Composite Structures 54 (2001) 355±360

www.elsevier.com/locate/compstruct

Thermoplastic pultrusion of natural ®bre reinforced composites

Kathleen Van de Velde *, Paul Kiekens
Department of Textiles, Ghent University, Technologiepark 9, B-9052 Zwijnaarde, Belgium

Abstract
Thanks to the good mechanical properties and the ecological and environmental advantages, the natural ®bre ¯ax o€ers good
opportunities as a reinforcement material for composites, especially thermoplastic ones. One technique for the manufacture of
composites on a continuous basis is pultrusion. This paper describes the possibility of the use of ¯ax as reinforcement in ther-
moplastic pultruded composites. Ó 2001 Elsevier Science Ltd. All rights reserved.

Keywords: Thermoplastic pultrusion; Natural ®bre reinforced composites

1. Introduction 2. Thermoplastic pultrusion

Natural ¯ax ®bre o€ers good opportunities as a re-
inforcement material for composites thanks to the eco-
logical and environmental advantages and the attractive
mechanical properties. The production of ¯ax ®bre re-
inforced thermoplastic composites also might o€er an
interesting economic potential.
The composites industry has known a continuous
growth and will continue to extend its market in the next
millennium. However, it is foreseen that a move towards
thermoplastic composites will occur thanks to their
bene®ts over thermosets. The control of environmental
pollution, the high performance properties and the re-
cycling opportunity make thermoplastic composites
very attractive.
The strongest growth of any composites industry
sector is found in pultrusion, an established process for
the manufacture of both standard and custom pro®les.
Pultruded composites are traditionally manufactured
using thermosetting resin systems. Over the last few
years, the pultrusion of solvent free thermoplastic
composites has shown the ability of becoming a major
new force in the pultrusion industry.
The combination of thermoplastics and renewable
natural ®bres such as ¯ax ®bres as reinforcement in
composites will answer the demand for environmentally
friendly materials.
*
Corresponding author. Tel.: +32-9-264-5741; fax: +32-9-264-5846.
E-mail address: kathleen.vandevelde@rug.ac.be (K. Van de Velde).
2.1. Thermoplastic versus thermoset pultrusion
The rapidly expanding usage of composite compo-
nents in automotive, construction, sports and leisure
and other mass production industries has focused at-
tention on continuous production techniques. One
technique for the manufacture of structural pro®les
from composites on a continuous basis de®nitely is
pultrusion.
Pultruded composites are traditionally manufactured
using thermosetting resin systems. These pro®les are
produced by pulling a carefully speci®ed mass of wetted-
out reinforcement material through a heated metal die
containing a cavity of the desired cross-section. A
scheme of the thermoset pultrusion process is given in
Fig. 1.
The widely used thermosetting resin systems, such as
polyester resin are regarded as hazardous substances;
they require careful precautions for the storage, han-
dling and use of these materials if the risk of ®re and ill
health arising from exposure are to be avoided. In the
last few years, pultrusion of solvent free thermoplastic
composites (see Fig. 2) has shown the ability of be-
coming a major new force in the pultrusion industry.
Di€erent techniques can be used. Prepregs (e.g. hy-
brid yarns, pre- impregnated tapes, interweaved pre-
pregs) can be shaped and consolidated in the die, which
has a ®nal cooling zone. The impregnation of the rein-
forcement ®bres with the polymer can be done in line by
e.g. hot melt application and ¯uidised bed application.
Alternatively, the molten polymer can be screw-injected

0263-8223/01/$ - see front matter Ó 2001 Elsevier Science Ltd. All rights reserved.
PII: S 0 2 6 3 - 8 2 2 3 ( 0 1 ) 0 0 1 1 0 - 6
356 K. Van de Velde, P. Kiekens / Composite Structures 54 (2001) 355±360
Fig. 1. Conventional thermoset pultrusion process.
Fig. 2. Thermoplastic pultrusion process.
into the die cavity as if it were a liquid catalysed ther-
moset resin. The major areas of concentration for
thermoplastic pultrusion are the method of material
impregnation, preheating e€ects and die con®guration
for sucient compaction and resin ¯ow.
Thermoplastic matrices o€er high performance
properties compared to thermosetting matrix resins.
Thermoplastics are attractive thanks to their superior
toughness and impact resistance, their post-process
formability and improved repairability. Even tenfold
higher production rates for thermoplastic pultrusion
over thermosets seem possible. Thermoplastic pultruded
composites generally have a lower weight than the con-
ventional thermosets resulting in a more straightforward
and safer handling of the materials. Transportation is
easier and cheaper due to the lower energy costs. Ther-
moplastic pultrusions can live a second life as chopped
and moulded ®bre reinforced thermoplastics [1±13].
2.2. Thermoplastic pultrusion line
A thermoplastic pultrusion line has been developed
and designed at the Department of Textiles, University of
Ghent, Belgium. Flax ®bre reinforced thermoplastics as
well as glass ®bre reinforced composites can be pultruded
[14,15]. In the literature, few references of pultrusion with
natural ®bres are found [16]. A pultrusion line with dif-
ferent devices namely the creel, the reinforcement guides,
the heating system, the die, the cooling system, the pulling
device and the cut-o€ saw was designed, developed and
built. Following points were considered:
· Infeed of the material (guidance devices).
· Preheating is necessary to enhance the resin impreg-
nation into the ®bre bundles; the melt viscosity of
the thermoplastic resin should be as low as possible.
The required length and temperature of preheating
depend on the resin, the amount of reinforcing mate-
rial, the initial material temperature, and the pulling
speed. Drying of the reinforcement ®bres also takes
place while preheating. The temperature sensibility
of natural ®bres has to be taken into account when
they are used as reinforcement.
· The con®guration of the die is also an important fac-
tor in the pultrusion process. The purpose of a pul-
trusion die is to consolidate the resin/®bre mass to a
state where a uniform distribution of ®bres exists
within the resin matrix. To do this, a heated die must
be designed to create adequate pressure build-up as
the resin/®bre mass progresses through the die with
the die being long enough for sucient resin ¯ow.
· A cooling device. In contrast with pultrusion for ther-
moset resins a cooling device is necessary for thermo-
plastic pultrusion to ensure a dimensional stable end
product.
The outline of the thermoplastic pultrusion process is
given in Fig. 3.
The textile structures from the creel can be preheated
before entering the die to ensure the impregnation of the
reinforcing material with the thermoplastic matrix. In
the mean time, drying of the input material takes place.
Shaping and consolidation of the material take place in
the die. The die has di€erent heating zones and a ®nal
 K. Van de Velde, P. Kiekens / Composite Structures 54 (2001) 355±360 357

Fig. 3. Developed thermoplastic pultrusion process.

Fig. 4. Density of thermoplastic matrices. Fig. 6. Tensile strength of thermoplastic matrices.

Fig. 5. Process temperature of thermoplastic matrices. Fig. 7. Tensile strength of thermoplastic ®bres.

cooling zone. The pulled materials are sawn to an ap-

propriate length.

3. Materials

3.1. Thermoplastic matrix

Several thermoplastics were compared as far as their

characteristics are concerned. From them two or three
thermoplastic matrices were selected as candidates for
thermoplastic pultrusion. Processability, mechanical
properties, availability and cost were used as the selec-
tion criteria. The thermoplastic polymers that are
screened are polypropylene (PP), poly(etheretherketone)
(PEEK), polyvinylalcohol (PVA), polybutylene tere-
phthalate (PBT), polyethylene terephthalate (PET),
polyphenylenesulphide (PPS), polyetheneimide (PEI),
Fig. 8. E-modulus of thermoplastic matrices.
polyamideimide (PAI), polyacetal (acetal), polyamide 6
(PA-6), polyamide 6,6 (PA-6,6), polycarbonate (PC),
low-density polyethylene (LDPE), high-density poly-
ethylene (HDPE), poly(lactic acid) (PLA), polycapro-
lacton (PCL) and polycaprolactam. A schematic
overview of some properties (density, process tempera-
358 K. Van de Velde, P. Kiekens / Composite Structures 54 (2001) 355±360
Fig. 9. Flexural modulus of thermoplastic matrices.
Fig. 10. Notched Izod for thermoplastic matrices.
Fig. 11. Water absorption of thermoplastic matrices.
ture, tensile strength, tensile modulus, ¯exural modulus,
notched Izod impact strength and water absorption) of
the thermoplastic resins is given in the following ®gures
(Figs. 4±11). A schematic overview of the tensile
strength of the ®bres is also given.
Based on processability, properties, availability and
costs, the choice of common thermoplastics for pultru-
sion from among those mentioned would be polyethyl-
ene terephthalate and polypropylene. Polypropylene has
Table 1
Properties of ¯ax ®bre
+ 
Renewable raw materials Fast absorption/desorpion of water
High strength and elastic modulus Good thermal conductivity
Low density Biodegradability
Non-abrasive
Low sensitivity against fracture
No skin irritations
Leaves no residues when incinerated
the lowest density, absorbs least water and is the
cheapest. Polypropylene can easily be processed because
of the low melting and process temperature, whereas
polyethylene terephthalate requires a higher process
temperature but o€ers better temperature resistance.
Other possible thermoplastics, except for their cost, are
polylactic acid and acetal. The biodegradable poly-
hydroxybutyrate is also a valuable candidate for ther-
moplastic pultrusion, but is hardly available.
3.2. Reinforcement material
At present, mainly glass-, aramide- and carbon ®bres
are used as reinforcement material for composites.
Glass is mostly used as reinforcement material for
composites in a broad area of applications as a result of
the good mechanical properties and the quality/price
ratio. Glass is incombustible and this can be a minus
point for its use. One of the main disadvantages of glass
is the occurrence of health problems when handling
glass ®bres.
The use of natural ®bres can overcome this. A natural
alternative for the broadly used reinforcement ®bres is
the ¯ax ®bre. The advantage of the natural material ¯ax
in comparison with synthetic materials is that an inex-
haustible and renewable source is available, as it can be
harvested each year again and in a way that is ecologi-
cally justi®ed. The ¯ax ®bre can be recycled (e.g. waste
during production). Another advantage related to the
environment concerns the biological degradability of
¯ax. In case the ¯ax is burnt after having been used, no
residues remain [17±20]. Moreover, ¯ax is one of the
longest and strongest natural ®bres which exist, it is a
light ®bre and has a low cost. These are some interesting
advantages of ¯ax, which give it a competitive position
in relation to the traditional use of glass as reinforce-
ment material in composites. Therefore it seems possible
to realise a partial product diversi®cation from glass to
¯ax in certain areas of application of composites.
An overview of the speci®c properties of the natural
®bre ¯ax is given in Table 1.
In Table 2 some mechanical characteristics of sisal,
¯ax [21] and hemp are compared with glass ®bres.
Once natural ®bres and in this case ¯ax ®bres are
chosen as a reinforcing material, it has to be taken into
)
Thermal resistance
Quality di€erence
 K. Van de Velde, P. Kiekens / Composite Structures 54 (2001) 355±360 359

Table 2
Properties of natural ®bres and glass ®bre
Properties Sisal Flax Hemp E-glass
Tensile strength (MPa) 610 900 690 2300
Elastic modulus (GPa) 28 50 64 73
Elongation at break (%) 2.2 1.8 1.8 3.2
Density (g=cm3 ) 1.3 1.5 1.45 2.6
Speci®c strength (MPa/r) 470 600 476 880
Speci®c strength (cN/tex) 47 60 48 88
Speci®c sti€ness (GPa/r) 22 33 44 28
Speci®c sti€ness (N/tex) 22 33 44 28
Cost price (US$/kg) 1.2±1.75 1.5±5

account that the ®bre properties are in¯uenced by many
factors such as:
· cultivation: variety, climate, harvest, maturity, retting
degree;
· processing: decortication, disintegration (mechanical,
steam explosion treatment);
· ®bre modi®cation, textile and technical processes
(carding, spinning, etc.).
Both green and retted ¯ax can be used as reinforcement
material in composites. In comparison with retted ¯ax
®bres, green ¯ax shows more cohesion. The ®bres are
rougher, have a higher polarity and better mechanical
properties. The adhesion between green ¯ax ®bres and
polar matrices can be better than with retted ¯ax ®bres.
On the other hand, green, unretted ¯ax ®bres are more
sensitive to degradation.
3.3. Hybrid textile structures
By developing hybrid textile structures the impreg-
nation of the ®bres by the thermoplastic polymer and
the adhesive properties have to be taken into account.
The orientation of the reinforcement ®bres and the
volume percentages have to be considered. Actually
core-spun and commingled yarns of ¯ax/PP are devel-
oped. Other hybrid textile structures consisting of ther-
moplastic ®bres and ¯ax ®bres are under development.
Pultrusion test runs were done with ¯ax/PP
commingled yarn 2000 tex 50/50 w% (38/62 V%)
and glass/PP rovings Twintexâ 1500 tex 75/25 w%
(50/50 V%).
3.4. Pultruded composites
Round ¯ax/PP pro®les (£ 5 mm) and rectangular
glass/PP pro®les (side 5 mm) are made. The input ma-
terials are commingled ¯ax/PP yarns (38/62 V%) and
glass/PP rovings (50/50 V%). For the ¯ax/PP yarn a
maleic acid anhydride modi®ed polypropylene ®bre is
used. The measured density of the composites is, re-
spectively, 0:80  0:04 g=cm3 and 1:48  0:01 g=cm3 .
The ¯ax/PP pro®les are not free from voids. They also
have a lower reinforcement percentage than the glass/
PP composites. Some characteristics are given in
Tables 3±6.
The speci®c sti€ness properties of the ¯ax/PP pro®les
are good. Strength properties have to be improved by
optimisation of the impregnation of the reinforcement
®bres with the thermoplastic matrix. Besides this,
physico-chemical treatments of the ®bres and/or the use
of modi®ed thermoplastic polymers will a€ect the in-
terphase and the mechanical properties.
Optimisation of the materials and the thermoplastic
pultrusion process is currently in progress.

Table 3
Flexural properties of ¯ax/PP pro®les
P (N) r …N=mm2 † r (N m/g) Strainmax :F (%) Eb …N=mm2 † Eb (N m/g)
Mean 22 101 126 1.9 14 380 17 980
S.D. 2 14 18 0.3 2210 2760
CV 10 14 14 13 15 15

Table 4
Flexural properties of glass/PP pro®les
P (N) r …N=mm2 † r (N m/g) Strainmax :F (%) Eb …N=mm2 † Eb (N m/g)
Mean 165 335 226 1.2 28 800 19 460
S.D. 7 13 9 0.05 1200 810
CV 4 4 4 5 4 4
360 K. Van de Velde, P. Kiekens / Composite Structures 54 (2001) 355±360

Table 5
Tensile properties of ¯ax/PP pro®les
Fm (N) r …N=mm2 † r (N m/g) Strainmax :F (%) E …N=mm2 ) E (N m/g)
Mean 2117 145 181 1,4 15 190 18 980
S.D. 126 8 9 0,1 870 1090
CV 6 5 5 6 6 6

Table 6
Tensile properties of glass/PP pro®les
Fm (N) r …N=mm2 † r (N m/g) Strainmax :F (%) E …N=mm2 † E (N m/g)
Mean 12 158 515 348 1,6 33 460 22 610
S.D. 627 27 18 0,1 1870 1260
CV 5 5 5 7 6 6

4. Conclusion [8] Klinkm uller V, Friedrich K. Pultrusion of GF/PBT powder-

The natural ¯ax ®bre o€ers good opportunities as a
reinforcement material for composites thanks to the
good mechanical properties and the ecological and en-
vironmental advantages. One technique for the manu-
facture of composites on a continuous basis is
pultrusion. Thermoplastic pultrusion has shown the
ability of becoming a major new force in the pultrusion
industry. The development of ¯ax ®bre reinforced
thermoplastic pultruded composites may answer the
need to environmentally friendly continuous reinforced
pro®les.
References
[1] Larock JA, Hahn HT, Evans DJ. Pultrusion processes for
thermoplastic composites. In: 44th Annual Conference, Compos-
ites Institute, The Society of Plastics Industry, 1989 February 6±9,
session 8-A.
[2] Trevor FS. Composites: a pro®le of the worldwide reinforced
plastics industry. England: Elsevier; 1995.
[3] Maywood LW, John DB. The potential for low cost thermoplastic
pultrusion. J Reinforced Plastics Compos, 1994.
 om BT. Experimental investigation of thermoplastic pultru-
[4] Astr
sion: a manufacturing method with economic potential. In:
Presented at Verbundwerk '92, Wiesbaden, Germany, 1992 July
1±3.
[5] Saeys A, Vangheluwe L, Van de Velde K. Thermoplastische
pultrusie zet composieten in het verlengde van Textiel. In: Paper
presented at `Nieuwe Produkten, Nieuwe Produktietechnologie
voor een Nieuwe Textielindustrie 1995', So®tel Ghent, 1995 July 6.
[6] Kiekens P, Van de Velde K, Saeys A. Thermoplastic pultrusion: a
challenge for the composites industry. In: ICCE/4 (4th Interna-
tional Conference on Composites Engineering), 1997 July 6±9;
Hawaii.
[7] Klinkm uller V, Friedrich K. Pultrusion of ¯exible, continuous
glass ®bre/thermoplastic powder impregnated bundles. In: Comp
95 Symposium, 1995 September 18±22; Korfu, Greece.
impregnated ®bre bundles, Adv Compos 1994:222.
[9] Michaeli W, J urss D, Blaurock J. Development of a process
technology for powder impregnation of reinforcement ®bres for
the thermoplastic pultrusion process. Techtextil Symposium, lect.
321, 1995.
[10] Devlin BJ, Williams MD, Quinn JA, Gibson AG. Pultrusion of
unidirectional composites with thermoplastic matrices. Compos
Manufacturing 1991;2(3/4):203.
[11] Loubinoux D, Nemoz G. Pro®les pultrudes thermoplastiques a
renforts ®lamentaires continus. Text Compos Building Construc-
tion 1990;3:259.
[12] Miller AH, Dodds N, Hale JM, Gibson AG. High speed
pultrusion of thermoplastic matrix composites. Composites, Part
A 1998;29A:7:773±782.
[13] Carlsson A, Astrom TB. Experimental investigation of pultrusion
of glass ®bre reinforced polypropylene composites. Composites,
Part A 1998;29A(5±6):585±93.
[14] Van de Velde K, Van Langenhove L, Kiekens P. Research on the
use of ¯ax as reinforcement for thermoplastic pultruded compos-
ites. Nord¯ax I, Tampere, 1998 August 10±12; Finland.
[15] Van de Velde K, Kiekens P, Thermoplastic pultrusion of natural
®bre reinforced composites. SACAM 2000, International Confer-
ence on Applied Mechanics. In: Proceedings of the 3th Interna-
tional Conference on Composite Science and Technology,
Durban, 2000 Janunary 11±13; South-Africa. p. 381±8.
[16] Gensewich C, Riedel U. Pultrusion von konstruktionswerksto€en
aus nachwachsenden rohsto€en. Die Angewandta Makromoleku-
lare Chemie 1999;272:11±6.
[17] Kohler R, Wedler M. Non-Textile Applications of ¯ax ®bres.
Techtextil Symposium 1994, lecture 331.
[18] Mieck KP, Nechwatal A, Knobelsdorf C. Application of natural
®bres in composites. Techtextil Symposium 1993, lecture 311.
[19] Cruz-Ramos CA. Natural ®ber reinforced thermoplastics. In:
Clegg DW, Collyer AA, editors. Mechanical Properties of
Reinforced Thermoplastics. The Netherlands: Elsevier; 1986.
[20] Liljedahl S, Smeder B. Barriers in the development of non-textile
¯ax ®bre applications. Flax in the World, Workshop in Bonn,
Germany, 1993 June 15±17.
[21] Study on production of thermo-bioplastics and ®bres based
mainly on biological materials. European Commission, Science,
Research and Development 1994. p. 89.