J Mater Sci (2015) 50:7660–7672
DOI 10.1007/s10853-015-9330-4
Thermo-compression forming of flax fibre-reinforced polyamide 6
composites: influence of the fibre thermal degradation
on mechanical properties
Shaoxiong Liang1 • Hedi Nouri1 • Eric Lafranche1
Received: 24 April 2015 / Accepted: 3 August 2015 / Published online: 12 August 2015
Ó Springer Science+Business Media New York 2015
Abstract The thermal degradation of plant-based fibres at
high temperature is a main issue when manufacturing vegetal
fibres/thermoplastic composites due to the high melting point
of engineering polymers such as polyamide 6 (PA6). This
paper aims at investigating the influence of the thermo-com-
pression forming process parameters, such as the temperature
and consolidation time, on the mechanical properties of con-
tinuous flax fibre-reinforced PA6 composites. Woven fabric
flax/PA6 composites were prepared by compression moulding
using a film-stacking process under different consolidation
conditions according to a two-factor Doehlert design of
experiments. Tensile and flexural properties were assessed. A
second-order polynome was used to correlate the processing
parameters and the mechanical properties (i.e. stiffness,
strength and strain at break). Fracture mode changes with the
consolidation conditions. The weakening of the fibres and
eventually of the composite performances was ascribed to the
increase in flax fibre thermal degradation.
Introduction
The development of tailored high-performance natural
fibres makes it possible to use plant-based fibre-reinforced
composites in structural or semi-structural applications
& Shaoxiong Liang
Shaoxiong.liang@mines-douai.fr
Hedi Nouri
hedi.nouri@mines-douai.fr
Eric Lafranche
eric.lafranche@mines-douai.fr
1 (2–10 wt%) [16]. Since vegetal fibres contain about
Department of Polymers and Composites Technology &
Mechanical Engineering, Mines Douai, 941 rue Charles
Bourseul CS 10838, 59508 Douai, France
123
[1–3]. Thanks to their inherent advantages such as low
density and biodegradability, with specific mechanical
properties comparable to those of glass fibres, natural fibres
such as flax, hemp, jute, sisal, pineapple and wheat are
currently industrially developed for applications in auto-
motive, tertiary, aeronautic or other cutting-edge tech-
nologies [2, 4]. Particularly, flax is a locally abundantly
available and renewable resource in Europe. Flax fibre has
better mechanical properties [2] and thermal resistance [5,
6] than other natural fibres which makes it an ideal can-
didate, among vegetal fibres, for the polymer composites
reinforcement.
Most of the studies concerning vegetal fibre-reinforced
polymer composites have been focused on thermosetting
matrices due, on the one hand to the low viscosity of the
uncured resin which results in good fabric impregnation,
and on the other hand to the low curing temperature which
is beneficial to prevent fibre thermal degradation [7–13].
Nevertheless, thermoplastic matrices offer an attractive
alternative due to their high ductility, short processing
cycle time even for complex parts and their recycling
ability. For instance, the curing process of flax/epoxy
composite has a 2–8 h duration [7–9, 14] while the con-
solidation of flax/poly(lactic acid) composite takes only
7 min [15]. Among those thermoplastic polymers,
polypropylene and polyamide are widely used in particular
in the automotive industry. However, these polymers
require a processing temperature over 170 °C, whereas the
mechanical properties of plant-based fibres are prone to be
affected above this temperature due to the presence of
thermally sensitive constituents such as cellulose
(60–70 wt%), hemicelluloses (10–20 wt%) and lignin
10 wt% water, even drying at high temperature can cause
irreversible change of the fibre structure (closure of small
J Mater Sci (2015) 50:7660–7672 7661

pores in the cellulosic structure) and decrease the fibre degradation and the mechanical properties of woven fabric
plasticity to make it more brittle [17]. This structural flax fibre/PA6 composite moulded by film stacking method.
change, associated with the cellulosic depolymerization
when exposed to high temperature, leads to mechanical
performance loss. Baley et al. [18] reported that drying at Experimental
elevated temperature leads to a significant decrease in flax
fibre tensile strength from 1500 to 870 MPa. Gourier et al. Materials
[19] studied the effect of thermal processing cycle of 8 min
at different temperatures on the flax fibre mechanical Flax woven fabric (3 9 1 twill) of 600 g m-2 (dry) was
properties, showing that the heating cycles affect the provided by Dehondt TechnologiesÒ (France) under the
mechanical behaviour by changing the shape of the stress– trade name NATTEX N/2D600 (Fig. 1).
strain curves and tensile properties. The mechanical prop- PA6 (AkulonÒ grade K222-D) was purchased from
erties are stable up to a processing temperature of 190 °C Royal DSM Company (The Netherlands). The PA6 used
and significantly drop (-30 to -66 %) at 250 °C. Besides, had a melting temperature of 220 °C and density of
Wielage et al. [20] measured a decrease of 17 and 41 % in 1130 kg m-3. The main mechanical properties of the
flax fibre tensile strength after heating cycles at 180 and polymer and flax fabrics are summarized in Table 1.
220 °C, respectively, for a period of 15 min. Thus, the
thermal degradation of the cellulosic fibres in natural fibre/ Composite materials processing
thermoplastic composites manufacturing is a main concern.
Thanks to their relatively low melting temperature Flax/PA6 composite plates of 270 9 340 9 2 mm3 were
associated with their good economical/performance bal- manufactured by compression moulding using the film
ance, natural fibre/polypropylene composites have been
widely studied especially in the form of chopped fibres
[21–29]. Regarding natural fibre/polyamide 6 (PA6) sys-
tems, a lack of studies is noticed probably due to the high
melting temperature (*220 °C) of this matrix. Ozen et al.
[30] investigated 20 wt% short flax fibre-reinforced PA6,
showing an increase in mechanical properties sufficient to
compete with the conventional glass fibre-reinforced
composites. In the case of chopped cellulose fibre/PA6 and
PA6.6 composites, Xu [31] reported a significant decrease
in strength due to the thermal degradation of the fibres. El-
Sabbagh et al. [6] prepared flax/PA6 composite by injec-
tion moulding. Tensile modulus of 50 wt% flax/PA6
composite increases up to 6 GPa compared to neat PA6
(*1.3 GPa). It is worth mentioning that the very limited
number of studies concerning flax/PA6 composites
addressed extrusion compounding followed by injection
moulding with chopped fibres. This processing method
involves short manufacturing times (‘‘compounding ? in-
jection’’ cycle) of about 8 min [19] and hence good
preservation of the fibre. However, better mechanical per-
formances can be achieved when using continuous fibres to
reinforce the composite materials. For example, a flax mat/
PLA composite fabricated by film stacking achieves a
tensile strength of 89 MPa while that of injection-moulded
short flax fibre/PLA is 46 MPa only [15].
To our better knowledge, there is nevertheless no com-
prehensive study reported in the literature detailing the
influence of processing parameters on thermal degradation
and resulting mechanical behaviour of continuous flax fibre/
PA6 composites. Thus, this paper aims investigating the effect
of process parameters (time and temperature) on the fibre Fig. 1 Nattex N/2D600 flax fibre woven fabric: a top side; b rear side

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stacking process. 0.15-mm-thick PA6 films were first Table 2 Compression moulding conditions
obtained by cast-extrusion process at a temperature of Processing parameter Set-up conditions
250 °C using a Collin single-screw extruder (Germany),
then stored at 23 °C and 50 % relative humidity (RH). Pre-heating timea Fixed 3 min
Before manufacturing, the PA6 films were dried under Pre-heating pressure Fixed 0.44 MPa
vacuum at 0.2 bar and 80 °C for 4 h. According to Santo Compression/impregnation temperature Variable 230–250 °C
et al. [33], fibre drying is not necessary for flax/PA6 pro- Compression/impregnation time Variable 2–8 min
cessing. In the present study, flax fabrics stored at 23 °C Compression pressure Fixed 2.17 MPa
and 50 % RH conditions were not dried to minimize fibre Cooling temperature Fixed 20 °C
damage due to the loss of moisture [18]. Dried PA6 films Cooling time Fixed 10 min
and two layers of flax fabric were then placed alternately in a
Pre-heating temperature is equal to that in the phase of compres-
an aluminium mould following a stacking sequence PA6/ sion/impregnation
Flax/PA6/Flax/PA6. The compression moulding was
achieved in a Dolouet press (France) according to the
processing conditions summarized in Table 2.
A second-ordered two-factor Doehlert design of exper-
iments (DOE) [34] was used to establish the relationship
between processing parameters and mechanical properties.
According to the literature, the temperature and time are
the main parameters controlling the fibre/matrix impreg-
nation quality and the fibre thermal degradation. Thus,
these parameters were chosen as processing variables in
this study. This DOE consists in distributing uniformly the
7 experimental points within the experimental domain
(Fig. 2). These points are placed in equal distance (coding
value) to each other.
This DOE uses commonly coded value (normalized
value) in order to compare the effect of the parameters
having different nature. The relation between coded value
ðXÞ and physical value ðxÞ is obtained through Eq. 1:
x  Center
X¼ ; ð1Þ
Step Fig. 2 Two-factor Doehlert DOE. The point number 8 is an extra
condition
where Step ¼ ðxmax  xmin Þ=2 and Center ¼ ðxmax þ
xmin Þ=2, where xmax and xmin are the ultimate values of
parameter x. This method allows to establish a second- Y ¼ a0 þ a1 X1 þ a2 X2 þ a11 X12 þ a22 X22 þ a12 X1 X2 ; ð2Þ
ordered polynomial relation (Eq. 2) between the response
ðYÞ (mechanical properties), and the experimental vari- where an are the regression coefficients to be determined,
ables (compression moulding temperature ðX1 Þ and com- and a0 is the average experimental response. Graphically,
pression time ðX2 Þ) Eq. 2 is a three-dimensional spherical surface.
According to the two-factor Doehlert DOE, the pro-
cessing conditions of different experimental points (N°1 to
Table 1 Mechanical properties of the dried and conditioned (23 °C, N°7) are presented in Table 3. The specimens are desig-
50 % RH) materials
nated according to their processing conditions (e.g.
PA 6 Flax fibre [32] 230d5mn corresponds to sample cut from a flax/PA6
Dry Conditioned composite plate moulded at 230 °C for 5 min).

Tensile modulus (GPa) 3.8 1.2 54 Mechanical testing

Yield tress (MPa) 95 55 –
Yield strain (%) 3.5 25 – Rectangular samples of 250 9 25 9 2 mm3 were cut for
Stress at break (MPa) 1339 tensile testing according to ISO 527-4 standard. No end-
Flexural modulus (GPa) 2.6 – taps were used. Tensile properties were measured using a
Flexural strength (MPa) 100 – 100 kN tensile machine (Instron 8501, UK) with a

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J Mater Sci (2015) 50:7660–7672
Table 3 Composite materials processing variables
Experiment number Composite reference Processing temperature
Physical value x1 (°C)
1 230d5mn 230
2 240d5mn 240
3 250d5mn 250
4 235d2mn 235
5 235d8mn 235
6 245d2mn 245
7 245d8mn 245
8a 230d2mn 230
a
Extra condition
crosshead speed of 2 mmmin-1 at 23 °C and 50 % RH.
Five specimens were tested for each processing condition.
The average value and the standard deviations (SD) were
reported. For Young’s modulus measurement, a digital
image correlation (DIC) method was used in order to
improve the precision of the strain measurement (cf
‘‘Young’s modulus’’ section). An Allied camera (Germany)
of 4 M pixel resolution associated with the Vic-2D 2009
software was used for the strain measurement.
Three-point bending tests were performed using an
Instron 1185 machine (UK) equipped with a 1 kN force
cell. The sample dimension was 40 9 15 9 2 mm3 and the
span/depth ratio 16/1 (32 mm in span), according to the
ISO 14125 standard. Ten specimens were tested per con-
dition. The average values and the standard deviation were
reported.
All (tensile and flexural) specimens were cut using a
Charly-4U milling robot (France) with a 2-mm steel drill.
Samples were firstly conditioned under vacuum of 0.2 bar
and 50 °C for 72 h, then at 23 ± 3 °C and 50 ± 5 % RH
for 360 h before mechanical testing.
Microscopy observation
A Leica DM 2500 M microscope and a Leica DFC420
camera (USA) were used for the observation of the com-
posite impregnation quality. A Philips SEM 525 M scan-
ning electron microscope (SEM) (The Netherlands) was
used to observe fracture surfaces of flax/PA6 composites
sputtered with a thin layer of gold.
Thermal gravimetric analysis (TGA)
Thermal gravimetric analysis (TGA) was performed to
evaluate the flax fibre and PA6 thermal degradation. The
measurements were carried out using a Mettler Toledo
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Compression time
Coded value X1 Physical value x2 (min) Coded value X2
-1 5 0
0 5 0
1 5 0
-0.5 2 -0.866
-0.5 8 0.866
0.5 2 -0.866
0.5 8 0.866
-1 2 -0.866
TGA/DSC1 device (USA) in a 10 mlmin-1 constant
nitrogen flow. The heating rate was 10 °C min-1 over a
temperature range from 25 to 700 °C. Isothermal gravi-
metric analysis was conducted for flax fibre and for PA6 at
three constant temperature levels (230, 240 and 250 °C).
The weight loss was measured during 12 min.
Rheological characterization
Capillary flow measurements were carried out on a capil-
lary rheometer (Model 75 Rheograph, Göttfert, Germany)
at 230, 240 and 250 °C in the range of 10 to 104 s-1 with a
1-mm-diameter die. The length/diameter (L/D) ratios of the
capillary were 20, 40 and 60. The apparent viscosity
obtained was corrected for both the non-Newtonian beha-
viour (Rabinowitsch correction) and the elastic effect
(Bagley correction). The curves were interpolated accord-
ing to the Carreau Yasuda law (Fig. 3).
Results and discussion
Impregnation and porosity
Before mechanical analysis, optical microscopy observa-
tions were carried out in order to ensure the good fibre
impregnation and an acceptable porosity level in the
composites. Figure 4 shows a representative optical
micrograph of the composites. The flax woven fabric used
was composed by a majority of technical fibres (fibre
bundles) rather than by elementary separated fibres (fila-
ments). A very good fibre impregnation quality, even in
fibre rich area (Fig. 4a), is observed. Limited air pocket
porosities are visible (Fig. 4b), representing less than 1 %
of the area of a total of 75 microscope images. It is well
known that the presence of porosity has a negative effect
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on the mechanical performance of composite materials.
Using the correction factor ð1  Vp Þ2 proposed by Madsen
et al. [35] for plant-based fibre composites, with Vp the
porosity volume fraction, 1 % void fraction can have 2 %
Fig. 3 Capillary rheological behaviour of PA6
Fig. 4 Optical micrographs of the fibre/matrix impregnation quality:
a impregnation in fibre rich area, b air pocket porosity
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J Mater Sci (2015) 50:7660–7672
influence on the stiffness of the composite, which is small
and can be neglected compared to the differences observed
between samples consolidated under different processing
conditions (‘‘Mechanical behaviour’’ section). Therefore,
the influence of the porosity is ignored in the following
discussion.
Young’s modulus
The main difficulty to evaluate the elastic modulus of the
studied composite materials comes from the fabric struc-
ture itself (size and linear weight of the fibre strand)
inducing local inhomogeneity represented by the distribu-
tion of plastic zones (matrix accumulations) and elastic
zones (continuous fibre strands). Thus, a 12.5-mm strain
extensometer (Ext.) placed on the sample edge or strain
gauges (KFG-10-120-C1-11L1M2R unidirectional strain
gauge) attached on the composite surface (GC) can exhibit
a discrepancy in strains measurement (Fig. 5b).
Figure 5a illustrates a typical longitudinal strain field
obtained by DIC. Because of the large size of the flax
strands (7–8 mm width) and the 3/1 twill woven architec-
ture of the fabric (Fig. 1), the strain field is particularly
heterogeneous. In order to increase the accuracy of the
strain measurement, longitudinal strains were calculated by
DIC. Three virtual strain gauges of 3 9 10 mm2 corre-
sponding to the above-mentioned unidirectional strain
gauge size were defined and placed at the centre (GC) and
at locations where the maximum (GMax) and minimum
(GMin) strains were measured. Also, a global strain (Glb)
was calculated corresponding to the average values of a
20 9 90 mm2 area located in the middle of the sample.
The tensile stress–strain curves recorded from different
measurement methods and locations were compared in
Fig. 5b. The strain measured by the gauge located at the
centre (GC) shows higher values than the global strain
Fig. 5 Tensile strain measurement with different methods: a longitu-
dinal tensile strain field, by DIC; b tensile stress–strain curves using
different methods
J Mater Sci (2015) 50:7660–7672
(Glb) due to a high strain zone nearby. The extensometer
records lower strain (Ext.) than the global strain (Glb) due
to the influence of a low strain area. This discrepancy in
strain measurement can highly affect the mechanical
properties yielded from these curves in particular when the
Young’s modulus is considered.
Finally, the influence of gauge size on the strain mea-
surement by DIC was studied by varying the gauge size
from 5 9 5 to 20 9 90 mm2. The gauge shape was also
changed from square to rectangular for size bigger than
20 9 20 mm2 due to the specimen width limitation. Strains
have been measured in several random locations on the
surface of the same specimen according to different gauges
sizes. The strain at break is plotted as function of the gauge
size in Fig. 6. The scattering of the strain measurement
decreases when the gauge size increases. A convergence
towards the average value is noted from gauge sizes of
20 9 80 mm2. Logically, smaller gauge sizes provide more
precise local information of the specimen behaviour.
However, the present paper focuses on the global behaviour
of the flax/PA6 composite. Therefore, all strain data will be
calculated hereafter using the 20 9 90 mm2 gauge size.
Mechanical behaviour
The tensile and flexural stress–strain curves of composites
having the highest and lowest mechanical performance are
Fig. 6 Convergence of the strain measurement as function of the
gauge size
7665
plotted in Fig. 7. The tensile stress–strain curves show a
knee point at about 0.1 % of strain. This change of slope is
commonly observed for continuous flax fibre-reinforced
composites [7] and attributed to the flax fibre tensile
behaviour [18, 32].
Due to the complex combination of normal and shear
stresses in the sample and the smaller size of the flexural
specimens compared to that of the tensile ones, the flexural
curves show larger scattering.
For both tensile and flexural tests, a significant gap in
terms of strength and strain at break can be observed
(Fig. 7) between the two sets of composites having the
highest and the lowest performances, respectively, refer-
enced as 230d2mn and 250d5mm. Whereas the elastic
moduli of both composites, calculated as the linear
regression slope of the stress–strain curves in the strain
range of 0.05–0.25 %, are very similar.
The tensile and flexural properties of the neat PA6 and
flax/PA6 composites consolidated in the experimental
domain are reported in Table 4. Lower values in tensile
properties are noticed for neat PA6 compared to those of
fully dried PA6 (Table 1) due to the drying conditions
Fig. 7 a Tensile and b flexural stress–strain curves of 230d2mn and
250d5mn composite samples
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used in this study (cf ‘‘Composite materials processing’’
section).
The Young’s moduli of the composites are above
10 GPa and the flexural moduli are higher than 8 GPa,
indicating a significant reinforcement effect brought by the
flax fabric. Besides, their variations in the experimental
domain, from 10.4 to 12.7 GPa (22 %) for Young’s mod-
ulus and from 8 to 9.1 GPa (14 %) for the flexural modulus
indicate a minor influence of the time/temperature param-
eters on these properties within the experimental domain.
The strain at break of 0.29–0.92 % (i.e. 217 % differ-
ence) in tension and 1.01–2.63 % (i.e. 160 % difference) in
bending shows a particular sensitivity on these two pro-
cessing parameters [15, 33, 36]. Indeed, the temperature
and time directly affect the mechanical properties of the
vegetal fibre reinforced composites. In general, lower
temperature and shorter processing time lead to higher
composite performance [15, 36]. The tensile strength of
230d2mn composites shows a significant improvement
compared to that of neat PA6 (?30 %), whereas it is 53 %
lower than neat PA6 when flax/PA6 was consolidated at
250 °C, 5 min (250d5mn). In the same way, in bending,
the samples moulded with the lower temperature (230 °C)
and shorter consolidation time (2 min) display the highest
flexural strength (?60 % compared to neat PA6).
Although the high viscosity of the PA6 matrix (Fig. 3)
should induce an increase of either processing temperature
or compression time, the preservation of flax fibre from
thermal degradation requires a temperature and time
reduction. The results of the extra experimental point
(230d2mn), which is consolidated at the lowest tempera-
ture and shortest time within the experimental domain,
confirm thus a significant increase in composite properties.
Analysis of the DOE response surfaces
The coefficients of the polynomial representation (Eq. 2),
identified for the DOE response surfaces of the mechanical
properties of the flax/PA6 composites are reported in
Table 5. The statistical analysis confirms the significance
of all coefficients, with the exception of a12 for tensile
modulus and a11 for flexural modulus, which are non-sig-
nificant for a significance level (p value) of 5 %. The sig-
nificant coefficients of the non-zero second-ordered terms
(a11 and a22 ) indicate that the influence of time and tem-
perature on the mechanical properties is non-linear. The
interaction term (a12 ) reveals that the effects of compres-
sion time and heating temperature on the mechanical
properties are dependent on each other.
The response surfaces as well as the experimental results
(spherical points) are plotted in Figs. 8 and 9. All response
surfaces, with the exception of the flexural moduli, indicate
better performances with a decrease in the moulding tem-
perature and compression time. Hence, the extra experi-
mental sample 230d2mn has the highest strength and strain
under both loading types (Table 4). The predicted results
correlate well with the experimental ones (Table 4). The
experimental tensile modulus of 230d2mn sample is not
higher than that of 230d5mn (longer processing time) or
235d2mn (higher temperature) ones. This can be explained
by the fact that, for this property, the experimental results
between composites manufactured under different pro-
cessing conditions are quite close. In fact, both the response
surfaces of tensile and flexural moduli are relatively flat,
and they have small coefficients (a1 ; a2 ; a11 ; a22 and a12 )
with respect to the average value a0 (Table 5). According to
the literature [36], the modulus is less influenced by the

Table 4 Mechanical properties (average value ± standard deviation) of the flax/PA6 composites, PA6 and corresponding predictions
Material Tensile properties Flexural properties
Modulus (GPa) Strength (MPa) Max strain (%) Modulus (GPa) Strength (MPa) Strain at max stress (%)

230d5mn 12.7 ± 1.2 68.7 ± 3.7 0.64 ± 0.08 9.13 ± 1.53 133 ± 22 2.41 ± 0.31
240d5mn 11.5 ± 0.9 42.2 ± 2.6 0.39 ± 0.03 8.40 ± 1.28 89 ± 13 1.37 ± 0.27
250d5mn 11.0 ± 0.5 32.2 ± 2.4 0.29 ± 0.03 8.00 ± 1.59 66 ± 13 1.01 ± 0.14
235d2mn 12.2 ± 0.3 76.7 ± 2.1 0.78 ± 0.08 8.37 ± 1.44 125 ± 20 2.13 ± 0.35
235d8mn 10.8 ± 0.5 40.2 ± 5.5 0.40 ± 0.07 9.68 ± 1.27 90 ± 18 1.22 ± 0.26
245d2mn 11.6 ± 0.4 54.4 ± 2.9 0.54 ± 0.04 8.55 ± 1.05 102 ± 13 1.65 ± 0.29
245d8mn 10.4 ± 1.5 33.9 ± 4.5 0.36 ± 0.02 8.81 ± 1.02 75 ± 8 1.16 ± 0.20
230d2mn 12.0 ± 1.0 90.2 ± 3.6 0.92 ± 0.02 8.34 ± 0.98 140 ± 16 2.63 ± 0.20
PA6 2.91 ± 0.2 68.4 ± 2.6 19.2 ± 0.5 2.10 ± 0.03 88 ± 1 6.79 ± 0.07
P230d2mna 13.0 96.7 0.99 8.54 154 2.92
a
Response surfaces of the DOE for 230d2mn sample

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Table 5 Identified coefficients of the polynomial response for different mechanical properties
Coefficient Tensile properties
Modulus (GPa) Strength (MPa) Max. strain (%)
a0 11.51 42.22 0.388
a1 -0.74 -16.91 -0.165
a2 -0.76 -16.46 -0.162
a11 0.36 8.22 0.080
a22 -0.50 9.38 0.151
a12 0.16a 9.23 0.121
a
Non-significant value (p value \ 5 %)
processing parameters than the strength and strain due to its
lower sensitivity to the adhesion quality between fibres and
matrix.
From these response surfaces, it is clear that, mechanical
properties decrease when moulding temperature and com-
pression time increase. Both parameters favour the thermal
degradation of the natural flax fibre [19, 20].
The best mechanical properties of flax/PA6 composite
tensile strength (90.2 MPa) and flexural strength
(140 MPa) are significantly higher than those of neat PA6
(68.4 MPa in tension and 88 MPa in bending). It is worth
noting that, this composite material was consolidated under
230 °C/2 min conditions; the total processing time of
5 min (3 min for preheating and 2 min for consolidation) is
long compared to that of injection-moulded small plastic
parts (several seconds to tens of seconds) but in the same
range (several minutes) as that of injection-moulded big
automotive components. Nevertheless, the processing cycle
is shorter than that of plant-based fibre/thermoplastic
composites (7–22 min [2, 15, 19]) generally found in the
literature. Using thermoplastic polymers compared to
thermosetting resins as composite matrix makes it possible
to reduce processing time (several hours [9, 11, 18]) and
warrants recyclability of the material.
Fracture surfaces
Figure 10 shows the SEM images of the tensile fractured
surfaces of composites processed under different condi-
tions of the Doehlert DOE. The processing conditions have
a significant influence on the fracture behaviour of the
composites. With the increase of temperature (i.e. Fig. 10a
to b, c to e, f to g) as well as the compression time (i.e.
Fig. 10f to a, g to b), the length of the fibre pull out
decreases. In the case of the most severe conditions
(250 °C, 5 min), the flax fibres were broken just near the
transverse fracture plane (Fig. 10 e) indicating a resistance
of the flax fibre lower than that of the fibre/matrix interface.
7667
Flexural properties
Modulus (GPa) Strength (MPa) Strain at max. stress (%)
8.40 89.35 1.365
-0.49 -28.62 -0.551
0.45 -18.18 -0.404
a
0.17 10.81 0.351
0.55 8.32 0.117
-0.61 4.23 0.247
Thermal analysis of flax fibre and PA6
TGA of flax fibre and PA6 matrix is reported in Fig. 11.
According to the literature [23, 37–39], flax fibre is char-
acterized by four weight loss stages. The first one corre-
sponds to the water release (dehydration) corresponding to
the moisture weight in the material, which is approximately
5 % in our case. The second stage characterized by a
weight loss starting at around 200 °C with a plateau
(shoulder) at 260 °C, corresponds to the hemicelluloses
degradation. The major weight loss starts at 260 °C with a
maximum peak value at 350 °C and the end at 385 °C.
This stage is linked to the cellulose pyrolysis. Afterwards,
the weight continues to decrease in a stable way until the
end of the scanning temperature which is 700 °C related to
the non-cellulosic substances [37] (such as lignin and sugar
Maillard derivatives).
The TGA leads to the conclusion that the lignin is more
thermally stable than hemicelluloses and cellulose with a
decomposition temperature range of 150–900 °C [40, 41].
Besides, Yang et al. [40] have demonstrated that the ther-
mal degradation of these components depends on their
inherent structures and chemical nature. The hemicellulose
is constituted of various random and amorphous polysac-
charides which can be easily removed at low temperature,
while the cellulose is constituted of highly ordered glucose,
a polymer without branches giving high thermal stability.
The lignin formed of aromatic rings associated with vari-
ous branches shows a wide degradation temperature range
[40]. The residual weight of 20 % currently observed at the
end of the TGA test (700 °C) is consistent with the values
reported in the literature [23].
The TGA and DTGA curves of PA6 show a first mass
loss (2.1 %) corresponding to the presence of water in the
matrix [42]. The beginning of decomposition is noticed at
370 °C and reaches a maximum rate at 455 °C much
higher than those of flax fibre. Moreover, isothermal TGA
curves (Fig. 12) of the PA6 indicate a minor weight loss of
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Fig. 8 Response surfaces of

tensile properties of flax/PA6
composites as a function of
compression time and heating
temperature: a Young’s
modulus, b tensile strength,
c maximum tensile strain. Each
point represents an experimental
result

about 0.2 % during the first 10 min at 250 °C. The thermal The isothermal gravimetric analysis (Fig. 12) of flax
degradation of the matrix does not seem to happen under fibre shows a non-linear mass loss, the thermal degrada-
the present composite processing conditions (230–250 °C tion increasing as a function of the processing time. The
for several min). mass loss caused by the fibre dehydration is not taken into

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Fig. 9 Response surfaces of

flexural properties of flax/PA6
composites as a function of
compression time and heating
temperature: a flexural modulus,
b flexural strength, c flexural
strain at maximum stress. Each
point represents an experimental
result

account here due to the preheating period of the apparatus 250 °C, indicating a decrease in the kinetic of
(3 min) where the water contained in the flax fibre is degradation.
vaporized. According to Fig. 12, the flax fibre mass loss is Regarding the experimental domain, the composite
higher between 230 and 240 °C than between 240 and plates were moulded between 230 and 250 °C for 2 to

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Fig. 10 SEM images of tensile

fractured surfaces for different
processing conditions of the
Doehlert DOE

Fig. 11 Thermal gravimetric analysis of the PA6 and flax fibre

Fig. 12 Isothermal gravimetric analysis of the PA6 and flax fibre

8 min. Thermal degradation should have occurred in flax Conclusion

fibres. In the elementary flax fibre, the cellulose forms
crystalline mesofibrils, structured in spirals within amor-
phous matrix made of hemicelluloses while the lignin acts
as an adhesive between them [32, 43]. The decomposition
of lignin and hemicelluloses destroys the fibrils network
and hence results in the drop in the mechanical properties
of the reinforcement fibre and consequently the mechanical
properties of the composites.
The thermo-compression moulding of flax fibre fabric-re-
inforced PA6 was experimentally investigated in order to
minimize the thermal degradation of the flax fibres during
processing. The influence of the processing temperature
and time on the tensile and flexural mechanical behaviour
was evaluated using a second-ordered two-factor Doelhert
DOE.

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The DOE response surfaces of the mechanical properties
of flax/PA6 composites have shown a decrease in perfor-
mance when the consolidation temperature and time
increase. The increase of the temperature from 230 to
250 °C and of the time from 2 to 5 min results in a drop of
tensile strength of the flax/PA6 composite from 90.2 to
32.2 MPa (-64 %). The dependence of the mechanical
properties on the processing parameters is non-linear.
The mechanical strengths of flax/PA6 composite con-
solidated at 230 °C, 2 min are significantly higher than
those of the neat PA6 (?32 % in tension and ?60 % in
bending). The total processing time of 5 min (3 min for
preheating and 2 min for consolidation) is shorter than
those usually used to prepare vegetal fibre/thermoplastic
composite materials reported in the literature (7–22 min).
The fracture mode of the composites (length of fibre
pull-out) depends on the severity of the processing condi-
tions. The TGA has highlighted four decomposition stages
of the flax fibre: dehydration (25–150 °C), decomposition
of hemicelluloses (200–260 °C), cellulose (260–385 °C)
and lignin (from 170 °C). Also, the time/temperature
dependence in the flax fibre degradation process was con-
firmed. A maximum loss of 3.5 % in mass is measured for
flax fibres exposed at 250 °C for 11 min.
Acknowledgements Thanks are due to Dehondt TechnologiesÒ
(France) for kindly supplying flax fibre fabric (Nattex N/2D600) and
to the Nord-Pas-de-Calais Region (France) for funding Hedi Nouri’s
post-doctoral grant (Contract No. 14002212). The authors also
acknowledge International Campus on Safety and Intermodality in
Transportation (CISIT), European Community (FEDER) and Nord-
Pas-de-Calais Region for funding the TGA equipment.
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