coatings
Article
Elaboration by Wrapping Process and Multiscale
Characterisation of Thermoplastic Bio-Composite Based on
Hemp/PA11 Constituents
Chaimae Laqraa * , Manuela Ferreira






Citation: Laqraa, C.; Ferreira, M.;
Rashed Labanieh, A.; Soulat, D.
Elaboration by Wrapping Process and
Multiscale Characterisation of
Thermoplastic Bio-Composite Based
on Hemp/PA11 Constituents.
Coatings 2021, 11, 770. https://
doi.org/10.3390/coatings11070770
Academic Editor:
Fengwei (David) Xie
Received: 1 June 2021
Accepted: 24 June 2021
Published: 26 June 2021
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Copyright: © 2021 by the authors.
Licensee MDPI, Basel, Switzerland.
This article is an open access article
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Attribution (CC BY) license (https://
creativecommons.org/licenses/by/
4.0/).
Coatings 2021, 11, 770. https://doi.org/10.3390/coatings11070770
, Ahmad Rashed Labanieh and Damien Soulat
Centrale Lille, Laboratoire de Génie et Matériaux, Gemtex, Ensait, F-59000 Roubaix, France;
manuela.ferreira@ensait.fr (M.F.); ahmad.labanieh@ensait.fr (A.R.L.); damien.soulat@ensait.fr (D.S.)
* Correspondence: chaimae.laqraa@ensait.fr; Tel.: +33-7-67-49-99-22
Abstract: The present work investigates the potential of developing bio-composites based on ther-
moplastic polymers reinforced with natural fibres by using hybrid yarns. The hybrid yarns were
produced by the wrapping technique, in which a multifilament of polyamide 11 (PA11) was wrapped
around an untreated low-twisted hemp roving to produce a yarn with sufficient tenacity and stiffness
for the next step of weaving. The tensile behaviour of the wrapped yarns was identified both in the
dry- and thermo-state. Then, two different fabrics were woven and tested to study the influence
of yarn densities and weave diagrams on the tensile and flexural properties. At this fabric scale,
properties of fabrics made from hybrid yarns were compared with those of fabrics from a previous
study made from 100% hemp roving. Composites made from these fabrics, with stacking of two
cross-plies, were produced by thermocompression and characterised regarding mechanical strength.
Keywords: hybrid yarns; hemp; PA11; woven fabric; bio-based composite; mechanical characterisa-
tion
1. Introduction
Among plant fibres, flax (Linum Usitatissimum L.) and hemp (Cannabis Sativa) fibres
are now the two most-produced bast fibres in Europe [1]. Due to their properties, such
as important environmental advantages, good specific mechanical properties, and often
a viable cost [1], these fibres have emerged as an alternative to synthetic fibres, and the
use of plant fibre composites (PFCs) has become a market reality [2–4]. Despite numerous
similarities (cell wall, thicknesses, and numbers of layers/sub-layers, biochemical composi-
tion, cellulose microfibril angle, MFA), these two bast fibres generally exhibit differences
in their tensile properties and their global tensile behaviour. Flax fibres generally have
slightly better tensile properties than hemp fibres, especially in terms of tensile strength
and stiffness; on the other hand, they reach a lower tensile strain at failure than hemp [5]. If
a lot of studies are conducted at the scale of fibres to explain these differences [1,5–7], few
papers are dedicated to the development of hemp-continuous fabrics used as reinforcement
of composite samples [4,8,9]. This deficit for hemp could be attributed to technological
barriers, such as fibre separation and the alignment of fibres throughout the transformation
process and consequently the unavailability of these products on an industrial scale [10].
Hemp fibres are naturally discontinuous; therefore, hemp reinforcements have so far been
based on twisted yarns of staple fibres by means of long-staple spinning techniques, mainly
ring spinning. However, the high twist level in the yarns leads to fibre misalignment in
composite materials and thus reduced stiffness. Furthermore, the high twist level compacts
the yarn section and reduces the inter-fibre gaps, making it very difficult for the resin to
penetrate inside the yarn structure [11]. Therefore, the use of very low twisted yarns is
advised for composite application [12,13]. However, a low twist implies poor inter-fibre
cohesion, and the yarn loses its otherwise good weaveability properties which are due to
good tenacity and low hairiness.
https://www.mdpi.com/journal/coatings
Coatings 2021, 11, 770 2 of 16

Along with this fibrous reinforcement, the challenge is to identify new combinations
of raw materials for the production of green composites whose performance is good
enough to propose their use in suitable applications. Among the various bio-based ther-
moplastic resins, polyamide 11 (PA11) is a semi-crystalline bio-polyamide produced using
11-aminoundecanoic acid derived from castor oil and has gained a special industrial interest
due to a good combination of mechanical properties and chemical resistance [14]. In partic-
ular, PA11 exhibits good toughness, compared to other bio-based thermoplastic resins, such
as, polylactic acid (PLA), which is often proposed as a matrix for bio-composites [15,16]. The
natural fibre/PA11 combination has been used to study the performance of bio-composites.
Haddou et al. [17] associated long bamboo fibres with PA11 films to analyse the tensile
behaviour. Gourrier et al. [18] studied the tensile, impact, and thermal properties of unidi-
rectional flax tape with PA11 films. In these studies, composites were made by film stacking,
but other processes offer a route for efficient manufacturing of thermoplastic composites
due to the reduced flow distance of resin in reinforcement to optimise impregnation. Awais
et al. [19] compared tensile, flexural and impact behaviour of commingled fabrics (woven
and knitted) based on jute/flax/hemp fibres with PP yarns. To improve the impregnation of
thermoplastic resin into fibre yarns, Kobayashi et al. [20] used the micro-braiding method
to mix hemp roving and PLA multifilament in the yarns. These micro-braided yarns
were placed in a pre-heated moulding die for consolidation by compression moulding to
produce composite specimens. Zhai et al. [21] compared yarn morphologies, structures,
mechanical tensile properties, and braidabilities of commingled flax/PP yarns obtained
by micro-braiding or wrapping methods. In the wrapping process [22,23], a thermoplastic
multifilament is wrapped around hemp roving, resulting in increased inter-fibre friction
and improved yarn cohesion. This manufacturing process was successfully used by Corbin
et al. [8] to produce a commingled yarn based on hemp roving and PA12 multifilament
and associated woven fabrics and composite samples. In all of these studies, although
the mechanical and thermal properties of thermoplastic polymers are described, as in Di
Lorenzo et al. [24], few papers [25] deal with the identification of the thermomechanical
properties of commingled yarns, which can be essential to improve parameters of impreg-
nation during the thermocompression process. This paper deals with hemp roving and
PA11 multifilament and describes the wrapping process, and how the hybrid yarns are
used to weave fabrics. Composite samples reinforced by these fabrics were manufactured
by thermocompression. The tensile properties of these commingled yarns were studied
according to temperature and strain rates, and the mechanical properties of the woven
fabrics and the composite samples were identified.

2. Materials and Methods

2.1. Materials
An extruded PA11 multifilament yarn produced at GEMTEX Laboratory was used as
the matrix material and as the wrapping material for the production of the hybrid yarn. The
PA11 yarn was made from Rilsan® PA11 pellets supplied by Arkema, Colombes, France.
This thermoplastic matrix has a density of 1.03 g/cm3 , a melt temperature of 190–195 ◦ C,
and a glass transition temperature of 55–60 ◦ C. Hemp roving with a twist of 37 turns per
meter (TPM) was used as the core yarn of the hybrid yarns. This untreated roving was
supplied by the Italian company Linificio e Canapificio Nazionale, Villa d’Almè, Italy. The
main properties of these yarns are shown in Table 1.

Table 1. The main properties of the raw materials.

Linear Density Deformation at

Yarns Density (g/cm3 ) Twist Level (tpm) Tenacity (cN/Tex)
(Tex) Break (%)
Hemp roving 1.50 312 ± 19 37 ± 2 10.09 ± 2.48 3.67 ± 0.42
PA11 1.03 111 ± 3 – 27.02 ± 0.95 35.02 ± 5.43
 2.2.1. Manufacturing of Hemp/PA11 Hybrid Yarns
The hemp/PA11 hybrid yarns were produced by the wrapping process, on a hollow
spindle machine, Gualchieri e Gualchieri shown in Figure 1. In the wrapping process, the
thermoplastic multifilament yarns (PA11) are wrapped around low twisted and untreated
Coatings 2021, 11, 770 3 of 16
hemp roving. These wrapping yarns will melt during the thermocompression process,
thus forming the matrix part of the composite material. The wrapping process is mainly
used to increase the inter-fibre cohesion of the core yarn to sustain the tension loads ap-
plied during the transformation
Their linear into reinforcement.
density was measured accordingFurthermore, the outer
to the NF G07-316 wrapped
standard [26],yarn
the
protects the core yarn from rubbing aggression when passing machinery
twist level according to the NF G07-079 standard [27], and tenacity at break according to surfaces during
these
the NF processes.
EN ISO 2062These manufacturing
standard [28]. loads represent the basic required weaveability
conditions.
2.2. During
Methodsproduction, the hemp roving passes through a roving condenser and drafting
2.2.1. Manufacturing
rollers and then is guided of Hemp/PA11 Hybrid
inside the hollow Yarns together with the PA11. The PA11 is
spindle
wrapped around the core roving by
The hemp/PA11 hybrid yarns were producedrotational movement
by theof the hollow
wrapping spindle
process, ontoa obtain
hollow
the wrapped
spindle hemp/PA11
machine, Gualchieri yarn. During the
e Gualchieri wrapping
shown process,
in Figure 1. In the
the ratio between
wrapping hollow
process, the
spindle rotational
thermoplastic speed and yarns
multifilament yarn delivery speed
(PA11) are wrappeddetermines
aroundthelowPA11 wrapping
twisted turns
and untreated
per
hempmeter and These
roving. the mass proportion
wrapping yarnsofwill
twomelt
yarns for athe
during given linear density. As
thermocompression output,thus
process, to
obtain
forming the matrix part of the composite material. The wrapping process is mainly used a
the desired hybrid yarns with a mass ratio of hemp between 43% and 60% and to
tenacity
increaseallowing its weaveability,
the inter-fibre cohesion of thethe wrapping turn
core yarn to number
sustain and spindle
the tension loadsspeed areduring
applied fixed
atthe
500transformation
tpm and 5000 turns/min, respectively.
into reinforcement. The linear densities
Furthermore, the outerofwrapped
the hybrid yarns
yarn were
protects
measured according
the core yarn to the NFaggression
from rubbing G07-316 standard [26], and
when passing the twist level
machinery according
surfaces duringtothese
the
NF G07-079These
processes. standard [27].
manufacturing loads represent the basic required weaveability conditions.

Thewrapping
Figure1.1.The
Figure wrappingprocess.
process.

During production,
2.2.2. Weaving theHemp/PA11
Process with hemp rovingYarns
passes through a roving condenser and drafting
rollers and then is guided inside the hollow spindle together with the PA11. The PA11 is
The hybrid yarns were woven on a Leclerc Weavebird manual loom in the GEMTEX
wrapped around the core roving by rotational movement of the hollow spindle to obtain
laboratory (Roubaix, France). After the different preparation steps of the weaving process
the wrapped hemp/PA11 yarn. During the wrapping process, the ratio between hollow
spindle rotational speed and yarn delivery speed determines the PA11 wrapping turns
per meter and the mass proportion of two yarns for a given linear density. As output, to
obtain the desired hybrid yarns with a mass ratio of hemp between 43% and 60% and a
tenacity allowing its weaveability, the wrapping turn number and spindle speed are fixed
at 500 tpm and 5000 turns/min, respectively. The linear densities of the hybrid yarns were
measured according to the NF G07-316 standard [26], and the twist level according to the
NF G07-079 standard [27].

2.2.2. Weaving Process with Hemp/PA11 Yarns

The hybrid yarns were woven on a Leclerc Weavebird manual loom in the GEMTEX
laboratory (Roubaix, France). After the different preparation steps of the weaving process
(warping and drawing-in), two woven fabrics with different weaving diagrams were
produced, twill 6 weft effect and satin 6 weft effect. The two fabrics were woven with the
Coatings 2021, 11, 770 4 of 17

Coatings 2021, 11, 770 4 of 16

(warping and drawing-in), two woven fabrics with different weaving diagrams were pro-
duced, twill 6 weft effect and satin 6 weft effect. The two fabrics were woven with the
same hybrid yarns in both directions and have the same warp density at 6 yarns/cm but
same hybrid
different weft yarns in both
densities, directions
namely, and have
11 yarns/cm forthe same
twill warp
6 and density at
6 yarns/cm for6 satin
yarns/cm
6. but
different weft densities,
The textile properties namely, 11fabrics
of these yarns/cm for twill
in terms 6 and
of yarn 6 yarns/cm
densities, arealfor satin 6.thick-
density,
The air
ness, and textile propertieswere
permeability of these fabricsand
identified in terms
will be of presented
yarn densities,
later.areal
Arealdensity,
densitythick-
was
ness, and air permeability were identified and will be presented later.
measured according to the NF EN 12127 standard [29], thickness according to NF EN ISO Areal density was
measured according to the NF EN 12127 standard [29], thickness according
5084 standard [30], and air permeability according to the NF EN ISO 9237 [31]. The crimp to NF EN ISO
5084 of
level standard
warp and [30],weft
andyarns
air permeability
after weavingaccording to the NFfor
was measured ENboth
ISO fabrics
9237 [31]. The crimp
according to
level
the NFofISO
warp and weft
7211-3 yarns[32].
standard after weaving was measured for both fabrics according to the
NF ISO 7211-3 standard [32].
2.2.3. Composite Manufacturing
2.2.3. Composite Manufacturing
Composite plates based on hemp/PA11 satin 6 fabric and hemp/PA11 twill 6 fabric
Composite plates
were manufactured based on hemp/PA11
by thermocompression satin 6 fabric
moulding on anand
Agilahemp/PA11
Press 100 kN twill 6 fabric
hot-press
were manufactured by thermocompression moulding on an Agila Press 100 kN hot-press
(Menen, Belgium). The fabrics were cut into 300 × 300 mm2 2squares and conditioned at a
(Menen, Belgium). The fabrics were cut into 300 × 300 mm squares and conditioned at a
temperature of 23 °C and relative humidity of 50% for at least 24 h prior to the composite
temperature of 23 ◦ C and relative humidity of 50% for at least 24 h prior to the composite
manufacturing. For the two types of fabrics, two cross-plies (0/90°) were◦ stacked, as shown
manufacturing. For the two types of fabrics, two cross-plies (0/90 ) were stacked, as
in Figure 2a. Then, they were placed between two Teflon-coated plates. The melting tem-
shown in Figure 2a. Then, they were placed between two Teflon-coated plates. The
perature of PA11 is 190 °C and the degradation temperature of hemp roving is 276 °C [8];
melting temperature of PA11 is 190 ◦ C and the degradation temperature of hemp roving is
therefore,
◦ to produce the composite plates, the process temperature was fixed at 200 °C to
276 C [8]; therefore, to produce the composite plates, the process temperature was fixed at
preserve the hemp fibre properties and avoid its degradation. The composites were then
200 ◦ C to preserve the hemp fibre properties and avoid its degradation. The composites
prepared by pressing the layers at a temperature of 200 °C and according to the cycle
were then prepared by pressing the layers at a temperature of 200 ◦ C and according to
presented in Figure 2b. These temperature and pressure cycles are specific to the combi-
the cycle presented in Figure 2b. These temperature and pressure cycles are specific to
nation of constituents involved (hemp/PA11) in the commingled yarn and to the stacking
the combination of constituents involved (hemp/PA11) in the commingled yarn and to
chosen in this chosen
the stacking study (two cross-plies
in this of woven
study (two fabrics).
cross-plies Specimens
of woven for the
fabrics). mechanical
Specimens fortest-
the
ing were cut according to the appropriate standard, given later, and before
mechanical testing were cut according to the appropriate standard, given later, and before the testing,
they were conditioned
the testing, for at least 24for
they were conditioned h at
at least
23 °C24 and 50%
h at 23 ◦relative
C and 50%humidity.
relative humidity.

(a)The
Figure2.2.(a)
Figure Thestacking
stackingof
offabrics,
fabrics,adapt
adaptfrom:
from:[8];
[8];(b)
(b)the
thethermocompression
thermocompressionmoulding
mouldingcycle.
cycle.

2.3. Characterisation Steps

2.3. Characterisation Steps
2.3.1. Properties of the Hybrid Yarns
2.3.1. Properties of the Hybrid Yarns
First, dry-state tensile tests were performed on the hybrid yarns at different test speeds
First,todry-state
in order tensile
investigate tests were
the influence performed
of this parameter ononthe
thehybrid yarns
behaviour of at
thedifferent test
hybrid yarns.
speeds in were
The tests orderperformed
to investigate the
on an influence
MTS of this
Criterion parameter
45 universal on the
tensile behaviour
apparatus of the
(Eden hy-
Prairie,
brid
MN,yarns.
USA) The tests were
according performed
to the NF EN ISO on2062
an MTS Criterion
standard 45 universal
[28] with a gauge tensile apparatus
length of 200 mm,
(Eden
withoutPrairie, MN, USA)
pretension, according
and with to the NFtest
three different ENspeeds:
ISO 2062 20,standard
100, and [28] with a gauge
200 mm/min. For
length of 200 mm, without pretension, and with three different test speeds:
each crosshead speed, the test was repeated 20 times. In addition, tensile tests were 20, 100, and
200
alsomm/min.
conducted Foron
each
thecrosshead speed,
hemp roving, theonly
but test at
was200repeated
mm/min 20 test
times. In addition,
speed, tensile
to compare its
behaviour with the hybrid yarns.
Then, thermo-state tensile tests were performed on these yarns in order to study the
effect of temperature on the yarn properties and to understand the behaviour of these
hybrid yarns at the chosen temperature. Tensile tests were then conducted on the same
 Coatings 2021, 11, 770 5 of 17

tests were also conducted on the hemp roving, but only at 200 mm/min test speed, to
Coatings 2021, 11, 770 compare its behaviour with the hybrid yarns. 5 of 16
Then, thermo-state tensile tests were performed on these yarns in order to study the
effect of temperature on the yarn properties and to understand the behaviour of these
hybrid yarns at the chosen temperature. Tensile tests were then conducted on the same
machine as the dry-state tests, using an isothermal oven. Due to the size of the oven, the
machine as the dry-state tests, using an isothermal oven. Due to the size of the oven, the
gauge length of the yarn was 100 mm, the crosshead speed was 100 mm/min, and the
gauge length of the yarn was 100 mm, the crosshead speed was 100 mm/min, and the
temperature was set at 50, 70, 100, 120, and 150 ◦ C. The single yarn was first inserted in
temperature was set at 50, 70, 100, 120, and 150 °C. The single yarn was first inserted in
the oven and clamped between the two jaws, and then the desired temperatures were set.
the oven and clamped between the two jaws, and then the desired temperatures were set.
Once the temperature was reached and stabilised, the test started.
Once the temperature was reached and stabilised, the test started.
2.3.2. Properties of the Produced Fabrics
2.3.2. Properties of the Produced Fabrics
Tensile tests were performed on the woven fabrics according to the NF EN ISO
13934-1Tensile tests [33]
standard wereand
performed on theout
were carried woven
on an fabrics
MTSaccording
Criterion to 45the NF ENatISO
machine 13934-
ambient
1 standard [33] and were carried out on an MTS Criterion
temperature. The two main directions of the woven fabrics were tested and for each45 machine at ambient temper-
ature. Thefive
direction, twosamples
main directions
were used, of the
withwoven
a lengthfabrics
of 300 were
mmtested
and aandwidth for of
each direction,
50 mm. For
fivetensile
the samples were
test, the used,
gaugewith
lengtha length
was 200 of 300
mm,mm the and
test aspeed
widthwas of 50
20 mm. For the
mm/min, andtensile
the
test, the gauge length was 200 mm, the test speed was 20 mm/min,
preload wad 5 N. To present the properties of the two woven fabrics, we studied the and the preload wad
5 N. To present
maximum load/yarn theand
properties
strain atof the two load
maximum woven fabrics,
for each weinstudied
fabric order tothe maximum
eliminate the
load/yarn and strain at maximum load for each fabric in order
effects of the density of yarns. The bending rigidity of the fabrics was also identified to eliminate the effectsbyof
the density
using of yarns.
a cantilever The bending
apparatus according rigidity
to the ofISO
the 4604
fabrics(05)was also identified
standard [34], withby theusing
samea
cantilever
samples usedapparatus according
for the tensile tests to the ISO
(Figure 3). 4604 (05) standard
As described in the[34], with the
literature same
[35,36], thesamples
fabric
used foristhe
sample tensile testsadvanced
progressively (Figure 3).until
As described
the end, underin the literature [35,36],isthe
its own weight, in fabric
contact sample
with
is progressively
the inclined plane at 41.5◦ . until
advanced Then,the theend, under length
overhang its ownofweight,
the fabricis iniscontact
measured with thethe
and in-
clined plane
bending at 41.5°.
stiffness Then, theaccording
is computed overhangto length
Equationof the(1)fabric is measured and the bending
as follows:
stiffness is computed according to Equation (1) asfollows:
lm 3

G = 9.81 × ms × 𝑙 (1)
𝐺 = 9.81 × 𝑚 × 2 (1)
2
where G𝐺isisthe
where thebending
bendingstiffness
stiffnesscoefficient
coefficient(N ·mm), m𝑚s isisthe
(N·mm), theareal
arealdensity
densityofofthethefabric
fabric
(g/m 2 ), and l is the overhanging length (m).
(g/m2), and 𝑙m is the overhanging length (m).

Figure3.3.Cantilever
Figure Cantilevertest
testbench.
bench.

2.3.3.
2.3.3. Properties
Propertiesofofthe
theComposite
CompositePlates
Plates
The
The tensile and
and flexural
flexuralbehaviours
behavioursofofhemp/PA11
hemp/PA11 composites
composites were were tested
tested in aninMTS
an
MTS Criterion 45 universal testing machine. The tensile properties of the
Criterion 45 universal testing machine. The tensile properties of the composite specimens composite
specimens were performed
were performed according toaccording
the ASTMtoD3039-00
the ASTM D3039-00
standard [37],standard
while the [37], whileprop-
flexural the
flexural properties were tested according to the NF EN ISO 14125 standard [38].
erties were tested according to the NF EN ISO 14125 standard [38]. The tensile tests were The tensile
tests were
carried outcarried
over aout overlength
gauge a gaugeof length
150 mm of and
150 mm
a testand a test
speed ofspeed of 1 mm/min.
1 mm/min. The
The reported
reported modulus was calculated (between 0% and 1% strain) for all composite
modulus was calculated (between 0% and 1% strain) for all composite samples. Thus, the samples.
Thus, the strength and strain at break were calculated from the recorded force–displacement
curves. For flexural behaviour, tests were performed at a test speed of 1 mm/min, with
specimens of 25 mm width and 64 mm span length. For both tensile and flexural tests,
five samples were tested in the two main directions of the composite plates which are
Coatings 2021, 11, 770 6 of 17

Coatings 2021, 11, 770
strength and strain at break were calculated from the recorded force–displacement curves.6 of 16
For flexural behaviour, tests were performed at a test speed of 1 mm/min, with specimens
of 25 mm width and 64 mm span length. For both tensile and flexural tests, five samples
were tested in the two main directions of the composite plates which are direction 1 (as-
direction
sociated 1with
(associated
the warpwith the warp
direction ofdirection
the upperof ply)
the upper ply) and direction
and direction 2 (associated
2 (associated with the
with the weft direction of the upper
weft direction of the upper ply). ply).

3. Results and Discussion

3. Results and Discussion
3.1. Yarn Properties
3.1. Yarn
3.1.1. Properties
Textile Properties of the Hybrid Yarns
3.1.1.The
Textile Properties
measured textileofproperties
the Hybridof Yarns
the hybrid hemp/PA11 yarns and hemp roving are
listedThe measured
in Table 2. The textile
hybridproperties
yarn has a of the hybrid
higher hemp/PA11
linear density yarns roving,
than hemp and hempas a roving
result
the addition of the thermoplastic multifilament PA11 (111 ±
are listed in Table 2. The hybrid yarn has a higher linear density than hemp roving, as a
of 3 Tex). Moreover, adding
the wrapped
result PA11 multifilament
of the addition leads to amultifilament
of the thermoplastic decrease in the hybrid
PA11 (111yarn hairiness.
± 3 Tex). This
Moreover,
decrease
adding the is due to thePA11
wrapped removal of most impurities
multifilament leads to aduring theinwrapping
decrease the hybridprocess. Figure
yarn hairiness.
4This
presents
decreasethe isvisual
due to aspect of the core
the removal untreated
of most impuritieshemp roving
during theand the wrapped
wrapping process.yarn.
Fig-
There are no more
ure 4 presents defects
the visual on the
aspect of surface
the coreofuntreated
the hybrid yarn
hemp in comparison
roving to the hemp
and the wrapped yarn.
roving.
There areAfterno wrapping,
more defects theon
yarn
thestructure
surface ofbecomes
the hybridmore compact
yarn and uniform,
in comparison to theand its
hemp
section is more circular. In addition, the wrapping process preserves
roving. After wrapping, the yarn structure becomes more compact and uniform, and its the structure of the
core roving
section and circular.
is more its properties by creating
In addition, a mechanical
the wrapping bond
process betweenthe
preserves thestructure
two materials,
of the
unlike conventional
core roving methods used
and its properties to improve
by creating the interfacial
a mechanical bond bond with polymer
between matrices,
the two materials,
which
unlikeuse chemical, physical
conventional methodsorused biological treatments
to improve instead [39].
the interfacial bondThis
withhybrid yarn
polymer has, in
matrices,
weight, 50% of hemp fibre and 50% of PA11.
which use chemical, physical or biological treatments instead [39]. This hybrid yarn has,
in weight, 50% of hemp fibre and 50% of PA11.
Table 2. The textile properties of the hybrid yarns and hemp roving.
Table 2. The textile properties of the hybrid yarns and hemp roving.
Hemp Fibre Mass
Yarns Linear Density (Tex) Twist Level (tpm) Hairiness (H ± sh)
Yarns Linear Density (Tex) Twist Level (tpm) Hairiness (H ± sh) Fraction
Hemp Fibre Mass (%) (%)
Fraction
Hybridyarns
Hybrid yarns 9 ±9
486 ±486 400 400 10.05 ± 2.86
10.05 ± 2.86 50 50
Hemp roving
Hemp roving 313
313 ± 19 ± 19 37 ± 2 37 ± 2 18.96 ± 3.31 ± 3.31
18.96 100 100

Figure4.
Figure 4. The
The visual
visual aspect
aspect of
of aa hybrid
hybridyarn
yarnand
andaahemp
hemproving.
roving.

3.1.2.
3.1.2. Dry-State
Dry-State Tensile
TensileBehaviour
Behaviour
•• Comparison
Comparison of HempRoving
of Hemp Rovingand
andHemp/PA11
Hemp/PA11 Hybrid
Hybrid Yarn
Yarn Behaviour
Behaviour
Figure 5 shows the tenacity–strain curve of the hybrid yarn and the hemp roving at
ambient temperature and at a speed of 200 mm/min. The behaviour of the hybrid yarn has
the first peak of tenacity at a strain of around 3%, corresponding to the roving breakdown.
At this first peak, tenacity reaches 8 cN/Tex. This peak is followed by a high deformation
phase before the full breakdown of the hybrid yarn at a strain of 35% (Figure 6a), the same
 Figure 5 shows the tenacity–strain curve of the hybrid yarn and the hemp roving at
ambient temperature and at a speed of 200 mm/min. The behaviour of the hybrid yarn has
Coatings 2021, 11, 770 the first peak of tenacity at a strain of around 3%, corresponding to the roving breakdown. 7 of 16
At this first peak, tenacity reaches 8 cN/Tex. This peak is followed by a high deformation
phase before the full breakdown of the hybrid yarn at a strain of 35% (Figure 6a), the same
as
asthatthatof
ofthe
thePA11
PA11 multifilament
multifilament (Table
(Table 1).
1). This
This part
part of
of the
the curve
curve cancan be
be attributed
attributed to to the
the
elongation of the PA11 multifilament, with compacting of the hemp roving
elongation of the PA11 multifilament, with compacting of the hemp roving around which around which
ititisiswrapped,
wrapped,as asthe
theload
loadincreases.
increases. By
Byincreasing
increasing the
the elongation,
elongation, occasional
occasional slippage
slippage cancan
occur
occur between the PA11 filaments and the broken hemp roving, and the filaments can
between the PA11 filaments and the broken hemp roving, and the filaments can bebe
stretched
stretchedunevenly,
unevenly, leading
leading to
to their
their rupture
rupture that
that appears
appears on on the
the tenacity–strain
tenacity–strain curve
curve as as aa
non-smooth
non-smoothpart. part.In
Inthis
thispart
partof
ofthe
thecurve,
curve,some
somesmall
smallbreaks
breaksarearedetected
detected byby the
the load
load cell
cell
and involve a high standard deviation between samples on the
and involve a high standard deviation between samples on the measured load. measured load.

Figure
Figure5.5.The
Thetensile
tensilebehaviour
behaviourof
ofthe
thehybrid
hybridyarn
yarnand
andhemp
hemproving
roving alone.
alone.

From these
From these results, itit can
canbebeconcluded
concludedthatthatthe
the wrapped
wrapped multifilament
multifilament PA11 does
PA11 not
does
induce
not a significant
induce increase
a significant in the
increase in roving tenacity
the roving and and
tenacity rigidity. During
rigidity. the first
During phase
the first (low
phase
tenacity),
(low the roving
tenacity), curve
the roving corresponds
curve correspondsto the fibrefibre
to the redressing in the
redressing axial
in the load
axial direction.
load direc-
This results from the roving tension applied during the wrapping process.
tion. This results from the roving tension applied during the wrapping process. Thus, Thus, even if the
hybrid yarn did not reach the required tenacity for weaving, which
even if the hybrid yarn did not reach the required tenacity for weaving, which is 15 is 15 cN/Tex, it can be
woven because
cN/Tex, it can beadding
wovenPA11 during
because the wrapping
adding PA11 duringprocess
the increases
wrappingthe inter-fibre
process cohesion
increases the
and protects
inter-fibre them from
cohesion and damage
protects during the weaving
them from process.the
damage during Weaveability of natural
weaving process. fibre
Weave-
reinforcement
ability of naturalcan be also
fibre improved can
reinforcement by other methods,
be also improved as by
described in [8,40,41].
other methods, as described
in
• [8,40,41].
Tensile Behaviour of the Hybrid Yarns at Different Test Speeds
Figure 6a shows the tensile behaviour of the produced hybrid yarns for different test
• Tensile Behaviour of the Hybrid Yarns at Different Test Speeds
speeds (20, 100, and 200 mm/min) at ambient temperature. For these different speed
tests,Figure 6a shows
the shape of thethe tensile behaviour
tenacity–strain curve ofremains
the produced hybrid
the same. yarns
High for different
rigidity test
is observed
speeds (20, 100, and 200 mm/min) at ambient temperature. For these
in the first phase up to a peak, followed by a non-smooth part characterised by a high different speed tests,
the shape ofand
elongation the fluctuation
tenacity–strain curve
of the remains
tenacity around the the
same. High of
tenacity rigidity is observed
the first in the
peak. However,
first phase up to a peak, followed by a non-smooth part characterised by
a dependence of the tenacity at the first peak on the test speed can be seen in Figure 6b. a high elongation
and fluctuation
At the 200 mm/min of thespeed,
tenacity around
the tenacitytheistenacity
70% higherof thethan
firstatpeak. However,Ina addition,
20 mm/min. depend-
ence
the behaviour of yarns at 100 and 200 mm/min is almost the same: in the range of the
of the tenacity at the first peak on the test speed can be seen in Figure 6b. At 0 to200
5%
mm/min speed, the tenacity is 70% higher than at 20 mm/min. In addition,
strain with a difference of 10% for the tenacity. These results match the results obtained in the behaviour
of yarns atstudies
previous 100 and 200 mm/min
conducted is almost the
on commingled same: inand
glass/PP theon
range of 0 to yarns
flax/PA12 5% strain with a
at different
difference of 10% for the tenacity. These results match the results
test speeds and in which the tenacity increases with increasing the test speed [25,35].obtained in previous
studies conducted on commingled glass/PP and on flax/PA12 yarns at different test
speeds and in which the tenacity increases with increasing the test speed [25,35].
 Coatings2021,
Coatings 11,770
2021,11, 770 8 of8 of
1716

Figure
Figure 6.6.(a)(a) Tenacity–straincurve
Tenacity–strain curveofofhybrid
hybridyarns
yarnsat
at different
different test speeds; (b) tenacity
tenacity at
atfirst
firstpeak
peakat
atdifferent
differenttest
testspeeds.
speeds.

3.1.3.Thermo-State
3.1.3. Thermo-StateTensileTensileBehaviour
Behaviour
The tensile behaviour of of
The tensile behaviour thethe hemp/PA11
hemp/PA11 yarns
yarns at different
at different temperatures
temperatures is shown
is shown in
in Figure 7a. The tensile tests for the different temperatures were performed
Figure 7a. The tensile tests for the different temperatures were performed at the same test at the same
test speed
speed of 100 mm/min.
of 100 mm/min. Depending Depending on the temperature,
on the temperature, the results
the results obtained canobtained
be divided can
be divided into three groups, namely, around the glass transition of PA11 (T = 50 ◦ C),
into three groups, namely, around the glass transition of PA11 (T = 50 °C), above the glass
◦ C), and below the melting temperature
above the
transition (T glass
= 70, transition
100, and (T =°C),
120 70,and
100,below
and 120the melting temperature (T = 150 °C). The
(T = 150 ◦ C). The first phase of the different curves at the studied temperatures differs from
first phase of the different curves at the studied temperatures differs from the one at room
the one at room temperature, as does the second phase. In contrast, the curves obtained
temperature, as does◦the second phase. In contrast, the curves obtained at T = 100 and 120
at T = 100 and 120 C show almost similar trends in the first and second phases. Hence,
°C show almost similar trends in the first and second phases. Hence, the tensile behaviour
the tensile behaviour of these yarns depends strongly on the temperature setting. When
of these yarns depends strongly on ◦the temperature setting. When the temperature is in-
the temperature is increased to 50 C (upper glass transition), the tenacity of the wrapped
creased to 50 °C (upper glass transition), the tenacity of the wrapped yarn decreases as a
yarn decreases as a result of the modification in the multifilament around the hemp roving,
result of the modification in the multifilament around the hemp roving, which becomes
which becomes softer by passing the transition temperature and the interaction between
softer by passing the transition temperature and the interaction between hemp fibres and
hemp fibres and PA11 filaments changes. As the temperature increases (but is still far from
PA11 filaments changes. As the temperature increases (but is still far from the melting
the melting temperature), the PA11 filaments keep slipping over the core hemp roving. This
temperature), the PA11 filaments keep slipping over the core hemp roving. This is because
is because adhesion between the filaments and fibres increases with increasing temperature.
adhesion between the filaments and fibres increases with increasing temperature. This
This increased adhesion strengthens the yarn and increases its tenacity, Figure 7b. Then,
increased
at T = 150 adhesion strengthens
◦ C, the maximum the yarn
tenacity of and increases
the first phaseits tenacity,significantly
decreases Figure 7b. Then,
becauseat Tthe
=
150 °C, the maximum
temperature nears the tenacity
meltingof temperature,
the first phasewhich
decreases significantly
strongly because
affects the the tem-
structure of the
perature nears the melting temperature, which strongly affects the structure
hybrid yarn: the PA11 begins to stick locally to hemp fibres without creating a continuous of the hybrid
 fibres. The same trend is observed in the presented results for tests below the melting
temperature (Figure 7a). This can be attributed to the helical path of the wrapped PA11
filaments and the change in the interaction properties with the hemp fibres. At the ambi-
ent temperature, the spiral filaments stretch until they become aligned with the longitu-
Coatings 2021, 11, 770
dinal axis of the yarn (unfolding). However, as the temperature increases, the PA11 fila- 9 of 16
ments stick more locally to the hemp fibres, and that leads to concentrating the defor-
mation at weak places on the wrapped yarn instead of having complete unfolding. Figure
7b shows the evolution of the tenacity at the first peak at different temperatures. As ex-
medium
plained to distribute
before, the efforts
this tenacity between
increases the
initially hemp
with fibres. temperature
increasing This was observed
up to 100on °Cthe
structure
and of the yarnbut
then decreases, once
at extracted from the climatic
higher temperatures chamber
(120 and afterthe
150 °C), thestandard
tests. In the sections
deviation
iswhere the
greater yarn
than athad become
lower solid in comparison
temperatures (50° and 70to thewhich
°C), original wrapped
is mainly yarn,
due it accordingly
to the irregular
displayed decreased extensibility.
behaviour of these yarns at high temperature.

Figure
Figure7.7.(a)(a)
Tenacity–strain
Tenacity–straincurve
curveofofthe
thehybrid
hybridyarns
yarnsatatdifferent
differenttemperatures;
temperatures;(b)
(b)tenacity
tenacityatatfirst
first
peak
peakatatdifferent
differenttemperatures.
temperatures.

According to previous results obtained on flax/PA12 hybrid yarns [25], when the
temperature increases and nears the melting value, the strain at break decreases, compared
to the strain obtained at ambient temperature, whereas the deformation of hybrid yarns
increases with increasing temperature above the melting temperature because below this
temperature, the PA12 is fluid enough to increase the slippage between broken fibres. The
same trend is observed in the presented results for tests below the melting temperature
(Figure 7a). This can be attributed to the helical path of the wrapped PA11 filaments and
the change in the interaction properties with the hemp fibres. At the ambient temperature,
the spiral filaments stretch until they become aligned with the longitudinal axis of the yarn
(unfolding). However, as the temperature increases, the PA11 filaments stick more locally
to the hemp fibres, and that leads to concentrating the deformation at weak places on the
wrapped yarn instead of having complete unfolding. Figure 7b shows the evolution of
the tenacity at the first peak at different temperatures. As explained before, this tenacity
increases initially with increasing temperature up to 100 ◦ C and then decreases, but at
higher temperatures (120 and 150 ◦ C), the standard deviation is greater than at lower
temperatures (50◦ and 70 ◦ C), which is mainly due to the irregular behaviour of these yarns
at high temperature.
Coatings 2021, 11, 770 10 of 16

3.2. Fabric Properties

3.2.1. Textile Properties
At this scale, the properties of the fabrics developed in this study will be compared to
the properties of fabrics made in a previous study from 100% hemp roving. Table 3 shows
the textile properties of these produced woven fabrics. For fabrics based on hybrid yarns,
the twill 6 fabric has the higher weft density, its areal density and thickness are greater than
satin 6. The areal density of this woven fabric depends mainly on the weft density, which,
in turn, depends on how the fabric is packed during weaving and on the weave diagram.
In addition, these fabrics are made of hybrid yarns that are heavier than conventional 100%
natural fibre yarns. However, the air permeability of satin 6 is five times greater than that
of twill 6, which highlights the higher inter-yarns gap, and it is correlated with a lower
areal density, in comparison with twill 6, since it contains higher weft density. On the
other hand, the fabrics in this study are heavier and thicker than the satin 6 and twill 6 of
the previous study [42] manufactured with only hemp roving. This difference could be
explained by the difference in the linear density of yarns which is higher for hybrid yarns
(486 Tex) than for 100% hemp roving (259 Tex). In addition, even if the areal density of
commingled fabrics is higher than that of 100% hemp fabrics, the air permeability is still
higher. This could be due to the structure of the yarn used. In the case of hybrid yarns, the
structure is more compact and the surface of the yarn contains less fibrils, compared to the
structure of the roving, which is hairier, flat, and contains more fibrils.

Table 3. The textiles properties of the woven fabrics of this study and Corbin et al. [42] study.

Twill 6 from Hybrid Satin 6 from Hybrid Satin 6 with 100% Twill 6 with 100%
Fabric Pattern
Yarns Yarns Hemp Roving [42] Hemp Roving [42]
Warp density
6 6.4 6 6
(yarns/cm)
Weft density
10 6 9.5 9.5
(yarns/cm)
Areal density (g/m2 ) 827 ± 15 583 ± 16 426 ± 8 402 ± 3
Thickness (mm) 2.19 ± 0.05 2.13 ± 0.04 1.55 ± 0.05 1.59 ± 0.06
Air permeability
605 ± 91 3485 ± 239 401 ± 46 670 ± 115
(L/m2 /s)
Warp crimp (%) 0.67 ± 0.16 2.38 ± 1.11 2.24 ± 0.20 2.56 ± 0.34
Weft crimp (%) 2.65 ± 0.47 1.20 ± 0.30 1.90 ± 0.30 1.58 ± 0.22

3.2.2. Mechanical Properties

• Tensile Behaviour
Figure 8a shows the tensile properties of the two commingled fabrics and the two
fabrics made from 100% hemp roving both in warp and weft direction. The tensile load is
given in cN/yarn/Tex to remove the effects of the density and linear density of yarns and
concentrate on the effect of the weave pattern and tenacity at the break of the roving. For
the commingled satin 6 and twill 6 fabrics, a small difference in maximum tensile load is
noted between the two directions. In terms of breaking strain, the weft direction of twill 6
is 55% higher than the warp direction, whereas the strain of satin 6 is similar for the two
directions even if the crimp level is higher in the warp direction (Figure 8b). The high strain
at break of twill 6 weft direction results from the higher crimp level of weft yarns as the
warp yarns are under higher tension than weft yarns during the weaving process. Thus,
the twill 6 fabric exhibits better tensile properties, both in warp and weft direction, than
satin 6, and this difference can be explained by the difference of weave diagram between
the structure and the arrangement of yarns inside the structure. In comparison to the
previous study [42], it can be seen that twill 6 and satin 6 structures made from 100% hemp
roving exhibit better maximum loads than twill 6 and satin 6 made from hybrid yarns, in
the two directions for satin 6 structure and only in weft direction for twill 6 structure. That
is mainly attributed to the low tenacity of these hybrid yarns (8 cN/Tex), compared to the
 Coatings 2021, 11, 770 11 of 17
Coatings 2021, 11, 770 11 of 16

ture. That is mainly attributed to the low tenacity of these hybrid yarns (8 cN/Tex), com-
pared toof
tenacity the tenacity
100% hemp of roving
100% hemp roving (24
(24 cN/Tex) cN/Tex)
[42]. [42]. Furthermore,
Furthermore, the higher the higherlevel
hairiness hair-
iness
of hemplevel of hemp
roving rovinghigher
conduces conduces higher inter-roving
inter-roving friction,
friction, leading leading
to higher to higherloads.
maximum maxi-
mum at
Strain loads. Strain at
maximum loadmaximum load fabrics
of the woven of the woven fabrics
is balanced is balanced
between between
the two the two
directions for
directions
these for these
structures structures
except except for
for commingled commingled
twill 6 structure,twill 6 structure,
which which
has a high strainhas
at abreak
high
strain
in at break
the weft in theinweft
direction directionwith
comparison in comparison with the other structure.
the other structure.

Figure8.8.(a)
Figure (a)The
Thetensile
tensileload
load(in
(incN/yarn/Tex)
cN/yarn/Tex) of the woven fabrics;
fabrics; (b)
(b) the
the tensile
tensilestrain
strainat
atbreak
breakof
of the
the woven
woven fabrics.
fabrics.

•• FlexuralBehaviour
Flexural Behaviour
Figure99shows
Figure showsthe theflexural
flexuralrigidity
rigidityofofthe
thetwo
twofabrics.
fabrics.TheThetwo
twofabrics
fabricshave
havethethesame
same
warpdensity
warp densityandanddiffer
differonly
onlybybytheir
theirweft
weftdensity
densityand andstructure.
structure.TwillTwill66exhibited
exhibitedbetter
better
rigidity than
rigidity than satin
satin 66 in
inthe
thetwo
twodirections,
directions, and
and this
thisdifference
differenceisismainly
mainlydue duetotothe
thehigh
high
arealdensity
areal densityof ofthe
thefabric
fabric(42%
(42%higher
higherthan
thanthat
thatofofsatin
satin6)6)and
andits
itsyarn
yarndensity
densityin inthe
theweft
weft
direction. The flexural rigidity depends strongly on those two parameters. However, aa
direction. The flexural rigidity depends strongly on those two parameters. However,
high weft
high weft density
density and
and linear
lineardensity
densityresult
resultininaaheavy
heavyfabric.
fabric. The
Theflexural
flexuralrigidity
rigidityalso
also
depends on
depends on the
thecrimp
crimplevel
levelofofyarns
yarnsinside
insidethe
thestructure.
structure. In Inthe
thecase
caseof oftwill
twill66fabric,
fabric,the
the
shrinkage of
shrinkage of weft
weft yarns
yarns isisgreater
greaterthan
thanwarp
warpyarns,
yarns,and andthat
thatled
ledtotohigher
higherrigidity
rigidityininthe
the
weftdirection
weft directionof ofthe
thefabric
fabricthan
thanininthe
thewarp
warpdirection.
direction.By Bycontrast,
contrast,forforsatin
satin66fabric,
fabric,the
the
warpyarns
warp yarnsexhibit
exhibithigher
highercrimp,
crimp,which
which results
results in in a higher
a higher rigidity
rigidity in this
in this direction
direction thanthan
in
the weft direction.
in the weft direction.
Coatings 2021, 11, 770 12 12ofof17
16

Figure 9.
Figure The flexural
9. The flexural rigidity
rigidity of
of the
the two
two fabrics.
fabrics.

3.3. Composite Properties

3.3. Composite
3.3.1. Properties
Composition of the Composite Plates
3.3.1.The
Composition of the Composite
obtained physical Platesof the two composite plates are summarised in
compositions
TableThe obtained
4. The physical
two types compositions
of composites of the
were two composite
produced plates
by stacking two are summarised
cross-plies. Asina
Table
result,4.the
The two types
thickness of composites
of twill 6 hemp/PA11werecomposite
produced(C2)by stacking two cross-plies.
is 28% higher As a
than composite
result, the thickness
made from of twill
satin 6 (C1). 6 hemp/PA11
The weight composite
of the two types of(C2) is 28% higher
composites than and
is the same composite
differs
made from satin 6 (C1). The weight of the two types of composites is the same
from that in the original (50% of hemp and 50% of PA11), which is explained by the loss and differs
from thatduring
of PA11 in the the
original (50% of process.
compression hemp and By50% of PA11),
contrast, which is
the volume of explained
fibre in thebyC2the loss
is 22%
of PA11than
greater during
C1.the compression process. By contrast, the volume of fibre in the C2 is 22%
greater than C1.
Table 4. The physical properties of the two composites.
Table 4. The physical properties of the two composites.
Composite Plates Thickness (mm) Density (g/cm3 ) Fibre Mass Fraction (%) Fibre Volume Fraction (%)
Composite Plates Thickness (mm) Density (g/cm3) Fibre Mass Fraction (%) Fibre Volume Fraction (%)
Hemp/PA11 Satin 6
Hemp/PA11 Satin(C1)
composite plate plate±(C1)
6 composite1.01 0.01 1.01 ± 0.011.01 ± 0.01
1.01 ± 0.01 52 ±52
1 ±1 35.1±± 0.1
35.1 0.1
Hemp/PA11 Twill
Hemp/PA11 Twill 66 composite plate (C2) 1.39 ± 0.01 1.24 ± 0.03 52 ± 0.1 42.8 ± 1.2
1.39 ± 0.01 1.24 ± 0.03 52 ± 0.1 42.8 ± 1.2
composite plate (C2)
3.3.2. Tensile Properties of the Composite Plates
3.3.2.The tensile
Tensile strength,ofstrain
Properties at break, and
the Composite modulus of the two types of composites are
Plates
shown Thein tensile
Figure 10. For each
strength, structure,
strain the and
at break, properties
modulusareof
almost
the twothe types
same for both direc-
of composites
tions of the in
are shown composite
Figure 10.plates, whilestructure,
For each at the same
thetime, the tensile
properties properties
are almost differfor
the same slightly
both
per composite. The tensile stress and modulus of C1 exceed those of C2, and
directions of the composite plates, while at the same time, the tensile properties differ the opposite
is the case
slightly perfor strain. Even
composite. Theiftensile
the fibre content
stress of C1 composites
and modulus is lower
of C1 exceed thosethan thatand
of C2, of C2,
the
their tensile properties are higher. At the fabric scale, the twill 6 fabric exhibited
opposite is the case for strain. Even if the fibre content of C1 composites is lower than better
that
properties,
of C2, theirboth in tensile
tensile and are
properties flexural rigidity,
higher. At thewhereas this isthe
fabric scale, notwill
larger than the
6 fabric case at
exhibited
the composite
better scale.
properties, both in tensile and flexural rigidity, whereas this is no larger than the
case at the composite scale.
Coatings 2021, 11, 770 13 13ofof17
16

(a) Tensile
Figure 10. (a)
Figure Tensile strength of composite
composite materials;
materials; (b)
(b) strain
strainat
atthe
themaximum
maximumstrength;
strength;(c)
(c)modu-
mod-
ulus.
lus.

3.3.3. Flexural
3.3.3. Flexural Behaviour
Behaviour ofof the
the Composite
Composite Plates
Plates
The results
The results of
of the
the flexural
flexural testing
testing are
are shown
shown in in Figure
Figure 11. For the
11. For the satin
satin 66 composites
composites
(C1), direction 2 presents better properties than direction 1, while for twill
(C1), direction 2 presents better properties than direction 1, while for twill 6 (C2) 6 (C2) the
the op-
opposite is the case. The flexural strength is not balanced between the two directions
posite is the case. The flexural strength is not balanced between the two directions of the of
the composite plates even if the stacking is balanced. This difference is explained by the
Coatings 2021, 11, 770 14 of 17
Coatings 2021, 11, 770 14 of 16

composite plates even if the stacking is balanced. This difference is explained by the ar-
rangement and the orientation of the yarns inside the structure of the composite. In the
arrangement and the orientation of the yarns inside the structure of the composite. In the
case of satin 6 composite plates (C1), the float yarns of direction 2 are located outside the
case of satin 6 composite plates (C1), the float yarns of direction 2 are located outside the
specimen,
specimen, and that provides
and that provides additional
additional rigidity
rigidity to
to this
this direction.
direction. The
The same
same phenomenon
phenomenon
happens
happens to direction 1 of the twill 6 composite plates (C2). This behaviourbeen
to direction 1 of the twill 6 composite plates (C2). This behaviour has has iden-
been
tified in previous work within the same project [8] and confirmed in this
identified in previous work within the same project [8] and confirmed in this study. study. TheThe
ar-
rangement
arrangement ofof
yarns
yarnsinside
insidethethecomposite
compositeplates
platesdepends
dependsstrongly
stronglyonon the
the nature
nature of the
of the
fabric structure used and on the way of stacking the different
fabric structure used and on the way of stacking the different layers. layers.

Figure 11. The flexural strength of the two composite materials.

Figure 11. The flexural strength of the two composite materials.
4. Conclusions
4. Conclusions
This study investigated the multiscale analysis of bio-based composite materials made
This study commingled
of hemp/PA11 investigated yarns.
the multiscale analysisthe
Understanding of different
bio-basedmanufacturing
composite materials
stages
made of hemp/PA11 commingled yarns. Understanding
and the influence of process parameters on yarn, fabric, and composite properties the different manufacturing
allows
stages andtothe
materials be influence
producedof process
which parameters
better fit the final onapplication
yarn, fabric,requirements.
and composite properties
allowsIn materials
this work,tothe be hybrid
produced which
yarns werebetter fit theby
produced final
theapplication requirements.
wrapping process on a hollow
In this
spindle work,by
machine thewrapping
hybrid yarns were produced
a thermoplastic PA11 bymultifilament
the wrappingaround processan onuntreated
a hollow
spindle machine
hemp roving by wrapping
in order to producea yarns
thermoplastic PA11tenacity
with sufficient multifilament around
(allowing them an untreated
to be woven)
hemp roving in order to produce yarns with sufficient tenacity
and with a fibre content of no less than 40%. This process improves the hemp roving (allowing them to be wo-
ven) and with a fibre content of no less than
structure, which becomes more compact and less hairy. 40%. This process improves the hemp roving
structure,
At thiswhich
yarn becomes more
scale, tensile compact
tests and lessconducted
were initially hairy. at different test speeds includ-
At speed
ing the this yarn scale, tensile
involved during tests
fabricwere initially
testing conducted
in order at different
to investigate test speeds
its influence in-
on the
cluding
mechanical the properties,
speed involved then atduring fabric
different testing in including
temperatures order to investigate
a temperatureits influence
in the rangeon
the mechanical
of the properties,
glass transition then at different
temperature temperaturesResults
of the multifilament. includingfroma temperature
this test show in the
the
range of the glass
dependence of yarn transition temperature
properties on test speed of the
and multifilament.
temperature, Results
which isfrom thisdue
mainly test to
show
the
the dependence
nature of yarn properties
of the multifilament used. on test speed and temperature, which is mainly due to
Then, of
the nature these yarns were used
the multifilament in weaving to produce two different fabrics with ap-
used.
proximately the same
Then, these yarnswarpweredensity
used in and different
weaving toweft densities
produce two and weavefabrics
different diagrams.
with The
ap-
textile and mechanical
proximately the same warp properties
densityofandthese fabricsweft
different weredensities
determined, and thediagrams.
and weave results showThe
the dependence
textile and mechanicalof these properties
properties ofon the fabrics
these production wereparameters:
determined,preform
and the properties
results show in
terms of maximum load and strain are either balanced or unbalanced
the dependence of these properties on the production parameters: preform properties in between the warp
and weft
terms directions. load and strain are either balanced or unbalanced between the warp
of maximum
At the
and weft composite scale, tensile strength and stiffness for each structure are almost
directions.
balanced
At thebetween
composite the two main
scale, directions
tensile of the
strength andcomposite
stiffness plates.
for eachInstructure
addition, are
composite
almost
made from
balanced a satin 6the
between fabric
twoshows an improvement
main directions of its mechanical
of the composite plates.properties
In addition, even though
composite
at the fabric
made from scale,
a satinthe 6 twill
fabric6 fabric
showspresented better properties.
an improvement of its mechanical properties even
The aim of future work will be the testing
though at the fabric scale, the twill 6 fabric presented of other parameters
better at each scale in order
properties.
to produce a light structure adapted to the end-use application. Moreover, the thermome-
chanical behaviour of hybrid yarns and commingled fabrics will be tested across a range of
Coatings 2021, 11, 770 15 of 16

temperatures, including the melting temperature of PA11, in order to better understand

the behaviour of these materials at high temperatures. Thus, the hydrophilic behaviour of
these hybrid yarns will be characterised and compared with that of hemp roving [43].

Author Contributions: Investigation: C.L.; writing—original draft preparation: C.L.; validation;

supervision: M.F., A.R.L. and D.S.; writing—review and editing: M.F., A.R.L. and D.S.; All authors
have read and agreed to the published version of the manuscript.
Funding: This project was funded by “Bio-Based Industries Joint Undertaking” under the “European
Union’s Horizon 2020” Research and Innovation Program with Grant Agreement No. 744349—
SSUCHY Project and Hauts de France Region.
Institutional Review Board Statement: Not applicable.
Informed Consent Statement: Not applicable.
Data Availability Statement: Data are contained within the article.
Acknowledgments: The authors gratefully acknowledge the Italian company Linificio and Canapifi-
cio Nazionale (LCN) for providing the hemp roving used in this study.
Conflicts of Interest: The authors declare no conflict of interest.

References
1. Bourmaud, A.; Beaugrand, J.; Shah, D.U.; Placet, V.; Baley, C. Towards the design of high-performance plant fibre composites.
Prog. Mater. Sci. 2018, 97, 347–408. [CrossRef]
2. CELC. Flax and Hemp Fiber Composites, a Market. Reality: The Biobased Solutions for the Industry; JEC Group: Paris, France, 2018;
ISBN 978-2-490-26300-4.
3. Mohanty, A.K.; Vivekanandhan, S.; Pin, J.-M.; Misra, M. Composites from renewable and sustainable resources: Challenges and
innovations. Science 2018, 362, 536–542. [CrossRef] [PubMed]
4. Sala, B.; Gabrion, X.; Trivaudey, F.; Guicheret-Retel, V.; Placet, V. Influence of the stress level and hygrothermal conditions on the
creep/recovery behaviour of high-grade flax and hemp fibre reinforced greenpoxy matrix composites. Compos. Part A Appl. Sci.
Manuf. 2021, 141, 106204. [CrossRef]
5. Del Masto, A.; Trivaudey, F.; Guicheret-Retel, V.; Placet, V.; Boubakar, L. Investigation of the possible origins of the differences in
mechanical properties of hemp and flax fibres: A numerical study based on sensitivity analysis. Compos. Part A. Appl. Sci. Manuf.
2019, 124, 105488. [CrossRef]
6. Baley, C.; Gomina, M.; Breard, J.; Bourmaud, A.; Davies, P. Variability of mechanical properties of flax fibres for composite
reinforcement. A review. Ind. Crop. Prod. 2020, 145, 111984. [CrossRef]
7. Réquilé, S.; Mazian, B.; Grégoire, M.; Musio, S.; Gautreau, M.; Nuez, L.; Day, A.; Thiébeau, P.; Philippe, F.; Chabbert, B.; et al.
Exploring the dew retting feasibility of hemp in very contrasting european environments: Influence on the tensile mechanical
properties of fibres and composites. Ind. Crop. Prod. 2021, 164, 113337. [CrossRef]
8. Corbin, A.-C.; Ferreira, M.; Labanieh, A.R.; Soulat, D. Natural fiber composite manufacture using wrapped hemp roving with
PA12. Mater. Today Proc. 2020, 31, S329–S334. [CrossRef]
9. Corbin, A.-C.; Sala, B.; Soulat, D.; Ferreira, M.; Labanieh, A.-R.; Placet, V. Development of quasi-unidirectional fabrics with hemp
fiber: A competitive reinforcement for composite materials. J. Compos. Mater. 2021, 55, 551–564. [CrossRef]
10. Placet, V.; François, C.; Day, A.; Beaugrand, J.; Ouagne, P. Industrial hemp transformation for composite applications: Influence
of processing parameters on the fibre properties. In Advances in Natural Fibre Composites: Raw Materials, Processing and Analysis;
Springer: Berlin/Heidelberg, Germany, 2018; pp. 13–25. ISBN 978-3-319-64640-4.
11. Shah, D.U.; Schubel, P.J.; Clifford, M.J. Modelling the effect of yarn twist on the tensile strength of unidirectional plant fibre yarn
composites. J. Compos. Mater. 2013, 47, 425–436. [CrossRef]
12. Goutianos, S.; Peijs, T.; Nystrom, B.; Skrifvars, M. Development of flax fibre based textile reinforcements for composite applications.
Appl. Compos. Mater. 2006, 13, 199–215. [CrossRef]
13. Omrani, F.; Wang, P.; Soulat, D.; Ferreira, M. Mechanical properties of flax-fibre-reinforced preforms and composites: Influence of
the type of yarns on multi-scale characterisations. Compos. Part A Appl. Sci. Manuf. 2017, 93, 72–81. [CrossRef]
14. Russo, P.; Simeoli, G.; Vitiello, L.; Filippone, G. Bio-polyamide 11 hybrid composites reinforced with basalt/flax interwoven
fibers: A tough green composite for semi-structural applications. Fibers 2019, 7, 41. [CrossRef]
15. Lebaupin, Y.; Chauvin, M.; Hoang, T.-Q.T.; Touchard, F.; Beigbeder, A. Influence of constituents and process parameters on
mechanical properties of flax fibre-reinforced polyamide 11 composite. J. Thermoplast. Compos. Mater. 2017, 30, 1503–1521.
[CrossRef]
16. Oliver-Ortega, H.; Méndez, J.A.; Reixach, R.; Espinach, F.X.; Ardanuy, M.; Mutjé, P. Towards more sustainable material
formulations: A comparative assessment of PA11-SGW flexural performance versus oil-based composites. Polymers 2018, 10, 440.
[CrossRef]
Coatings 2021, 11, 770 16 of 16

17. Haddou, G.; Dandurand, J.; Dantras, E.; Maiduc, H.; Thai, H.; Giang, N.V.; Trung, T.H.; Ponteins, P.; Lacabanne, C. Mechanical
properties of continuous bamboo fiber-reinforced biobased polyamide 11 composites. J. Appl. Polym. Sci. 2019, 136, 47623.
[CrossRef]
18. Gourier, C.; Bourmaud, A.; Le Duigou, A.; Baley, C. Influence of PA11 and PP Thermoplastic polymers on recycling stability of
unidirectional flax fibre reinforced biocomposites. Polym. Degrad. Stab. 2017, 136, 1–9. [CrossRef]
19. Awais, H.; Nawab, Y.; Amjad, A.; Anjang, A.; Md Akil, H.; Zainol Abidin, M.S. Effect of comingling techniques on mechanical
properties of natural fibre reinforced cross-ply thermoplastic composites. Compos. Part B Eng. 2019, 177, 107279. [CrossRef]
20. Kobayashi, S.; Takada, K. Processing of unidirectional hemp fiber reinforced composites with micro-braiding technique. Compos.
Part A Appl. Sci. Manuf. 2013, 46, 173–179. [CrossRef]
21. Zhai, W.; Wang, P.; Legrand, X.; Soulat, D.; Ferreira, M. Effects of micro-braiding and co-wrapping techniques on characteristics
of flax/polypropylene-based hybrid yarn: A comparative study. Polymers 2020, 12, 2559. [CrossRef]
22. Alagirusamy, R.; Fangueiro, R.; Ogale, V.; Padaki, N. Hybrid yarns and textile preforming for thermoplastic composites. Text.
Prog. 2006, 38, 1–71. [CrossRef]
23. Asghar, A.; Imad, A.; Nawab, Y.; Hussain, M.; Saouab, A. Effect of yarn singeing and commingling on the mechanical properties
of jute/polypropylene composites. Polym. Compos. 2020, 42. [CrossRef]
24. Di Lorenzo, M.L.; Longo, A.; Androsch, R. Polyamide 11/poly(butylene succinate) bio-based polymer blends. Materials 2019, 12,
2833. [CrossRef] [PubMed]
25. Xiao, S.; Wang, P.; Soulat, D.; Gao, H. Thermo-mechanical characterisations of flax fibre and thermoplastic resin composites
during manufacturing. Polymers 2018, 10, 1139. [CrossRef]
26. NF G07-316. Textiles—Tests of Yarns—Determination of Linear Density; AFNOR: La Plaine Saint-Denis, France, 1988.
27. NF G07-079. Textiles—Testing Threads—Determining the Twisting of Threads by Untwisting/Retwisting with a Double Re-Test; AFNOR:
La Plaine Saint-Denis, France, 2011.
28. NF EN ISO 2062. Textiles—Yarns from Packages—Determination of Single-End Breaking Force and Elongation at Break Using Constant
Rate of Extension (CRE) Tester; AFNOR: La Plaine Saint-Denis, France, 2010.
29. NF EN 12127. Textiles—Fabrics—Determination of Mass per Unit Area Using Small Samples; AFNOR: La Plaine Saint-Denis, France,
1998.
30. NF EN ISO 5084. Textiles—Determination of Thickness of Textiles and Textile Products; AFNOR: La Plaine Saint-Denis, France, 1996.
31. NF EN ISO 9237. Textiles—Determination of Permeability of Fabrics to Air; AFNOR: La Plaine Saint-Denis, France, 1995.
32. NF ISO 7211-3. Textiles—Woven Fabrics—Construction—Methods of Analysis—Part 3: Determination of Crimp of Yarn in Fabric;
AFNOR: La Plaine Saint-Denis, France, 2017.
33. NF EN ISO 13934-1. Tensile Properties of Fabrics—Part 1: Determination of Maximum Force and Elongation at Maximum Force Using the
Strip Method; AFNOR: La Plaine Saint-Denis, France, 2013.
34. ISO 4604. Reinforcement Fabrics—Determination of Conventional Flexural Stiffness—Fixed-Angle Flexometer Method; AFNOR: La Plaine
Saint-Denis, France, 2011.
35. De Bilbao, E.; Soulat, D.; Hivet, G.; Gasser, A. Experimental study of bending behaviour of composite reinforcements. Int. J. Mater.
Form. 2009, 2, 205–208. [CrossRef]
36. Bilisik, K. Bending behavior of multilayered and multidirectional stitched aramid woven fabric structures. Text. Res. J. 2011, 81,
1748–1761. [CrossRef]
37. ASTM D3039/D3039M-17. Standard Test. Method for Tensile Properties of Polymer Matrix Composite Materials; ASTM International:
West Conshohocken, PA, USA, 2017.
38. NF EN ISO 14125. Fibre-Reinforced Plastic Composites—Determination of Flexural Properties; AFNOR: La Plaine Saint-Denis, France,
1998.
39. Tanasa, F.; Zănoagă, M.; Teacă, C.; Nechifor, M.; Shahzad, A. Modified hemp fibers intended for fiber-reinforced polymer
composites used in structural applications—A review. I. Methods of modification. Polym. Compos. 2019, 41. [CrossRef]
40. Baley, C.; Gomina, M.; Breard, J.; Bourmaud, A.; Drapier, S.; Ferreira, M.; Le Duigou, A.; Liotier, P.J.; Ouagne, P.; Soulat, D.; et al.
Specific features of flax fibres used to manufacture composite materials. Int J. Mater. 2019, 12, 1023–1052. [CrossRef]
41. Corbin, A.-C.; Soulat, D.; Ferreira, M.; Labanieh, A.; Gabrion, X.; Placet, V. Improvement of the weavability of natural-fiber
reinforcement for composite materials manufacture. RCMA 2019, 29, 201–208. [CrossRef]
42. Corbin, A.-C.; Soulat, D.; Ferreira, M.; Labanieh, A.-R. Influence of process parameters on properties of hemp woven rein-
forcements for composite applications: Mechanical properties, bias-extension tests and fabric forming. J. Nat. Fibers 2020, 1–13.
[CrossRef]
43. Bismarck, A.; Aranberri, I.; Springer, J.; Lampke, T.; Wielage, B.; Stamboulis, A.; Shenderovich, I.; Limbach, H.-H. Surface
characterization of flax, hemp and cellulose fibers; Surface properties and the water uptake behavior. Polym. Compos. 2002, 23,
872–894. [CrossRef]