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Cite This: ACS Appl. Mater. Interfaces 2018, 10, 34502−34512 www.acsami.org

High-Performance Graphene-Based Natural Fiber Composites

Forkan Sarker,†,‡,⊥ Nazmul Karim,*,∥,⊥ Shaila Afroj,§,∥ Vivek Koncherry,†,‡ Kostya S. Novoselov,§,∥
and Prasad Potluri*,†,‡
†
School of Materials, ‡Northwest Composites Centre, and §School of Physics & Astronomy, The University of Manchester, Oxford
Road, Manchester M13 9PL, U.K.
∥
National Graphene Institute (NGI), The University of Manchester, Booth Street East, Manchester, M13 9PL, U.K.
*
S Supporting Information
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ABSTRACT: Natural fiber composites are attracting significant

interest due to their potential for replacing synthetic composites
at lower cost with improved environmental sustainability.
However, natural fiber composites suffer from poor mechanical
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and interfacial properties. Here, we report coating of graphene

oxide (GO) and graphene flakes (G) onto natural jute fibers to
improve mechanical and interfacial properties. The coating of
graphene materials onto jute fibers enhanced interfacial shear
strength by ∼236% and tensile strength by ∼96% more than
untreated fibers by forming either bonding (GO) or mechanical
interlocking (G) between fibers and graphene-based flakes. This
could lead to manufacturing of high-performance and environ-
mental friendly natural fiber composites that can potentially
replace synthetic composites in numerous applications, such as the automotive industry, naval vessels, household products, and
even in the aerospace industry.
KEYWORDS: natural fibers, jute fibers, composites, graphene, graphene oxide, interfacial shear strength and tensile properties

■ INTRODUCTION
Natural fibers are becoming increasingly attractive to
The alkali treatment of jute fiber usually removes non-
cellulosic materials, predominantly hemicellulose and some
composite manufacturers and material scientists due to their lignin.7−10 Hemicelluloses are present in the interfibrillary
lower environmental impact, such as less carbon emission and region of jute fiber. The deformation of this fibrillary network11
fossil fuel consumption, biodegradability, lower cost, lower is mainly responsible for the stress development and relaxation
density, and ease of fabrication.1 The utilization of lightweight in stretched jute fiber, whereas the lignin is located in the
natural fibers such as jute, flax, kenaf, hemp, and sisal could intercellular region and the behavioral change in that region
potentially replace a large amount of glass and mineral fillers in plays a dominant role in determining tensile characteristics of
numerous automotive and aerospace applications (Table S1, jute fibers. The alkali treatment removes noncellulosic
Supporting Information).2 Flax, hemp, and jute are dominating materials and impurities from the interfibrillar region of jute
natural fibers in the European automotive industry. Among fibers, which makes the fibrils more capable of rearranging
them, jute fibers have attracted significant interest given that themselves along the direction of tensile deformation. This will
they may be able to replace glass fibers (GFs) partially or fully allow fibrils to have a better load sharing capability between
due to their lower specific gravity (∼1.3) compared to that of themselves to contribute in higher stress development during
glass (∼2.5) and a higher specific modulus (∼40 GN/m2) than the tensile test.12 While lignin is removed gradually, the middle
that of glass (∼30 GN/m2).3 Moreover, jute is the second- lamella becomes more plastic as well as homogenous due to
most produced (mainly in Bangladesh, India, and China) the gradual elimination of microvoids. As suggested in a
natural fiber after cotton and is at least 50% cheaper than flax previous study,8 the treatment with a lower alkali concen-
and other natural fibers.4 However, jute fiber experiences lower tration (∼0.5 wt %) for a prolonged time is an effective
mechanical properties and poor interfacial shear strength technique to enhance the mechanical properties of jute fiber.
(IFSS) while reinforced with epoxy matrix, due to the presence However, the enhancement is limited and not even close to
of large amounts (20−50 wt %) of noncellulosic materials, glass fiber properties. Moreover, the treatment with a higher
such as hemicellulose and lignin (Table S2, Supporting alkali concentration may reduce the hydrophilicity by
Information). These noncellulosic materials are responsible
for the lower crystallinity5 and hydrophilic nature of jute Received: August 1, 2018
fibers6 and play an important role in determining the Accepted: September 17, 2018
characteristic properties of fibers. Published: September 17, 2018

© 2018 American Chemical Society 34502 DOI: 10.1021/acsami.8b13018

ACS Appl. Mater. Interfaces 2018, 10, 34502−34512
ACS Applied Materials & Interfaces Research Article

Figure 1. SEM images of (a) untreated jute fiber (X250); (b) GO-coated jute fiber (X250), and (c) G flake-coated jute fiber (X1500); (d) the
diameter of untreated and treated jute fibers; (e) thermogravimetric analysis (TGA) curves for treated and untreated fibers; (f) wide-scan XPS
spectra of untreated, GO, and G flake-treated jute fibers; (g) high-resolution (C 1s) XPS spectra of untreated jute fiber; (h) high-resolution (C 1s)
XPS spectra of GO-coated jute fiber; and (i) high-resolution (C 1s) XPS spectra of G flake-coated jute fiber.

removing more hydroxyl components,13 thus creating an reduced graphene oxide (rGO)21 in stable forms. Moreover,
adverse effect on the tensile and interfacial properties of jute GO sheets show good chemical reactivity and handling
composites.14,15 Several studies16,17 also reported surface characteristics due to their intrinsic functional groups.22
treatment of alkali-treated jute fiber with organosilane16 and Furthermore, the scalable production of graphene flakes (G)
plasma18 to further improve interfacial shear strength; by microfludization technique and their applications for
however, the improvement is not significant and some of the making smart composites is demonstrated.23 Recent stud-
treatments are expensive and time consuming. Therefore, there ies24−26 have reported improvement of the mechanical and
remains a need for a new kind of surface treatment for jute interfacial properties due to the grafting of GO onto synthetic
fibers that could improve both tensile and interfacial shear fiber surfaces such as carbon, glass, and poly(p-phenylene
strength significantly and potentially outperform glass fiber benzobisoxazole) (PBO). For example, interfacial shear
composites. strength (IFSS) has been increased by 70.8% by uniform
Graphene, a single-atom-thick sheet of hexagonally arrayed coating of GO on a carbon fiber surface.25 GO has also been
sp2-bonded carbon atoms, has attracted tremendous attention coated covalently onto glass fibers (GFs) by amidation
for high-performance composite applications due to its reaction24 between the carboxyl groups of GO and the
incredible mechanical properties.19 The graphite oxide route amino groups of amino-terminated GFs to improve the IFSS of
is the most attractive method for producing huge quantities of glass/epoxy composites. Moreover, a GO coating on a (PBO)
graphene materials such as graphene oxide (GO)20 and fiber surface with a silane coupling agent (KH-540) enhances
34503 DOI: 10.1021/acsami.8b13018
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ACS Applied Materials & Interfaces Research Article

Figure 2. (a) Optical images of the microdroplet on (a) untreated jute fiber (X200); (b) HA 0.5-treated jute fiber (X200); (c) GO-coated jute
fiber (X200); (d) G flake-coated jute fiber (X200); (e) interfacial shear strength (IFSS) of untreated, GO, and G flake-coated jute fibers; (f)
interfacial shear strength data fitted to a two-parameter Weibull distribution as a function of surface treatment; (g) ln curve of Weibull parameter
plot distribution considering interfacial shear strength; (h) SEM image of microdroplets of epoxy on jute fiber before microbond test (X250); (i)
SEM image of microdroplets of epoxy on jute fiber after microbond test (X250), and (j) SEM image of debonded area (red circle line) after
microbond test (X250).

IFSS by 61.6%.27 Furthermore, the surface treatment of Here, we report for the first time coating of graphene
naturally derived fibers with nanofunctional materials is materials such as GO and G flakes onto alkali-treated jute
becoming an attractive choice to the researchers due to their fibers to improve mechanical and interfacial properties. The
biocompatibility and strong interfacial interactions with jute fibers were first treated with a lower concentration (0.5 wt
% NaOH) of alkali to remove noncellulosic materials. The
multiple reactive sites.28−30 Although a very few studies
alkali-treated fibers were then coated uniformly with GO and
reported grafting of nanoparticles such as NanoTiO231 and G flakes. The surface characteristics of graphene-coated jute
ZnO226 on natural fibers, no study has been found so far on fibers were analyzed using scanning electron microscopy
coating graphene or graphene derivatives on commonly used (SEM) and X-ray photoelectron spectroscopy (XPS). The
natural fibers such as jute and flax. change in fiber diameter was observed using an optical
34504 DOI: 10.1021/acsami.8b13018
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ACS Applied Materials & Interfaces Research Article

microscope. A microbond test was conducted to study the spectrum of GO-coated jute fibers is almost similar to that
effect of GO and G flakes on the interfacial properties of jute/ of untreated jute fibers, shown in Figure 1h. For G 10-coated
epoxy composites and also evaluate the mechanical properties jute fibers, C 1s is mainly dominated by C−C/CC (Figure
of graphene material-coated jute fibers. 1i), which is similar to graphene or graphite and in agreement

■ RESULTS AND DISCUSSION

Characterization of Coated Jute Fibers. Figure 1a−c
with previous results.23,40 The G flakes provide less adhesion to
cellulosic jute fibers, due to the absence of oxygen-containing
functional groups. Fourier transform infrared spectroscopy
shows SEM micrographs of untreated and coated jute fibers. (FTIR) analysis of untreated and graphene material-treated
Figure 1a shows SEM images of a smooth and featureless jute fiber provides further evidence of the removal of
untreated jute fiber surface, which may be due to the presence hemicellulose after alkali treatment and also the coating with
of a cementing layer that is composed of waxes, fats, lignin, GO and G flakes (Figure S3a,b, Supporting Information).
pectin, and hemicelluloses.32 After heat and alkali treatment, Interfacial Shear Strength. Interfacial shear strength
the surface roughness of the jute fiber increases,16 due to (IFSS) is one of the key parameters to determine the
partial removal of that cementing layer (Figure S1, Supporting performance of fiber-reinforced polymer composites. The
Information). Generally, a grooved appearance with micro- efficient load transfer from matrix to reinforcement can be
voids is visible after the alkali treatment (Figure S1b, achieved by good interfacial bonding at fiber/matrix interface.
Supporting Information). The coating of GO shows a more This can then reduce the stress concentration and improve the
uniform and evenly coated fiber surface with only a few flakes overall mechanical properties of composites. There are a
present on the surface (Figures 1b and S1c, Supporting number of composite properties that are significantly
Information), which may be due to chemical bonding provided influenced by IFSS, such as compressive strength and strain
by the functional groups of GO.22 For graphene flakes (G 10), to failure, impact properties, damage initiation threshold,
however, a uniform coating is achieved with plenty of unfixed fracture toughness, and fatigue life.41 We use a single-fiber
graphene flakes being present on the fiber surface, shown in microbond pull-out test to measure IFSS at the fiber/matrix
Figures 1c and S1d, Supporting Information. Moreover, the interface. Figure 2a−d shows the optical images of micro-
color of HA 0.5-treated jute fibers changes from brown to droplets used for different treated jute fibers. Figure 2e shows
yellowish for GO and black for G flakes (Figure S2c,d, that IFSS values are relatively lower (∼4.16 MPa) at the
Supporting Information). The diameter of untreated jute fibers untreated jute fiber/epoxy interface. This may be due to the
is found to be 55 ± 12 μm, shown in Figure 1d. After alkali presence of a waxy cementing layer on the fiber surface, which
treatment, we observe that the diameter of the jute fibers (HA contains low molecular weight fats, lignin, pectin, and
0.5) is reduced by 23.5% to 43 ± 8 μm, which is in agreement hemicellulose, as discussed earlier. After heat and alkali
with previous studies.8,33,34 The reduction of fiber diameter treatment, the cementing layer is removed, providing a rough
may be due to the removal of hemicellulose, pectin, and fiber surface and better interlocking of the fiber with epoxy
lignin.14,16,35 However, coating of graphene materials onto HA resin. Therefore, the IFSS value increases to 7.37 MPa after
0.5-treated jute fibers shows an overall increase in the fiber HA 0.5 treatment, shown in Figure 2e. Previous stud-
diameter. As expected, the diameter of GO-coated fibers ies10,16,42−45 also suggested that the alkali treatment improves
increases with the increase of GO concentration, shown in the IFSS of jute and other natural fiber composites by 30−
Figure 1d. 140% (Table S4, Supporting Information).
TGA analysis of untreated and graphene material-coated The single-fiber microbond test shows further significant
samples show that the thermal stability of jute fibers reduces improvement in IFSS after coating of graphene materials onto
after heat and alkali treatment, due to the removal of HA 0.5-treated jute fibers. The coating of GO onto HA 0.5-
hemicellulose and lignin, shown in Figure 1e (and Table S3, treated jute fibers enhances IFSS with the increase of GO
Supporting Information). However, coating of graphene concentration, shown in Figure 2e. The IFSS of GO 1.0-coated
materials onto jute fibers improves their thermal stability by fibers is found to be 14 MPa, which is 245 and 89% more than
at least 11 °C, which is in agreement with a previous study.36 that of untreated fibers and HA 0.5-treated fibers, respectively,
This could be explained by the formation of a carbonaceous although several previous studies25,27 reported that the coating
shield of graphene materials on the fiber surface,37,38 which with GO improved IFSS of synthetic fiber-reinforced
delays the degradation and improves thermal stability of the composites by 40−60%. However, this is the first report of
fiber. We use XPS analysis to characterize surface function- such a study on natural fiber composites to the best of our
alities of untreated and graphene material-coated jute fibers, knowledge and the highest reported improvement in IFSS of
shown in Figure 1f−i. The wide-scan XPS spectra show that any fiber-reinforced composites after coating with GO. (Please
the C/O ratio of jute fibers decreases from 5.49 to 3.78 after see the comparison in Table S4, Supporting Information.)
coating with GO, due to the presence of oxygen-containing As seen from the XPS analysis (Figure 1h), GO-coated fibers
functional groups in GO,20,22 whereas C/O ratio of G 10- contain a significant amount of oxygen-containing functional
coated samples increases to 16.36 after grafting graphene flakes groups such as hydroxyl (−OH), epoxide (C−O−C), carbonyl
onto jute fiber surfaces, due to the absence of oxygen- (CO), and carboxyl (O−CO). These functional groups
containing functional groups in their structures.23 These could interact with the groups of epoxy resin and form a strong
further be explained from the deconvolution analysis of C 1s mechanical interlocking at the fiber/matrix interface by
spectra of untreated and graphene derivative-coated jute suitable bonding. Moreover, we use an amine-based hardener
fibers.21 Figure 1g shows a high-resolution C 1s XPS spectrum to solidify the fiber/epoxy network, which may form C−N
of untreated jute fibers, which confirms the presence of three bonds through ring opening polymerization.25,46,47 Further-
main components: C−C bond (∼284.5 eV) in cellulosic more, GO provides strong adhesion and uniform coating on
structure, C−O−C groups (hydroxyl and epoxy, ∼286.5 eV), the fiber surface due to the better hydrophilicity of HA 0.5-
and CO groups (carbonyl, ∼288.3 eV).39 The C 1s treated jute fibers. SEM images (Figure 2h−j) of typical
34505 DOI: 10.1021/acsami.8b13018
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Figure 3. (a) Young’s modulus and (b) tensile strength of untreated, GO-treated, and G flake-coated jute fibers; (c) comparative analysis of
theoretical and experimental Young’s modulus of untreated and graphene-based jute fibers; (d) Young’s modulus data fitted to a two-parameter
Weibull probability distribution as a function of surface treatment; (e) tensile strength data fitted to a two-parameter Weibull probability
distribution as a function surface treatment; (f) ln curves of Weibull parameter plot distribution considering the tensile strength; (g) SEM image of
the failure area of untreated jute fiber (X250); (h) SEM image of the failure area of GO-coated jute fiber (X250); and (i) SEM image of the failure
area of G flake-coated jute fiber (X250).

microdroplets before and after the microbond test show a ∼164 and ∼65% more than the IFSS of untreated and HA 0.5-
strong interface between the jute fiber and the epoxy matrix, as treated jute/epoxy composites, respectively. This may be due
in Figure 2j (circle line). Moreover, the alkali treatment of jute to the formation of a mechanically interlocked coating of G
fiber removes the cementing layer to produce a rough surface, flakes on the fiber surface, by the diffusion of highly
which is similar to that observed in the previous study.16 GO concentrated G flakes into alkali-treated rough and porous
flakes may act as fillers on that rough surface and cluster jute fiber structure (Figure S1d, Supporting Information).
between the cellulosic chains of fibers, thus forming a strong We use Weibull statistics to analyze the type of failure that
hydrogen bond and enhancing IFSS at the fiber/matrix happens at the fiber/matrix interface. The cumulative
interface. In contrast, the coating with 1 wt % G flakes (G probability of failure is given by the following formula.

ijij τ yz yz
P = 1 − expjjjjjjj s zzz zz
1.0) does not show much improvement in IFSS, may be due to

zz
jjk τo z{
m

z
the absence of oxygen-containing functional groups. However,

k {
the higher concentration (10 wt %) of G flakes (G 10)
improves IFSS of treated jute fibers to 11 ± 5 MPa, which is (1)

34506 DOI: 10.1021/acsami.8b13018

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where τs is the shear strength, τo is the Weibull scale parameter, fibers. After coating GO (1 wt %) onto jute fibers, Young’s
and m is the Weibull shape parameter. On the basis of the eq 1, modulus increases from 30 to 48 GPa and the tensile strength
a double natural logarithm is taken on both sides, which is from 295 to 575 MPa, which are 60 and 94%, respectively,
shown in eq 2 more than those with the untreated jute fiber. The enhanced
mechanical properties of GO-coated jute fiber could again be
ln(− ln(1 − P)) = m ln(τs − m ln τo) (2) due to the strong adhesion between functional groups of GO
The Weibull scale parameter and Weibull shape parameter of and those of HA 0.5-treated jute fibers via suitable bonding.
the untreated and treated fibers to an epoxy resin are calculated Also, GO flakes possess an extremely high modulus that could
by plotting the Weibull probability distribution curves, as possibly stiffen the jute fiber and remove stress concentrations
shown in Figure 2f,g. The higher number of defects will reduce on the fiber surface during tensile loading, thus enhancing the
the Weibull modulus and therefore will result in lower tensile properties of jute fiber. Moreover, the SEM image of a
interfacial shear strength of the jute/epoxy composites. We GO-coated jute fiber shows that pores of cellulose microfibrils
observe that the Weibull modulus of untreated jute fibers is are filled with GO flakes (Figure S1c, Supporting Information),
2.06, which gradually increases to ∼3 with the increase of which increases fiber packing (Figure 3h) and provides better
concentrations after coating of GO onto a jute fiber surface. It tensile properties. We also observe that the tensile properties
indicates that GO flakes are actively working at the interface to of jute fibers improve with the increase in GO concentrations,
reduce any defects present in the fiber. However, this value as in Figure 3a,b.
reduces to 1.87 (Table S5, Supporting Information) for G Similarly, the coating with higher concentration of G flakes
flakes and shows scattered failure at the interface of jute/epoxy (G 10) on HA 0.5-treated jute fibers increases Young’s
composites. modulus and tensile strength by ∼73% (to 52 GPa) and ∼60%
Tensile Properties. Figure 3a−c shows the effect of (to 474 MPa), respectively, more than that of untreated jute
graphene material coatings on the tensile properties of single fibers. The improvement in tensile strength from G flakes is
jute fibers (Table S6, Supporting Information). As tensile lower than that of GO-coated fibers. However, Young’s
properties of natural fibers vary largely due to the variations in modulus of G flake (G 10)-coated jute fibers is higher than
fiber fineness, we use 50 single fibers for each test. We then that of any other coated fiber, probably due to the uniform
plot average results from these 50 samples in Figures 3, S4, and deposition of a large amount of flakes on the fiber surface, as
S5, Supporting Information. The values of tensile strength and evident from SEM image, in Figures 1c and S1d, Supporting
Young’s modulus obtained from mechanical characterization Information. We also compare diameter versus tensile
are statistically analyzed using a two-parameter Weibull properties of untreated and treated jute fibers (Figure S4,
distribution (eqs S1−S4, Supporting Information). The tensile Supporting Information). It shows that the increase of
modulus and strength of untreated fibers are found to be ∼30 diameter has an effect on both Young’s modulus and tensile
GPa and ∼295 MPa, respectively, which are similar to those strength of jute fiber.
reported in previous studies.5,48 We use a well-established Halpin−Tsi model50,51 to
After HA 0.5 treatment, the tensile modulus and strength is theoretically predict the reinforcing mechanism of coated
increased by 26 and 26.5%, respectively, as in Figure 3a,b. jute fibers with graphene materials. The modulus of the
However, the breaking force and extension at break is reduced graphene-based jute fibers can be calculated from the following
by 23.5 and 11%, respectively (Table S6, Supporting equations.
Information). This could possibly be because of voids that
3 (1 + ξηLVG) 5 (1 + εηW VG)
are created due to the irregular removal of impurities from the EC = × EM + = × EM
fiber surface by heat and alkali treatment (Figure S1b, 8 (1 − ηL*VG) 8 (1 − ηW VG)
Supporting Information). Several previous studies reported (3)
the effect of alkali treatment on jute fibers9,11,15 and indicate
that the tensile properties of jute fiber depend on its diameter (EG /EM − 1)
ηL =
and cellulose content. NaOH (alkali) solution has a strong (EG /EM + ξ) (4)
bleaching effect; thus, it removes impurities from the fiber
surface. The alkali treatment also degrades hemicellulose from (EG /EM − 1)
the interfibrillar region and removes lignin from the ηW =
intercellular region of jute fibers, causing separation of fibers (EG /EM + 2) (5)
from the cell and reduction in fiber diameter.11 They reported
that the removal of a significant amount of lignin could be (w + l)/2
ξ=2
responsible for the reduction in breaking force and breaking t (6)
extension of the jute fiber. Moreover, when the tensile force is
applied, the intercell of the jute fiber can shear easily at lower VG =
WG
force and extend due to the removal of lignin. Figure 3g shows WG + (ρG /ρM )(1 − WG) (7)
the broken surface of an untreated single jute fiber and
demonstrates an irregular pattern of breakage due to the where EC is the tensile modulus of graphene-based jute fibers,
angular arrangement of microfibrills. Baley and his co- VG is the effective volume fraction of graphene-based jute
workers49 observed a similar series of events in flax fibers fibers, EG and EM are the effective modulus of graphene and
where they explained that the slipping of these microfibrils fiber, respectively. The parameter ξ depends on the size and
happens during axial loading due to the local shear stress that is shape of the graphene used in this study and is determined by
developed between them. eq 6. L, W, and t represent the average graphene length, width,
Further treatment with graphene materials significantly and thickness. WG is the weight fraction of graphene and ρG
improves Young’s modulus and the tensile strength of jute and ρM are the density of graphene and jute fiber, respectively.
34507 DOI: 10.1021/acsami.8b13018
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Figure 4. Comparison of specific tensile properties: (a) specific Young’s modulus and (b) specific tensile strength of untreated and graphene
material-treated jute fibers with glass fiber (glass fiber value taken from the literature62).

Table 1. Tensile Properties of Natural Fiber before and after Modification Reported in the Literaturea
Young’s modulus, GPa Tensile strength, MPa
fibers treatment before treatment after treatment change % before treatment after treatment change % reference
jute NaOH 0.32% 17 14 −17.64 475 400 −15.78 15
jute NaOH 1%    250 360 +44 8
jute NaOH 5% + silane 5%    550 540 −1.82 52
jute nano-SiO2 21.5 23.1 +7.44 471.8 501.2 +6.23 53
flax NaOH    934 423 −54.7 54
flax (y) nano TiO2    5545 6344 +14.4 55
flax nano TiO2 (∼4%) 30.6 31.9 +4.24 464.0 480.6 +3.57 31
flax CNT (∼2%) 32 30 −6.25 400 300 −25 56
sisal SNC    512 451 −11.91 57
sisal NaOH 2% + silane 2% 12.2 7.5 −38.52 345 138 −60 58
kenaf NaOH 6% 40.32 37.82 −6.2 501.56 483.16 −3.66 59
jute GO 1% 30 48 +60 295 578 +95.93 this study
G 10% 30 52 +73.33 295 474 +60.67
a
SNC, starch nanocrystals; CNT, carbon nanotube’;  information not given; Y, yarn.

The parameters used for graphene (such as length, width, Figure 3d,e shows the Weibull probability distribution plots for
thickness, modulus, and density) in this study are tabulated in treated and untreated jute fibers considering the Young’s
Table S7, Supporting Information. We use eqs 3−7 to predict modulus and strength, respectively. Both distributions are
the theoretical values of Young’s modulus and then compare shifted significantly from the left to right side after fibers are
with the experimental results, in Figure 3c. As seen from the treated with graphene materials (GO and G). We obtain the
results, Young’s modulus increases with the increase of GO Weibull modulus from ln curves of both Young’s modulus and
concentrations both in experimental and theoretical results. tensile strength, Figures 3f and S5b, Supporting Information.
Moreover, the predicted tensile modulus of graphene-coated The untreated jute fibers provide a lower value of Weibull
fibers (HA−GO and HA−G) is slightly (∼6%) less than the modulus (∼1.86), which indicates a high scattering in the
experimental results, which is acceptable, as explained by Tian tensile properties of untreated jute fiber due to the non-
et al.50 They mention that the tensile modulus of graphene- homogenous nature of the fiber. However, the Weibull
based fibers is lower due to the wrinkled structure of graphene; modulus increases up to ∼2.95 after GO grafting, which may
whereas we consider a rectangular shape for graphene flakes in be due to the better bonding between fibers and GO, as
our theoretical calculation. On the basis of the results obtained, explained earlier. However, the Weibull modulus is reduced
we could say that the Halpin−Tsi model is an effective way to (∼1.67) for jute fibers treated with G flakes.
predict the tensile modulus of graphene-based fibers. We compare the specific properties (the ratio of the
Like IFSS, we carry out statistical analysis for jute fiber’s experimental value and density) of jute fiber with glass fibers.
tensile properties as well, as they exhibit scattered results for Figure 4a,b shows the comparison of the specific Young’s
tensile strength and Young’s modulus. We again use two- modulus and the specific tensile strength of jute and glass
parameter (scale parameter, α and shape parameter, β) Weibull fibers, respectively (Table S8, Supporting Information).
distribution for this analysis (Table S6, Supporting Informa- Specific properties of alkali-treated fiber are almost equal to
tion), where α predicts experimental results and β indicates the those of glass fiber. After graphene-based treatments, we
modulus of Weibull distribution known as Weibull modulus. achieve 15.6 and 18.5% higher specific modulus for GO-coated
34508 DOI: 10.1021/acsami.8b13018
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Figure 5. Microdroplet preparation: (a) microdroplet of jute/epoxy specimen and (b) schematic diagram of a microbond testing device using a
microvise.

(32 GPa/g/cm3) and G 10 (36 GPa/g/cm3)-coated fibers, 10 g of SDC and 50 g of flake graphite are added into a glass bottle
respectively, than that of glass fiber (27 GPa/g/cm3). Although and mixed with 500 mL of deionized (DI) water and sonicated for 30
the specific tensile strength of glass fiber is still higher than that min. This mixture is then passed through “Z-type” microfluidic
of GO- and G-treated fibers, graphene material treatment on channels of 200 and 87 mm diameter with diamond construction of a
Microfluidizer (M-110P Microfluidizer, Microfluidics Corp) at high
jute fibers shows a significant improvement in specific strength
pressure, which allows the exfoliation of graphite to few-layer
after grafting with GO and G flakes. We finally compare graphene (G Flakes) under a high shear rate (108 s−1). A modified
obtained results (the tensile properties) in this study with the Hummer’s method that was described elsewhere was used to prepare
recently published works, in Table 1. Although direct graphene oxide (GO) in water.60
comparison may be difficult as all results collected from the Alkali Treatment and Graphene Material Coating. Untreated
literature were obtained under different experimental con- jute fibers were washed with deionized (DI) water after cutting into
ditions. Table 1 shows a brief comparison between the results 30 cm long pieces, and they were then dried at 80 °C until a constant
obtained with various surface treatments on jute and other weight was achieved. These fibers were treated in warm water at 60
natural fibers. The traditional alkali treatment followed by °C for 60 min and then boiled at 100 °C for 30 min. The weight of
nanomodification of jute fiber in the literature does not show a fibers was reduced by 6 wt %, labeled as heat treated (HT) fibers.
significant improvement in the tensile properties. However, After these cleaning procedures, HT jute fibers were dipped in 0.5 wt
% NaOH solutions with a 1:50 material-to-liquor ratio (M/L) to
jute fiber treated by GO and graphene flakes in our study
remove hemicelluloses. The fibers obtained after two cycles of alkali
shows a fairly large increment in the both Young’s modulus treatment are termed as HA 0.5 and undergo losses of almost similar
(∼73.33% for G flakes) and tensile strength (∼95.9% for the weight ∼6 wt %, as reported in previous work.8
GO-treated jute fibers) than the untreated fiber. HA 0.5 jute fibers were then coated with GO and G flakes using a

■ CONCLUSIONS
We report grafting of graphene oxides and graphene flakes
simple dip coating for 30 min and subsequently dried at 80 °C for 30
min. The various concentrations of GO such as 0.25, 0.5, 0.75, and 1
wt % were used to prepare GO-coated samples: GO 0.25, GO 0.5,
onto jute fibers to produce high-performance graphene-based GO 0.75, and GO 1.0, respectively. Graphene flakes (1 and 10 wt %,
natural fiber composites. The graphene material-coated jute G 1 and G 10) were used to compare the performance with GO-
coated fibers. The concentrations of GO on the weight of jute fibers
fibers thus produced exhibit significant increase in the tensile
(owf %) were calculated as 0.34, 0.71, 0.97, and 1.54 wt % for GO
and interfacial properties and comparable specific properties to 0.25, GO 0.50, GO 0.75, and GO 1, respectively. Also, the
those of glass fibers. We believe that our graphene-based high- concentrations of graphene flakes (G 1 and G 10) were obtained as
performance natural fiber composite is an important step 1.53 and 2.41 wt %, respectively, on the weight of jute fibers (owf %).
toward replacing synthetic composites for some real world Characterization. A Philip XL-30 field emission gun scanning
applications. electron microscope (SEM) was used to analyze the surface

■ EXPERIMENTAL METHODS
Materials. The plant material (Corchorus Olitorious) known as
topography of the treated and untreated jute fibers. The surface
characteristics of untreated and graphene material-coated jute fibers
was analyzed using a Kratos axis X-ray photoelectron spectroscopy
(XPS) system and Fourier transform infrared spectroscopy (FTIR).
“Tossa white jute” was obtained from Bangladesh, cultivated on the
sandy loam plateau in the Northeast of Dhaka. The sample was The thermal decomposition of untreated and coated jute fibers from
cultivated from February to May in 2015. The annual rainfall of this room temp to 1000 °C in a nitrogen atmosphere at 10 °C/min
area is 500−1500 mm and the temperature ranges from 20 to 33 °C. heating rate was analyzed using a TA instrument (TGA Q5000, U.K.).
The content of long fibers in the bundles is 98−99 wt %, whereas the Tensile Testing of Elementary Fibers. The graphene material-
remaining 1−2 wt % is shives (cortical tissues and dust). The coated jute fibers were fibrillated using an inhouse handmade comb
untreated long jute fiber has a golden color with an average length and (Figure S6a, Supporting Information) and mixed together. The
diameter of 2.9 m and 0.059 mm, respectively. Analytical grade elementary fibers are separated from the fibrillated fiber bundle
sodium hydroxide (NaOH) pellets (product no: 10502731) were (technical fiber) (Figure S7, Supporting Information). These were
purchased from Fisher Scientific, U.K. EL2 Epoxy Laminating Resin then mounted on a paper frame using superglue and left overnight to
and AT30 Epoxy Hardener were purchased from Easy Composites, be cured properly. The average fiber diameter was measured from five
U.K. The natural flake graphite (average lateral size 50 mm) was measurements for every fiber using a digital microscope (Keyence
kindly supplied by Graphexel Limited, U.K. Sodium deoxycholate digital microscope VHX-500F, U.K.). These fiber samples were then
(SDC) powder, potassium permanganate (KMnO4), sulfuric acid kept in a standard laboratory atmosphere (55% relative humidity and
(H2SO4, ∼99%), and hydrogen peroxide (H2O2, ∼30%) were 20 ± 2 °C) for 24 h before further testing. A Zwick tensile testing
purchased from Sigma-Aldrich, U.K. machine (Zwick/Roell, U.K.) with a load cell of 20 N was used to
Graphene Material Synthesis. Our previously reported method measure the uniaxial tensile strength and elongation at break of jute
was followed to prepare microfluidized graphene flakes (G).23 Briefly, fibers. A gauge length of 20 mm was used with a crosshead speed of 2

34509 DOI: 10.1021/acsami.8b13018

ACS Appl. Mater. Interfaces 2018, 10, 34502−34512
ACS Applied Materials & Interfaces Research Article

mm/min according to ASTM standard D3822-01.8 The moduli of the

fibers were calculated from the slope at 0.1−0.3% strain of the fiber.
Single-Fiber Microbond Test. As previously reported,61 all
■ ACKNOWLEDGMENTS
Authors kindly acknowledge Commonwealth Scholarship
elementary fibers with a length between 30 and 50 mm were Council, U.K. and the Government of Bangladesh for the
separated manually for single-fiber microbond test. Elementary fibers PhD funding of Forkan Sarker and Shaila Afroj, respectively.
were then attached to a window of the paper card frame (25 × 10 This work was supported by EU Graphene Flagship Program,
mm) using superglue with a very negligible amount of tension (Figure European Research Council Synergy Grant Hetero2D, the
S6b, Supporting Information). Microdroplets of epoxy resin were Royal Society, and Engineering and Physical Sciences Research
created using a glass fiber, as in Figure 5a, and then applied to test Council, U.K. (Grant Number: EP/N010345/1, 2015).

■
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