Composites: Part A 155 (2022) 106805

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Composites Part A
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The influence of the humidity on the mechanical properties of 3D printed

continuous flax fibre reinforced poly(lactic acid) composites
Charles de Kergariou a ,∗, Hind Saidani-Scott c , Adam Perriman b , Fabrizio Scarpa a ,
Antoine Le Duigou d
a
Bristol Composites Institute, School of Civil, Aerospace and Mechanical Engineering, University of Bristol, University Walk, Bristol BS8 1TR, UK
b School of Cellular and Molecular Medicine, University of Bristol, University Walk, Bristol BS8 1TD, UK
c School of Civil, Aerospace and Mechanical Engineering (CAME), University of Bristol, Bristol BS8 1TR, UK
d University Bretagne Sud, IRDL, Polymer and Composites, UMR CNRS 6027, 56100 Lorient, France

ARTICLE INFO ABSTRACT

Keywords: The paper describes the influence provided by the humidity on the mechanical and failure properties of 3D
A. Bio-composites D. Mechanical testing D. printed composites made by continuous flax fibres reinforcing a poly-lactic acid matrix. The bulk in-plane
Moisture E. 3D printing shear, transverse and longitudinal samples considered here have 28%–31% fibre volume fraction and 3%–6%
porosity. The longitudinal and transverse elastic moduli of the composites, together with their transverse and
shear strengths show an almost exponential decay with the increase of the moisture content. The longitudinal
strength remains however constant over the range of relative humidity considered in this work. A fractographic
inspection shows that the exposure of the 3D printed composites to large relative humidity values facilitates the
interlaminar fracture. The influence of the 3D printing process on the fracture and the mechanical properties is
also described. Moreover, the paper provides a comprehensive benchmark of the properties of our 3D printed
composites against analogous data from open literature.

1. Introduction appears to be particularly suited to bond with natural fibres [11–13].

The development of polymer 3d printing technologies over the
past decade has mostly been based on new bulk resins and short
fibre composites. Novel continuous fibre printing technologies are also
being developed to limit the loss of mechanical properties in these
materials, compared to more conventional ways of producing com-
posites [1–4]. Often associated with polyamide resin, glass, carbon
and aramid 3D printed composites have shown promising longitudinal
transverse and shear properties [5–7]. The development of 3D printed
fossil fibres composites is more advanced compared to their natural
fibres-based counterpart [4]. Natural fibres bring though additional
benefits compared to fossil ones. Natural fibres are environmentally
friendly, widely available around the world and have a relatively low
cost, all aspects that are extremely beneficial for industry and broad
technological applications [8]. Matsuzaki et al. have evaluated the
mechanical properties of 3D printed continuous jute fibre compos-
ites [9]. Continuous flax fibre yarn also possesses promising mechanical
performance for 3D printed applications [10]. The recycling efficiency
of 3D printed composites with natural fibres is enhanced by the use
of a thermoplastic matrix (like Poly(Lactic Acid) (PLA)) that can be
melt and re-used several times. Despite being a thermoplastic resin, PLA
Graupner et al. have shown that PLA slightly shrinks during processing,
limiting a potential debonding between the fibre and the matrix [14].
Graupner et al. have also highlighted the presence of a strong interfacial
bonding due to the hydrogen bond between PLA and cellulose. All
these characteristics tend to improve the wetting of the cellulose with
the PLA, compared to other thermoplastics like polypropylene (PP),
and limit the fibre matrix interface voids between the fibre and the
matrix [14].
A previous study has focused on the development of 3D printed
continuous flax fibre/PLA composites [15]. A modulus of 23.3 GPa
and a strength of 253.7 MPa were achieved in this study. 3D printing
allows the tailoring of the distance between filaments when building
the specimens, with 0.8 mm shown to be the interfilament distance that
provides the largest longitudinal stiffness to be obtained (amongst 0.4,
0.6 and 0.8 mm interfilament distance values previously tested) [16].
The highest values for the strength and the strain at failure were how-
ever obtained for a smaller interfilament distance value (0.6 mm). Due
to impregnation, flax fibres in 3D printed filaments tend to embed poly-
mers, which have a tendency to absorb water [17]. Water absorption
during immersion, or when the samples are conditioned at high levels

∗ Corresponding author.
E-mail address: charles.dekergariou@bristol.ac.uk (C. de Kergariou).

https://doi.org/10.1016/j.compositesa.2022.106805
Received 9 September 2021; Received in revised form 25 December 2021; Accepted 3 January 2022
Available online 15 January 2022
1359-835X/© 2022 Elsevier Ltd. All rights reserved.
C. de Kergariou et al.
of Relative Humidity (RH) induces a modification of the mechanical
properties of the composites [15,18,19]. To the best of the authors’
knowledge, the influence of the relative humidity and its variation on
the moisture content and mechanical properties of 3D printed contin-
uous flax fibre/PLA composites (FFRPLA) in non-immersed conditions
has not been evaluated as yet.
The different phases in a composite material create complex and di-
verse fracture patterns that depend among other things on the materials
implemented, the orientation of the fibres, their morphology and the
test conditions [20]. Fractographic inspection of polymeric composites
has been extensively studied, because of the critical importance of a
potential catastrophic failure in primary structural parts [20]. As the
interest to use natural fibres for structural applications increases [8],
the need to understand their failure mechanisms becomes also more
important, as it occurred for their fossil counterparts [21–23]. The
impact of the humidity on such fracture mechanism is of prime interest
due to the interaction that natural fibres have with water. For instance,
several research groups have looked at the impact of the humidity
conditioning on the fibre matrix interface properties in natural fibres
composites [24,25]. The influence of the humidity on the mechanical
properties of PLA and of flax fibres has also been evaluated [26–31].
Hence, humidity affects how the composite deforms and break under
loading, but it does not explain how it fails. Morissa Lu et al. have
highlighted the debonding between fibre (flax) and matrix (polyester)
due to high humidity conditioning (97%), followed by drying [32]. The
fractographic inspection conducted in that work highlighted the impact
of the resin absorption by the fibre on the swelling of the composite.
To the best of the Authors’ knowledge, very little investigation has
been performed on the observation of the impact of the humidity on
the fracture process of continuous flax PLA composites when loaded in
tension a fortiori, if this material is 3D printed.
The present work includes a discussion about the manufacturing of
the 3D printed samples and the assessment of the porosity of those
FFRPLAs to optimize the printing parameters. The specific influence of
the relative humidity on the stiffness and failure properties of samples
maintained in non-immersed conditions (i.e., the samples not immersed
in water) is then evaluated. The mechanical properties considered here
are the longitudinal, transverse and shear stiffness and strength of
the samples. The impact of the relative humidity on the fracture of
the specimens is also evaluated to obtain a comprehensive view of
the mechanical performance of these 3D printed natural fibre com-
posites. The mechanical properties obtained in this work are then
further compared to analogous values from literature to benchmark our
results and provide a comprehensive view on how 3D printed flax fibre
reinforced/PLA composites finds features in the materials design space
for 3D printing reinforced filaments.
2. Material and methods
2.1. Filament and 3D printed specimens
The flax/PLA filament used in this work was produced via coating of
a continuous flax fibre by PLA in a 190 ◦ C heated die. The parameters
of extrusion were optimized in a previous study by some of the Au-
thors [10,16]. Continuous flax yarn from SAFILIN and NatureWorks® ’s
Ingeo™ Biopolymer 3001D PLA are used to produce the filament. A
customized Prusa i3 MK3S printer is used to extrude the filament
with a tailored flat head nozzle heated at 195 ◦ C. The height of the
layers has been adjusted, so that the flat head nozzle could squeeze
the filament on its support layer and pull it out of the machine. A
second fan is also used to force a quick cooling of the material after
the filament is deposed on a plate at 6 mm/s and a temperature of
60 ◦ C. A 0.8 mm inter filament distance is considered for the specimens
produced here because that distance allows a facile production of high
stiffness specimens with complex geometries and tight angles [16].
Supplementary data 1 shows the process for the measurement of the
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Composites Part A 155 (2022) 106805
porosity and the fibre volume fraction for the different specimens used
during the mechanical tests. It also provides the discussion around
the values obtained (3%–6% for porosity, 28%–31% for fibre volume
fraction). The G-code are handwritten as conventional slicers cannot be
used for continuous filament.
2.2. Measure of the mechanical properties
Before tensile tests, glass fibre (6 plies: 165 g*m−2 each) reinforced
epoxy (Epolam 2020) end tabs were glued with epoxy resin (Arladite
420) onto the specimens. The ASTM D570-98 standard is here adopted
to dry the specimen. The temperature suggested in this standard is
however 50 ◦ C, while the T𝑔 of the resin used in this work is 55 ◦ C. The
standard suggests drying the specimens for 24 h. It is evident that by
letting the specimens at 50 ◦ C for 24 h one incurs the risk of modifying
the crystalline structure of the matrix of the specimens and relax some
internal constraints [12]. To avoid these changes in the material, the
drying of the samples produced in this work is performed at 40 ◦ C
under vacuum for at least 72 h. Preliminary studies have been con-
ducted to ensure the same drying state is achieved at 40 ◦ C in vacuum
and the procedure suggested by the ASTM standard. It is observed that
although the drying is slower, identical Moisture Contents (MC) are
reached when using the two procedures. After drying, the specimens
are placed in hermetically closed boxes containing de-ionized water
saturated with different salts to obtain specific RH values. The duration
of the environmental conditioning varied between the different salts
used. The specimens were tested when their weight was stable after
conditioning. The values of the RHs used in this work are presented in
Table 1.
Tensile tests to measure both longitudinal and transverse prop-
erties have been carried out following the ASTM D3039 standard.
The transverse modulus has been measured within the 1000-3000𝜇𝜖
strain interval. Instructions from Shah et al. have been followed to
determine the tensile moduli E1 within the 200-1200𝜇𝜖 strain interval
and the E2 one between 4000𝜇𝜖 and 13000𝜇𝜖 [33]. The ASTM D3518
standard has been adopted to determine the in-plane shear, with the
relevant stiffness measured within the 1500-5500𝜇𝜖 strain interval.
An assessment of the energy dissipated before failure is provided by
the area underneath the stress–strain curve. The specimens have been
produced individually to limit edge and cutting effects, as suggested
by the standards ASTM D3039 and D3518. However, as it will be
discussed later in the paper, the individual production of these samples
creates an edge effect on some of them. Table 2 shows the dimensions
of the 3D printed specimens. The stacking sequences do not fully
respect the ones suggested by the ASTM standard. The architectures
of the specimen have been adapted to the constraint imposed by the
production technique, which makes the printing of thick individual
specimens rather difficult. The G-code and examples of the printed
specimens are presented in Fig. 1. Testing has been performed at
1 mm/min for all specimens as suggested in other works related to
the mechanical properties of 3D printed FFRPLAs [5,15,34]. For each
RH value, one conditioned specimen undergoing shear testing had its
strain fields measured with a Digital Image Correlation (DIC). MTS
criterion model 42 traction machine with a 5 kN load cell was used
for the transverse properties. An Instron 8800 with a 25 kN load cell
was implemented to test the shear and longitudinal specimens.
Five specimens are tested for each RH value. After screening the
results, only three transverse specimens have been considered to mea-
sure the transverse moduli at 10%, 33% and 50% RH. Three samples
have also been considered for the transverse strength of the printed
composites conditioned at 75% RH.
C. de Kergariou et al. Composites Part A 155 (2022) 106805

Table 1
Different RHs values used for the conditioning in the chambers and the corresponding salts used.
Salts Potassium Hydroxide Magnesium Chloride Magnesium Nitrate Sodium Chloride Potassium Sulphate
RH at 20 ◦ C 11% 33% 54% 75% 98%

Fig. 1. G-code and specimens produced. From left to right: shear, longitudinal and transverse. The top left figure illustrates the cross section of the longitudinal specimens. This
figure shows that flax yarns sit on top of each other. The bottom left figures are zooms of the printing pattern from above.

Table 2
Size of the specimen used for the tensile tests.
Specimens Length (mm) Width (mm) Thickness (mm) Stacking Sequence
Shear 120 17.0 1.00 [-45◦ ;45◦ ]𝑠
Longitudinal 110 15.0 1.00 [0◦ ]4
Transverse 100 20.0 1.00 [90◦ ]4

2.3. Statistical analysis and interpolation
The Matlab function anova1 has been used to perform a one-way
analysis of variance (ANOVA) to compare the statistical performance of
the measured data. Sets of data are considered as statistically equivalent
if p >0.005, i.e. they have a 5% or less chance of being statistically
different. In ANOVA studies, the F(k-1,N-k) values given represents the
ratio of the variance between the group compared and the variance
within the groups compared. The F values are given with k: the num-
ber of groups of data compared and N: the total number of values
considered in the groups compared. Consequently, the higher the F
value the more different the values compared are. The relation between
material properties and RH is modelled using a continuous interpo-
lation function. Linear, exponential and sigmoid interpolation were
considered. The exponential and linear interpolations are performed
using the options of the fit function (exp1 and poly1, respectively).
The sigmoid interpolation is performed using the Sigm_fit function. The
highest correlation coefficient between the three types of fitting allows
selecting the best interpolation. The coefficient of variation (CV) is
calculated via the standard deviation to average ratio.
3. Results and discussion
3.1. Printing pattern and specimen quality
The filament cannot be cut during the deposition. Therefore, the
change of direction of the nozzle when the edge of the specimen is
reached creates a filament loop. These u-turns of the nozzle at the edges
Fig. 2. Example of the edge of a specimen for shear loading (SEM image). The full
dark blue arrows point to the macro voids created at the edge due to the u-turn of the
nozzle. The dashed light blue arrows point to the stair like edges.
are highlighted in Fig. 1 for the different types of specimens. The u-
turn edges are problematic due to the difficulty of for the filament
to stick to its support layers. After each u-turn, the contact surface
between the filament and the support is not large and the filament
is pulled out from the same surface over a short distance. The small
distance the filament needs to stick to the support layer creates stepped-
like edges, as displayed in Fig. 2. The difficulty for the filament to
stick to its support layer and the stepped-like edges currently prevent
this technique from being used to build thick individual specimens for
transverse and shear test specimens. Such stepped-like edges lead to an
underestimation of the stiffness and strength due to an overestimation
of the section measured.
In Supplementary data 1. is described the process for porosity and
fibre volume fraction measurement. For both these properties, intervals
of 3%–6% and 28%–31% were obtained respectively. A previous study
provides a summary of the porosity in continuous flax fibre composites
from several references in the open literature [35]. Porosity measured
via gravimetric techniques in ethanol provide values ranging from
6.9% to 8.3%. SEM and optical microscopy provide porosity between
1.5% to 10.3%. The porosity measured is indicative of the quality
of the material produced. Further work must still be carried out in
future to increase the fibre volume fraction of the flax/PLA 3D printed
composites without degrading the quality.

3
C. de Kergariou et al. Composites Part A 155 (2022) 106805

Fig. 3. (a) : Influence of the MC on the transverse modulus: E𝑡 ; (b): Influence of MC on the longitudinal moduli E1 and E2 .

Table 3
Strength and strain at failure at different MC values: 𝜎𝑡 , 𝜎𝑙 and 𝜏 transverse, longitudinal and shear strength, respectively. 𝜈,
𝜖 and 𝛾 are the transverse, longitudinal and shear strain at failure, respectively.
MC (%) 0.24 0.96 1.65 2.31 6.01
𝜎𝑡 (MPa) 7.97 ± 1.39 7.62 ± 0.59 6.48 ± 1.49 5.79 ± 0.98 4.45 ± 0.81
𝜈(𝜇𝜖) 6.11 ± 1.83*103 5.71 ± 2.34*103 5.63 ± 1.98*103 4.56 ± 0.90*103 1.80 ± 4.98*103
𝜎𝑙 (MPa) 186 ± 11.5 201 ± 4.76 193 ± 11.2 194 ± 11.4 178 ± 13.4
𝜖(𝜇𝜖) 1.39 ± 0.75*104 1.78 ± 0.76*104 1.97 ± 1.03*104 2.47 ± 1.08*104 3.20 ± 0.32*104
𝜏 (MPa) 20.5 ± 1.54 20.2 ± 0.45 18.0 ± 0.87 16.2 ± 0.53 11.2 ± 0.53
𝛾(𝜇𝜖) 3.11 ± 0.42*104 3.31 ± 0.19*104 3.12 ± 0.36*104 4.88 ± 0.38*104 4.98 ± 0.94*104

Fig. 4. Influence of MC on the shear modulus G12 .
3.2. Mechanical properties
Figs. 3 (a), 3 (b) and 4 show the influence of the MC on the
stiffness of transverse, longitudinal and shear specimens. Examples
of stress strain curves obtained for specimens subjected to different
relative humidity conditioning are presented in Supplementary data 2.
All the stiffness values are interpolated with exponential functions. A
similar interpolation approach has been used in the past for thermo-
compressed FFRPLAs [15]. Table 3 shows the values of strength and
strain at failure for the transverse, longitudinal and shear specimens.
The decrease of the transverse modulus between specimens condi-
tioned at 10% RH and those at 98% RH is here close to 64%. To the
best of the authors’ knowledge, the effect of not immersed RH conditions
on Young’s modulus of pure PLA specimens has not been evaluated
so far. On the other hand, immersion has been demonstrated to lower
the T𝑔 of the PLA matrix [26]. The softening of the PLA due to water
molecules is responsible for the lowering of the stiffness when the RH
levels increase. The values of the CVs for the modulus show very similar
trends as those related to the strength (10.9%, 5.6%, 4.9%, 24.1%
and 32.7% for specimens conditioned at 10%, 30%, 50%, 75% and
98%). The large scatter observed for the high RH values highlights the
difficulty of producing composites with repeatable filament distribu-
tion, bonding between filaments and flax yarn matrix bond strengths.
The fracture inspection section highlights the key role of these param-
eters during failure of transverse specimens. The average transverse
strength exponentially decreases by 44.4% from 10% to 98% RH. The
coefficients of variation are 17.4%, 7.7%, 22.9%, 16.9%, 18.2% for
the strength of the specimens conditioned at 10%, 30%, 50%, 75%,
98%, respectively. The variability in the transverse filament properties
and in fibre matrix interface due to the heterogeneous microstructure
of the fibres, the printing and the co-extrusion techniques used to
produce the filament are causes for this large scatter. All the specimens
failed at the junction of two successive filament superpositions (see
Supplementary data 3.). As it will be described in the fracture analysis
section, the transverse strength is mostly driven by the matrix and the
flax yarn matrix interface properties. Hence, the value of the relative
humidity to condition the specimens has an impact on one or both of
these properties. Foruzanmehr et al. and Deroine et al. have shown
the potential to damage the PLA by immersion [29,30]. High values
of humidity conditioning contribute to weakening the flax yarn matrix
interface of the specimen [20].
The longitudinal modulus is shown to exponentially decrease with
the increase of the RH. Decreases of 63.8% and 58% are observed
between the 10% RH conditioned specimens and the 98% for E1 and
E2 , respectively. Low CVs are obtained: 4.9%, 12.6%, 13.6%, 2.2%,
8.4% for the E1 and 3.6%, 1.4%, 4.1%, 7.3%, 5.5% for the E2 for
the specimens conditioned at 10%, 30%, 50%, 75%, 98%. Despite the
natural origin of the fibres, the low CVs measured here highlight the
efficiency of the print to obtain repeatable longitudinal stiffness at
every RH tested. The stiffness of the longitudinal specimens is mostly
driven by the fibres. Vincent et al. specify that water molecules tend to
penetrate the cellulose network via bonding to the amorphous polymers
inside the flax fibre to lower the rigidity of flax fibres [27,28]. The
variation of the stiffness versus the RH level in two different types of
flax fibres has been described in a previous study [36]. One type of

4
C. de Kergariou et al.
fibre used in that study showed a stiffness level off over the entire
range of RH values considered (from 21% to 85%). The other type of
fibre tested was however stiffer when the RH range varied from 21%
to 68% and then dramatically increased for 85% RH. Similar behaviour
was highlighted by Davies et al. with a stiffness increase from 30% to
50% and then decreasing when 60% and 70% were reached [37]. The
stiffness was however observed as decreasing over the full RH range
considered (30% to 70%) when adjusted to the amount of damage
(i.e., non-homogeneous cell wall structure) inside the fibres. Flax fibres
are softened by increasing levels of RH conditioning. Their internal
quality affected by the production process and the format in which they
are used (twisted yarn or straight fibre) have, however, an important
influence on the properties of the resulting composite. It is hence
important to consider the structural configuration in which the fibres
are used. In the present study, the flax fibres are twisted together to
form the flax yarn used in the printing filament. The plasticizing effect
of the water on the polysaccharide inside natural flax fibre leads to
lowering the flax yarn stiffness when the moisture content goes from
1.8% to 7.6% [38,39]. Such reduction of the stiffness of the flax yarn
is also a reason for the lowered rigidity of the 3D printed composites of
the present study. The longitudinal strengths are considered statistically
equivalent over the four smallest MCs (F(3,15) = 1.84; p = 0.1826).
In all the different specimens, part of the failure section is located
at the end tab junction (see Supplementary data 3.). Consequently,
the end tabs influence the values of the strength obtained. Water
has been demonstrated to provide a positive plasticizing effect on the
strength of flax fibres [40]. Requile et al. have observed increasing
values of the tensile strength between 9% and 75% RH for hemp fibre
reinforced epoxy composites [31]. The plasticization of the fibre was
described as a potential factor playing a significant role. The greater
stress transfer at the fibre matrix interface due to the expansion of
the fibres was also quoted as a potential source of strength increase.
Similarly to what has been observed in the present study, the strength
decreased for larger RH values (98%RH). Moudood et al. have also
shown the tendency of the moisture to debond fibres from the matrix,
leading to the lowering of the composite strength [41]. However, such
debonding can occur differently at the yarn scale. From single yarn
tensile tests, Masseteau et al. have shown an increase of the tensile
strength when the MC inside the fibres was increased from 1.5% to
7.6% [39]. These influences tend to compensate each other, causing
the presence of a statistically constant strength value over small MC
variations, with CVs equal to 6.2%, 2.4%, 5.8%, 5.9% and 7.6% for
specimens conditioned in ascending order of RH. The lowering of the
strength in longitudinal composites intensify for the highest RH (98%
RH) and leads to statistically different longitudinal strength for the
five sets of specimens conditioned at different RH (ANOVA: F(4,19)
= 3.06, p = 0.042). The values obtained do not allow to obtain an
interpolation for the longitudinal strength versus the variation of the
moisture content.
The shear modulus and strength exponentially decrease when the
moisture content increases. The ASTM D3518 specifies that the stiffness
of the shear specimens is driven by the ductility of the matrix, the
strength of the flax yarn matrix interface and the number of plies.
The latter is not be affected by the change in relative humidity, hence
it is ignored. In the previous discussions about transverse stiffness,
the PLA matrix was shown to be softened by humid conditions [26].
The fractographic inspection highlights indeed the weakening of the
fibre–matrix bonding with the relative humidity. The causes for the
influence of the RH on the shear stiffness are therefore similar to those
described when discussing the transverse modulus. A very low scatter
is observed for the measured values of the shear strength and stiffness.
The CVs are 4.6%, 3.6%, 4.4%, 5.9%, 4.3% for the shear modulus,
and 7.5%, 2.2%, 4.8%, 3.3%, 4.7% for the shear strength at the 10%,
30%, 50%, 75%, 98% RH, respectively. Those coefficients show that the
overall production, conditioning and testing processes were efficient
and allowed to measuring consistent shear mechanical properties. As
5
Composites Part A 155 (2022) 106805
described in the fracture inspection section, the interlaminar cracks
generated between two plies can be responsible for the complete failure
of the specimen. The interlaminar cracks also facilitate the initiation
of the intralaminar fissures that are responsible for the failure of the
shear specimens. The interlaminar cracks are more likely to appear
and propagate in high RH conditioned specimens, leading to a 44.3%
decrease in shear strength between 10% and 98% RH. As described
previously for the transverse and longitudinal specimens, both flax
fibres and PLA are softened by the RH conditioning, leading to the 48%
decrease of shear modulus observed between 10% and 98% RH.
The mechanisms used to discuss the influence of the relative hu-
midity on the transverse, longitudinal and shear strength is extended
to explain the behaviour of the strain at failure.
The discussions about the coefficients of variation for the different
specimens have shown the robustness of the production, conditioning
and testing processes in this work, with small scatter associated with
the longitudinal and most shear mechanical properties. The large scat-
ter obtained for the transverse strength and modulus highlights some
room for improvement to obtain consistency regarding the flax yarn
matrix interface properties.
The edges of the u-turn filament depositions affect the transverse
mechanical properties. Todoroki et al. have shown that cutting the u-
turn edges reduces the strength and stiffness of transverse specimens,
however, it increases the shear strength [34]. The ASTM 3039 standard
specifies that both the cutting and edge effects have an impact on the
material properties measured, without specifying which has the great-
est impact. The production of individual specimens allows identifying
in a more high-fidelity manner the material properties by limiting the
impact of the cutting technique. On the other hand, the presence of the
u-turns increases the gap between the effective material and the mea-
sured properties. The ideal specimens should be individually moulded
without the presence of u-turn edges. To the best of our knowledge,
an open 3D printing machine capable of cutting during production the
filament still has to be designed. The impact of edges of the u-turns
is negligible for the longitudinal specimens, as the filament loops are
located between the end tabs. In that sense, the longitudinal specimens
fit the recommendations from the ASTM standard, as neither the cut
nor the edge effects have an impact on the measured properties. On the
contrary, the present study shows a significant impact on the properties
of the longitudinal specimens provided by the variation of the RH.
This proves the existence of an effect of the edges of the filament u-
turns on the behaviour of material properties in the transverse and
shear specimens as the u-turns are longitudinal yarns in these tests. A
quantification of this impact is beyond the scope of this study.
3.3. Fractography
Figs. 5, 7 and 9 show examples of failed longitudinal, shear and
transverse specimens conditioned at 10% and 98% RH, respectively.
Fig. 6 shows in three stages the evolution of a crack during tensile
loading. The first stage is highlighted in Fig. 5 with the full arrows
pointing towards the multiple resin cracks appearing along the speci-
men length. In the second stage, these intralaminar cracks propagate
in the material perpendicularly to the loading direction, until they
reach the filaments. When those cracks end at the fibres, two different
events can occur (see Fig. 6: third stage). The fibre may break in
tension and the crack then propagates in the same plane; an example
of such fracture is given in Fig. 5 (a). The cracks can also split the
yarn matrix interface, therefore creating a deflection in the crack path.
This phenomenon is pointed out by the dashed arrows on Figs. 5 (e)
and (f). The specimens conditioned at 10%, 30%, 50% and 75% show
little debonding between yarn and matrix and fail almost entirely with
fibre fracture (a typical failure crack path is shown in Fig. 5 (c), the
red lines present little deflection in the crack path highlighted). On the
other hand, the specimens conditioned at 98% present a great amount
of flax yarn matrix debonding (Typical failure in Fig. 5 (d), the red lines
C. de Kergariou et al. Composites Part A 155 (2022) 106805

Fig. 5. Fractured longitudinal specimen and corresponding microscope images: (a), (b) and (c) images correspond to 10% RH and the (d), (e) and (f) correspond to the 98%
RH conditioned specimens. (a), (b), (c) and (d) are microscope images. Full arrows pointing upwards point to matrix fractures. Dashed arrows pointing downwards point to yarn
matrix splitting. The red lines in images (c) and (d) present the crack path which failed the specimens.

Fig. 6. Schematics of the three stages associated to the failure of the longitudinal specimens. Inspired by the Cook and Gordon mechanism in Greenhalgh et al. [20]. The three
stages mechanisms are common to all the RH conditioned specimen. For the third stage, the 98% RH conditioned specimens present larger amount of matrix debonding from the
yarn than in specimens conditioned at lower humidity.

presents a highly deflected crack path). As specified by Greenhalgh
et al. high moisture content tends to deteriorate significantly the fibre
matrix interface for fossil fibre composites [20]. The strength of the
interface between hemp fibre and epoxy was shown to increase from
9% to 50% and decrease from 50% to 98% [24]. Raj et al. observed
an increased interfacial strength between flax and PLA with rising RH
levels (between 2% and 56%) due to the formation of a meniscus at
the interface [25]. Such adhesion by capillarity is combined at low
RH levels with an expansion of the flax yarn, creating a greater stress
transfer at the interface and enhancing the bonding. Such phenomenon
was proposed by Requile et al. for hemp epoxy composite [31]. To
explain the decrease of the interfacial strength between 50% and 98%
RH, Requile et al. provided a model in which the condensation of the
water at the interface leads to a thick layer of water being created [24].
This water creates hydrogen bonds with the hydroxyl groups of the
natural fibres and the matrix. This phenomenon leads to a reduction
of the interaction between the fibre and the matrix, hence lower
interfacial strength. The mechanisms of interaction between fibre and
matrix are considered as the main cause for the difference in fracture
patterns.
In Fig. 7 the full and dashed arrows point at failed fibres and
at the matrix failure, respectively. Fig. 8 presents schematics of all
different types of fracture mechanisms described in the present section.
The DIC inspection shows that the shear deformation occurs along
the length of the specimens for all the relative humidity values here
considered. However, the failure aspect of the specimens changes with
the specific relative humidity. Fig. 7 (c) shows the presence of wavy
yarns at the fracture surface. In such specimens, the stresses break
the matrix, leading to an intralaminar propagation of the crack. An
example of such fracture is given in Fig. 7 (a). Once the matrix has
failed the fibres are subjected to tension parallel to the loading direction
and hence deform in the wavy shape of Fig. 7 (a) and (b). At this
stage, the fibres inside the filament fail. The specimens conditioned
at high RH values (98% RH) show a little presence of fibre fracture.
The full arrow pointing downwards on Fig. 7 (d) highlights a filament
debonded from its layer and also its support layer, but not broken.
Similarly to the case of the longitudinal specimens, high RH values
here weaken the yarn matrix interface. In Fig. 7 (f) the half arrow
indicates the direction of propagation for the filament–matrix shear
debonding. Fig. 7 (e) shows the filament matrix debonding between the
upper and its support laminae. The dashed arrows pointing downwards
indicate specifically the support laminae. The 90◦ difference in filament
orientation between these two plies leads to the generation of stresses at
the interface of the two plies. The weak yarn matrix interface then fails
and initiates delamination, while a shear deformation common to all
specimens occurs. Such interlaminar failure propagates along the length
of the specimen at the interface of the plies. Delamination can fail the
specimen on its own, see Fig. 7 (d). It can also facilitate the intralaminar
fracture common to specimens conditioned at lower RH. Delamination
also explains the decrease in shear strength shown in Fig. 4.
In Fig. 9 the full and dashed arrows indicate the failure of the
matrix and the yarn matrix interface fracture surface, respectively. For
all the relative humidity values used here, the failure of the trans-
verse specimens initiate at the edge of the samples and propagates

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C. de Kergariou et al. Composites Part A 155 (2022) 106805

Fig. 7. Fractured in-plane shear specimen and microscope images: (a), (b) and (c) images correspond to 10% RH and the (d), (e) and (f) correspond to the 98% RH conditioned
specimens. (a), (b), (c) and (d) are microscope images. Full arrows pointing upwards present fibre fracture. The full arrow pointing downwards highlight the support ply of
delamination for specimens conditioned at high RH. The dashed arrows pointing upwards indicate the matrix fracture in shear. The dashed arrows pointing downwards are related
to the resin fracture during delamination, as the yarn do not present any matrix on their surface. Dashed blue arrows show the shear deformation occurring inside the specimens.

Fig. 8. Schematics of the different ways the cracks propagates in the shear specimens. The yarn fracture is observed for 11%, 35%, 50% and 75% RH. On the other hand,
interlaminar delamination is noted for the 98% RH conditioned specimens.

perpendicularly to the load direction between fibres (see interfilament
debonding in Fig. 10). The optical microscope showed that failure
alternates between filament–matrix interface debonding and matrix
fracture at the interface between filament through the entire width
of the specimens (see yarn matrix debonding in Fig. 10). The crack
jumps occasionally through a yarn (see crack jump through yarn in
Fig. 10). Such type of fracture is however rare and cannot explain
the influence of the RH conditioning on the transverse properties of
the composite. No significant differences are observed between the
specimens conditioned at different RH values.
3.4. Energy dissipated during tests
Fig. 11 presents the area underneath the stress–strain curve for the
transverse, longitudinal and shear specimens.
The area underneath the stress–strain curve represents the energy
dissipated during the fracture of the transverse specimens. Fig. 11 (a)
shows the presence of a constant area underneath the stress–strain
curve related to the first four MC values. Only the 98% RH conditioned
specimens display an increase in energy dissipated. The following
distribution of the CVs is obtained for transverse specimens: 41.3%,
53.4%, 21.6%, 39.9% and 30.2% for the specimens conditioned at 10%,
30%, 50%, 75% and 98% RH, respectively. Those high values of the
coefficients of variation also explain the statistical equivalence between
the areas underneath the stress–strain curves of the different RH con-
ditioned sets of specimens (F(4,12) = 5.76 𝑝 = 0.008 from ANOVA).
The failure surface inspection of transverse specimens described frac-
ture characteristics as independent from their conditioning RH. Hence,
relative humidity has a small impact on the energy dissipated during
failure of a transverse specimens.

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C. de Kergariou et al. Composites Part A 155 (2022) 106805

Fig. 9. Fractured transverse specimen and microscope images: (a), (b) and (c) images correspond to 10% RH and the (d), (e) and (f) correspond to the 98% RH conditioned
specimens. (a), (b), (c) and (d) are microscope images. Dashed arrows pointing downwards indicate yarn matrix debonding. Full arrow directed upwards point to matrix fracture.

Fig. 10. Schematics of the three different ways the cracks propagates in the transverse specimens.

Fig. 11. Area underneath the stress–strain curve (AUC) for the following specimens: (a): Transverse, (b): Longitudinal, (c): In-plane shear.

The area underneath the stress–strain curve of longitudinal speci-
mens increases by 91.5% from 10% RH until it plateaus at high relative
humidity values (Fig. 11 (b)). The CVs in this case are 11.7%, 6.8%,
9.9%, 6.4%, 6.3% for the specimens conditioned at 10%, 30%, 50%,
75% and 98% RH. The coefficients of variations show that the values of
the energy dissipated are all statistically reliable. The area underneath
the stress–strain curve obtained from tensile tests on flax fibre yarns
increases with an increase of the moisture content [39]. Hence, the
plasticization of the flax fibre polysaccharides by water leads to an
increase in energy dissipated by the flax fibres during the longitudinal
tensile test. Another parameter that affects the energy dissipated during
the test is the crack propagation process described in the fracture
inspection section of the paper. The influence of the crack propagation
in the energy dissipation has been also observed by Bensadoun et al. in
flax epoxy composites [42]. Specimens conditioned at 98% RH tended
to fail more under flax yarn matrix debonding leading to larger crack
deflection compared to specimens conditioned at lower RH values.
The fracture of more material is indicative of greater amounts of
energy dissipated. The areas underneath the longitudinal stress–strain

8
C. de Kergariou et al.
curve was approximated by the sigmoid interpolation function f(MC) =
−1
-7.4*107 +7.7*107 /(1+10(−(5.3+𝑀𝐶)∗3.1∗10 ) ).
The area underneath the stress–strain curve for the in-plane shear
specimens (Fig. 11 (c)) is shown to be statistically identical over the
range of the RH values tested (F(4,20) = 3.51 p = 0.025), with the
following CVs observed (18.9%, 5.9%, 13.6%, 8.7% and 22.9% for
the specimens conditioned at 10%, 30%, 50%, 75%, and 98% RH,
respectively). The large scatter observed is explained by the difficulty
to obtain identical internal structures for the specimens due to the 3D
printing process, natural characteristics of flax fibre and the quality of
the yarn. The results of the ANOVA are also partially explained by the
large standard deviation obtained, specifically within the 10% and 98%
RH conditioned specimens. The in-plane shear specimens area under-
neath the stress–strain curve is affected by the deformation and fracture
mechanisms highlighted by the DIC and fracture inspections. The DIC
inspection performed on the shear specimens showed the formation
and presence of shear bands. The distribution of the shear strain on
the upper surface of specimens conditioned at different RH values is
found in the Supplementary data 4. These shear bands parallel to the
fibre direction are observed along the length of the entire specimen
for all the different RH values. The DIC inspection shows the creation
of shear bands across the length of each specimen, independently of
the value of RH. The ASTM D3518 standard specifies that the ±45◦
laminae tend to align the fibres with the load direction, when loaded in
tension. The standard specifies that each 2000𝜇𝜖 corresponds to 1◦ re-
orientation of the fibres. The standard also indicates that the weaker the
fibre–matrix interface and the more ductile the matrix, the larger the
fibre scissoring causing the realignment. The PLA 3001D matrix shows
some plastic deformation capability [43]. Furthermore, the 0.8 mm
distance between filaments creates a small resin-rich area between
the same filaments, see porosity measurement in Supplementary data
1. During scissoring, the yarns compress and pull the surrounding
matrix rich areas, with the induced stresses dissipating energy. The
higher the interfilament distance, the lower the support between yarns
and the greater the energy dissipated with this mechanism. Table 3
shows that the three sets of specimens conditioned with the lowest
RH value present identical and low strains at failure compared to the
75% and 98% RH conditioned specimens. This explains the large area
underneath the stress–strain curve of the 75% conditioned specimens.
The high energy dissipated during the scissoring of the yarns of the
98% RH specimens is however compensated by another mechanism.
The inspection of the related fractures has shown that the low flax
yarn matrix interface strength resulting from the high moisture content
in the specimen led to interlaminar failure, whereas for the other
specimens intralaminar failures were responsible for the breakage of
the samples. de Moura et al. showed that in DCB test 60% of the energy
dissipated is due to fibre bridging [44]. As described in the fracture
section of the paper interlaminar failure limits the importance of the
fibres on the fracture behaviour. The interlaminar fracture responsible
for the premature failure of the composite (see Table 3) explains
the lower area underneath the stress–strain curve exhibited by the
specimen conditioned at 98%.
4. Comparison with data from open literature
Fig. 12 shows a comparison between the shear, transverse and
longitudinal properties of continuous fibre 3D printed composites of
this study and analogous values found in the open literature. The
comparison is made taking into account the resin and fibres. Fossil fibre
filaments are the most widely used compared to their natural counter-
part, and they are also considered in this benchmark. Polyamide is the
most widely used matrix due to its extended use in Markforged supplied
materials. Natural fibres filaments lack however such availability at the
moment, and they are mainly produced in house.
A rule of mixture interpolation is plotted in Figs. 12 (a) and (b)
via the curve_fit Python function from the scipy.optimize library. The
9
Composites Part A 155 (2022) 106805
impact of the matrices was neglected compared to the fibres for this
rule of mixture interpolation. These interpolations show that carbon
and aramid fibre specimens are obviously stiffer and stronger in the
direction of the fibres, compared to the analogous natural fibre com-
posites. The FFRPLAs also present a lower strength compared to glass
fibres. However, in terms of stiffness, identical ranges are achievable
by glass and natural fibres, although more tensile stiffness and strength
values for natural fibre 3D printed composites are necessary to confirm
this trend. Non-3D printed continuous flax fibres composites usually
present tensile strength and stiffness in the same range as 3D printed
continuous synthetic fibres composites [4]. Fig. 12 also shows the
limited fibre volume fraction currently achievable in natural fibres
3D printed composites compared to their fossil fibres composite coun-
terparts. This reduces the available range of stiffness and strengths.
The properties obtained in the present study are however amongst the
best ones featured by natural fibre 3D printed composites, despite the
environmental conditioning they underwent. The CVs range between
0.14% [45] and 47.9% [46] with a 8.58% average for the longitudinal
stiffness. The present study features an 8.33% average for the CV. The
CV ranged from 0.22% [45] to 25.36% [47] with a 6.98% average for
the longitudinal strength. The same coefficient in the present study is
however lower (5.55%). These two comparisons show that the results
of our work present similar if not lower scatters than those found in
the open literature.
Figs. 12 (c), (d), (e) and (f) show that limited investigation has
been made so far on the transverse and shear properties of 3D printed
composites with continuous fibres. Figs. 12 (c) and (d) shows that
polyamide and carbon-based composites appear to be superior in terms
of transverse and shear stiffness and strength, compared to PLA-based
natural fibres composites. In terms of transverse stiffness, aramid fi-
bres are stiffer than their natural counterparts. However, in terms
of transverse strength and shear strength and stiffness, the natural
fibres achieve similar performances to their aramid counterparts. The
transverse properties of glass and natural fibre composites appear to
be similar. To the best of the authors’ knowledge, the present study
is the first to describe the shear properties of 3D printed continu-
ous natural fibres filament composites. It is also the second time the
transverse properties of this type of 3D printed composite material
are measured. More measurements are however required to confirm or
overturn these trends. As described in previous paragraphs, the relative
humidity conditioning impacts the fibre–matrix interface, hence the
transverse and shear properties of the 3D printed composites. The
comparison of the transverse properties found in the open literature
for non conditioned specimens (the green circles in Fig. 12 (c) and (d))
gives a greater insight into the properties achievable by this type of
material. The behaviour of the matrix is essential for the mechanical
transverse and shear properties. The use of a different matrix from the
conventional PLA one is a solution to improve the material properties
of FFRPLAs. The CVs for the transverse stiffness in the literature range
from 1.94% [5] to 47.55% [5] with a 15.72% average. The average
CV value obtained here is 14.32%. The CVs of the transverse strength
range from 0.26% [46] to 65.24% [7] with a 17.1% average. The
CV obtained in this study is consistent, being equal to 16.62%. The
large scatter for the measurement of the transverse properties also
observed in the present study confirms the difficulty in obtaining stable
3D printed materials. The CVs of the shear stiffness identified within
the few papers publishing standard deviations of the shear mechanical
properties range from 2.98% [5] to 11.36% [48], with an average of
5.2%. The CV observed in the present study is 4.55%. The CVs for
the transverse strength range from 2.18% [46] to 44.99% [7] with an
average of 8.62%. The average of CV obtained in the present study
is a lower 4.52%. One aspect to notice is the small scatter of the
shear properties amongst the few statistical values available in the open
literature.
C. de Kergariou et al.
Fig. 12. Comparison with data from open literature related to 3D printed continuous fibre composites: (a) Longitudinal tensile modulus, (b) Tensile strength, (c) Transverse Young’s
modulus, (d) Transverse strength, (e) Shear stiffness and (f) Shear strength. The references for this graph are presented in a Table in Supplementary data 5.
5. Conclusion
In this work, 3D printed 30% fibre volume fraction continuous flax
fibre reinforced PLA specimens have been produced to observe the
impact of the environmental conditioning via not immersed relative
humidity on the transverse, longitudinal and in-plane shear mechanical
properties. The printing pattern was shown to influence the porosity of
the composite obtained. The porosity of the material has been estimated
with a gravimetric measure in ethanol to be 4.32%, 5.31% and 6.2%
for the shear, longitudinal and transverse specimens respectively. SEM
measures of the porosity have provided analogous values of 2.73%,
3.15% and 3.6%. From this study the following conclusions are drawn:
• Shear, transverse strength and stiffness and longitudinal stiffness
show an exponential decrease as the moisture content condition-
ing increases.
• Decreases of 44%, 64%, 64%, 58%, 48% and 44% have been
observed between 10% and 98% conditioning humidity for the
transverse strength and modulus, longitudinal modulus E1 , E2 ,
shear strength and modulus, respectively.
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Composites Part A 155 (2022) 106805
• Conditioning the specimens at different humidity levels leads to
an evolution of the failure of the composites. Higher humidity lev-
els lead to greater yarn matrix debonding for the longitudinal ten-
sile tests. High RH values also lead to lower intralaminar fracture
and greater interlaminar failure in shear specimens. No significant
difference in the failure process is observed between the various
transverse specimens conditioned at different humidity levels.
3D printed continuous natural fibre composites, including the ones
described in the present study, show promising longitudinal, transverse
and shear stiffness values when compared against their glass and
aramid counterparts. On the other hand, the strength provided by the
three types of specimens was low compared to analogous one from
fossil fibres-based 3D printed composites. The increase of the fibre
volume fraction for the composites produced in the present study will
reduce the performance gap with the carbon fibres-based mechanical
properties. An improvement of the low transverse and shear properties
might require the use of different types of matrices. The broader use
of 3D printed natural filaments in the industry will require more
investigations to deepen our knowledge of the transverse and shear
properties of 3D printed sustainable composites.
C. de Kergariou et al.
CRediT authorship contribution statement
Charles de Kergariou: Investigation, Methodology, Writing – orig-
inal draft, Conceptualisation, Formal analysis, Software, Visualization.
Hind Saidani-Scott: Supervision, Resource. Adam Perriman: Super-
vision. Fabrizio Scarpa: Supervision, Methodology, Writing – review
& editing, Conceptualisation, Funding acquisition, Project administra-
tion, Resources. Antoine Le Duigou: Supervision, Writing – review &
editing, Resources, Methodology.
Declaration of competing interest
The authors declare that they have no known competing finan-
cial interests or personal relationships that could have appeared to
influence the work reported in this paper.
Acknowledgement
The author would like to thank the UK Defence Science and Tech-
nology Laboratory for the funding received for this project through the
UK-France Ph.D. Scheme. Grant ID: DSTLX-1000141168
Appendix A. Supplementary data
Supplementary material related to this article can be found on-
line at https://doi.org/10.1016/j.compositesa.2022.106805. Informa-
tion about porosity and fibre volume fraction, examples of stress-strain
curves, macro images of failed specimens, DIC images of shear speci-
mens and references for comparison of the mechanical properties can
be found in Supplementary data.
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