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Editor: Giovanni Palmisano Wastewater remediation and pollutants removal, such as organic pollutants and heavy metals, have become
increasingly important or the protection o environment. Numerous technologies, such as adsorption, membrane
Keywords: separation and photocatalysis, have been proposed to solve this problem. However, these methods also have
g-C3N4 some disadvantages, such as the inability to mineralize the pollutants during the adsorption process and the
Modication strategies
serious membrane ouling. Thereore, g-C3N4 as a photocatalyst has been widely used to remove pollutants rom
Water remediation
wastewater due to graphitic like structure, adjustable morphology, low cost, acile preparation and high chemical
Removal mechanisms
stability. However, the pristine g-C3N4 suers rom issues such as small specic surace area, low utilization o
visible light and serious photogenerated carrier recombination. Hence, various modication strategies, such as
doping, deects, morphology control, metal deposition and heterojunction construction, have been developed to
improve its photocatalytic activity. In this review, the synthesis and modication techniques o novel g-C3N4
materials were systematically introduced. Their application and related mechanisms in wastewater remediation
and pollutant removal were discussed. Their eciency, limitations and advantages were also compared and
discussed. Furthermore, the promising perspectives and the potential directions o g-C3N4-based materials in
environmental applications were put orward and discussed. In the uture, materials modications through su-
pramolecular sel-assembly method and S-scheme heterojunction structure still need to be urther explored. And
it is o great signicance or industrial applications to design new processes that are conducive to material re-
covery and simultaneous treatment o multiple pollutants.
* Corresponding author.
** Corresponding author at: National Engineering Research Center o Industrial Crystallization Technology, School o Chemical Engineering and Technology,
Tianjin University, Tianjin 300072, People’s Republic o China.
E-mail addresses: wangna224@tju.edu.cn (N. Wang), hongxunhao@tju.edu.cn (H. Hao).
https://doi.org/10.1016/j.jece.2022.108782
Received 5 August 2022; Received in revised orm 7 October 2022; Accepted 13 October 2022
Available online 17 October 2022
2213-3437/© 2022 Elsevier Ltd. All rights reserved.
J. Xing et al. Journal of Environmental Chemical Engineering 10 (2022) 108782
sodium persulate, which urther increase the cost, and the low regen- that the C and N atoms in g-C3N4 are hybridized with sp2 to orm a
eration eciency o Fe(II)/Fe2+ also limits the reaction eciency [12]. highly delocalized π-conjugated system, and the conduction band (CB)
Harsh experimental conditions during catalytic wet air oxidation and and valence band (VB) are mainly composed o the Pz orbitals o C and
SCWO increase costs and remain a signicant challenge when operating N, respectively, so that the g-C3N4 has a suitable optical bandgap (about
at ambient temperatures.[10,11] In addition, ozone-based AOPs have 2.7 eV) and can absorb visible light less than 460 nm [19].
problems such as poor utilization rate, high process cost and high energy The g-C3N4 only contains C and N elements that are abundant on
consumption, and may also produce some harmul by-products [13]. earth, and its surace activity can be changed without signicantly
However, semiconductor photocatalysis technology driven by solar en- changing its composition and structure.[21] However, g-C3N4 is con-
ergy, which is inexhaustible clean energy, has been widely used in structed by C and N atoms alternating with each other, which results in
recent years to remove pollutants rom wastewater due to its low cost its poor electrical conductivity poor. The photo-generated electrons in
and environmental riendliness [1]. the bulk phase need to consume a large amount o energy to migrate to
Up to now, a variety o semiconductor photocatalysts have been the surace, which reduces the reduction potential energy o the
developed, such as TiO2,[14] ZnO,[15] SnO2,[16] CdS,[17] MoS2,[18] photo-generated electrons. Moreover, the chemical reaction can occur
and g-C3N4.[19] Among them, UV light-responsive photocatalysts such only when the photogenerated electrons migrate rom the bulk phase to
as TiO2 and ZnO have been widely studied due to their strong chemical the catalyst surace. Thereore, or the pristine g-C3N4, only ew pho-
stability, non-toxicity and low cost. However, the wide band gap o TiO2 togenerated electrons are transerred to the surace, resulting in a low
and ZnO limit their urther applications. To urther improve the utili- quantum yield. Although g-C3N4 has many advantages and many po-
zation o solar energy, researchers have developed a series o tential applications, the pristine g-C3N4 still exhibits poor photocatalytic
visible-light-driven catalysts, among which the metal-ree g-C3N4 has activity due to the problems o small specic surace area, ast recom-
attracted great attentions as a visible-light-responsive organic polymeric bination o photogenerated carriers and low utilization o visible light.
semiconductor photocatalyst. Since the rst successul application o [25] In order to solve the above problems and improve the photo-
g-C3N4 in photocatalytic water splitting or hydrogen production in catalytic eciency, many researchers have proposed dierent modi-
2009 by Wang et al. [19], the g-C3N4-based materials have become one cation strategies, such as doping, deects, morphology control, metal
o the popular materials in the eld o photocatalysis due to its suitable deposition and heterojunction construction, especially advanced
optical band gap, non-toxicity, low cost and high chemical stability. And S-scheme heterojunction.
it has also been widely used in the eld o wastewater treatment. Based on the above background, this paper mainly reviews the latest
In 1996, Teter and Hemley proposed ve theoretical structures o development o g-C3N4-based materials which are applied to treat the
carbon nitride, namely α-C3N4, β-C3N4, g-C3N4, cubic C3N4 and the pollutants in wastewater, as well as its working mechanism in the eld
quasi-cubic phase C3N4. And their relative stability, structure, and o wastewater treatment. Meanwhile, the preparation and modication
physical properties were urther calculated based on the rst-principle, methods o g-C3N4 are systematically introduced. Finally, the applica-
and it was ound that g-C3N4 was the most stable one at normal tem- tion prospects and uture directions o g-C3N4-based materials in water
perature and pressure.[20] Generally, g-C3N4 has graphene-like layered remediation are also proposed.
planar structure, and the interlayer is connected by van der Waals
interaction and/or hydrogen bonding while the C and N atoms in the 2. Synthesis and modication
plane are connected by covalent bonds to orm a triazine ring (C3N3) or
tri-s-triazine ring (C6N7) (Fig. 1) [21–23]. Moreover, the stacking o As a polymer semiconductor containing only C and N, g-C3N4 does
interlayer van der Waals interactions makes g-C3N4 highly chemically not exist naturally in nature and needs to be synthesized experimentally.
stable, resistant to acids and alkalis, and insoluble in most solvents [24]. At present, the precursors used to prepare g-C3N4 mainly include mel-
Meanwhile, the large interlayer distance limits the transer o photo- amine,[26] urea,[27] dicyandiamide,[28] cyanamide,[19] thiourea,
generated electrons between layers, so that they can preerentially move [29] etc. And the main synthesis methods are thermal polycondensation
reely on the plane. Additionally, g-C3N4-based materials exhibit method,[26] solvothermal method,[30] solid-phase synthesis method
excellent thermodynamic stability, and the theoretical calculated energy [31] and electrochemical deposition method.[32] Among them, the
o g-C3N4 based on the tri-s-triazine ring structural unit is much lower, thermal polycondensation method is commonly and widely used
about 30 kJ mol1.[21–23] And it starts to decompose above 600 ◦ C, because o the advantages o cheap and easy-to-obtain raw materials,
and completely decomposes at 750 ◦ C. Theoretical calculations show simple and easy-to-control preparation process, and suitability or
2
J. Xing et al. Journal of Environmental Chemical Engineering 10 (2022) 108782
large-scale industrial production. However, the g-C3N4 catalyst products using melamine and cyanuric chloride as raw materials at
synthesized by this method usually have small specic surace area and 1–1.5 GPa/500–600 ◦ C [31]. However, the reaction pressure o the
serious recombination o photogenerated carriers, which restricts its solvothermal method is very high (> 10,000 times atmospheric pres-
urther development. Thereore, the development o new methods or sure) and the conditions are extremely harsh. On the contrary, the
g-C3N4-based materials that can eectively improve the visible light electrochemical deposition method is more suitable or the industrial
absorption ability and redox ability and promote the ecient separation production o g-C3N4 with good application prospects. It can be carried
o electrons and holes, has been the ocus o research in this eld. out under normal pressure and low temperature with ecient and mild
reaction conditions, etc. Bai et al. successully synthesized hollow car-
2.1. Synthesis o g-C3N4 bon nitride microspheres with particle size o 80–250 nm, which were
consisted o nanoparticles with particle size o 5–30 nm, by liquid-phase
The common method or preparing g-C3N4 is to heat treatment o electrodeposition technology [32].
nitrogen-rich precursors (such as melamine, urea, cyanamide, dicyan-
diamide, thiourea, etc.) (Fig. 2),[21] such as high-temperature calcina- 2.2. Modifcation o g-C3N4
tion. Although the chemical reaction process is relatively complicated,
the high-temperature calcination has the advantages o low cost, mild Although g-C3N4 has many advantages, it also has many disadvan-
reaction conditions, and easy control. Moreover, the properties o the tages such as small specic surace area, low utilization rate o visible
obtained g-C3N4 are closely related to the types o precursors and re- light and serious photo-generated carrier recombination, which limit its
action parameters. Some researchers ound that, compared with the practical application. Thereore, dierent modication methods have
calcination o melamine at 450–550 ℃ in nitrogen, calcining g-C3N4 at been developed to improve its photocatalytic activity. The commonly
600 ℃ and 650 ℃ not only enhances the visible light absorption, but used modication strategies o g-C3N4 include doping,[33] deects,[34]
also narrows the band gap.[26] Furthermore, many researches have morphology control,[35,36] metal deposition,[37] and heterojunction
suggested that the g-C3N4 synthesized by heat treatment with urea as the construction [38].
precursor has an optimal calcination temperature (550 ℃).[27] At this
temperature, the specic surace area o the g-C3N4 is signicantly 2.2.1. Doping Strategies
increased, and its optical band gap is signicantly reduced.[27] And
compared with using urea as precursor, the band gap o g-C3N4 prepared In the modication strategy o g-C3N4, doping is an eective method
with thiourea as the precursor is smaller, and the catalytic perormance to adjust the band gap o g-C3N4, which can eectively broaden the light
is higher.[29] Additionally, a ew studies have indicated that the calci- absorption range and speed up the eective separation o photo-
nation atmosphere may also lead to structural disorder and deects, generated carriers. Doing strategies can be mainly classied into
which can urther aect the structure and properties o g-C3N4.[21]. element doping at the atomic level and copolymerization at the mo-
Solvothermal, solid-phase synthesis and electrochemical deposition lecular level [39].
methods can also be used to prepare g-C3N4. The solvothermal method
has the characteristics o good raw material dispersibility and uniorm 2.2.1.1. Element doping
reaction process, and the product can be controlled by changing the
solvent. Montigaud et al. attempted to use triethylamine as the solvent As an eective strategy to adjust the band gap o g-C3N4, element
to condense melamine and cyanuric chloride to prepare graphite-like g- doping has been extensively studied by many researchers. Element
C3N4 as macroscopic sample under supercritical conditions doping can adjust the band structure o g-C3N4 by regulating the lowest
(P = 130 MPa, T = 250 ℃).[30] However, the crystallinity o the nal unoccupied molecular orbital (LUMO) and the highest occupied mo-
product was low due to the partial condensation.[30] Subsequently, lecular orbital (HOMO).[40,41] It can also aect its surace properties,
they tried to use hydrazine as solvent, and successully obtained brown thereby enhancing its photocatalytic perormance [40,41]. Element
black solid with structure similar to the theoretical g-C3N4 through py- doping mainly includes metal doping, such as transition metals, rare
rolyzing melamine at high temperature and high pressure (P = 2.5 GPa, earth metals, alkali metals, etc., non-metal doping, such as P, B, S, O, C,
T = 800 ℃) [30]. Zhang et al. synthesized g-C3N4 with high crystallinity N, halogen etc. and co-doping.
Fig. 2. Schematic illustration o the synthesis process o g-C3N4 by melamine, cyanamide, dicyanamide, urea, and thiourea.
Reproduced with permission rom re. [21], Copyright © 2016, American Chemical Society.
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J. Xing et al. Journal of Environmental Chemical Engineering 10 (2022) 108782
(1) Metal element doping which can eectively improve the degradation o pollutants, and reduce
The introduction o metal impurities into g-C3N4 will generate the leaching o Co during recycling (Fig. 3a-c) [43]. In addition, rare
additional binding eects to orm metal-Nx active sites, which can earth metals are also considered as ideal dopants because the unoccu-
accelerate the charge transer and narrow the band gap to enhance the pied 4 s orbitals and the vacant 5 s orbitals can act as electron trapping
light absorption ability and improve the adsorption capacity or the centers [45,46]. Wang et al. introduced Eu(III) species into g-C3N4 to
reactants, thereby improving the photocatalytic activity [42]. g-C3N4 deorm the nanosheets into hollow lanterns, which could increase the
has six electron-rich N-atoms cavities, which can provide stable coor- specic surace area and orm the impurity energy level [46]. Compared
dination environment or transition metals.[43] Yu et al. perormed with the pristine g-C3N4, the absorption edge o Eu-doped g-C3N4
atomic structure engineering modication by doping transition metals showed a signicant red shit, resulting in narrower band gap and
(Fe, Co or Ni) into g-C3N4, which can induce the ormation o metal-N shorter electron transport distance, which could urther improve the
bonds as the "electron transer bridges".[44] And the "electron transer degradation eciency o rhodamine B to 98% and increase the degra-
bridges" can act as new reactive sites to signicantly enhance the sep- dation eciency by 5-olds [46].
aration eciency o photogenerated charges, restorative ability and Alkali metals are also commonly used to modiy g-C3N4 due to their
light absorption range [44]. It was ound that the Co-doped g-C3N4 has advantages o non-toxic and low-cost. Generally, alkali metal has strong
the highest photocatalytic activity. This is because that, when Co is interaction with the C-N heterocyclic structure o g-C3N4, which can
introduced into g-C3N4 to activate peroxymonosulate (PMS), the strong narrow the band gap and change the electronic structure, so as to
coordination o N atoms can signicantly improve the stability o Co, improve the utilization o visible light and broaden the visible light
Fig. 3. (a) Schematic diagram o Co-NG activation o PMS; (b) BA degradation and (c) Co leaching in ve consecutive experiments o the Co-NG catalyst.
(a-c) Reproduced with permission rom re. [43], Copyright © 2020, Elsevier.
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J. Xing et al. Journal of Environmental Chemical Engineering 10 (2022) 108782
response range [47]. Moreover, they are urther used or the separation suppress the separation o photogenerated carriers.[51,52] Commonly
o highly polycondensed stacking materials due to their intercalation used phosphorus sources are phosphoric acid, phosphate, etc. The
properties [48]. Wu et al. ound that the peeling and delamination o introduction o B can not only reduce the band gap but also increase the
tube walls can be achieved by changing the g-C3N4 interlayer spacing specic surace area o the catalyst.[53] Generally, in the preparation
through potassium ion-regulated supramolecular sel-assembly and process o B-doped g-C3N4, H3BO3 and BH3NH3 are oten used as boron
thermal polymerization process [48]. DFT calculations showed that the sources. In addition, since the decomposition temperature o H3BO3 and
N atom in g-C3N4 exhibited anionic properties, which could enhance the volatilization temperature o H2O are almost the same, the use o
ionic interactions between K-N (Fig. 4a, b) [48]. And the decrease o boric acid is conducive to the ormation o porous materials.[40] Yellow
work unction also indicated that less energy was required or electrons sponge-like B-g-C3N4 can be obtained by one-pot thermal poly-
to escape rom the bulk phase o the material to the surace, and the condensation o dicyandiamide, NH4Cl and BH3NH3.[53] The S-doped
binding orce was weaker (Fig. 4c, d), so that the electrons were more g-C3N4 is mainly realized by replacing the N atoms with S atoms. And
easily separated and transerred to the photocatalyst surace.[48] the introduction o S can increase the specic surace area, and reduce
Furthermore, the K 2p orbital also played an important role in the CB o the band energy, enhance the light absorption ability and promote the
the material, and the CB was staggered with the ermi level, which was separation o photogenerated carriers with the interaction between the
conducive to the separation o photogenerated carriers (Fig. 4e, ).[48] 2p state o S and the 2p state o N.[40] Usually, various sulur sources
Meanwhile, multi-metal atom doping could urther enhance the pho- such as thiourea, H2S, and thiocyanate can be used or S doping. Wang
tocatalytic activity o g-C3N4 due to the synergistic eect between et al. ound by DFT calculation that the photocatalytic perormance o
metals. The addition o Co/V to g-C3N4 could induce bimetallic syner- S-doped g-C3N4 nanosheets was signicantly improved.[54] Compared
gistic regulation o electronic structure, promote the transer and sepa- with the pristine g-C3N4, the introduction o S atoms made the band gap
ration o photogenerated electron-hole pairs and enhance the become smaller (Fig. 6a, b) and the ermi level transer to the bottom o
photocatalytic activity [49]. However, the introduction o oreign metal the CB (Fig. 6c, d), which indicated that it might have a stronger ability
elements is not always benecial to improve the photocatalytic activity. to reduce electrons.[54] Moreover, except or the N atoms surrounding
The addition o alkali metals (Na, K, Rb, and Cs) into g-C3N4 fakes the S atoms, HOMO is mainly distributed on other N atoms, while LUMO
destroyed the mesoporous properties o the fakes and changed the op- is mainly distributed on S atoms (Fig. 6e), indicating that S atoms
tical properties and the electronic properties o the material (Fig. 5a, b) participate in the composition o CB and make the orbital distribution
[50]. This is because the photogenerated electrons may be captured by change obviously, and e-/h+ separate signicantly.[54] Oxygen-doped
alkali metal ions, which inhibits the transer o charges to the reaction one-dimensional porous g-C3N4 nanorods can be obtained by direct
site (Fig. 5c, d) and aects the ormation o active species (Fig. 5e, ) calcination o melamine nanobers which were precipitated in mel-
[50]. amine aqueous solution.[55] Since the doping o oxygen atoms into
(2) Non-metal element doping g-C3N4 breaks the symmetry o the pristine g-C3N4, the separation e-
Due to the problems o metal ion leaching in metal doping, re- ciency o photogenerated electron-hole pairs is improved and the bulk
searchers have also developed the non-mental doping strategies. The structure stacking problem is also overcome.[55] In successul cases,
most prominent eature o non-metal doped g-C3N4 is that the metal-ree halogen atoms (F, Cl, Br or I) are also commonly used to embed g-C3N4.
nature o g-C3N4 is maintained when improving the photocatalytic ac- [56] For the halogen-doped g-C3N4 monolayer, it is most stable when
tivity. The introduction o P atoms into the g-C3N4 network can reduce halogen atoms occupied the interstitial space surrounded by three
the energy band gap, improve the light absorption perormance and tri-s-triazine units.[56] And the introduction o halogen atoms changes
Fig. 4. The ELF o CN (a) and KCN (b); the scale o ELF between 0 and 1, corresponding color card range goes rom blue to red; the work unction o CN (c) and KCN
(d); the partial density o states (PDOS) o CN (e) and KCN (d).
(a-) Reproduced with permission rom re. [48], Copyright © 2021, Elsevier.
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J. Xing et al. Journal of Environmental Chemical Engineering 10 (2022) 108782
Fig. 5. (a) DRS plots or GCN and MGCN10 (M = Na, K, Rb and Cs) sheets; (b) band diagram; (c, d) proposed mechanism or the degradation o AR 94 over GCN and
MGCN photocatalysts; (e, ) pseudo rst order kinetics tting.
(a-) Reproduced with permission rom re. [50], Copyright © 2021, Elsevier.
Fig. 6. Band structure o g-C3N4 (a) and S-doped g-C3N4 (b); PDOS o g-C3N4 (c) and S-doped g-C3N4 (d); (e) LUMOs and HOMOs o g-C3N4 and S-doped g-C3N4.
(a-e) Reproduced with permission rom re. [54], Copyright © 2018, American Chemical Society.
the density o states and redistributes LUMO and HOMO (Fig. 7a-d).[56] study ound that, or C-doped g-C3N4, the color o the product gradually
Due to the large electronegativity o the F atom, it tends to occupy the deepened with the increase o carbon content (Fig. 8a).[58] The
VB and LUMO, while Cl, Br and I participate in the CB and LUMO, which mechanism o C sel-doped g-C3N4 with high light absorption ability and
eventually can narrow the band gap (Fig. 7e-h), enhance visible light eective charge separation lies in that the C atom can enter the g-C3N4
absorption capacity and improve the photocatalytic eciency o the network by substituting the bridged N atoms or replace the N atoms at
material.[56]. the end, then orm large delocalized π bonds between adjacent heptazine
(3) Self-doping strategies rings, which can urther overcome the problems o poor visible light
Since the introduced oreign element may become into the photo- response and serious photo-generated carrier recombination.[58–60]
generated carriers’ recombination centers and reduce the photocatalytic Using chitosan as carbon source, melamine and chitosan are dissolved in
eciency, many researchers have pioneered the sel-doping strategy o water or supramolecular sel-assembly or direct mixing, then the C
C and N atoms. Mohamad et al. prepared biomimetic carbon-doped sel-doped g-C3N4 is obtained by thermal polycondensation treatment
graphitic carbon nitride with mesoporous microstructure by hydro- (Fig. 8b).[58,59] Additionally, glucose is also commonly used as carbon
thermal method using urea as precursor and kapok ber as biological source or the preparation o C sel-doped g-C3N4.[60] Some researchers
template and carbon source, respectively.[57] And the mesoporous have prepared C sel-doped graphitic carbon nitride nanotubes by hy-
microtubule structure and in-situ C doping signicantly enhanced the drothermal treatment o melamine and glucose, which resulted in the
light-harvesting ability in the near-inrared band.[57] The experimental redshit o the absorption edge, narrowed the orbidden band width and
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J. Xing et al. Journal of Environmental Chemical Engineering 10 (2022) 108782
Fig. 7. Calculated HOMO o (a-1) F-, (b-1) Cl-, (c-1) Br- and (d-1) I- doped g-C3N4. Calculated LUMO o (a-2) F-, (b-2) Cl-, (c-2) Br- and (d-2) I- doped g-C3N4. The
isovalue is set as 0.05 electron/Å3; (e-h) calculated band structure and corresponding DOS o halogen interstitial-doped monolayer o g-C3N4.
(a-1-d-1, a-2-d-2, e-h) Reproduced with permission rom re. [56], Copyright © 2017, Elsevier.
suppressed the recombination o photogenerated carriers (Fig. 8c, ). also be improved [21,67].
[61] The introduction o N atoms will make the π-conjugated system o Inspired by the Schi base chemistry, Wang et al. used copolymeri-
the copolymer expand and delocalize, enhance the light-harvesting zation to extend the π-conjugated structure o g-C3N4.[68–72] They used
ability and suppress carrier recombination.[62] Meanwhile, the melamine, dicyandiamide, cyanamide and urea as precursors to copo-
doping o N atoms can urther cause the redistribution o charges around lymerize with a series o polymerized monomers, such as barbituric acid
the doping point.[63] The substitution o N generally introduces itsel (BA), 2-aminomaleonitrile (ABN), 2-aminothiophene-3-carbonnitrile
into the inter-band state, which will signicantly shorten the transer (ATCN), 2,6-triaminopyridine, etc [68–72]. The extended π-conju-
path o photogenerated electrons and is benecial to the separation o gated system also promoted the red-shit o light absorption and
electron-hole pairs.[63] Both experiments and theoretical calculations improved the charge separation eciency, by introducing the aromatic
showed that the band gap o N sel-doped g-C3N4 was reduced rom the motis ATCN into the nanoshells o carbon nitride hollow nanospheres
original 2.51–1.82 eV.[63]. [68]. With the development o g-C3N4 modication strategies, a growing
(4) Polyatomic Doping number o organic comonomers were used to copolymerize with g-C3N4
In recent years, polyatomic doping [64–66] o g-C3N4, by intro- to modulate the π-conjugated system o g-C3N4, such as malondiamide
ducing dierent atoms and then introducing a simple donor-acceptor (MLDD),[73] thiophene,[74] ormamide,[75] etc. Li et al. introduced
co-doping, has also attracted extensive attentions. Compared with MLDD and urea into the melon networks through a special polymeri-
single-element doping, the co-doping can urther reduce the band gap, zation reaction (Fig. 9a) [73]. It shows that the introduction o bridged C
suppress photogenerated carriers recombination, and synergistically replaces the original bridged N, a highly electronegative sp3 hybrid,
expand the visible light response range [40]. Hu et al. obtained a highly which can enhance the conjugation o the system and improve the en-
visible-active and eective metal-ree photocatalyst with the co-doped S ergy band structure (Fig. 9b) [73]. In addition, the bridged C generated
and P in g-C3N4 by thermal condensation.[64] In the heptazine ring unit, more structure edge deects, endowing the material with abundant pore
P replaced C to orm a new covalent bond with N, while S was located at structure and huge surace area (Fig. 9c, ) [73]. It can be seen that
the interstitial sites with relatively weak bonding with N, which was molecular doping can eectively control the physical and chemical
prominently able to enhance the charge transer through the properties o g-C3N4, such as specic surace area, band gap structure
N-S-N-C-N-P pathway to cross the heptazine ring or the photocatalytic and electronic structure.
reaction [64]. Fang et al. synthesized (Na, O)-g-C3N4 with tremendously
improved photocatalytic hydrogen production activity by co-doped Na 2.2.2. Defects regulation strategies
and O in g-C3N4 using solvothermal method [66]. And the apparent
quantum yield was as high as 22.3% at 420 nm, under visible light [66]. It was ound that intrinsic deects are eective in promoting the
transer and separation o charges in the plane or between layers.[74] It
2.2.1.2. Copolymerization regulation strategies can also broad the photoresponse range and provide more reactive sites.
[74] Generally, the introduction o intrinsic deects will aect the
It is well known that the photocatalytic activity o pristine g-C3N4 electronic structure o g-C3N4, change the positions o CB and VB, aect
mainly comes rom the π-conjugated structure [21]. Copolymerization the size o the band gap and regulate the redox ability and visible light
regulation strategy is based on the π-conjugated structure o g-C3N4. absorption ability o photogenerated carriers. In addition, the deects
Through copolymerization with another structure-matching molecule will act as electron or hole traps to optimize the conjugated system o
(aromatic or organic small molecule), the electron delocalization o the g-C3N4, and promote charge redistribution and the participation o
π-conjugated structure can be broadened [21,67]. The light absorption electrons in photocatalytic reactions.[74] Vacancy deects (such as N
and the separation eciency o photogenerated electron-hole pairs can vacancies,[75–78] C vacancies,[79,80] cyano deects,[78] etc.), are the
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J. Xing et al. Journal of Environmental Chemical Engineering 10 (2022) 108782
Fig. 8. (a) Photographs o g-C3N4 and CCNx; (b) scheme illustration o carbon bridged g-C3N4. (c) UV–vis DRS spectra, (d) XPS valence band spectra, (e) band
structure alignments o CNT and C-CNT-0.01, and () PL spectra o CNT and C-CNT-x (x = 0.005, 0.01, 0.02 and 0.03).
(a, b) Reproduced with permission rom re. [58]. Copyright © 2018, Elsevier. (c-) Reproduced with permission rom re. [61]. Copyright © 2019, Elsevier.
main regulation means. And the vacancy deects will be mainly dis- but also help to orm more reactivity sites and shorten the photo-
cussed as a result o the elaboration o C or N sel-doping in the element generated carrier transer distance.[78] However, excessive deects may
doping section. increase the risk o reduced photocatalytic activity. Thereore, how to
The introduction o C deects in g-C3N4 could weaken the interlayer balance various actors and optimize the overall photocatalytic peror-
periodic stacking and the internal conjugation system o g-C3N4, adjust mance is worth urther exploration.[74].
the energy change o molecular structure and signicantly improve the
photocatalytic perormance o g-C3N4.[79] Liao et al. successully 2.2.3. Morphological regulation strategies
introduced N deects into the g-C3N4 ramework by heating g-C3N4
powder in hydrogen atmosphere to make the N atoms react with Generally, photocatalytic reactions occur on the surace o semi-
hydrogen and be partially removed. The N deects were located at N2 C, conductor catalysts, and the microscopic morphology and size are
and can be regulated by the hydrogen treatment temperature.[75] closely related to the specic surace area and the exposed reactive sites
Compared with the pristine g-C3N4, the band gap o the obtained o the material, which can aect its photocatalytic perormance. The
product was narrower and both the photo-generated carrier separation specic surace area o bulk g-C3N4 prepared by thermal poly-
ability and the active oxygen generation ability were improved. More- condensation method is about 10 m2 g1, which is not sucient or
over, atomic layered g-C3N4 containing N vacancies and cyano deects, providing catalytic reaction active sites. The morphological regulation
synthesized by high temperature treatment and thermal exoliation, has o g-C3N4 is an eective means to improve the specic surace area. It is
excellent absorption wavelength with 650 nm.[78] These vacancies also a promising method to urther improve the photocatalytic activity
and/or deects can not only suppress the quantum size eect o g-C3N4, o g-C3N4. The morphologies o g-C3N4 mainly include 0D (quantum
8
J. Xing et al. Journal of Environmental Chemical Engineering 10 (2022) 108782
Fig. 9. (a) Illustration or abrication o GCN and CBCN samples; (b) scheme illustration o carbon-bridging modied g-C3N4 nanosheet; SEM images o (c) GCN and
(d) CBCN-30, TEM images o (e) GCN and () CBCN-30, SEAD images o CBCN-30 (inset o ).
(a-) Reproduced with permission rom re. [73], Copyright © 2020, Elsevier.
9
J. Xing et al. Journal of Environmental Chemical Engineering 10 (2022) 108782
dots, QDs), 1D (nanorods, nanobers, nanotubes), 2D two-dimensional topographic height o 1.5–2.5 nm.[86] Moreover, the tunable emission
(nanosheets) and 3D (porous materials). And g-C3N4 with dierent o g-C3N4 QDs can be achieved by adjusting the ratio o reactants.[86]
morphologies can be transormed into each other. Microwave processing is also commonly used to synthesize g-C3N4 QDs.
Li et al. prepared oxygen and sulur co-doped green luminescent g-C3N4
2.2.3.1. 0D g-C3N4 QDs by microwave treatment o thiourea and citric acid.[87] Tang et al.
obtained g-C3N4 QDs with a fuorescence quantum yield up to 35% by
0D g-C3N4, also known as g-C3N4 QDs, is a new type o material with microwave-assisted preparation using EDTA and guanidine hydrochlo-
a size o less than 10 nm. And the smaller size can generate strong ride as precursors, and realized the sensitive detection o ree chlorine in
quantum connement and edge eects, making it possess controllable water by injecting them into NaClO.[88].
optical, electrical and thermal properties, so that the solar spectrum can
be ully utilized and its applications in the eld o photocatalysis can be 2.2.3.2. 1D g-C3N4
promoted [20,81,82]. In addition, the electrons and holes o g-C3N4 QDs
can’t move reely, and their CB and VB are opposite to those o bulk Beneting rom the one-dimensional structure that enables electrons
g-C3N4, leading to obvious dierences in the photophysical properties to move reely in the axial direction without lateral migration, 1D g-
and photogenerated carrier separation o g-C3N4 QDs.[35]. C3N4 can signicantly improve the photo-generated carrier separation
The current synthesis methods o g-C3N4 QDs mainly include top- eciency in photocatalytic reactions. And the tunability o the physi-
down and bottom-up routes.[82] Although bulk g-C3N4 can gradually cochemical properties o 1D g-C3N4 can be achieved by changing the
transorm into 2D, 1D materials and even g-C3N4 QDs by top-down precursor types, experimental parameters and other actors. At present,
methods such as ultrasound, hydrolysis, and hydrothermal treatment, 1D g-C3N4 photocatalysts include nanobers, nanowires, nanorods, and
the products obtained by ultrasound are usually mixtures or composites nanotubes.
g-C3N4 QDs and other morphologies.[83,84] Zhou et al. synthesized Mo et al. obtained g-C3N4 nanotubes with abundant specic surace
g-C3N4 QDs with C-N conjugated structure, strong electron connement area by in-suit hydrolysis to orm rod-like supramolecular intermediates
eect and uniorm morphology by hydrolysis o bulk g-C3N4 in acidic and urther calcination o melamine (Fig. 10a).[89] And light-harvesting
aqueous solution.[84] And the g-C3N4 QDs exhibited intrinsic UV ability could be enhanced through multiple refections o incident light.
emission at 367 nm and has a photoluminescence quantum yield o up to [89] Rapid and long-distance electron transer could be also achieved
46%.[84] Zhan et al. prepared g-C3N4 QDs with uniorm scale as well as and separation eciency o photogenerated carriers could be improved.
good dispersion.[85] But the process is complicated and the yield is low, [89] Subsequently, they prepared porous nitrogen-rich g-C3N4 nano-
and the steps o heat treatment, dialysis, centriugation, and tubes by supramolecular sel-assembly o melamine and hydroxylamine
reeze-drying are generally required.[85] The bottom-up route usually hydrochloride (Fig. 10b-e).[90] P-doped g-C3N4 nanotubes can also be
uses carbon and nitrogen sources as precursors to synthesize g-C3N4 QDs obtained by copolymerizing melamine with sodium hypophosphite
by solid-phase reaction, microwave-assisted methods, etc. The monohydrate (NaH2PO2⋅H2O) at high temperature, and the phosphine
solid-phase method can tune the constituent elements, size, deects, and gas generated by the thermal decomposition o NaH2PO2⋅H2O can
surace unctional groups o g-C3N4 QDs by changing the ratio o raw urther induce the transormation o 2D nanosheets to 1D nanosheets
materials, and has the advantages o simple operation, solvent-ree, and (Fig. 10).[91] However, photogenerated carrier separation is inhibited
high cost-eectiveness.[82] Heating urea and sodium citrate at 180 ℃ due to high polymer packing in the tubular structure. Fortunately, by
or 1 h in autoclave, and the g-C3N4 QDs can be obtained with a quan- introducing potassium ions in the hydrothermal reaction o melamine,
tum yield o 42%.[86] The diameter distribution range o g-C3N4 QDs is Wu et al. perectly peeled o the tube wall while ensuring the integrity
in the range o 2.6–5.5 nm, with average size o 4.3 nm, and the o the tube structure, eectively promoting the separation o
Fig. 10. (a) The ormation process o the g-C3N4 nanotubes. (b, c) SEM images o TCN (NH3) and (d) TEM images o TCN (NH3). (e) proposed ormation process o P-
g-C3N4.
(a) Reproduced with permission rom re. [89], Copyright © 2018, Elsevier. (b-d) Reproduced with permission rom re. [90], Copyright © 2019, Elsevier. (e)
Reproduced with permission rom re. [91], Copyright © 2018, American Chemical Society.
10
J. Xing et al. Journal of Environmental Chemical Engineering 10 (2022) 108782
photogenerated charges.[48] What is more, Wang et al. prepared porous supramolecular sel-assembly method.[99–102].
nanobrous Ag/g-C3N4 nanocomposites with higher specic surace By calcining the melamine three times in air, She et al. obtained high
area (18.5 m2 g1) by using a simple supramolecular hydrogel method crystalline oxygen-containing monolayer carbon nitride with increased
as a sel-template, to improve visible light absorption and the photo- gap and ecient separation o electron-hole pairs (Fig. 11a-d), with
generated carrier separation eciency.[92] Besides nanobers, nano- enhanced photocatalytic activity.[94] Meanwhile, Li et al. also obtained
tubes, nanorod and nanowire structures have also been used to enhance conventional 2D nanosheets by thermally treating bulk g-C3N4 in air or
the photocatalytic activity o g-C3N4. 1D porous g-C3N4 nanorods with a long time.[95] And with the prolongation o calcination time, some
good 2,4-dinitrophenol degradation activity can be prepared by directly tri-s-triazine units composed o C-N were urther thermally oxidized to
calcining the melamine nanobers precipitated rom melamine aqueous orm oam-like g-C3N4 ultrathin nanosheets with macroscopic
solution.[55] Zhang et al. reported a g-C3N4 nanowire that signicantly morphology and non-uniorm pore size.[95] The experimental results
promoted the separation o photogenerated carriers and eectively and the original density unctional theory (ODFT) calculation shows that
broadened the light absorption range due to the structure rearrangement the specic surace area o ultrathin nanosheets is 26 times higher than
and distortion.[93] The g-C3N4 nanowire was ormed by iodine doping that o bulk, and the porous structure can also provide more catalytically
and oxidation o g-C3N4 nanosheets.[93]. active sites, which are conducive to the rapid cross-plane diusion o
photogenerated carriers.[95] Furthermore, Xu et al. eectively exoli-
2.2.3.3. 2D g-C3N4 ated the bulk g-C3N4 into single atomic-layer nanosheet with a thickness
o only 0.4 nm, with the aid o the ultrasound and a high concentrated
2D g-C3N4 generally reers to g-C3N4 nanosheets whose electrons are suluric acid (98 wt%).[98] However, although g-C3N4 nanosheets can
mainly conned in the thickness direction.[35] At present, the prepa- be obtained by thermal oxidation and liquid exoliation, the thermal
ration methods o g-C3N4 nanosheets mainly include thermal oxidation oxidation method has disadvantages o low yield and high ultrasonic
exoliation method,[94–96] liquid exoliation method[97,98] and energy consumption, while the liquid exoliation process may use
Fig. 11. (a-d) Schematic illustration o the thermal exoliation method to orm O-g-C3N4 nanosheet.
(a-d)Reproduced with permission rom re. [94], Copyright © 2016, Elsevier.
11
J. Xing et al. Journal of Environmental Chemical Engineering 10 (2022) 108782
organic solvents, strong acids and strong bases. Moreover, the exolia- et al. introduced a acile NaCl-assisted ball-milling strategy to abricate a
tion process can’t simultaneously achieve precise control o nanosheet 3D porous g-C3N4 network (Fig. 12a), which can be used as biunctional
thickness, specic surace area, deects, and energy band structure. catalyst or both photocatalytic hydrogen evolution and electrocatalytic
Thereore, there is still a need to explore and develop ecient, oxygen evolution reaction.[106] In the ormation process, the 3D NaCl
controllable and environmentally riendly preparation methods or ul- particles acted as movable templates to promote the ormation o 3D
trathin nanosheets. porous g-C3N4 structures, which can prevent the aggregation o g-C3N4
In addition to the exoliation o bulk g-C3N4 into g-C3N4 nanosheets, during calcination.[106].
g-C3N4 nanosheets grown by anisotropy and sel-assembly o organic Generally, 3D layered porous g-C3N4 can be abricated by using
molecules have also been extensively studied in recent years. Generally, ethanol or water as solvent and melamine and cyanuric acid as pre-
melting process is involved during the direct calcination o nitrogen- cursors.[107] And cyanuric acid can also be used as a polymerization
containing precursors into g-C3N4, and the obtained g-C3N4 mostly inhibitor, to promote the ormation o the 3D g-C3N4 structure.[107]
exhibit dense block-like structure morphology. The melting point o Chen et al. obtained porous 3D g-C3N4 assembled by ultrathin nano-
supramolecular precursors ormed by melamine and cyanuric acid is sheets with high crystallinity ater reeze-drying and high-temperature
higher than the temperature at which g-C3N4 is ormed, so that the polycondensation o equal amounts o melamine and cyanuric acid
morphology o g-C3N4 can be adjusted to a certain extent by regulating using water as solvent (Fig. 12b-e).[108] The 3D porous interconnected
the morphology o supramolecular precursors.[99,100] Wang et al. open-ramework suppressed the agglomeration o nanosheets and pro-
prepared petal-like Cl-doped g-C3N4 nanosheets by adding NH4Cl to the vided a pathway or photo-generated electron transport with stable.
system o melamine and cyanuric acid.[99] The synergistic eect o [108].
supramolecular sel-assembly and Cl doping enables the specic surace
area o g-C3N4 nanosheets to be as high as 98.330 m2 g1, and the 2.2.4. Metal deposition
removal eect o rhodamine B is 5.8 times higher than that o bulk
g-C3N4.[99] Hu et al. synthesized g-C3N4 nanosheets by sel-assembly o Dierent rom the doping o metal elements into the g-C3N4 network,
melamine and L-cysteine.[100] And they ound that the g-C3N4 nano- metal deposition involves depositing the metal on the surace o the
sheets olded to orm a porous structure with more reactive sites ater semiconductor. Because the Fermi level o the semiconductor is higher
introducing enough L-cysteine.[100] However excessive L-cysteine than that o the metal, when the metal contacts with the semiconductor,
would cause unnecessary deects and structural distortions, increase the the photogenerated electrons will transer rom g-C3N4 with a higher
recombination rate o photogenerated carriers and be unavorable or Fermi level to the metal to orm a Schottky barrier. Thereore, the
the photocatalytic reaction.[100] Compared with bulk g-C3N4, g-C3N4 deposition o metals on the surace o the semiconductor can promote
nanosheets prepared based on supramolecular sel-assembly generally the separation o photogenerated carriers and improve photocatalytic
have the characteristics o larger specic surace area, abundant reactive activity.
sites, and excellent separation ability o photogenerated carriers, and Generally, depositing noble metals (such as Pt, Pd, Ag, Au, etc.) on
have great application potential in the eld o photocatalysis. However, the surace o semiconductor catalyst will urther broaden the light
the substances that can participate in supramolecular sel-assembly are absorption range o semiconductor materials thanks to the surace
still limited. Hence, it is necessary to expand the sel-assembly raw plasmon resonance eect.[37] Samanta et al. deposited Au nano-
materials and design materials with higher photocatalytic perormance. particles on g-C3N4, and the synergy o the CB minima o g-C3N4 and the
plasmonic band o Au nanoparticles made the composite material have
2.2.3.4. 3D g-C3N4 good light absorption capacity and low photoluminescence intensity.
[109] Furthermore, ater heat treatment in a mixed gas o argon and
The existence o van der Waals orces between 2D g-C3N4 ultrathin hydrogen, the Pt nanoparticles were selectively immobilized on the
nanosheets will inevitably lead to interlayer agglomeration, and aect tri-coordination graphitized nitrogen o g-C3N4 to obtain a photocatalyst
its catalytic perormance. Porous 3D g-C3N4 with a larger specic sur- with uniorm particle size and good dispersibility.[110] And the syn-
ace area could prevent interlayer accumulation and provide an electron ergistic eect o Pt0 and Pt2+ species signicantly improved the photo-
transer paths. It can also maximize the use o multiple refected incident catalytic activity.[110] Hak et al. deposited Pd, Ag, and Au
light in an open rame. 3D g-C3N4 is usually composed o one or more nanoparticles on the g-C3N4 surace by natural illumination, respec-
0D, 1D, 2D g-C3N4. Compared with other sizes o g-C3N4, 3D g-C3N4 tively.[111] It is worth nothing that the noble metal nanoparticles are
generally exhibits a 3D ordered macroporous structure, which can more than electron acceptors to reduce the recombination rate o pho-
provide more reactive sites. Moreover, steric hindrance can eectively togenerated carriers and it can also signicantly enhance the light ab-
prevent the agglomeration o catalysts and improve light absorption sorption perormance.[111] And bisphenol A can be completely
eciency by delaying and storing incident light o specic wavelengths. degraded by the composites within 90 min[111] However, due to the
[103] And beneting rom its excellent catalytic perormance, it has high price and scarcity o precious metals, many scholars have tried to
become one o the research hotspots in the eld o nanomaterials. modiy the surace o g-C3N4 by depositing non-precious metals such as
Luo et al. synthesized the 3D network g-C3N4 assembled by nanorods Bi,[112] Ni, [113] Cu[114] and Co[115].
by chemical tailoring, sel-assembly and repolymerization o bulk g-
C3N4.[104] The obtained product showed larger specic surace area 2.2.5. Heterojunction construction
and lower photo-generated electron-hole pair recombination than bulk
g-C3N4 and exhibited good photocatalytic activity in phenol degrada- Many studies have shown that the heterojunctions constructed by
tion.[104] However, the preparation process is complex and large combining g-C3N4 with other semiconductors with matching band
amount o strong acids and bases need to be used.[104] Some re- structures can combine the advantages o each component and the di-
searchers ound that the salt template method is saer and more ecient erence o the energy band structure to orm a built-in electric eld
without using organic solvents and harmul substances to remove the between the materials to accelerate the transer o photogenerated
template. Chen et al. prepared 3D porous g-C3N4 with cyano groups carriers and inhibit the recombination o photogenerated electrons and
using thiourea by a acile two-step process that combines NaCl-assisted holes, thus improving the photocatalytic perormance. According to the
reeze-drying with calcination.[105] And NaCl not only acted as a dierent separation/transer mechanisms o photogenerated electron-
template or the 3D open-pore structure, but also promoted the hole pairs, g-C3N4-based heterojunctions mainly include Type-II, p-n,
decomposition o g-C3N4. Meanwhile, a moderate amount o cyano Z-scheme, new S-scheme and Schottky heterojunctions. The charge
group could act as an electron capture center.[105] Aterwards, Qian transer path o Type-II heterojunction is shown in Fig. 13a. [116,117]
12
J. Xing et al. Journal of Environmental Chemical Engineering 10 (2022) 108782
Fig. 12. (a) Schematic illustration o the synthesis procedure o porous g-C3N4. (b) schematic illustration o the bottom-up supramolecular sel-assembly route or
synthesizing 3D g-C3N4 NS; (c) SEM image, (d) TEM image (HRTEM image inset) and (e) AFM image o 3D g-C3N4 NS-2.
(a) Reproduced with permission rom re. [106], Copyright © 2019, American Chemical Society. (b-e) Reproduced with permission rom re. [108], Copyright ©
2019, Elsevier.
The semiconductor is excited by light to generate electrons and holes. separated.[116,117] Various p-type semiconductors such as LaFeO3,
Under the action o the potential dierence, the electrons in the semi- [126] BiOI,[127] CoNiO2[38] have been used to construct p-n
conductor I (SC I) are transerred to the CB o the semiconductor II (SC heterojunctions.
II), while the holes in the VB o the SC II are transerred to the VB o the
SC I. And the ecient separation o the photogenerated carriers enables 3. g-C3N4-based materials for wastewater remediation and
the CB o the SC II, mainly composed o the photogenerated electrons pollutants removal
and holes, and the VB o the SC I to participate in the reduction reaction
and oxidation reaction, respectively, and eventually enhance the pho- g-C3N4-based materials are considered as ideal materials or
tocatalytic activity. Although Type-II heterojunctions can inhibit the removing various pollutants such as organics and heavy metal ions in
recombination o photogenerated charges, it reduces the redox ability o wastewater due to their outstanding advantages o suitable optical band
compound semiconductors, and it is dicult to continuously transer gap, abundant reactive sites, high specic surace area and high chem-
electrons and holes due to electrostatic repulsion. In response to the ical stability. And they have been widely applied in the eld o water
above problems o Type-II heterojunctions, inspired by natural photo- remediation and pollutants removal.
synthesis, the g-C3N4-based Z-scheme heterojunction[118,119] was
constructed (Fig. 13b-c). Dierent rom Type-II heterojunction, the 3.1. g-C3N4-based materials or removing organic pollutants
electrons on SC II with a lower CB position recombine with the holes on
the VB o SC I through the heterojunction or the intermediate con- Various toxic and reractory organic pollutants, such as dyes, pesti-
ducting medium under visible light irradiation, so that strong redox cides and PPCPs, have been released into the environment and caused
ability o the photocatalyst could be maintained. serious harm. And the pollutants have become one o the major chal-
In recent years, Fu et al. proposed a novel S-scheme heterojunction lenges in the eld o environmental remediation. The removal o organic
with staggered band structures, composed o two n-type semiconductor pollutants in wastewater by g-C3N4-based materials mainly include
photocatalysts (Fig. 13d), in which SC I and SC II represent reduction adsorption, photocatalysis, and synergistic treatment o adsorption and
photocatalysts and oxidation photocatalysts, respectively.[120,121] photocatalysis.
And driven by the built-in electric eld, band bending and Coulomb
gravity, photogenerated electrons and holes o the S-scheme hetero-
3.1.1. Adsorption
junction recombine at the heterojunction interace, improving the
charge separation eciency. Meanwhile, the original high redox ca-
Treating wastewater by adsorbents has become one o the most
pacity is retained.[120–123] Additionally, the composite materials such
eective methods. High specic surace area, abundant unctional
as cocatalyst-ree 2D/2D CdS/g-C3N4 S-scheme and ultrathin S-scheme
groups and active sites are the excellent eatures o g-C3N4-based ma-
heterojunction g-C3N4/TiO2/C have also been successully abricated,
terials, which can realize the removal o organic pollutants in waste-
which provide a good opportunity to improve the separation eciency
water, through dierent interactions (hydrogen bonding, hydrophobic
o photogenerated carriers.[124,125] Furthermore, g-C3N4, as a typical
interaction, electrostatic attraction, etc.) between materials and pollut-
n-type semiconductor, can suppress photogenerated carrier recombi-
ants. And the adsorption perormance is closely related to the unctional
nation by constructing a p-n heterojunction with a suitable p-type
groups and structures on the surace o g-C3N4-based materials, the
semiconductor (Fig. 14e). In the p-n heterojunction, in general, the
structure o organic pollutants and the solution environment.[128] The
Fermi level (EF, p) o the p-type semiconductor is near its VB, while the
2D layered structure, multiunctional groups and/or deect sites o
Fermi level (EF, n) o an n-type semiconductor is generally near its CB,
g-C3N4 make it an excellent adsorbent.[129] The two-dimensional
thereore, a built-in electric eld is ormed at the interace rom the
porous g-C3N4 nanosheets abricated by an acidic hydrothermal
n-type semiconductor to the p-type semiconductor. [116,117] Once
method, exhibited good selective adsorption perormance or anionic
irradiated by visible light, the photogenerated electrons will transer
methyl orange by means o strong electrostatic attraction.[129]
rom the CB o the p-type semiconductor to the CB o the n-type semi-
Furthermore, the g-C3N4-ZnO@graphene aerogel heterojunction
conductor through the interace, while the holes will transer in the
showed good adsorption perormance or rhodamine B, methyl orange
opposite direction, so that the photogenerated carriers can be eectively
and other organic dyes, which provided a good basis or urther
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J. Xing et al. Journal of Environmental Chemical Engineering 10 (2022) 108782
Fig. 13. Schematic illustration o the transer o photoinduced charge carriers or various types o heterojunction nanocomposites: (a) type-II heterojunction; (b)
semiconductor-semiconductor Z-scheme heterojunction; (c) semiconductor-conductor-semiconductor Z-scheme heterojunction; (d) S-scheme heterojunction; (e) p-n
heterojunction.
photocatalytic degradation.[130] The g-C3N4/MoO3 nanocomposites irradiation. The application o it in water remediation has been studied
synthesized by co-precipitation method exhibited 162 mg g1 adsorp- by many researchers. The porous g-C3N4 nanosheets obtained by ther-
tion capacity or 300 mg L1 dicloenac with solution concentration o mal condensation o melamine and cyanuric acid showed excellent
1 g L1 at pH= 6.[131] The Cu2MoS4/g-C3N4 with unique fower degradation activity to tetracycline (over 60%) and rhodamine B
structure abricated by a one-step hydrothermal method showed higher (100%) ater 15 min o visible light irradiation, mainly due to super-
adsorption properties than other adsorbent materials and good cycle oxide radicals and holes generated by the photocatalytic process.[25]
stability, with the adsorption o rhodamine B as high as 420.2 mg g1. Beneting rom the synergistic eect o Eu(III) doping and hollow
[132] However, the selective adsorption o organic pollutants is still a structure, the carrier separation eciency o the Eu(III)-doped g-C3N4 is
challenge or g-C3N4-based materials, due to the high similarity o higher, and the degradation rates o rhodamine B and tetracycline in
organic molecular structures.[128]. wastewater is as high as 98% and 82%, respectively.[46] Moreover, the
Ag-deposited g-C3N4 exhibits degradation eciency o bisphenol A 3.15
times higher than that o pristine g-C3N4 due to ormation o Schottky
3.1.2. Photocatalysis barrier at the interace, which promotes the separation o photo-
generated carrier.[111] The g-C3N4-CdS/Bi4O5I2 heterojunction pro-
The g-C3N4-based materials with suitable optical bandgap and good vides multiple channels or photogenerated charge transer and could
light absorption ability can eciently mineralize organic pollutants into degrade acetaminophen at degradation rate o 80% within 25 min[133]
non-toxic substances such as CO2 and H2O under visible light
14
J. Xing et al. Journal of Environmental Chemical Engineering 10 (2022) 108782
Fig. 14. (a) Schematic illustration o the simultaneous photocatalytic reduction o Cr(VI) and oxidation o BPA over a direct Z-scheme MIL-101(Fe)/g-C3N4 het-
erojunction under visible light irradiation. (b) simultaneous photocatalytic reduction o Cr(VI) and degradation o BPA over MIL-101(Fe)/g-C3N4 at dierent initial
concentration ratios under visible light irradiation. (c) proposed adsorption and photocatalytic mechanism o P/S-g-C3Nx in BH and Cr(VI) coexistence environment
under air ambient.
(a-b) Reproduced with permission rom re. [145], Copyright © 2020, Elsevier. (c) Reproduced with permission rom re. [146], Copyright © 2020, Elsevier.
Furthermore, taking advantage o unique upconversion photo- heavy metal can through adsorption, photocatalysis or through combi-
luminescence properties and ecient charge separation ability o CDs, nation o adsorption and photocatalysis.
Li et al. utilized the as-prepared CDs/g-C3N4/SnO2 composites or the For example, the hydroxyapatite modied g-C3N4 powders, with rich
photocatalytic degradation o indomethacin under visible light irradia- surace hydroxyl, phosphate and -NH2/-NH-/=N- and other surace
tion and the degradation rate was 5.62 times higher than that o pristine unctional groups to orm chemical interactions with metal ions, were
g-C3N4.[134]. used to treat wastewater containing Cu2+, Mn2+, Zn2+, Pb2+, Fe3+ and
Cd2+ metal ions, and exhibited high adsorption capacity.[138] And with
3.1.3. Adsorption and photocatalysis synergistic treatment the increase o pH, the divalent metal ions were rst adsorbed to the
catalyst surace and then substituted with Ca2+ o the hydroxyapatite.
By the virtue o the excellent structure, g-C3N4-based materials also [138] Huang et al. used mesoporous g-C3N4 or the selective adsorption
show synergistic adsorption and photocatalysis o organic pollutants in o thorium ions rom polyionic solutions, which showed high selectivity
wastewater (adsorption and enrichment o organic pollutants rst, and and eciency (93.53%), and the maximum selective adsorption o Th
then decomposition and mineralization o organic pollutants through (IV) could be up to 108.18 mg g1.[139] Under visible light irradiation,
photocatalytic process), which can solve the problems o adsorption the mesoporous Bi2WO6/g-C3N4 heterojunction was used as a photo-
saturation and regeneration, and realize the long-term recycling.[135] A catalyst or photocatalytic reduction o mercury ions.[140] The orma-
3D–2D-3D BiOI/porous g-C3N4/graphene hydrogel composite photo- tion o the heterojunction not only increased the specic surace area o
catalyst with excellent adsorption perormance and charge separation the catalyst, but also promoted the eective separation o photo-
ability, synthesized by a two-step hydrothermal method, exhibited good generated carriers.[140] Thereore, compared with the single catalyst,
adsorption-photocatalytic synergistic treatment perormance and ease the mesoporous Bi2WO6/g-C3N4 heterojunction exhibited excellent
o recycling.[135] When it was applied to a static wastewater system, photocatalytic reduction activity o mercury ions (700 µmol g1 h1)
the synergistic degradation eciencies o methylene blue and levo- and photocatalytic reaction eciency (100%).[140].
foxacin hydrochloride were 7.2 and 2.7 times higher than that o BiOI, In addition to adsorbing heavy metal ions rom aqueous solutions,
respectively.[135]. high-valent heavy metal ions can also be reduced to low-valent metal
ions by adsorption reduction or photocatalytic reduction under visible
light irradiation, and then can be in situ precipitated and immobilized
3.2. g-C3N4-based materials or removing heavy metals
on solid particles, avoiding the transmission o heavy metal ions into the
ood chain.[128] Chen et al. used Fe0 @PTA/g-C3N4 composite or the
Heavy metals are highly toxic and dicult to degrade. With the rapid
adsorption and removal o As(V) in water.[40] The removal o As(V) was
development o industry, the concentration o heavy metals in waste-
mainly through the reduction o As(V) and the oxidation o Fe0, and the
water is getting higher and higher, which will cause irreversible damage
maximum adsorption capacity could reach 70.3 mg g1.[141] Tang
to humans and the environment.[136] Among them, Hg, Pb, Cr, Cd, As,
et al. used g-C3N4 fakes as a carrier to stabilize nanoscale zero-valent
Th and U are considered to have severe impact on human health and
iron (nZVI), and the reduction rate o Pb(II) o the obtained product is
even a small amount o exposure can cause serious damage to body
twice higher than that o nZVI alone.[142] When ZIF-8/g-C3N4 was used
organs.[137] Thereore, nding a suitable treatment method is one o
or photocatalytic reduction o U(VI), it exhibited excellent photo-
the hotspots in the eld o water remediation. The g-C3N4-based mate-
catalytic activity and chemical stability, and the photocatalyst partially
rials show great potential and advantages or the removal o heavy metal
photoreduced the adsorbed U(VI) to U(IV) within 30 min[143]
ions. And the application o g-C3N4-based materials or the removal o
15
J. Xing et al. Journal of Environmental Chemical Engineering 10 (2022) 108782
However, the photoreduction rate decreased signicantly with the in- attraction, π-π interaction, hydrogen bonding, and surace complexa-
crease o pH.[143] In another study, Ou et al. used the adsorption and tion. For the treatment o heavy metal ions and surace-charged or-
photocatalytic synergy o CoFe-LDH/g-C3N4 to adsorb 60% Cr(VI) ganics, electrostatic attraction and surace complexation are generally
(50 mg L1) in 10 min, and Cr(VI) could be completely reduced to Cr the main interactions, which can be conrmed by FTIR spectroscopy,
(III) under visible light irradiation or 90 min[144]. XPS spectroscopy and other analyses. In addition, the pH o the solution
is an important actor aecting the adsorption perormance o g-C3N4-
3.3. Simultaneous decontamination based materials. It was ound that the electrostatic attraction interaction
is the main reason when the negatively charged Cu2MoS4/g-C3N4
The composition o actual wastewater is complex, usually containing composite was used to treat the cationic rhodamine B.[132] At low pH,
many dierent types o pollutants, such as heavy metal ions, organic the adsorption capacity did not change much, while at pH= 9, the
pollution, biomass, etc. Under visible light irradiation, organics and dissociation o carboxylic acid groups in rhodamine B and the depro-
heavy metal ions could interact each other, so that the synergistic tonation o nitrogen groups accelerated, which increased the electro-
removal can be achieved. static repulsion between them and reduced the adsorption perormance.
Currently, or the simultaneous decontamination system, wastewater [132] FTIR and XPS spectra showed that the surace o g-C3N4/β-CD
containing with Cr(VI) and organic pollutants is mainly studied. For material obtained by β-cyclodextrin modication had abundant unc-
example, Zhao et al. obtained a biunctional MIL-101(Fe)/g-C3N4 pho- tional groups and active sites (such as C– – O, C-O-C, -OH, etc.).[149]
tocatalyst by in situ growth o MIL-101(Fe) on the surace o g-C3N4, or When treating Pb(II) wastewater, pH could aect the surace properties
the simultaneous photocatalytic treatment o Cr(VI) and bisphenol A. o g-C3N4/β-CD and the degree o protonation o oxygen-containing
[145] As shown in Fig. 14a, the photogenerated electrons participated in unctional groups. It can also aect the morphological distribution o
the reduction o Cr(VI) and the degradation o bisphenol A simulta- Pb(II).[149] When pH< 7.0, Pb2+ and Pb(OH)+ are dominant, and the
neously, in which bisphenol A acted as a hole scavenger to promote the adsorption process is mainly the surace complexation and electrostatic
separation o photogenerated carriers, enhancing the photocatalytic attraction between hydroxyl or heptazine ring and Pb(II), while when
reduction ability o Cr(VI).[145] In coexisting system o dierent pol- pH> 7.0, the adsorption process is mainly surace complexation o Pb
lutants, the reduction rate o Cr(VI) and the degradation rate o (II) with hydroxyl groups.[149] In addition, when g-C3N4/β-CD was
bisphenol A by the catalyst could reach 97.1% and 87.7%, respectively, used to adsorb methyl orange, the adsorption behavior was mainly due
which were much higher than 26.2% and 46.6% o the single pollutant to hydrogen bonding and van der Waals orce.[149] Rashid et al. also
system (Fig. 14b).[145] P and S co-doped g-C3N4 with eeble N va- ound that the π-π interaction and hydrogen bonding interaction were
cancies (P/S-g-C3N4) prepared by supramolecular sel-assembly could the main reasons or the adsorption o dicloenac by g-C3N4/MoO3,
also treat wastewater containing berberine hydrochloride and Cr(VI) which could also be conrmed by the π-π stacking o dicloenac on the
through synergistic eect o adsorption and photocatalysis, as shown in nanocomposite and the tendency o -NH to increase the adsorption o
Fig. 14c.[146] The adsorption process o P/S-g-C3N4 accelerated the dicloenac molecules.[131].
photocatalytic degradation process and promoted the removal o Moreover, the determination o the kinetics is critical or the design
berberine hydrochloride.[146] Meanwhile, berberine hydrochloride o adsorption systems. The commonly used adsorption kinetic models
also promoted the surace adsorption o Cr(VI) on the catalyst, which include the pseudo-rst-order kinetic model and the pseudo-second-
was benecial to the reduction o Cr(VI).[146] Ater 2 h o visible light order kinetic model,[149,150] which describes the relationship be-
irradiation, the berberine hydrochloride degradation rate and the tween the adsorption capacity o the adsorbent and the contact time, as
reduction rate o Cr(VI) could reach 90.05% and 73.83%, respectively. shown in as Eq. (1) and Eq. (2), respectively.[151].
[146] When N-TiO2/O-doped N vacancy g-C3N4 was used to treat
ln(qe qt ) = lnqe k1 t (1)
wastewater containing tetracycline hydrochloride and Cr(VI)[147] and
RP/g-C3N4 heterojunction was used to treat in wastewater containing Cr t 1 t
(VI) and rhodamine B,[148] signicantly increase o removal eciency = + (2)
qe k2 q2e qe
due to synergistic eect were also observed. Table 1 summarizes the
related researches on the treatment o pollutants with g-C3N4-based Where qe (mol g1) and qt (mol g1) are the adsorption capacity o the
materials in recent years. adsorbent at equilibrium state and time t. k1 (h1) and k2 (g mol1 h1)
are the rate constants o the pseudo-rst-order kinetic equation and the
4. Mechanism pseudo-second-order kinetic equation, respectively. The adsorption o
methyl orange and Pb(II) by g-C3N4/β-CD ts the pseudo-second-order
In order to better illustrate the pollutants removal behaviors and kinetic model, so that the rate-limiting step is the chemisorption pro-
provides theoretical basis or improving the wastewater treatment ca- cess, which is related to valance orces arising rom the sharing or ex-
pacity and eciency o g-C3N4 materials, the mechanisms o adsorption change o electrons between the adsorbent and the adsorbate.[149,152].
and photocatalysis are discussed. The adsorption thermodynamics can be revealed through the study
o adsorption isotherms. The Langmuir model and the Freundlich model
4.1. Adsorption mechanism, kinetics and thermodynamics are extensively used.[150] The Langmuir model assumed that all
adsorption active sites have the same adsorption energy and can only
Adsorption usually occurs in the process o water remediation. The bind a single adsorbate. Once the adsorptive sites are occupied, there
main unctional groups o g-C3N4 prepared by direct calcination o will be no more adsorption behaviors on these sites, which can well
nitrogen-rich precursors are -NH2/-NH-/=N-, which can be modied describe the ideal monolayer homogeneous adsorption, as shown in Eq.
with dierent unctional groups (such as carboxylic acid, hydroxyl, etc.) (3).[152] While the Freundlich model is an empirical model that con-
by constructing a heterojunction to improve the adsorption perormance siders the heterogeneous energy distribution o active sites.[151,152] It
or dierent pollutants.[149] In general, the adsorption mechanism o is conrmed to be consistent with the exponential distribution o
g-C3N4-based materials is generally investigated rom two aspects: (1) non-uniorm surace active centers, and can well describe the non-ideal
the interaction between g-C3N4-based materials and pollutants during multi-layer adsorption, as shown Eq. (4).[152].
the adsorption process; (2) the kinetics and thermodynamics o the
adsorption process. bqmax Ce
qe = (3)
The adsorption behavior between g-C3N4-based materials and pol- 1 + bCe
lutants is usually induced by the interactions such as electrostatic
16
J. Xing et al. Journal of Environmental Chemical Engineering 10 (2022) 108782
Table 1
Removal eciency o g-C3N4-based materials or wastewater pollutants.
g-C3N4 based Mechanisms Conditions Pollutants Removal eciency/ Sorption capacity Re.
materials
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J. Xing et al. Journal of Environmental Chemical Engineering 10 (2022) 108782
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J. Xing et al. Journal of Environmental Chemical Engineering 10 (2022) 108782
Table 2
The evolution o research on photocatalytic treatment o pollutants by g-C3N4-based materials during the last 10 years.
g-C3N4 based Synthetic methods Modication strategies Conditions Photocatalytic eciency Re.
photocatalysts
g-g-C3N4-P3HT Solvothermal method Type-II heterojunction Phi-lips lamp (40 W/ Methylene blue (1 × 105 M): > 90% [157]
230 V)
(λ > 400 nm)
PANI–g-C3N4 In situ deposition oxidative Type-II heterojunction 500 W Xe lamp Methylene blue (10 mg L1): 92.8% within [158]
polymerization (λ ≥ 420 nm) 120 min
Mesoporous g-C3N4 Template method Morphological regulation 300 W Xe lamp 4-CP (1.2 × 104 M): nearly 100% within [159]
(λ ≥ 420 nm) 60 min
phenol (1.2 × 104 M): nearly 96% within
90 min
AuNP/g-C3N4 Ultrasonication-assisted liquid Morphological regulation and 500 W Xe lamp Methyl orange (10 mg L1): 92.6% within [160]
nanohybrids exoliation and photoreduction metal deposition (λ ≥ 400 nm) 150 min
Single layer g-C3N4 Chemical exoliation method Morphological regulation 500 W Xe lamp Phenol (2 × 105 M): 0.2589 h1 [98]
nanosheets (λ > 420 nm)
AgBr/g-C3N4 Water bath method Type-II heterojunction 300 W Xe lamp Methyl orange (10 mg L1): 91% within [161]
(λ > 420 nm) 10 min
N-TiO2/g-C3N4 In situ microwave-assisted Type-II heterojunction 300 W xenon arc lamp Methylene blue (10 mg L1): 0.070 min1 [162]
synthesis approach (λ > 400 nm)
g-C3N4/SmVO4 Mixing-calcination method Type-II heterojunction 350 W Xe lamp Rhodamine B (10 mg L1): nearly 100% [163]
(420 nm < within 120 min
λ < 800 nm)
Sphere-like g-C3N4/ One-pot EG-assisted Type-II heterojunction 300 W Xe lamp Bisphenol A (10 mg L1): 97% within 60 min [164]
BiOI solvothermal process (λ > 400 nm)
g-C3N4/F-TiO2 Hydrothermal method Type-II heterojunction 50 W 410 nm LED Methyl orange (10 mg L 1
): 0.0374 min 1
[165]
light
Ag@AgBr/g-C3N4 Deposition-precipitation method Z-scheme heterojunction 300 W Xe lamp Methyl orange (10 mg L1): 95% within [166]
(400 nm < 10 min
λ < 680 nm) Rhodamine B (10 mg L1): 95% within
10 min
Magnetic core–shell Sel-assembly method Type-II heterojunction 500 W Xe lamp Orange II (0.028 mM): nearly 98% within [167]
CuFe2O4 @C3N4 (λ > 420 nm) 210 min
g-C3N4/TiO2 Biomimetic approach Type-II heterojunction 500 W Xe lamp Rhodamine B (10 mg L1): 84% within [168]
(λ ≥ 420 nm) 300 min
Acidied g-C3N4/g- Ultrasonic dispersion assisted Type-II heterojunction 300 W Xe lamp Methyl orange (10 mg L1): 0.0216 min1 [169]
C3N4 hybrids electrostatic sel-assembly (λ > 420 nm)
strategy
Nb2O5/g-C3N4 One-step heating strategy Type-II heterojunction 250 W Xe lamp Tetracycline hydrochloride (20 mg L1): [170]
(λ > 420 nm) 76.2% within 150 min
V2O5/g-C3N4 In-situ growth strategy Direct solid-state Z-scheme 250 W Xe lamp Tetracycline (10 mg L1): 75.7% within [171]
heterojunction (λ > 420 nm) 120 min
Bi12GeO20/g-C3N4 Sol-gel method Solid state Z-scheme 300 W Dy lamp Rhodamine B (5 mg L1): 1.992 h1 [172]
heterojunction (λ > 400 nm) Cr (VI) (10 mg L1): almost 100% within
180 min
OA-g-C3N4 Catalytic redox-based advanced No-metal elemental doping 500 W Xe lamp Bisphenol A (15 mg L1): 100% within [173]
oxidation process 180 min
PCN-S Thermal exoliation method Morphological regulation and 300 W Xe lamp 2,4-diclorophenol (80 mg L1): nearly 100% [174]
no-metal elemental doping (λ > 400 nm) within 120 min
Cr (VI) (20 mg L1): nearly 100% within
120 min
h-BN/g-C3N4 In-situ growth strategy Metal-ree heterojunction 300 W Xe lamp Tetracycline (10 mg L1): 79.7% within [175]
(λ > 420 nm) 60 min
Rhodamine B (20 mg L1): 99.5% within
40 min
WO3/g-C3N4/Bi2O3 One step co-calcination method Direct solid-state dual Z- 300 W Xe lamp Tetracycline (10 mg L1): 0.02367 min1 [176]
scheme heterojunction (λ > 420 nm)
g-C3N4/TiO2 Thermal polymerization Type-II heterojunction 300 W Xe lamp Uranium (VI) (20 mg L1): 83% and Arsenic [177]
(320 nm ≤ (III) (20 mg L1): 40% within 4 h
λ ≤ 780 nm) simultaneously
BCM-C3N4 Supramolecular preassembly Morphological regulation and 300 W Xe lamp Sulamethazine (10 mg L1): over 90% [178]
no-metal elemental doping (λ > 420 nm) within 60 min
Ag/AgBr/BiVO4 Hydrothermal method and Z-scheme heterojunction 300 W Xe lamp Ciprofoxacin (10 mg L1): 91.4% and Cr (VI) [179]
photoreduction process (λ > 420 nm) (10 mg L1): 91.72% within 120 min
simultaneously
Ag@U-g-C3N4-NS Mussel-inspired dopamine Morphological regulation and 300 W Xe lamp Methylene blue (10 mg L1): 88.5% within [180]
polymerization modication metal deposition 40 min
Phenol (10 mg L1): 89% within 40 min
CQDs modied g- Thermal polymerization method Carbon quantum dots 300 W Xe lamp Dicloenac (10 mg L1): 100% within 100% [181]
C3N4 modied (λ ≥ 400 nm)
Cl-doped porous g- Bottom-up synthetic route Morphological regulation and 300 W Xe lamp Tetracycline (10 mg L1): 92% within [182]
C3N4 no-metal elemental doping (λ > 420 nm) 120 min
2D/3D Z-scheme g- Ball-milling method Z-scheme heterojunction 300 W white light Cr (VI) (10 mg L1): 99% within 40 min [183]
C3N4/UiO-66
g-C3N4/ZrO2 Calcination method S-Scheme heterojunction Rhodamine B (10 mg L 1
): 82% within [184]
150 min
(continued on next page)
19
J. Xing et al. Journal of Environmental Chemical Engineering 10 (2022) 108782
Table 2 (continued )
g-C3N4 based Synthetic methods Modication strategies Conditions Photocatalytic eciency Re.
photocatalysts
300 W Xe lamp
(420 nm ≤
λ ≤ 760 nm)
g-C3N4/Bi/BiVO4 Chemical deposition Biunctional S-scheme 350 W Xe lamp Rhodamine B (10 mg L1): 100% within [185]
heterojunction (λ > 420 nm) 40 min
2D/2D Bi2MoO6/g- Photoreduction and hydrothermal S-Scheme heterojunction 300 W Xe lamp Rhodamine B (5 mg L1): 95.4% within [186]
C3N4 (λ > 420 nm) 40 min
2D–2D WO3/g-C3N4 Template-assisted method S-Scheme heterojunction 300 W Xe lamp Tetracycline (20 mg L1): 0.0378 min1 [187]
(λ > 420 nm)
g-C3N4 @ZIF-8 In-situ growth Core-shelled structure 300 W Xe lamp Tetracycline (20 mg L 1
): 89% within 60 min [188]
(λ > 430 nm)
VC-OCN One-step ormaldehyde-assisted Deect and no-metal 300 W Xe lamp P-nitrophenol (10 mg L ): 99.7% within
1
[189]
thermal polycondensation elemental doping (400 nm ≤ 60 min
λ ≤ 750 nm) atrazine (10 mg L1): 99.1% within 60 min
Carbon dots modied Thermal polymerization Z-scheme heterojunction 350 W Xe lamp Indomethacin (10 mg L1): 90.8% within [134]
g-C3N4/SnO2 (λ > 420 nm) 80 min
Nitrogen doped g- Thermal polymerization No-metal elemental doping 300 W Xe lamp Phenol (10 mg L1): 0.00626 min1 [63]
C3N4 (λ > 420 nm)
PA-CN Heating Co-monomer polymerization 300 W Xe lamp Sulamethazine (20 mg L 1
): 0.0737 min 1
[190]
condensation (λ > 400 nm)
Cu-pCN Pre-organized template sel- Metal elemental doping and 300 W Xe lamp Tetracycline (30 mg L1): 98% within [191]
assembly morphological regulation (λ > 420 nm) 120 min
CN Thermal polymerization Carbon vacancies and 300 W Xe lamp Tetracycline (30 mg L1): 87.9% within [192]
morphological regulation (λ > 420 nm) 75 min
5. Conclusions and prospects interests or personal relationships that could have appeared to infuence
the work reported in this paper.
g-C3N4-based materials exhibit excellent properties as ecient and
sustainable material or the removal o wastewater pollutants. Never- Data Availability
theless, some issues need to be solved to realize the industrial applica-
tion o g-C3N4-based materials in wastewater treatment and pollutants Data will be made available on request.
removal:
(1) Morphology regulation is a widely used modication method. Acknowledgement
However, the use o substances such as templates, strong acids and bases
urther complicates the experiments. In recent years, supramolecular The authors are grateul to the nancial support o the National
sel-assembly method or adjusting the morphology o materials has Natural Science Foundation o China (NO. 21978201).
become a research hotspot. However, at present, the substances which
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