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Sustainable and Multifunctional Composites

of Graphene-Based Natural Jute Fibers
Nazmul Karim,* Forkan Sarker, Shaila Afroj, Minglonghai Zhang, Prasad Potluri,
and Kostya S. Novoselov

concerns with plastics and synthetic fibers

Smart and sustainable natural fiber-based composites are of great interest such as glass and carbon. The environ-
due to their biodegradability, recyclability, and environmental benefits over mental impact of plastics and synthetic
synthetic fiber composites. In addition, the environmental impact of plastics fibers are widespread and substantial
(Table S1, Supporting Information). For
and synthetic fibers are widespread and substantial, as they can stay in the
example, plastics can hang around the envi-
environment for hundreds of years and contribute significantly to global ronment for ≈450 years[4] and contribute to
carbon emissions. Natural fibers such as jute can potentially replace syn- ≈15% of global carbon emissions;[5] glass
thetic fibers to manufacture environmentally sustainable, biodegradable, and and carbon fibers have an impact of ≈2.5
lightweight composites with improved properties, good thermal and acoustic and ≈29.4 tonnes CO2-eq per tonne of
fiber production, respectively.[6] Therefore,
insulation, and a smaller carbon footprint. However, natural jute fiber-based
there is a pressing need for sustainable,
composites suffer not only from poor mechanical properties but also being biodegradable, and lightweight materials
inherently electrically insulating, which limits their applications as multifunc- for structural composite applications, that
tional composites. Here multi-functional and environmentally sustainable would offer unprecedented combinations
smart composites of graphene-based natural jute fibers with excellent tensile of stiffness, strength and toughness at
and interfacial properties are reported. The reduced graphene oxide-based low density, and could be manufactured at
high volume and low cost.[7] Natural fiber
natural jute fiber enhance the Young’s modulus of the composites by ≈450%,
composites have shown great potential to
and tensile strength by ≈183% after physical and chemical treatment. Such replace synthetic fiber-based composites,
high-performance composites can also be used as multifunctional smart due to their higher specific mechanical
composites, as demonstrated by effective electro-magnetic interference properties, good thermal and acoustic
shielding performance. This may lead to manufacturing of next generation insulation, and smaller carbon foot print
(Table S2, Supporting Information).[8]
smart, strong, and sustainable natural fiber composites for high performance
Jute, known as the “golden fiber” which
engineering applications without conferring environmental problems. is extracted from the bark of the white
jute plant (Corchorus capsularis), and is a
100% bio-degradable, recyclable, and envi-
1. Introduction ronmentally friendly natural fiber. It is also the second mostly
produced natural fiber in the world after cotton, mainly in devel-
In recent years, sustainable and biodegradable natural fibers[1–3] oping countries such as Bangladesh, China, and India, and at
have attracted significant interests due to growing environmental least ≈50% cheaper than flax and other similar natural fibers.[9]

Dr. N. Karim, Dr. S. Afroj Dr. F. Sarker

Centre for Fine Print Research Department of Textiles Engineering
The University of West of England Dhaka University of Engineering and Technology
Bristol BS3 2JT, UK Gazipur, Bangladesh
E-mail: [email protected] Dr. F. Sarker, Prof. P. Potluri
Dr. N. Karim, Dr. S. Afroj, Prof. K. S. Novoselov The Department of Materials
The National Graphene Institute (NGI) The University of Manchester
The University of Manchester Oxford Road, Manchester M13 9PL, UK
Booth Street East, Manchester M13 9PL, UK M. Zhang
Institute of Textile and Clothing
The ORCID identification number(s) for the author(s) of this article
The Hong Kong Polytechnic University
can be found under https://doi.org/10.1002/adsu.202000228.
Hong Kong, China
© 2021 The Authors. Advanced Sustainable Systems published by Prof. K. S. Novoselov
Wiley-VCH GmbH. This is an open access article under the terms of the Department of Materials Science and Engineering
Creative Commons Attribution License, which permits use, distribution National University of Singapore
and reproduction in any medium, provided the original work is properly 9 Engineering Drive 1, Singapore 117575, Singapore
cited. Prof. K. S. Novoselov
Chongqing 2D Materials Institute
DOI: 10.1002/adsu.202000228 Liangjiang New Area, Chongqing 400714, China

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However, jute fiber reinforced composites suffer from lower properties of our graphene-based natural jute fiber-reinforced
mechanical and poor interfacial properties, due to the lower composites were analyzed and compared with that of synthetic
crystallinity and hydrophilicity introduced via larger amount fiber-reinforced composites.
(≈20–50 wt%) of non-cellulosic materials in their structure.[10,11]
Moreover, jute fibers are inherently electrically insulating, which
limits their application as multifunctional composites, when 2. Results and Discussion
electrical conductivity is required.
“Smart” multifunctional composites are very popular at the 2.1. Scalable Production of Graphene-Based Natural Jute Fibers
moment, due to their ability to reversibly respond to one or
more environmental stimuli such as chemical, electrical, light, rGO is a graphene derivative, composed of perfect graphene
temperature, and mechanical. Traditionally, smart composites sheet with small number of hydroxyl epoxy and other groups
are based on metals, polymers, and carbon-based nanomate- attached to it. As a result, it demonstrates similar mechan-
rials.[12–14] However, metals and polymer-based composites suffer ical and electronic properties to pristine graphene. Though
from oxidation and poor mechanical properties, respectively. In numerous efforts have been made to produce pristine graphene-
contrast, carbon nanomaterials have potential for “smart” mul- like materials via reduction of GO to rGO, only partial restoration
tifunctional composites, as they are usually cost-effective, stable, of graphene-like structure is possible with residual functional
mechanically strong and flexible, and electrically and thermally groups and structural defects.[24] However such residual func-
conductive.[15] Carbon nanotubes (CNT) have been investigated tional groups are perfect for creating suitable bonding with that
extensively as “smart” materials,[16] however the process of of natural fibers to enable durable and uniform rGO coatings.
CNT synthesis is expensive and complicated. Conversely, gra- Moreover, rGO could be produced in a scalable quantity due
phene demonstrates multifunctional properties such as large to simple and cheap production process of its precursor: GO.
specific surface areas, high electrical and thermal conductivity, Here, a previously reported process to prepare GO via a modi-
and excellent mechanical properties.[17–19] In addition, graphene fied Hummers method was used, with subsequent reduction to
derivatives such as reduced graphene oxide (rGO) can not rGO via an in situ-chemical reduction process of GO.[23,25,26] The
only be produced in a scalable and cost-effective way, but also average flake thickness and size of as prepared rGO is found to
be grafted into natural fiber via suitable bondings. Thus, gra- be ≈2.26 nm and ≈4.86 µm, respectively, confirming the pres-
phene-based materials are ideal candidate for making “smart” ence of single to few layers of graphene flakes in the dispersion.
natural fiber-reinforced composites with capability of electro- Raman spectra of rGO show the shifting of characteristics D
magnetic interference (EMI) shielding, structural health moni- and G peaks toward lower wave numbers: ≈1327.4 cm−1 (D) and
toring (SHM), de-icing, and energy storage. In our previous ≈1596.82 cm−1 (G), which is due to the recovery of hexagonal
studies,[20,21] graphene materials such as graphene oxide (GO) symmetry of the lattice. The intensity ratio of the D and G band
and graphene flakes (G) were deposited on jute fibers which (ID/IG) is also increased from ≈0.98 (GO) to ≈1.73 (rGO).
improved tensile and interfacial properties significantly. How- Before rGO coating, jute fibers were cleaned, and pre-treated
ever, GO is electrically insulating and not suitable for “smart” with heat and alkali (NaOH) as per the previous study.[20] Sur-
composite applications; whereas G flakes are almost without face pre-treated jute fibers (HA0.5) were then coated with rGO
any oxygen-containing functional groups, and suffer from poor using a simple dip-coating technique and oven dried at 80 °C
interfacial properties due to the absence of a suitable bonding for 30 min, Figure 1a. XPS analysis was used to characterize
with natural fibers. Thus, rGO could be an ideal material for surface functionalities of untreated and rGO-coated jute fibers,
making high performance, multifunctional, and environmen- Figure 1b–d. The wide scan XPS spectra shows that the C/O
tally sustainable natural fiber composites. It could provide excel- ratio of jute fibers decreases from ≈5.5 to ≈3.8 after coating
lent mechanical properties due to specific interaction between with GO, due to the presence of oxygen containing functional
residual oxygen functional groups of rGO and that of natural groups in GO.[27,28] After rGO coating, C/O ratio increased
fibers,[22,23] as well as imparting electrical and thermal proper- to ≈7.1, due to the partial restoration of graphene structures,
ties required to make next generation “smart” composites. Figure 1b. The high resolution C1s X-ray photoelectron spec-
Here, we report multi-functional and environmentally sus- troscopy (XPS) spectrum of untreated jute fibers confirms the
tainable smart composites of rGO-based natural jute fibers with presence of three main components: CC bond (≈284.5 eV)
excellent tensile and interfacial properties. We used scalable in cellulosic structure, COC groups (hydroxyl and epoxy,
synthesis of rGO in a water-based and biocompatible disper- ≈286.5 eV) and CO groups (carbonyl, ≈288.3 eV), Figure 1c.[24]
sion, and a facile coating technique to produce graphene-coated After coating with rGO, the peaks associated with the oxygen
unidirectional jute fiber preforms with new fiber architec- functional groups significantly diminished with small amounts
ture, before jute/epoxy composites were manufactured via a of residual oxygen functional groups left as evident from the
simple vacuum resin infusion process. Graphene-based single peak around 287.5 eV, Figure 1d.[23,25,26]
jute fibers were characterized, tested, and analyzed to investi- Figure S1a, Supporting information shows SEM images of a
gate tensile and interfacial properties. The improvement in smooth and featureless untreated jute fiber surface, which may
longitudinal and transverse mechanical properties of com- be due to the presence of a cementing layer that is composed of
posites, and their fracture surface was tested and analyzed. A waxes, fats, lignin, pectin, and hemicelluloses.[29] The coating
potential application of multifunctional graphene-based nat- of rGO results in a more uniform, highly individualized, and
ural fiber composites as EMI device is demonstrated. Finally, evenly coated fiber surface with only a few flakes present on
the environmental impact, sustainability, and mechanical the surface (Figure S1d, Supporting Information), which may

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Figure 1. a) Schematic diagram showing rGO coating process on jute fibers and the preparation of rGO-coated jute fibers preforms, b) wide scan XPS
spectrum of graphite, G flakes, GO, and rGO, c) high resolution C(1s) XPS spectrum of untreated jute fiber, and d) high resolution C(1s) XPS spectrum
of rGO-coated jute fiber.

be due to chemical bonding provided by the functional groups jute fiber on the behavior of final jute fiber reinforced compos-
of rGO.[22] The diameter of untreated jute fibers is found to ites. Static and dynamic single fiber tests (Figure 2a) are more
be ≈55 ± 12 µm, which is reduced to ≈43 ± 8 µm (Figure S1c, difficult to conduct due to the small diameter of the fiber, which
Supporting Information) after heat and alkali treatment, which imposes great challenges in fiber handling and clamping due
may be due to the removal of hemicellulose, pectin, and lignin. to the slippage. We used 50 single fibers for each test and then
The diameter of rGO-coated jute fibers (HA rGO5) reduced plotted average results from those 50 samples in Figure 2b–d
further by ≈34.5% to ≈36 ± 16 µm (Figures S2b and S4a, Sup- and Table S3, Supporting Information. The tensile modulus
porting Information), unlike the previously reported study and strength of UT are found to be ≈30 GPa and ≈295 MPa,
where coating with GO and G flakes increase the diameter of respectively, which increase slightly after heat and alkali treat-
HA0.5 jute fibers slightly.[20] Fourier transform infrared spec- ment (HA0.5) and are similar to those reported in our previous
troscopy (FTIR) analysis confirms the removal of hemicellulose study.[20] After rGO5 (5 wt%) coatings, the Young’s modulus
and lignin after rGO coatings. Moreover, a characteristic peak of jute fiber increases from ≈30 to ≈78 GPa, and the tensile
is identified at ≈2400 cm−1 band for rGO-coated fiber indicates strength from ≈295 to ≈814 MPa, which are ≈160% and ≈174.5%
the conjugated CC bonding between the functional group of increment compared to that of UT. This is the highest tensile
rGO and jute fiber (Figure S3a, Supporting Information). TGA properties obtained so far with alkali treatment and nanosur-
analysis shows that rGO coating improves the thermal stability face engineering of jute fibers to the best of our knowledge.
of HA0.5 jute fibers, which may be due to the formation of a As expected, the tensile properties of jute fibers improve with
carbonaceous coating of graphene like materials on the fiber the increase in rGO concentrations (0.5–5 wt%), Figure 2b,c.
surface, which delays the degradation and improves thermal Although fiber breaking strain and breaking force reduced
stability of the fiber. This was confirmed by the increase of res- initially after alkali treatment, they are increased by 38% and
idue% from ≈17% for untreated fibers (UT) to ≈36% for rGO- 71%, respectively, after rGO5 coating on jute fibers, Figure 2d
coated jute fiber (Figure S3b, Supporting Information). and Table S3, Supporting Information. In addition, the area
under the stress–strain curve provides the higher extension,
which demonstrates excellent flexibility and higher toughness
2.2. Single Fiber Tests: Tensile and Interfacial Properties against fracture of rGO5-coated jute fibers under tensile stress.
(Figure S4b, Supporting Information).
First, a single fiber test was used to get an insight into the effect The excellent tensile properties with rGO coatings could be
of tensile and interfacial properties of individual rGO-coated explained by Faber and Evan’s crack deflection theory.[30] The

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Figure 2. Single fiber tensile and interfacial properties. a) Sample preparation for single fiber test, b) Young’s modulus, c) tensile strength and d) tensile
strain% of untreated, HA0.5, and rGO-coated jute fibers. e) SEM images of the fracture specimen after single fiber tensile test without any treatment
(X250) and f) SEM images of the fracture specimen after tensile test of single jute fiber after rGO coating (X250). g) Young’s modulus and h) tensile
strength data fitted to a two-parameter Weibull probability distribution as function of surface treatment. i) Comparative analysis of theoretical and
experimental Young’s modulus of untreated and graphene-based jute fibers. Optical images of microdroplets of rGO-coated fiber: j) Before testing and
k) after testing. l) Interfacial shear strength (IFSS) of untreated, HA0.5, and rGO-coated jute fibers, m) Interfacial shear strength (IFSS) data fitted to
a two-parameter Weibull probability distribution as function of surface treatment.

rGO flakes could possibly increase the crack area by deflecting an enhancement of the stress transfer and the tensile strength
any advancing crack and thus reducing the stress generated at of jute fibers. The fracture specimen after tensile test was also
their tip. This is because the rate of effective crack deflection investigated, which shows uneven microfibrils fracture for
depends on the orientation of platelet particles perpendicular untreated jute fibers due to stress concentration between the
to the crack growth. Additionally, in a neat graphene system cellulosic microfibrils in the fiber, Figure 2e. However, when
three types of dominant interactions exist between graphene the fibers are coated with rGO5, a linear breakage of microfi-
sheets: van der Waals interaction, hydrogen bonds, and coor- brils is observed which is responsible for more loading capacity
dinative cross-linking. After the chemical reduction of GO, the along the tensile deformation, Figure 2f.
van der Waals interaction along the decreasing interlayer space A two-parameter (scale parameter, α and shape parameter, β)
and the hydrogen bonds between residual oxygen functional Weibull distribution was used (Equations (S1)–(S6) and Table S3,
groups are increased. As a result, the mechanical properties Supporting Information), where α predicts experimental
of coated fibers are enhanced.[31] Furthermore, the presence results and β indicates the modulus of Weibull distribution
of PSS polymers in rGO dispersions, and partial reduction of known as Weibull modulus. Figure 2g,h shows that the distri-
GO might increase the stacking and slippage of the graphene bution for both Young’s modulus and tensile strength shifted
sheets stacking and slip, which enhances the elongation and significantly from the left to right side after fibers are treated
breaking force.[32] SEM of the rGO-coated jute shows highly with rGO. The untreated jute fibers provide a lower value of
individualized fibers, in Figure S1d, Supporting information. Weibull modulus ≈1.86 (Figure S6a,b, Supporting Information),
The pores on the fiber surface are filled with rGO flakes, which which indicates higher scattering in the tensile properties of
improve the uniformity in the network structure, resulting in untreated jute fiber, due to the non-homogenous nature of the

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fiber. However, the Weibull modulus increases up to ≈2.46 after treatments together with rGO coating results in ≈450% and
rGO grafting, which may be due to the better bonding between ≈183% improvement in the Young’s modulus and tensile
fibers and rGO as explained earlier. A well-established Halpin– strength of the composites, which is the highest improvement
Tsi model was also used to theoretically predict the reinforcing in the tensile properties of any kind of natural fiber compos-
mechanism of rGO-coated jute fibers and calculate theoretical ites reported in the literature (Table 1). As per rule-of-mixture,
value of Young’s modulus (Equations (S7)–(S11) and Table S4, such massive improvement in tensile properties of natural jute
Supporting information).[20] Figure 2i shows that the Young’s fiber composites may be due to the significant increment in
modulus increases with the increase of rGO concentrations fiber volume fraction (Vf ) (Table S7, Supporting Information)
both in experimental and theoretical results. The predicted ten- after combined physical (individualization and compaction)
sile modulus of graphene-coated fibers (rGO5) is slightly (≈5%) and chemical (alkali and rGO) treatments. To better understand
less than the experimental results, which is acceptable due to the effect of rGO coating on the IFSS at composite level, we
the wrinkled structure of graphene flakes rather than the rec- carried out tensile testing in transverse direction of the com-
tangular shape, which was assumed in our theoretical calcula- posites, Figure 3e–g. As expected, the untreated fiber and fiber
tion and detailed by Tian et al.[33] Figure 2j,k shows the optical with new architecture shows relatively lower transverse tensile
images of microdroplets before and after a micro-bond test. properties, due to the fiber impurities that caused poor interfa-
The micro-bonding test of untreated jute fibers shows relatively cial adhesion between the fiber and matrix. After rGO coatings,
lower interfacial shear strength, IFSS (≈4.16 MPa) for untreated transverse tensile properties of jute fiber composites improve
jute fiber-epoxy micro-composites, which increases to ≈7.37 MPa almost ≈100% in comparison to that of untreated fiber. This
after heat alkali treatment (HA0.5), Figure 2l. After coating may be due to the increased surface roughness and mechanical
with rGO5, IFSS increases slightly to ≈8.2 MPa, Figure 2l and inter-locking between the fiber and matrix with rGO coating.
Table S5, Supporting Information. Like tensile properties the A stress–strain curve clearly shows uninterrupted stress
Weibull distribution for IFSS shifted from the left to right, development for rGO-coated jute fiber composites, which can
Figure 2m and Figure S6c, Supporting Information. Compara- be considered as a similar behavior to glass or carbon like
tive study (Table S6, Supporting Information) confirms the monolithic reinforcing materials in composites, Figure 3h.
effect of rGO on improving the IFSS value is better than other We examine the fracture surface of the composites specimen
natural and synthetic fibers modified by traditional alkali and after tensile test using a scanning electron microscope (SEM),
nanomaterials. Figure 3i,j. For the untreated jute fiber composite, the surface of
the composites fails predominantly due to the weak interfacial
bonding and the fiber pull-out, Figure 3i. The fracture surface
2.3. Ultra-Strong Composites of Graphene-Based of rGO-coated jute fiber composites shows an uneven scat-
Natural Jute Fibers tered failure of fibers and also a strong inter-fibrillar connection
between each individual jute fiber, Figure 3j and Figure S8a,
The untreated unidirectional jute fiber composites have Supporting Information. However, SEM images of fractured
relatively lower tensile properties: The Young’s modulus of surfaces in traverse directions show a complete matrix failure
≈10 GPa and tensile strength of ≈180 MPa is due to presence (matrix debonding) from the fiber, which is the reflection of
of excessive amount of non-cellulosic materials like hemicel- poor interfacial shear failure of the composites (Figure S8b,
lulose and lignin, Figure 3a–c. We therefore developed new Supporting Information).[34] We then examined the cross sec-
jute fiber architecture to remove those non-cellulosic mate- tion of coated jute fiber composites to study the packing order
rials, and to obtain Young’s modulus of ≈27.6 GPa and tensile and porosity related issues of the composites. Natural fiber-
strength of ≈232 MPa (Table S7, Supporting Information). Such based composites are always susceptible to producing different
improvement could be explained by the individualization and porosities[35] such as matrix porosity, impregnation porosity,
compaction of fibers to increase the fiber volume fraction (Vf ) and luminal porosity, due to inherent flaws and lower crystal-
(Equations (S12) and (S13), Supporting Information) and load- linity.[36] In contrast, rGO-coated jute fibers composites show
bearing capacity of the composites.[21] Further treatment with strong packing of fibers and no such porosity related issues
alkali and a hot press improves the fiber packing (Figure S7b, (Figure S7b, Supporting Information).
Supporting Information) and fiber-matrix interfacial adhesions.
Our previous studies[20,21] reported that coatings of graphene
materials (GO and G flakes) on surface pre-treated jute fibers 2.4. Multifunctional Composites of Graphene-Based
could increase the surface wettability and roughness of the Natural Fibers
fiber; thus, enhance the interfacial and mechanical properties
of the composites significantly. Similarly, we prepared unidirec- High performance, multi-functional, and bio-compatible com-
tional rGO-coated new jute fiber preform by combining physical posites are becoming increasingly attractive to composite
and chemical treatment (NFHP), and then used those preforms manufacturers and material scientists, due to their ability to
to prepare fiber reinforced composites via a simple vacuum provide excellent mechanical, thermal, electrical, and opto-elec-
resin infusion process, Figure 3d.[21] The Young’s modulus and trical properties.[37] Recently nanomaterials such as conductive
tensile strength of as prepared composites increase signifi- polymers, metals, CNT, and other carbon-based materials have
cantly, from ≈27.6 to ≈55 GPa and ≈232 to ≈510 MPa with rGO5 been investigated to make electrically and thermally conductive
(0.5 wt%) coated jute fibers. (Figure 3a–c; Table S7, Supporting “Smart Composites” with improved mechanical properties for
Information). The combination of all physical and chemical multifunctional applications such as SHM, EMI shielding, and

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Figure 3. a) Young’s modulus, b) tensile strength, and c) strain % of untreated, new fiber architecture, and different concentrations of rGO-coated
jute fiber epoxy composites in longitudinal direction. d) Schematic of rGO-coated jute fiber reinforced composites manufacturing process, e) Young’s
modulus, f) tensile strength, and g) strain % of untreated, new fiber architecture, and different concentrations of rGO-coated jute fiber epoxy compos-
ites in transverse direction. h) Stress–strain curves of untreated, HA0.5 treated, rGO1, and rGO5 treated jute fiber reinforced composites. i) SEM image
of the fracture surface of UT fiber reinforced composites, and j) SEM image on the fracture surface of rGO-coated composites in longitudinal direction.

joule heating.[13,38,39] The outstanding electrical, mechanical, natural fiber composites not only demonstrate excellent tensile
and thermal properties, high surface area, and cost-effective properties but also demonstrate relatively high electrical and
production cost of graphene-based materials[17–19] made them thermal conductivity. Thus, they could potentially be applied for
perfect material for multi-functional “smart” composite appli- smart composites applications with capabilities of EMI, SHM,
cation. Our multifunctional composites of graphene-based de-icing, and energy storage. Here, we demonstrate potential

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Table 1. Comparative tensile properties of graphene-coated jute fiber/epoxy composites with other surface-treated natural fiber composites in the
literatures.

Fibers Vf [%] Young’s modulus, GPa Tensile strength, MPa Ref.

Before treatment After treatment Change [%] Before treatment After treatment Change [%]
Fiber scale

Sisal (SNC) – – – – 512 451 +115.9 [46]

Oil Palm (CuNP) – 4.1 4.5 +9.75 213 255 +18.6 [47]

Flax (Ti O2 2.35%) – 30.5 32.5 +6.55 380 490.2 +29 [48]

Jute (GO 0.25%) – 30 37 +23.3 295 394 +33.5 [20]

Jute (GO 0.5%) – 30 44 +46.6 295 436 +47.7 [20]

Jute (GO 0.75%) – 30 46 +53.3 295 501 +69.8 [20]

Jute (GO 1.0%) – 30 48 +60 295 575 +94.9 [20]

Jute (rGO 1.0%) – 30 50 +66.6 295 604 +104.7 This study

Jute (rGO 5.0%) – 30 78 +160 295 814 +175.9 This study

Composites scale

Ramie (CNT 0.7%) – 6 7 +16.6 57 78 +36.8 [49]

Oil Palm (CuNP) – – – – 255 350 +37.25 [47]

Jute (GO 0.25%) 54 27.6 36.9 +33.6 232 295 +27.1 [21]

Jute (GO 0.5%) 54 27.6 42.8 +55 232 337 +45.2 [21]

Jute (GO 0.75%) 56 27.6 44.6 +61.5 232 379 +63.3 [21]

Jute (GO 1.0%) 55 27.6 37.8 +36.9 232 292 +25.8 [21]

Carbon (GO 5%) 48 45 55 +22.2 1750 2000 +14.28 [50]

Jute (rGO 1.0%) 59 27.6 40 +44.9 232 370 +59.4 This study

Jute (rGO 5.0%) 60 27.6 55 +99.2 232 510 +119.8 This study

– stands for information not given.

EMI shielding application of three composite samples com- and the layered structure of graphene flakes; thus, this dissi-
prised of five layers of UD jute fiber preforms (HA0.5 treated, pates EMI waves and improves the SE.
rGO coated, and G flake coated).
EMI is perceived as new form of pollution due to increased
use of electronics and instrumentation in commercial and 2.5. Sustainability, Environmental Impacts,
industrial settings.[40] EMI could interact with biological sys- and Comparative Study
tems and, at high intensities can potentially damage the human
body’s DNA structure.[41] The EMI shielding mechanism of nat- Millions of people, especially from developing countries are
ural fiber composites samples (Figure 4a) could be explained involved in natural fiber industries, and as such, fiber-based
by a combination of the high conductivity, smaller thickness products are processed and manufactured in many small and
(which guarantees significant transmission through a single large industries around the world. Thus, the economic impact
layer), and layered structure (which ensures multiple reflec- of the consumption of natural fiber-based products has been
tions) of rGO. At 8.2 GHz frequency, the shielding effective- quite significant. For example, Jute is the second most pro-
ness (SE)% increases from ≈49.2% for HA0.5 treated jute fiber duced natural fiber in the world after cotton (≈3.63 million
composites to ≈77.1% for natural composites of rGO-coated tonnes annually, Figure 5a), and at least ≈50% cheaper than
jute fibers, Figure 4b. As expected the highest SE% (≈92.9%) flax and other similar natural fibers. The use of jute for various
is obtained for composites of G flake-coated jute fibers applications could boost the farming economies of developing
(Figure 4b), due to higher conductivity of G-coated jute fibers. countries such as Bangladesh and India, where it is mostly pro-
Similarly, absorption% increased with the increase of the elec- duced. Jute is extracted from the bark of the white jute plant
trical conductivity of the sample, Figure 4c. The shielding (C. capsularis), and a 100% bio-degradable, recyclable, and envi-
mechanism of graphene material-coated jute composites is the ronmentally friendly natural fiber. However, natural fibers lost
combination of reflection and absorption of EM waves. Once its glaze with the introduction of cheaper and high-performance
EM waves are absorbed into the graphene-coated composites, it synthetic fibers such as polyester and nylon for textile applica-
undergoes internal reflection due to the porous fiber structure tions, and glass and carbon fiber for composites applications.

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Figure 4. Multifunctional smart composites of graphene-based natural fiber. a) Schematic diagram of EMI shielding mechanism and graphene-based
natural jute composites; b) shielding effectiveness% versus frequency and c) absorption% versus frequency.

Nevertheless, with growing environmental concerns with plas- natural fibers consume less energy but more water during
tics and synthetic fibers, the use of natural fibers such as jute is their production process than synthetic fibers.[42] The most
on the rise again. Here, we compare the environmental impact, pressing environmental impact with natural fiber production
Materials Sustainability Index (MSI) score and properties of is the water usage during their cultivation. About 3% of global
jute with their synthetic counterparts such as such as glass and irrigation (≈44 trillion liters annually) water is used for textile
carbon. It is worth mentioning that the composite preparation fiber productions.[43] Indeed, jute has a higher water foot-print
is similar for both synthetic and natural fiber reinforcements; (0.08 m3 kg−1 fiber) as per the water scarcity weighting than that
we therefore analyses fiber performance for sustainability and of carbon (0.03 m3 kg−1 fiber) and glass fibers (0.01 m3 kg−1 fiber),
environmental impact. Figure 5a–c. However, the energy consumption for jute fiber
The production of glass and carbon fibers (≈1.14 and ≈0.15 production (≈9.6 MJ kg−1 fiber) is ≈6 times and ≈30 times lower
million tonnes, respectively, in 2018) is increasing globally, due than that of glass (≈54.7 MJ kg−1) and carbon (≈286 MJ kg−1)
to the rise in the demand for high-performance and lightweight fibers, respectively. Such higher energy consumption with
materials, Figure 5a–c. However, jute fibers are produced in synthetic fiber production is associated with their produc-
larger quantities (≈3.63 million tonnes in 2018) with a rapidly tion process and higher manufacturing temperature for glass
increasing amount in recent years, and have always been the (1400–1500 °C) and carbon (≈1000 °C). As a result, the carbon
most dominant bast fiber, Figure 5d. The environmental impact footprint with synthetic fibers is significantly higher. For
of fiber production varies between their types. For example, example, virgin carbon and glass fiber emits ≈29.4 and ≈2.5 tonne

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Figure 5. Environmental sustainability, impacts, and comparative study. Fiber production, energy consumptions, water scarcity, and carbon emissions
for a) jute, b) glass fiber, and c) carbon fiber; d) total bast fiber production globally from 2008 to 2018; e) Materials Sustainability Index (MSI) score for
jute, glass, and carbon fiber and f) comparative specific properties of jute, flax, and glass fiber composites.

CO2 for per tonne fiber production. In contrast, plant fibers fiber and their composites modified with nanomaterials, as
such as jute act as a carbon sink by sequestering atmospheric reported in the literature. rGO-coated jute fibers show signifi-
carbon.[44] For example, one tonne of dry jute fiber could absorb cantly higher Young’s modulus of ≈78 GPa and tensile strength
≈2.4 tonnes of CO2. We also compare cradle-to-gate Higgs MSI of ≈814 MPa, which is the highest reported value of mechanical
score from the life cycle assessment to understand and quantify properties based on natural fiber modified with nanomate-
the sustainability impacts of jute, carbon, and glass fibers.[45] rials. In order to check the suitability of our newly developed
Carbon and glass fibers contribute toward global warming and rGO-coated jute fiber/epoxy composite in high-performance
fossil fuel consumption significantly higher than jute. How- applications where mainly glass and carbon fiber are used, we
ever, jute fiber contribution to water scarcity is substantial, and compare its tensile properties with both S-glass and E-glass
its eutrophication is comparable to that of carbon fiber. Never- fiber composites (Table S7, Supporting Information). In addi-
theless, the replacement of synthetic fibers with natural plant- tion, Young’s modulus of rGO-coated jute fiber/epoxy com-
based jute for multi-functional composite applications could posite is found to be ≈55 GPa, which is ≈18% and ≈40% higher
potentially provide sustainable and environmentally friendly than that of S-glass (≈33.5 GPa) and E-glass (≈45.1 GPa) fiber/
composites; thus, reduces the greenhouse-gases impact with epoxy composites, respectively. The value of Young’s modulus
fiber reinforce composites significantly. of rGO-coated jute fiber composites is even similar to that of
We then compare specific properties of untreated and treated GO-coated carbon fiber composites (≈55 GPa) as reported in
jute fiber composites with that of flax, E-glass, and S-glass the literature (Table 1). Thus, newly developed rGO-coated jute
fiber composites Figure 5f. The specific Young’s modulus of fiber composites cannot only be used as a replacement for glass
untreated jute fiber composites is found to be ≈8.7 GPa g−1 cm−3, for specific property-driven applications but also in stiffness-
which increases to ≈42.3 GPa g−1 cm−3 for composites with HA- driven high-performance engineered structure applications.
treated and rGO-coated fibers, Figure 5f. Thus, the Young’s
modulus of newly developed rGO5.0 coated jute fiber compos-
ites is ≈139% and ≈79% higher than that of E (≈17.7 GPa g−1 cm−3) 3. Conclusion
and S (≈23.6 GPa g−1 cm−3) glass fibers, respectively. The spe-
cific strength of rGO-coated jute composites is found to be In this study, we report the formation of multi-functional
similar to that of E-glass fibers. Table 1 shows a comparison of and environmentally sustainable smart composites of rGO-
rGO-coated jute fiber and their composites with other natural based natural jute fibers with excellent tensile and interfacial

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properties. Morphological and micro-structural investigations A simple dip coating technique was used to coat the alkali-treated
reveal that rGO is uniformly coated onto jute fiber surface. jute fiber with rGO. An optimized time of 30 min with M:L of 1:10 was
Thus, it shows a remarkable improvement in fiber and com- used in this coating technique to create stable and uniform surface
coating (Figure S11a, Supporting Information). The coated fibers were
posite mechanical properties, as well as electro-magnetic subsequently dried in the oven for 30 min at 80 °C. A range of rGO
properties of the composites, possibly due to the formation concentrations (0.25, 0.5, 0.75, 1, and 5 wt%) was used to prepare rGO-
of suitable bonding between the residual oxygen functional coated samples, which were labeled as rGO 0.25, rGO 0.5, rGO 0.75,
groups of rGO and the hydroxyl groups of jute fibers. There- rGO 1, and rGO 5, respectively.
fore, smart, strong, and sustainable rGO-based jute fiber Manufacturing of rGO-Coated Jute Fiber Preforms: The development
composites offer a great opportunity to replace its synthetic of rGO-coated jute fiber preforms comprised of several steps which
include the combination of physical, chemical, and mechanical actions.
counterparts for high-performance engineered application,
A highly aligned unidirectional preform with improved fiber packing of
with an objective to develop next generation environmentally elementary jute fiber was prepared by following the previous study.[21]
sustainable composite. In such technique, the single elementary fiber was separated via hand
combing of HA treated jute fiber, where heat and alkali treatment
ensures nearly 100% single fiber separation (Figure S10a–d, Supporting
Information). The alignment of such highly individualized fibers
4. Experimental Section was maintained by putting a both-sided tape at both ends of the tow
Materials: Field retted “Tossa white Jute” fiber was collected from (Figure S10d, Supporting Information). They were then dipped into
Bangladesh, cultivated in the northeast of Dhaka capital. Generally, the GO dispersions 30 min with M:L of 1:10 (Figure S11a,b, Supporting
fiber cultivation starts from summer and finishes at the end of rainy Information). After that, rGO-coated fibers were then hand sprayed with
season. The raw fiber bundles are commonly known as raw jute sliver epoxy compatible water-based sizing materials to confirm a dry non-
collected after dew retting under the water of a pond or a river where woven structure before hot press treatment (Figure S11c, Supporting
there is continuous flow of water (Figure S9a,b, Supporting Information). information). Finally, the coated fibers were hot press at 1 ton inch−2
The collected raw sliver contains ≈98–99% of technical fiber bundles pressure at elevated temperature of 120 °C for 30 min (Figure S12a,b,
and the rest of them are shives (the remainder of cortical tissues and Supporting Information). Preforms with untreated fiber were labeled as
impurities). Raw jute sliver has an average length of ≈2.9 m and diameter UT, heat alkali-treated jute fiber after individualization and compaction
of ≈0.06 mm, respectively. Sodium hydroxide (NaOH) was purchased as HA0.5, and rGO treated jute fiber preform with 0.25, 0.5, 0.75, 1,
as pellets from a commercial supplier, Fisher Scientific, UK. Graphexel and 5 mg mL−1 as rGO 0.25, rGO 0.5, rGO 0.75, rGO 1, and rGO 5,
Limited, UK kindly supplied the natural flake graphite. The average respectively.
lateral size of the flake was 50 mm. Sodium deoxycholate powder, Manufacturing of Composites: A vacuum assisted resin infusion
potassium permanganate (KMnO4), sulfuric acid (H2SO4, ≈99%), process (VARI) was used to manufacture rGO-coated composites
ammonia, poly(vinyl alcohol), poly(sodium 4-styrenesulfonate), sodium (Figure S12c, Supporting Information). A room temperature cured
hydrosulfite, and hydrogen peroxide (H2O2, ≈30%) were purchased from EL2 laminating resin and AT30 amine hardener were used in the VARI
Sigma Aldrich, UK. EPI-REZTM epoxy compatible water borne sizing process. UD jute fiber preforms were dried in an oven at 50 °C for 5 h to
(product no 7520-W-250) was purchased from Hexion, UK. S and E-glass ensure there was no moisture left in the fibers. Four layers of dried UD
were purchased from AGY, USA. A room temperature cured epoxy EL2 preforms were placed on a metal plate, which was previously cleaned
laminating resin and AT30 slow hardener were purchased from Easy with acetone and sprayed with PVA release agent on its surface. A peel
Composites, UK. AT30 is cycloaliphatic amine-based mixture which ply was used on the bottom and top side of the preform to ensure easy
forms a co-polymer with the expoxy resin to enable efficient curing. de-molding of composites. In addition, a mesh fabric was also placed
Synthesis of Graphene Oxide and Reduced Graphene Oxide: GO was on top to ensure even flow of resin during the infusion process. Finally,
prepared using a modified Hummers method as described elsewhere.[51] such arrangement was fully sealed with nylon plastic bag to ensure
80 mg GO was added to 160 mL deionized water (DI), and left for at negative atmospheric pressure inside the bag upon pumping. Resin and
least 30 min sonication to form a brownish dispersion of GO with a hardener were separately de-gassed for 30 min in a degassing chamber
concentration of ≈0.5 mg mL−1. After that, 500 mg PVA was added to of vacuum pump, and after that they were mixed and again de-gassed
GO dispersion with rigorous stirring. The GO dispersion with PVA was for 15 min to ensure there were no bubbles inside the resin. The pump
then moved to a round bottomed flask and placed into an oil bath. was then ran and ensured the bag was air-tight with no leakage. Finally,
1.2 gm of L-ascorbic acid and sufficient amount of NH3 was added the resin was infused inside the bag by using inlet pipe and maintained
to the dispersed solution to maintain the pH level from 9 to 10 while a constant flow of 1 mm s−1. Infused preforms were kept for 24 h inside
maintaining a rigorous stirring. The mixed solution was kept in a closed the bag at room temperature to ensure full curing of composites
chamber and heated at 90 °C for 24 h so that the mixture became black (Figure S12e,f, Supporting Information).
in color. To obtain the dispersion volume of 200 mL, DI water was Characterization: A digital optical microscope (Keyence VHX-500F, UK)
added to this dispersion. The resulted rGO was then thoroughly washed was used to quantitatively measure the diameter of fibers, microdroplet
to remove the residues and finally dispersed into DI water to obtain lengths of fiber/epoxy micro-composites, and cross-sectional image of
required concentrations. composites to observe fiber packing. Surface topography of untreated
Chemical Treatment and Graphene Materials Coating: Chemical and graphene treated jute fibers were analyzed by using a Philip XL30
treatment (alkali treatment) was used to improve the surface properties field emission gun SEM. Kratos axis XPS system and FTIR were used
of jute fiber. Untreated jute fibers of 30 cm length were prepared, to conduct the surface characterization of untreated and treated jute
thoroughly washed with DI water, and dried in an oven at 80 °C to fibers. Flake thicknesses were measured with a Dimension Icon (Bruker)
achieve a constant weight. Hot water treatment is one of the effective atomic force microscope. Raman spectra of graphene flakes were
ways of removing non-cellulosic materials. Therefore, the washed and collected by using a Renishaw Raman system equipped with a 633 nm
dried fiber was treated with warm water at 60 °C for 60 min, and then laser. A TA instrument (TGA Q5000, UK) was used to study the thermal
at 100 °C for 30 min (Figure S9c, Supporting Information). In this way, decomposition behavior of untreated and treated jute fibers from room
fiber weight was reduced by 6 wt% in comparison to untreated fiber. This temperature to 1000 °C in a nitrogen atmosphere at a constant heating
cleaned fiber was then treated with 0.5% NaOH solution, with a material rate of 10 °C min−1.
to liquor ratio (M:L) of 1:50. Alkali treatment together with hot water Tensile Testing of Elementary Fibers: ASTM D3822-01 standard was
treatment further reduced 6 wt% of the fiber. Alkali was used to dissolve followed to conduct the single fiber tensile test. Single elementary fibers
the hemicellulose, and this treated fiber was labeled as HA0.5. (40–50 mm in length) were manually separated from the fiber bundles.

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Single jute fiber was then placed and glued in a paper card frame Acknowledgements
(Figure 2a), and left for 24 h to ensure the full curing of the glue. Before
tensile testing, the diameter of the fiber was measured by horizontally The authors kindly acknowledge the funding from UKRI Research
placing them under the digital microscope. A total of five different England E3 funding (U.K.), European Research Council (ERC) Synergy
places were selected to determine the average diameter of the fiber. As Grant Hetero2D, and Engineering and Physical Sciences Research
prepared samples were kept in a standard laboratory atmosphere (≈55% Council, UK (EPSRC Grant No. EP/N010345/1, 2015). P.P. acknowledges
RH and ≈20 ± 2 °C) for at least 24 h. The tensile test of single fibers was the funding from the EPSRC Future Composites Hub (EPSRC Grant No.
conducted on a Zwick-Roell tensile testing machine (Zwick/Roell, UK) EP/P006701/1). The authors also kindly acknowledge Commonwealth
with a load cell of 20 N (Figure S13a, Supporting Information). A 20 mm Scholarship Commission, UK and the Government of Bangladesh
gauge length and 2 mm min−1 crosshead speed were selected as per for the Ph.D. funding of F.S. and S.A., respectively. The authors also
ASTM D3822-01 standard. Young’s modulus of the fibers was calculated acknowledge Dr Sean Butterworth and Bruno Pirollo form BAE Systems
from the slope of the stress–strain curve at 0.1–0.3% strain. for participating in the discussion on EMI shielding results, and Laura
Single Fiber Micro-Bond Test: A micro-bond test was carried out Clarke Oaten for the professional help and excellent support with the
to measure the IFSS by following the previously reported work graphics for this paper.
(Figure 2h).[20] Fiber and paper frame were prepared by following the
similar method as single fiber tensile test. In order to prepare micro-
droplet of resin on a single jute fiber, a single glass fiber strand was
used. The tip of the glass fiber was dipped into the previously mixed
Conflict of Interest
resin and hardener. A micro-droplet of resin was stuck on the tip of The authors declare no conflict of interest.
the glass fiber, and then carefully mounted on the jute single fiber. Two
droplets were placed in a single paper frame and left it overnight to cure
the resin with jute fiber. A digital microscope was used to measure the
diameter and embedded microdroplet length of the resin on jute fiber. A Authors Contributions
microvice, with one-sided rotating shaft with two sharp blades, was used
N.K. conceived, planned, and designed the study. F.S. prepared graphene-
to conduct the micro-bond test (Figure S13b, Supporting Information).
coated jute fibers under N. K’s guidance. F.S. developed, prepared and
A Zwick-Roell tensile testing machine (UK) was used with 20 N load
characterised jute fibre composites, and performed measurements,
cell at a crosshead speed of 0.25 mm min−1. 30 samples were tested for
and data analysis for those samples under P.P’s supervision. S.A.
each set and calculated the average IFSS. It was assumed that the force
developed, prepared, and characterized rGO and graphene dispersions,
generated during test to de-bond the interface of jute fiber and matrix
and performed XPS analysis of rGO and graphene-coated jute fibers
was uniformly developed and therefore, the following Equation (1) could
under supervision of K.S.N. and N.K. EMI shielding measurements were
be used to calculate the IFSS.
carried out and analyzed by M.Z. and N.K., respectively. N.K. performed
F analysis and discussed on sustainability and environmental impacts.
τ IFFS = (1) N.K. wrote the manuscript with inputs from F.S., S.A., K.S.N., P.P., and
π Dl e
M.Z. The supporting information was prepared by F.S. with inputs from
where, τIFFS is the IFSS, F is the maximum pull-out force, le is embedded N.K. All authors reviewed and approved the manuscript.
droplet length and D is the fibre diameter.
Mechanical Testing of the Composites: ASTM D3039 standard was
followed to carry out the longitudinal and transverse tensile test of
untreated and rGO-coated jute fiber/epoxy composites. A total of five Keywords
specimens (size: 250 mm × 15 mm) were prepared for testing each type
of composites. Glass fiber tabbing was used on each sample to ensure graphene, jute fibers and smart composites, natural fiber composites,
even stress development and avoid any premature failure. An Instron sustainability
5985 tensile testing machine (UK) was used, which was equipped with
100 kN load cell and a video extensometer to record the extension of Received: September 28, 2020
materials (Figure S13c,d, Supporting Information). The crosshead speed Revised: December 14, 2020
was kept 2 mm min−1 for this test. Young’s modulus, tensile strength, Published online: January 12, 2021
and failure strain for each sample were collected from the machine
exported datasheet.
Electro-Magnetic Interference Shielding Tests: A Vector network analyzer
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