type, which presents
pellets is limited due to their reduced properties and to considerably less batch to batch property fluctuations
possible contamination, which prevents their use in food compared to domestic polymer waste. The blend is a
contact applications. An alternative approach, explored proprietary polymer formulation containing both semi-
in this study, consists of upgrading plastic recyclates by crystalline and amorphous thermoplastics in order to
the addition of rigid fillers to improve their structural achieve a good balance between toughness and stiffness.
properties and to make them suitable for long term Although details on blend composition cannot be
(semi)structural applications. disclosed, all the components were commodity polymers
Polymers have many advantages compared to con- typically very abundant in landfills, and the results
ventional materials for structural applications, especially presented in this study are generally relevant for the
if their stiffness and strength can be improved. Using recycling of commingled polymer waste streams.
recycled materials reduces cost significantly; however, Previous studies from Rutgers University4 have shown
that it is possible to achieve polymer blend morphologies
1
with high mechanical properties without the addition of
Department of Mechanical Engineering, The University of Sheffield,
Sheffield S1 3JD, UK compatibilisers through correct blend formulation and
2
Department of Materials Science and Engineering, The University of processing.
Sheffield, Sheffield S1 3JD, UK The effect of filler on the mechanical properties will
*Corresponding author, email [email protected] depend upon its chemical composition, particle shape

ß Institute of Materials, Minerals and Mining 2011

Published by Maney on behalf of the Institute
Received 16 September 2010; accepted 19 September 2010
DOI 10.1179/1743289810Y.0000000008 Plastics, Rubber and Composites 2011 VOL 40 NO 6/7 317
Hugo et al. Recycled polymer composites for structural applications

and size, size distribution, specific surface area, sur- study of mica filled PP based glass mat thermoplastic,
face chemistry, interparticle spacing and extent of the addition of up to 15 wt-% mica enhanced the fibre–
agglomeration.5 Higher aspect ratio fillers give greater matrix adhesion while improving the tensile, flexural and
reinforcement and produce higher stiffness, heat distor- impact properties.10
tion temperature and creep resistance. Fillers naturally have a lower CTE than polymers.
The typical spherical fillers are calcium carbonate, The CTE of filled compounds can depend upon particle
clay, glass beads, carbon black and alumina trihydrate. size, distribution and specific surface area.12 Increasing
Among these, calcium carbonate is the most widely used the interfacial area increases the constriction of the
filler as it is readily available and of low cost.5 It reduces matrix and decreases the CTE. However, poor adhesion
warpage, increases modulus and, in virgin materials, between filler and matrix can lead to an increase in the
reduces the cost of the material. In such applications, thermal expansion coefficient.13 For some systems (e.g.
strength is normally reduced slightly. Impact toughness silica filled epoxy composites), decreasing the filler
is also reduced, with the exception of very fine additive crystallinity decreases the CTE.12
grades, which can act as impact modifiers.5 Stearate The majority of plastics are inherently flammable.
coatings are often used to improve surface bonding and Reduced flammability is desirable for many building
dispersion. The type of polymer is also important where applications and often mandatory for products designed
filler/matrix interfaces are considered. For example, the for indoor use. Conventional halogenated systems are
coated filler increased the impact toughness in poly- banned in many applications due to smoke toxicity and
propylene (PP) homopolymer; however, it decreased the environmental concerns. Zero halogen systems are
toughness in high density polyethylene and PP.6 available, such as alumina trihydrate and magnesium
Plate-like fillers are better reinforcements than sphe- hydroxide. Loadings of 60 wt-% are required to produce
rical fillers. Examples are talc, mica and kaolin.7 the same level of flame retardancy to the detriment of
Modulus, shrinkage, warpage and heat distortion strength and impact resistance. Intumescent phosphor-
temperature have been improved by the addition of all ous based systems require ,30 wt-% loading. At this
these fillers to polymers. However, tensile strength, level, the mechanical properties are still affected.5
impact strength and elongation at break tend to
decrease.8 Experimental
Mica has an aspect ratio only rivalled by fibrous Materials
materials. For good bonding to non-polar plastics, it
needs to be silane treated or mixed with maleic The polymer used was a proprietary blend of common
anhydride modified polymers. Most commercial appli- amorphous and semicrystalline recycled polymers. The
plastics were shredded and granulated to 10 mm sized
cations do not justify the addition of expensive silane
flakes and then tumble mixed. The blend had a melt flow
treatment.8 Mica has low CTE and good weathering
index of 11?1 g/10 min at 230uC. Four different addi-
performance.7 A synergy was found by some authors9,10
tives were compounded with the blend.
when adding low quantities of mica to glass fibre
(i) Omyalene 102M calcium carbonate from Omya
reinforced polyolefins to increase modulus, improve
UK: an 86 wt-% stearic acid coated chalk
dimensional stability and reduce cost. The increase in
whiting in a polyolefin carrier. The particles
properties was attributed to a positive effect of mica on
have an aspect ratio of 1 and an average particle
the fibre–matrix adhesion.
diameter of 2 mm. The specific surface area is
Fibre fillers have the highest aspect ratio and give
2?5 m2 g21 according to BET ISO 4652
significant reinforcement. Examples are glass, carbon,
(ii) Micro Mica W160 from Norwegian Talc AS
straw, flax, hemp and kenaf. The degree of reinforce-
and distributed by Omya: a muscovite with
ment is significantly affected by fibre modulus, aspect
aspect ratio 20 : 1 and a median particle size of
ratio, length and orientation in the product. Glass fibre
13?5 mm (wet analysis Malvern Mastersizer X)
is the most common reinforcement for polymers. As or 4?2 mm (X-ray analysis Sedigraph 5001). The
reported by several industrial and academic studies, it specific surface area is 6?8 m2 g21 according to
can be used to upgrade recycled thermoplastics into long BET ISO 4652
life products.11 It improves strength, stiffness, fracture (iii) 3299 EC13 chopped strand glass fibre from
toughness and heat resistance.5,9 An increase in the heat PPG Industries: a silane treated fibre of 14 mm
deformation temperature from 60 to 150uC for a 40 diameter and 4?5 mm length. For additional
wt-% loaded PP has been reported.5 Titanate or silane coupling, 2% Bondyram 1001 maleic anhydride
coatings and maleic anhydride or acrylic acid coupling modified homo-polypropylene from Polyram
agents are required for optimum fibre–matrix bonding. was added
Fibre lengths .0?5 mm are required for optimum (iv) 58578-M1-300 Superex POV0-HF flame retar-
strengthening, and the properties are dramatically dant masterbatch from Americhem, a proprie-
improved above 1 mm. tary halogen free intumescent flame retardant in
A study on 30 wt-% long glass fibre PP showed that low density polyethylene carrier.
the addition of 20 wt-%CaCO3 to the PP matrix gave an Table 1 shows the additive combinations used with the
increase of 10% in tensile modulus. Such an increase recycled blend in this study.
exceeded the modulus enhancements predicted by the The flame retardant was added at a suitable level to
rule of mixtures and was therefore attributed to give UL 94 V0 rating.14
synergistic interactions between the glass fibres and
CaCO3. However, tensile strength and fracture tough- Sample preparation
ness decreased.9 Short glass fibre and mica have been The materials were compounded using a Berstorff ZE25
shown to increase stiffness and reduce warpage.10 In a co-rotating twin screw extruder with a temperature

318 Plastics, Rubber and Composites 2011 VOL 40 NO 6/7

 Hugo et al. Recycled polymer composites for structural applications

profile of 180–210uC and a speed of 430 rev min21. The

compounded material was pelletised into 5 mm long
pellets. Standard test specimens were injection moulded
using a NegriBossi V55-200 with a 62 ton maximum
clamp force. The temperature profile was 200–230uC.
The mould was not cooled.
Mechanical testing
Specimens were tested using a Hounsfield HK100-S.
Type 2 ISO 1367 dog bone specimens were tensile tested
at a speed of 5 mm min21. ASTM D 970 flexural
specimens (127612?763?2 mm) were tested to flexural
three-point bend test with a span of 51?2 mm at a speed
of 2 mm min21. The support noses had a diameter of
5?95 mm. The loading nose had a diameter of 6?3 mm.
Linear CTE
Two different methods were used to measure the linear
CTE. A Perkin Elmer Diamond thermomechanical
analyser was used over the range of 220–60uC and at
a ramp rate of 2uC min21. Measurement of the change
in length of the flexural test bars after conditioning at
218 and 55uC was carried out using a standard
laboratory oven and freezer. Vernier callipers were used
to measure the change in dimensions.
Scanning electron microscopy 1 Tensile and flexural modulus of systems developed in
Flexural test bars were dipped in liquid nitrogen, this study: a tensile modulus and b flexural modulus
clamped in a vice and fractured by a hammer blow. of particle reinforced recycled polymers
The samples were carbon coated during the sample
preparation procedure. The fracture surfaces were
is consistent with the literature. Mica has a far higher
examined using a Philips XL 40 in secondary electron
aspect ratio than calcium carbonate, which increases the
and backscattered electron modes.
contact area between the mica and the matrix and leads
to a more significant effect on properties. The increased
Results surface area enables improved stress transfer to the
CaCO3 and mica were added to the recycled polymer filler.12 In addition, mica has a higher tensile modulus
blend to evaluate the potential property improvements (over 100 GPa) compared to CaCO3 (35 GPa).
that can be achieved using low cost fillers. The proper- Tensile strength decreases, and flexural strength
ties resulting from the addition of a fire retardant are increases slightly (Fig. 2). The reduction of tensile
also reported for comparison. Subsequently, the effect of strength for the CaCO3 filled systems indicated poor
glass fibre reinforcement was evaluated to assess whether interfacial adhesion for this system. The stearic acid
the higher enhancement in properties justifies their coating on CaCO3 generally improves dispersion, but
additional cost and processing complexity. A further has no or limited coupling effect.5 For the mica filled
step was the investigation of hybrid systems containing system, the tensile strength was practically unchanged,
glass fibre and a lower aspect ratio filler in order to as mica possesses better reinforcing ability than calcium
obtain a wider range of property enhancement and carbonate and typically does not depress strength
further improvement of certain properties through considerably.5 In flexure, the stress is maximum at the
synergistic effects. surfaces. The force is compressive on the loaded surface
with an equal and opposite tensile stress on the opposite
Mechanical properties surface. The increase in flexural strength for both
The effect of each filler is dependent on the method of particulate filled systems was in turn attributed to the
loading. The particulate fillers increase tensile and compressive component of the mechanical response. The
flexural moduli significantly (Fig. 1). The higher compressive strength of filled systems tends to increase
enhancement of tensile modulus for mica filled systems even for uncoupled systems. This is consistent with

Table 1 Additive combinations compounded with proprietary recycled plastic blend used in this study (GF: glass fibre,
M: mica, FR: flame retardant)

Amount of additive in compound/wt-%

20% 20% Flame 15% 15%GF 15%GF 30% 30%GF

Additive CaCO3 Mica retardant GF z5%C z5%M GF z5%M

Calcium carbonate 20 5
Mica 20 5 5
Glass fibre 15 15 15 30 30
Flame retardant masterbatch 40

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Hugo et al. Recycled polymer composites for structural applications

2 Tensile and flexural strength of systems developed in

3 Tensile and flexural modulus of fibre reinforced materi-
this study: a tensile strength; b flexural strength of
als developed in this study: a tensile modulus; b flex-
particle reinforced recycled polymers
ural modulus of recycled systems

previous studies on filled thermoplastics, which reported

caused a slight increase in the mechanical properties,
the compressive strength to be directly proportional to
except for the tensile strength.
Young’s modulus.13
The addition of small proportions of mica to the glass
The addition of an intumescent flame retardant
fibre reinforced blend resulted in an increase, rather than
increases tensile modulus, but is very detrimental to
a decrease (observed for CaCO3), in tensile strength.
strength and causes an unexpected decrease in flexural
Since 20 wt-% of mica alone did not alter the tensile
modulus. The proprietary masterbatch (40 wt-%) was
required to give the required improvement on flamm-
ability properties. This high level would be expected to
have a significant effect on mechanical properties.
Intumescent flame retardant systems are not reported
to have a reinforcing effect, plus their hydrophilic nature
creates a poor interfacial bond with hydrophobic
polymers. Studies have reported an increase in modulus
and heat deflection temperature, but a decrease in
impact strength and other mechanicals.5 Coupling
agents have been studied, showing improvements in
mechanical properties without a detrimental effect on
flammability.15,16
Elongation in tension was reduced for all fillers, in
particular for glass fibres. However, elongation at break
for all systems was above 3?5%. Such values of
elongation at break are sufficient to guarantee a
satisfactory performance in semistructural applications,
which are generally designed for stiffness with high
safety factors.17
Glass fibre significantly increased the strength and
modulus of the recycled polymer blend (Figs. 3 and 4).
Owing to the cost and processing limitations for the
recycled composite, the maximum amount of glass fibre
incorporated in the product was 30 wt-%. A secondary
filler was added to the glass fibre reinforced systems to
further enhance the structural properties without
increasing the cost. Calcium carbonate had a similar 4 Tensile and flexural strength of fibre reinforced sys-
effect in the glass filled blend as with the pure polymer tems developed in this study: a tensile strengths;
blend. In both cases, the addition of calcium carbonate b flexural strength modulus of recycled systems

320 Plastics, Rubber and Composites 2011 VOL 40 NO 6/7

 Hugo et al. Recycled polymer composites for structural applications

5 Linear CTE for systems developed in this study

strength of the material (Fig. 2), it was concluded that a

synergistic interaction took place between mica and
glass fibre reinforcement. Such a positive effect was
observed both at 15 and 30 wt-% glass fibre loading and
was particularly marked during the tensile tests. The
addition of 5 wt-% mica into 30 wt-% glass fibre
reinforced blend resulted in an increase in tensile
strength of 20%. For the same material system, an even
more remarkable synergy was observed in terms of
tensile and flexural modulus, which increased by 35 and
7% respectively. An explanation for this effect has been
proposed in the section on ‘Discussion’.
6 Scanning electron microscopy images showing fracture
Linear CTE surface morphology of 30 wt-% glass fibre and 5 wt-%
Thermomechanical analysis measurements produced mica filled compound: a secondary electron mode and b
complex results due to the number of transitions for backscattered electron mode showing filler distribution
the separate polymers. Measurement of the test speci-
mens produced reasonably consistent results (Fig. 5). The tensile modulus was increased by 86%, and the
The standard deviation was appreciable due to the small strength decreased marginally. This improvement is in
changes in size. Particulate fillers appeared to increase line with other studies that reported 50–100% higher
the linear CTE, while it was significantly reduced in the properties compared to talc or calcium carbonate, with
presence of fibre reinforcement. The increase in CTE for little or no reduction in impact strength.5 In flexural
the particulate systems can be attributed to the poor mode, the modulus increased by 114% and strength
adhesion between these fillers and the polymer matrix.13 increased slightly.
The reduction in CTE for the glass fibre reinforced The silane treated glass fibre with maleic anhydride
systems is consistent with a strong coupling between polypropylene compatibiliser significantly improved the
glass fibres and the polymer matrix, which was achieved strength and modulus of the blend, as predicted. The
by the addition of silane coating and maleic anhydride 15 wt-% glass fibre increased the tensile strength by 70%
grafted PP. and the elastic modulus by 63%. The flexural strength
Scanning electron microscopy was again increased by 60% and the flexural modulus by
210%. The 20 wt-% mica increased the tensile modulus
Scanning electron microscopy showed a well dispersed
to the same degree as 15 wt-% glass fibre, however
blend of different polymers. The orientation of the fibres
without the increase in strength. Mica could be used as
in the direction of process flow (perpendicular to the
an alternative to glass fibre for certain applications. The
fracture surface) can be observed at the fractured surface
30 wt-% glass fibre increased the tensile strength by 85%
(Fig. 6). The calcium carbonate addition showed good
and the modulus by 240%. The flexural strength was
distribution with a little agglomeration (Fig. 7). The
increased by 115% in this case, and the flexural modulus
maximum agglomerate size observed was below 10 mm
by 445%, as expected in a well oriented and consolidated
(Fig. 7b).
glass fibre composite.
The addition of 5 wt-% calcium carbonate to 15 wt-%
Discussion glass fibre in the recycled polymer blend increased the
Stearate coated calcium carbonate behaved as predicted tensile and flexural moduli by further 20%, while the
from the earlier reported literature.5 The modulus was strength was decreased in tension. The 15 wt-% glass
increased by 24%, and the strength was decreased fibre reinforced PP (GRPP) samples reinforced with
slightly. In flexural mode, the modulus was increased 5 wt-% mica presented similar property enhancements,
by 40%, and the strength was also increased slightly. The with the difference that mica improved the tensile
higher improvement in flexural properties was due to the strength. However, a much more pronounced synergistic
combination of tensile and compressive modes. effect was observed for the addition of mica to 30 wt-%
The uncoated mica resulted in an increased reinforce- filled glass fibre blend. For this system, mica improved
ment effect as expected with the increase in aspect ratio. the tensile modulus by as much as 35% and flexural

Plastics, Rubber and Composites 2011 VOL 40 NO 6/7 321

Hugo et al. Recycled polymer composites for structural applications

reinforced glass fibre thermoplastic systems with the

incorporation of particulate fillers.
The proprietary intumescent flame retardant reduced
all mechanical properties by 10–30%, except the tensile
modulus, which was increased by 20%. The particles had
little reinforcing effect in this case. Use of flame
retardants is undesirable due to the reduction in
mechanical properties and higher cost. Reinforcement
additives and impact modifiers could be added to
counterbalance the property reduction.5
The glass fibre gave a significant reduction in CTE.
The 15 wt-% glass fibre gave 3061026 uC21, which is
close to that of wood across the grain.19 The 30 wt-%
glass fibre gave 1861026 uC21 values in line with steel,
concrete and wood along the grain.19–21 The fibres were
oriented parallel to the direction of the flow, and the
large interfacial area constricted the expansion of the
matrix. The increase in CTE for calcium carbonate is
unexpected compared to another study, which gave a
12% reduction in a 40 wt-% filled PP blend,12 and was
attributed to the weak interfacial adhesion.

Conclusions
The effect of the addition of various commercially
available fillers to a blend of recycled polymers was
investigated to evaluate the simultaneous enhancement
7 Images (SEM) showing fracture surface morphology of of key structural properties (stiffness, strength and CTE)
20 wt-% calcium carbonate filled compound: a second- of the blend.
ary electron mode; b back scattered electron mode Varying results were obtained by the incorporation of
showing calcium carbonate distribution a single filler (CaCO3, mica or glass fibre), depending on
the aspect ratio of the filler and the method of loading.
modulus by 7%, with a marginal increase in strength. A Hybrid systems containing glass fibre and a lower aspect
similarly remarkable effect has been observed for mica ratio filler achieved a wider range of property enhance-
filled glass fibre reinforced PP by Zhao and co-workers10 ment and further improvement of certain properties
The authors found that the addition of moderate loadings through synergistic effects.
of mica to glass fibre mat reinforced thermoplastic PP led Spherical calcium carbonate gave a modest increase in
to a substantial increase in tensile and flexural modulus (in tensile and flexural modulus to the detriment of tensile
the order of 100%), combined with a moderate improve- strength, while plate-like mica increased the moduli
ment of strength. This synergy was explained by the significantly with minor improvements in strength. Glass
increase in radial compressive residual stresses on the glass fibre reinforcement contributed a significant increase in
fibres (and therefore an enhanced fibre–matrix adhesion) strength and moduli, particularly in flexural mode. The
brought about by the addition of mica. During solidifica- 20 wt-% mica increased the modulus to the same degree
tion, the difference in CTE between polymer matrix and as the 15 wt-% glass fibre without causing an increase in
glass fibres generated a compressive radial stress at the strength. Mica could be used as a replacement for glass
interface, which is proportional to the difference in fibre in certain applications. The addition of mica to
glass fibre resulted in a further improvement of
thermal expansion coefficient and to the elastic modulus
mechanical properties, particularly in tensile mode.
of the matrix.18 The main effect of adding mica to the
The substantial increase in modulus with the addition
polymer matrix is an increase in elastic modulus, whereas
of 5% mica and 30% glass fibre to the recycled polymer
the variation in CTE is only moderate. This can lead to a
blend was explained in terms of improved interfacial
stronger interfacial interaction between the glass fibres
adhesion between glass fibres and polymer matrix due to
and the polymer matrix, leading to a significant increase in
the effect of mica on the polymer properties. Further
stiffness. The present work seems to indicate that to obtain
investigations will be needed to comprehensively under-
this effect, mica does not need to be surface treated. The
stand such a remarkable effect. The addition of
untreated mica used in this study tended to increase the
particulate fillers without chemical coupling to the
CTE of the polymer blend, which could lead to a further
polymer blend seemed to increase the CTE, but material
increase in compressive stress at the interface and a more systems containing adequately coupled glass fibre
significant improvement in the elastic modulus. It is reinforcement showed a reduction in the CTE to the
expected that the fibre–matrix adhesion strength would be same level as concrete, steel and wood.
significantly decreased in the presence of higher loadings
of mica because of the contact of the glass fibres and the
mica flakes at the interface. However, it is still unclear why
Acknowledgements
this synergy was observed only for 30% and not for 15% The authors wish to acknowledge Z. B. Marzuki for his
glass fibre loading and why similar trends have not been assistance in the mechanical testing and C. Magnus for
previously reported by other authors on a variety of highly his assistance in dynamic mechanical analysis testing. In

322 Plastics, Rubber and Composites 2011 VOL 40 NO 6/7

 Hugo et al. Recycled polymer composites for structural applications

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