Composites: Part A 107 (2018) 260–270

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Composites: Part A
journal homepage: www.elsevier.com/locate/compositesa

Effect of interface on composites made from DREF spun hybrid yarn with
low twisted core flax yarn
Mahadev Bar a,⇑, Apurba Das a, R. Alagirusamy a
a
Department of Textile Technology, Indian Institute of Technology Delhi, New Delhi, India

a r t i c l e i n f o a b s t r a c t

Article history: In the present work, the influence of interface and hybrid yarn structure on flax-PP based unidirectional
Received 22 May 2017 composite properties have been studied thoroughly. Flax-PP based core-sheath structured DREF spun
Received in revised form 31 December 2017 hybrid yarns are manufactured after varying the core yarn twist and sheath percentage at three different
Accepted 2 January 2018
levels and using MAgPP treated and untreated flax yarn as core. These hybrid yarns are consolidated to
Available online 4 January 2018
manufacture unidirectional composite samples and the resultant composites are tested accordingly. It is
observed that MAgPP treatment of the core flax yarn improves the tensile and flexural properties of the
Keywords:
hybrid yarn reinforced unidirectional composites while impact strength decreases after the treatment. A
A. Biocomposite
A. Hybrid
negative impact on the tensile and flexural properties of the unidirectional composite samples is
A. Yarn observed with increasing core twist and sheath content of the reinforcing hybrid yarn. The impact
B. Interface/interphase strength of the composite samples increases for similar changes in hybrid yarn parameters.
Ó 2018 Published by Elsevier Ltd.

1. Introduction
The ever growing problem related to solid waste disposals, leg-
islative pressures related to environment and people’s growing
interest on sustainability have bolstered the interest in sustainable,
environment friendly materials in consumer industry [1–7]. Use of
vegetal resources and recyclable thermoplastic matrices for com-
posite manufacturing fit well into this picture. Moreover, vegetal
fibre reinforced thermoplastic composites have several advantages
which resulted in exponential market growth of these materials
[8–11].
However, the vegetal fibre reinforced thermoplastics have some
drawbacks such as poor fibre-matrix interaction due to the non-
compatibility between the hydrophilic vegetal fibres and hydropho-
bic thermoplastic resins. The fibre-matrix non-compatibility
restricts the full strength utilization of the vegetal fibre to the resul-
tant composite [12–15]. The fibre-matrix interaction of a vegetal
fibre composite system can be enhanced either through the surface
modification of vegetal fibres or through the modification of the
matrix forming polymers or through their combinations. The vege-
tal fibre surface can be modified either by physical means or by
chemical means or by the combination of both the means. Plasma
treatment, corona discharge, ultra sonication, etc. are the example
of physical means of fibre treatment whereas the treatment with
⇑ Corresponding author.
E-mail address: mahadevbar07@gmail.com (M. Bar).
MAgPP, Silane coupling agents, benzoic acid, isocyanates, etc. are
the example of chemical means of fibre treatment [12–18]. Among
all these methods, vegetal fibre surface modification with MAgPP
is more effective when PP is chosen as matrix [18–20].
Besides interphase, fibre orientation and fibre resin distribution
in the composite structure are two other major parameters which
determine the mechanical properties of the fibre reinforced com-
posites. Fibre reinforced composite materials are anisotropic in
nature and exhibit maximum mechanical properties along the fibre
direction [21]. Goutianos et al. [22] have reported that a woven
fabric reinforced composite shows at least 3 to 4 time better
mechanical properties than a nonwoven mat reinforced composite.
Hence, it is concluded that a composite will exhibit the highest
mechanical properties when the reinforcing materials are com-
pletely aligned along the direction of applied load [22–24]. Unlike
synthetic fibres, vegetal fibres have short fibre length and it is dif-
ficult to control the short fibre alignment in the composite struc-
tures [25–27]. Twisted yarn or twisted yarn based textile
structure can control the fibre orientation in the composite struc-
ture but, twist diminishes the maximum fibre strength utilization
due to obliquity effect. Unlike thermoset resins, conventional ther-
moplastic resins (except liquid thermoplastic resins) have very
high melt viscosity which restricts the thermoplastic resin pene-
tration in the twisted yarn structures as well as to the interlace
point of the twisted yarn based woven fabrics [28,29].
Hybrid yarns are the yarns having both the reinforcing as well
as matrix forming fibre components in its structure. Alagirusamy

https://doi.org/10.1016/j.compositesa.2018.01.003
1359-835X/Ó 2018 Published by Elsevier Ltd.
 M. Bar et al. / Composites: Part A 107 (2018) 260–270
et al. [30] have summarized different methods of manufactured
fibre based hybrid yarn manufacturing and have explained their
effectiveness for thermoplastic composite reinforcement. George
et al. [31] have developed a bio-commingled composite using PP
filament and twisted jute yarn. Bio-commingling improves the
wetting of reinforcing jute fibres which ultimately results in supe-
rior composite property. A similar result is observed in case of
micro-braided hybrid yarn reinforced composites where the
micro-braided yarn is manufactured using twisted jute yarn as
core and PP filament as sheath [32]. Although, micro-braiding
and bio-commingling enhance the vegetal fibre reinforced com-
posite properties by lowering effective resin flow distance but
these methods are not commercially viable. Because, the rate of
production of the micro-braided yarn is very low and the bio-
commingling method is suitable for producing small and simple
structures only. Zhang et al. [33] have designed and fabricated a
composite using flax-PP comingled wrap spun yarn. It is observed
that twist-less wrap spun yarn based composite provides better
mechanical properties compared to flax-PP based twisted yarn
reinforced composite. However, in the process of fabric formation,
wrap spun yarns are not suitable as warp and even as a weft in
high speed weaving due to their poor mechanical behavior.
Besides research institutions, many industries such as Libeco
Lagae (Belgium), Lineo (Belgium) and NPSP (Netherlands) have
shown their interest over vegetal fibre reinforced thermoplastic
composites. Considering the accelerating commercial importance,
the development of a commercially viable, economical, vegetal
fibre based, strong thermoplastic composite is becoming very
essential. In our earlier study, a set of thermally treated, vegetal
fibre based DREF spun hybrid yarn has been developed using flax
yarn of different twist level as core and PP fibre as sheath. Different
properties of the hybrid yarn samples such as tenacity, modulus,
flexural rigidity and weaveability have been analyzed. The test
results conclude that one can manufacture a woven prepreg in a
conventional loom using these hybrid yarns [34].
In the present work, initially the flax yarns of different twist
levels are treated with MAgPP. Afterwards, core-sheath structured
hybrid yarns having different core to sheath ratios are manufac-
tured in a DREF spinning machine using both the treated and
untreated flax yarns as core and PP as sheath. In this way, total
10 sets of hybrid yarn are manufactured. The hybrid yarns are then
consolidated in a compression molding machine to manufacture
unidirectional composites which are tested for tensile, flexural
and Izod impact properties. Finally, the combined effect of MAgPP
treatment of the core flax yarn and the hybrid yarn parameters i.e.,
core twist and sheath ratios on different composite properties have
been analyzed and reported.
2. Materials and methods
2.1. Materials
PP fibre, having a density of 0.91 g/cm3, melting temperature of
165 °C and melt flow index 10 g/10 min, as matrix or sheath com-
ponent and flax yarn of 165 tex (made of flax fibre having stiffness
ranges between 30 GPa and 55 GPa; breaking strength ranges
between 500 MPa and 900 MPa and average strain at break
3.74%) as core or reinforcing component, have been chosen for this
study. PP fibre in sliver form is supplied by M/s Zenith Fibre Ltd.,
Gujarat, India while the flax yarn is procured from M/s Jayashree
Textile Ltd. West Bengal, India. Maleic Anhydride grafted
Polypropylene (MAgPP) having Maleic Anhydride content between
1 and 1.5% and melt flow index of 50 g/10 min is used as a coupling
agent. It is procured from Pluss Polymers Pvt. Ltd., Gurgaon, India.
261
2.2. MAgPP treatment of flax yarns
Literature reveals that the surface modification of the vegetal
fibres with 5 wt% MAgPP improves the vegetal fibre reinforced
composite interface significantly. Above 5 wt% MAgPP treatment,
no significant improvement in fibre-matrix interface is observed
[27,29]. In the present study, MAgPP treatment of the flax yarns
are carried out in a boiling solvent medium which is made of
80% xylene and 20% toluene. The process is conducted in a reaction
kettle which is fitted with a flowing water condenser to avoid the
solvent lost during the treatment. 5 wt% MAgPP is dissolved in the
boiling solvent (T = 130 ± 5°C) with a yarn to solvent ratio of 1:25.
The yarns in hank form are then socked in the boiling solvent for
10–15 min. After socking, the hanks are washed several times with
the xylene heated just above 80 °C to remove the un-bonded
MAgPP from the yarn surface. Finally, the washed samples are
dried in an air oven at 105 °C for overnight.
2.3. Hybrid yarn preparation
Initially, a flax yarn having an average Z-twist of 8.12 TPI has
been taken for this study. It is further fed to the front delivery roller
nip of a laboratory scale ring spinning frame and twisted in the S-
direction to the pre-determined twist level. In this way flax yarns
having Z-twist level equal to 8.12 TPI, 4.42 TPI and 0.73 TPI are
obtained by the untwisting process. These yarns are further treated
with MAgPP as mentioned earlier. According to the experimental
design, the MAgPP treated or untreated flax yarns are fed to the
DREF 3 spinning system, as core yarn to produce core-sheath struc-
tured hybrid yarn. In DREF-3 spinning, PP slivers are fed from the
back side of the machine. After feeding, slivers are opened-up into
individual fibre entity by a pinned beater and then transferred to
the yarn forming zone and wrapped over the core flax yarn. In this
way, hybrid yarns of different core-sheath ratios are manufactured
by varying the PP sliver feed rate with respect to constant core yarn
feed rate of 40 m/min. A schematic diagram demonstrating the
untwisting of flax yarn in a ring frame and hybrid yarn manufac-
turing in DREF spinning machine are shown in Fig. 1.
2.4. Composite preparation
Hybrid yarn reinforced unidirectional composites are manufac-
tured through hot compression molding process which involves
the following steps. Initially, flax core based hybrid yarns are
wound in a parallel configuration over a spring loaded metallic
frame as shown in Fig. 2. The spring mechanism adjusts the yarn
tension variation caused by thermal shrinkage during consolida-
tion. After winding, the hybrid yarn bundle is placed into the grove
of female mold part and subjected to hot compression after closing
the male mold halve. During hot compression, some resin comes
out from the mold through both open ends. Keeping that squeeze
out matrix in view, corresponding volume of PP in film form is
pre-added which ultimately compensates the matrix loss. Hot
compression is carried out for 5 min at 190 °C temperature, 8 bar
consolidation pressure and 8 bar vacuum pressure. After curing,
whole set-up is cooled down to below 100 °C without releasing
the consolidation pressure. During cooling the molten PP matrix
turns into a solid and holds the fibres in definite positions.
2.5. Experimental design
In this study, the effect of interface and hybrid yarn structure
i.e. core yarn twist (twist per inch) and sheath percentage on dif-
ferent composite properties such as tensile, flexural and impact
behaviors have been studied thoroughly. Initially, hybrid yarns
with different sheath ratios i.e. 40%, 50% and 60% respectively are
262 M. Bar et al. / Composites: Part A 107 (2018) 260–270

Fig. 1. Schematic diagram of hybrid yarn manufacturing (a) Untwisting of flax yarn in ring frame (b) DREF-3 spinning. (For interpretation of the references to colour in this
figure legend, the reader is referred to the web version of this article.)

Table 1
The details of hybrid yarns used for composite manufacturing.

Untreated flax core MAgPP treated flax core

Core twist Natural fibre Core twist Natural fibre
(twists/inch) percentage (twists/inch) percentage
0.72 40 0.72 40
50 50
60 60
4.42 60 4.42 60
8.12 60 8.12 60

behavior are tested according to ASTM D790 test method. Tensile

Fig. 2. Schematic diagram of hybrid yarn based UD-Composite fabrication. (For
interpretation of the references to colour in this figure legend, the reader is referred
to the web version of this article.)
manufactured using untreated flax yarn of 0.72 TPI as core. Then,
hybrid yarns having 60% sheath content are manufactured using
untreated flax yarn of 8.12 TPI and 4.45 TPI respectively as core
to study the effect of core yarn twist on composite properties. In
this way, five sets of hybrid yarn are manufactured after varying
sheath content, core flax yarn twist and using untreated flax yarn
as core. Afterward, hybrid yarns with same structural parameters
are manufactured using MAgPP treated flax yarns of different twist
levels as core. Hence, total ten different sets of hybrid yarn are pro-
duced. The hybrid yarns are then consolidated in a compression
molding to manufacture unidirectional composite samples. The
details of the hybrid yarns used for composite manufacturing are
tabulated in Table 1.
2.6. Testing of composite samples
The tensile and flexural behaviors of the hybrid yarn reinforced
unidirectional composite samples are tested in a Zwick-Roell uni-
versal testing machine, Model No. Z052 with 50 KN load cell
attachment. The tensile properties of the composite samples are
tested according to ASTM D638 test method whereas the flexural
behavior of the composite specimens is tested at 10 mm/min test
speed after clamping the specimen over an area of 40 mm  20
mm at both ends leaving 100 mm gauge length. On the other hand,
flexural behaviors of the composite specimens are tested at 2 mm/
min test speed where the specimens have a nominal width of 20
mm and a span length of 56 mm. All composite specimens, tested
for the tensile and flexural properties have a thickness between
3.3 mm and 3.7 mm and are cut in the length of fibre orientation
direction. The notch Izod impact behaviors of the hybrid yarn rein-
forced composite samples are tested in an impact strength tester.
The notch Izod impact tests are carried out according to ASTM
D256-97 test method. All tests are carried out at 27 ± 2 °C temper-
ature and 65 ± 2% RH. Each reported value represents the average
of five samples.
2.7. FTIR analysis
The Fourier Transform Infra-red spectra of untreated and
MAgPP treated flax fibres are recorded on a Perkin–Elmer
Spectrum-BX FTIR system from 400 to 4000 cm 1 region using
KBr pellet technique. Untreated and MAgPP treated flax fibres are
chopped several times until the fibres become powder. Then one
part of flax powder sample is mixed and grounded with 9 parts
of special grade KBr and pressed in an evacuated die under suitable
pressure to get pallets. The pallets are then used for FTIR analysis.
 M. Bar et al. / Composites: Part A 107 (2018) 260–270 263

2.8. Scanning electron microscopy
Thermoplastic resin distributions in the composite structure are
studied using the scanning electron microscopic images of the frac-
tured composite surfaces. This study is carried out in the following
manner. A Small piece of fractured composite surface obtained
from broken tensile tested sample is placed over a metallic sample
holder with the help of a double sided carbon tape and is subjected
to a gold coating. After coating, the samples are examined using a
scanning electron microscope (SEM ZEISS EVO 50) at an accelerat-
ing 5–10 AC voltage.
3. Results and discussions
3.1. Effect of MAgPP treatment on flax yarns
Flax fibres are hydrophilic in nature and it does not adhere
strongly with the hydrophobic thermoplastic matrices. This
resulted in poor fibre-matrix interfacial bonding leading to a com-
posite with poor mechanical properties [12,15]. In this study, flax
yarns are treated with 5 wt% MAgPP to improve the flax-PP inter-
action in the hybrid yarn reinforced composites. The SEM images of
the untreated and MAgPP treated flax fibres are shown in Fig. 3.
The SEM images display that untreated flax fibres have a clean
surface while after MAgPP treatment, a continuous layer of MAgPP
as well as some micro particles of MAgPP are observed over the flax
fibre surface. Fig. 4 illustrates the IR-spectra of MAgPP treated and
untreated flax fibres. The IR-Spectra of the untreated flax fibre dis-
plays strong peaks located at 3376 cm 1, 2896 cm 1 and 1642
cm 1 which are assigned to the hydroxyl stretching vibration,
CAO stretching vibration and C @ O stretching vibration of the
alpha-keto carbonyl groups respectively [28]. These functional
groups are mainly present in the cellulose and lignin (although
the flax cell-walls have very low lignin content) of the flax fibre.
The IR spectra of MAgPP treated flax fibre indicates that the peaks
assign for hydroxyl stretching vibration, CAO stretching vibration

(a) (b)

Flax MAgPP

Fig. 3. SEM images of (a) untreated flax fibre (b) MAgPP treated flax fibre. (For interpretation of the references to colour in this figure legend, the reader is referred to the web
version of this article.)

Fig. 4. IR-spectra of MAgPP treated and untreated flax fibre. (For interpretation of the references to colour in this figure legend, the reader is referred to the web version of this
article.)
264 M. Bar et al. / Composites: Part A 107 (2018) 260–270

and C@O stretching vibration of the alpha-keto carbonyl groups are
shifted to 3430 cm 1, 2952 cm 1 and 1778 cm 1 respectively.
Beside this, some new peaks are also observed between 1200
cm 1 and 1000 cm 1 i.e. at 1278 cm 1, 1164 cm 1, 1110 cm 1
and 1059 cm 1 respectively. The literatures suggest that the above
mentioned peaks arise due to the ether linkage formation [27–29].
Hence, it can be concluded from the changes observed in the SEM
images and in the IR-spectra that the MAgPP reacts with the vari-
ous functional groups of flax the fibre through ether linkage
formation.
3.2. Hybrid yarn reinforced unidirectional composites
In the present study, the effect of composite interface and
hybrid yarn structure on the tensile, flexural and Izod impact prop-
erties of the flax-PP based unidirectional composite specimens
have been explored thoroughly. Total ten sets of unidirectional
composite specimens as mentioned in Table 1 are manufactured
and are tested accordingly. The photographs of the tensile failure
surfaces of the untreated and MAgPP treated flax core based hybrid
yarn reinforced unidirectional composite specimens are shown in
Fig. 5 and in Fig. 6 respectively. The photographs reveal that all
the tensile tested composite specimens fail normally. However,
in case of untreated flax yarn reinforced composite specimens
and twisted, MAgPP treated flax yarn reinforced composite speci-
mens, the failure is rather dominated by shear due to poor interfa-
cial bonding between the fibres and matrices. It can be predicted
that in the above mentioned cases, the matrix failure occur first
and then fibre slippage become more dominant. This resulted in
tensile failure composite ends with lot of pulled out fibres. How-
ever, the fibre pullout length decreases significantly with decreas-
ing flax yarn twist and flax content in the composite structure.

TPI- 0.73; C: S ratio- 40 : 60 TPI- 0.73; C: S ratio- 50 : 50 TPI- 0.73; C: S ratio- 60 : 40

TPI- 4.42; C: S ratio- 60 : 40 TPI- 8.12; C: S ratio- 60 : 40

Fig. 5. Photographs of the tensile failure ends of untreated flax core based hybrid yarn reinforced unidirectional composites. (For interpretation of the references to colour in
this figure legend, the reader is referred to the web version of this article.)

TPI- 0 73; C: S ratio- 40 : TPI- 0 73; C: S ratio- 50 : TPI- 0.73; C: S ratio- 60 :

TPI- 4.42; C: S ratio- 60 : TPI- 8.12; C: S ratio- 60 :

Fig. 6. Photographs of tensile failure ends of MAgPP treated flax core based hybrid yarn reinforced unidirectional composites. (For interpretation of the references to colour in
this figure legend, the reader is referred to the web version of this article.)
 M. Bar et al. / Composites: Part A 107 (2018) 260–270 265

High twist restricts the resin penetration in the reinforcing yarn
structure and the molten resin pressure is less when the composite
is manufactured with low resin content. Hence, the resin distribu-
tion in the composite structure hinders significantly with increas-
ing flax content and flax yarn twist. The photographs of the tensile
failure composite ends also reveal that the flax fibres in the com-
posite structure are remain in the bundle form which resulted in
inhomogeneous fibre-matrix distribution. The inhomogeneity is
evidenced in the form of matrix rich zone (i.e. between two yarn
bundles) and fibre rich zones (i.e. the yarn bundles). The inhomo-
geneity or the bundle to bundle distance decreases with increasing
flax content in the composite structure. On load application, the
matrix rich zones behave as weak spots and fail before the fibre
rich regions.
MAgPP treatment of flax fibres improve the fibre-matrix bond-
ing as a result the length of pulled out fibres decreases significantly
after the MAgPP treatment of flax fibres. However, no fibre pull out
at the tensile failure end is observed, in case of low twisted, MAgPP
treated flax reinforced composites. It seems that in the above men-
tioned cases the fibre and matrix both behave as one unit and fail
together almost in a straight line. While in all other cases the line
of failure is an inclined curvy line.
SEM images of the tensile fracture composite ends are shown in
Figs. 7 and 8 respectively. SEM images reveal that the molten PP in
the composite structures does not penetrate in the high twisted
flax yarns. However, in case of partially untwisted flax yarn rein-
forced composites the resin penetrates upto the yarn surface only
while the yarn core remains dry. Complete wetting of the reinforc-
ing yarns are only observed in case of low twisted flax yarn rein-
forced composites. Like the photographs of tensile failure
composite ends, Lot of pull out fibres are observed in the SEM
images of untreated flax yarn reinforced composites and MAgPP
treated, twisted flax yarn reinforced composites. In contrast, no
fibre pullout is observed in case of MAgPP treated, untwisted flax

Matrix Matrix
Matrix

Fibre Fibre
Fibre

TPI- 0.73; C: S ratio- 60 : 40 TPI- 0.73; C: S ratio- 50 : 50 TPI- 0.73; C: S ratio- 40 : 60

Fibre

Fibre

Matrix

TPI- 4.42; C: S ratio- 40 : 60 TPI- 8.12; C: S ratio- 40 : 60

Fig. 7. SEM images of untreated flax core based hybrid yarn reinforced, tensile fracture composite ends. (For interpretation of the references to colour in this figure legend, the
reader is referred to the web version of this article.)

Matrix Matri
Fibre Matri
Fibre
Fibre

TPI- 0.73; C: S ratio- 60 : 40 TPI- 0.73; C: S ratio- 50 : 50 TPI- 0.73; C: S ratio- 40 : 60

Matri
Fibre

Fibre
TPI- 4.42; C: S ratio- 40 : 60 TPI- 8.12; C: S ratio- 40 : 60
Fig. 8. SEM images of MAgPP treated flax core based hybrid yarn reinforced, tensile fracture composite ends. (For interpretation of the references to colour in this figure
legend, the reader is referred to the web version of this article.)
266 M. Bar et al. / Composites: Part A 107 (2018) 260–270

yarn reinforced composites due to the complete wetting of the
reinforcing flax fibres and improved bonding between the fibres
and matrices.
The effect of core yarn twist and the flax content on the tensile
stress and modulus of the MAgPP treated and untreated flax core
based hybrid reinforced unidirectional composite samples are
graphically presented in the Fig. 9 and in Fig. 10 respectively. Flax
fibres are the prime load bearing components of the flax-PP based
hybrid yarn reinforced unidirectional composites and the fibre-
matrix interface becomes stronger after the MAgPP treatment of
flax fibre [11,18]. Hence, upto 25% improvement in the tensile
strength and upto 33% improvement in tensile modulus of the uni-
directional composites are observed after the MAgPP treatment of
reinforcing flax yarns. Similar results are noted when the flax con-
tent in the composite structure increases from 40% to 60%. Low
yarn twist enhances the fibre orientation in the composite struc-
ture. However, it does not exhibit any significant influence on
the tensile strength and modulus of the untreated flax yarn rein-
forced unidirectional composites due to poor interfacial perfor-
mance. In contrast, around 20% improvement in tensile strength
and 25% improvement in tensile modulus are observed while the
reinforcing untwisted yarns are treated with MAgPP. This is mainly
the result of improved fibre-matrix interaction and improved resin
distribution into the composite structure.
Flexural strength and modulus of the flax-PP based hybrid yarn
reinforced composite samples are tested according to three point
bending test method. During three point bending test, one side of
the composite specimen is subjected to a compressive force while
the other side is subjected to the tensile force. The photographs of
tensile and compression side of the untreated and MAgPP treated
flax core based hybrid yarn reinforced unidirectional composite
specimens are presented in Fig. 11 and in Fig. 12 respectively.
The photographs show that, after 3-point bending test PP matrix
is accumulated on the compression side and no fracture is
observed on the tensile side of the high twisted, untreated flax core
based hybrid yarn reinforced unidirectional composite.
Few kinks on the compression side and some line of fracture on
the tensile side are observed in case of low twisted, untreated flax
reinforced composite and highly twisted, MAgPP treated flax rein-
forced composites. However, no matrix accumulation or kinks on
the compression side are observed while a sharp line of fracture
is observed on the tensile side of the MAgPP treated, low twisted

Fig. 9. Ultimate tensile strength of the hybrid yarn reinforced unidirectional composites. (For interpretation of the references to colour in this figure legend, the reader is
referred to the web version of this article.)

Fig. 10. Tensile Modulus of the hybrid yarn reinforced unidirectional composites. (For interpretation of the references to colour in this figure legend, the reader is referred to
the web version of this article.)
 M. Bar et al. / Composites: Part A 107 (2018) 260–270 267

Matrix
accumulaon
Compression
Side

TPI- 8.12; C: S ratio- 60 : 40 TPI- 0.73; C: S ratio- 60 : 40

Tensile Side

TPI- 8.12; C: S ratio- 60 : 40 TPI- 0.73; C: S ratio- 60 : 40

Fig. 11. The photographs of untreated flax core based hybrid yarn reinforced, 3-point bending tested unidirectional composite specimens. (For interpretation of the
references to colour in this figure legend, the reader is referred to the web version of this article.)

Compression
Side

TPI- 8.12; C: S ratio- 60 : 40 TPI- 0.73; C: S ratio- 60 : 40

Tensile Side Line of Line of

Fracture Fracture

TPI- 8.12; C: S ratio- 60 : 40 TPI- 0.73; C: S ratio- 60 : 40

Fig. 12. The photographs of MAgPP treated flax core based hybrid yarn reinforced, 3-point bending tested unidirectional composite specimens. (For interpretation of the
references to colour in this figure legend, the reader is referred to the web version of this article.)

flax reinforced composite. The flexural stress-deformation curves
of untreated and MAgPP treated composite samples are shown in
Fig. 13 and in Fig. 14 respectively. It is observed that the MAgPP
treated composite samples have reached to a maximum stress
level and then experienced a sharp fall. After that, it continues to
take load for a certain deflection and fail eventually. On the other
hand, the untreated twisted flax yarn reinforced composites reache
Fig. 13. Bending stress-Deflection curves of untreated flax core based hybrid yarn
reinforced composite samples. (For interpretation of the references to colour in this
figure legend, the reader is referred to the web version of this article.)
to a maximum stress level and then fail gradually after experienc-
ing some deflections. However, a sharp fall after reaching the max-
imum stress is observed in case of low twisted, untreated flax yarn
reinforced composite specimens. The interfacial bonding of the
MAgPP treated flax yarn reinforced composite samples is better
than the untreated flax yarn reinforced composites. Hence, the
MAgPP treated flax yarn reinforced composites and low twisted,
untreated flax yarn reinforced composites show a sharp fall in
the flexural stress-deformation curves. On the other hand, due to
poor interface, no such sharp fall in the flexural stress-
deformation curve of the untreated, twisted flax yarn reinforced
composite is observed.
The above mentioned observations also conclude that the fail-
ure of the high twisted, untreated flax core based hybrid yarn rein-
forced unidirectional composites is mainly dominated by the
compressive force. Hence, the matrix accumulation on the com-
pression side is observed in case of high twisted, untreated flax
reinforced composite. In contrast the 3-point bending failure of
the low twisted, MAgPP treated flax reinforced composites are
mainly dominated by the tensile forces which is indicated by the
prominent line of failure on the tensile side of the respective com-
posite samples.
Figs. 15 and 16 represent the flexural strength and modulus of
the hybrid yarn reinforced unidirectional composite samples. It is
observed that around 40% improvement in flexural strength and
around 70% improvement in flexural modulus is experienced when
the flax fibre content into the composite increases from 40% to 60%.
However, at constant flax content, upto 20% improvement in
268 M. Bar et al. / Composites: Part A 107 (2018) 260–270

flexural modulus and 7% improvement in flexural strength is

Fig. 14. Bending stress-Deflection curves of MAgPP treated flax core based hybrid
yarn reinforced composite samples. (For interpretation of the references to colour in
this figure legend, the reader is referred to the web version of this article.)
observed when the reinforcing flax fibres are treated with MAgPP.
Similar changes are also observed, when the flax yarn twist is
decreased from 8.12 TPI to 0.73 TPI. In the present composite sys-
tem, flax fibres are the main load bearing component and the
homogeneity in fibre-matrix distribution in the composite struc-
ture increases with increasing flax content. Moreover, the fibre-
matrix interface become stronger after the MAgPP treatment of
the flax fibres. Hence, the flexural strength and modulus of the
composite samples increase after MAgPP treatment of flax yarn
and with increasing flax fibre content in the composite structures.
Yarn twist distorts the alignment of the reinforcing flax fibres and
it also restricts the PP resin penetration in the reinforcing yarn
structures. Therefore, the flexural strength and modulus of the
composite samples increase with decreasing reinforced flax yarn
twist level.
The impact properties of the unidirectional composite samples
are tested according to Izod impact test method. The photographs
of the Izod impact tested, composite samples are shown in Fig. 17

Fig. 15. Ultimate flexural strength of the hybrid yarn reinforced unidirectional composites. (For interpretation of the references to colour in this figure legend, the reader is
referred to the web version of this article.)

Fig. 16. Flexural modulus of the hybrid yarn reinforced unidirectional composites. (For interpretation of the references to colour in this figure legend, the reader is referred to
the web version of this article.)
 M. Bar et al. / Composites: Part A 107 (2018) 260–270 269

TPI- 8.12; C: S ratio- 60 : 40 TPI- 4.42; C: S ratio- 60 : 40 TPI- 0.73; C: S ratio- 60 : 40

TPI- 0.73; C: S ratio- 50 : 50 TPI- 0.73; C: S ratio- 40 : 60

Fig. 17. Photographs of the Izod impact failure ends of the untreated flax core based hybrid yarn reinforced unidirectional composites. (For interpretation of the references to
colour in this figure legend, the reader is referred to the web version of this article.)

TPI- 8.12; C: S ratio- 60 : 40 TPI- 4.42; C: S ratio- 60 : 40 TPI- 0.73; C: S ratio- 60 : 40

TPI- 0.73; C: S ratio- 50 : 50 TPI- 0.73; C: S ratio- 40 : 60

Fig. 18. Photographs of the Izod impact failure ends of the MAgPP treated flax core based hybrid yarn reinforced unidirectional composites. (For interpretation of the
references to colour in this figure legend, the reader is referred to the web version of this article.)

Fig. 19. Impact strength of the hybrid yarn reinforced unidirectional composites. (For interpretation of the references to colour in this figure legend, the reader is referred to
the web version of this article.)
270 M. Bar et al. / Composites: Part A 107 (2018) 260–270
and in Fig. 18 respectively. Like tensile fracture samples, lot of
pulled out fibres are observed at the impact fracture end of the
untreated flax reinforced composite samples as well as at the
twisted, MAgPP treated flax reinforced composite samples. During
impact testing, the above mentioned composites do not break
completely and some deformation is sighted at the impact fracture
zone. The fracture length decreases with increasing reinforcing
yarn twist and with decreasing flax fibre content. On the other
hand, almost complete fracture with prominent fibre breakage is
observed at impact failure ends of the low twisted, MAgPP treated
flax reinforced composites. Fig. 19 exhibits the effect of core yarn
twist and flax content on the Izod impact strength of the flax-PP
based unidirectional composite samples. It is observed that the
impact strength of the composite samples decrease up to 33% as
the flax fibre content in the composite structure increases from
40% to 60%. A further 30% decrement in the impact strength of
the unidirectional composite samples are observed after the
MAgPP treatment of core flax yarn. A similar change in the impact
properties of unidirectional composite samples are observed when
the core flax yarn twist is reduced from 8.12 TPI to 0.73 TPI.
It is observed that high core yarn twist and untreated core flax
yarn offers a poor fibre matrix interfacial bonding. MAgPP treat-
ment of the reinforcing yarn and low reinforcing yarn twist
improves the fibre-matrix interaction. Although a strong flax-PP
interface is beneficial to the tensile and flexural properties of the
composite samples but, it has a detrimental effect on the impact
strength. Because, the energy absorption during impact testing in
the form of fibre- matrix de-bonding, sample deformation and fibre
pull out is suppressed by the strong interface [35–37]. Hence,
untreated and twisted flax yarn reinforced composites show higher
impact strength than the MAgPP treated, untwisted flax reinforced
composites.
4. Conclusions
In the present work, a set of DREF spun hybrid yarns has been
manufactured after varying the core flax yarn twist and sheath
ratios and using MAgPP treated and untreated flax yarn as core.
The hybrid yarns are then consolidated in a compression molding
machine to manufacture unidirectional composite samples. The
samples are further tested for tensile, flexural and Izod impact per-
formance to study the effect of interface and hybrid yarn structure
on the composite properties. It is observed that low flax yarn twist
and high PP content improve the resin distribution in the compos-
ite structure and the MAgPP treatment of flax yarn improves the
fibre-matrix interaction. Hence, the tensile and flexural properties
of the unidirectional composites enhance after the MAgPP treat-
ment of the flax yarn and with decreasing flax yarn twist and with
increasing flax fibre content. However, a negative effect on the
impact properties of the composite samples is observed for the
similar changes.
References
[1] Pickering KL, Efendy MGA, Le TM. A review of recent developments in natural
fibre composites and their mechanical performance. Compos Part A
2016;83:98–112.
[2] Netravali AN, Chabba S. Composites get greener. Mater Today 2003;6(4):22–9.
[3] Oksman K, Skrifvars M, Selin JF. Natural fibres as reinforcement in polylactic
acid (PLA) composites. Compos Sci Technol 2003;63(9):1317–24.
[4] Bar M, Alagirusamy R, Das A. Flame retardant polymer composite. Fibre Polym
2015;16(4):705–15.
[5] Dittenber DB, GangaRao HVS. Critical review of recent publications on use of
natural composites in infrastructure. Compos Part A 2012;43:1419–29.
[6] Pickering K, Beckermann G, Alam S, Foreman N. Optimizing industrial hemp
fibre for composites. Compos Part A 2007;38:461–8.
[7] Davoodi MM, Sapuan SM, Ahmad D, Ali Aidy, Khalina A, Jonoobi Mehdi.
Mechanical properties of hybrid kenaf/glass reinforced epoxy composite for
passenger car bumper beam. Mater Des 2010;31(10):4927–32.
[8] Faruk O, Bledzki AK, Fink HP, Sain M. Biocomposites reinforced with natural
fibers: 2000–2010. Prog Polym Sci 2012;37:1552–96.
[9] Joshi SV, Drzal LT, Mohanty AK, Arora S. Are natural fiber composites
environmentally superior to glass fiber reinforced composites? Compos Part
A 2004;35:371–6.
[10] Gurunathan T, Mohanty S, Nayak SK. A review of the recent developments in
biocomposites based on natural fibres and their application perspectives.
Compos Part A 2015;77:1–25.
[11] Mohanty AK, Misra M, Drzal LT. Sustainable bio-composites from renewable
resources: opportunities and challenges in the green materials world. J Polym
Environ 2002;10:19–26.
[12] Torres FG, Cubillas ML. Study of the interfacial properties of natural fibre
reinforced polyethylene. Poly Test 2005;24:694–8.
[13] Zafeiropoulos NE, Baillie CA, Hodgkinson JM. Engineering and characterisation
of the interface in flax fibre/polypropylene composite materials. Part II. The
effect of surface treatments on the interface. Compos Part A 2002; 33:1185–
1190.
[14] Lu JZ, Wu Q, McNabb HS. Chemical coupling in wood fiber and polymer
composites: a review of coupling agents and treatments. Wood Fiber Sci
2000;32(1):88–104.
[15] de Farias JGG, Cavalcante RC, Canabarro BR, Viana HM, Scholz S, Simão RA.
Surface lignin removal on coir fibers by plasma treatment for improved
adhesion in thermoplastic starch composites. Carbohydrate Poly
2017;165:429–36.
[16] Xie Yanjun, Hill Callum AS, Xiao Zefang, Militz Holger, Mai Carsten. Silane
coupling agents used for natural fiber/polymer composites: a review. Compos
Part A 2010;41:806–819.
[17] Mohanty AK, Khan Mubarak A, Hinrichsen G. Surface modification of jute and
its influence on performance of biodegradable jute-fabric/biopol composites.
Compos Sci Technol 2000;60(11):15–24.
[18] Bera M, Alagirusamy R, Das A. A study on interfacial properties of jute-PP
composites. J Reinf Plast Compos 2010;29:3155–61.
[19] Ibrahim MM, Dufresne A, El-Zawawy WK, Agblevor FA. Banana fibre and
microfibrils as lignocellulosic reinforcement in polymer composites.
Carbohydrate poly 2010;81:811–9.
[20] Arbelaiz A, Fernandez B, Ramos JA, Mondragon I. Thermal and crystallization
studies of short flax fibre reinforced polypropylene matrix composites: effect
of treatments. Thermochim Acta 2006;440:111–21.
[21] Herrera-Franco PJ, Valadez-Gonzalez A. A study of the mechanical properties
of short natural-fiber reinforced composites. Compos Part B 2005;36
(8):597–608.
[22] Goutianos S, Peijs T, Nystrom B, Skrifvars M. Development of flax fibre based
textile reinforcements for composite applications. Appl Compos Mater
2006;13(4):199–215.
[23] Shah DU. Damage in biocomposites: stiffness evolution of aligned plant fibre
composites during monotonic and cyclic fatigue loading. Compos Part A
2016;83:160–8.
[24] Santamala H, Livingston R, Sixta H, Hummel M, Skrifvars M, Saarela O.
Advantages of regenerated cellulose fibres as compared to flax fibres in the
processability and mechanical performance of thermoset composites. Compos
Part A 2016;84:377–85.
[25] Amor IB, Rekik H, Kaddami H, Raihane M, Arous M, Kallel A. Effect of Palm tree
fiber orientation on electrical properties of palm tree fiber-reinforced
polyester composites. J Compos Mater 2010;44(13):1553–68.
[26] Norman DA, Robertson RE. The effect of fiber orientation on the toughening of
short fiber-reinforced polymers. J Appl Polym Sci 2003;90(10):2740–51.
[27] Kobayashi S, Takada K. Processing of unidirectional hemp fiber reinforced
composites with micro-braiding technique. Compos Part A 2013;46:173–9.
[28] Ma H, Li Y, Luo Y. The effect of fiber twist on the mechanical properties natural
fiber reinforced composites, 18th International Conference on Composite
Materials (2011).
[29] Omrani F, Wang P, Soulat D, Ferreira M. Mechanical properties of flax-fibre-
reinforced preforms and composites: influence of the type of yarns on multi-
scale characterization. Compos Part A 2017;93:72–81.
[30] Alagirusamy R, Fangueiro R, Ogale V, Padaki N. Hybrid yarns and textile
preforming for thermoplastic composites. Text Prog 2006;38(4):1–71.
[31] George G, Jose ET, Jayanarayanan K, Nagarajan ER, Skrifvars M, Joseph K. Novel
bio-commingled composites based on jute/polypropylene yarns: effect of
chemical treatments on the mechanical properties. Compos Part A
2012;43:219–30.
[32] Khondker OA, Ishiaku US, Nakai A, Hamada H. A novel processing technique for
thermoplastic manufacturing of unidirectional composites reinforced with
jute yarns. Compos Part A 2006;37:2274–84.
[33] Zhang L, Miao M. Commingled natural fibre/polypropylene wrap spun yarns
for structured thermoplastic composites. Compos Sci Technol 2010;70:130–5.
[34] Bar M, Das A, Alagirusamy R. Studies on flax-polypropylene based low-twist
hybrid yarns for thermoplastic composite reinforcement. J Reinf Plast Compos
2017;36(11):818–31.
[35] Fung KL,Li RKY, Tjon SC. Interface modification on the properties of sisal fiber-
reinforced polypropylene composite. J. Appl Polym Sci 2002; 85:169–176.
[36] Chow CPL, Xing XS, Li RKY. Moisture absorption studies of sisal fibre reinforced
polypropylene composites. Compos Sci Technol 2007;67:306–13.
[37] Ranganathan N, Oksman K, Nayak SK, Sain M. Regenerated cellulose fibers as
impact modifier in long jute fiber reinforced polypropylene composites: Effect
on mechanical properties, morphology, and fiber breakage. J. Appl Polym Sci
2015;132:41301–413011.