Composites: Part A 40 (2009) 404–412

Contents lists available at ScienceDirect

Composites: Part A
journal homepage: www.elsevier.com/locate/compositesa

Mechanical properties of PLA composites with man-made cellulose and abaca fibres
Andrzej K. Bledzki a,*, Adam Jaszkiewicz a, Dietrich Scherzer b
a
Institut für Werkstofftechnik, Kunststoff- und Recyclingtechnik, University of Kassel, Mönchebergstr. 3, 34109 Kassel, Germany
b
BASF SE, Global Polymer Research – Biopolymers, 37056 Ludwigshafen, Germany

a r t i c l e i n f o a b s t r a c t

Article history: PLA biocomposites with abaca and man-made cellulose fibres were processed by using combined mould-
Received 10 July 2008 ing technology: two-step extrusion coating process and consecutively injection moulding. By adding
Received in revised form 19 December 2008 30 wt% of man-made cellulose, the Charpy impact strength at ambient temperature increased by factor
Accepted 2 January 2009
3.60, compared to unreinforced PLA. Tensile strength rose by factor 1.45 and stiffness by approx. 1.75.
Reinforcing with abaca fibres (30 wt%) enhanced both E-Modulus and tensile strength by factor 2.40
and 1.20, respectively. The Charpy A-notch impact resistance of PLA/abaca could be improved by factor
Keywords:
2.4.
A. Polymer-matrix composites (PMCs)
B. Mechanical properties
SEM photographs show fibre pull-outs from the polymer matrix. The fibre orientation was analysed via
E. Extrusion optical microscopy. The after-process fibre length was significantly affected already during compounding
E. Injection moulding process.
Ó 2009 Published by Elsevier Ltd.

1. Introduction choice of tailor-made reinforcing fibres is of dominant importance.

1.1. Motivation
By using biopolymers as a composite matrix some common
composites, the matrix of which is made of crude oil, can be substi-
tuted. However, to achieve high mechanical parameters, the biog-
enous matrix needs to be reinforced. By using natural fibres only, a
full ‘‘biocomposite” can be produced. One of the main advantages
of natural fibres (NF) is their ‘‘light weight potential”. Natural fibres
have a significant lower density than glass fibres (GF), which al-
lows the construction of lighter parts, compared to parts reinforced
with GF or filled with minerals.
Polylactide has still not found any meaningful market accep-
tance as an engineering resin, because of its non-satisfying impact
resistance and low heat distortion temperature. Therefore, manu-
facturing of PLA light-weight parts with a high impact resistance
would lead to new application fields, e.g. automotive or electrical
industry.
In both sectors the major engineering resin is still the PP based
composite, as its cost is low and properties are good enough. Add-
ing new biocomposites to these existing and well working material
systems requires specific fundamental basics, for example compet-
itive prices and comparable or improved mechanical properties.
Therefore, material data of biocomposites, which are in competi-
tion to PP equivalents, should reference to adequate values of poly-
propylene reinforced with natural fibres (PP NF). For this purpose a
* Corresponding author. Tel.: +49 561 804 3690; fax: +49 561 804 3692.
E-mail address: kutech@uni-kassel.de (A.K. Bledzki).
Although natural fibres showing potential as reinforcement for
composites, their properties vary depending on several factors,
such as species, grade, harvest quality and yield, etc. Only natural
fibres of technical quality guarantee sufficient reproducibility of
mechanical characteristics. Hence, composites described in this pa-
per were reinforced with abaca fibre grade, which is used in PP
compounds for under-floor covering of the Mercedes A Class.
Man-made cellulose fibres from Cordenka are well-known high-
quality technical textiles in the automobile industry (tyre cord in
high-speed tyres).
The objective of this investigation was to show the potential of
PLA short-fibres biocomposites reinforced with cellulosic fibres of
such technical quality in reference to equivalent PP NF composites.
In order to present comparable and reproducible results only injec-
tion moulded specimens were investigated.
1.2. Biopolymers
Permanent crude oil price stagflation as well as the ecological
aspect of both production and disposal of standard oil-based plas-
tics are presently two of the main concerns worldwide.
Substitute materials can be novel, renewable biopolymers. In
comparison to other common polymer groups the progress of bio-
polymers R&D, as well as their production have been the fastest for
several years [1–7]. The production capacity and the amount of
manufacturers and processors have also increased significantly
[8–13].
State of art within the biogene thermoplastic group is the
starch-based lactic family or other bio-polyesters, like

1359-835X/$ - see front matter Ó 2009 Published by Elsevier Ltd.

doi:10.1016/j.compositesa.2009.01.002
 A.K. Bledzki et al. / Composites: Part A 40 (2009) 404–412
poly(hydroxyalkanoates) (PHA) synthesised by microorganisms.
Other examples are thermoplastic starch and cellulose derivatives.
At present only few groups of the mentioned biopolymers are of
market importance [14–18]. The principal reason for the neglected
importance is their price level, which is not yet competitive –
current turnover in this field is not really profitable due to high
synthesis costs, unsatisfactory production capacity, poor and not
transparent regulations.
Until now biopolymers found market acceptance in the packag-
ing and medicine sector, but they are still underestimated as engi-
neering resins due to the poor thermo-mechanical properties.
Engineering resins are characterised by a very high stiffness and
strength as well as long-term behaviour under circular loading. To
achieve these valuable parameters a reinforced matrix is required.
Indeed, most of the common technical non-reinforced resins are
unable to meet all requirements. Additional disadvantages of these
materials are their price level and finally recycling, particularly
when being reinforced with glass fibres. Nearly all substantial
requirements can be satisfied by renewable resource based mate-
rials with natural fibres [19].
1.3. Abaca and man-made cellulose fibres
The abaca fibre is a vegetable fibre that grows rapidly. It belongs
to the family of the abaca-banana tree ‘‘musa textilis”. The Philip-
pines are the worldwide leader in the production of abaca fibres
with 85% of the market share. The abaca fibres are used in many
technical applications [20,21], mostly because of their high tensile
properties [22].
Cellulose is a basic component of plants, thus it is a nearly inex-
haustible source of raw material. Man-made or ‘‘regenerated” cel-
lulose fibres are produced in chemical–technical viscose processes,
in which raw cellulose is modified into cellulose fibres and deriva-
tives [23,24].
In the last years options for reinforcement with natural and cel-
lulose spun fibres have also been intensively researched, especially
regarding common polymers like PP, PVC or PE [25,26]. The idea of
the development deals with the combination of two inexpensive
commodity materials, polypropylene and natural fibres or Rayon-
tyre cord [27]. By combining them into a polymer composite, pro-
duction of stronger components can be achieved. In addition, it
would enter the application field of engineering materials, such
as PP-GF or PC/ABS [19,28].
1.4. Biocomposites on PLA basis
PLA biocomposites have been studied for numerous research
groups [29–34]. Pluta et al. investigated PLA/montmorillonite
micro- and nanocomposites, and showed that the microcompos-
ites have formed a phase-separation between the matrix and
reinforcement. Furthermore, nanocomposites can be very easily
processed by using nanofillers; however, the biodegradability of
the composite was affected. Moreover, the thermal stability in
oxidative atmosphere of PLA/montmorillonite could be improved
[29]. The influence of chopped glass and recycled newspaper in
PLA composites was assayed by Huda et al. With addition of
30 wt% of both fibres the stiffness rose from 3.3 GPa (origin
PLA) to 5.4 GPa by recycled newspaper fibres and to 6.7 GPa by
glass fibres. The tensile strength was improved from 62.9 MPa
(origin polymer) to 67.9 and 80.2, respectively [30]. Also wood
polymer composites (WPC) on PLA basis were studied [31]. With
addition of different contents of wood flour (WF) the flexural
strength improvement from 98.8 to 114.3 MPa could be ob-
served. The modulus of elasticity increases proportionately as
the amount of WF increases. However, the thermal stability de-
creases with the increase of WF. A study on PLA composites with
405
microcrystalline cellulose (MCC) [32] briefed that both PLA/WF
and PLA/wood pulp (WP) have better mechanical properties than
PLA/MCC. This is due to the poor interfacial adhesion of PLA and
MCC, which was observed via scanning electron microscopy. Also
a higher level of matrix crystallinity of PLA/WF and PLA/WP as
PLA/MMC could be seen. It was considered as a reason for the
improved stiffness, if compared to PLA/MCC. The influence of
cellulose reinforcement on crystallinity of PLA composites was
studied in later paper by Mathew et al. [33]. They showed
shown that MCC has better potential as nucleating agent and
causes higher degree of crystallinity like WF or cellulose fibres
which were investigated.
Biocomposites of PLA/abaca were investigated by Shibata et al.
[34]. In this research three different kinds of chemical treatment
were used: esterification, mercerization, cyanoethylation. It has
been shown that for reinforced PLA the flexural strength could
not be improved significantly, even if the fibres were treated. In
contrast the stiffness increases continuous from approx. 3.6 to
6.0 GPa, depending on the fibre content and treatment method.
The biodegradation rate of PLA/untreated abaca fibre (90/10) was
much higher, as the neat PLA and PLA/esterificated abaca fibre
(90/10). Other natural fibres used as reinforcement for PLA com-
posites were jute [35], flax [36] and kenaf [37]. The reinforcing ef-
fect of most of them brought an increase in stiffness and
sometimes in strength. The ductility of the composites was overall
worst, which resulted in lower impact strength. To improve this
drawback, some other fibrous reinforcement must be used. How-
ever, to keep the concept of ‘‘biocomposites”, the reinforcement
should be obtained from renewable raw materials, for example a
viscose fibre made of native cellulose (man-made cellulose) [26].
Ganster and Fink [28] published results of PLA/man-made cellulose
in comparison to PP composites. They reported that with addition
of 30 wt% of regenerated cellulose an improvement of most
mechanical characteristics can be achieved. The unnotched and
notched Charpy impact strength can be improved by factor 3.8
and 2.0, respectively. The modulus and strength increase to 150%
of origin PLA.
Generally in research papers about bioplastics and their com-
posites, the most described processing methods are compression
moulding, mixing or other, non-common techniques for thermo-
plastic polymers.
However, the injection moulding is in common use for thermo-
plastics; this technology was underestimated for short-fibre bio-
composites and was not systematically investigated [25,38].
2. Experimental part
2.1. Materials
The tested composites consist of polylactide matrix with natu-
ral and man-made fibres. The components were prepared at a
weight ratio of 70/30 (polymer/fibre). The matrix used is PLA
4042D, Mw = 166,000, MVR = 5.7 (190 °C/2.16 kg) manufactured
by NatureWorks LLC/USA.
Abaca fibres from Manila Cordage (with the friendly assistance
of Rieter Automotive) were processed as endless fibres (filament
yarn). The density of the fibre is 1.5 g/cm3, single fibre diameter
is 10–30 lm, tensile strength over 900 MPa [39]. The fibre quality
owing to FIDA (Fiber Industry Development Authority) is S3. Man-
made cellulose fibre (CordenkaÒ 700 Super3) from the company
Cordenka/Germany, was delivered as industrial yarn; linear den-
sity (nominal) dtex = 2440, number of filaments 1350, breaking
force 128.6 N, single fibre diameter 12 lm. All fibres were used
as delivered, without any chemical treatment; for PLA composites
no coupling agent was used.
406 A.K. Bledzki et al. / Composites: Part A 40 (2009) 404–412
2.2. Fabrication of composites
The compounds were processed by using a special coating tech-
nique. In a first step the PLA matrix was compounded together
with endless fibres via a coating die and cooled to ambient temper-
ature (twin-screw extruder from Haake, Rheomex PTW 25/32, L/
D = 32, D = 25 mm). The fibre cord was pre-dried online (umpteen
seconds at 170 °C). Further, the pellets were dried and com-
pounded on single-screw extruder (Schwabenthan, Polytest 30P,
L/D = 25, D = 30 mm) and again processed into pellets (cut length
15 mm) (Fig. 1).
The melt temperature in the coating was of approx. 200 °C,
screw speed was set at 100 rpm. Process temperature during com-
pounding was approx. 180 °C, at 20 rpm screw speed.
To prevent hydrolysis and pores’ formation, the matrix polymer
as well as pellets were dried in a convection oven with fan before
further processing (moisture content after drying at 80 °C/16 h:
PLA 6 0.02%; composite pellets 6 0.2%).
To compare the properties with common composites, all values
are referenced to PP homopolymer (Sabic/Germany, PP 575P) and
its composites (with the addition of 5 wt% of MAH-PP coupling
agent relate to the fibre weight) that were processed separately
by using same processing methods.
The standard test specimens according to DIN EN ISO 527
(‘‘dog-bone” tensile test specimen with shoulders), were produced
using an injection moulding machine Klöckner Ferromatik FM 85
at a temperature of approximately 180 °C in the melt, injection
pressure was about 500 bar and injection speed was 200 mm/s.
Additionally, because of the strongly hydrophilic nature of cellu-
losic fibres, the injection moulding machine’s hopper was heated
to 80 °C and rinsed with nitrogen gas with approx. 4 l/min
(N2 P 99.999 vol %, Air Liquide Deutschland, Düsseldorf/
Germany).
The test samples according to DIN EN ISO 178 and 179-II
(flexural and Charpy tests) were cut out according to DIN
EN ISO 2818 from the injection moulded standard test
specimens.
Fig. 1. Depicting of two-step extrusion principle (above) with successive injection moulding (below).
2.3. Methods
2.3.1. Mechanical testing
The mechanical characteristics were established on a universal
mechanical testing machine (Zwick/Roell 1446), using a quasi-stat-
ically flexural and tensile test in line with DIN EN ISO 178 and 527.
Charpy A-notch impact test was performed on a Zwick/Roell im-
pact-machine due to DIN EN ISO 179-II. All presented results are
the average values of 10 measurements.
2.3.2. Dynamic mechanical analysis (DMA)
The storage modulus, loss modulus and loss factor were mea-
sured as a function of temperature (from 0 to 90 °C). In this paper
only storage and loss modulus are presented. A TA Q800 Dynamical
Analyser with a dual-cantilever bending fixture in Multi-Fre-
quency-Strain modus was used. The frequency of 1, 3 and 10 Hz
at the amplitude of 10 lm and the heating rate of 3 K/min were
investigated. The geometry of the sample was 35  10  4 mm.
2.3.3. Optical and scanning electron microscopy
To test the fibre/matrix adhesion and composites morphology,
scanning electron microscopy (SEM) and optical microscopy
(OM) investigations were undertaken. The SEM fracture surfaces
were prepared in a cryo-break process (the ‘‘dog-bone” test speci-
mens were stored in liquid nitrogen for at least 10 min, after that
removed and immediately broken). A CamScan MV 2300 scanning
electron microscope with a wolfram cathode emission gun and
acceleration voltage of 20 kV was used. Optical microscopy speci-
mens were cut out from ‘‘dog-bone” samples and incorporated into
transparent epoxy resin. After cross-linking, the specimens were
fine polished and the surfaces were observed under Zeiss Axioplan
optical-microscope.
2.3.4. Evaluation of fibre length
To analyse the fibre length of pellets after compounding as well
as injected dog-bone specimens, composites were dissolved in
dichloromethane (DCM) at ambient temperature. Single fibres
 A.K. Bledzki et al. / Composites: Part A 40 (2009) 404–412 407

were extracted from whole investigated volume and their length Tensile
was measured under the Zeiss Axioplan optical microscope. Flexural
[MPa]
Approximately 500 fibres were measured.
PLA composites PP composites

3. Results and discussion 8000

3.1. Mechanical properties

6000

Fig. 2 shows tensile and flexural strength results of tested com-

posites. It can be observed that composites reinforced with man- 4000
made cellulose fibres achieve the highest strengths of around
92 MPa in tensile and 152 MPa in flexural test.
2000
The origin PLA shows tensile strength of 63 MPa and modulus of
3400 MPa. With the addition of 30 wt% of man-made cellulose fi- 3373 3690 8032 7890 5846 6510 1497 1318 4931 4192 4005 3661

bres, an improvement of tensile strength by factor 1.45 and tensile 0

PLA PLA/abaca PLA/cellulose PP PP/abaca PP/cellulose
modulus by 1.70 can be achieved (Fig. 3). In the flexural test an up-
grade in strength is even higher and it can be improved by factor Fig. 3. Tensile and flexural E-Modulus of PLA and PP composites (DIN EN ISO 524
1.50. The flexural modulus’s change is the same as in tensile test and 178).
(factor 1.7). Oksman et al. [36] investigated the influence of natural
fibre reinforcement on mechanical properties of compression
+23°C
moulded PLA composites. They showed that by the addition of
[kJ/m²] -30°C
30 wt% of flax fibre tensile strength increases slightly. The fibre
PLA composites PP composites
content of 40 wt% decreases the tensile stress. The modulus in-
crease was almost exact as in our research, from approx. 3.7 to 12
8 GPa at matrix/fibre ratio 70/30, and it increases with increasing
fibre load.
9
Abaca fibres cause in general better stiffness (improvement in
tensile modulus by factor 2.4, flexural modulus by factor 2.1)
(Fig. 3), than man-made cellulose. In comparison to unreinforced 6

polymer, abaca fibre improves mechanical characteristics. How-

ever, this increase is not as significant as by using man-made cel- 3
lulose fibre, where the tensile strength rise up to 74 MPa
2,2 2,7 5,3 5,2 7,9 7,4 3,5 1,4 5,3 4,1 11,1 9,8
(improvement by factor 1.2) and flexural strength up to 124 MPa 0
(factor 1.15). PLA PLA/abaca PLA/cellulose PP PP/abaca PP/cellulose

The ductility of each composite decreases, if compared to native

Fig. 4. A-notch Charpy impact strengths of PLA composites (DIN EN ISO 179-2/1eA).
PLA. Shibata et al. [34] reported that with the increasing abaca fibre
content the modulus enhancement is linearly. This result is similar
to our observations and the values of stiffness are also comparable. Fig. 4 represents results of Charpy A-notch impact tests, both at
However, the strength was not improved, even though several fibre +23 °C and at 30 °C. It can be seen that with the addition of
treatments were tested [34]. The unchanged composites’ flexural 30 wt% of man-made cellulose fibres, A-notch impact strength at
strength can be explained with other materials preparation proce- +23 °C increases by factor 3.60. The virgin PLA has impact strength
dure, where the compound was agglomerated on twin-rotary mix- of 2.2 kJ/m2, in contrast to 7.9 kJ/m2 of PLA/cellulose. Furthermore,
er and not like in this research in two-step extrusion process. Also at 30 °C this value remains almost without any change.
moisture content of the fibres and composites was not described, Ganster et al. [28] tested composites of PLA/man-made cellu-
what in case of aliphatic polyesters and hydrophilic fibres can be lose and they showed a similar tendency. In our test the Charpy
arbitrative, e.g. in view of hydrolysis of polymer chain. impact resistance increased by factor 3.60, compared to factor
2.0 of Ganster at al. [36].
They described a comparable improvement of unnotched sam-
ples. In general, the improvement of fibrous reinforcement by
Tensile Charpy is more significant with unnotched specimens than with
[MPa] Flexural notched ones. So the enhanced value by factor 3.6 of A-notched
samples that we achieved is especially noticeable.
PLA composites PP composites
160 The significant increase in impact strength can be referenced to
much lower diameter (higher aspect ratio) and smooth surface of
man-made cellulose fibre, in comparison to the irregular abaca fi-
120
bre. It affects the fibre/matrix interaction, whereby pull-outs ap-
pear more often with regenerated cellulose than with abaca fibre.
80 We suppose that for this reason the path length of initiated crack
is being enlarged which increases the energy amount needed to
break the sample (Fig. 5).
40
The addition of 30 wt% of abaca fibres leads to an improvement
63 109 74 124 92 152 29 42 44 72 72 104
by factor 2.4 at +23 °C and 2.0 at 30 °C. Oksman et al. [36] pre-
0 sented a decreased Charpy impact strength of the PLA/flax compos-
PLA PLA/abaca PLA/cellulose PP PP/abaca PP/cellulose
ites (60/40). This result is in opposite to our observation that the
Fig. 2. Tensile and flexural strengths of PLA and PP composites (DIN EN ISO 524/ addition of 30 wt% of abaca fibre enhanced the impact resistance
178). significantly.
408 A.K. Bledzki et al. / Composites: Part A 40 (2009) 404–412
Fig. 5. Scheme of initiated crack path: left, before break; right, after break.
Composites of PP/abaca are defined with increased values of
notched impact strength as compared to origin PP. This is due to
fibre reinforcement and strong interfaces, which results from
MAH-PP addition. Because of very good adhesion, fibres are able
to transfer stress better as by PLA composites. Moreover, PP is
more ductile as PLA. In consequence PP composites characterise
with higher impact values.
All mechanical properties of PLA composites in contrast to poly-
propylene made with comparable processing conditions show
much better results (Figs. 2 and 3). Exceptions are Charpy impact
strength (Fig. 4) and tensile/bending elongation, where PP compos-
ites show slightly better values than PLA composites caused by
their much higher ductility.
The differences in mechanical properties are due to molecular
structure of both, polypropylene and polylactide. Regarding to
methyl group, polypropylene is a highly non-polar polyolefin. For
that reason the bonding between well polar cellulosic fibres
(–OH groups) and PP is very poor; however, it can be significantly
improved by adding coupling agents, e.g. maleic acid anhydride
grafted PP copolymers. Basically, PP is very ductile, but only medi-
ocre stiff. As a result, this polymer characterises with lower stiff-
ness expressed via E-Modulus but improved toughness shown in
impact strength. PLA is in opposite to polypropylene, aliphatic
polyester that contains functional ester groups in the main chain.
6000
4000
Storage Modulus (MPa)
3000
2000 2000
1000
0
60 65
0
0 20
Fig. 6. Temperature dependence of storage modulus of PLA and PLA-based composites (f = 1 Hz).
Reinforcing PLA with natural fibres leads to better chemical bond-
ing on the interphase as for PP composites without coupling agent.
In addition PLA is from the nature very stiff, and contrasting to PP
the impact resistance of PLA is very poor.
3.2. Dynamic mechanical properties
The DMA investigation was performed to study the effect of fi-
brous reinforcement incorporation on the dynamic-mechanical
performance of native PLA and its composites. In this case the tem-
perature range within 0 and 90 °C was taken under examination.
The secondary crystallisation for PLA begins above 90 °C [41].
Fig. 6 shows the dynamic storage modulus curves of the origin
PLA and PLA-based composites as a function of temperature. The
storage modulus of PLA composites is much higher then of PLA.
This is due to fibre reinforcement, which allows better stress trans-
fer from the matrix to the fibre. The highest value of the dynamic
modulus can be achieved for PLA/abaca, than for PLA/cellulose
and PLA. The tendency corresponds to the statically tensile and
bending test as well. The abaca fibre from the nature is very stiff,
where the man-made cellulose is more flexible. This performance
allows achieving a higher modulus of abaca reinforced composites
and better impact resistance of cellulose ones.
It can also be seen that below 70 °C native PLA characterises
with the lowest storage modulus. In this temperature range PLA
based composites have slightly higher values of the storage modu-
lus. The fibrous reinforcement affects the chain mobility. The com-
posite remains stiffer and the polymer flow is restricted. This effect
can also be observed in changing of the glass transition temperature
(Tg) derived from the loss modulus curves (Fig. 7). It is obvious that
incorporating of fibres enhances the Tg. The slightly shifting (few
degrees) of Tg to higher temperature indicates an affected mobility
of polymer chains. As the volume fraction of man-made cellulose is
higher than abaca (because of the fibre diameter), the Tg of PLA/cel-
lulose is higher and amounts to approx. 68 °C, if compared to 66 °C
of PLA/abaca and 64 °C for native PLA. It corresponds to the loss of
storage modulus below 70 °C. Mathew and Averous et al. [32,42]
discuss, that the shift to higher temperature usually indicates re-
stricted molecule movement because of better interaction between
––––––– PLA
–––– PLA-Abaca
––––– · PLA-Cellulose
70 75 80 85
40 60 80
Temperature (°C) Universal V4.1D TA Instruments
 A.K. Bledzki et al. / Composites: Part A 40 (2009) 404–412 409

1200
––––––– PLA
–––– PLA-Abaca
––––– · PLA-Cellulose
1000

800
1000
Loss Modulus (MPa)

800

600 600

400

200
400
0
60 65 70 75 80 85

200

0
0 20 40 60 80
Temperature (°C) Universal V4.1D TA Instruments

Fig. 7. Temperature dependence of loss modulus of PLA and PLA-based composites (f = 1 Hz).

the fibre and the polymer matrix. Furthermore, the a-relaxation in-
volves the movements of polymer chains. The presence of crystal-
line structures or reinforcement could also act as a physical cross-
linking, decreasing the mobility of amorphous regions and conse-
quently increasing the composite’s stiffness.
3.3. Morphology
The morphology of fracture surfaces was studied by SEM as
shown in Fig. 8. The photographs indicate fibre pull-outs at the
scanned surface. Furthermore, abaca fibres seem to be better
coated with PLA matrix as man-made cellulose. Probably, this is
due to the surface roughness, which is very smooth with regener-
ated cellulose and quite irregular with abaca fibres. The adhesion is
not strong in any of the composites.
Because of different fibre diameters (Abaca fibres approx.
150 lm, cellulose fibres of around 12 lm) the chosen magnifica-
tion had to be different accordingly.
The optical microscopy photographs (Fig. 9) show typical
after-process fibre orientation, which is elliptical and axially al-
most symmetric in reference to the melt flow direction during
injection moulding. This can explain the higher values of flexural
strength, where the fibre orientation is much more favourable, if
the load direction is taking into consideration. Moreover, a fine
dispersion of fibres in the polymer can be seen, due to two-step
processing; it can be achieved by using an additional compound-
ing step.
3.4. After process fibre length
Regarding mechanical properties of short-fibres composites, the
main attention should be paid to the fibre length. This property is
one of the key parameters in the composites fracture mechanic.
While the fibres’ length in compounds is not of major importance,
their length in the composite can be the main factor determining
failure mechanisms of the cross-section.
Fibres’ length distribution in pellets after compounding and in
samples after injection moulding is depicted in Fig. 10. The mea-
surement was evaluated on approx. 500 fibres. A significant de-
crease in the fibre length after compounding on the single-screw
extruder can be observed, from the cut length of 15 mm to about
1.0–2.0 mm. Moreover, the injection moulded samples show only

Fig. 8. SEM photographs of PLA/cellulose (500) and PLA/abaca (100).

410 A.K. Bledzki et al. / Composites: Part A 40 (2009) 404–412

Fig. 9. Optical microscopy photographs of PLA/cellulose and PLA/abaca composites (magnification 17).

an insignificant drop of length, if put side by side to pellets, which of the fibre length seems to be more uniform. As a result, most of
indicates to massive fibre length reduction during extrusion pro- the fibres, which remain longer than 2 mm after compounding,
cess. Processing on the single-screw extruder already affected the are being shortened below 2 mm during injection moulding.
length significantly. Compounding on twin-screw extruders, which Critical fibre length for PLA/abaca composites was determined
is often carried out in composites processing, can surpassingly according to Eq. (3.1) and amounts Lc = 1.843 mm.
influence the fibre length even more. The minimal fibre length is
rmax
f D
already being achieved during compounding and is not being af- Lc ¼ ð3:1Þ
fected during injection moulding process; however, the occurrence 2s

Fig. 10. After process fibre length of PLA/abaca 70/30 composites.

 A.K. Bledzki et al. / Composites: Part A 40 (2009) 404–412
where Lc, critical fibre length; 1.843 mm, D, fibre diameter;
0.271 mm, rmax
f , fibre tensile stress at maximum; 489 MPa, s, inter-
facial or matrix shear strength; 35.96 MPa.
s was determined according to Eq. (3.2);
rmax
s ¼ pmffiffiffi ¼ 0:58rmax
m ð3:2Þ
3 pounding and is not being significantly affected during injection
rmax
m , matrix tensile stress at maximum; 62 MPa.
Fibre aspect ratio according to Eq. (3.3) amounts kc = 6.8
L c rf
max
kc ¼ ¼ ð3:3Þ
D 2s
From literature the range of abaca fibre tensile stress is quite wide
and includes values from 400 to 1100 MPa [16,34,40]. For that rea-
son we determined this property by ourselves and calculated it to
489 MPa. The value was estimated in a tensile test of a single fibre
bundle from 30 measurements. To determine the fibre diameter, an
optical microscopy was undertaken. The average value was calcu-
lated from 140 measurements of the middle section of the fibre
and estimated at 0.271 mm. Hence, for calculation of fibre cross-
section in the tensile test, a value of 0.271 mm was used.
Most of the tested fibres have a measured fibre length of 1.0–
1.5 mm, whereas the critical fibre length is 1.8 mm. In such case
the load cannot be transferred from the polymer matrix to the fibre
completely. As a result, tested specimens break too early. More-
over, the pull out mechanism is taking place. This scenario can
be partly seen in SEM pictures. However, the theory assumes a per-
fect adhesion on the fibre/matrix interphase (absence of any struc-
ture defects). A perfect adhesion cannot be achieved, especially if
no coupling agent was used. This requirement could partially be
fulfilled only for PP with natural fibre reinforcement, in composites
of which, the maleic acid anhydride (MAH) was applied.
Specht [43] discussed the influence of MAH in PP NF compos-
ites. He showed that by adding small quantities of coupling agent
a significant enhancement of shear strength could be achieved. It
indicates an improvement of fibre/matrix interaction, which re-
sults in better adhesion on the interphase. Moreover, he showed
that addition of maleic acid anhydride to PP matrix induces gentler
processing. Consequently, decreased fibres damage was observed;
probably, because of lubricant effect of MAH in PP.
4. Conclusions
Mechanical properties like tensile, flexural and impact strength
and stiffness of man-made cellulose and abaca fibre reinforced PLA
have been investigated. The test results of PLA composites were
found to have significantly improved, if compared to native PLA
matrix. Furthermore, man-made cellulose fibres showed a much
better potential as reinforcement for polylactides than abaca fibre.
However, abaca fibres seem to allow a higher composite stiffness.
The most significant improvement was achieved in Charpy
A-notch impact strength of PLA/cellulose 70/30, which increased
by factor 3.6 of the origin PLA value. The impact strength of PLA/
abaca has improved by factor 2.4.
The dynamic mechanical analysis showed that incorporation of
fibrous reinforcement causes a decrease in polymer chains mobil-
ity. The storage modulus of PLA-based composites remained much
higher than of unreinforced PLA. The glass transition temperature
derived from loss modulus characterises with a slight shift to high-
er temperatures, if compared to matrix polymer.
Morphology was evaluated by SEM and optical microscopy. The
SEM pictures showed several fibre pull-outs. Abaca fibres seem to
have improved physical bonding to the matrix in opposite to man-
made cellulose fibres, probably due to fibre surface roughness. The
optical microscopy photographs demonstrated typical after-pro-
411
cess fibre orientation, which is almost perfectly symmetric due to
the flow direction of polymer melt. The fibre dispersion is very fine,
because of the two-step processing.
The investigated fibre length was significantly reduced during
the compounding step on single-screw extruder already. The
minimal fibre length is already being achieved during com-
moulding.
Further research will focuses on improvement of fibre/matrix
interphase, e.g. by optimising the process parameters, using chem-
ical fibre treatment, or coupling agents. The after-process fibre
length and structure are very important, as both strongly influence
the properties of the end-product. The process optimisation as re-
gards more gentle process parameters or other screw geometry
will be undertaken in the near future.
Acknowledgements
The authors express their appreciation to BASF, Ludwigshafen/
Germany, Rieter Automotive, Sevelen/Switzerland and IAP Pots-
dam-Golm/Germany for supplying the PLA polymer, abaca and
man-made cellulose fibres.
References
[1] Bioplastics Online. Available from: http://www.eplastics.pl [accessed 29.01.07]
[in Polish].
[2] News on Plastic Industry. Available from: http://www.plastemart.com
[accessed 31.01.07].
[3] Bioplastics Online. Available from: http://www.eplastics.pl [accessed 23.09.06]
[in Polish].
[4] Bioplastics newsletter. Available from: http://www.bioplastics24.com
[accessed 04.12.06].
[5] KunststoffWeb News. Available from: http://www.kunststoffweb.de [accessed
8.12.06].
[6] Plasticker-News. Available from: http://www.plasticker.de [accessed
24.11.06].
[7] European Bioplastics press release, Brüssel, 21 November 2006.
[8] Uhde Inventa-Fischer Company announcement. Available from: http://
www.uhde-inventa-fischer.com.
[9] CentreDaily.com newsletter. Available from: http://www.centredaily.com
[accessed 11.12.06].
[10] KunststoffWeb News. Metabolix. Available from: http://
www.kunststoffweb.de [accessed 02.01.07].
[11] Bioplastics Online. Available from: http://www.eplastics.pl [accessed
10.10.06] [in Polish].
[12] Novamont press release, Novara, 25 October 2006.
[13] DuPont Company announcement. Available from: http://www2.dupont.com.
[14] Doi Y. Microbial polyesters. Nagatsuta, Japan: Wiley-VCH; 1990.
[15] Bastioli C. Handbook of biodegradable polymers. Shawbury, UK: Rapra
Technology; 2005.
[16] Mohanty AK, Misra M, Drzal LT. Natural fibres, biopolymers and
biocomposites. Boca Raton, USA: Taylor&Francis Group; 2005.
[17] Mohanty AK, Misra M, Hinrichsen G. Biofibres, biodegradable polymers and
biocomposites: an overview. Macromol Mat Eng 2000;276/277:1–24.
[18] First european bioplastics conference proceedings. European Bioplastics,
Brussels, 21–22 November 2006.
[19] Serizawa S, Inoue K, Iji M. Kenaf-fiber-reinforced poly (lactic acid) used for
electronic products. J Appl Polym Sci 2006;100:618–24.
[20] Scherübl B. An innovative composite solution in the new Mercedes a class – a
successful story about the natural fibre ABACA. In: Proceedings of sixth global
wood and natural fibre composites symposium, Kassel, April 2006. p. A 12.
[21] Bledzki AK, Faruk O, Sperber VE. Cars from Bio-Fibres. Macromol Mat Eng
2006;291:449–57.
[22] Eichholzer W. Natural fibre applications in automotive manufacturing. In:
Proceedings of sixth global wood and natural fibre composites symposium,
Kassel, April 2006. p. A 11.
[23] Weigel P, Ganster J, Fink HP, Gassan J, Uihlein K. Polypropylene-cellulose-
compounds. Kunststoffe 2002;5:95–7.
[24] Klemm D, Heublein B, Fink HP, Bohn A. Cellulose: faszinierendes biopolymer
und nachhaltiger Rohstoff. Angew Chem 2005;117:3422–58.
[25] Faruk O. Microcellular wood fibre reinforced polypropylene composites/
injection, extrusion and compression moulding process. Publicised Ph.D.
Thesis on Chair of Polymer and Recycling Technology, University of Kassel,
ISBN 83-60140-95-2, Kassel, Germany, 2005.
[26] Bledzki AK, Jaszkiewicz A, Sperber VE. Abaca and cellulose fibre reinforced
polypropylene. In: Proceedings of fourth international workshop on green
composites, Tokyo, September 2006. p. 1–5.
412 A.K. Bledzki et al. / Composites: Part A 40 (2009) 404–412
[27] Weigel P, Ganster J, Fink HP. Cellulose: faszinierendes biopolymer und
nachhaltiger Rohstoff. In: Proceedings of fourth International wood and
natural fibre composites symposium, Kassel, April 2002. p. 25–31.
[28] Ganster J, Fink HP. Rayon reinforced thermoplastics for injection moulding. In:
Proceedings of fifth international symposium: materials made of renewable
resources, Erfurt, September 2005. p. 1–9.
[29] Pluta M, Galeski A, Alexandre M, Paul MA, Dubois P. Polylactide/
montmorillonite nanocomposites and microcomposites prepared by melt
blending: structure and some physical properties. J Appl Polym Sci
2002;86:1497–506.
[30] Huda HS, Drzal LT, Mohanty AK, Misra M. Chopped glass and recycled
newspaper as reinforcement in injection molded poly(lactic acid) (PLA)
composites: a comparative study. Comput Sci Technol 2006;66:1813–24.
[31] Huda MS, Drzal LT, Misra M, Mohanty AK. Wood-fiber-reinforced poly(lactic
acid) composites: evaluation of the physicomechanical and morphological
properties. J Appl Polym Sci 2006;102:4856–69.
[32] Mathew AP, Oksman K, Sain M. Mechanical properties of biodegradable
composites from poly lactic acid (PLA) and microcrystalline cellulose. J Appl
Polym Sci 2005;97:2014–25.
[33] Mathew AP, Oksman K, Sain M. The effect of morphology and chemical
characteristics of cellulose reinforcements on the crystallinity of polylactic
acid. J Appl Polym Sci 2006;101:300–10.
[34] Shibata M, Ozawa K, Teramoto N, Yosomiya R, Takeishi H. Biocomposites made
from short abaca fiber and biodegradable polyesters. Macromol Mat Eng
2003;288:35–43.
[35] Plackett D, Logstrup Andersen T, Batsberg Pedersen W, Nielsen L.
Biodegradable composites based on L-polylactide and jute fibres. Comput Sci
Technol 2003;63:1287–96.
[36] Oksman K, Skrifvars M, Selin JF. Natural fibres as reinforcement in polylactic
acid (PLA) composites. Comput Sci Technol 2003;63:1317–24.
[37] Nishino T, Hirao K, Kotera M, Nakamae K, Inagaki H. Kenaf reinforced
biodegradable composite. Comput Sci Technol 2003;63:1281–6.
[38] Bledzki AK, Faruk O, Mamun AA. Influence of compounding processes and fibre
length on the mechanical properties of abaca fibre–polypropylene composites.
Polimery 2008;53:35–40.
[39] Kozlowski R, Wladyka-Przybylak M, Kicinska-Jakubowska A. State of art in the
research on natural fibres and their properties used in composites. In:
Proceedings of seventh global WPC and natural fibre composites
symposium, Kassel, June 2008. p. A 14.
[40] Dippon K. Geotextilien aus Naturfasern für die Renaturierung von Gewässern
am Beispiel Japan. In: Proceedings of Geo- und Agrartextilien aus Hanffasern:
Technik, Bremen, October 1999.
[41] Pyda M, Bopp RC, Wunderlich B. Heat capacity of poly(lactic acid). J Chem
Thermodyn 2004;36:731–42.
[42] Averous L, Fringant C, Moro L. Plasticised starch–cellulose interactions in
polysaccharide composites. Polymer 2001;42:6565–72.
[43] Specht K. Holz- und hanffaserverstärktes Polypropylen in der
Spritzgießverarbeitung. Publicised Ph.D. Thesis on Chair of Polymer and
Recycling Technology, University of Kassel, ISBN 978-83-751805-1-0, Kassel,
Germany 2007.