Composites
for recyclability
Polypropylenes reinforced with oriented
polypropylene fibers, so-called all-PP composites,
have specific economic and ecological advantages
over composites based on glass fibers since, upon
recycling, a PP-blend is obtained that can be reused
to make all-PP composites or be used for other
PP-based applications. Recent studies show the large
potential of a newly developed manufacturing route
for all-PP composites based on coextruded tapes.
These tapes are highly oriented providing high
strength and stiffness and are coated with a
specially formulated, thin layer of PP, which seals the
tapes together in a subsequent consolidation process.
The material can be processed using a wide range of
composite processing technologies including
thermoforming, as well as filament winding.
Queen Mary, University of London,
Department of Materials,
Mile End Road,
London E1 4NS, UK
E-mail: t.peijs@qmul.ac.uk
30 April 2003
by Ton Peijs
Environmental legislation, consumer concern, and
waste management approaches based on concepts
like the polluter pays are all increasing the pressure
on manufacturers of materials and end-products to
consider the environmental impact of their products
at all stages of their life cycle including ultimate
disposal, a cradle to grave approach. At this
moment, designing for recycling or eco-design is
becoming a philosophy that is applied to more and
more materials and products. Recycling must be an
important part of our daily lives if we are to preserve
the natural resources of our planet.
The automotive industry, in particular, is now trying to
make every component recyclable because of a new
European Union (EU) directive on the end-of-life of vehicles
(ELV). This states that by 2015 vehicles must be made of
95% recyclable materials, of which 85% can be recovered
through reuse or mechanical recycling and 10% through
energy recovery or thermal recycling. The ELV Directive
(2000/53/EC) came into force in October 2000 and all
member states were required to transpose the directive into
national law by April 2002. The directive aims to reduce the
amount of waste from vehicles (automobiles and vans) and
includes requirements for member states to introduce strict
standards for the treatment of ELVs at authorized treatment
facilities.
Polymers are a material of this century and have enjoyed
an enormous growth since the 1960s. Notably, in the
automotive industry polymers are currently used to make
parts such as body panels, underbody structures, dashboards,
ISSN:1369 7021 Elsevier Science Ltd 2003 Open access under CC BY-NC-ND license.

seating components, front ends, and bumpers. Recycling has
been especially promoted in the plastics industry because of
the complex issues involved and, at this moment, the amount
of plastic being recycled in Europe is growing at more than
20% per year. Recycling issues have been responsible for a
clear change in the use of polymers in the automotive
industry. In the 1980s, the automotive industry was using a
large number of different polymeric materials, including a
range of polymer blends and glass fiber reinforced plastics.
However, since the mid-1990s the major trend has been
towards simple monocomponent systems rather than
complex polymer blends and alloys. Although, in theory, all
thermoplastic polymers can be remelted and recompounded
into a new grade, the presence of certain additives, blends, or
fillers like glass fibers may limit the application area of the
recyclate.
Currently, polypropylene (PP) is used for a large number of
applications. It is cheap, can be reprocessed several times
without significant loss of properties, and can be easily
modified to achieve specific requirements. Of all the
thermoplastics, the growth of PP over its 40 years of
existence has been the most vigorous in plastics history. In
the past decade alone, PP has been the fastest growing major
plastic at some 7% per year. An important growth area for PP
is that of engineering plastics and it is now penetrating into
market areas formerly covered by engineering plastics like
ABS or polyamides. In order to be able to compete with these
resins in engineering applications and to meet the high
demands on stiffness and strength, PP has to be reinforced.
Glass fibers are the major reinforcing elements used for this
purpose. Although both PP and glass are perfectly recyclable
individually, when combined they are not easy to recycle.
State-of-the-art constructions are composed of PP with PP
foam (e.g. the all-PP dashboard), but often these products
still contain glass fibers as a foreign component. As these
recycled materials often suffer from significant loss in
mechanical properties during recompounding, further use in
critical application areas may be limited. Glass fibers are,
therefore, the main component in many plastic products that
still cause environmental problems, both in mechanical
recycling and end-of-life disposal through incineration
(thermal recycling).
Current trends toward environmentally-friendly composite
systems focus on the use of natural fibers like flax and hemp
as alternatives to glass fibers. Although these fibers do have
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some ecological advantages over glass fibers, since they are
renewable and can be incinerated, natural fibers do not have
advantages with respect to mechanical recycling. In fact, next
to mechanical degradation, the relatively poor thermal
stability of these lignocellulose fibers may lead to severe
additional thermal degradation during subsequent recycling
or reprocessing steps. Especially in the case of a polymer like
PP, which has the lowest environmental impact of all
polymers because it is lightweight and has excellent
recyclability, the addition of natural fibers may significantly
lower the eco-performance of these materials!
All-PP composites
One of the important rules in designing for recycling is
based on selecting the smallest possible number of different
constituents in a material system or, alternatively, in the case
of plastics, selecting compatible polymers, which in practice
means the use of monomaterials. As automotive
manufacturers are forced to make every component
recyclable, this leaves little scope for fiber reinforced plastics.
As the introduction of any foreign filler, including natural
fibers, is in conflict with the basic idea behind designing for
recycling, an obvious reinforcing element for PP would
therefore be the use of a high-performance PP fiber.
High-performance PP fibers in combination with PP
matrices will lead to a fully recyclable, all-PP composite that
has major ecological advantages. Upon recycling of all-PP
composites, a PP blend is obtained that can be reused to
make all-PP composites or, alternatively, be used for other
high value PP-based applications. Besides recyclability, the
use of PP fibers has a number of other ecological and
technological advantages compared with glass fibers. PP
fibers are nonabrasive to processing equipment, can be
thermally recycled at the end of their lifetime for energy
recovery (they have a calorific value similar to oil), and have
a very low density, which can potentially lead to lightweight
parts, lowering fuel consumption and gas emissions. Another
advantage of using a more flexible and ductile fiber will be
improved crash behavior. All-PP composites will not splinter,
but fail in a more ductile manner. Such soft crash behavior is
of significant interest for various inner-trim parts as well as
for external panels, bumper bars, etc. since it will lead to
safer automobiles.
In order to develop such all-PP composites, a consortium
was formed by the end of 1998 including two universities
April 2003 31
 REVIEW FEATURE

Table 1. Typical values of mechanical properties of fibers. reached, which results in PP filaments with Youngs moduli
up to 18 GPa and tensile strengths of 650 MPa. Table 1
Density Tensile Stiffness Specific Specific
strength strength stiffness shows some typical values for mechanical properties of PP
fibers in comparison with glass and flax fibers. Clearly, the
g.cm-3 MPa GPa MPa/g.cm-3 GPa/g.cm-3
newly developed high-performance PP fibers can compete
E-glass 2.6 2000 70 770 27
Flax 1.4 600 40 430 28 with or even out-perform glass or flax fibers on a weight
PP 0.9 650 18 720 20 basis when specific properties are compared.

Eindhoven University of Technology in the Netherlands and
Queen Mary, University of London in the UK and four
industrial partners all from the Netherlands: Lankhorst-
Indutech, BW Industrial, Polynorm Plastics, and DSM. The
joint R&D project entitled PURE was partly funded by the
Economy, Ecology, Technology (EET) program of the Dutch
Government, which supports innovative projects in the area
of eco-design and sustainable development.
High-performance PP fibers
One of the first challenges in the PURE project was to
develop a high performance PP reinforcement that enables
all-PP composites to be competitive with glass fiber systems
like glass mat reinforced thermoplastics (GMTs) or long fiber
reinforced thermoplastics (LFTs). The tensile properties of
melt-spun PP fibers (or tapes) are influenced by their physical
structure, which is determined by the fiber formation
conditions. Common PP fibers produced by a commercial
spinning line have relatively low draw-ratios and Youngs
moduli of around 3-5 GPa. By optimizing the cold-drawing
process of PP filaments, a high overall draw-ratio can be
Processing route for all-PP composites
A major challenge in the development of all-PP composites is
the creation of a processing window where PP fibers can be
combined with PP resins. This is of eminent importance, as
one has to combine two materials with basically the same
chemical structure and, thus, melting temperature. The
challenge is to find a processing window that is large enough
to keep the oriented PP fibers intact while being impregnated
with PP resin. One method that can be used to develop such
a single polymer composite is the use of the so-called
overheating behavior of constrained oriented polymer fibers1.
Using this overheating behavior, it should be possible to
embed an oriented PP fiber in a molten polymer matrix of the
same grade. Fig. 1 shows typical differential scanning
calorimetry (DSC) traces of constrained and unconstrained PP
fibers. Constraining the same fiber results in a different DSC
trace, with the melting temperature shifted to higher values,
hence offering a temperature window for processing of single
polymer composites2.
Fig. 2 shows the morphology of such a PP single fiber
model composite, as developed by Loos et al.2. The

14

12
Unconstrained fiber
Constrained fiber
10
Heat flow [mW]

0
100 120 140 160 180 200
Temperature [C]

Fig. 1 DSC plots of constrained and unconstrained PP fibers showing the overheating behavior.

32 April 2003

Fig. 2 Optical micrograph, showing transcrystalline interfacial regions in between a PP
fiber and a PP matrix. Both fiber and matrix are of the same polymer grade and show the
potential of constrained overheating to impregnate PP fibers with the same PP matrix.
transmission optical microscopy image shows three areas
with different features typical in such a composite: the PP
fiber (i) partially embedded in a transcrystalline layer (ii)
surrounded by PP matrix material (iii) consisting of spherulitic
superstructures. In this case, the PP grade used for fiber and
matrix are identical, proving that it is possible to make all-PP
composites out of a single polymer material using the
constraint overheating concept.
Based on the results shown above on single fiber
composites, it should be possible to impregnate a bundle of
PP fibers with a PP matrix using traditional solution or
powder impregnation routes. Such a process would be very
similar to the ones used for manufacturing continuous glass
fiber reinforced PP composites. Impregnation of fiber bundles
with highly viscous resins is, however, one of the main
bottlenecks in the cost-effective manufacturing of
thermoplastic composites. In order to facilitate impregnation
of the fiber bundles, low molecular weight grades of PP with
sufficiently low viscosities to wet-out the fiber bundles are
often used. But this practice compromises the mechanical
properties of the polymer matrix. The impregnation process is
also relatively slow and, therefore, costly because the
polymer needs to flow within the fiber bundle in order to
fully wet the individual filaments.
An interesting alternative to melt impregnation routes for
the development of single polymer composites is the hot-
compaction route originally developed at the IRC at the
University of Leeds in the UK. As a starting point, the process
takes oriented polymer fibers that are then compacted to an
REVIEW FEATURE
oriented polymer sheet material under suitable conditions of
temperature and pressure. The preparation route relies on
selective surface melting of the oriented fiber, which upon
cooling recrystallizes to form a matrix binding the fibers
together. The result is a fully recyclable, self-reinforced
polymer material. The method was initially developed for
melt-spun polyethylene fiber3, but subsequent studies have
shown that the process is applicable to a number of oriented
polymers, including gel-spun polyethylene fibers
(Dyneema)4, poly(ethylene terephthalate) (PET)5, and PP
fibers6-8. Recent efforts have mainly focused on PP and the
material9 is now commercially available from BP Amoco
under the trade name Curve. Although the hot-compaction
method developed at the University of Leeds is a very elegant
method for the production of single polymer composites, its
main disadvantage is the narrow processing window of a few
degrees. The material has to be processed in a very controlled
way, since overheating will destroy the fiber properties. Only
when processed in this rather narrow temperature window
will a large percentage of the fiber (>70%) be retained and a
self-reinforced polymer material be produced that exhibits
reasonable mechanical properties6,7.
Pure technology
Because of the above mentioned drawbacks in existing
technologies for the processing of thermoplastic composites,
the PURE technology follows a different and, in the context
A
B
Cold drawing
A
Co-extrusion
Consolidation
Fig. 3 Co-extrusion technology is used for the development of high-performance PP tapes.
These tapes consist of a highly oriented core (B) and a thin polymer skin (A) to weld the
tapes together in a subsequent consolidation process. This process results in all-PP
composites with very high reinforcement content (>80%).
April 2003 33
 REVIEW FEATURE

of all-PP composites, new approach. It combines coextrusion

of PP tapes using two types of PP with different melting
temperatures, cold drawing of these tapes to increase the
mechanical properties, and, at a final stage, welding the tapes
together (Fig. 3). These coextruded tapes are 100% PP-based
and consist of an oriented PP core, which provides strength
and stiffness, and a thin polymer skin, with a lower melting
temperature than the core material, which forms the matrix.
One of the advantages of using tapes instead of fibers is
the more effective packing that flat tapes enable compared
with circular fibers. This can lead to higher reinforcement
contents in the final product. The coextruded tapes can be
woven into fabrics, which can be stacked and consolidated
into flat laminates, which can be thermoformed subsequently
(Fig. 4). During consolidation, the oriented PP tapes can be
constrained by the molding pressure to increase the melting
point of the oriented core material and further extend the
processing window. Constraining plus co-extrusion
technology has led to a processing temperature window that
can be tailored through the selection of the polymer coating,
but is generally in the order of 20-40C. The process of co- Fig. 4 All-PP prototype product manufactured by thermoforming technology from
consolidated woven fabric sheet.
extrusion and tape welding has enormous advantages over
conventional manufacturing technology for thermoplastic
composites. Consolidation is achieved by simply welding the These values compare very favorably to GMTs, which have
tapes together, thus avoiding the typical impregnation typical stiffness and strength values of 4-5 GPa and
problems encountered in traditional thermoplastic composite 80-100 MPa, respectively. For some applications PURE
manufacturing. Because long flow paths of the matrix are not material is entering or in the case of toughness even
necessary, the autoadhesion process is much faster and exceeding the performance window of composite systems
results in high-quality, void-free composites with a high based on continuous glass fibers like Twintex.
fiber volume fraction (>80%). Despite the fact that the Processing of PURE involves consolidation by hot- or
mechanical properties of the PP tapes themselves at least belt-pressing woven fabrics into flat laminates, which can
in terms of stiffness are lower than those of glass fibers, be subsequently thermoformed into end-products.
current all-PP laminates already out-perform GMTs. This is Alternatively, the fabrics can be directly shaped into parts
because of the continuous tape structure and high using techniques such as matched-die molding, rubber
reinforcement component in comparison with GMTs, which forming, vacuum forming, or even simple vacuum-bag
typically have fiber volume fractions of 20-30%. The molding. The first prototypes have been developed to show
combination of continuous reinforcement and exceptionally the feasibility of the concept of all-PP composites and,
high reinforcement contents is very significant as it means recently, one of the UKs leading thermoformers, Linecross,
that the success of the all-PP material does not depend on teamed up with Lankhorst-Indutech to develop the
the need for a PP tape, which on a weight basis should out- processing and production of PURE composite parts on an
perform E-glass. The material is currently being industrial scale.
commercialized by Lankhorst-Indutech in the Netherlands Alternatively, all-PP tapes can be wound onto a mandrel
under the name PURE10 and laminates based on woven and subsequently heated for consolidation. Upon heating, the
fabrics have been shown to exhibit a typical stiffness of oriented PP is constrained by the mandrel and as the thermal
6-8 GPa and tensile strength of around 200-250 MPa11. expansion of the oriented PP tape is negative, consolidation is

34 April 2003
 REVIEW FEATURE

achieved. Furthermore, promising all-PP sandwich panels of

high stiffness can be obtained by combining all-PP plates
with PP honeycomb cores or PP foams (Fig. 5). This allows
for development of fully recyclable structural sandwich
panels, which is of great significance because the recycling
of traditional composite sandwich panels is very complex
as they generally consist of a minimum of three different
materials.

Potential applications
The current market for PP-based composites can be
segmented into four sectors: transport (45%), electrical
(35%), consumer and domestic appliances (10%), and
industrial (10%).
In the automotive industry, in particular, there is a clear
trend towards the replacement of metal body parts with
plastic body parts. The reasons for this development are
mainly associated with the lowering of production costs and
weight reduction. GMTs and LFTs, which are both PP-based,
are generally considered as strong candidates to penetrate
the automotive markets where performance, fabrication
speed, and total cost are critical issues. Consequently, they
are among the fastest growing composite systems on the
market. Because of the ELV Directive, the development of
fully recyclable all-PP composites is especially attractive for
this market sector and it is expected that the first
applications will be to replace current GMT-based products
such as body panels, underbody structures, seating
components, and bumper bars. Based on the properties of
all-PP composites, the first commercial applications of these
materials are likely to be in strength and impact critical
applications like underbody shields or as an alternative to
natural fiber reinforced plastics for inner-trim parts.
At the same time, all-PP composites offer a fully
recyclable, lightweight alternative to continuous glass fiber
reinforced PP materials like Twintex, notably for
Fig. 5 All-PP pipes and pressure vessels produced by SICOMP of Sweden (top) and an
all-PP sandwich panel based on all-PP skins and PP honeycomb core (bottom).
thermoforming applications or as facing materials for all-PP
sandwich structures like floor panels. Besides the automotive
industry, PURE material also has potential for the
development of high-pressure tubes and pipes. At this
moment, several commercial applications are under
development for a wide range of products and market
segments. MT
Acknowledgments
The development of the PURE technology, as described above, represents the efforts of
many individuals both in academia and industry. I wish to thank all of them for their
invaluable contributions to the PURE project. At Queen Mary, University of London I wish
to thank my coworkers Norbert Cabrera, Benjamin Alcock, and Nektaria Marianthi
Barkoula. At Eindhoven University of Technology, the contributions made by Tilo
Schimanski, Joachim Loos, Jeroen Hofman, Edwin Klompen, and Piet Lemstra are gratefully
acknowledged. Finally, I would like to thank Hans Jacobs and Fokke Bloemhof at
Lankhorst-Indutech and Peter Meijnen at BW Industrial for their continuing support. This
work is sponsored by the Dutch Governments Economy, Ecology, and Technology (EET)
program for sustainable development, under grant number EETK97104.

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April 2003 35