Journal of Environmental Chemical Engineering 10 (2022) 107260

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Journal of Environmental Chemical Engineering

journal homepage: www.elsevier.com/locate/jece

Emerging trends in the application of carbon-based materials: A review

Abisola Opeyemi Egbedina a, *, 1, Oladotun Paul Bolade b, 3, Ugochukwu Ewuzie c, 4,
Eder C. Lima d, *, 2
a
Department of Chemistry, Faculty of Science, Oduduwa Road, University of Ibadan, Nigeria
b
Department of Petroleum Chemistry, American University of Nigeria, Yola, Nigeria
c
Analytical Chemistry Unit, Department of Pure and Industrial Chemistry, Abia State University, PMB 2000 Uturu, Nigeria
d
Institute of Chemistry, Federal University of Rio Grande do Sul (UFRGS), Porto Alegre, RS ZIP 91501–970 , Brazil

A R T I C L E I N F O A B S T R A C T

Editor: Vítor Jorge Vilar Climate change, environmental pollution, and the need for cleaner alternative energy sources have opened
several areas of research interest. Carbon-based materials (CBMs), in all their versatility, have shown the po­
Keywords: tentials to be applied in these areas and more, and so far, the results are promising. CBMs possess excellent
Graphene mechanical, electrical, thermal, optical, and chemical properties, which have prompted significant research
Biochar
interest in various fields of application. However, as their uses increase by the day, there is a need to track their
Biomedical engineering
destiny in the environment and update their negative impacts on cellular compartments and biological systems.
Energy storage
Water purification This process will develop some guidelines for producing and using CBMs or their end-used products to reduce
Carbon-based materials these negative impacts worldwide. This review article provides some major historical evolution of various CBMs
and their emerging applications in water purification, clean energy conversion and storage, and biomedical
engineering. It also describes the fate of CBMs in the environment and their toxicity to humans and other living
organisms. Finally, the future trends in research and the challenges in developing CBMs have been highlighted.

1. Introduction [5–7]. They possess remarkable electrical conductivity [8], ultrahigh

The search for materials with superior properties tailored to meet the
specific needs of key industrial applications has opened up new areas of
research interest. It is at the core of recent research activities in medi­
cine, science, and engineering [1,2]. In order to find applications in
these fields, these materials are required to possess enhanced structural,
electronic, and optical properties that will boost their functionalities for
specific applications [3].
Carbon-based materials (CBMs) have received attention because of
their significant role in the development of materials science [4]. These
materials include both the traditional carbon materials, such as acti­
vated carbon and biochars, and the new range of CBMs such as graphene
and its derivatives (graphene oxide, reduced graphene oxide, and
functionalized graphene nanosheets), single- and multi-walled carbon
nanotubes (CNTs), carbon nanofibre (CNF), fullerenes, and carbon dots
optical [9], thermal and mechanical properties [10], chemical stability
[11], high surface area, low cost [12], and highly developed and tunable
porosity [13]., These characteristics have made them attractive for use
in a wide range of processes, including water purification [14], catalysis
[15], oxygen reduction reactions [8], clean energy conversion and
storage, polymer reinforcement [16], solar steam generation [17],
biomedical engineering [11], advanced information encryption [13],
and CO2 capture [18].
Despite these numerous benefits of CBMs, toxicity effects through
occupational exposure to workers during production and usage or
leaking into the environment are expected [19]. Therefore, several
studies have explored the synthesis of these materials, particularly from
environmentally benign biomass, and their use in various applications
[20–23]. However, since the first production and application of CBMs
some thousands of years ago, more and more applications have been

* Corresponding authors.
E-mail addresses: ao.egbedina@ui.edu.ng (A.O. Egbedina), oladotun.bolande@aun.edu.ng (O.P. Bolade), ewuzieug@gmail.com (U. Ewuzie), eder.lima@ufrgs.br
(E.C. Lima).
1
https://orcid.org/0000–0002-8589–3025
2
https://orcid.org/0000–0002-8734–1208
3
https://orcid.org/0000-0001-9783-8376
4
https://orcid.org/0000-0003-3975-0370

https://doi.org/10.1016/j.jece.2022.107260
Received 16 October 2021; Received in revised form 28 December 2021; Accepted 22 January 2022
Available online 25 January 2022
2213-3437/© 2022 Elsevier Ltd. All rights reserved.
A.O. Egbedina et al.
found for the traditional and new range of CBMs, so much so that
nano-based products have had a 30-fold increase between 2011 and
2015 [24]. In addition, comprehensive reports tracing the evolution and
applications of CBMs together with their fate and toxicity are scarce.
Therefore, in this review, we focus on presenting the historical
advancement of CBMs, including graphene and its derivatives, biochars,
activated carbons, fullerenes, carbon nanotubes, and graphitic carbon
nitride. We then present their recent applications in water purification,
clean energy conversion and storage, and biomedical engineering.
Additionally, we provide an overview of the fate and transport behaviors
of CBMs and describe the potential toxicity to humans or other living
organisms in the environment. Finally, challenges to the development
and large-scale industrial production of CBMs are highlighted.
2. Historical development of carbon-based materials
2.1. Biochar and activated carbon
The emergence of carbon materials dates back thousands of years,
particularly activated carbon and biochar. The use of biochar is closely
related to human civilization, perhaps dating back to the paleolithic era.
However, several archaeological findings have unearthed the use of
biochar from prehistoric times. Fig. 1 illustrates different classes of
carbon-based materials.
An archaeological finding in 1971 revealed that China’s Han dynasty
had used charcoal to preserve a corpse, which was still well preserved
> 2000 years after it was unearthed [25]. Findings also reveal that
Egyptians used liquid biochars to embalm the dead more than 7000
years ago [26]. One of the most significant findings was made by Will
Sombroek, who discovered soil rich in a black matter – also called ‘Terra
Preta’, in Brazil’s Amazon rainforest in 1960. Biochar has been applied
in soil amendment – dating back more than 2000 years, and its impor­
tance in carbon sequestration also continues to grow [26].
Activated carbon or charcoal is a unique carbon material with high
surface area and porosity. The use of activated charcoal by the Egyptians
dates back thousands of years [27]. Perhaps, the earliest known study on
the adsorptive capacity of activated charcoal was carried out in 1773 by
the Swedish Chemist, Carl Scheele. By the end of the eighteenth century,
researchers recognized activated carbon’s ability to decolorize aqueous
Fig. 1. Illustration of the different carbon-based materials.
2
Journal of Environmental Chemical Engineering 10 (2022) 107260
solutions [28]. The next hundred years witnessed significant break­
throughs in the use of activated carbon, notably in 1822, when Antoine
Busy and his colleagues prepared activated carbon by combusting blood
with potash, thereby making it 50 times more active than bone char.
This marked the first attempt at combining physical and chemical acti­
vation [29]. Subsequent research towards the end of the nineteenth
century focused on preparing activated carbon from diverse sources
such as coconut shell and paper mill waste, using physical and chemical
activation methods [28]. Finally, the onset of the twentieth century
witnessed pioneering industrial production and commercialization of
activated carbon. The first commercially available activated carbon was
marketed under the name Eponit [27]. Significantly, during the first
world war, activated carbon prepared from coconut shells was used to
adsorb poisonous respiratory gases [28]. In recent times, activated
carbon is routinely prepared from vast species of carbon-rich biomass or
agricultural waste via physical or chemical activation processes and
used for water and wastewater treatment in the adsorption of dyes and
other contaminants, catalysis amongst others [30–33].
2.2. Graphene, graphene oxide, and graphite
The history and chemistry of graphene, graphene oxide, and graphite
are interwoven. Graphene is a 2-dimensional solitary graphite sheet
packed in a hexagonal lattice. It is reputed to be the hardest, thinnest,
and lightest material known to man, with unparalleled heat and elec­
trical conductivity potential. The atomic structure of graphene can serve
as the building block for other carbon allotropes or graphitic materials
such as carbon nanotubes, buckyballs, and graphite. A graphene layer is
so thin that stacking a million sheets of paper will equal 1 mm thick
graphene [34]. Graphene, once regarded as an unstable 2-dimensional
material that could not exist, except theoretically or as part of a 3D
structure, is now readily synthesized and manufactured commercially.
Geim et al. carried out significant research on the synthesis of graphene
in 2004 by isolating graphene on silicon dioxide substrate [34]. Using
mechanical exfoliation, these scientists used sticky tape to remove flakes
from a lump of graphite, transferred to a silicon substrate and carried out
the first isolation of graphene (one atom thick) by repeatedly separating
fragments of graphite. Ulrich Hofmann and Hanns-Peter Boehm are
considered the fathers/pioneers of functionalized graphene research
[35].
A British scientist devised graphene oxide (GO) synthesis, William
Hummers, in the late 1950 s by using strong acids and oxidizers to strip
layers of graphene off high-quality graphite powder. Graphene oxide is
produced, which is further reduced to graphene (termed reduced gra­
phene oxide, rGO) either thermally or chemically [36]. Graphene oxide
is water-soluble, and this is accounted for by the presence of
oxygen-containing functional groups (OCFGs) such as hydroxyl and
carboxyl groups [37]. A chronology of some significant findings in the
discovery of graphene and some derivatives is presented in Table 1.
2.3. Graphitic carbon nitride
The discovery of graphitic carbon nitrides (gCN) dates back to the
early nineteenth century (1834) and coincides with the onset of modern
chemistry when Berzelius, a Swedish chemist, discovered a polymeric
triazine derivative, which would eventually become an important
starting material for the synthesis of carbonic nitride [61,62]. He had
attempted to obtain thiocyanogen (SCN)2 by heating mercury II iso­
thiocyanate - a new compound he created. However, carbon disulfide
and hydrogen were given off, while mercuric sulfide sublimed. Building
on his failed experiment, he added elemental sulfur and repeated the
process. Similar products were obtained, except in this case, a small
quantity of thiocyanogen was obtained in place of HgS, and one other
thing – a polymeric solid residue was formed. The polymer was later
found to consist of triazine cores linked by nitrogen atoms at the corners
and was popularized as ‘melon’, by Justus Liebig. However, the term
A.O. Egbedina et al.
Table 1
Historical evolution of graphene, graphene oxide, and graphite.
Year Findings
1840 Swelling behavior of graphite in concentrated H2SO4 studied
by Schafhautl.
1859 English chemist Collins Brodie reported the atomic weight of
graphite, having noticed the layered arrangement of
thermally reduced graphene oxide.
1900 Improved synthesis of graphene oxide was performed by
replacing nitric acid with sulphuric acid by Staudenmaier.
1916 Peter Debye and Paul Scherrer deciphered the graphite
structure using powder XRD.
1947 P. R. Wallace developed the theory of graphene to explain
the electronic properties of bulk graphite.
1948 Ruess and Vogt obtained the first electron microscopy image
of graphite layers.
1958 Preparation of graphene oxide via the widely recognized
Hummers Method was performed by oxidation of graphite
using sodium nitrate and potassium permanganate dissolved
in sulphuric acid - William Hummers and Offeman.
1962 One of the earliest known experimental studies on single or
multilayer graphite flakes and transmission electron
microscopy (TEM) image for reduced graphene oxide was
accomplished by Boehm, who coined the term ‘graphene’ to
describe single sheets of graphite.
2004 Andre Geim and Kostya Novoselov proved the existence of
monolayer graphene in a stable form.
2008 Early reports of the application of graphene for carbon
capture.
2010 Andre Geim and Konstantin Novoselov received the Nobel
Prize in Physics for "groundbreaking experiments regarding
the two-dimensional material graphene."
2010 An early report on the use of novel magnetically-separable
reduced graphene oxide for water purification via arsenic
removal was published.
2010 Researchers proposed a simple and improved method for
exfoliating graphene bundles from graphite for application
as catalyst supports in fuel cells.
2011 A graphene oxide-based bioassay was successfully deployed
for fluorescent biosensing of pathogenic organisms
(Escherichia coli and Concanavalin A).
2012 Studies emerged showing the efficient photocatalytic
properties of graphene composites towards water
purification.
2013 Use graphene composites in lithium (Li) ion batteries for
potential application in mobile phones, electric vehicles, and
other energy storage devices.
2014 Studies emerged on the application of dispersed graphene
oxides for solid-phase microextraction during sample
preparation and subsequent instrumental analysis of
contaminants in biological and environmental samples.
2014 The use of graphene and graphene oxide as hole conductors
and functional interface modifiers to improve wettability in
perovskite solar cells was reported
2015 The excellent sorption capacity of graphene for waste gases
(air purification) has been reported.
2016 A novel mechanically-assisted electrochemical technique for
fabricating graphene oxide from graphite was studied.
2017 Researchers in China reported using a smartphone-based
cyclic voltammetric system with a graphene-modified screen
for electrochemical detection of glucose.
2018 Graphene-coated carbon-fiber-reinforced composite fabrics
with outstanding electromagnetic shielding effectiveness for
aeronautics, air travel, mobile phones, and military
application were developed.
2019 Self-alarm health monitoring device designed for
simultaneous physiological signal detection and sound
alarm using graphene-based electronic skin.
2021 Bitumen hot mix asphalt modified with graphene oxide
showed promise for road construction due to improved
tensile strength and resistance to moisture and cracking.
2021 The impact of reduced graphene oxides additives on the
improved optoelectronic performance of perovskite solar
cells was reported.
Journal of Environmental Chemical Engineering 10 (2022) 107260
carbonic nitride was not introduced until nearly a century later, when in
1922, it was described as one of several products obtained from the
Reference reaction of ammonium carbonic acids, with melon as the precursor.
Eventually, in 1937, with x-ray crystallography, the structure of this
[38]
compound was deciphered by famous scientist Linus Pauling and his
[38,39] research assistant Holmes Sturdivant as tri-s-triazine, the repeating
monomer for graphitic carbon nitride. Subsequent studies on planar
structure and size showed the similarities between graphite and melon,
[37]
the precursor of graphitic carbon nitride. Much later, it was predicted to
[40] be as hard as or harder than diamond, a significant finding [62]. It is
clearly understood that Liebig’s melon is made up of linked heptazine
[41] rings. Thus, in most literature, g-C3N4 has been suggested and widely
used as the general formula of graphitic carbon nitrides. However,
[42]
Miller et al. [61] argued that this is misleading, hence proposing CxNyHz
[37] as a more appropriate nomenclature, or gCN in broader terms, to reflect
the presence of carbon and nitrogen as the major components. The
synthesis process produces substantial hydrogen alongside carbon and
[39]
nitrogen in most cases. The preparation of gCN from melon and thio­
cyanate is presented in Fig. 2.
2.4. Fullerenes and carbon nanotubes
[43]
The first known synthesis of fullerenes was serendipitous (1985).
[44] Although the discovery of fullerenes is credited to researchers at Rice
University in 1985 (Richard E. Smalley and his colleagues), scientists in
[45] Japan and the USA had earlier predicted the structure of fullerenes,
particularly C60H60, more than a decade earlier. However, their findings
[46] did not receive widespread backing within the scientific community due
to insufficient evidence/structural elucidation [45]. Carbon nanotubes
(CNTs), which, unlike C60, are cylindrical and not closed fullerenes,
[47]
were discovered much later. Although the bulk of fullerenes is prepared
artificially, there is evidence for their occurrence in nature. In 1996, the
[48] Nobel Prize in Chemistry was awarded to Richard Smalley, Robert Curl,
and Harold Kroto to discover fullerenes, also called buckyballs.
In 1952, Radushkevich and Lukyanovich published early images of
[49]
carbon nanotubes in a report on hollow carbon fibers [64]. Decades
later, in1976, Agnes Oberlin and a group of researchers, including
[50] Morinobu Endo, posited that CNTs could be prepared using vapor
deposition. They presented the first viewgraph of what is today termed
single and double-walled CNTs [65]. Shortly afterward, in 1979, John
[51,52]
Abrahamson reported the preparation of CNT using the arc discharge
method. Both techniques have become part of the foremost routes for
synthesizing single and multi-walled CNTs [66]. However, the most
[53,54] significant discovery of CNTs is credited to a Japanese scientist – Sumio
Iijima, who elucidated the atomic and helical structure of CNTs pro­
duced using arc discharge technique in 1991 and presented his findings
in a paper famously titled ‘Helical microtubules of graphitic car­
[55] bon’[67]. Since then, the field of CNTs research has experienced expo­
nential growth over the past three decades. In Fig. 3, the surface and
[56]
internal views of carbon nanotubes are shown.
[57] 2.5. Nanodiamonds
The first synthesis of artificial diamond was in the mid-twentieth
[58] century/the 1950 s. However, the discovery of nanodiamonds, also
called ultrafine dispersed diamonds, is traced to Russian scientists who
worked separately for two decades (1963–1982) and accidentally syn­
[59]
thesized the material three different times. Volkov and co-workers in
1963, Staver and Lyamkin in 1982, and Savvakin in the same year had
[60] chanced upon this material while attempting to prepare diamond via
detonation technique [69]. Most earlier techniques focused on shock
compression of graphite to obtain diamonds, and although there was
little success at diamond synthesis initially, Zababakhin substantiated
the possibility of preparing diamonds this way in 1960. Eventually, the
first documented breakthrough of nanodiamonds synthesis from the
carbon of explosion products by Volkov, Danilenko, and Elin was
3
A.O. Egbedina et al. Journal of Environmental Chemical Engineering 10 (2022) 107260

Fig. 2. Preparation of gCN via pyrolysis of melon and thiocyanate [63].

Fig. 3. Surface and internal views of (a) single-walled, (b) double-walled, and (c) multi-walled carbon nanotubes.
Adapted from Rathinavel et al. [68].

reported in 1963 [69]. Subsequently, Russian chemist G.V. Sakovich and

colleagues carried out the pioneer industrial production of nano­
diamonds. One of the earliest known applications of nanodiamonds is
the production of anti-wear additives for automobile lubrication oils.
While detonation techniques remain the most published technique for
the production of nanodiamonds, their use has become expansive,
covering biological and cellular imaging, electrochemical sensing, dye
removal, catalysis, amongst others [70–72].

3. Emerging trends in CBMs applications

Here, a detailed discussion of the recent applications of CBMs -

highlighted in Fig. 4, for water purification, energy conversion and
storage, and biomedical engineering is given.

3.1. Water purification

Water pollution is a global challenge because of the threats the

various pollutants found in waters pose to human and animal health
[73]. Therefore, research in water remediation has received attention in
keeping with the sustainable development goal (SDG) of providing clean
water for all. Adsorption and photocatalysis are two modern techniques
that have attracted attention in water treatment because of their effi­
ciency in removing a wide variety of pollutants. While adsorption offers
the advantages of ease of operation, low cost, high efficiency, and
availability of various materials with diverse physicochemical proper­
ties and functionalities that can serve as adsorbents, photocatalysis is a
technique that uses green technology which results in the destruction of
pollutants [74]. There is a wide range of pollutants found in water,
including heavy metals, dyes, polycyclic aromatic hydrocarbons (PAHs),
pharmaceuticals, hormones, personal care products, plastics, pesticides,
surfactants, and flame retardants [75]. These pollutants are known to be
carcinogenic, mutagenic, genotoxic [73]. They also cause reproductive
system failure associated with abnormalities in sex organs, sperm
Fig. 4. Illustration of emerging trends in the application of CBMs.
quality, fertility, endometriosis, and early puberty. In addition, they
impact the nervous system, immunological, and respiratory function
and cause metabolic dysfunctions, diabetes, neurological and learning
disabilities, and cardiovascular disorders [73].
Carbon materials have unique structure and properties such as
excellent electrical and thermal conductivity, good chemical stability,
environmentally benign nature, and ease of functionalization [6,76].
They have been used to adsorb and degrade pollutants with varying
degrees of effectiveness. Graphene with a specific surface area as high as

4
A.O. Egbedina et al.
2630 m2/g and high electron mobility [77,78] has been utilized in the
removal of dyes [79,80]; heavy metals [81,82]; endocrine-disrupting
compounds, and other micropollutants [83]. A study was carried out,
which involved synthesizing zeolite imidazole loaded on a graphene
composite [84]. The adsorbent material was utilized to remove three (3)
tetracyclines from wastewater. The adsorbent gave adsorption capac­
ities as high as 608 mg/g. This adsorbent could also be regenerated at
least 5 times without losing activity, demonstrating its ability for prac­
tical removal of pharmaceuticals in water. Also, a graphene oxide
magnetic composite, modified with polyacrylic acid, was used to remove
Cu, Cd, and Pb ions from water [85]. This adsorbent offers a low-cost,
high-efficiency solution for heavy metal removal, with up to 85% effi­
ciency after five cycles.
The widespread use of graphene oxide composite as photocatalyst
support is due to its high intrinsic electron mobility, which allows it to
act as an electron acceptor and prevent electron hole-pair recombina­
tion. Graphene also has high adsorption in the spectrum visible light
range. Therefore, it has been employed in combination with several
metal photocatalysts, such as TiO2 [79,80,86], to lower their bandgap,
allowing absorption in the visible region of the spectrum and increasing
efficiency.
Nevertheless, graphene is prone to agglomeration, which results in
reduced adsorption or loss of catalytic activity, low sorption capacity
due to surface hydrophobicity, and recyclability from solution. As a
result of this behavior, functionalized graphene has been widely devel­
oped to improve the dispersion of graphene and the stability of graphene
sheets [74].
Several chemical modifications have been embarked upon to
improve the dispersion of graphene and enhance the stability of the
graphene sheets. These include attaching oxygen-containing functional
groups to graphene’s backbone, resulting in graphene oxide (GO) or
reduced graphene oxide (rGO). Janik et al. [82] and Guerrero-Fajardo
et al. [87] studied the removal of pollutants using GO and rGO as ad­
sorbents. While the latter utilized the pristine GO prepared via the
conventional Hummer’s method in the adsorption of Pb(II) and Zn(II)
ions, the former modified the prepared GO with several amino silanes
for the removal of Cr(VI). Functionalization of graphene provides
additional active sites to the adsorbent, potentially improving adsorp­
tion and overall efficacy for pollutant removal. It also reduces the ten­
dency of the adsorbent particles to agglomerate by reducing π -π
interactions. This makes the adsorbent’s active sites available for
adsorption [88].
In order to tackle the problem of aggregation, 3-D graphene mate­
rials have also been produced. They are broadly divided into aerogels
and hydrogels [7] and are prepared using mild synthesis methods,
making them relatively low-cost and straightforward to make.
Furthermore, 3-D adsorbents also have a greater surface area and
porosity, showing better efficiency than the 2-D adsorbents. Chang et al.
[89] synthesized a bismuth bromide/graphene hydrogel in the shape of
a 3-D flower. The photocatalytic efficiency of the material for removing
potassium butyl xanthate was 70% even after 6 cycles. Compared to 2D
adsorbents, 3D adsorbents provide fewer possibilities for the adsorbent’s
particles to interact because the degree of π -π interactions is lower,
resulting in reduced aggregation and increased surface area [88,90].
Activated carbon produced from low-cost, environmentally friendly
and waste materials such as cocoa shells [91], potato peels [92], and
date stones [93] has long been used in the remediation of polluted water.
However, due to high energy consumption and regeneration costs, as a
result of easily clogged pores, these materials are still expensive [94,95].
This attribute has led to the fabrication of materials that overcome these
disadvantages yet possess very high surface area and adsorption
efficiency.
The use of biochar as an eco-friendly, low-cost, and porous material
has risen to prominence. Biochar produced from different precursors has
effectively removed dyes [96] and heavy metals [97,98]. Although the
efficiency of biochar is lower than activated carbon, its low cost, coupled
5
Journal of Environmental Chemical Engineering 10 (2022) 107260
with its high porosity and good surface functionalities, have made it an
excellent material. Its characteristics, however, vary according to the
composition of the starting material. Thus, to compete with other CBMs,
biochar requires additional chemical treatment and activation to
improve efficiency [99,100].
Biochar derived from Ashe juniper and treated with H2SO4 was
employed to treat dye-contaminated water [99]. This treatment
improved its surface area and functionalities, resulting in an adsorption
capacity of 714 mg/g compared with 324 mg/g obtained for the pristine
biochar. Similarly, Faheem et al. [100] modified biochar prepared from
rice husk with MnO2 nanoparticles to remove lead ions. The adsorption
capacity of pure biochar was about five times higher after this chemical
treatment. The adsorption of metals from water has been linked to many
mechanisms, including electrostatic interactions, hydrogen bonding,
and pore-filling (Fig. 5a and b). These mechanisms can all occur
simultaneously on the surface of an adsorbent. In addition, an increase
in porosity can lead to an increase in the number of adsorbate molecules
that interact with the adsorbent, resulting in higher adsorption capacity.
Shan et al. [101] studied the effects of several activation agents on
biochar’s efficiency for removing Cr(VI). All the modified biochar pro­
duced better results than the pristine biochar. Of the activating agents,
however, ZnCl2 gave the best performance. The surface area and
porosity of adsorbents are improved by activation. Activating agents like
alkalis – NaOH [102], KOH [103,104]; acids - HCl, H2SO4, HNO3 [105],
H3PO4 [106], C2H4O2; Salts - ZnCl2 [107], K2CO3 [108], Na2CO3,
Na2HCO3 [109] have all been employed.
The introduction of a magnetic property into the structure of CBMs
results in materials that are easy to separate from an aqueous solution
after adsorption or photocatalytic application. Magnetite (Fe3O4) is
either produced via a solvothermal method with FeCl3 or via chemical
co-precipitation by Fe2+ and Fe3+. Magnetite (Fe3O4), which is the most
used, imparts properties such as increased surface area [110]. The use of
magnetic biochar was investigated, in which the presence of Fe on the
surface of the biochar resulted in increased surface area and increased
adsorption efficiency [111]. Increasing the Fe concentration beyond a
certain ratio, adsorption capacities for Cu, Cd, and Pb ions were reduced.
This behavior could be attributed to the Fe atoms etching into the
already formed pores leading to blockage of pores and reduced surface
area. Biochars have also been applied in the removal of organic con­
taminants such as pharmaceuticals [112–114], pesticides [115], phe­
nolics [114,116], phthalates [117,118],; CO2 adsorption [23,119,120],;
and oxyanions [121,122].
CNTs have also been actively explored in water purification, with
multi-walled carbon nanotubes (MWCNTs) receiving more attention
than single-walled carbon nanotubes (SWCNTs) due to their lower cost,
even though the latter generally have a higher adsorption capacity [125,
126]. Comparing the adsorption capacities of CNTs as adsorbent mate­
rials for phenanthrene, a polycyclic aromatic hydrocarbon, SWCNT
showed a higher adsorption capacity than MWCNT- as much as four
times [126]. CNTs have also been utilized in the removal of phthalate
esters [127]; tetracycline, bisphenol A, sulfamethoxazole [128]; hor­
mones [129]; benzoic acid [130], heavy metals [131], phenol [132],
and pesticides [133].
As with other carbon-based materials, CNTs have been modified by
doping with nitrogen [134], HNO3 [135,136], and ferrocene [130] to
tune their properties for the selective and enhanced removal of target
pollutants. Similarly, when benzoic acid was employed to enhance the
surface properties of SWCNTs, an improved adsorption capacity was
observed, especially when compared to other materials such as activated
carbon, clay, and graphite [130]. A series of CNT/TiO2 composites for
use in methyl orange degradation was prepared [137]. This composite
was functionalized with NaOH and SDS and calcined at temperatures
between 350 ◦ C and 550 ◦ C. Though the surface area decreased with
CNT modification and increasing temperature, the highest catalytic ac­
tivity was observed for the composite calcined at 450 ◦ C. Also,
increasing the amount of CNT in the composite reduced catalytic
A.O. Egbedina et al.
Fig. 5. (a) Overview of mechanisms for adsorption of organic and inorganic pollutants using biochar [123]. (b) Illustration of the mechanism of metal sorption via
complexation and cation exchange using biochars [124].
activity due to excess carbon in the system, resulting in photon scat­
tering. CNT/TiO2 has also been modified with FeCO-Al2O3 to degrade
methylene blue under sunlight irradiation. Degradation was studied as a
function of time, dye concentration, and catalyst dose. The presence of
CNT resulted in a lesser irradiation time compared with TiO2 catalyst
[138].
Additionally, Deshpande et al. [139] prepared Co/Ni/Fe – CNT
magnetic composite for the comparative degradation of methylene blue,
methyl orange, congo red, and rhodamine B dyes. Essentially, surface
area and porosity increased with the increasing addition of CNT,
resulting in more efficient adsorption and photodegradation. Similarly,
MWCNT – 20% wt Fe2O3 nanoparticles were prepared for benzene
removal [140]. Again, the removal increased with iron concentration,
which can be attributed to the increased surface area because of the Fe.
6
Journal of Environmental Chemical Engineering 10 (2022) 107260
3.2. Clean energy conversion and storage
Energy is required in everyday life to meet heating, lighting, cooking,
transportation, and communication needs. Rising energy demand and a
growing human population have increased energy consumption. The
dependence on fossil fuels has had negative consequences on the envi­
ronment, such as increased CO2 emissions, which have resulted in global
warming and climate change [141]. The search for more efficient,
low-cost, sustainable, near-zero emissions and cleaner energy sources,
such as supercapacitors and lithium-ion batteries, has been forced by
those factors coupled with their limited supply [142].
Energy can be converted from natural, infinite sources such as sun
and water using oxygen reduction reaction to electricity or fuel; this is
applied in fuel cells and solar cells [143]. Low-cost, ecologically
A.O. Egbedina et al.
friendly, and high-performing materials, on the other hand, are required
to store and release energy in devices efficiently. Batteries and super­
capacitors are examples of these storage devices [144]. Compared with
conventional capacitors and batteries, nascent supercapacitors, batteries
(lithium-ion batteries, sodium batteries), solar cells, and fuel cells have
attracted attention due to their long-life cycle, high energy density,
high-power capability, high charging-discharging capabilities, and low
cost [10,143,145]. As a result, they are widely used in various consumer
gadgets, including micro-batteries, industrial power systems, airline
emergency doors, low-emission hybrid electric vehicles, and fuel cell
vehicles [10,146].
In addition, carbon materials from biodegradable and naturally
available feedstock are widely utilized as electrodes due to their desir­
able properties, including chemical inertness, low cost, tunable porosity,
surface area, and electrocatalytic redox-active sites [143]. They can be
used in powders, fibers, foils, and monoliths [147]. Due to its pore
structure, which can be adjusted in a variety of ways depending on the
activation method, activated carbon has been widely employed as an
electrode material [148]. Carbon produced from rotten carrot [148],
lignin [146], apricot seeds [149], sawdust [150] has been utilized as
electrode materials for storage devices.
Current research activities are generally centered on improving the
energy density of CBMs [147]. Materials possessing highly mesoporous
and microporous structures have increased capacitance and produced
excellent electrode materials [146,151]. Activation has been found to
give favorable and enlarged surface area, resulting in a greater capaci­
tance. CBMs produced from various precursors have been activated with
ZnCl2 and KOH. Comparing activated carbon with and without activa­
tion post-treatment gave results that showed that activation increased
micropores and mesopores, which generally resulted in increased spe­
cific capacitance. [146]. However, an understanding of the activation
limit is needed because increasing the activating agent beyond a certain
limit can result in the deactivation of the active sites, reducing effi­
ciency. For example, a maximum specific capacitance (180 Fg-1) was
found when KOH was applied to apricot before carbonization in a 1:1
ratio. Increasing the KOH beyond this ratio decreased the specific
capacitance to 152 Fg-1 [149].
Although a large specific surface area is desirable, other properties of
carbon-based materials, such as pore size distribution, surface func­
tionalities, and pore shape, can influence its electrochemical activity to a
large extent. Furthermore, carbon nanofibers (CNFs) have been used as
electrode material, electrocatalyst support in supercapacitors, fuel cells,
and batteries [152–154]. Similarly, both SWCNTs and MWCNTs have
been explored as energy storage materials. However, compared to
activated carbons and CNFs, CNTs are more expensive and possess low
energy density due to their lower surface area. This is coupled with the
fact that there is a difficulty in retaining the intrinsic properties of in­
dividual CNTs on a macroscopic scale [155].
Chemical activation, non-metal doping, metal oxide doping, and
hybridization of CBMs have all been used to impart desirable structures,
resulting in improved energy densities and capacitance [156]. For
instance, KOH activation of CNF improved electrochemical properties,
resulting in 95% cycle stability and 440 Fg-1 capacitance after 5000
cycles, compared with 261 Fg-1 for the pure CNF [153]. Jeon et al. [157]
researched the comparative use of RuO2-CNF and the pristine CNF.
RuO2-CNF had a three-fold greater specific capacitance and 93%
retention rate after 3000 cycles [157]. Also, Lin et al. [158] applied
nitrogen-doped CNF that had been modified with perovskite nano­
particles as an oxygen electrocatalyst for Zn-air batteries. Nitrogen
doping was discovered to allow for the homogenous encapsulation in the
CNF, resulting in increased current density, a stronger positive onset
potential for oxygen reduction processes, and better electrochemical
performance and endurance in the battery. He et al. [155] were able to
control the pore structure of CNF prepared from polyacrylonitrile (PAN)
and modified with polymethyl methacrylate (PMMA) in a 7:3 ratio,
resulting in maximum specific capacitance of 140 Fg -1 at 0.5 Ag-1. This
7
Journal of Environmental Chemical Engineering 10 (2022) 107260
is significant because less porous CNF results in lower charge-transfer
resistance and, as a result, decreased efficiency [159].
A blend of CBMs improves the pore volume, specific capacitance, and
cyclic stability of CNF for use in supercapacitors. Kshetri et al. [160]
blended graphene, CNTs, and CNF to illustrate the CBMs’ blend’s per­
formance in supercapacitors. This blended material exhibited superior
electrochemical performance with a specific capacitance of 521.5 Fg-1 at
0.25 Ag-1 and 98% retention after 10,000 charge-discharge cycles at 5
Ag-1. As a result, the blend served as an excellent negative electrode
material for energy storage application in a hybrid supercapacitor.
Graphene and its derivatives are better electrode materials than acti­
vated carbon and CNTs because their performance does not depend on
the distribution of pores in the solid-state. Besides, the external pores of
the graphene sheet are accessible by the electrolyte [147], increasing its
conductivity and hence its capacitance. In addition, when graphene
oxide was activated with phosphoric acid, it resulted in a high packing
density material with high volumetric performance [161]. Furthermore,
a nanohybrid of MoS2 on rGO gave a material three times the perfor­
mance of pure MoS2 [162]. The improved electrochemical performance
of the MoS2/rGO electrode is induced by the presence of rGO that oc­
casioned a rapid diffusion pathway. Azizi et al. [163] used a combina­
tion of NiFe magnetic nanoparticles and rGO as electrode material in
supercapacitors. Again, the presence of rGO resulted in enhanced spe­
cific capacitance of up to 1224 Fg-1 at a scan rate of 10 mVs-1. However,
this value decreased with an increase in scan rate due to the electrolyte
ions’ difficulty accessing the electrodes’ inner surface. Additionally,
silver nanowires (AgNWs) [164], Na-MnO2 via intercalation [165],
CeO2/Ce2O3 [166], sulfanilic acid azocromotrop [167], polymers [168],
and non-metals [169,170] have all been modified with graphene and its
derivatives for application in solar cells, supercapacitors, fuel cells, and
batteries.
3.3. Biomedical engineering
Biomedical engineering covers a wide range of topics, including the
interpretation of bioelectric data for diagnostic purposes, the creation of
artificial organs for replacement and augmentative therapy, and the
detection, measurement, and monitoring of physiological signals. The
area of biomedicine has welcomed CBMs as promising materials because
of their ease of functionalization, biocompatibility, and availability of
delocalized electrons. These characteristics impart solubility, selectivity,
chemical stability, and purity on them [11,78]. These properties have
been further improved by combination with moieties, such as polymers,
and oxygen-containing functional groups such as epoxy, carboxylic
acids, hydroxyls [6]. Important applications of CBMs in this field include
biosensing and bioimaging, drug delivery, photodynamic and photo­
thermal therapy, tissue engineering [6171].
3.3.1. Photothermal and photodynamic therapy
Photothermal therapy (PTT) and photodynamic therapy (PDT)
involve the use of photosensitizing agents, such as noble metals, tran­
sition metal sulfides, and oxides, porphyrins, dye molecules [172], in a
minimally invasive technique. This method selectively targets and kills
cancerous cells on exposure to light irradiation without harming normal
organs [11,173,174]. They are also applied to treat bacterial and fungal
infections [175]. While PTT uses photothermal agents to absorb light
and convert it to heat, which is utilized selectively to target abnormal
cells and tissues, PDT uses photosensitizers activated by the absorption
of light to generate reactive oxygen species through a series of photo­
chemical reactions. However, this mechanism causes cytotoxicity in the
target cell [172,175]. As a result, developing effective and safe photo­
sensitizing agents is critical to the success of PTT [176]. Importantly,
because of the ability of CBMs to absorb near-infrared (NIR) light and
convert it to heat, they have been investigated for use in PTT and PDT as
opposed to traditional photosensitizers, which are activated by visible
light that cannot penetrate and reach deep tumor tissues [172,177].
A.O. Egbedina et al.
CNTs (SWCNTs and MWCNTs) are at the forefront of CBMs used to
produce advanced biomaterials for use in photothermal and photody­
namic therapy. MnO2 was doped with MWCNT, and a series of polymers
were added to give it biocompatibility, water dispersibility, and tumor
target ability [178]. NIR irradiation triggered phototherapy using the
photosensitizer chlorine e6. At low doses, the progressive breakdown of
MnO2 into Mn2+ enabled image-guided therapy and suppressed cancer
cell proliferation in vitro without causing systemic damage.
The synthesis of CBMs for these applications has been observed to be
affected by several reaction conditions. They include pH, reducing
agent, the concentration of reactants, and the ratio of reagents. These
parameters were carefully controlled in the 2-step reduction synthesis of
a hybrid of gold nanoparticles (Au NPs) and MWCNT [179]. In addition,
the PTT conversion of the generated biomaterial was high. Compared
with Au NPs alone, the hybrid material showed a 12.4% higher photo­
thermal conversion and a 2.4-fold increase over Au NPs using laser
irradiation of 808 nm.
In addition to CNTs, magnetic graphitic carbon-containing Fe(III)
diethylenetriaminepentaacetic acid complex was synthesized and
applied to human adenocarcinoma A549 cells, resulting in almost 98%
of cancer cells dying in 10 min under 808 nm of light [180]. Similarly,
Yao et al. [181] used a one-step hydrothermal approach to make pho­
toluminescent ginsenoside Re-carbon dots (Re-CD). The produced sub­
stance was used to destroy cancer cells by photothermal destruction.
Ginsenoside Re-CD had a stronger inhibitory efficiency and
excitation-dependent fluorescence imaging than ginsenoside Re. The
benefits of combining both phototherapy methods rather than using one
alone have also been investigated. Zhang et al. [182] studied the efficacy
of Ru(II) complex loaded SWCNTs in vitro treatments employing a
combination of PTT and PDT under an 808 nm diode laser with a power
density of 0.25 W/cm2 for 5 min. The combined phototherapy approach
was found to have strong anticancer efficacy.
3.3.2. Biosensing and bioimaging
Biosensing materials are used in the in-situ sensing of biomolecules
such as nucleic acids, proteins, and carbohydrates to monitor target-
specific electrical charge changes at a high signal-to-noise ratio. CBMs
have been explored especially in composites as materials for potential
use in biosensing and bioimaging. The impacts of different pretreatment
methods in preparing a series of carbon dots (CDs) doped with varying
amounts of O, N, and S using cellulose hydrogel have been explored
[183]. Essentially, fluorescence quantum yield increased as particle size
was reduced, and N improved fluorescence than the elements used in
doping. However, the fluorescence was found to be quenched in the
presence of Hg, suggesting its suitability for Hg detection. This behavior
is comparable to that observed in cancer cell detection using N-doped
folic acid-derived CBM, resulting in increased interest in using
polymer-CBM composites [184].
Zhang et al. [185] described a simple method for making a
water-soluble CD/polyvinyl alcohol (PVA) composite that can be used
for both H2O2 and glucose biosensing, and bioimaging Avrossa et al.
[186] used two polymers (polystyrene and poly-hydroxybutyrate) to
create a graphene porphyrin nanofiber composite. The resultant mate­
rial was placed on an electrode and utilized to determine the appropriate
working temperature for driving sensitivity and selectivity. Between 50
and 70 oC, the sensor worked reliably and consistently without sub­
stantial degradation.
Several studies have employed simple and environmentally friendly
ways to synthesize CBMs for various sensing applications. Cabral et al.
[187] utilized PVA and water-soluble CDs produced from citric acid to
create luminous materials at a low cost. This sensor was designed to
detect glucose with high efficiency in the 1–10 mM range, with a
detection limit of 12 μM. CBMs have also been prepared from low-cost
and environmentally friendly precursors to detect cancer cells and
heavy metals [188,189]. Microwave-assisted preparation of
bi-functional ibuprofen-based CBM was prepared for simultaneous
8
Journal of Environmental Chemical Engineering 10 (2022) 107260
bioimaging and anti-inflammatory properties [190]. In vivo, the material
showed good imaging ability and excellent anti-inflammatory effects.
Zhang et al. [45] used a microwave-assisted one-pot synthesis of
protamine-CDs for nucleolus imaging and tracking. This was achieved
because fluorescence was enhanced on binding to RNA. For long-term
imaging tests of up to 12 h, the produced CDs could traverse the cyto­
plasm and nuclear membranes and locate at the nucleolus. As a result, it
might be used as a nanoprobe for in vitro transfection investigations. All
of these materials have shown great promise in clinical as well as in
environmental applications.
3.3.3. Tissue engineering
CBMs are utilized as scaffolds for cell culture and tissue engineering,
and they have exhibited excellent adhesion properties and minimal
cytotoxic effects on cells. The current tissue engineering research wave
focuses on enhancing CBM’s biodegradability and mechanical proper­
ties. Traditional scaffolding materials, such as hydrogels lack the
required mechanical strength, necessitating their augmentation [171].
As a result, most studies involved the modification of CBMs with poly­
mers [191], gelatin [192], and biomass [193].
Meckael et al. [194] synthesized a biodegradable
polymer/water-dispersible CNT composite scaffold. Scaffolds have been
employed as extracellular matrix analogs to stimulate cell migration,
cell attachment, and cell proliferation [195]. The scaffold demonstrated
compressive modulus and strength in the range of human cancerous
bone. The use of blood vessel engineering to treat cardiovascular dis­
orders is another promising method Tondnevis et al. [196] developed a
composite of SWCNT and polyurethane nanofiber similar to the native
artery. After 7 days, in vivo cell studies revealed that a dense layer of
endothelial cells crucial for blood vessel tissue engineering was grown.
Compared with pure polyurethane, a 2% wt CNT enhanced stress, young
modulus, and electrical conductivity.
In another experiment, a polyurethane-gelatin-SWCNT composite
was used. With the inclusion of gelatin, the scaffold degradation profile
was altered. As a result, after 7 days of growth, a dense layer of cardiac
myoblast and endothelial cells formed an important discovery for the
treatment of cardiovascular disease [196].
Jafarkhani et al. [197] synthesized a nanoGO/chitosan hydrogel
composite for nerve regeneration and used machine learning to assess
the nerve cells’ adhesion and proliferation rate. Findings revealed that
the right concentration of nanoGO could successfully drive cell growth,
laying the groundwork for designing and developing functional hydro­
gels for nerve regeneration. The osteoblasts were seeded over a highly
porous collagen-alginate-GO aerogel that had been created [195]. The
results were promising as a promoter for cell adhesion and proliferation,
and it might be used as a platform for tissue engineering research.
Furthermore, Ketabi et al. [191] produced a 4% CNT in poly­
caprolactone with potential application in dental tissue engineering and
odontoblast cell interactions. For in vitro experiments on human cardiac
progenitor cells, Nazari et al. [198] synthesized a GO-Ag nanocomposite
and incorporated it into polyurethane nanofibers. The synthesized
scaffold showed good compatibility and adhesion to the scaffold.
3.3.4. Drug/gene delivery
Purity, biocompatibility, high drug loading bio-functionalization,
and ability to interact with diverse biomolecules, such as proteins and
nucleic acids, are some of the properties of CBMs exploited in drug de­
livery [171]. Drug delivery involves efficient in vitro loading and
controlled release of drugs such as anticancer drugs [199,200],
non-steroidal drug, ibuprofen [201], and chloroquine [202] through π-π
stacking.
Water-soluble fullerene has been shown to pass the exterior cellular
membrane and preferentially localize to the mitochondria [203]. This
behavior could be utilized for the targeted delivery of drugs to specific
parts of the system. The possibility of a boron nitride (B24N24) fullerene
as a carrier for the anti-cancer drug 5-fluorouracil was investigated using
A.O. Egbedina et al.
density functional theory (DFT) [199]. Because of the weak interaction
of the pristine fullerene with the medication, this material was modified
with aluminum. Likewise, a B24N24 fullerene nanostructure was utilized
as a carrier for the anti-cancer drug hydroxyurea [204]. Studies found
that such modification with B24N24 improved fullerene’s capabilities for
drug adsorption; thus, indicating its potential use as an optical sensor for
detecting and monitoring drug molecules.
For drug delivery of ibuprofen, researchers modified fullerene with a
porphyrin-like transition metal. The alteration considerably improved
fullerene’s ability as a potential delivery system for ibuprofen. Novir &
Aram [202] have investigated the effects of fullerene and chloroquine in
treating COVID-19. DFT was used to explore several doping materials -
Boron, Aluminium, and Silicon. Because of their significantly higher
energetic and electrical properties on chloroquine adsorption, results
suggested that doped fullerene, mainly Al- and Si-doped fullerene, could
be a better drug delivery method for chloroquine.
CNTs have also attracted interest due to their ability to lead a variety
of biomolecules. To illustrate, Falank et al. [205] synthesized a series of
MWCNTs that were loaded with Doxorubicin (DOX) for targeted drug
delivery for bone and bone marrow diseases. More so, SWCNTs were
used as carriers in a study of the anti-nervous necrosis virus activity of
isoprinosine, an immunomodulatory, antiviral medication, to improve
the activity compared to isoprinosine alone [206]. A magnetic drug
delivery system based on functionalized CNTs and gemcitabine it was
developed and compared with a similar system that is based on activated
carbon and gemcitabine [207]. Both demonstrated high anti-tumor
effectiveness in vivo and in vitro, but the CNT system outperformed
the activated carbon system. In addition, subcutaneous delivery of the
loaded medicines resulted in the successful prevention of lymph node
metastasis.
The use of CNFs has also been investigated. The chemical vapor
deposition approach was used to generate Cu/Zn bimetallic NPs
distributed in CNF [208]. The drug delivery system treats bacterial in­
fections effectively and can be utilized for wound healing and antibiotic
dressing. A DOX/ CNF delivery system was prepared [209]. The CNF
was made by electrospinning PAN and PMMA together, resulting in a
porous material. In addition, the device had a dual-sensitive drug release
response to pH and NIR irradiation, which enhanced DOX release at
acidic pH.
CBMs have also been blended in various studies. For example, by
reversibly encapsulating fullerenes in large diameter SWCNTs, their
potential was utilized for enhanced drug delivery [210]. Letrozole and
Metronidazole, two drugs widely used to treat breast cancer, were also
investigated on a blend of fullerene and graphene [200]. Self-assembly
was discovered to occur during adsorption that improved all the mole­
cules’ attributes, including biological activity. This characteristic can
aid in the development of drug delivery methods and novel sensor-based
devices that can detect their presence in a mixture.
More importantly, the production of CBMs is increasing as new ap­
plications are discovered. As a result, a wide range of consumer products
incorporating CBMs is increasingly available such as cosmetics, cleaning
supplies, lubricants, and textiles. Therefore, this necessitates a consid­
eration of the fate of CBMs in such household goods and their potential
environmental and human toxicity.
4. Fate and toxicity of CBMs
Many natural, produced, and waste materials from households and
industrial activities end up in the soil, air, and water. Carbon-based
materials are no exception when it comes to their fate in the environ­
ment. Their current uses in pharmaceuticals, construction, automobile,
biomedicine, the food industry, electronics, cosmetics, laboratory, and
water treatment make it clear that their residues will end up in the
environment sooner than later. In the scientific literature, the fate and
movement of these materials are being discussed [211,212]. Fabricated
CBMs can be inadvertently released to the environment through the
9
Journal of Environmental Chemical Engineering 10 (2022) 107260
disposal of liquids or solids from wastewater treatment plants, factories,
hospitals, agro-based materials, disposal of used electronic gadgets,
among others. However, once released (during production, trans­
portation, or product disposal), they penetrate the soil and aquatic
systems and pollute the food chain [213]. In the soil, the fate of CBMs is
influenced by their physicochemical properties (surface coatings, size,
morphology, zeta potential) as well as those of the soil (soil composition,
grain size, soil pH, cation exchange capacity, moisture content, dis­
solved organic matter), environmental factors, and the influence of the
other chemical species [214,215]. In order to explore the impact of soil
composition, MWCNTs were passed through fine, medium, and coarse
sand. Fine sand retained less (approximately 85% less) MWCNTS than
coarse sand [216]. This observation indicates that the greater the soil
porosity, the lesser chances the soil will act as a sink for CBMs.
Carbon-based materials enter the air through various natural (e.g.,
volcanic eruption, spontaneous wild-fires, etc.) and anthropogenic (e.g.,
during production, burning of municipal wastes, electronic waste
burning to recover precious materials, etc.) sources. Because of their
high mobility, CBMs can mix quickly in the air. They are exposed to
sunlight in the atmosphere, particularly UV radiation, which increases
their chances for photochemical transformations [217]. Such trans­
formation and degradation may alter the pristine state of these mate­
rials, consequently affecting their fate, transport, and toxicity [218]. For
instance, exposure to sunlight destabilizes and alters GO, leading to its
partial conversion to rGO or transformed graphene oxide (TGO), CO2,
and low molecular weight PAHs [219]. Fig. 6a depicts the mechanism
behind this process. Hou and Wang [220] reported the photocatalytic
generation of hydrogen peroxide via irradiation of GO. pH was discov­
ered to be a crucial factor in the process (Fig. 6b). In the presence of
nutrients like nitrate, phosphate, and natural organic matter, indirect
photo-transformation may occur in aquatic environments. This is
because nutrients can produce hydroxyl radicals when exposed to sun­
light. These then react with graphene oxide that has been altered,
resulting in still another compositional shift [221]. Tan et al. [222]
devised a spectrophotometric in-situ tracking system to track the dete­
rioration of GO under sunshine. To accurately track this photo­
degradation of GO, the system used a chemical vapor production reactor
(Fig. 6c and d).
Because large materials settle out considerably quicker than the
smaller ones, agglomeration of CBMs significantly enhances their
deposition. This procedure could indicate a pathway of entrance into
soil or water. Undoubtedly, the emission of CBMs from road traffic (i.e.,
fumes from diesel engine exhaust) has become the most significant and
straightforward source of respiratory exposure for people residing close
to highways and in most urban areas [223]. CBMs tend to partition
between water and specific materials in the water, thereby conglomer­
ating with dissolved organic matter, suspended particles, or colloids,
and then depositing into the sediment. Also, they can re-enter the sur­
face water through hydrodynamic processes and resuspension [224]. In
addition, CBMs may also enter aquatic systems via direct channels such
as sewage and water effluents or indirect routes such as atmospheric
deposition and run-off [225]. Some CBMs are readily dissolved in water
than others due to different solubilities. For instance, as previously
noted, CNTs in their pristine state are practically insoluble in any sol­
vent, including water. However, functionalization with
oxygen-containing groups, such as carboxyl groups, provides active sites
that enhance water solubility [226]. Moreover, unlike the
equilibrium-based partitioning process in dissolved chemicals, the fate
and transport processes of CBMs are largely kinetically controlled [227].
The detection and quantification of CBMs in environmental matrices
using current analytical techniques is still a work in progress. This is
owing to the difficulty of discriminating between natural and manu­
factured CBM concentrations at the low levels expected in diverse
environmental matrices [228]. Despite the lack of measurable concen­
trations, fate and transport models can offer geographical but temporal
estimates of their environmental concentration to assess potential
A.O. Egbedina et al.
Fig. 6. (A). Schematic representation of the photo-chemical transformation of GO to TGO and LW PAHs [221]; (B) Photocatalytic production of H2O2 by GO [220];
(C) In-situ tracking system for photodegradation of GO [222]; (D) Schematic of the detection system [222].
Photo transformation of GO under sunlight irradiation (Adapted from Zhao et al. [221]).
ecological risks [229]. When substantial observational data is insuffi­
cient, modeling relies on current materials or new-to-market items to
estimate the probable environmental concentration. The results of such
well-structured models could predict concentrations in potential expo­
sure hotspots and other environmental partitions [230]. The level of
detail required to capture all of the aspects of CBM fate in the envi­
ronment is a point of contention, and the model’s lack of data for cali­
bration and validation is a fundamental flaw. Nonetheless, there is a
significant improvement in the range of questions that the models can
answer, as well as some levels of confidence in the outcomes [224].
Several models have been proposed and employed in modeling the
fate of CBMs in the environment. Material flow analysis (MFA) is a
simple method for modeling the fate of substances or materials over
their entire lifecycle in the environment [228]. It was used to quantify
CBMs from products to water, air, and soil in Switzerland [225]. The
input parameters used were the estimated global production volume,
apportionment of the volume to product categories, substance release
from products, and flow coefficients within the compartments. MFA has
made it feasible to have a better understanding of the properties,
amounts, and locations of CBMs [231]. Static [231] and dynamic [232,
233] MFA methods have been used, with the latter relying on historical
data to predict future production rates and market dynamics. Release
data fused into a probabilistic MFA model was employed considerably
more than earlier models that assumed that CBMs remained in their
pristine state throughout their existence. This model quantified their
proportions in not only product-embedded but also matrix-embedded,
transformed, pristine, and dissolved forms in all technical and envi­
ronmental compartments [234].
Despite this advancement, the paucity of data on the annual pro­
duction rate of produced CBMs makes estimating the distribution and
10
Journal of Environmental Chemical Engineering 10 (2022) 107260
market dynamics of CBM-containing items challenging [24]. Another
model based on the Bayesian method, FINE (Forecasting the Impacts of
Nanomaterials in the Environment), allows new data to be updated as
they become available, which is a potential feature for estimating the
risk associated with CBMs [235]. Furthermore, RedNano (Release and
environmental distribution of Nanomaterials), MendNano (Multimedia
environmental distribution of Nanomaterials), and SimpleBox4nano
models allow for the evaluation of the various factors affecting CBMs
production, distribution, and potential release and release rates. In
addition, they predict their distributions, concentrations, and specia­
tion, which are suitable for research and regulatory purposes [236,237].
Other models that have been used include NanoDUFLOW [229] and
NanoFate [238], which are adaptable to a variety of processes and
environmental sub-compartments, and Fractal modeling [239], which
complements the current fate models. The Fractal model adds density
and collision efficiency parameters and exact explanations of shape and
structure to improve the description of homo- and hetero-aggregations.
The clamor for the use and inclusion of CBMs in products used by
humans may be connected to the assumption that they are no more
harmful than graphite. On the contrary, several studies continue to
reveal their likely toxicity [240,241]. Mice showed unusual pulmonary
effects coupled with early onset of acute inflammation but with
increasing granulomas and fibrosis, which were a consequence of
pharyngeal aspiration of SWCNT [242]. Fig. 7 depicts the micrograph of
lung tissues of C57BL/6 mice that were exposed to MWCNT suspensions
through pharyngeal aspiration. The histological assessment revealed
granulomatous lesions after 56 days of exposing each mouse to 40 or
80 μg of MWCNTs [243]. In addition, collagen was deposited in all the
exposed mice. Also, distinct and agglomerated macrophages, shown as
dark particulate matter, were present (Fig. 7).
A.O. Egbedina et al.
Fig. 7. Photomicrographs of lung tissues of C57BL/6 mice administered 40 μg and 80 μg of MWCNTs per mouse, and the control.
Red arrows point to MWCNT-laden macrophages (Reproduced from Scala et al. [243]).
Moreover, the result was dose-dependent, and the outcomes wors­
ened at 80 μg dosage compared to 40 μg and the control. Similarly,
when the mesothelial lining of the mice’s body cavity– which was
substituted for the mesothelial lining of the chest cavity– was exposed to
MWCNTs, it resulted in inflammation and granulomas. This pathogenic
behavior was comparable to the outcome of the exposure of lungs’ lining
to asbestos [244]. CNTs pose more toxicity to the lungs than carbon
black and quartz, which is regarded as a severe occupational health
hazard in chronic inhalation exposures Lam et al., 2003). Specifically,
CNTs have triggered dose-dependent epithelioid granulomas in mice
after 7 days and interstitial inflammation in some cases, generating
persistent lesions that were noticeable in 90 days [245].
Nevertheless, some studies utilizing rat and guinea pig specimens
could not establish a direct association between CNTs exposure and
pulmonary toxicity. For example, Warheit et al. indicated that although
about 15% of the rats instilled with SWCNTs at 5 mg/kg dosage died
24 h post-installation, the death was a consequence of the mechanical
blockage of the upper airways rather than the intrinsic pulmonary
toxicity of the instilled SWCNT particulate [246]. Also, a method for the
pathophysiological assessment of asbestos-induced diseases was used to
examine the pulmonary toxicity of CNTs. The results showed that soot
with a high content of CNTs did not cause any abnormalities of pul­
monary function or quantifiable inflammation in guinea pigs [247].
Notably, environmental concentrations of CBMs do not constitute a
threat to aquatic organisms on their own, based on their observed
concentration in the aquatic environment or differences in the target
organisms [240]. However, there is still evidence of the potential
toxicity of CBMs on aquatic organisms and humans. For example,
Bluegill sunfish cells depicted a time- and dose-dependent cytotoxicity
when exposed to about 40 μg/mL of GO for 24 h [248]. Similar cytotoxic
effects were induced by graphene and SWCNT in an in vitro test using
neuronal PC12 cells [249]. The effects were said to be shape- and
concentration-dependent. However, SWCNT elicited more intense
metabolic activity at higher concentrations than graphene, whereas the
reverse was at low concentrations.
Moreover, the exposure to graphene generated reactive oxygen
species in a concentration- and time-dependent manner, which depicted
an oxidative stress process [249]. Additionally, Kalman and the team
evaluated the efficacy of using fish cell lines to characterize the toxicity
and cellular fate of graphene-related materials [241]. They observed
that the membrane integrity, metabolic activity, and lysosomal function
of fish hepatoma cells and macrophages were affected differently.
However, GO induced lesser toxicity than CNFs, with the graphitization
of the latter resulting in lower toxicity [241].
For humans and other living organisms, their toxicity disorders
include cardiotoxicity, hepatotoxicity, genotoxicity, neurotoxicity,
nephrotoxicity, dermatotoxicity, epigenetic toxicity, immunotoxicity,
and carcinogenicity, which have been well documented in recent liter­
ature [19]. It has been indicated that though CBMs are toxic, their
hazardous effect is size-dependent [250]. However, even structurally
related CBMs may induce different toxicities. For instance, the toxicity
of CNFs in the human lung-tumor cell line (H596) was more than that of
11
Journal of Environmental Chemical Engineering 10 (2022) 107260
SWCNTs or MWCNTs [250]. It was further observed that the toxicity of
these CNTs significantly increased when they were modified with
oxygen-containing groups. In another study, minute-sized GO displayed
the highest hemolytic activity instead of graphene sheets; however,
covering GO with chitosan almost jettisoned hemolytic activity [251]. It
was shown that graphene’s particulate size, shape, and functionaliza­
tion/surface charge strongly influence red blood cells’ tox­
icological/biological responses. Again, the toxicity of MWCNT and its
functionalized derivatives to human alveolar macrophages (AMs) was
evaluated. Evidence of decreased cell viability and amplified inflam­
matory mediator release confirmed the more toxic nature of acid puri­
fied MWCNT (AP-MWCNT). Specifically, there was an appreciable
increase (3.5–2.4-fold) in interleukin (IL-1β and IL-8) released by the
AMs, a day after treatment with AP-MWCNT [252]. Conversely, there
was no significant change in IL-1β and IL-8 released by AMs within the
same length of time after treatment with functionalized-MWCNT. This
study was vital to ascertain the effects of MWCNTs and surface modifi­
cation on extremely vital human alveolar macrophages, which remove
foreign matter; thus, providing the front line of cellular immune defense.
Because graphene and its derivatives have been widely employed for
biomedical applications, studies on interacting with primary human
cells are increasing. Cell-based analyses depicted an organized oxidative
stress paradigm involving lipid peroxidation, mitochondrial superoxide
generation, cytosolic reactive oxygen stress, glutathione oxidation,
enhanced calcium efflux, and mitochondrial membrane depolarization
death of the cell by apoptosis/necrosis [253]. Similarly, the dynamic
light scattering and methyl-thiazolyl-diphenyl-tetrazolium bromide
assay demonstrated that GO could induce apoptosis and cytotoxicity in
human lung cells (BEAS-2B) [254]. In addition, a reduction in cell
viability, which significantly depended on concentration
(10–100 μg/mL) and time (after 24 and 48 h) of exposure, was observed,
as well as a substantial increase of early and late apoptotic cells [254].
Multi-walled carbon nanotubes have also been implicated in
inducing apoptosis in human cells. Exposure to MWCNT decreased the
viability of human umbilical vein endothelial cells (HUVECs) and
induced apoptosis [255]. Also, as shown by the formation of γH2AX foci,
MWCNTs may likely cause DNA damage, affect malondialdehyde levels,
intracellular reactive oxygen species, and alter glutathione peroxidase
level and superoxide dismutase activity [255]. Hence, oxidative damage
pathways are the likely mechanism by which MWCNTs induce genotoxic
and cytotoxic effects in HUVECs. In addition, cytotoxicity effects of
MWCNTs on human embryonic kidney cell lines (HEK293) have been
reported [256]. Exposure of HEK293 to different sizes of MWCNTs at
different concentrations caused a concentration-dependent reduction in
the cell viability, with a concomitant increase in oxidative stress. Again,
the effects of multiwall carbon nano-onions (MWCNOs) and MWCNTs
were assessed on human skin fibroblast cells. The exposure of the cells to
MWCNO and MWCNT was reportedly involved in the activation of genes
responsible for metabolism, cell cycle regulation, cellular transport, and
stress response [257]. In general, exposure to CBMs, particularly at high
concentrations over some time, could likely result in sub-lethal injuries,
including inflammation, photosensitization, and induction of oxidative
A.O. Egbedina et al.
stress [258].
5. Challenges
Despite the significant progress made in the fabrication and appli­
cation of engineered carbon materials, some limitations need to be
overcome to maximize their vast potential. These include safety and
toxicological implications and limited understanding of carbocatalysis,
reaction mechanisms, and surface chemistry.
1. Safety and toxicity of CBMs – To a large extent, toxicity results from
the small size, large surface area, and high concentration of these
carbon-based materials. For instance, nanodiamonds have been re­
ported to cause damage in stem cells. On the other hand, graphene
nanomaterials have been reported to kill tumor cells and facilitate
targeted drug delivery but have also led to decreased fertility in fe­
male mice. Furthermore, while some studies indicated no toxicities
with graphene in-vitro studies, others presented contrasting findings.
These variations further suggest that extensive research needs to be
conducted on the cytotoxicity of carbon materials [259].
2. The mechanism of carbocatalysis and the synthesis of carbon-based
materials are pretty complex and not adequately understood. This
is perhaps aided by the lack of standardization and regulatory
framework. For instance, in environmental studies, there are hun­
dreds of graphene composites being fabricated and tested for
adsorption of different pollutants – mostly one group at a time, with
varying, sometimes contrasting results, making it daunting to
streamline and identify the most efficient materials, their surface
chemistry, and optimal synthetic route.
3. Also, limited knowledge of reaction mechanisms and inadequate
standardization probably contribute to the bias in applying carbon-
based materials in lab-scale studies rather than industrial-scale
field applications - particularly fullerenes, CNTs, graphenes, and
nanodiamonds.
4. Better understanding and control of surface chemistry are needed.
This will potentially improve tunability, reduce agglomeration and
prevent these materials from losing their intrinsic properties during
synthesis. In addition, surface chemistry plays an essential role in
determining physicochemical behavior and electrochemical perfor­
mance when used in supercapacitors for materials such as graphene.
6. Prospects and recommendations
Carbon materials can be used as additives, supports, composites,
scaffolds, and reactive barriers in different fields such as environmental
studies and biomedicine. This is particularly relevant in advanced
oxidation processes, for instance, where they can facilitate the slow
release of chemicals to degrade organic contaminants and/or adsorption
of toxic metals. Graphene is a good candidate, particularly when used as
composites and permeable reactive barriers for removing contaminants
such as phenols, antibiotics, and PAHs. It is more effective than when
used in its pristine form or as reduced graphene oxide. In contrast,
graphene could act as an impermeable barrier in therapeutic studies, in
which case, graphene scaffolds need to be degraded post cell prolifera­
tion. To this end, the development of multifunctional carbon-based
materials, such as functionalized polymer-composited nano adsorbents
should be prioritized.
Eco-friendly, green synthesis of carbon materials using biodegrad­
able waste precursors could pioneer a new generation of green and
sustainable electronic devices and support electronic waste manage­
ment. For electronic applications, CBMs synthesized from waste- mate­
rials can be potentially used as nanofillers in electrical devices. Future
research into greener synthesis routes should pay attention to the
principles of green chemistry by exploring the use of greener feedstock,
less toxic solvents, and improvement in energy efficiency, amongst
others.
12
Journal of Environmental Chemical Engineering 10 (2022) 107260
Environmental monitoring and sensing are other exciting aspects
where carbon materials could find extensive relevance. Most studies on
carbon materials have focused more on removing dyes and toxic metals
from water and wastewater. However, it is also pertinent to pay atten­
tion to their application to eliminate emerging contaminants and
micropollutants such as antibiotics, per- and polyfluoroalkyl substances
(PFAS), and disinfection by-products. Also, the applications of CBMs for
gas-phase reactions are an exciting and burgeoning area of research.
Thus, carbon nanotubes are potentially suitable candidates for consid­
eration owing to their ability to absorb gases.
Cancer research and targeted drug delivery are receiving attention in
biomedicine, evidenced by enormous research output. One clear
advantage of carbon-based nanomaterials over conventional carriers in
this area of research is their large surface area and potential for strong
non-covalent bonding with proteins, which facilitates delivery of anti­
gen to antigen-presenting cells. This opens up the possibility of anti-
tumoral ‘in-situ vaccination’ – a potentially significant and exciting
area of cancer research.
Three-dimensional fully-carbon architectures, which involve pre­
paring materials with a 3D configuration, hold promise because they
possess significantly improved surface chemistry, reduced aggregation,
and large surface area with the potential for accelerated throughput.
Other areas for future applications include aviation/airspace - where
CBMs can be used to monitor potential structural defects in airplanes to
prevent in-flight failure and assemble aircraft wings cheaply and effi­
ciently; maritime - for coating marine structures to reduce corrosion;
and energy storage devices/supercapacitors. Composites of CBMs and
dichalcogenides, for example, could be used as solar paint, presenting a
renewable energy source capable of generating electricity [260].
7. Conclusion
A large number of carbon-based materials, including graphene,
CNTs, CNFs, biochar, and fullerene, have been extensively utilized in
various fields of science owing to their specific properties such as large
specific surface areas and tunable pore structure. They have proved to be
promising materials for addressing world challenges such as environ­
mental pollution, global warming, and fuel and energy shortages.
Despite the advances made, there are still a number of obstacles to
overcome, such as improving their mechanical strength, energy den­
sities, and adsorption capacities to compete with existing materials
utilized in these industries. Moreover, as the applications of CBMs in
various fields continue to grow, there is the likelihood of exposure that
negatively affects humans, animals, and the environment. Thus,
continuous appraisal of the risk and toxicity of CBMs would hasten the
development of regulations to produce, handle, and use CBMs safely. In
addition, understanding and optimizing synthetic methods for CBM
production to produce materials that can be modified irrespective of
precursors for specific applications is critical to achieving these. This
process would ultimately promote large-scale production, widespread
use, and open up new application areas and ensure maximum efficiency.
Declaration of Competing Interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Acknowledgments
The authors thank CNPq, CAPES, and FAPERGS for financial support
and fellowships.
A.O. Egbedina et al. Journal of Environmental Chemical Engineering 10 (2022) 107260

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