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Fibre matrix adhesion of natural

fibres cotton, flax and hemp in
polymeric matrices analyzed with the
single fibre fragmentation test
a b
Tim Huber & Jörg Müssig
a
Hochschule Bremen, University of Applied Sciences,
Biomimetics/Biological Materials, Neustadtswall 30, 28199
Bremen, Germany
b
Hochschule Bremen, University of Applied Sciences,
Biomimetics/Biological Materials, Neustadtswall 30, 28199
Bremen, Germany
Version of record first published: 02 Apr 2012.

To cite this article: Tim Huber & Jörg Müssig (2008): Fibre matrix adhesion of natural fibres
cotton, flax and hemp in polymeric matrices analyzed with the single fibre fragmentation test,
Composite Interfaces, 15:2-3, 335-349

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 Composite Interfaces, Vol. 15, No. 2–3, pp. 335– 349 (2008)
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Fibre matrix adhesion of natural fibres cotton, flax and

hemp in polymeric matrices analyzed with the single fibre
fragmentation test
Downloaded by [University of Arizona] at 19:13 10 December 2012

TIM HUBER and JÖRG MÜSSIG ∗

Hochschule Bremen, University of Applied Sciences, Biomimetics/Biological Materials,
Neustadtswall 30, 28199 Bremen, Germany

Received 31 May 2007; accepted 8 July 2007

Abstract—In this research the adhesion and the resulting interfacial shear strength (IFFS) between
the natural fibres flax, hemp and cotton and the polymer matrices polypropylene with coupling agent
(MAPP) and polylactide acid (PLA) was surveyed with the single fibre fragmentation test (SFFT).
The adhesion between MAPP and the fibres was good enough to produce fragments, whereas the
adhesion between PLA and flax was too weak to transmit enough tension for fibre cracks which is
clearly visible on SEM-photographs.
Comparing the IFFS values of the fibres in MAPP with an equal fibre diameter shows that the IFFS
value of flax is highest with 7.09 N/mm2 followed by hemp 6.13 N/mm2 . The IFFS of cotton is a lot
smaller (0.664 N/mm2 ).
The critical fragmentation or fragmentation length of the bast fibres flax (3.16 mm) and hemp
(3.20 mm) in MAPP is smaller than the critical fragmentation length of cotton (5.03 mm).
The adhesion between the lignocellulosic fibres and MAPP is much better than between the lignin
and pectin free cellulose fibre and MAPP. Possible reasons for this — the surface structure of the
cotton fibre and its different chemical composition being made up of only cellulose, hemi-cellulose
and wax with no pectin or lignin present — are discussed.

Keywords: Natural fibres; MAPP; PLA; adhesion; critical fibre (fragmentation) length; interfacial
shear strength.

1. INTRODUCTION
1.1. Fibre reinforced composites
There is constantly increasing interest in fibre reinforced composites because of
their mechanical properties. They are very light weight and stiff and the orientation
of the fibres is customizable to almost every load.

∗ To whom correspondence should be addressed. E-mail: joerg.muessig@hs-bremen.de

 336 T. Huber and J. Müssig

In recent years more and more biological materials are being used, such as natural
fibres or bio-based polymers as polylactide acid or polymers made from starch.
This might be caused by a constantly rising oil price and thus higher costs for
petrochemical materials on the one hand and on the other by a growing awareness
of environmental needs. Especially the automobile industry has started to use more
and more natural fibre reinforced composites [1 –3].

1.2. Natural fibres

Most natural fibres consist of cellulose, hemicellulose, lignin and pectin [4]. Their
properties are heavily influenced by their growing circumstances and processing.
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Hollow cellulose fibres are held together by a matrix made up of lignin and
hemicellulose. Each fibril consists of a thin primary cell wall that surrounds a
secondary wall which is itself made up of three layers, of which the thick middle
layer determines the mechanical properties. Helically wound microfibrils out of
long-chain cellulose molecules form this middle layer. The angle between these
microfibrils and the fibre axis, the microfibrillar angle, the cellulose content and the
degree of polymerization influence the mechanical properties of the fibre [5].
A problem with the use of natural fibres is their hydrophilic character that is
caused by the structure of the cellulose molecules. Its 1,4-β-glucose monomers
and hydroxyl groups are able to develop hydrogen bonds within the molecule as
well as with other macromolecules or even the hydroxyl groups in the air [4, 6]. As
result of this, adhesion between the hydrophilic fibres and the hydrophobic matrix
is difficult to accomplish and when exposed to humidity the fibres start to swell,
which causes a decrease in dimensional stability [7].

1.3. Fibre–matrix adhesion

The bonding between fibre and matrix and the resulting properties of the composite
strongly depend on the fibre–matrix adhesion. Only a strong fibre–matrix adhesion
provides a stress transfer from matrix to fibre [8]. Weak adhesion leads to a failure
in the fibre–matrix interface and therefore to worse mechanical properties of the
composite [9] like a lower flexural stiffness and compressive strength [10].

1.4. Polymers
A frequently used polymer in combination with natural fibres is polypropylene (PP)
whose adhesive properties can be improved by a coupling agent [3, 8, 11].
Polylactic acid (PLA) is the polymer of lactic acid and it is more hydrophilic than
pure PP; for that reason it may be expected to bond more strongly with natural fibres
[12]. Current research results are controversial. Oksman et al. [13] found a weak
fibre–matrix adhesion for PLA and flax fibres while Nishino et al. [14] report strong
interaction between PLA and kenaf fibres. The used polymers in this research will
be polypropylene with the coupling agent maleic anhydride and PLA.
 Fibre–matrix adhesion of natural fibres with polymers 337
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Figure 1. The process of fragmentation under tension σ to the fragments with the critical fragmenta-
tion length lc [17].

1.5. Single-fibre fragmentation test

The assay of the adhesion between fibre and matrix of the different composites will
be made with the help of the single fibre fragmentation test (SFFT). This is one
of the most common methods to characterize the fibre–matrix interface [8, 15, 16].
A tensile load will be placed on a single fibre embedded in the matrix. If the strain of
the matrix is higher than the strain of the fibre and the stress transferred from matrix
to fibre is higher than the fibre break stress σbf the fibre will break into fragments
until a saturation point is reached and the stress transferred from matrix to fibre
is no more high enough to cause further fragmentation (Fig. 1). The minimum
length of the fibre is usually called critical fibre length lc but as the flax and hemp
fibres are present in fibre bundles the expression critical fragment length lfc will be
used further on. With the help of lfc the interfacial shear strength (IFSS) τ can be
calculated if σbf is known [17].
One big advantage of the SFFT is that, due to the critical fibre length, direct
conclusions about the fibre–matrix adhesion can be drawn [10]. Furthermore, if
the matrix is transparent, the fragmentation can be directly observed [18]. To gain
proper results the strain of the matrix has to be three times as high as the strain of the
fibre. Moreover, the model does describe ideal systems with a plastic deformation
of the matrix and constant stress along the complete specimen [17].

2. MATERIALS AND METHODS

2.1. The fibres
2.1.1. Flax (Linum usitastissimum L., Linacea). According to literature, the flax
cell wall is made up of about 62% cellulose, 17% hemicellulose, 1.8% pectin, 2%
lignin and about 1.5% wax. The microfibrillar angle is 10◦ [4, 5].
 338 T. Huber and J. Müssig

Flax of the type Holstein flax HO-0401b, planted in 2003 was used. For this type
the fibre strength is 874 N/mm2 , Young’s modulus is 14583 N/mm2 and the strain
is 6.6% [19].

2.1.2. Hemp (Cannabis sativa L., Cannabacea). Hemp is, on average, made up
of about 67% cellulose, 16.1% hemicellulose, 3.3% lignin, 0.8% pectin and 0.7%
wax. The microfibrillar angle of hemp is 6.2◦ [4, 5].
The hemp fibres used (GDE-02, harvested in 2002) have a strength of 827 N/mm2 ,
a Young’s modulus of 12984 N/mm2 and a strain of 8.8% [19].

2.1.3. Cotton (Gossypium spp., Malvacea). The cellulose content of cotton

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is 92.7%. The average amount of hemicellulose and wax are 5.7% and 0.6%,
respectively. Pectin and lignin are not present in cotton fibres [4, 5].
The strength of the cotton fibres (US-Pima) is 618 N/mm2 , Young’s modulus is
11 844 N/mm2 and the strain is 7.3% [19].

2.2. Polymers
2.2.1. Polypropylene with coupling agent. Polypropylene granules of the type
SABIC® PP 755P with 2% maleic anhydride as coupling agent were used. The
Copolymer (type Licomont® AR 504), has a melting temperature of 156◦ C, an acid
number of 41 mg KOH/g and a density of about 0.91 g/cm3 .

2.2.2. PLA. NatureWorks™ PLA-Polymer granules (type 4042D) were used.

The specific density of this material is 1.24 g/cm3 , the melting density at 230◦ C is
1.08 g/cm3 . The melt index at 210◦ C is 15–30 g/10 min and the glass transition
temperature is 60–65◦ C.

2.3. Specimen preparation

Sheets of polypropylene with 2% maleic anhydride (MAPP) and PLA were pro-
duced in the following way. Five grams of the granules were placed between two
Teflon sheets and compression moulded by two iron plates in a Rucks® -laboratory
press type KW 214.1 at 220◦ C and 4 MPa for 10 min.
To control the thickness of the sheets, 4 thin metal plates (0.075 mm) were placed
on the Teflon sheets. The moulded sheets were cooled down at room temperature
(20–23◦ C).
The PLA granules were dried for 3 h at 80◦ C to impede a depolymerisation. The
single sheet thickness was about 0.2 mm.
A single polymer sheet was placed on the Teflon sheet and single fibres for cotton,
fibre bundles for flax and hemp were separated and attached to the polymer sheet
with adhesive tape. A second polymer sheet was placed on the top of the first one
and the two sheets with the fibres in between were again pressed between the two
metal plates and Teflon sheets in the laboratory press at 185◦ C and 20 MPa for
 Fibre–matrix adhesion of natural fibres with polymers 339

90 s to mould the test specimen. Straight fibres with surrounding polymer matrix
were cut out after cooling down the fibre–polymer sheet complex. Again the 4
thin metal plates were placed between the Teflon sheets to control the specimen
thickness which was between 0.22 and 0.28 mm.

2.4. SFFT

The fragmentation test was carried out on an Instron® testing machine type 4502
with a 10-kN load cell. The machine was controlled by a computer with Instron
software (Instron Series IX). Specimen width and thickness was measured and
entered into the computer system. The cross-head speed was 0.2 mm/min. Gauge
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lengths of 15.5 mm (MAPP-flax, MAPP-Hemp and MAPP-Cotton) and 30 mm

(MAPP-flax, PLA-flax) were used. The load was constantly applied to a strain of
16% or failure of the specimen. The data was saved automatically to the computer.
Two polarization filters with a diameter of about 40 cm were used during the
loading to improve the visibility of fibre breaks and debonding.
After the loading, the specimens were analyzed with an optical microscope
(Zeiss® MC80) and the fibre diameter and the fragment lengths were measured
with the help of a positive ocular with micrometer. To normalize the fibre and fibre
bundle diameters, each fibre or fibre bundle was measured five times and the mean
value of these five measurements was used as value for the fibre diameter.
A total of 8 specimens for MAPP-hemp and MAPP-flax and 7 specimens for
MAPP-cotton were taken into account. For PLA-flax 9 specimens were analyzed.
Figure 2 shows a typical specimen of MAPP-flax after fragmentation.

Figure 2. A specimen of MAPP-flax after fragmentation. The cracks are clearly visible.
 340 T. Huber and J. Müssig

2.5. Determining the critical fragmentation length and the interfacial shear
strength
Critical fragmentation length was calculated after Tripathy et al. [16] with:
4
li
n
4
Lfc = l = , (1)
3 3 i=0 n

where Lfc is the critical fragmentation length, l the average fragment length and li
are the single fragment lengths.
With the critical fragmentation length the interfacial shear strength τ is deter-
minable with the Kelly–Tyson Model:
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σf df
τ= , (2)
2Lfc
where σf is the fibre strength and df is the fibre diameter [16].
Based on an expected fragment length of about 3 mm [3] and as the fibre strength
depends on the fibre diameter, data from Müssig et al. [19] were used to put
diameter and strength in relation with the software curveExpert™ 1.3 by Daniel
G. Hyams, because the data for the fibre strength in this research were determined
at a gauge length of 3.2 mm.
The fibre strength was calculated with following formula:
d
y = −ab exp(−cx ) , (3)
where y is the fibre strength, x is the fibre diameter and a, b, c and d are parameters
of the used Weibull distribution model.

2.6. Scanning electron micoscropy

SEM analysis was made with a scanning electron microscope type CS 24 from
Obducat CamScan® with an accelerating voltage of 20 kV.
The specimens were due to their specific shape sputtered twice for 3 min with
platinum-iridium.

3. RESULTS

3.1. Determination of fibre strength with the fibre diameter

Figure 3 shows mean values and standard deviations for the measured fibre
diameters of flax, hemp and cotton fibres. Those were measured within the
specimens. The data are normal distributed (α = 5%, David et al. test); the cotton
diameter (14.40 µm) is significantly smaller than the values of flax (58.20 µm) and
hemp (65.02 µm) (α = 5%, Weir test). The high standard deviations are caused by
the different sizes of the fibre bundles. Fibre strength is calculated with the help of
 Fibre–matrix adhesion of natural fibres with polymers 341
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Figure 3. Mean values and standard deviations of the different fibres measured in the MAPP matrix.

Figure 4. Mean values and standard deviations of the critical fragmentation length of MAPP–flax,
MAPP–hemp and MAPP–cotton at 15.5 mm gauge length.

equation (3) based on results with a clamping length of 3.2 mm using the fibre and
fibre bundle diameters measured in the SFFT samples.

3.2. Critical fragmentation length

Critical fragmentation length was calculated with the help of equation (1). All
values for the critical fragmentation length are normal distributed (α = 5%, David
et al. test) and presented in Fig. 4. Flax (3.20 mm) and hemp (3.16 mm) do not
differ significantly from each other (α = 5%, t-test) but are significantly lower than
the value of cotton (5.03 mm) in MAPP (α = 5%, Weir-test for flax and α = 5%,
t-test for hemp).
 342 T. Huber and J. Müssig

3.3. IFFS

The data for the IFFS calculated with equation (2) are normal distributed (α = 5%,
David et al. test). All values differ significantly from each other (α = 5%, Weir test
for hemp and cotton; α = 5%, t-test for flax and cotton and flax and hemp). Hemp
has the highest IFFS with 14.33 N/mm2 , followed by flax with 12.03 N/mm2 and
cotton has the lowest IFFS with 0.664 N/mm2 .
To compare the different fibres more directly the data for the IFFS was recalcu-
lated with the fibre diameters of the cotton fibres as flax and hemp consist of fibre
bundles of different sizes.
IFFS of flax and hemp calculated with the diameter of the cotton fibres is higher
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for flax with 7.09 N/mm2 than for hemp with 6.13 N/mm2 . Results can be seen in
Fig. 5.

3.4. MAPP-flax at different gauge lengths

Critical fragmentation length of MAPP-flax was determined at 15.5 mm and 30 mm

gauge length and calculated with the help of equation (1). Figure 6 shows the
determined mean values and standard deviations. The data is normal distributed
(α = 5%, David et al. test). The critical fragmentation length does not differ
significantly for 15.5 mm (3.16 mm) and 30 mm (3.62 mm) gauge length (α = 5%,
t-test).

Figure 5. Mean values and standard deviations of MAPP–flax, MAPP–hemp and MAPP cotton IFFS
and the IFFS mean values and standard deviations of MAPP–flax and MAPP–hemp calculated with
an assumed diameter taken from the diameter values of cotton.
 Fibre–matrix adhesion of natural fibres with polymers 343
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Figure 6. Mean values and standard deviations of the critical fragmentation length of MAPP–flax at
15.5 mm and 30 mm gauge length.

3.5. Flax and PLA at 30 mm gauge length

As no difference between 15.5 mm and 30 mm gauge length for MAPP-flax was
visible, the PLA-flax specimen were tested at 30 mm gauge length as the process of
possible fragmentation was easier to observe during the test at higher gauge lengths
due to the geometry of the testing machine.
Sixteen specimens were tested of which 9 were taken into account. Only two
specimens produced clear fragments during loading while the other 7 showed no
effects of a load transfer from matrix to fibre. Figures 7 and 8 show a PLA-flax
specimen after load in a SEM. A clear gap between fibre (A) and matrix (B) can be
seen.
Figure 8 shows a magnification of the gap area between fibre (A) and matrix (B).
There are no adhesive structures identifiably.

4. DISCUSSION
4.1. Different fibres in MAPP
Numbers of fragments, critical fragmentation length and IFFS values for flax
in MAPP have the expected range. Number of fragments (5.5) and critical
fragmentation length (3.20 mm) accord well with the results of Bos [3] of 2.8 mm
for flax with 1% — MAPP. The small difference between these and the values of
Bos is probably caused by the different amount of maleic anhydride, which has a
big influence on the fibre–matrix adhesion even in such small amounts, because
the interaction possibilities between the polar and hydrophilic fibre and the non-
polar hydrophobic matrix are improved [3, 20 –22]. The anhydride groups of the
 344 T. Huber and J. Müssig
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Figure 7. SEM picture of a flax fibre (A) embedded in a PLA matrix (B) after the tensile load with
30 mm gauge length. A clear debonding between fibre and matrix is visible.

Figure 8. Magnification of the adhesive area of the fibre (A) matrix (B) complex. There are no
adhesive structures between fibre and matrix visible.
 Fibre–matrix adhesion of natural fibres with polymers 345

coupling agent are able to form hydrogen as well as covalent bonds with the fibre
surface [23, 24].
The IFSS value for flax/MAPP of 12.03 N/mm2 is also in the expected range. Bos
[3] (12 N/mm2 ) reports similar values for the single fibre fragmentation test. So do
Eichhorn et al. [25] with 11.4 N/mm2 whereas this value was achieved with the pull-
out test. The IFFS values for a combination of flax with pure PP in the mentioned
research works are all lower than for flax with MAPP thus it can be concluded that
described interactions between coupling agent and fibre actually take place.
Number of fragments and critical fragmentation length of flax-MAPP show no
significant difference to hemp-MAPP but the IFFS does. This might be explained by
the similar but slightly different composition of these fibres. Even small differences
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might have an influence on the mechanical properties [5]. A known trend for natural
fibres is that a higher rate of cellulose and a smaller microfibrillar angle result in a
higher fibre strength and a higher Young’s modulus although a direct link has not
been proved because of the complex fibre structures [4, 5, 26]. The values for fibre
strength and Young’s modulus reported in Müssig et al. [19] for the used fibre types
are higher for flax (874 N/mm2 and 14 583 N/mm2 ) than for hemp (827 N/mm2
and 12 984 N/mm2 ) and do not validate the reported trend. Consequently the
higher IFFS values of hemp cannot be explained with the mechanical properties
of the fibres and are probably caused by the fibre diameter and the chosen model to
calculate the fibre strength.
The theoretical values for the IFFS with fibre diameters of the cotton fibres show
higher values for flax (7.09 N/mm2 ) than for hemp (6.13 N/mm2 ). This confirms
the reported mechanical properties of Müssig et al. [19] and shows that the IFFS
does not only depend on the fibre matrix adhesion but also on the fibre strength.
The low IFFS of cotton/MAPP (0.664 N/mm2 ) thus might also be explained by
the smaller fibre strength (681 N/mm2 in Müssig et al. [19]) and higher strain with
a high plastic deformation.
But as the IFFS for cotton–MAPP is even for equal fibre diameters a lot lower than
for flax–MAPP and hemp–MAPP the critical fragmentation length and therefore
the fibre–matrix adhesion is very likely to have a big influence on the IFFS. Fibre–
matrix adhesion depends on the chemical composition of the fibre. The wax layer
coating the fibre might influence the adhesion but as the exact amount of wax for
the used fibres is not known and the values from literature do not show any trend,
the influence of the wax cannot be confirmed.
Another aspect that might have an influence on the fibre–matrix-adhesion is the
lignin. It is a 3-dimensional-copolymer with aliphatic and aromatic units. Per
lignin unit 5 hydroxyl and methoxyl groups are identified [4], whereas the exact
composition still remains unclear [7]. Thus it is possible that the lignin is able to
bond with the polypropylene or the maleic anhydride, respectively. In flax fibres,
lignin is present in the middle lamella, in cell wall junctions and in the first of the
three layers forming the secondary cell wall [27]. In hemp fibres, lignin can be
localized in the primary wall-middle lamella component [28]. Although the amount
 346 T. Huber and J. Müssig

of lignin in the fibre is rather small, it still might have a significant influence as the
cellulose that is mainly responsible for the fibre–matrix adhesion, when present in
crystalline form, does not bond easily with new substances [5, 25].
As the critical fragmentation length of cotton is significantly higher than the
critical fragmentation length of flax and hemp a worse fibre–matrix adhesion can be
assumed [10, 29]. The fact the cotton fibres consist mostly of crystalline cellulose
supports the assumption that the lignin might play an important role within the
fibre–matrix adhesion [30].
But as the exact composition of the used fibres types is unknown it cannot be
finally said whether and if which role the single components play.
Another aspect that has an influence on the fibre–matrix adhesion is the mechan-
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ical interlocking between fibre surface and matrix. SEM analyses of the used bast
fibres (not presented in this paper) have shown very similar surface structures of
hemp and flax. In bigger bundles vestiges of the middle lamellae can be spotted
but as the used fibre diameters of flax and hemp are very similar it seems more
likely that the differences concerning IFFS of flax and hemp is caused by the higher
strength of the flax fibre. The mechanical interlocking between cotton fibre and
MAPP could influence the helicoidal structure of the fibre and therefore be another
reason for the lower IFFS value. The structure might chance when experiencing a
tensile load what could cause a debonding between the fibre and matrix.

4.2. Flax fibre in PLA-matrix

During the tensile load no fragments of the flax fibre in the PLA matrix could be
generated. This strongly indicates that the adhesion between fibre and PLA is not
strong enough to transmit forces from the matrix to the fibre. The SEM pictures
support this assumption, as there are no adhesive structures visible. Oksman et
al. [13] and Lanzilotta et al. cited in Plackett and Soedergård [31] also tested
flax fibres PLA composites and present similar results of weak adhesion between
flax and PLA. As Heinemann and Fritz [12] point out, the interaction between
PLA and natural fibre is supposed to be better than between natural fibre and pure
polypropylene because of its hydrophilic nature, but still not good enough to assure
a constant and sufficient load transfer from matrix to fibre.
To improve the adhesion between fibre and PLA it seems necessary to pre-process
either the matrix or the fibre. The plasma treatment of the flax fibre resulting in a
higher amount of reactive molecule groups or giving the fibre a nonporous structure
to improve mechanical locking as done at the EMPA institute [32] seems promising
as fragmentation during the tensile loading can be observed. A SEM analysis of the
different treated fibres in the PLA matrix seems reasonable to control the adhesive
mechanisms.
The good interaction between kenaf fibre and PLA reported by Nishino et al. [14]
is contradictory to the observed interactions and seems therefore strongly dependent
on the fibre used.
 Fibre–matrix adhesion of natural fibres with polymers 347

5. CONCLUSIONS

The single fibre fragmentation test provides reasonable results concerning the fibre–
matrix adhesion between natural fibres and polymers. Polypropylene combined
with a coupling agent shows good interaction with bast and cotton fibres. Hence
it is possible to calculate the mechanics of natural fibre reinforced composites with
the help of the micromechanical models and the determinable variables Lfc and τ .
Cotton as fibre made up of only cellulose and hemicellulose compared with the
bast fibres hemp and flax with lignin and pectin content indicates that the fibre
content influences the fibre–matrix adhesion.
The results of flax in combination with PLA confirm the reported poor adhesion
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of these two materials. The improvement of the adhesion with pre-processing the
fibres should be extended to different fibre types to enlarge the field of application
of biodegradable composites.

Acknowledgements
This research was done at the Faserinstitut Bremen FIBRE e.V., Bremen, Germany.
The flax fibres were provided by Egon Heger from Hostein Flachs, Mielsdorf, Ger-
many, the hemp fibres from Georg Goedecke from NAFGO, Neerstedt, Germany.
The PLA granules were provided by Martin van den Oever from A&F, Wageningen,
the Netherlands, and the MAPP granules from Markus Murr from the University of
Kassel, Germany. The support from Hanne Gerardi, Gevork Babaian and Tanja
Slootmaker from the Faserinstitut Bremen FIBRE e.V. during this research is also
acknowledged.

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