Industrial Crops and Products 8 (1998) 105 112

Influence of natural fibres on the mechanical properties of

biodegradable polymers

Martina Wollerdorfer a,*, Herbert Bader b

a
Institute for Agrobiotechnology, Department of Natural Materials and Packaging Technology, Konrad Lorenz Strae 20,
3430 Tulln, Austria
b
Fraunhofer Institute for Food Technology and Packaging, Department of Materials De6elopment, Giggenhauserstrae 35,
85354 Freising, Germany

Received 17 July 1996; accepted 3 October 1997

Abstract

Fibre reinforced plastics are used whenever there is the need for very high mechanical properties combined with low
weight. In that respect natural fibres are of basic interest since they not only have the functional capability to
substitute the widely used glass fibres but they also have advantages from the point of view of weight and
fibrematrix adhesion, specifically with polar matrix materials. They have good possibilities in waste management due
to their biodegradability on the one hand and their much lower production of ash during incineration on the other.
The influence of plant fibres such as flax, jute, ramie, oil palm fibres and fibres made from regenerated cellulose on
the mechanical properties of biodegradable polymers was investigated using thermoplasts like polyesters, polysaccha-
rides and blends of thermoplastic starch. The composites were produced by extrusion compounding with a co-rotating
twin screw extruder. The pellets obtained were further processed into tensile test bars by injection moulding.
Depending on the kind of polymer, a fibre content of 20 35% could be achieved. Generally a considerable tensile
strength improvement of polyesters could not be observed. However the chemical similarity of polysaccharides and
plant fibres, which consist mainly of cellulose, resulted in an increased tensile strength of the reinforced polymers. For
reinforced thermoplastic wheat starch, it was four times better (37 N/mm2) than without fibres. The reinforcement of
cellulose diacetate and starch blends caused a stress increase of 52% (55 N/mm2) and 64% (25 N/mm2), respectively.
1998 Elsevier Science B.V. All rights reserved.

Keywords: Fibre reinforcement; Composite material; Plant fibres; Biodegradable polymers

* Corresponding author. Tel: +43 2272 66280306; fax: + 43 2272 66280303; e-mail: woller@ifa1.boku.ac.at

0926-6690/98/$19.00 1998 Elsevier Science B.V. All rights reserved.

PII S0926-6690(97)10015-2
106 M. Wollerdorfer, H. Bader / Industrial Crops and Products 8 (1998) 105112
1. Introduction
Fibre reinforced polymers, specifically with
glass fibres, have gained importance in technical
applications such as the automotive sector,
where high mechanical properties and dimen-
sional stability have to be combined with low
weight. During the last few years many efforts
have been made to investigate the suitability of
natural fibres as a reinforcing component for
thermoplastic and injection mouldable materials
because of their low density and ecological ad-
vantages. They open up further possibilities in
waste management as they are biodegradable
and therefore can lead to highly functional com-
posite materials if used in combination with
biodegradable thermoplastic polymers.
The current biodegradable polymers may be
divided into synthetic and natural polymers,
while the latter are classified into those of plant
and microbial origin (Endres and Pries, 1995).
The degradation of such polymers includes the
disintegration into their monomers. Therefore
unstable and hydrolyzable linkages are required,
where chemical, biological or photochemical re-
actions take place. Some polyesters (e.g. poly-b-
hydroxybutyrate) and polysaccharides like
thermoplastic starch or modified cellulose are
well suited for that purpose. On the one hand,
water solubility raises the degradability, but on
the other, in most cases a water-resistant mate-
rial should be obtained for most applications.
This problem can be avoided by blending such
soluble polymers like thermoplastic starch with
insoluble polyesters which additionally show
very good manufacturing properties (Fritz et al.,
1995).
As these materials have limited mechanical
properties for several applications, an increase
of tensile strength can be achieved by com-
pounding them with fibres provided that the
fibres show a higher tensile strength and
Youngs modulus and a lower elongation than
the matrix (Ehrenstein, 1992). The quality of a
fibre reinforced composite depends considerably
on the fibrematrix interface because only a
well formed interface allows stress transfer from
the matrix to the fibre. The extent of the adhe-
sion between fibre and matrix can be described
by the critical fibre length resulting from the
balance of interface shear force and normal
force in the fibre. Sufficient adhesion, low fibre
diameter and high tensile strength allow short
critical fibre lengths. The maximum tensile
strength of fibres can only be exploited if they
can be stressed until they break without being
pulled out. The critical fibre length can be esti-
mated by the surface of fracture since the aver-
age pull out length of a fibre cannot be longer
than half of the critical fibre length. This is im-
portant during extrusion compounding and in-
jection moulding when fibres are shortened
considerably. The tensile strength of the com-
posite is proportional to the volume fraction of
fibres assuming that the orientation of the fibres
and the direction of the applied stress are paral-
lel (Voss, 1987; Gachter and Muller, 1989).
Because of their static function in plant tis-
sues, bast (e.g. flax, ramie, jute or hemp), leaf
(e.g. sisal) and fruit fibres (e.g. cotton) are also
expected to act as reinforcing components in
composite materials. Information concerning the
mechanical properties of fibres can be found in
the literature. The tensile strength of flax ranges
from 254390 N/mm2 (Folster and Michaeli,
1993) to 1100 N/mm2 (Flemming et al., 1995),
that of jute varies between 187 N/mm2 (Hinrich-
sen, 1991) and 533 N/mm2 (Flemming et al.,
1995). Ramie has a very high tensile strength at
850900 N/mm2 (Hock, 1995). There are several
advantages of plant fibres in comparison to cus-
tomary glass or carbon fibres. Besides their low
density they reduce the abrasion of screw and
barrel and the energy input for distributing
them in the polymer melt. The low sensibility
against mechanical treatment results in longer
fibres. Finally the biodegradability of this renew-
able raw material is important (Kohler and
Wedler, 1994; Mieck and Reumann, 1995).
While processing plant fibres, their thermal sta-
bility is limited to temperatures below 200C.
One problem that arises is the high variation of
mechanical properties due to climatic and grow-
ing conditions, the different preparation meth-
ods and water adsorption (Flemming et al.,
1995).
 M. Wollerdorfer, H. Bader / Industrial Crops and Products 8 (1998) 105112 107

2. Materials and methods 3030 and Rokramar VP 1681) were obtained from
Robert Kraemer (Delmenhorst, Germany).
2.1. Matrix polymers and fibres
2.2. Compounding of thermoplastic starch (TPS)
Available polyesters, polysaccharides and
During the high-temperature short-term reac-
blends of thermoplastic starch were selected for
tion in an extruder, partly crystalline starch gran-
the experiments. Polybutylene succinate adipate
ules can be converted into a homogeneous plastic
copolymer is a biodegradable, aliphatic polyester
matrix. The degree of conversion is determined by
(Bionolle, type 3020, Showa Highpolymer,
the mechanical shear, the thermal stress as a
Tokyo). The poly-b-hydroxybutyrate copolyester
function of temperature and time and the content
(Biopol D300G) was obtained from Zeneca Bio
of water and other plasticizers for adjusting the
Products (Billingham, UK). Cellulose diacetate
glass transition temperature (Wiedmann and Stro-
(Biocell 163) was supplied by Tubize Plastics
bel, 1991).
(Groupe Rhone-Poulenc, Belgium). For the pro-
The plastification of starch was carried out with
duction of thermoplastic starch (TPS), wheat
a co-rotating twin screw extruder (Leistritz, type
starch (Definol WN) from Crespel and Deiters
LSM 30.34, Germany) at 115C and 50 rev./min.
(Ibbenburen, Germany) was plastified with sor-
The screws with a diameter of 34 mm and a L/D
bitol (DHW Deutsche Hydrierwerke Rodleben,
ratio of 26.47 were equipped with kneading ele-
Rolau/Elbe, Germany) and glycerol (Fauth,
ments. To prevent the plastified starch from ex-
Mannheim, Germany). Commercially available
panding at the nozzles, surplus steam was
thermoplastic starch blends used in this study
removed with a degassing zone operating at atmo-
were Bioplast GS 902 (Biotec, Emmerich, Ger-
spheric pressure. After leaving the nozzles with a
many), a blend consisting of potato starch,
diameter of 2 mm, the extrudate was pelletized.
modified cellulose and synthetic polymers, and
Investigations have shown that the thermal
Mater-Bi, type ZI01U (Montedison Deutsch-
stress can be reduced by increasing the water
land, Eschborn, Germany). This blend consists of
content of starch to 22%its maximal equi-
corn starch and a biodegradable polyester. A
librium moisture content. Glycerol (86% in water)
further starch blend was produced by compound-
and sorbitol were identified as the most suitable
ing thermoplastic wheat starch with 40% poly(e-
plasticizers (Utz et al., 1994). The mixing ratio of
)caprolactone (PCL) of the type Tone Polymer
sorbitol and moist starch was 1:6.4. About 13%
P-787 from Union Carbide Benelux (Antwerp,
glycerol was added to get a well disintegrated
Belgium).
thermoplast.
Flax and jute were delivered as long fibres from
Fuessener Textil (Fuessen im Allgau, Germany) 2.3. Fibre compounding
Jute-Spinnerei and Weberei Bremen (Delmen-
horst, Germany), respectively. The ramie fibres For compounding the fibre reinforced com-
with a length of 12 mm were obtained from posites, the same extruder was equipped with a
Fischer Doticon (Switzerland). Oil palm fibres are 4-mm nozzle and a new screw configuration. The
a by-product of the palm oil industry. They were kneading elements were substituted by transport
supplied by the Palm Oil Research Institute of elements to minimize the shearing of the fibres.
Malaysia. Long fibres made from regenerated cel- Because of the low bulk density an automatic
lulose were delivered from Lotteraner Wustner dosing of the fibres was impossible so the fibres
(Mellau, Austria). had to be fed manually. The resins were pulver-
As resins are usually used as bonding agents for ized and mixed with the polymer pellets. The
glues and varnishes they also seemed to be suited temperature profile along the extruder barrel was
to improve the fibre matrix interface. The ap- adjusted according to the requirements of the
plied resins based on colophony (Kolophonium) different polymers. The screw rotation speed was
and maleinate-modified colophony (Rokramar 50 rev./min.
108 M. Wollerdorfer, H. Bader / Industrial Crops and Products 8 (1998) 105112

Table 1
Processed polymer-fibre composites with the fibre content in % (w/w)

Flax Ramie Jute Oil palm fibre Cellulose fibre

Polyesters
Bionolle 25 25 25 25 25
Biopol 25a 25
Polysaccharides
Biocell 15/25/35 25 25
TPS 10/15a/20 15
Starch blends
Bioplast 15/25/35 15
Mater-Bi 15/20/25 15
TPS/PCL 15 15

a
These compounds have also been alloyed with resins.

The pellets were processed into tensile speci- the method suggested by Thieltges (1991), the
mens according to DIN 53455 by injection mould- matrix polymer was dissolved in suitable solvents
ing (Boy 50M, Germany). The following over several days at a temperature of 70C: water
parameters were adjusted for the various compo- for TPS, acetone for Biocell and ethylacetate for
sitions: temperature profiles, injection and cooling Bionolle. The fiber suspension produced was dis-
time, mould temperature and pressure. tributed on an object slide of a microscope. Com-
Table 1 shows the processed compounds with puter aided measurements were carried out on 150
their fibre contents in % (w/w). These combina- fibres of each sample.
tions of polymers and fibres were investigated
regarding their compatibility and reinforcing ef-
fect. This work concentrated particularly on ther- 3. Results and discussion
moplastic starch and its blends, as these are
renewable raw materials, and on flax as a Eu-
ropean fibre plant. In most cases the maximum
3.1. Mechanical properties
fibre content was restricted by insufficient distri-
Figs. 17 demonstrate the tensile strengths ob-
bution in the matrix or the limited extruder per-
tained for several fibre reinforced compounds
formance. The increasing fibre contents in some
compared to the pure matrix.
compounds should demonstrate the correlation
The tensile strength of Bionolle compounds in-
between fibre content and tensile strength.
creased only in combination with ramie. An
2.4. Analytical methods

According to DIN 53455, the tensile strength

was tested on 10 specimens after conditioning for
3 days at 23C and 50% relative humidity. The
testing machine (Schenk Trebel, type RM 50 kN,
Germany) was operated with a velocity of 100
mm/min.
The fibre length was analyzed in some selected
reinforced pellets and injection moulded speci-
mens to investigate the effect of fibre content,
processing step and matrix polymer. According to Fig. 1. Tensile strength of Bionolle fibre compounds.
 M. Wollerdorfer, H. Bader / Industrial Crops and Products 8 (1998) 105112
Fig. 2. Tensile strength of Biopol fibre compounds.
amount containing 25% fibres could be processed
quite well. With oil palm fibres, the tensile
strength decreased, basically because of the high
content of impurities leading to fractures in the
matrix. Apart from the oil palm fibre compound,
the Youngs modulus of about 460 N/mm2 could
at least be doubled. The elongation was consider-
ably reduced from 274% to about 5%.
The mechanical properties of Biopol com-
pounds behaved in a similar manner. Fig. 2 shows
that the application of the resin Rokramar 3030
gave only a negligible improvement.
Compared with a fibre content of 25%, an
increase up to 35% did not improve the tensile
strength of the Biocell 163 composite due to in-
sufficient incorporation of this high fibre amount
(Fig. 3). The elongation of 9.1% was reduced to
values between 3.0 and 4.2%. Also in this case, the
initial Youngs modulus of about 1500 N/mm2
increased by 80%. The high processing tempera-
tures of Biocell 163, ranging from 180 to 200C,
caused thermal stress on the fibres which became
apparent in combustion smell.
Fig. 3. Tensile strength of Biocell fibre compounds.
109
Fig. 4. Tensile strength of TPS fibre compounds.
Remarkable results were achieved by com-
pounding thermoplastic starch with plant fibres. It
was possible to increase the initial tensile strength
by four times up to nearly 37 N/mm2. Fig. 4
demonstrates the correlation between the content
of flax fibres and the tensile strength. The elonga-
tion was reduced from 45% to about 1.32.0%.
The Youngs modulus of thermoplastic starch
(420 N/mm2) behaved analogous to the tensile
strength as a consequence of compounding with
fibres. A higher fibre content could not be ob-
tained because of the great increase in the process-
ing viscosity. Two other kinds of resins were
tested as Rokramar 3030 was too sticky for pro-
cessing fibre composites with thermoplastic
starch. Both resulted in a significant improve-
ment. The tensile strength of compounds with
15% flax and 1% resin was the same as with 20%
fibres.
Very different results were obtained by the fibre
reinforced starch blends. The independence of the
fibre content with respect to the missing reinforce-
Fig. 5. Tensile strength of Bioplast fibre compounds.
110 M. Wollerdorfer, H. Bader / Industrial Crops and Products 8 (1998) 105112
Fig. 6. Tensile strength of Mater-Bi fibre compounds.
ment of Bioplast compounds was probably a re-
sult of incompletely disintegrated starch grains
(Fig. 5). The tensile strength of Mater-Bi rises
considerably as an effect of compounding but as
Fig. 6 shows there is no obvious increase with a
flax content greater than 15%. While the elonga-
tion decreased a little, the Youngs modulus rose
from 540 N/mm2 to about 1400 N/mm2. Apart
from the missing reinforcement by ramie, the
TPS/PCL compounds have similar properties to
those based on Mater-Bi.
3.2. Fibre length studies
Some compounds with either good or missing
reinforcing effects were selected to study the dis-
tribution of the fibre length. Figs. 8 10 demon-
strate the influence of the processing steps
extrusion and injection moulding and the fibre
content on the resulting fibre length in TPS flax
compounds. The peak becomes narrower and
shifts to fibre lengths of 101 200 mm with in-
Fig. 7. Tensile strength of TPS/PCLfibre compounds.
Fig. 8. Fibre length distribution in TPS compound with 10%
flax.
creasing fibre content. But there are hardly any
fibres which are shorter than 100 mm. The fibres
are also shortened by injection moulding. But
even these short fibres provide a considerable
reinforcing effect. Scanning electron microscopy
(SEM) images show a smooth fracture surface,
indicating that no fibres have been pulled out.
Therefore extremely short critical fibre lengths can
be assumed for this compound.
The Biocellflax compound has a similar distri-
bution but still with a peak maximum at 201300
mm (Fig. 11). The SEM image of the fracture
surface (Fig. 12) demonstrates that the critical
fibre length of this compound is about 150 mm,
but the residual fibres longer than 150 mm are
sufficient to increase the tensile strength.
Fig. 9. Fibre length distribution in TPS compound with 15%
flax.
 M. Wollerdorfer, H. Bader / Industrial Crops and Products 8 (1998) 105112
Fig. 10. Fibre length distribution in TPS compound with 20%
flax.
For the Bionolle flax compound, the wide dis-
tribution with quite long fibres (Fig. 13) may
result from the low melt viscosity of Bionolle and
thereby the low mechanical stress during the com-
pounding process. But nevertheless no reinforce-
ment is present as the critical fibre length of a few
hundred mm (Fig. 14) cannot be obtained by the
major part of the fibres.
4. Conclusion
From the material side, the fibre content is
limited by insufficient compatibility or high vis-
cosity on the one hand, and on the other by the
drastic shortening of fibres during processing. It
Fig. 11. Fibre length distribution in Biocell compound with
25% flax.
111
Fig. 12. Fracture surface of Biocell flax compound.
can be concluded that the fibre length distribution
depends in a very complex manner on the kind of
matrix polymer and its rheological properties, the
fibre content and the resulting interactions. The
results show that polyesters are not very well
suited as matrix polymers for native natural fibres
as a considerable increase of tensile strength was
not observed. On the other hand, the polysaccha-
rides and most likely starch blends appear to be
compatible matrices. The reasons are due to the
remarkable intrinsic adhesion of the fibrematrix
interface caused by the chemical similarity of such
thermoplasts and the plant fibres.
Fig. 13. Fibre length distribution in Bionolle compound
with 25% flax.
112 M. Wollerdorfer, H. Bader / Industrial Crops and Products 8 (1998) 105112
Fig. 14. Fracture surface of Bionolle flax compound.
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