Article

Impact of Defects on Tensile Properties of Ancient and Modern

Egyptian Flax Fibers: Multiscale X-Ray Microtomography and
Numerical Modeling
Vasuki Rajakumaran 1, *, Sofiane Guessasma 1 , Angélina D’Orlando 1 , Alessia Melelli 2 , Mario Scheel 2 ,
Timm Weitkamp 2 , Jonathan Perrin 2 , Alain Bourmaud 3 , Henry Proudhon 4 and Johnny Beaugrand 1, *

1 UR1268 Biopolymères Interactions Assemblages, INRAE, F-44316 Nantes, France;

sofiane.guessasma@inrae.fr (S.G.); angelina.dorlando@inrae.fr (A.D.)
2 Synchrotron SOLEIL, F-91190 Saint-Aubin, France; alessia.melelli@synchrotron-soleil.fr (A.M.);
mario.scheel@synchrotron-soleil.fr (M.S.); timm.weitkamp@synchrotron-soleil.fr (T.W.);
jonathan.perrin@synchrotron-soleil.fr (J.P.)
3 IRDL, University Bretagne Sud, UMR CNRS 6027, F-56100 Lorient, France; alain.bourmaud@univ-ubs.fr
4 MINES Paris, MAT—Centre des matériaux, PSL University, CNRS UMR 7633, BP 87, F-91003 Evry, France;
henry.proudhon@minesparis.psl.eu
* Correspondence: vasuki.rajakumaran@inrae.fr (V.R.); johnny.beaugrand@inrae.fr (J.B.)

Abstract: Flax fibers, while offering numerous benefits, are susceptible to mechanical weakening
due to the presence of kink-bands within their structure. The novelty of this study lies in linking
mechanical behavior to fiber morphology and defects at multiple scales by utilizing X-ray microto-
mography to generate detailed 3D images of elementary flax fibers, enabling the creation of accurate
finite element (FE) models for analysis. Aging reduces flax fibers’ strength, so both modern and
ancient fibers were analyzed to understand their structural evolution over time. Static X-ray mi-
crotomography images were converted into 3D FE models for tensile simulations, and tensile tests
Citation: Rajakumaran, V.; Guessasma,
provided essential properties for numerical modeling. Morphological analysis for both fiber types
S.; D’Orlando, A.; Melelli, A.; Scheel, M.;
revealed that kink-bands contain multiple pores oriented ~45◦ to the fiber/lumen axis, with ancient
Weitkamp, T.; Perrin, J.; Bourmaud, A.;
fibers showing higher porosity (5.6%) and kink-band density (20.8 mm−1 ) than modern fibers (3.3%
Proudhon, H.; Beaugrand, J.. Impact of
and 16.6 mm−1 ). SEM images confirmed that the intricate lumen and kink-bands lead to fiber failure
Defects on Tensile Properties of
Ancient and Modern Egyptian Flax
under tensile loading. Numerical analysis highlighted higher stress concentrations at the kink-band
Fibers: Multiscale X-Ray region, particularly at pores in the kink-band region, which can initiate cracks and lead to rupture.
Microtomography and Numerical
Modeling. Fibers 2024, 12, 111. Keywords: morphology; ancient fibers; microstructure; kink-bands; FEM
https://doi.org/10.3390/
fib12120111

Academic Editor:
1. Introduction
Francesco Bencardino
Composite materials are replacing metals, ceramics, and wood due to their specific
Received: 31 August 2024
superior properties. Typically made with carbon, glass, and aramid fibers, they are expen-
Revised: 17 October 2024
sive, non-recyclable, non-biodegradable, and pose health risks [1]. Plant fibers like flax and
Accepted: 2 December 2024
hemp offer an eco-friendly alternative for reinforcement [2,3]. However, defects occurring
Published: 16 December 2024
during the extraction process or authentic to the plant growth conditions can reduce their
mechanical properties [4,5]. To optimize their use, it is crucial to understand the relation-
ship between these structural defects and mechanical properties at multiple scales [6],
Copyright: © 2024 by the authors. including elementary and bundle fibers. To address this, a combination of experimental
Licensee MDPI, Basel, Switzerland. and numerical analysis was applied in this study for both elementary and bundle flax
This article is an open access article fibers. Aging can reduce the strength and stiffness of flax fibers, impacting the durability
distributed under the terms and and performance of composites [7]. Research on fiber aging examines how durability and
conditions of the Creative Commons degradation affect structural changes over time [8,9]. This study uses ancient Egyptian flax
Attribution (CC BY) license (https:// fibers to explore how structural morphology evolves and investigates the effects of defects
creativecommons.org/licenses/by/ on mechanical responses.
4.0/).

Fibers 2024, 12, 111. https://doi.org/10.3390/fib12120111 https://www.mdpi.com/journal/fibers

Fibers 2024, 12, 111 2 of 22

Elementary flax fibers have a complex structure composed of multiple cell wall layers,
including the primary cell wall (PCW) and the secondary wall (S), which is further divided
into S1, S2, and S3 layers. The S2 layer, being the thickest, significantly contributes to the
fiber’s strength and stiffness due to its microfibrils oriented nearly parallel to the fiber
axis [10]. The central hollow cavity, or lumen, runs through the length of the fiber, varying
in size and shape [11]. Flax fiber bundles are composed of multiple elementary fibers bound
together by middle lamella, which is composed of pectin and hemicellulose [12,13]. This
structure varies in regions with defects, which can undermine reinforcing capabilities. Kink-
bands are areas with irregular cellulose microfibril arrangement that disrupt mechanical
properties [14]. Despite dislocations in up to 20% of hemp fiber cell walls, they showed no
significant impact on tensile properties [15]. However, a negative correlation was found
between kink-band area and Young’s modulus, with flax fibers over 75 GPa typically having
less than 15% kink-band density [16]. Defects in elementary fibers cause significant shifts
in cellulose orientation (30◦ –40◦ ) and increased porosity, especially in the S2 layer [17–19].
These issues lead to microfibril angle deviations and localized pore formation, which act as
rupture points and affect mechanical properties [18,20]. Despite experimental studies at
the elementary scale, only a few research efforts include numerical analysis using finite
element (FE) models of the fiber’s real 3D structure [21,22].
In the previous study, we reported an analysis of modern Egyptian flax fiber bundles
using in situ tensile testing, X-ray microtomography, and numerical analysis [23]. The
innovative aspect of the present study lies in analyzing the actual morphology of fibers and
constructing a real 3D model of elementary fibers for tensile simulations. Additionally, the
study examines the structural evolution and mechanical response of fibers using ancient
samples. However, this study does not include experimental testing for ancient fiber
bundles. The reason is the degradation of the middle lamella, which prevented us from
obtaining sufficiently long fiber bundles. Instead, a shorter fiber length of 50 µm was
used for numerical analysis. A significant degradation of non-cellulosic cell wall polymers,
ensuring cohesion between cellulose fibrils, was observed [24,25], and this decrease in
parietal components can affect the mechanical behavior of flax fibers. The study aims to
assess how kink-bands affect the strength of both modern and ancient Egyptian flax fibers
at multiple length scales. Understanding the mechanical properties of ancient Egyptian
flax is crucial for evaluating modern flax as a viable alternative to synthetic materials in
composites, particularly in enhancing its durability. Examining the mechanical properties
of ancient and modern flax fibers is important, as it offers insights into how material
properties have evolved over time. Understanding these differences allows us to evaluate
the effects of structural degradation. Additionally, this comparison sheds light on the
durability and performance of ancient fibers in various applications, which can contribute
to the development of sustainable materials in modern contexts. The objectives of this study
include: 1) analyzing the morphology of ancient flax fibers by considering the modern
flax fibers as a reference, with a focus on defect structures and the impact of aging on the
ancient fibers; and 2) performing tensile simulations on the real 3D fiber structures derived
from static tomography images to investigate the consequences of fiber morphology under
tensile loading. The main goal is to investigate how kink-bands impact tensile properties
by examining stress concentrations in these regions.

2. Materials and Methods

2.1. Materials
Modern elementary flax fibers (MF) of the Eden variety were sourced from fabric at
the Institut Français d’Archéologie Orientale (IFAO) in Cairo. Ancient elementary flax
fibers (AF), ancient bundle flax fibers (ABF) which is composed of three elementary fibers,
were obtained from a flax fabric preserved at the Louvre Museum in Paris (inv. E 13593G).
Radiocarbon dating (Laboratoire de Mesure du Carbone 14, SacA70167, CEA-Saclay, Gif-
sur-Yvette, France) dates this fabric to between 4324 and 4053 BCE, corresponding to the
First Intermediate Period and the early Middle Kingdom.
Fibers 2024, 12, 111 3 of 22

2.2. X-Ray Microtomography

Inline phase-contrast microtomography scans of the samples were performed in the
second ANATOMIX hutch at a 200 m distance from the X-ray source. Two different setups
were used for a robust solution. In the first setup, the elementary fiber and bundle were
attached to the ends of support needles, which were subsequently fixed to the sample
holder. A camera CMOS ORCA Flash 4.0 V2 (Hamamatsu, Hamamatsu city, Japan) was
used in full-frame unbinned mode (2048 × 2048 pixels, physical pixel size 6.5 µm) coupled
with a 20 × M Plan APO (Mitutoyo, Kawasaki, Japan) objective to reach a pixel size of
0.325 µm. The sample-detector distance was set at 7 mm. X-ray radiographs were taken
over a range of 180◦ (standard geometry) with 2000 projection angles per tomography
scans at 300 ms exposure. A Paganin filter [26] with a length of 15 pixels (Paganin unsharp
filter length: 2 pixels; Paganing unsharp filter coefficient 0.5) and flat field correction for
ring artefacts were used. In the second setup, samples were glued to cardboard with a
10 mm gauge length and mounted on a tensile test system. Unlike the dynamic images
used in previous study [23], this study used only static images for analysis and model
development. A 40 keV white beam was employed, and a 10 × M Plan APO objective
was used, achieving a 0.65 µm pixel size. Filters included brazed CVD diamond with Au
coatings (10 µm) and a 100 µm Cu filter. The scan geometry was 180◦ with 2000 projections
per scan, and reconstruction was performed using PyHST2 software Version 2021c with
Paganin correction.
The reconstructed 3D volumes were analyzed using FIJI software (Version 1.54) [27].
Three-dimensional segmentation of the fibers and bundle volumes was performed to
separate voids from the solid phase. This involved converting images from 32-bit to 8-bit,
filtering, rotating, applying thresholds, selecting Regions of Interest (ROI), and image
segmentation. Finally, a flooding procedure was used to distinguish fibers and porosity
from the background [23]. The volumetric analysis of these fibers was performed to
understand the morphology of the fibers. The shape factor was calculated from the ratio
between the major and minor axes of the particle’s fitted ellipse, and was determined
using transversal cross-sections of the fibers. The porosity content was determined for each
transverse cross-section of the fiber using Equation (1). The mean porosity content was
determined as the average of the cross-sectional porosity values along the fiber.

Porosity % = 100 × (ΣV P /ΣV f (1)

where VP represents the voxel counts of porosities and Vf represents the voxel counts of
solid phase within the fiber.
The quantification of kink-bands was carried out by assessing the kink-band density,
defined as the number of kink-bands per unit length of the fiber (mm) [28], and the
average distance between kink-band was determined from tomographic images. Due to the
degradation of the middle lamella, this measurement was not conducted for ancient bundle
fibers, as only shorter lengths were obtained. Additionally, the porosity in the kink-band
region was determined for both elementary and bundle fibers.

2.3. Tensile Testing

The tensile properties of elementary flax fibers to be incorporated into numerical
models were determined through a tensile experiment utilizing the Dia-Stron LEX820
Extensometer (Dia-Stron Limited, Andover, UK) with a 20N load cell and a displacement
rate of 1 mm/min. Tests were conducted in a controlled environment at 25 ◦ C with 55%
relative humidity. The fibers were extracted manually, placed in plastic tabs, and bonded
with adhesive, which underwent exposure to ultraviolet light for 15 s to facilitate adhesive
curing, maintaining a sample length of 4 mm. The dedicated software UvWin V4.2.6.3
served as an interface to both control and analyze the measurements obtained by the
LEX820. The diameter of the fibers was determined using Fiber Dimensional Analysis
system (FDAS) (Dia-Stron Ltd., Andover, UK). Prior to tensile testing, the fibers were
Fibers 2024, 12, x FOR PEER REVIEW 4 of 25

curing, maintaining a sample length of 4 mm. The dedicated software UvWin V4.2.6.3
Fibers 2024, 12, 111 served as an interface to both control and analyze the measurements obtained by 4 ofthe
22
LEX820. The diameter of the fibers was determined using Fiber Dimensional Analysis sys-
tem (FDAS) (Dia-Stron Ltd., Andover, UK). Prior to tensile testing, the fibers were ob-
served
observed under
underan an
optical microscope
optical microscope to determine
to determine the scale
the of the of
scale fiber
the(elementary or bun-
fiber (elementary
dles),
or which which
bundles), furtherfurther
highlighted the kink-bands
highlighted present in
the kink-bands elementary
present fibers, as fibers,
in elementary shownas in
Figure in
shown 1. Ten samples
Figure 1. Tenfrom MF were
samples fromutilized.
MF were The extraction
utilized. Theofextraction
ancient fibers provedfibers
of ancient chal-
lengingchallenging
proved due to theirdue degradation and brittleness.
to their degradation A total of 70
and brittleness. samples
A total of 70were prepared.
samples were
prepared.
However,However,
due to thedue to thenature
fragile fragileofnature
these of theseseveral
fibers, fibers, several
samplessamples broke before
broke before tensile
tensile
testingtesting while observed
while being being observedunderunder the microscope.
the microscope. Additionally,
Additionally, some some
fibersfibers
were were
dam-
damaged
aged duringduring diameter
diameter measurements,
measurements, and some
and some failedfailed
duringduring the installation
the installation of theofsam-
the
sample in tensile
ple in tensile equipment.
equipment. AsAs a result,
a result, only5 5samples
only samplesout outofof7070 samples
samples of ancient
ancient fibers
fibers
were
wereused
usedfor
fortensile
tensiletesting,
testing,providing
providingaasuccess
successrate rateof of7%.
7%.TheTheaverage
averageand andstandard
standard
deviation
deviationof ofthe
thetensile
tensiletest
testresults
resultswere
were calculated,
calculated, along
along with
with the
the coefficient
coefficient of of variation,
variation,
which
whichrepresents
representsthetheratio
ratioofofthe
thestandard
standarddeviation
deviationto tothe
themean.
mean.AfterAftertensile
tensiletesting,
testing,thethe
fracture
fracture surface was examined by SEM, which was performed using a Quattro SS ESEM
surface was examined by SEM, which was performed using a Quattro ESEM
(Thermo
(ThermoScientific)
Scientific)microscope
microscopeat atINRAE,
INRAE,Nantes,
Nantes,France.
France. Images
Images were
were recorded
recordedusing
usingaa
low-vacuum
low-vacuum detector
detector toto prevent
prevent sample
sample deformation
deformation due due toto the
theuse
useofofhigh
highvacuum
vacuumand and
without
withoutmetallization.
metallization.An Anacceleration
accelerationvoltage
voltageof of1010kVkVwaswasused,
used,thethe pressure
pressurewas wasaround
around
100
100PaPaat
atan
anenvironmental
environmentaltemperature,
temperature,and andthe theworking
workingdistance
distanceranged
rangedfromfrom88mm mmto to
10 mm. Images were obtained in low-vacuum
10 mm. Images were obtained in low-vacuum conditions. conditions.

Figure 1.1. Modern

Figure Modern and
and ancient
ancient Egyptian
Egyptian flax
flax fibers
fibersobserved
observed under
underoptical
opticalmicroscope
microscope(polarized
(polarized
light top and bright field bottom), with some kink-bands present in
light top and bright field bottom), with some kink-bands present in fiber.fiber.

2.4.
2.4. Finite
Finite Element
Element Computation
Computation
The
The static
static images
images captured
captured fromfrom the
the X-ray
X-ray microtomography
microtomography were were transformed
transformed into into
numerical models through a combination of surface tessellation using
numerical models through a combination of surface tessellation using triangular elements triangular elements
and
andpropagating
propagatingtetrahedral
tetrahedralelements
elementsininthe
thecore.
core.FIJI
FIJIVersion
Version1.54
1.54(https://fiji.sc/
(https://fiji.sc/ (accessed
(accessed
on 1 December 2024)) and Simpleware ScanIP Version 2021.03 (https://www.synopsys.com/
on 1 December 2024)) and Simpleware ScanIP Version 2021.03 (https://www.synop-
simpleware.html (accessed on(accessed
sys.com/simpleware.html 1 Decemberon 12024)) software
December weresoftware
2024)) used to convert
were used3D images into
to convert
3D 5 × 10 5 to 2 × 106 ,
3Dmodels.
images intoThe meshed fibers
3D models. Theexhibited
mesheddegrees of freedom
fibers exhibited rangingoffrom
degrees freedom ranging from
with
5 × 10a 5mean
to 2 ×volume
106, withelement
a meanof 128 × 10−element
volume
3 µm3 and 231 × 10− 3 µm33 . The meshed−3volume
of 128 × 10−3 µm and 231 × 10 µm3. The of
elementary fibers featured a height of approximately 120 µm. For the
meshed volume of elementary fibers featured a height of approximately 120 µm. For the bundles, the degrees of
freedom
bundles,were 6 × 105,of
the degrees with a height
freedom wereof 50 105, The
6 ×µm. withtotal number
a height of 50of µm.
elements for elementary
The total number of
and bundle fibers ranged from 1 × 105 to 4 × 105 . All computations were carried out using the
elements for elementary and bundle fibers ranged from 1 × 105 to 4 × 105. All computations
structural
were carried mechanics
out usingmodule
the in COMSOL
structural software (Version
mechanics module5.6).
in COMSOL software (Version
5.6). Five models were created: one from modern fiber with kink-bands (MF), one from
ancient fiber with kink-bands (AF), a model with porosity
Five models were created: one from modern fiber with kink-bands artificially filled in modern
(MF), one fiber
from
(MFF), an elliptical model derived from real ancient fiber geometry (GF),
ancient fiber with kink-bands (AF), a model with porosity artificially filled in modern fiber and finally, the
ancient bundle fiber (ABF), composed of three elementary fibers glued together by a middle
lamella with a kink-band. The elliptical model was chosen because the cross section of the
elementary fiber closely resembled an elliptical shape [29]. The material was assumed to
be linear, elastic, and isotropic, with an experimentally obtained Young’s modulus and
Fibers 2024, 12, 111 5 of 22

a Poisson’s ratio of 0.2 [22], and the change in microfibril angle was not considered. In
order to replicate the tensile conditions, the following boundary conditions were used: the
lower surface of the fiber was clamped (i.e., displacement was equal to 0 in all directions at
all nodes of the surface), and a displacement ‘d’ was applied in the z-direction to the top
surface using the following equations:

Ux = Uy = Uz = 0 For the lower sur f ace (2)

Ux = Uy = Uz = 0 For the upper sur f ace (3)

The applied displacement (d) was 1.2 µm and 0.5 µm for the elementary and bundle
fiber, which corresponded to 1% strain over the entire simulated length L. The average
stress (σ) and strain values (ε%) were determined using the Equations (4) and (5), where
Fz is the total nodal reaction force in the z-direction, S is the surface of the filled fiber, d is
the imposed displacement, and L is the length of the fiber. Given that the reaction forces at
the nodes of both fiber edges had distinct transverse surface areas, the resultant stress was
computed from the mean between these integrals (Equation (4)).

1 x Fz( x=0) x Fz( x=d)

σ= + (4)
2 S ( x =0) S( x = d )

d
ε% = 100 ∗ ( ) (5)
L

3. Results and Discussion

3.1. Morphological Analysis
Figure 2 shows volumetric and cross-section images of MF and AF, highlighting the kink-
band region, while Figure 3 shows similar images for ABF. Figure 2a,d provide a volumetric
view in the XZ plane, revealing the central cavity lumen and the kink-band region (emphasized
in the white box). The pores in the kink-band region (Figure 2b,c) are oriented at approximately
45◦ to the lumen axis [18,23]. Similarly, Figure 2e,f shows the lumen and pores in the kink-band
region of AF, where discontinuities in the lumen and structural differences in the kink-band
compared to MF are evident. AF showed a higher porosity in the kink-band region, reaching
5.6%, compared to MF, which had a porosity of 3.3% (Table 1). Additionally, the kink-band
density was higher in AF (20.8 mm−1) compared to MF (16.6 mm−1), indicating a greater
number of kink-bands in AF. Similarly, many defects were observed in same variety of ancient
yarns compared to modern ones [24]. The average distance between kink-bands along the fiber
length was greater in MF (114 µm) than in AF (77 µm). This structural difference could be due
to the varying processing methods used during fiber extraction, as well as potential alterations
in the structure of ancient fibers over time [30]. The pore orientation in the kink-band region for
AF was also about 45◦ to the fiber/lumen axis. It can be observed that the pores were scattered
and arranged concentrically around the lumen [18,23]. Figure 3a shows tomographic images
of ABF in the YZ plane, emphasizing the kink-bands in the white box. As with AF, lumen
discontinuities in elementary fibers of ABF are visible. The structure of kink-bands in the bundle
was almost similar to modern fiber bundles [23]. Although the pores in the kink-band region
of bundle fibers are not clearly visible, a small area in the fiber cross-section (Figure 3b) shows
that the pore orientation was similar to that in MF and AF relative to the fiber/lumen axis. The
porosity measured in the kink-band region for ABF was 2.6%.
Fibers 2024, 12, 111 6 of 22
Fibers 2024, 12, x FOR PEER REVIEW 6 of 25
Fibers 2024, 12, x FOR PEER REVIEW 6 of 25

Figure 2. X-ray microtomography images of fibers: (a) 3D volumetric view of MF in XZ plane; (b)
Figure
magnified
Figure
X-ray
2.view
2. X-ray
microtomography
of kink-band
microtomographyregion; images
(c) longitudinal
images
of fibers:
of fibers: (a)cross
(a) 3D
section volumetric
at kink-band
3D volumetric view of MF
view
region;
in XZ(d)
of
3DMF
plane; vol-
(b)
in XZ plane; (b) magnified
view
umetricofview
magnified kink-band
of of
view region;
AFkink-band
in XZ plane;(c)
(e)longitudinal
region; magnified viewcross
(c) longitudinal ofcrosssection
kink-band atkink-band
kink-band
sectionregion;
at region;
(f) longitudinal
region; (d)vol-
cross
(d) 3D 3D volumetric view of AF in
sec-
tion at kink-band
umetric view of AF region.
in XZ plane; (e) magnified view of kink-band region; (f) longitudinal cross sec-
XZ plane; (e) magnified view of kink-band region; (f) longitudinal cross section at kink-band region.
tion at kink-band region.

Figure 3. X-ray microtomography images of ABF: (a) 3D volumetric view in YZ plane; (b) longitu-
dinal cross
Figure section
3. X-ray in YZ plane. images of ABF: (a) 3D volumetric view in YZ plane; (b) longitu-
microtomography
Figure X-rayinmicrotomography
3. section
dinal cross YZ plane. images of ABF: (a) 3D volumetric view in YZ plane; (b) longitudinal
cross section in YZ plane.

Table 1. Structural properties of elementary and bundle flax fibers.

Average Average Distance

Fiber Length Shape Volume Porosity Porosity (%) Kink-Band
Diameter Between Kink-
Type (µm) Factor (µm3 ) (%) at Kink-Band Density (mm−1 )
(µm) Bands (µm)
1.89 ×
MF 120 18.5 1.01 1.4 3.3 16.6 114
105
2.09 ×
AF 120 15.8 1.07 1.6 5.6 20.8 77
104
1.27 ×
ABF 50 20.5 1.11 1.7 2.6 - -
104
 Average Average Distance
Fiber Length Shape Volume Porosity Porosity (%) Kink-Band
Diameter Between Kink-
Type (µm) Factor (µm3) (%) at Kink-Band Density (mm−1)
(µm) Bands (µm)
MF 120 18.5 1.01 1.89 × 105 1.4 3.3 16.6 114
FibersAF 120
2024, 12, 111 15.8 1.07 2.09 × 104 1.6 5.6 20.8 77 7 of 22
ABF 50 20.5 1.11 1.27 × 104 1.7 2.6 - -

Table 11 presents
Table presents datadata extracted
extracted from
from tomography
tomography images.images. The The lengths
lengths of of the
the elemen-
elemen-
tary fibers, MF and AF, were 120 µm, while the bundle fiber
tary fibers, MF and AF, were 120 µm, while the bundle fiber ABF was 50 µm. The shorter ABF was 50 µm. The shorter
length of
length of ABF
ABF was was duedue toto the
the degradation
degradation of of the
themiddle
middlelamella
lamellain inancient
ancientbundles.
bundles. The The
shape factor
shape factor forfor both
both elementary
elementary and and bundle
bundle fibers
fibers was
was approximately
approximately 1. 1. The
The volume
volume of of
elementary fibers was
elementary was higher
higherthanthanthat
thatofofbundle
bundle fibers. Among
fibers. Among thethe
elementary
elementary fibers, MF
fibers,
hadhad
MF a larger volume
a larger volumethanthan
AF, with a volume
AF, with ratio of
a volume ratio9:1,ofwhich may suggest
9:1, which may suggestfiber degra-
fiber
dation in AF. Table 1 also shows the porosity percentage, which
degradation in AF. Table 1 also shows the porosity percentage, which includes both the includes both the lumen
and pores
lumen andinporesthe kink-band region. This
in the kink-band percentage
region. was higher
This percentage was in higher
ancientin fibers compared
ancient fibers
to modernto
compared fibers.
modern Figure 4 shows
fibers. Figurethe4 porosity
shows the percentage along the 2D
porosity percentage stacks
along theof2Dthestacks
fiber,
of the
i.e., fiber,the
along i.e.,length
along of thethe
length
fiber,offor
theMF,
fiber,
AF,for MF,
and AF, Variations
ABF. and ABF. Variations
in porosity inalong
porositythe
along
fibers the
were fibers
evidentwere forevident
all threefor all three
types. types. The
The largest peaks largest
in thepeaks
graphin the graph
indicate indicate
regions with
regions
lumen and with lumen
pores andkink-band,
in the pores in the kink-band,
confirmed confirmedcross-sections
by transverse by transversethat cross-sections
correspond
that
to the peak region, as shown in Figure 4. In bundle fibers, the presence of lumen, pores of
correspond to the peak region, as shown in Figure 4. In bundle fibers, the presence in
lumen, pores in and
the kink-band, the kink-band,
degradation and
of degradation of the middle
the middle lamella lamella were
were observable andobservable
confirmedand by
confirmed
transverseby transverse cross-sections.
cross-sections. The graphs show The graphs
that ABF show hasthat ABFporosity
higher has higher forporosity for
every slice,
every slice, that
indicating indicating
porosity that porosity
is not only is
duenottoonly due to or
the lumen thepores
lumen in or
thepores in the kink-band,
kink-band, but also to
but
the also
pores toinduced
the poresbyinduced by the degradation
the degradation of the middle of the middle
lamella lamella
along along the fiber.
the fiber.

Figure 4.
Figure 4. Porosity
Porosity along
along the
the length
length of
of the
the fiber
fiber (emphasizing
(emphasizing the
the transverse
transverse cross
cross section
section at
at high
high
peaks),obtained
peaks), obtainedfrom
frommicrotomography
microtomographydata.data.

3.2.
3.2. Tensile
Tensile Results
Results
Stress–strain
Stress–strain curves for formodern
modernandandancient
ancient elementary
elementary flaxflax fibers
fibers are are
shownshown in
in Fig-
Figure 5. Generally, the tensile behavior of fibers can be categorized into three
ure 5. Generally, the tensile behavior of fibers can be categorized into three types: Type types: Type
one
one (TI)
(TI) exhibited
exhibited aa linear
linear and
and purely
purely elastic
elastic tensile
tensile response.
response. Type
Typetwotwo(TII)
(TII) showed
showed two
two
distinct linear section, and type three (TIII) showed a nonlinear section up to a threshold
point, followed by an increase in the tangent modulus until failure. A similar type of
tensile behavior (TIII) was also observed in [31], where the authors hypothesized that
the nonlinear behavior was due to alignment of cellulose micro fibrils with the tensile
axis, and this could be interpreted as an elasto-visco-plastic deformation, which happens
specifically in the secondary cell wall (S2, thickest cell wall). This type of behavior was
also observed for hemp [32]. Type III (TIII) is most commonly seen in ligno-cellulosic fibers
and exhibits higher mechanical properties. However, this trend varies across studies. For
example, Type I was identified as the predominant behavior for hemp [33], while Type
 distinct linear section, and type three (TIII) showed a nonlinear section up to a threshold
point, followed by an increase in the tangent modulus until failure. A similar type of ten-
sile behavior (TIII) was also observed in [31], where the authors hypothesized that the
nonlinear behavior was due to alignment of cellulose micro fibrils with the tensile axis,
Fibers 2024, 12, 111 and this could be interpreted as an elasto-visco-plastic deformation, which happens spe- 8 of 22
cifically in the secondary cell wall (S2, thickest cell wall). This type of behavior was also
observed for hemp [32]. Type III (TIII) is most commonly seen in ligno-cellulosic fibers
and exhibits higher mechanical properties. However, this trend varies across studies. For
III was found
example, to be
Type I was predominant
identified for flax [34].
as the predominant The extraction
behavior for hemp [33],processes
while Type differed
III in these
studies:
was found[33] to beused water-retted
predominant for flaxhemp fibers,
[34]. The whereas
extraction [34]differed
processes utilizedin scutched
these stud- fibers. In the
present study,
ies: [33] used all three hemp
water-retted typesfibers,
of curves were
whereas [34]observed for bothfibers.
utilized scutched modern
In theand
pre-ancient fibers.
sent study,
Type I andallType
threeIItypes
wereofpredominantly
curves were observed for both
observed inmodern
modern and ancient
fibers fibers.
(MF), while Type III
Typepredominantly
was I and Type II were predominantly
observed observed
in ancient fibersin(AF).
modernThe fibers (MF), while
difference Type III between MF
in behavior
was predominantly observed in ancient fibers (AF). The difference in behavior between
and AF may be attributed to the different extraction processes used for these fibers as well
MF and AF may be attributed to the different extraction processes used for these fibers as
as the contribution of structural defects and morphological variations of the fibers, which
well as the contribution of structural defects and morphological variations of the fibers,
is predominant.
which is predominant.

Figure 5. Stress–strain graph: (a) MF, (b) AF.

Figure 5. Stress–strain graph: (a) MF, (b) AF.
Table 2 presents a summary of the tensile properties of both Modern Egyptian and
Table 2 presents a summary of the tensile properties of both Modern Egyptian and
Ancient Egyptian fibers. A significant difference is evident in the Young’s modulus and
Ancient Egyptian fibers. A significant difference is evident in the Young’s modulus and
tensile strength between modern and ancient flax fibers, with modern fibers exhibiting
higher strength and modulus compared to the ancient fibers. The lower properties observed
in ancient fibers may result from potential long-term alterations in mechanical integrity
or fiber polymer degradation [24,25]. Additionally, the variability in stiffness is higher in
ancient fibers compared to modern fibers, possibly attributable to variations in microstruc-
tural parameters such as microfibril angle and porosity [11,17,19], alongside biochemical
changes due to fiber degradation. Nevertheless, the elongation at break (%) appears to be
nearly identical for both modern and ancient fibers. However, a high standard deviation
in elongation at break (%) is observed in ancient fibers, along with a significant standard
deviation in tensile strength with coefficient of variation of ~40% for both modern and
ancient fibers, leading to variations in their properties. The post-treatment analysis of
the fibers was conducted using SEM. Figure 6 displays the SEM images of MF and AF
after tensile testing, revealing crack initiation and fiber failure at the kink-band regions for
both fibers [4]. Additionally, the failed regions of the fibers reveal the presence of lumen
 biochemical changes due to fiber degradation. Nevertheless, the elongation at break (%)
appears to be nearly identical for both modern and ancient fibers. However, a high stand-
ard deviation in elongation at break (%) is observed in ancient fibers, along with a signif-
icant standard deviation in tensile strength with coefficient of variation of ~40% for both
Fibers 2024, 12, 111 modern and ancient fibers, leading to variations in their properties. The post-treatment 9 of 22
analysis of the fibers was conducted using SEM. Figure 6 displays the SEM images of MF
and AF after tensile testing, revealing crack initiation and fiber failure at the kink-band
at those for
regions specific locations,
both fibers which may indicate
[4]. Additionally, theregions
the failed impactof ofthe
cavities
fiberson fiberthe
reveal failure [22].
presence
Kink-bands
of lumen at initiate cracks,locations,
those specific and the deviation
which may in microfibril
indicate theangles
impact at of
these regions
cavities may
on fiber
leads
failureto[22].
shear failures in initiate
Kink-bands the fiber, ultimately
cracks, causing
and the its rupture.
deviation Additionally,
in microfibril angles pores
at thesein
the kink-band region may contribute to fiber failure. Also, the presence
regions may leads to shear failures in the fiber, ultimately causing its rupture. Addition- of significant
kink-bands canthe
ally, pores in lower the tensile
kink-band strength
region may of the fibersto[4,23],
contribute fiber which
failure.can be attributed
Also, to the
the presence of
low properties of ancient fibers.
significant kink-bands can lower the tensile strength of the fibers [4,23], which can be at-
tributed to the low properties of ancient fibers.
Table 2. Tensile properties of elementary flax fibers.
Table 2. Tensile properties of elementary flax fibers.
Young’s Modulus Elongation at Break Tensile Strength
Sample Number of Samples Diameter (µm)
(GPa)Modulus
Young’s (%) (MPa)
Tensile Strength
Sample Number of Samples Diameter (µm) Elongation at Break (%)
MF 10 17.4 ± 4.23 (GPa)
45.4 ± 13.2 2.91 ± 0.55 1321(MPa)
± 533
MF
AF 510 17.4
16.1 ± 4.23
± 3.85 45.4
28.2 ± 13.2
± 19.9 2.91
3.07 ± ±1.89
0.55 1321
643 ± 533
± 267
AF 5 16.1 ± 3.85 28.2 ± 19.9 3.07 ± 1.89 643 ± 267

.
Figure 6. SEM
Figure 6. SEM images
images after
after tensile
tensile testing:
testing: (a,b)
(a,b) MF
MF and
and (c,d)
(c,d) AF.
AF.
3.3. Numerical Results
3.3. Numerical Results
Figures 7a and 8a display the Z-direction displacement for all fibers, confirming bound-
Figures 7athe
ary conditions: and 8a display
bottom surface the Z-direction
is clamped, displacement
and the fordisplaced
top surface is all fibers,
by confirming
1% (1.2 µm
boundary conditions: the bottom surface is clamped, and the top surface
for MF, MFF, AF, GF, and 0.5 µm for ABF). Comparing the Z-direction displacement is displaced
field by
of
fiber models to geometrical model, it is evident that the displacement field in AF is less
homogeneous compared to MF, which may be due to the influence of structural changes in
ancient fibers over time. Figures 7b and 8b show the axial stress (σ33) distributions, with
the elliptical model having uniform stress and other models showing heterogeneity. The
maximum stress exceeds 1000 MPa, with higher concentrations in boundaries of kink-band
regions highlighted in black boxes in Figures 7b and 8b. The pores in the kink-band region
are assumed to be located at the boundaries, especially within the S2/G layer, which
may explain the higher stress in this area [23]. This behavior is further illustrated using
longitudinal cross sections of the fibers. Increased stress concentration in the kink-band
region can initiate cracks, leading to fiber breakage [4,35]. Despite the lumen and pores
being artificially filled in MFF, stress heterogeneity is observed, especially in the kink-band
region with high stress. This suggests that, in addition to the pores, structural alterations
 placement field of fiber models to geometrical model, it is evident that the displacement
field in AF is less homogeneous compared to MF, which may be due to the influence of
structural changes in ancient fibers over time. Figures 7b and 8b show the axial stress (σ33)
distributions, with the elliptical model having uniform stress and other models showing
heterogeneity. The maximum stress exceeds 1000 MPa, with higher concentrations in
boundaries of kink-band regions highlighted in black boxes in Figures 7b and 8b. The
Fibers 2024, 12, 111 10 of 22
pores in the kink-band region are assumed to be located at the boundaries, especially
within the S2/G layer, which may explain the higher stress in this area [23]. This behavior
is further illustrated using longitudinal cross sections of the fibers. Increased stress con-
centration in the kink-band region can initiate cracks, leading to fiber breakage [4,35]. De-
such as deviations in the MFA in this region also influence the stress distribution. Visual-
spite the lumen and pores being artificially filled in MFF, stress heterogeneity is observed,
izations
especially are inkink-band
in the the XZ planeregionfor
withelementary fibers
high stress. This and the
suggests that,YZ plane for
in addition the bundle to better
to the
show kink-band
pores, structural regions.
alterations suchFigures 8a and
as deviations in the9MFA
show transverse
in this region alsodisplacements
influence the (y and x) with
lateral shrinkageVisualizations
stress distribution. due to z-direction
are in theelongation.
XZ plane forAdditionally,
elementary fibers the
andfibers
the YZexhibit asymmetric
plane for thecompared
shrinkage bundle to better
to theshow kink-band
elliptical regions.
model, Figures 8a andthe
highlighting 9 show transverseimpact on uniaxial
geometry’s
displacements (y and x) with lateral shrinkage due to z-direction elongation. Additionally,
extension [22]. Figure 10a presents the average elastic modulus, matching the experimental
the fibers exhibit asymmetric shrinkage compared to the elliptical model, highlighting the
values forimpact
geometry’s MF and AF. It extension
on uniaxial can be observed
[22]. Figurethat ABF exhibited
10a presents the averageaelastic
lower modulus, likely due
mod-
to higher
ulus, porosity
matching within the
the experimental bundle
values for MF(measured
and AF. It canover be aobserved
shorterthatlength of 50 µm compared
ABF ex-
hibited
to 120 aµmlower
formodulus, likely due
elementary to higher
fibers), porosity
which may within
have theresulted
bundle (measured
from the overdegradation of the
a shorter length of 50 µm compared to 120 µm for elementary fibers), which may have
middle lamella and structural changes over time. The calculated mean axial stress (σ33)
resulted from the degradation of the middle lamella and structural changes over time. The
ranged
calculatedfrom
mean280
axialMPa
stressto 450ranged
(σ33) MPa.from 280 MPa to 450 MPa.

Fibers 2024, 12, x FOR PEER REVIEW 11 of 25

Figure 7. (a) Displacement in tensile direction (z) in the plane XZ. (b) Resulting axial stress (σ33)
Figure 7. (a) Displacement in tensile direction (z) in the plane XZ. (b) Resulting axial stress (σ33)
contour plot in the plane XZ.
contour plot in the plane XZ.
 Fibers 2024, 12, 111 11 of 22
Figure 7. (a) Displacement in tensile direction (z) in the plane XZ. (b) Resulting axial stress (σ33)
contour plot in the plane XZ.

Fibers 2024, 12, x FOR PEER REVIEW 12 of 25

Fibers 2024, 12, x FOR PEER REVIEW 12 of 25

Figure 8. (a) Displacement in tensile (z) and transverse (y,x) directions in the plane YZ for ABF. (b)
Figure 8. (a) Displacement in tensile (z) and transverse (y,x) directions in the plane YZ for ABF. (b)
Resulting axial stress (σ33) contour plot in the plane YZ.
Figure 8. (a) axial
Resulting Displacement in tensile
stress (σ33) (z) and plot
contour transverse
in the(y,x) directions
plane YZ. in the plane YZ for ABF. (b)
Resulting axial stress (σ33) contour plot in the plane YZ.

Figure 9. Cont.
Fibers 2024, 12, 111 12 of 22
Fibers 2024, 12, x FOR PEER REVIEW 13 of 25
Fibers 2024, 12, x FOR PEER REVIEW 13 of 25

Figure 9. Displacement in transverse direction in the plane XZ: (a) y direction, (b) x direction.
Figure 9. Displacement in transverse direction in the plane XZ: (a) y direction, (b) x direction.
Figure 9. Displacement in transverse direction in the plane XZ: (a) y direction, (b) x direction.

Figure 10. (a) Predicted elastic modulus (E) as a function of fibers. (b) Maximum axial and shear
stress in10.
Figure longitudinal cross
(a) Predicted section
elastic of the fibers.
modulus (E) as a function of fibers. (b) Maximum axial and shear
Figure 10. (a) Predicted elastic modulus (E) as a function of fibers. (b) Maximum
stress in longitudinal cross section of the fibers.
axial and shear
stress in longitudinal cross section of the fibers.

To understand the stress distribution, we examined the stress evolution in the longitu-
dinal cross-section of the fibers. Figure 10b shows the maximum axial and shear stress for
all models. Figure 11 illustrates the axial stress (σ33) distribution. Modern, ancient, and
porosity-filled fibers exhibit stress variations, while elliptical models display homogeneous
stress distribution, indicating that defects like kink-bands and pores cause stress hetero-
geneities. The highest stress levels occur in pores within kink-band regions of modern and
ancient fibers. For porosity-filled fibers, higher stress levels are observed on the surface,
with reduced stress in filled pores. Figure 11b,c (σ22 and σ11) show symmetric stress distri-
bution in elliptical and filled models compared to modern and ancient fibers, indicating
 Fibers 2024, 12, x FOR PEER REVIEW 14 of 25

To understand the stress distribution, we examined the stress evolution in the longi-
tudinal cross-section of the fibers. Figure 10b shows the maximum axial and shear stress
Fibers 2024, 12, 111 for all models. Figure 11 illustrates the axial stress (σ33) distribution. Modern, ancient, 13 of 22
and porosity-filled fibers exhibit stress variations, while elliptical models display homo-
geneous stress distribution, indicating that defects like kink-bands and pores cause stress
heterogeneities. The highest stress levels occur in pores within kink-band regions of mod-
ern and ancient fibers. For porosity-filled fibers, higher stress levels are observed on the
the stress induced by defects in fiber models. Similarly, Figure 12a shows the axial stress
surface, with reduced stress in filled pores. Figure 11b,c (σ22 and σ11) show symmetric
stress distribution in elliptical and filled models compared to modern and ancient fibers,
distribution for bundles, highlighting higher stress in pores within kink-band regions. This
indicating the stress induced by defects in fiber models. Similarly, Figure 12a shows the
suggests that pores in these areas can initiate cracks under tensile loading.
axial stress distribution for bundles, highlighting higher stress in pores within kink-band
regions. This suggests that pores in these areas can initiate cracks under tensile loading.

Fibers 2024, 12, x FOR PEER REVIEW 15 of 25

Figure 11. Axial stress contour plot in longitudinal cross section of the fibers in the XZ plane. (a)
Figure 11.
σ33, (b) σ22, Axial stress contour plot in longitudinal cross section of the fibers in the XZ plane. (a) σ33,
(c) σ11.

(b) σ22, (c) σ11.

Fibers 2024, 12, 111 14 of 22
Fibers 2024, 12, x FOR PEER REVIEW 16 of 25

Figure 12. Stress contour plot in longitudinal cross section of the fiber bundle in the YZ plane. (a)
Figure 12. Stress contour plot in longitudinal cross section of the fiber bundle in the YZ plane.
Axial plot, (b) shear plot.
(a) Axial plot, (b) shear plot.
The shear stress distribution (σ12, σ13, σ23) for all models is illustrated in Figures
12b andThe13,shear stress distribution
highlighting heterogenous (σ12, σ13,
stress σ23) for allalong
distributions models is illustrated
the fiber, in Figures 12b and 13,
specifically
higher stress levels in defective regions and on surfaces, which
highlighting heterogenous stress distributions along the fiber, specifically were potentially caused
higher stress levels in
by factors like porosity, kink-bands, and surface roughness. Similarly to strain compo-
defective regions and on surfaces, which were potentially caused by factors like porosity, kink-
nents, i.e., displacement in the transverse direction, the values range from negative to pos-
bands, and surface
itive, indicating roughness.
the asymmetric Similarly
shrinkage to strain
effect, which components, i.e., displacement
is due to the influence of the ge- in the transverse
direction,
ometry in the thesurface
valuesonrange from negative
the effectiveness of the to
testpositive,
to produce indicating the asymmetric
uniaxial extension. Com- shrinkage effect,
paring stress
which is due levels within
to the the fibers
influence of(Figure 10b), we noticed
the geometry in the higher
surface axial
onstress (σ33) in
the effectiveness of the test to
the tensile direction across all models compared to other axial and shear stresses. Modern
produce uniaxial extension. Comparing stress levels within the fibers (Figure 10b), we noticed
and ancient fibers exhibited the highest stress levels, reaching up to 2700 MPa and 1600
higher axial stressand
MPa, respectively, (σ33) in the tensile
the bundle direction
fiber reached up toacross all models
600 MPa. compared
Conversely, ellipticalto other axial and shear
and
stresses. Modern
filled fibers showed and ancient fibers
comparatively lower exhibited
stress levels,the highestthe
indicating stress
impactlevels, reaching up to 2700 MPa
of structural
and 1600
defects MPa,
in the respectively,
fibers. However, the and thestress
mean bundlevaluesfiber reached
were up toin600
insignificant σ22MPa. Conversely, elliptical
and σ11
and filled fibers showed comparatively lower stress levels, indicating the impact of structural
defects in the fibers. However, the mean stress values were insignificant in σ22 and σ11 compared
to σ33, and the report will not delve further into them. Similarly, the shear stress related to the
tensile direction (σ13 and σ23) was higher compared to σ12, and it will not be further addressed
in the report.
 Fibers 2024, 12, x FOR PEER REVIEW 17 of 25

Fibers 2024, 12, 111 compared to σ33, and the report will not delve further into them. Similarly, the shear stress 15 of 22
related to the tensile direction (σ13 and σ23) was higher compared to σ12, and it will not
be further addressed in the report.

Fibers 2024, 12, x FOR PEER REVIEW 18 of 25

Figure 13. Shear stress contour plot in longitudinal cross section of the fibers in the XZ plane a)
Figure
σ12 b) σ13 13. Shear stress contour plot in longitudinal cross section of the fibers in the XZ plane (a) σ12
c) σ23.

(b) σ13 (c) σ23.

The primary stress components, σ33, σ13, and σ23, were measured by plotting their
maximum stress on transverse cross-sections spaced 20 µm apart in the XY plane (Figures
14 and The primary
15). The stress
average axial stresscomponents,
of σ33 was lower σ33,
in ancient
σ13, and
fibers σ23, were
(reaching around measured by plotting their maxi-
300 MPa) compared to modern (reaching around 460 MPa) and elliptical fiber models (Fig-
mum
ure 14a).stress
In modernonfibers
transverse cross-sections
(MF and MFF), σ33 was higher spaced 20 µm
than in ancient fibersapart in the XY plane (Figures 14 and 15).
(AF), par-
ticularly
The between axial
average 20 µm stress
to 60 µmof along
σ33thewasfiber’s length,in
lower which reflectsfibers
ancient the kink-band
(reaching around 300 MPa) compared
region (Figure 14b). For ancient fibers, higher stress was seen between 40 µm and 80 µm,
to modern
which (reaching
is also the around
kink-band region. The 460 MPa)
elliptical modeland elliptical
showed constant fiber models (Figure 14a). In modern fibers
stress around
450 MPa, except in the clamping region, where it reached 650 MPa. In bundle fibers (ABF),
higher axial stress (σ33) was found between 30 µm and 40 µm along the fiber’s length,
reaching around 720 MPa (Figure 15).
 Figure 13. Shear stress contour plot in longitudinal cross section of the fibers in the XZ plane a)
Fibers 2024, 12, 111 σ12 b) σ13 c) σ23. 16 of 22

The primary stress components, σ33, σ13, and σ23, were measured by plotting their
maximum stress on transverse cross-sections spaced 20 µm apart in the XY plane (Figures
14 and and
(MF 15). The average
MFF), σ33 axial
wasstress of σ33than
higher was lower in ancient
in ancient fibers (AF),
fibers (reaching around
particularly between 20 µm to 60 µm
300 MPa) compared to modern (reaching around 460 MPa) and elliptical fiber models (Fig-
along
ure 14a).the fiber’sfibers
In modern length, which
(MF and MFF),reflects
σ33 was the kink-band
higher region
than in ancient fibers(Figure
(AF), par-14b). For ancient fibers, higher
stress was
ticularly betweenseen between
20 µm to 60 µm 40 µm
along theand
fiber’s80length, which
µm, which is also
reflects the kink-band region. The elliptical
the kink-band
region (Figure 14b). For ancient fibers, higher stress was seen between 40 µm and 80 µm,
model showed constant stress around 450 MPa, except in
which is also the kink-band region. The elliptical model showed constant stress around
the clamping region, where it reached
650MPa,
450 MPa. Ininbundle
except fibers
the clamping (ABF),
region, wherehigher axial
it reached stress
650 MPa. (σ33)fibers
In bundle was(ABF),
found between 30 µm and 40 µm
higher
alongaxial
thestress (σ33)
fiber’s was found
length, betweenaround
reaching 30 µm and 40 µm
720 MPa along the fiber’s
(Figure 15).length,
reaching around 720 MPa (Figure 15).

Fibers 2024, 12, x FOR PEER REVIEW 19 of 25

(e)

Figure 14. (a,b) Axial stress along transverse cross section of fibers with varying lengths (dash line
Figure
represents14. (a,b) Axial
the average ultimatestress along
stress) and transverse
(c,d) shear cross
stress along section
transverse of fibers
cross section with varying lengths (dash line
of fibers
with varying lengths.
represents the average ultimate stress) and (c,d) shear stress along transverse cross section of fibers
with varying lengths.
Fibers 2024,12,
Fibers2024, 12,111
x FOR PEER REVIEW 20
17 of 25
of 22

Fibers 2024, 12, x FOR PEER REVIEW 20 of 25

Figure15.
Figure 15.Maximum
Maximumaxial
axial and
and shear
shear stress
stress alongalong transverse
transverse cross of
cross section section
fibers of fibers
with withlengths.
varying varying
lengths.
Longitudinal cross-sections ranging from 20 µm to 60 µm along the fiber’s length were
Figure 15. Longitudinal
analyzed by creating
Maximum cross-sections
axial and twostress
shear lines:
alongranging
one from
encompassing
transverse 20 the
µm
cross section to 60
pores
of fibers µm
in
with thealong the fiber’s
kink-band
varying length
region and
lengths.
were analyzed by creating two lines: one encompassing the pores in the kink-band region
the other covering the non-porous region within the kink-band (Figure 16a). For modern
and
fibers, the
Longitudinal other
the maximum covering
cross-sections the
axial non-porous
stress
ranging region
to 60 within
σ3320corresponding
from µm µm along tothe thekink-band
these lineslength
fiber’s (Figure 16a).
is depicted For mod-
in Figure 16b.
were ern fibers,
Similarly,
analyzed by the maximum
forcreating
modern two filled axial
lines: one stress
fibers, σ33 corresponding
longitudinal
encompassing the porescross-sections to
in the kink-bandthese lines
from
region is depicted in
20 µm to 60 µm alongFigure
16b.
andthe Similarly,
the other
fiber’s covering
length for modern
thewere
non-porous filled
examined, region fibers,
within
lines the longitudinal
were kink-band
drawn, cross-sections
(Figure
and 16a). For mod-from
the maximum 20 µm
axial to 60
stress σ33µmis
ern fibers,
alongthe maximum
the fiber’s axial stress
length σ33 corresponding to these linesdrawn,
is depicted in Figure
illustrated in Figure 17. were
Likewise,examined, lines
for ancient were
fibers, sections andfromthe40maximum
µm to 80axial stress
µm along
16b. Similarly, for modern filled fibers, longitudinal cross-sections from 20 µm to 60 µm
alongσ33
the the isfiber’s
fiber’sillustrated
length
length were in Figure
were studied,
examined, 17.lines
Likewise,
two lines
were drawn,for
were ancient
andgenerated, fibers,and
the maximum sections
their
axial from 40 µm
maximum
stress to 80
axial µm
stress
along
σ33σ33 is shown
the fiber’s
is illustrated in Figure
in Figurelength 18.
were
17. Likewise,Notably,
studied, the
for ancient twohighest
fibers,lines axial
were
sections fromstresses
generated,
40 µm σ33to 80 were
and
µmtheirobserved
maximum in pores
axial
located
alongstress
the fiber’swithin
σ33 length the
is shown werekink-band
in Figure
studied, tworegion
18. [36,37]
Notably,
lines were forhighest
the
generated, both modern
and their axial andaxial
stresses
maximum ancient fibers,
σ33 were reaching
observed in
stress
2400 σ33 is
MPa shownand in Figure
1200 18.
MPa, Notably, the
respectively, highest axial
and stresses
this
pores located within the kink-band region [36,37] for both modern and ancient fibers, σ33
aligns were
with observed
the in
ultimate stress obtained
pores located within the kink-band region [36,37] for both modern and ancient fibers,
experimentally,
reaching
reaching 2400 MPa 2400and suggesting
MPa1200andMPa,1200
thatMPa, the pores
respectively,
in kink-band
respectively,
and this aligns with and the have
this potential
aligns
ultimate withtothe
stress
initiate the cracks
ultimate stress
under
obtained
obtained tensile loading.
experimentally,
experimentally, Thissuggesting
suggesting behavior
that the pores was
that consistent
the pores
in kink-band haveat the bundle
inpotential
kink-band scale potential
have
to initiate as well (Figure 19),
to initiate
the reaching
the cracks
cracks under 610 MPa.
under
tensile In theThis
tensile
loading. case
loading. of filled
behavior wasfibers,
This behavior
consistent elevated
was
at stressscale
consistent
the bundle levels were
at well
as the notedscale
bundle on the asfiber
well
(Figure 19), reaching
surfaces
(Figure 19), 610 MPa. 610
in longitudinal
reaching In cross-sections,
the case of
MPa. Infilled
the fibers,
reaching
case elevated
of 600
filled stress
MPa.
fibers, levels
The were
elevated noted
stress distribution
stress appeared
levels were noted
on the fiber surfaces in longitudinal cross-sections, reaching 600 MPa. The stress distribu-
relatively constant, except on the surfaces or in the middle of the fibers, indicating areas
tionon the fiber
appeared surfaces
relatively in longitudinal
constant, except on the cross-sections,
surfaces or in the reachingmiddle of the 600fibers,
MPa. The stress distribu-
where
tion appeared
indicating pore closure
areas whererelatively led to reduced
pore closureconstant,
led to reduced stress
except levels
stress on reaching
the
levels surfaces
reaching around
aroundor 450 450
in MPa. MPa.
the middle of the fibers,
indicating areas where pore closure led to reduced stress levels reaching around 450 MPa.

Figure 16. Cont.

Fibers 2024, 12, x FOR PEER REVIEW 21 of 25

Fibers 2024, 12, 111 18 of 22

Fibers 2024, 12, x FOR PEER REVIEW 21 of 25

Figure 16.
Figure 16. (a) Axial
(a) Axial stressstress (σ33) distribution
(σ33) distribution in longitudinal
in longitudinal cross section ofcross section
the modern of(line
fiber the1modern fiber (line 1
Figure 16. pores
excludes the
(a) Axial
and
stress
lineline
(σ33)the
2 includes
distribution
pores);
in longitudinal
(b) resulting axial stress
cross along
profile
section of the modern fiber (line 1
two lines
excludes the pores and 2 includes the pores); (b) resulting axial stress profile along two lines (1 and 2),
excludes thethe
(1 and 2), with pores
blackand line 2 includes
line representing averagethetensile
pores); (b) resulting axial stress profile along two lines
strength.
with the black line representing average tensile strength.
(1 and 2), with the black line representing average tensile strength.

Figure 17. (a) Axial stress (σ33) distribution in longitudinal cross section of the modern fiber with
artificially filled porosity; (b) resulting axial stress profile along two lines (1 and 2).

Figure 17.
Figure 17. (a)
(a) Axial stress
stress (σ33)
(σ33) distribution
distribution in longitudinal
longitudinal cross section
section ofof the
the modern
modern fiber
fiber with
with
artificially filled
artificially filled porosity;
porosity; (b)
(b)resulting
resultingaxial
axialstress
stressprofile
profilealong
alongtwo
twolines
lines(1(1and
and2).
2).
Fibers 2024, 12, 111 19 of 22
Fibers 2024, 12, x FOR PEER REVIEW 22 of 25

Fibers 2024, 12, x FOR PEER REVIEW 22 of 25

Figure 18. (a) Axial stress (σ33) distribution in longitudinal cross section of the ancient fiber (line 1
Figure
excludes 18. (a) Axial
the pores stress
and line (σ33) the
2 includes distribution in longitudinal
pores); (b) resulting axial stresscross
profilesection of lines
along two the ancient
(1 fiber (line 1 excludes
the
and pores
2), withand line
the black 2 includes
line the
representing pores);
average (b)
tensileresulting
strength. axial stress profile along two lines (1 and 2), with the
Figure 18. (a) Axial stress (σ33) distribution in longitudinal cross section of the ancient fiber (line 1
blackthe
excludes line representing
pores average
and line 2 includes tensile(b)strength.
the pores); resulting axial stress profile along two lines (1
and 2), with the black line representing average tensile strength.

Fibers 2024, 12, x FOR PEER REVIEW 23 of 25

Figure 19. (a) Axial stress (σ33) distribution in longitudinal cross section of the ancient fiber (line 1
Figure 19. (a) Axial stress (σ33) distribution in longitudinal cross section of the ancient fiber (line 1 includes
includes the pores and line 2 excludes the pores); (b) resulting axial stress profile along two lines (1
the
and pores
2). and line 2 excludes the pores); (b) resulting axial stress profile along two lines (1 and 2).

4. Conclusions
X-ray microtomography revealed distinct internal structures in modern (MF), ancient
(AF), and bundle fibers (ABF). AF had higher porosity at the kink-band region (5.6%) and
a greater kink-band density (20.8 mm⁻¹) compared to MF, which showed 3.3% porosity
and a kink-band density of 16.6 mm⁻¹. The average distance between kink-bands is longer
in MF (114 µm) than in AF (77 µm). In both fiber types, kink-band pores were angled at
approximately 45° to the fiber axis. ABF exhibited similar kink-band structures, but likely
with more degradation. Ancient fibers exhibited higher porosity due to both inherent and
Fibers 2024, 12, 111 20 of 22

4. Conclusions
X-ray microtomography revealed distinct internal structures in modern (MF), ancient
(AF), and bundle fibers (ABF). AF had higher porosity at the kink-band region (5.6%) and
a greater kink-band density (20.8 mm−1 ) compared to MF, which showed 3.3% porosity
and a kink-band density of 16.6 mm−1 . The average distance between kink-bands is longer
in MF (114 µm) than in AF (77 µm). In both fiber types, kink-band pores were angled at
approximately 45◦ to the fiber axis. ABF exhibited similar kink-band structures, but likely
with more degradation. Ancient fibers exhibited higher porosity due to both inherent and
degradation-induced pores.
This study examined the tensile characteristics of both modern and ancient fibers,
revealing higher stiffness and strength in modern fibers compared to ancient ones. This
disparity may elucidate the effects of aging of fibers in terms of structural evolution and
fiber polymer degradation. Modern fibers have higher Young’s modulus and tensile
strength compared to ancient fibers, which may be due to degradation and microstructural
variability. SEM analysis reveals failure in both fiber types at kink-band regions, where
cracks and ruptures are influenced by structural deviations and pores.
By utilizing a finite element model within the elastic range, the impact of the intricate
structure of flax fibers on their tensile resistance was investigated. The calculated apparent
modulus closely matched experimental values for elementary fibers, but was lower for
bundle fibers. The numerical analysis revealed significant stress heterogeneity, especially
in modern, ancient, and porosity-filled fibers, with higher stress levels observed in axial
tensors near the kink-band region both volumetrically and in longitudinal cross-sections.
Notably, the maximum axial stress (σ33) was found in pores within the kink-band region,
with modern fibers (MF) exhibiting the highest stress at 2400 MPa, followed by ancient
fibers at up to 1200 MPa, and bundle fibers at up to 600 MPa—values that align with the
experimental ultimate stress. These high stress concentrations, particularly at pores in the
kink-band region, suggest potential for crack initiation and rupture, whereas elliptical and
filled fibers displayed more uniform stress distributions with lower maximum stresses,
highlighting the impact of structural defects like pores and kink-bands in influencing
stress distribution and fiber integrity under tensile loading. Additionally, apart from kink-
bands and pores, stress induced by surface irregularities, particularly in porosity-filled
fibers (MFF), was also noted. Overall, this study demonstrates both experimentally and
numerically that kink bands can initiate cracks in fibers under tensile loading, affecting
both individual and bundled fibers.

Author Contributions: Conceptualization, V.R., S.G., J.B. and A.B.; methodology, A.M., V.R., A.D., M.S.,
J.P., H.P. and T.W.; software, S.G. and V.R.; validation, S.G., V.R., J.B. and A.B.; formal analysis, S.G., J.B.
and V.R.; investigation, V.R. and S.G; resources, A.B.; data curation, S.G. and V.R; writing—original draft
preparation, V.R.; writing—review and editing, S.G., V.R., J.B., A.D., T.W., A.M., M.S., J.P., H.P. and A.B.;
supervision, S.G., J.B. and A.B.; project administration, A.B.; funding acquisition, A.B. All authors have
read and agreed to the published version of the manuscript.
Funding: This research was funded by the French National Research Agency (ANR) through the
Anubis project ANR-21-CE43-0010. ANATOMIX is an Equipment of Excellence (EQUIPEX) funded
by the Investments for the Future program of the French National Research Agency (ANR), project
NanoimagesX, grant no. ANR-11-EQPX-0031. Access to Anatomix was provided through SOLEIL
beamtime proposal #20221519.
Data Availability Statement: Data supporting the findings of this study are available upon simple
request from the corresponding author.
Conflicts of Interest: The authors declare no conflicts of interest.
Fibers 2024, 12, 111 21 of 22

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