Received: 16 May 2019 Revised: 2 August 2019 Accepted: 30 September 2019

DOI: 10.1002/pc.25410

REVIEW ARTICLE

Graphitic carbon nitride (g-C3N4) reinforced polymer

nanocomposite systems—A review

Sashivinay Kumar Gaddam1 | Ramyakrishna Pothu2 | Rajender Boddula3

1
LAMTUF Plastics Private Ltd, Hyderabad,
Telangana, India
Abstract
2
College of Chemistry and Chemical Research on polymer matrix-enhancement using a carbon nanomaterial as the high-
Engineering, Hunan University, Changsha, potential filler has attracted considerable attention to meet the increasing demand for
China
advanced polymer composites which show promising applications in a wide variety
3
CAS Key Laboratory of Nanosystem and
of fields. Graphitic carbon nitride (g-C3N4) is the most stable allotrope of carbon
Hierarchical Fabrication, National Center for
Nanoscience and Technology, Beijing, nitrides and its inherent electron-rich properties, basic surface functionalities, and
China hydrogen bond motifs make it a potential candidate in catalysis and in other fields.
Correspondence
This article reviews a new application of graphitic carbon nitride (g-C3N4) as a rein-
Rajender Boddula, CAS Key Laboratory of forcement material into polymer composites. It focuses on the enhancement of tribo-
Nanosystem and Hierarchical Fabrication, logical, thermomechanical, self-healing, anticorrosion, and flame-retardant properties
National Center for Nanoscience and
Technology, Beijing 100190, China. hybrid composite materials via the incorporation of g-C3N4 filler. The leading pur-
Email: research.raaj@gmail.com pose of this review is to stress the significance of g-C3N4 as a reinforcement material
in polymer composites.

KEYWORDS
epoxy composites, graphitic carbon nitride, polyimide, polymer composites, self-healing, tribological,
wood plastic

1 | INTRODUCTION oxide (GO), carbon nanotube (CNT), carbon black, graphite,

Synthetic polymers have taken a vital role in modern applica-
tions due to their advantages such as tunable properties, easy
processability, low cost, lightweight, high strength and stiffness,
resistance to chemicals, and physical degradation.[1–4] How-
ever, a major problem arises since most of these polymeric
materials suffer from the poor surface, thermal, mechanical, and
electrical properties.[5,6] The incorporation of a relatively small
quantity of organic and inorganic nanofillers has the potential to
dramatically improve those delicate properties of polymers.[7–9]
Thus, the investigation of nanofillers as reinforcing materials
has become ubiquitous in the field of polymer composites
which have diverse application in every sector of manufacturing
including aerospace, construction, automotive, marine, military,
sports, and biomedical industries.[10,11] Among the several rein-
forcing nanofillers, carbon nanomaterials (CNMs) comprise an
attractive and fascinating family including graphene/graphene
and carbon fiber (CF). Due to their extraordinary intrinsic
properties and ability to disperse in various polymer matrices,
CNMs have been widely used as reinforcing materials in
order to improve the thermomechanical,[12] barrier,[13,14]
conductivity,[15,16] corrosion resistance,[17,18] and flame-
retardant[19,20]performances of polymer composites.
Whenever a new member was discovered in the CNMs
family, such as fullerenes (1985), CNTs (1991), and graphene
(2004), a revolutionary development was observed in the field
of materials and polymer composites.[21] Unfortunately, even
having a long history, the potential value of graphitic carbon
nitride (g-C3N4) was not fully recognized until recent
decades.[22] Due to its chemical inertness, unrevealed structure,
and insolubility in all solvents, g-C3N4 has been forgotten for a
long time since its first discovery by Berzelius in 1834.[23]
However, the research works on g-C3N4 has been restimulated
in the early 1990s, based upon a theoretical prediction that

Polymer Composites. 2019;1–13. wileyonlinelibrary.com/journal/pc © 2019 Society of Plastics Engineers 1

2 GADDAM ET AL.
diamond-like β-C3N4 could have extremely high hardness
values.[24] The g-C3N4 is the most stable allotrope of carbon
nitrides at ambient atmosphere and its 2D aromatic tri-s-triazine
structure make this material possess high thermal and chemical
stability.[23] After the first successful demonstration of a novel
photocatalytic application of g-C3N4 for H2 evolution under
visible light irradiation,[25] g-C3N4 based photocatalysis has
become a very hot research domain. Many efforts have been
intensively focussed on the synthesis of g-C3N4 via the
annealing of nitrogen-rich organic precursors including
cyanamide,[26] dicyandiamide,[27] melamine,[28] urea,[29] and
thiourea.[30] Due to its tunable and high electron-rich structure
with a medium band gap of ca. 2.7 eV,[31] g-C3N4 has
become a next-generation, nontoxic, earth-abundant, low cost,
and visible-light-active catalyst in the field of solar energy con-
version, water splitting for H2 evolution, sensing, imaging,
organic synthesis, and CO2 reduction for environmental
purification.[24,32]
Many review articles can be found mainly focusing on
the description of several interesting applications of g-C3N4
in catalysis and the reasons why it has been used for such
applications. However, unlike on its heterogeneous catalyst
applications, no review article has been presented on the
reinforcement effect of g-C3N4 in polymer matrix till date.
This review article aims to highlight the progress and
provide a good source of literature on this trending research
topic.
2 | STRUCTURE OF g-C 3 N 4
The graphitic phase is more stable among the several existed
allotropes of carbon nitrides at ambient conditions.[33]
Inspired by the graphite configuration, triazine units (C3N3)
had been regarded to be the elementary building blocks of g-
C3N4. However, tri-s-triazine (heptazine, C6N7) structure,
which is structurally relevant to the melon structure, is more
energetically favored building block than triazine.[34]The
calculation based on the density-functional theory reveals
that tri-s-triazine structure is 30 kJ mol−1 more stable.[35]-
Figure 1 shows the triazine and tri-s-triazine tectonic units
which differ in their stability and sizes of the nitride pores.
Both structures are cross-linked by trigonal nitrogen atoms
to constitute potential allotropes of g-C3N4.
3 | MORPHOLOGY OF g-C3N4
Because of its immense applications in several fields, the
structural modifications of g-C3N4 are literally exploding
every day, to attain desired structure and morphology which
strongly relate to its final applications. Based on the decrease
F I G U R E 1 A, Triazine and B,
tri-s-triazine structures of g-C3N4 with
possible multiple surface
functionalities. Adapted with
permission from the American
Chemical Society and John
Wiley & Sons [Color figure can be
viewed at wileyonlinelibrary.com]
GADDAM ET AL. 3

of dimensions, we can classify the architectures of g-C3N4
as following.
3.1 | Bulky g-C3N4
Bulk g-C3N4 is a standard material for comparison and can
be synthesized by the thermal condensation of a variety of
nitrogen-rich precursors such as cyanamide, dicyandiamide,
melamine, thiourea, or urea. Bulk g-C3N4 usually possesses
relatively low surface area (10 m2 g−1), poor water solubil-
ity, slow reaction kinetics, and zero photoluminescence char-
acteristics in solvents.
3.2 | 3D porous structure
g-C3N4 with a porous structure is more attractive and effi-
cient because it can afford the desirable combination of wide
internal reactive surface area and straightforward molecular
transportation. The mesoporous g-C3N4 usually synthesized
through the template-induced method and the size and mor-
phology of pores can be adjusted by altering the sampling
selection.
3.3 | 2D nanosheets
g-C3N4 has a typical graphite-like layered structure with
weak van der Waals interactions across the layers. Hence,
similar to the successful exfoliation of graphene from bulk
graphite, exfoliation of ultrathin g-C3N4 nanosheets
(NS) from bulk g-C3N4 is also possible. The exfoliation usu-
ally takes place in a solvent medium with surface energy
matching with g-C3N4 and the strong repulsions among g-
C3N4 NS endow them with high stability in dispersion
medium for several months. Due to the extended surface
area with a 2D architecture, g-C3N4 NS exhibit distinct
physical features and prosperous electronic characteristics.
3.4 | 1D nanorods/nanotubes
By virtue of large aspect ratio, high surface area, smooth
mass transportation, and light-harvesting properties, nano-
structured 1D g-C3N4 hold good promise for the potential
optoelectric and electrochemical performances.
3.5 | 0D quantum dots
As a nanostructure with the size is less than 10 nm, g-C3N4
quantum dots (QDs) possess bright fluorescence, water solu-
bility, and nontoxicity which making them promising candi-
dates in place of typical semiconductor QDs. Unlike the
graphene and carbon QDs, g-C3N4 QDs have the advantage
of both electron-rich and nitrogen-rich properties and basic
surface functionalities as well.

FIGURE 2 A, TEM images of bulk g-C3N4. Reproduced with permission from the American Chemical Society. B, TEM of mesoporous g-
C3N4. Reproduced with permission from the Royal Society of Chemistry. C, TEM image of g-C3N4 NS. Reproduced with permission from John
Wiley & Sons. D and E, TEM images of g-C3N4 nanotubes. Reproduced with permission from the Royal Society of Chemistry. F and G, TEM of g-
C3N4QDs and their diameter distribution. Reproduced with permission from Elsevier Ltd. TEM, transmission electron microscopy [Color figure can
be viewed at wileyonlinelibrary.com]
4 GADDAM ET AL.
Figure 2 shows the transmission electron microscopy
(TEM) of the all above-mentioned architectures ofg-C3N4
illustrating the difference between their nanostructures.
4 | S Y N T H E T I C ME T H O D S O F
g-C 3 N 4
Since the efficiency of g-C3N4 in the area of photocatalysis
and many other fields had been known, various synthesis
methods and techniques had been induced such as thermal
condensation, solvothermal, chemical vapor deposition,
polymerization, microwave-assisted, and hydrothermal
method, and so on. Based on the synthesis technique, differ-
ent types of nitrogen-rich compounds can be used as precur-
sors such as cyanamide, dicyandiamide, melamine, urea, and
thiourea. Among the all above-mentioned methods, thermal
condensation of nitrogen-rich precursors is considered to be
the efficient synthesis strategy due to its simple and cost-
effective nature and earth-abundant precursors.
Bulk g-C3N4 usually synthesized by thermal condensation
of a variety of precursors between 400
C and 600
C. Because
of the graphitic layered structure, bulk g-C3N4 obtained by
direct polycondensation method usually possesses a lower
surface area. The reduction of the condensation temperature
may promote the surface area of the material due to the low
aggregation. During the thermal treatment process, the color
changed from white (precursor) to light yellowish (500
C)
and then dark orange (650
C).[25,36]
3D porous g-C3N4 had a great potential in photocatalysis
due to its high surface area (up to 830 m2 g−1) and larger
porosity (up to 1.25 cm3 g−1). Template-induced method is
a well-known method for the fabrication of porous g-C3N4
architecture. “Hard template” method has been widely used
for the synthesis of porous g-C3N4 through nanocasting/rep-
lication of mesoporous silica matrices.[37] In a typical proce-
dure, commercially available silica template and organic
precursor were mixed in an aqueous solution. After the com-
plete removal of water, the resulting composite material was
heated in a capped crucible for 4 hours at 550
C to condense
the precursor into polymeric C3N4. After removing the silica
template by NH4HF2 solution, porous g-C3N4 could be
obtained with the improved surface. By using the hard
templating strategy, the surface area and total pore volume
of g-C3N4 can be controlled by simply adjusting the weight
ratio of precursor to silica template.[38,39] In addition, synthe-
sis of porous g-C3N4 via “soft template” method, in which
surfactants or ionic liquids used as soft templates, is of
growing interest.[40,41] However, the obtained porous g-
C3N4 is black instead of yellow due to the contamination by
residual carbon coming from the template polymer.
2D g-C3N4 NS are usually obtained by two main synthetic
approaches: one is top-down approach and another one is
bottom-up approach. Chemical etching and ultrasonication
assisted liquid exfoliation of layered g-C3N4 solids into free-
standing NS are the two main technologies involved in the
top-down method. The anisotropic assembly of organic mole-
cules in a 2D manner via template-induced method, hetero-
atom mediated method, and additive mediated methods have
been employed for the bottom-up approach.[42]
Hollow 1D g-C3N4 nanostructures (nanorods/nanotubes)
have been developed by various methods including (a) direct
heating of nitrogen-rich precursors without any template,[43]
(b) template-induced methods involving sulfur-mediated self-
templating[44] and using templates such as chiral silica
nanorods,[45] SBA-15,[46]diatom frustules,[47] and porous
anodic aluminum oxide membrane,[48] (c) solvothermal,[49]
and (d) hydrothermal methods.[50]
Similar to the 2D g-C3N4 NS, fluorescent g-C3N4 QDs
have also been synthesized by top-down and bottom-up
approaches. Chemical etching and exfoliation of bulk g-
C3N4 are the key strategies in top-down approach to obtain
g-C3N4 QDs.[51,52]Hydrothermal and microwave heating
methods are the common strategies for the synthesis of g-
C3N4 QDs through bottom-up approach.[53,54] g-C3N4 QDs
also prepared by chemical tailoring strategy using NH3 and
H2O2 as controllable chemical scissors.[55]
5 | g-C 3 N 4 AS A REINFORCING
MATERIAL F ORPOLYMER
COMPOSITES
Because of its metal-free and lightweight nature, g-C3N4
exhibits higher mechanical strength. In a study, the shear
and bulk elastic moduli of the g-C3N4 were examined using
Brillouin light scattering and X-ray Raman scattering tech-
niques.[56] The estimated shear and bulk elastic moduli of
the g-C3N4 are of about 21.6 and 63.1 GPa, respectively. In
another study, the elastic modulus and tensile strength of the
two different structures (triazine and heptazine) of the g-
C3N4 were examined through uniaxial tensile simula-
tions.[57] Triazine g-C3N4 structure can exhibit an elastic
modulus of about 320 ± 5 GPa and tensile strength of
around 40 GPa. On the other hand, heptazine g-C3N4 struc-
ture can present elastic modulus of about 210 ± 5 GPa and
tensile strength of around 25 GPa. These studies suggest that
g-C3N4 is well suited as a flexible and strong 2D material
for reinforcement of properties of polymeric materials.
6 | g-C 3 N 4 R E I N F O R C E D
POLYIMIDE COMPOSITES
Polyimide (PI) is a well-known high-performance polymeric
material, that exhibits a wide range of applications in the field
GADDAM ET AL.
of electrical and electronics due to its excellent comprehensive
properties including high mechanical strength, low thermal
expansion coefficient, low dielectric constant, and good chemi-
cal and thermal resistance.[58,59] However, pure PI material had
certain shortcomings including low wear resistance, low tensile
strength, and a high coefficient of friction (COF),[60,61] which
made them unsuitable for the use alone in the modern electron-
ics and tribo-engineering materials. In this case, many studies
have been carried out on the structural modifications of PIs,
using the various carbon-based fillers such as CNTs,[62] CF,[63]
graphite,[64] graphene,[65] and GO[66] to develop the PI/carbon
nanocomposites. However, the reinforcing effect of g-C3N4 on
tribological and dielectric properties of the PI-based compos-
ites has been less investigated.
The effect of g-C3N4 on tribological properties of PIs was
investigated by Lin and co-workers.[67] In brief, the g-C3N4
powder is mixed with commercially available thermoplastic
PI powder (YS20) at different weight ratios (2.0, 5.0, 10, 20,
and 50 wt%) using ethanol as solvent. After the evaporation
of the solvent, PI tablet samples were prepared via hot press
molding under a pressure of 15 MPa at 300
C temperature.
The samples were also hardened at 230
C for 4 hours. The
thermal decomposition temperature (Td) of PI/g-C3N4 com-
posites gradually increased with increase in filler content. The
COF values and wear rate were gradually decreased up to
10 wt% of filler loading level and then increased further incre-
ment in filler content (Figure 3). This could be attributed
mainly due to the fact that the g-C3N4 filler was reduced the
roughness of counter face at lower filling levels up to 10 wt%
and its self-lubricating property facilitated to the generation of
the continuous transfer film on the mating surface during slid-
ing contact and hence reduce the COF values. On the other
hand, the filler particles were aggregated at higher loading
levels and weakened the interfacial bonding strength between
filler and polymer matrix. Hence, the transfer film was
F I G U R E 3 A, COF of composites as a function of the g-C3N4 content at different normal load and B, wear rate of the composites as a
function of the g-C3N4 content. Reproduced with permission from John Wiley & Sons. COF, coefficient of friction [Color figure can be viewed at
wileyonlinelibrary.com]
5
destroyed due to internal defects and resulted in severe abra-
sive wear and enhanced COF values.
Chunjian et al. studied the wear-resistant performance of
g-C3N4 reinforced thermosetting polyimides (TPI-1) and com-
paratively evaluated with neat TPI from room temperature to
350
C.[68] The TPI was developed by polycondensation
between s-BPDA and 4,40 -oxydianiline or 3,40 -oxydianiline
and reinforced by 0.5 wt% of g-C3N4 which was produced by
the calcination of melamine. Because of the tight interlayer
H-bonds, the filler g-C3N4 has exhibited a negative effect on
COF of TPI-1 which is higher than the neat TPI and the
values were decreased with increase in temperature
(Figure 4A). In addition, the formation of transfer film on the
counterface and the significant sharing of the load with high
E-modulus and hardness of the g-C3N4 in the contact surface
can avoid the direct contact between resin and counterpart.
Hence, TPI-1 exhibited low wear rate than neat TPI with
enhanced temperature and the lowest wear rate of TPI-1 is
7.29 × 10−7 mm3/N m at 350
C (Figure 4B).
Weichen et al. studied the properties of PI composite
films reinforced by g-C3N4.[69] Initially, g-C3N4 was synthe-
sized through the thermal condensation of DICY
(dicyandiamide) at 600
C. The precursor of PI, polyamic
acid (PAA) was synthesized by the reaction of PMDA with
BAPP in the DMAC solvent at the ice-cold condition for
12 hours. The suspension of g-C3N4/DMAC was added to
the PAA/DMAC solution and continuously stirred for
6 hours to result the g-C3N4/PAA solution. The composite
films were developed via curing of g-C3N4/PAA at high
oven temperatures and the concentration of the g-C3N4 in
the cured composite films is 1.0, 2.0, 4.0, and 8.0 wt%. The
composite films displayed optical transparency up to 4.0 wt
% filler loading and the films become totally opaque after
4.0 wt% of g-C3N4 loading. The composite films exhibited
high tensile strength compared with those of the neat PI film
6 GADDAM ET AL.
F I G U R E 4 A, COF and B, wear rate of g-C3N4 reinforced TPI composites as a function of the temperature. Reproduced with permission from
Elsevier Ltd. COF, coefficient of friction; TPI, thermosetting polyimides [Color figure can be viewed at wileyonlinelibrary.com]
and the maximum tensile strength (102 MPa) was achieved
with 2.0 wt% of g-C3N4 loading. The surface functional
groups (−NH/NH2) of the g-C3N4 covalently linked with
−COOH groups of PAA along the polymer chains and favor
the stress transfer from the polymer matrix to the filler parti-
cles, leading to the enhancement in the tensile strength.
However, at higher filler loading of over 2.0 wt%, the filler
particles agglomerated in the PI matrix and cause the deteri-
oration in the tensile strength. The thermal decomposition
temperatures (Td) of the composite films gradually increased
with increase in filler content and the values are higher than
the neat PI film. The dielectric constant (εr) and loss tangent
(tan δ) of the composite films were gradually increased with
increase in filler content and the film with 8.0 wt% of g-
C3N4 content exhibited high εr (5.42) and tan δ (0.00657) at
the sweep frequency of 10 kHz.
Jeetenda et al. studied the thermal and anticorrosion
(AC) properties of the g-C3N4 reinforced electroactive pol-
yimide (EPI) composites.[70] Thermal decomposition of mel-
amine at 550
C for 2 hours, results in g-C3N4 particles. The
precipitate of BSSA and N-phenyl-p-phenylenediamine in
water was dried at 60
C for 12 hours. The resulted
oligoaniline was dissolved in the solution of NMP + 1 M
HCl, and mixed with 1,4-phenylenediamine and g-C3N4.
The reaction mixture was turned into a blackish green pre-
cipitate in the presence of 1 M ammonium persulfate which
further heated over 180
C for 12 hours to get the final
EPI/g-C3N4 composites. The amount of g-C3N4 in the EPI
composite is ranged from 2.0 to 5.0, 10, and 20 wt%. The
thermal decomposition temperatures (Td) of the EPI/g-C3N4
gradually increased with increase in g-C3N4 content. The
composite material and a PU binder (DuPont) were mixed in
the presence of an activator fast (256S, DuPont) and the final
mixture was spin-coated on three different metal surfaces
including 316L SS, carbon steel and AA6061 to study the
corrosion resistance of EPI/g-C3N4 composites. The icorr
values obtained from the potentiodynamic polarization
method revealed that EPI/g-C3N4 (10 wt%) coated 316L SS,
and carbon steel and EPI/g-C3N4 (5 wt%) coated AA6061
exhibited good corrosion resistance. The aggregation of g-
C3N4 particles at a higher level of loading decreases the AC
property of composites.
7 | g-C 3 N 4 R E I N F O R C E D
POLYURETHANE COMPOSITES
Polyurethane (PU) is an important and very useful commer-
cial polymer that can be prepared via polyaddition reaction
between a diisocyanate and a petro-based macro diol or a
renewable polyol. PU's have attracted considerable attention
due to their potential broad applications such as coatings,
adhesives, sealants, elastomers, and foams.[71–74] However,
conventional PU's are mostly linear thermoplastics and have
poor surface, thermomechanical, and barrier properties.
These factors limit the commercial applications of PUs in
many fields. In order to overcome this, several methods have
been introduced, for example, reinforcing the PU matrix
with CNMs.[75,76] However, compared with other CNMs,
the reinforcement effect of g-C3N4 on properties of PUs has
been less investigated.
The combustible nature of PU leads to an increase in fire
risks and the releasing of toxic gases when PU exposed to
flame, have an adverse effect on human health and the envi-
ronment.[77] The concern regarding halogen-free fire retar-
dant additives such as ammonium polyphosphates (APP),
aluminum hypophosphites (AHPi), and CNMs have been
gradually increased in the field of flame-retardant PU appli-
cations.[78,79] The combinatorial flame-retardant application
of AHPi and g-C3N4 in thermoplastic PU was investigated
by Yongquian and co-workers.[80] Three different aluminum
hypophosphite/g-C3N4 hybrid fillers (CAHPi) were
GADDAM ET AL.
developed through the reaction of g-C3N4 with
hypophosphorous acid and aluminum salt solution
(Al2[SO4]318H2O). The weight ratio of g-C3N4 to AHPi
varied from 5.0 to 10 and 20 wt% and the developed hybrid
fillers denoted as CAHPi-5, CAHPi-10, and CAHPi-20,
respectively. The commercially available TPU (85E85) was
blended with 10 wt% of CAHPiχ (where χ was 5.0, 10, and
20) at 180
C and hot pressed under pressure of about 5.0 to
20 MPa. TPU composites exhibited lower thermal stability
and higher char yield than that of neat TPU with the incorpo-
ration of hybrid filler and the values increased with increase
in g-C3N4 content. The thermal degradation of AHPi which
is catalyzed by g-C3N4 leads to lower thermal stability and
higher char yields of composites. Furthermore, g-C3N4 pre-
vents the thermal oxidation of AHPi and induced AHPi to
release the free-radical capture agents and hence, the flame-
retardant properties of TPU composites gradually increased
with increase in g-C3N4 content. The TPU/CAHPi-20 com-
posite exhibited high fire resistance with lower heat release
rate (HRR, 622 kW m−2), total heat release (THR,
73.0 MJ m−2), smoke production rate (SPR, 0.05 m2 s−1),
total smoke production (TSP, 696.9 m2 m−2), fire growth
index (FGI, 4.013 kW m−2 s−1), and higher fire performance
FIGURE 5 A, HRR; B, THR; C, SPR; D, TSP curves of TPU and its nanocomposites during combustion. Reproduced with permission from
MDPI AG. HRR, heat release rate; SPR, smoke production rate; THR, total heat release; TSP, total smoke production [Color figure can be viewed at
wileyonlinelibrary.com]
7
index (FPI, 0.104 m2 s−1 kW−1). The curves of HRR, THR,
SPR, and TSP are illustrated in Figure 5.
Self-healing materials have been intensively investigated
over the past decade for applications which are prone to dam-
age, especially in the area of anticorrosion coatings.
Depending on the nature of the healing process, self-healing
coatings classified into two different classes: nonautonomous
and autonomous. The nonautonomous self-healing coatings
contain different covalent dynamic bonds including Diels-
Alder cycloaddition bonds, disulfide bonds, alkoxyamine
bonds, imine bonds, and azide-alkyne click linkers.[81] These
coatings require the input of external energy, like heat or UV-
light for the healing process and this could be limiting their
operation at ambient conditions. On the other hand, autono-
mous coatings loaded with microcapsules containing the
healing agents and the catalyst for healing polymerization.[82]
These coatings do not require any additional external trigger
and the detection of the damage as well as the repair proceeds
autonomously within the coating structure as presented in
Figure 6. However, autonomous self-healing coatings also
had some disadvantages such as (a) one-time healing process
due to the loss of capsule upon healing; (b) only micro-cracks
can repair due to the insufficient healing agent.[83] More
8 GADDAM ET AL.
recently, room temperature, autonomous self-healing supra-
molecular soft materials have been constructed based on
hydrogen bonds,[84] host-guest interactions,[85] and metal-
ligand bonds.[86] However, all these supramolecular motifs
impart the poor mechanical properties to the material and are
no better to adopt for the applications of self-healable AC
coatings.
Considering the all above aspects, Jian Hua et al. devel-
oped autonomous self-healing polyurethane-urea (PUU)
elastomer reinforced by g-C3N4 NS that possess a combina-
tion of excellent mechanical strength, high fracture tough-
ness, corrosion resistance, and room temperature self-
healable capacity.[87] The calcination of melamine results
the g-C3N4 powder which exfoliated into ultrathin NS via a
liquid exfoliation method. The reaction of tolylene
2,4-diisocyanate terminated polypropylene glycol (PPGTD)
with adipic dihydrazide (AD) results in the PU elastomer
which further cross-linked with g-C3N4 NS via nucleophilic
addition and rearrangement reactions to develop the PUU-g-
C3N4 NSs elastomeric composite material. The amount of g-
C3N4 NS in the composite elastomer was varied from 0.5 to
1.0 and 2.0 wt% and the hydrogen bonds between rigid
nanofiller and PUU matrix, serving as reversible sacrificial
bonds, enhances the tensile strength of the composite coat-
ing. The tensile strength values are gradually increased with
increase in g-C3N4 NS content and the value is highest for
PUU-g-C3N4 NS-2.0 (10.02 MPa). The self-healing effi-
ciency was examined using PUU-g-C3N4 NS-1.0 via tensile
tests at various healing times. The cut specimen after
24 hours healing under ambient conditions exhibited a ten-
sile strength of 6.10 MPa which is about 80.3% of its origi-
nal value. The self-healing efficiency can be attained by
FIGURE 6 Schematic of self-
healing process of autonomous coating
(light orange); A, loaded with
microencapsulated catalyst (yellow) and
healing agent (blue) coated on a metallic
substrate (gray); B, damage to the coating
layer releases catalyst and healing
agent; C, mixing of catalyst and healing
agent in the damaged region; D, damage
healed by cross-linked network structure
via healing polymerization. Reproduced
with permission from John Wiley & Sons
[Color figure can be viewed at
wileyonlinelibrary.com]
high mobility of elastomeric PUU chains, facilitated the con-
tact of dissociated hydrogen bonds on the fractured surface.
The PUU-g-C3N4 NS-1.0 was coated on aluminum alloy
(AA) 2024 by drop-casting method, and the coating was
exhibited good tear strength (45 ± 4 kN/m), hardness
(11.19 MPa), dolly adhesion test (3.8 ± 0.5 MPa), and
impact strength (>320 in. lbs). The filler g-C3N4 lowers the
penetration rate of corrosive species and also reduces the
moisture sensitivity of supramolecular hydrogen-bonded
PUU coating. Hence, the self-healing function of PUU-g-
C3N4 NS-1.0 AC coating resulted in its enhanced corrosion
resistance even under high humidity condition. The covalent
interaction of g-C3N4 with PUU matrix and the self-healing
process of PUU coating are illustrated in Figure 7.
Liao et al. examined the reinforcement effect of g-C3N4
on the thermomechanical properties of UV-curable water-
borne silicone PU-acrylate dispersions (Si-PUDA).[88] The
ultrasonic dispersion of different amounts (0.25, 0.50, 1.0,
and 2.0 wt%) of g-C3N4 into Si-PUDA results in the Si-
PUDA/g-C3N4 composites. From the experimental results, it
was cleared that, the homogeneous dispersion of filler into
the PUD matrix was achieved up to 1.0 wt% of filler loading
and further increment in filler content cause the agglomera-
tion (Figure 8). The homogeneous dispersion of g-C3N4
facilitates the enhancement in cross-linking network density
and hence the UV cured Si-PUDA/g-C3N4-1.0 composite
exhibited high tensile strength (12.8 MPa), pencil hardness
(4H), water resistance, and thermal stability. However, all
these properties decreased for Si-PUDA/g-C3N4-2.0 com-
posite due to the lower crosslink network density and phase
separation which could arise due to the agglomeration of
filler.
GADDAM ET AL. 9

F I G U R E 7 Schematic illustration of PUU-g-C3N4 NS composites A, PUU matrix with supramolecular multiple hydrogen bonds and the
covalent interaction of g-C3N4 with PUU matrix, and B, self-healing process of PUU-g-C3N4 NS composites at room temperature. Reproduced with
permission from the Royal Society of Chemistry. PUU, polyurethane-urea [Color figure can be viewed at wileyonlinelibrary.com]

FIGURE 8 TEM micrographs of

PUD filled with A, 0.25 wt%; B, 0.50 wt
%; C, 1.0 wt%; D, 2.0 wt% of g-C3N4.
TEM, transmission electron microscopy

8 | g - C 3 N 4 REINFORCED EPOXY superior mechanical properties to the composite materials

AND WOOD-PLASTIC COMPOSITES
Epoxy resins are the most common matrices for high-
performance CF reinforced polymer composites due to their
high cross-linking network structure which imparts the
including high modulus, high fracture strength, and solvent
resistance.[89] However, the interphase properties of CF
reinforced epoxy composites including resistance to delami-
nation and impact damage have a crucial influence on their
ultimate performance.[90] Various strategies have been
10
employed to improve the interfacial compatibility between
CF and epoxy resin. One of those important approaches is
additional reinforcement of epoxy matrix with interphase
containing nanomaterials like CNTs, graphene/GO, ZnO
nanowires, and TiO2 nanorods to construct the interphase
between CF and epoxy resin and to create the multiscale
hybrid composites. The effect of g-C3N4 on interfacial com-
patibility between CF and epoxy resin was investigated by
Bo Song and co-workers.[91] The in situ synthesis of g-C3N4
on CF surface was proceeds through dip-coating of CF sur-
face with a urea-ethanol solution followed by calcination at
550
C. The cured epoxy resin was reinforced with surface
modified CF (CF-g-C3N4) and the laminates were fabricated
via a vacuum bag-pressure molding method. The high sur-
face energy (59.49 mJ/m) and low water contact angle
(48.81
) values of CF-g-C3N4 effectively enhanced the inter-
facial compatibility between CF and epoxy resin and thus
improves the interfacial properties of composites. The com-
posite laminates made of CF-g-C3N4 exhibited high inter-
laminar shear strength (ILSS, 72.09 MPa),interfacial shear
strength (IFSS, 73.41 MPa), tensile strength (675.31 MPa),
bending strength (795.13 MPa), total absorbed energy of
GADDAM ET AL.
FIGURE 9 SEM micrographs
of A, g-C3N4; B, WPC; C, WPC/g-C3N4-
1.0; D, WPC/g-C3N4-3.0; E, WPC/g-C3N4-
5.0; F, WPC/g-C3N4-10. SEM, scanning
electron microscopy; WPC, wood-plastic
composites
impact (1.78 J), Tg (121.34
C) and low degradation in ILSS
during hydrothermal aging test (18.89%) than the laminates
made of neat CF and this could arise due to the increased
mechanical interlocking and chemical bonding in the inter-
phase formed during surface modification of CF with
g-C3N4.
Wood-plastic composites (WPC) are typically comprised of
natural plant fiber or wood flour (WF) in a thermoplastic resin
matrix-like polyethylene, polypropylene (PP), polyvinyl chlo-
ride, polystyrene, and so on, have been used as sustainable
green-composites in automotive and construction applica-
tions.[92] However, the highly hydrophilic nature of the ligno-
celluloses materials in WF leads to the moisture absorption of
the WPC resulting in debonding fibers and degradation of the
fiber-matrix interphase. Introduction of nanofillers is one of the
effective approaches to improve the physical and mechanical
properties of WPC. Bingrong et al. examined the
thermomechanical and water absorption properties of g-C3N4
reinforced PP based WPC.[93] The composite material was
developed through the mixing of g-C3N4 (1.0, 3.0, 5.0, and
10 wt%), WF, PP, stearic acid, and maleic anhydride grafted
PP using a twin-screw extruder. The experimental results
GADDAM ET AL.
revealed that a better homogenous dispersion of g-C3N4 filler
was achieved at a lower level of loadings up to 3.0 wt% and
beyond that limit filler particles agglomerate within the resin
matrix (Figure 9). Because of this, the lower level of filler load-
ings facilitates the better interfacial interactions between the
WF and resin matrix and leads to the enhancement in surface
and mechanical properties of WPC. On the other hand, a higher
level of filler loadings (5.0 and 10 wt%) creates more voids and
crack fractions during the compounding process which dis-
abled effective stress transferring from the matrix to fibers and
hence, reduce the surface and mechanical properties of WPC.
The WPC/g-C3N4-1.0 composite exhibited low water absorp-
tion and high flexural strength and the WPC/g-C3N4-3.0 com-
posite exhibited high tensile strength and Izod impact strength.
9 | CONCLUSIONS AND OUTLOOKS
The current review article summarizes the recent studies on the
reinforcement effect of g-C3N4 on tribological, thermo-
mechanical, and surface properties of different polymer com-
posites. It is observed that all the aforementioned properties
dramatically improved by the introduction of a small quantity
of g-C3N4. Most of the studies showed the agglomeration of
filler at a higher level of loadings which diminishes the proper-
ties of final composites. However, there are still many chal-
lenges to explore the full potential of this material as
reinforcement filler. Due to the incomplete polycondensation,
the g-C3N4 which is prepared via calcination method usually
suffers from the low surface area and exhibits poor perfor-
mance as reinforcement material at higher loading levels. Thus,
the search for a better procedure to develop the g-C3N4 with
improved surface area and structural stability is of crucial
importance. Furthermore, the exploration of methods for sur-
face functionalization of g-C3N4 is most crucial to improve its
reinforcement efficiency for the high-end composites applica-
tions. Overall, g-C3N4 represents a promising reinforcement
material with intrinsically superior properties and more techno-
logical breakthroughs in the field of polymer composites can
be expected soon.
ACKNOWLEDGMENT
Sashivinay Kumar Gaddam acknowledges the LAMTUF
Plastics management for their permission to publish this work.
O R C ID
Sashivinay Kumar Gaddam https://orcid.org/0000-0001-
9826-9515
Ramyakrishna Pothu https://orcid.org/0000-0002-5806-
9583
Rajender Boddula https://orcid.org/0000-0001-8533-3338
11
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