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Die Angewandte Makromolecular Chemie 272 (1999) 11–16 (No. 4746) 11

Pultrusion of construction materials from renewable ones


raw materials

Christian Gensewich*1 , Ulrich Riedel 2

1
Institute for Structural Mechanics, DLR Braunschweig, Lilienthalplatz 7, 38108 Braunschweig, Germany
2
German Aerospace Center, Institute for Structural Mechanics, Lilienthalplatz 7, 38108
Braunschweig, Germany

SUMMARY: Pultrusion technology is a continuous manufacturing process for the manufacture of profiles from fiber
composite materials. Usually, endless rovings made of glass or carbon fibers are used for this purpose, which are
soaked in a duroplastic synthetic resin and drawn through a mold. The profile hardened in the tool is removed from
the tool and cut to length with a saw.

This very cost-effective manufacturing process of fiber composite technology could be used for natural fiber
reinforced biopolymers. With a suitable choice of fiber material, the specific properties of GRP can even be
surpassed. This lightweight construction potential should be used in particular for applications in traffic engineering
and in the furniture sector.
Profiles made of natural fiber composites also offer great advantages when it comes to recycling compared to the
previously produced GRP profiles. They can be recycled without any problems in a CO2-neutral manner by thermal
recycling , depending on the degradation behavior of the matrix, biological degradability is also possible.
In order to be able to produce an NRP profile with similarly good specific properties as a GRP pultrudate, not only
the process but also the influence of the different fiber make-ups, such as card sliver, roving and yarn and the matrix
systems must be matched to one another. In order to keep the investment costs for natural fiber pultrusion low, the
same systems should be used here as for conventional GRP profile production.

There is a need for research primarily in reducing the moisture sensitivity of the composite and in the associated
reduction in fiber-matrix adhesion. With further advances, natural fibers can be used not only in cladding elements
and load-bearing structures indoors, but also for load-bearing components outdoors.

SUMMARY: Pultrusion is a continuous production technology for manufacturing fibre-reinforced plastic profiles.
Usually glass or carbon fibres are used which are impregnated with liquid petrochemical thermoset ting polymers,
e.g. unsaturated polyesters or epoxy resins, and cured while being pulled through a heated die.
The cured profile is then cut into parts as required.
This cost-effective production method from reinforced plastics technology is now used for profiles from natural
fibres. Choosing adequate natural reinforcing fibres, the properties of these composites can be even better than
those of glass fibre reinforced plastics (GFRP). This potential for light-weight structures should be especially used
for applications in the automotive and furniture industries.
Profiles made of natural fibres and biopolymers show decisive advantages in terms of recycling compared with
GFRP. Incineration of these materials is carbon dioxide-neutral. Using a biodegradable matrix, compos ting is
another interesting recycling option.
In order to manufacture natural fibre profiles with similar properties like GFRP, processing, fibre preforms, e.g.
slivers, preyarns, yarns and biopolymers have to be adapted to each other. To limit investments in new machinery,
the manufacture of natural fibre profiles should be possible in the same production plants as for GFRP profiles.

Research still has to be done to reduce the moisture sensitivity of these composites and increase the fibre
matrix-adhesion. At present, natural-fibre-composites are well apt for panelling elements and loaded structu res for
interior applications, in future also for exterior structural parts.

1 Introduction
Pultrusion technology is the continuous manufacturing made of glass or carbon fibers that are soaked in a
process used to manufacture profiles from fiber composite duroplastic synthetic resin and then drawn through a mold.
materials. Endless rovings are usually used for this

* Correspondence author.
a Vortrag anla¨ßlich des „2nd International Wood and Natural Fibre Composites Symposium“, 28.–29. Juni 1999 in Kassel.

Applied macromolecular chemistry 272 WILEY-VCH Verlag GmbH, D-69451 Weinheim 1999 0003-3146/99/0112–0011$17.50+.50/0
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12 C. Gensewich, U. Riedel

mix resistance or in electrical engineering because of


the low electrical conductivity.
To produce these profiles, a pultrusion system (Fig.
2) is required, which generally consists of the following
components: creel, guide system for fiber guidance,
impregnation device, shaping tool, stripping device and
rotating saw.
The roving spools required to produce a profile with
a certain fiber volume content are stored in the spool
creel. The rovings are continuously pulled out of the
stand and fed to the impregnation device by guide
systems that keep the fibers parallel.

Mat or fabric rolls can be attached to the guiding


devices, with which the mechanical properties are
changed compared to a pure UD reinforcement.
Furthermore, a fleece is placed on the fibers here, which
influences the properties of the surface. A typical layer
structure for a pultruded profile with inner UD rovings,
Fig. 1. Examples of pultruded profiles1). mats for transverse reinforcement and the surface
fleece is shown in Fig. 3.

Fibers and matrix systems made from renewable raw The fibers can be impregnated in an open soaking
materials are an alternative, so that the composite bath, in which the fibers are deflected by pins or rollers
material can be thermally recycled after use, for (Fig. 4,a). If synthetic resins containing styrene are
example in a CO2-neutral manner. For this purpose, used, however, without an adequate extraction system,
the same systems should be used for natural fiber there may be increased styrene pollution in the room
pultrusion as for conventional GRP profile production. air. An alternative to this system is resin injection, in
In order to be able to produce an NRP profile with which the matrix is injected into a closed mold through
similarly good specific properties as a GRP pultrudate, which the fibers are drawn (Fig. 4,b).
the semi-finished fiber products and the matrix systems
must be adapted to each other in addition to the process. The impregnated fibers are then fed through a mold
that is tempered to initiate a resin reaction. A typical
mold is about 1 m long and is divided into three or four
2 Process of pultrusion
zones with different temperature levels (Fig. 5). The first
Profiles are manufactured using the pultrusion process, zone of the mold is cooled to allow the profile to be
ranging from simple rectangular or round bars through formed into shape without the matrix beginning to gel.
U or I-beams to complicated special shapes (Fig. 1). In the heated second zone, the starting reaction takes
The profiles are used in a wide variety of areas, such place
as in apparatus engineering because of the good surface

Fig. 2. Components of a pultrusion line1); (a) creel, (b) control system and web feed, (c) impregnation
bath, (d) forming tool, (e) tandem take-off gripper, (f) carried saw1).
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Pultrusion of construction materials 13

Fig. 3. Layer structure of a pultrusion profile2).

Fig. 6. Characteristics of various natural fibers compared to E-


glass fibers.

up to 6 m min–1 can be achieved. On the other hand, the


significantly higher viscosity of the thermoplastics has a
disadvantageous effect on the wetting of the fibers, so that
at higher processing speeds matrix nests form and
unimpregnated fibers remain in the pultrudate. Because of
the poor quality of the pultrudate and the more complex
process, thermoplastic pultrusion has not yet established
itself.

Fig. 4. (a) open soaking bath, (b) injection impregnation tool1).


3 natural fiber composites

A duroplastic matrix system based on epoxy (EP),


unsaturated polyester (UP) or vinyl ester resins (VE) is
usually used in GRP pultrusion. In addition, organic additives
are added which influence the reaction kinetics or reduce
the resin viscosity.

However, GRP is difficult to recycle, so that at most


downcycling occurs when shredders are placed in concrete
or asphalt. As an alternative to these material systems, fibers
Fig. 5. Mold showing stages of resin solidification2). and matrix systems made from renewable raw materials are
therefore available, which can be thermally recycled after
resin, which then hardens in the third and fourth zones. use, for example in a CO2-neutral manner.

The pull-off device, which pulls it out of the mold, acts on


the resulting profile. If the same profile shape is often taken
3.1 Semi-finished fiber products
off at low speed, this system can be designed as a caterpillar
take-off. If the profile cross-section changes frequently and Natural fiber composites can be made from different plant
high take-off speeds are involved, a tandem system fibers. In order for a component to meet the mechanical
equipped with two grippers that work alternately is preferable. requirements, fibers with a high modulus of elasticity and
Depending on the wall thickness of the profiles, speeds of up high strength must be used. As Fig. 6 shows, hemp fibers
to 90 cm min–1 are common in GRP pultrusion. achieve the highest mechanical properties of natural fibers,
while flax and ramie fibers have a lower modulus of elasticity
with the same strength.
Finally, the profile is included in the ongoing process
cut to the desired length with a saw you carry with you. Cotton, on the other hand, only achieves half the strength of
the aforementioned fibers and is less suitable for use in fiber
Thermoplastic matrix systems have also been used for composite materials due to its higher elongation at break of
some time. Since thermoplastics harden quickly when the over 10%.
temperature drops, pull-off speeds of up to Hemp is a fiber plant that has been known for a long time
and, as a result of the previous ban on cultivation in Germany
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14 C. Gensewich, U. Riedel

mostly cultivated in Eastern European countries. In the sets a lower belt weight. In the ring spinning process,
past, hemp was used, for example, to make ropes and the fibers are spun into a roving with a slight twist and
transport bags because of its high strength. In addition then into a yarn
to fiber composite technology, more recent applications with.

include use in the area of insulating materials, since In composites, the fibers must be completely enclosed
plant fibers have better moisture-regulating properties by the matrix in order to achieve good transmission of
than mineral wool. the shear stresses between the fibers across the matrix.
Due to its relatively high price, ramie is only used in Excessive twisting of the fibers in the yarn is a
small quantities in the textile industry as a mixed hindrance, since the inner fibers of the yarn are shielded
component in cotton yarns. Due to the cultivation of the from the outer ones and are therefore not wetted. In
plants in the Far East, only a very small influence can addition, the twisting results in a reduction in the
be exerted on the fiber processing, so that the fiber modulus of elasticity, which has a negative effect on
properties cannot be adapted for use in composite the rigidity of the component.
materials. With a lightly twisted roving, the reduction in stiffness
The most common natural fiber after cotton is less than with fine yarn, while yarn strength sufficient
Flax, from which high-quality clothing and home textiles for the process and good impregnation are achieved.
are made. The cultivation and processing of flax takes
place in Central Europe, so that the fiber properties A cheaper alternative to roving are card slivers or
can be influenced by the use of different processing draw frame slivers manufactured in the spinning mill
techniques. In addition, flax fibers are easier to break by stretching the card slivers.
down and are therefore finer than hemp fibres, so that Since the dry tensile strength of the tapes is very low
flax has so far been preferred for use in fiber composite due to the lack of twisting, they can tear during
structures. processing and thus disrupt production.
So that flax fibers can be used in pultrusion to The fiber material is also not as uniform as in the roving,
produce profiles, when selecting a semi-finished so that there can be fluctuations in the fiber volume
product, attention must be paid to sufficient dry tensile content of the composite profile.
strength, adjustability of the fiber volume content and To produce the fleece, the tow is fed through a cutter
good impregnation properties. Since the preparation either in a tangled or parallelized form and cut to a
from the plant to the yarn is carried out in several length of around 60 mm.
steps, these different processes result in different semi- The fibers are then laid mechanically or aerodynamically
finished fiber products. to form a fleece.
When the flax plants have reached maturity, they are A schematic representation of the steps in flax
pulled up and laid out in the field to roast. The cement processing is shown in Scheme 1.
substances that connect the bast to other parts of the An interesting possibility is offered by the lyocell fiber
plant are broken down by bacteria. Depending on the produced from regenerated cellulose in a new process,
weather, this process is completed after three to five in which the properties can be varied via the process
weeks so that the mechanical digestion can begin. parameters. In contrast to natural fibers, it is a
When harvesting green flax, there is no need for field continuous fiber that can be processed into rovings or
roasting and the plants are sent directly to processing fleece. The fineness of the rovings can be adjusted by
after drying. the number of spinnerets, as with glass fiber rovings.
Therefore, when using Lyo cell, the pultrusion process
The mechanical separation of the fibers from the rest is similar to glass fiber processing (Fig. 7).
of the plant occurs through breaking and vibrating.
When breaking, the plant is buckled by corrugated The use of natural fibers that have been spun into an
rollers so that the fibers are exposed and the first endless yarn or lyocell filaments necessitate only a few
impurities are detached from the bast. The broken changes to the structure of the pultrusion plant. As
plants are guided past oscillating turbines, which comb with GRP pultrusion, the fiber spools are stored on
the wood and short fibers, the so-called tow, out of the shelves from which they are guided to the impregnation
fiber bundle. After hacking, a card sliver is produced tool via guide devices.
from the long fibers obtained.
The tow fibers freed from the shives are also processed
into a card sliver by being parallelized
tet. 3.2 Matrixsysteme
In order to get from a voluminous ribbon to a fine Offer as an alternative to the plastics commonly used today
yarn, the ribbons are stretched so that a matrix systems made from renewable raw materials.
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Pultrusion of construction materials 15

Scheme 1: Simplified schematic representation of flax processing according to 4, 5)


(bold: semi-finished fiber products that can be used in pultrusion).

Fig. 7. Manufacturing process of lyocell fibers according to3).

If these resins are used, a composite material is created Fig. 8. Specific characteristic values of the profiles made of fibers
based on renewable raw materials and a petrochemical matrix
which, when burned, releases the same amount of CO2 normalized to GRP with 50% fiber volume content in a tensile test.
as the plants absorbed during their growth.

The profiles currently being manufactured were made 4 Properties of the profiles
with thermoplastics made from renewable raw materials Profiles were made from various natural fibers using the
and duroplastics, some of which consist of renewable matrix systems listed above. In order to be able to
raw materials. A petrochemical matrix was also used for compare the properties of the profiles with GRP, the
comparison. characteristic values of the NRP test bodies were recorded
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16 C. Gensewich, U. Riedel

has a higher tensile strength when wet than when dry.

When using the matrix, which is partly based on


renewable raw materials, Fig. 9 shows a similar course
for flax fiber composites, but at a lower level. In the case of
the lyocell fibers, the characteristic values increase
compared to the pultrudates that were manufactured with
the petrochemical matrix.
Fig. 10 shows the characteristics of flax and hemp
embedded in a thermoplastic made from renewable raw
materials. In the case of the moistened samples, the
strength drops because the matrix is particularly sensitive
to moisture. Hemp also shows the high e-modulus of the
fiber in the composite, which exceeds the specific values
Fig. 9. Specific characteristic values of profiles made of natural fibers
and matrix standardized on GRP with 50% fiber volume content, e.g. T.
of GRP by 14% in the dry samples.
renewable raw material base in the tensile test.

5 Summary and Outlook With the


pultrusion process, a very cost-effective manufacturing
process of fiber composite technology for natural fiber-
reinforced biopolymers could be used.

The production of profiles from natural fiber composite


materials offers great advantages in recycling compared to
the previously produced GRP profiles. They can be
recycled without any problems in a CO2-neutral manner
by thermal recycling , depending on the degradation
behavior of the matrix, biological degradability is also possible.
With a suitable choice of fiber material, the specific
properties of GRP can be surpassed.
This lightweight construction potential should be used in
Fig. 10. Specific characteristic values of the profiles made of natural fibers particular for applications in traffic engineering and in the
and a thermoplastic based on renewable raw materials standardized on furniture sector.
GRP with 50% fiber volume content in a bending test.
There is a need for research primarily in reducing the
moisture sensitivity of the composite and the associated
reduction in fiber-matrix adhesion. With further advances,
natural fibers can be used not only in cladding elements
a fiber volume content of 50% is normalized and set in
and load-bearing structures indoors, but also for load-
relation to the properties of GRP. The pultrudates were
bearing components outdoors.
stored at 50% relative humidity until saturated and then
tested. The characteristics of the dry composite are given
as comparative values.

Fig. 8 shows the characteristic values for flax and


1) W. Mu¨ller, Material and Innovation 4(5) (1991) 28–37 2) M.
Lyocell UD profiles. Here, a modulus of elasticity of 101% Flemming, S. Ziegmann, S. Roth, Fiber Composite Constructions –
of the GRP value is measured for the flax composite Fibers and Matrices, Springer Verlag, Berlin (1995)
samples stored at 0% relative humidity. At 50% rel. 3) N. N., Courtaulds Lyocell – Technische U¨ bersicht, Cour taulds
moisture, the modulus of elasticity drops to 71%. The Fibres (1997)
4) DIN 60011: Flax fiber, processing stages, (October
same behavior can be seen with the lyocell fiber composite 1958)
profiles. The strength of the flax composite, on the other 5) DIN 60012: Operations in the flax spinning mill (October
hand, increases with higher humidity, since the flax fiber in the 1958)

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