Process Safety and Environmental Protection 139 (2020) 230–240

Contents lists available at ScienceDirect

Process Safety and Environmental Protection

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

Graphitic nitride-catalyzed advanced oxidation processes (AOPs) for

landfill leachate treatment: A mini review
Meina Han a , Xiaoguang Duan b , Guoliang Cao a , Shishu Zhu c,d,∗∗ , Shih-Hsin Ho a,∗
a
State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin, Heilongjiang
Province,150090, PR China
b
School of Chemical Engineering and Advanced Materials, The University of Adelaide, Adelaide, SA 5005, Australia
c
School of Environmental Science and Engineering, Sun Yat-sen University, Guangzhou 510275, PR China
d
Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology, Sun Yat-sen University, Guangzhou 510275, PR
China

a r t i c l e i n f o a b s t r a c t

Article history: Landfill leachate poses significant risks to public health via the release of high-toxicity contaminants,
Received 30 March 2020 including refractory organic compounds, ammonia-nitrogen compounds, and heavy metals. Significant
Received in revised form 29 April 2020 efforts have been made to develop useful methods for leachate disposition and treatment. Advanced
Accepted 29 April 2020
oxidation processes (AOPs) are one of the most promising methods, because they can rapidly degrade
Available online 5 May 2020
diverse pollutants and significantly improve the biodegradability of leachate. Graphitic carbon nitride
(g-C3 N4 ), a fascinating conjugated polymer, has become a hot topic in AOP research due to its metal-free
Keywords:
benefits and high photosensitivity. Thus, combining AOPs with g-C3 N4 achieves excellent degradation of
Graphitic carbon nitride
Advanced oxidation processes
refractory pollutants in leachate. Since the composition of leachate is complex in the practical conditions,
Leachate the information reported by current studies of using g-C3 N4 as a remediator is still incomplete and
Photocatalysis fragmented. Thus, in this review, the recent status of leachate treatment and approaches for its disposal
Pollutant degradation has been summarized and some conclusions have been drawn. In addition, a brief introduction to g-
C3 N4 and its application in AOPs for leachate treatment have been critically discussed and with its future
outlook assessed. Although the development of g-C3 N4 in AOPs for leachate treatment is highly efficient
and practical, comprehensive study about its application and technology expansion is urgently needed,
based on the complex operating conditions. Perspectives on the treatment of leachate using g-C3 N4 -AOPs
are also included. The information and perspectives provided in this review will provide guidance and
novel understanding to accelerate the development of g-C3 N4 -based AOPs for leachate treatment.
© 2020 Institution of Chemical Engineers. Published by Elsevier B.V. All rights reserved.

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 231
2. Graphitic carbon nitride (g-C3 N4 ) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 231
2.1. Brief introduction to g-C3 N4 . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 231
2.2. Preparation methods . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 232
2.3. g-C3 N4 -based nanocomposites . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 233
2.3.1. Carbonaceous nanomaterial-based g-C3 N4 . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 233
2.3.2. Metal-doped g-C3 N4 . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 233
2.3.3. Non-metal-doped g-C3 N4 . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 233
3. Advanced oxidation processes (AOPs) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 233
3.1. AOPs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 233
3.2. AOPs for leachate treatment . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 234

∗ Corresponding author.
∗∗ Corresponding author at: School of Environmental Science and Engineering, Sun Yat-sen University, Guangzhou 510275, PR China.
E-mail addresses: zhushishu@hit.edu.cn (S. Zhu), stephen6949@hit.edu.cn (S.-H. Ho).

https://doi.org/10.1016/j.psep.2020.04.046
0957-5820/© 2020 Institution of Chemical Engineers. Published by Elsevier B.V. All rights reserved.
 M. Han et al. / Process Safety and Environmental Protection 139 (2020) 230–240 231

3.3. Application of AOPs with g-C3 N4 for leachate treatment . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 234

4. Conclusion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 237
Acknowledgements . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 237
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 237

1. Introduction capacity, the low mass transfer efficiency of ozone from the gas
phase to the liquid phase and the release of excess ozone have
Landfills, the ultimate destination of most artificial wastes, negative impacts on the surrounding environment. In the Fenton
contain huge amounts of pollutants derived from industrial and oxidation process, the consumption of ferrous species increases
municipal solids. Due to naturally-occurring processes like weath- the high cost of the subsequent sludge treatment, while the Fen-
ering and runoff, high-concentration liquid leachates are released ton photo-assisted process is only effective in a narrow pH range.
and performed direct and potential threats to surface and subsur- Electrochemical advanced oxidation requires large amounts of
face water as well as flora, fauna, and human health, especially for energy and expensive metal electrodes. Among these techniques,
the unlined or old landfills localized near watercourses or in wet- semiconductor-induced photocatalysis has attracted significant
lands (Ford et al., 2011; Lorah et al., 2009). Therefore, successful attention because it produces large number of active radicals for
treatment of toxic substances in landfill leachate is a significant eliminating recalcitrant organic pollutants and uses economical
step towards the sustainable management of solid waste. Leachates and renewable solar energy. Thus, selection of a suitable semicon-
must be carefully treated before being released into the surround- ductor material is essential for photocatalysis-assisted AOPs.
ings or transferred to a secondary treatment plant. Unfortunately, Graphitic carbon nitride (g-C3 N4 ), a metal-free polymer, has
in many countries and regions, leachates have been overlooked. attracted extensive interest in various scientific applications due
Ford et al. conducted a field investigation to discover the source to its graphite-like structure, specific electronic structure, excellent
of arsenic at a Superfund site in Massachusetts (USA) and detected chemical stability, and large surface area. Fortunately, the proper-
the presence of leachate-derived arsenic in groundwater and sedi- ties of stabilization and low toxicity render g-C3 N4 as a relatively
ment (Ford et al., 2011). In addition, the presence of commonly used environment-friendly material with minor ecological or toxicologi-
pesticide residues in concentrated leachate poses a high acute and cal concerns. Coupling g-C3 N4 and AOPs enhances the effectiveness
chronic risk to the environment (Wang et al., 2019). of both materials and shows excellent results in degrading high
Different environmental factors and different properties of concentration refractory contaminants in leachate. Herein, we
the parent wastes lead to leachates with very diverse composi- present a brief review focusing on the development of graphitic car-
tions (Qasim, 2017). Generally, typical landfill leachates include bon nitride as a promising catalyst for landfill leachate treatment.
a large amount of organic matter, humic and fulvic acids, and Although only a limited number of systematic and comprehen-
xenobiotic organic compounds (such as aromatic hydrocarbons, sive studies using actual waste leachate have been performed,
phenolics, chlorinated aliphatics, pesticides, and plastizers). The the potentials of AOPs combined with g-C3 N4 for degrading the
dissolved organic carbon (DOC) and chemical oxygen demand possible pollutants in leachate is also examined. In addition, the
(COD) in leachate can be as high as 1341−3100 mg L−1 and possible practical applications to leachate treatment are explained
3385−5000 mg O2 L−1 , respectively. The common characteristics and concretely analyzed via a comparative discussion. The refer-
of landfill leachate are low biodegradability (five-day biochem- ences provided in this review also provide further insights to extend
ical oxygen demand to chemical oxygen demand (BOD5 /COD) the study of g-C3 N4 -based AOPs for leachate treatment.
ratios of 0.07−0.27). Leachate also contains a high content
of damaging inorganic ions (such as 2124−6200 mg L−1 chlo-
2. Graphitic carbon nitride (g-C3 N4 )
ride and 1125−3200 mg L−1 ammonium), a high conductivity
(12770–25000 S cm−1 ), and toxic heavy metals (cadmium,
2.1. Brief introduction to g-C3 N4
chromium, copper, lead, nickel and zinc) (Anglada et al., 2011;
Cabeza et al., 2007; Chiang et al., 1995; Moreira et al., 2015; Urtiaga
Graphitic carbon nitride has attracted much interest in the sci-
et al., 2009; Zhang et al., 2010a).
entific community due to its unique structures and remarkable
Numerous attempts have been made to develop efficient tech-
properties. The history of the discovery and development of this
niques for leachate treatment, including biodegradation (Miao
polymer dates back to the 1990s (Sudhaik et al., 2018). Among
et al., 2019; Rani et al., 2019; Song et al., 2019), coagulation (Xu et al.,
several developed allotropes, g-C3 N4 demonstrates outstanding
2019), adsorption (Lam et al., 2019), and membrane filtration (Zhou
advantages due to its graphite-like structure, huge surface area,
et al., 2020). However, most conventional approaches have limita-
specific electronic structure, excellent chemical stability and high
tions and do not eliminate all the negative impacts of the leachate
electron mobility (Kong et al., 2019; Thomas et al., 2008; Zhang
on the environment. For example, landfill aging processes and the
et al., 2011). Recently, research on g-C3 N4 has mainly focused on
low B/C ratio of leachate can decrease the efficacy of biodegrada-
energy generation and storage, heterogeneous catalysis, organic
tion. In addition, adsorption techniques have problems with the
synthesis, sensors, and environmental applications (Mamba and
recovery and disposal of irreversible adsorbents. Membrane tech-
Mishra, 2016; Mishra et al., 2019; Patnaik et al., 2018).
nologies have high operating costs and challenging problems with
The high performance and application of g-C3 N4 is highly
fouling.
structure-dependent. There are two main allotropes of g-C3 N4
AOPs are an efficient and powerful treatment for landfill
(Fig. 1(a) and Fig. 1(b)), periodic arrangements containing subunits
leachate. AOPs are classified into different types, including pho-
of triazine (C3 N3 ring) and tri-s-triazine (C6 N7 tri-ring), respectively
tocatalytic oxidation, Fenton or Fenton-like processes (Gode et al.,
(Zambon et al., 2016; Zhao et al., 2015). Theoretical calculations
2019), electrochemical oxidation (Nie et al., 2016), and persulfate-
have shown that the g-C3 N4 allotrope with C6 N7 segments is more
based AOPs (Roy and Moholkar, 2019; Zhou et al., 2019). However,
thermodynamically stable than the allotrope based on C3 N3 (Kroke
technical challenges limit their widespread applications. For exam-
et al., 2002). Thus, tri-s-triazine is widely regarded as a promising
ple, although AOPs based on ozone activation have a high oxidizing
candidate for g-C3 N4 -based applications (Kong et al., 2019). Unlike
232 M. Han et al. / Process Safety and Environmental Protection 139 (2020) 230–240

Fig. 1. Required temperatures for synthesizing g-C3 N4 using different precursors and details of the thermal polymerization pathway for the formation of g-C3 N4 using
cyanamide (CA) as the precursor. (a) Triazine and (b) Tri-s-triazine based structures are two main allotropes of g-C3 N4 .

conventional semiconductors (e.g. SiC, GaN, ZnO, etc.), g-C3 N4 has
unique stability with respect to heat treatment and chemical resis-
tance. Thermal gravimetric analysis (TGA) of g-C3 N4 suggested that
g-C3 N4 is not volatile at 600 ◦ C, while it can be completely decom-
posed at temperatures greater than 700 ◦ C (Lei et al., 2015; Li et al.,
2010; Gillan, 2000). g-C3 N4 also has high stability in extremely
acidic and basic media and is insoluble in conventional solvents,
including ethanol, water, tetrahydrofuran, toluene and diethyl
ether. The structural stability of g-C3 N4 may be due to the Van
der Waals forces between the stacked graphitic layers. In addition,
polymeric g-C3 N4 has also attracted growing interests as semicon-
ducting photocatalyst and has been named as the “holy grail” for
highly efficient photocatalytic hydrogen evolution reaction (HER)
due to its facile synthesis, fascinating electronic band structure,
reliable functionalization and unique visible-light responsiveness
(Liu et al., 2017). The g-C3 N4 prepared by the microwave-assisted
molten-salt strategy presents remarkable photocatalytic activity
with considerable quantum yield (up to 10.7 % at 420 nm), suit-
able alignment of energy bandgap structures, convenient carrier
transfer path, and more efficient separation of photo-generated
electron-hole pairs. Furthermore, the low cost, low toxicity, facile
and large-scale fabrication of g-C3 N4 improve the possibility of its
application in various types of AOPs.
2.2. Preparation methods
g-C3 N4 can be prepared via several different approaches and
the resulting products exhibit different physiochemical properties.
Common methods of synthesizing g-C3 N4 include thermal poly-
merization, solvothermal and sol–gel methods, template-assisted
methods, and chemical functionalization. Among these, thermal
polymerization is the most popular and commonly used method for
g-C3 N4 preparation, due to its outstanding technical simplicity and
low costs. Therefore, the thermal polymerization method is high-
lighted and emphasized in this review. The thermal polymerization
process is mainly achieved by thermally polymerizing nitrogen-
and carbon-rich precursors. The most frequently used organic
precursors include urea, melamine, trithiocyanuric acid, dicyandi-
amide, cyanamide, triazoles, thiourea, guanidine thiocyanate, and
guanidine hydrochloride. Formation of melamine by polyaddition
and the removal of amino groups by polycondensation are the
necessary processes during the formation of the g-C3 N4 polymer
network (Sudhaik et al., 2018). The thermal conditions play a cru-
cial role in preparing the target g-C3 N4 , and different precursors
require different thermal conditions for polymerization. As has
been effectively summarized by Sudhaik et al. (Fig. 1), the fabrica-
tion of g-C3 N4 using diverse precursors requires different thermal
decomposition temperatures (Sudhaik et al., 2018). In addition, the
 M. Han et al. / Process Safety and Environmental Protection 139 (2020) 230–240
thermal polymerization of cyanamide (CA) to synthesize g-C3 N4
was discussed as an example. Different poly-condensates can coex-
ist over a wide temperature range. When the temperature is higher
than 600 ◦ C, g-C3 N4 becomes unstable and partially or fully decom-
poses, generating NH3 and Cx Ny Hz . Thus, thermal polymerization
temperature between 550 and 600 ◦ C is generally chosen as the
optimal temperature for g-C3 N4 synthesis. Also, the properties of
the target g-C3 N4 , including the surface area, porosity, absorption,
photoluminescence, C/N ratio and nanostructure, can be strongly
affected by the technical parameters of the thermal polymerization.
2.3. g-C3 N4 -based nanocomposites
Even though the suitable structure, low cost, and highly stabil-
ity of g-C3 N4 make it a superior photocatalyst, many challenges
still remain for its practical applications. Some significant disad-
vantages, such as poor electrical conductivity, insufficient visible
light absorption, fast recombination of photoinduced charge carri-
ers, and low specific surface area, also significantly hinder the broad
application of g-C3 N4 (Chen et al., 2015a; Zhang et al., 2019b, b).
Consequently, considerable efforts have been directed to develop-
ing g-C3 N4 composites with high numbers of active sites and high
stability.
2.3.1. Carbonaceous nanomaterial-based g-C3 N4
Tailoring g-C3 N4 to obtain particular properties has been a target
in recent studies. Combining g-C3 N4 with carbonaceous nanopar-
ticles, nanosheets, and nanoribbons has attracted considerable
interests due to the excellent properties of the composites, such as
high specific surface area, remarkable adsorption properties, and
high plasticity. Coupling g-C3 N4 with nanocarbon materials is a
good strategy to exploit the synergistic effect of both materials and
broaden the applications of g-C3 N4 . Benchmark carbon materials,
such as graphene oxide (RGO), carbon nanotubes (CNTs), and car-
bon nanospheres (CNS), have been extensively studied. Graphene
is a potential candidate for constructing g-C3 N4 -based nanocom-
posites. For example, coupling graphene with g-C3 N4 produces
nanocomposites with new features (Bai and Shen, 2011; Chen et al.,
2013). Graphene@g-C3 N4 hybrids have been shown to be good cat-
alysts under visible light (Ai et al., 2015; Liao et al., 2012; Ong
et al., 2015a, b; Tong et al., 2015), with synergistically improved
photo-response of both materials in the visible region, prolonged
life of the photogenerated charge carriers, enhanced adsorption
properties and increased specific surface area. The coupling of g-
C3 N4 with CNTs also improved the efficiency of the photocatalytic
degradation of aqueous pollutants (Ma et al., 2014; Pei et al., 2015;
Wu et al., 2015). Other g-C3 N4 -based nanocomposites have also
been fabricated with properties enhancement, such as C60 /g-C3 N4
(fullerene/g-C3 N4 )(Bai et al., 2014; Chai et al., 2014), carbon quan-
tum dots (CQDs)/g-C3 N4 hybrid nanocomposite(Li et al., 2016b; Liu
et al., 2019; Zhao et al., 2020) and biochar/ g-C3 N4 (BC-g-C3 N4 )(Li
et al., 2019a, b). Hard and soft-templating procedures based on
carbonaceous nanomaterials have both been used to remarkably
improve the surface area of g-C3 N4 by introducing pores into its
structure (Chen et al., 2015b; Mo et al., 2014). Despite the successful
optimization of its specific surface area, the low conductivity, high
recombination rate, and low photocatalytic efficiency of g-C3 N4
limit its applications.
2.3.2. Metal-doped g-C3 N4
Rational design of g-C3 N4 with highly catalytic activity is
significant for its extensive application. Metal-doping has been
proved as a typical strategy to design the advanced g-C3 N4 with
boosting activity. Metal deposition, introducing heteroatoms, and
coupling g-C3 N4 with other semiconductors can further enhance
the catalytic performance and extend the scope of the potential
233
applications of g-C3 N4 . As reported, with metals addition, the active
species in localized space could be enriched by deposition of metal
nanoparticles into pores and channels, while the electronic struc-
ture of g-C3 N4 could be changed for enhancing H2 O adsorption and
oxidation (Huang et al., 2020; Li et al., 2020). The above modulation
of metals could regulate the tunes band edges and thus motivate
the generation of hydroxyl radical (·OH). Moreover, the formed
metal nanostructures could also attribute a portion of catalytic
activity of g-C3 N4 . Metals that are commonly used for decora-
tion or doping include alkali metals, transition metals, rare earth
metals and noble metals (Mamba and Mishra, 2016). For exam-
ple, sodium-doped g-C3 N4 showed a higher photocatalytic activity
for decomposing organic chemicals under visible light illumina-
tion compared to pure g-C3 N4 , due to the effects of sodium on
the band structure, narrowing the band gap and efficiently sep-
arating the charge carriers (Zhou et al., 2011). Similarly, doping
potassium into g-C3 N4 tuned the band structure and led a higher
photocatalytic activity (Zhang et al., 2015a). 0.5 % Fe(III) loading also
improved the catalytic degradation activity by improving the visi-
ble light absorption and inhibiting charge carrier recombination.
Zirconium, molybdenum, cerium and europium have also been
doped into g-C3 N4 (Jin et al., 2015; Wang et al., 2015b, 2016; Xu
et al., 2013).
Moreover, noble metal deposition has become a popular
approach for improving the photocatalytic performance of g-C3 N4 .
Li et al. found that Ag loading improved the photocatalytic prop-
erties of g-C3 N4 nanosheets by a factor of more than seven due to
the efficient utilization of visible light and improved charge sepa-
ration efficiency (Li et al., 2015). Other studies of Ag-doped g-C3 N4
have reported the removal of a series of environmental pollutants
including toluene, E. coli and S. aureus biofilms, and MB (Bing et al.,
2015; Fontelles-Carceller et al., 2015; Xiaojuan et al., 2014).
2.3.3. Non-metal-doped g-C3 N4
Non-metal heteroatoms, such as S, O and P, have been shown
to improve the degradation of organic pollutants by improving
the visible light absorption, altering the band gap, and enhanc-
ing charge carrier separation and transfer(Chai et al., 2017; Wang
et al., 2015a; Wu et al., 2018a). Moreover, doping non-metals into
g-C3 N4 has been explored to overcome the risks of secondary pol-
lution. Besides, to overcome the limitations of applying g-C3 N4 in
photocatalysis, strategies involving coupling two or more semi-
conductors to build heterojunctions have emerged as one of the
most promising ways for tailoring its photocatalytic properties
(Mamba and Mishra, 2016; Wu et al., 2018b). These attempts to
design heterostructures provide new ideas for g-C3 N4 applica-
tions.
3. Advanced oxidation processes (AOPs)
3.1. AOPs
AOPs have been proved to be the important and useful methods
of water treatment because of their high reactivity, rapid treatment
rate, and low environmental risk (Glaze et al., 1987). During the
AOP, organic chemicals are efficiently degraded by generating var-
ious reactive oxygen species (ROS). The popular ROS employed by
different types of AOPs included hydroxyl radicals (·OH), superox-
• •
ide anions (O –), sulfate radicals (SO4 –), and singlet oxygen (1 O2 ).
Since g-C3 N4 is a fascinating material for environmental remedi-
ation, much interest has been directed to expanding the scope of
its application. In view of the features of g-C3 N4 , its application in
AOPs was expected to yield positive results. Recently, the applica-
tion of g-C3 N4 in AOPs has been applied to the treatment of landfill
leachate.
234 M. Han et al. / Process Safety and Environmental Protection 139 (2020) 230–240
Fig. 2. Advanced oxidation processes for leachate treatment.
3.2. AOPs for leachate treatment
Reactive species generated by AOPs, such as hydroxyl radicals
(·OH), act as powerful oxidizers in the degradation of refractory
pollutants, with high rate constants of ∼108 -1010 M−1 s−1 (Gautam
et al., 2019; Stasinakis, 2008). Landfill leachate contains high con-
centrations of toxic and bio-refractory compounds, which cannot
be completely removed by conventional biological or physiochem-
ical treatment processes. Hence, AOPs are expected to be the very
applicable to the treatment of landfill leachate.
The most popular ROS, ·OH derived from the Fenton reac-
tion, exhibits low efficiency in the removal of refractory organics
and ammonia because it is rapidly quenched by untargeted com-
pounds. SR-AOP (sulfate radical-advanced oxidation process) has
been shown to be more effective than the Fenton process, since
•
SO4 – has a longer half-life than ·OH in the simultaneous decom-
position of refractory organics and ammonia (Guo et al., 2020; Jiang
et al., 2018). Thus, most of the refractory pollutants in leachate
can be degraded by coupling with various AOPs (Chen et al., 2019;
Deng and Ezyske, 2011). Recent research has focused on develop-
ing efficient AOPs for leachate treatment with low chemical use and
energy consumption. The available AOPs that have been studied for
leachate treatment can be categorized into ozone-based, photo-
assisted, electrochemical, and miscellaneous processes, as shown
in Fig. 2. The different AOPs had different advantages during the
treatment, but no single process delivered the desired removal per-
formance (Gautam et al., 2019). Details of various AOPs for leachate
treatment were listed as Table 1.
Hazardous leachate can be effectively treated by altering the
molecular structure of organic compounds and oxidizing them
into biodegradable species using the high oxidative activity of
ozone. However, ozone-based AOPs have limitations due to the
low mass transfer efficiency of ozone from the gas phase to
the liquid phase (El-Din and Smith, 2001; Gautam et al., 2019).
Moreover, partial leaching of the ozone may negatively impact
the surrounding environment. Because leachate has a complex
matrix with a high content of organic compounds, a high dose
of ozone is required to achieve the desired treatment efficiency.
To a large extent, their high energy consumption and massive
emission of ozone limit the application of ozone-based AOPs to
the pre-treatment or post-treatment of leachate. Critical issues
for application of the Fenton oxidation process include the nar-
row operating pH range (< 4), the rapid consumption of Fe2+ ,
and the high cost of follow-up sludge treatment. Moreover, a
high concentration of iron contaminants is produced and the sus-
pended solids in leachate could block or absorb the UV energy
during the photo-assisted Fenton process. Although electrochemi-
cal AOPs are easy to operate, needing for large amounts of energy
and the expensive metal electrodes dominated the main draw-
back. In addition to these issues with application of the AOPs
discussed above, the characteristics of leachate (e.g. the high con-
centration of contaminants and presence of various interfering
substances) undoubtedly increase the difficulty of efficient treat-
ment.
Combining AOPs with other methods has been shown to
improve the treatment of leachate. 1,4-dioxane, one of the common
organic chemicals in leachate, was not significantly degraded by
single AOPs due to the presence of other interfering substances. Pre-
adsorption on activated carbon (AC) in photocatalysis increased the
degradation of 1,4-dioxane and decreased the production of toxic
intermediates (Nomura et al., 2020). Poblete et al. further suggested
that the use of adsorption as a pretreatment method result in a
high removal rate for organic compounds and heavy metals dur-
ing photocatalysis (Poblete et al., 2019). Ultrasound is an efficient
assistance method, because it produces tiny bubbles that expand
and implode in the liquid, coupled with the effects of turbulence
and liquid circulation, and helped cleave H2 O molecules to generate
more hydroxyl radicals. Joshi and Saurabh found that combining
ultrasonication with the Fenton reaction resulted in the efficient
treatment of leachate (Joshi and Gogate, 2019). Anfruns et al.
proposed a useful approach for efficient leachate treatment that
combines AOPs with bio-anaerobic ammonium oxidation (anam-
mox), although it had a high nitrogen content and low BOD/N ratio.
This anammox-assisted AOPs achieved a high nitrogen removal
efficiency of up to 90 % (Anfruns et al., 2013). Furthermore, combin-
ing the Fenton reaction with membrane separation was very useful
for decreasing membrane fouling and provided complementary
treatment for leachate and produced effluent with contaminant
contents that met the required regulatory levels for environmental
release (Moravia et al., 2013).
3.3. Application of AOPs with g-C3 N4 for leachate treatment
Efficient practices implied that AOPs are technically achiev-
able for the degradation and treatment of leachate. Among
AOP methods, semiconductor-assisted photocatalysis has attracted
tremendous attention because it enhances the production of reac-
tive species by employing low cost, renewable solar energy.
 M. Han et al. / Process Safety and Environmental Protection 139 (2020) 230–240 235

Table 1
. Details of various AOPs for leachate treatment.

AOPs Mechanism Advantages Disadvantages Effectiveness

Photo-assisted light adsorption and Operation at ambient conditions with Energy reduction as declining Most of the biodegradable
process radical generation possible use of solar irradiation; opacity by excessive catalyst compounds were destroyed or/and
No mass transfer limitations; addition; fewer biodegradable intermediates
Oxidizing organic compounds into pH has a complex effect on were formed;
harmless ones such as CO2 and H2 O; photocatalytic oxidation;
Electrochemical indirect oxidation Bipolar electrochemical reactors are easy Energy intensive process and More significance in removing
process (oxidation through the to operate and control; formation of chlorinated color in comparison to COD;
mediator); Operating conditions under ambient organics; Organic pollutants could be
direct oxidation (oxidation temperature and pressure prevents High operating costs caused by converted into carbon dioxide and
at anode surface); discharge and volatilization of unreacted expensive metallic electrodes; water;
wastes;
Not chemicals;
Ozone-based Molecular ozone reactions; Enhance ozone consumption; Cannot meet the discharge Alter the molecular structure of the
process ·OH radical reactions; Increase efficiency of ozonation by standards alone; organic compounds and oxidize
controlling radical generation; High ozone dose makes energy them to more biodegradable
·OH radical generation at lower pH; intensive; compounds;
Promote surface reactions between the Low mass transfer from gas to Reduce COD and BOD in leachate
adsorbed ozone and pollutants; a liquid; extensively; a good option only for
pre- or post-treatment of leachate;
Miscellaneous (Including Wet air oxidation (WAO); ultrasound assisted process, persulfate oxidation and hydrodynamic cavitation (HC), etc.
process The outcomes of different AOPs were summarized as: (a) organic substances in leachate were oxidized into the highest stable oxidation
states; (b) biodegradability of recalcitrant compounds becomes more compatible with the subsequent biological treatment;
Mechanism, advantages and disadvantages of each process were omitted here.)

The main concerns of catalyst-based AOPs for the leachate treat-
ment are structural characterization and performance evaluation
(Hou et al., 2020; Kong et al., 2019; Lu et al., 2020; Mousavi et al.,
2018; Shao et al., 2019). Structural characterization features can be
represented by the spectroscopic or morphological methods. Cat-
alytic degradation performance as well as the cycle stability need to
be highly considered (Kumar et al., 2018; Li et al., 2016a; Liu et al.,
2016). The involved mechanisms mainly include the identification
of intermediate and end products as well as the relevant analysis
of degradation pathways.
The selection of a suitable semiconductor material is essential
for photocatalysis, consequently. Among the available semiconduc-
tors, including TiO2 , ZnO, CdS, SiC, WO3 , and WS2 , TiO2 is the most
widely applied and studied semiconductor material. For landfill
leachate treatment, the first study using photocatalysis involved in
application of TiO2 as a photocatalyst on a pilot-plant scale. In this
study, humic acid (HA), a model refractory organic compound for
leachate pollutants, was rapidly decolorized and degraded under
sunlight (Wiszniowski et al., 2004). These results showed that the
photo-induced AOPs approach significantly shortens the subse-
quent biodegradation process (10 min per sample) and decreases
the BOD5 (5 days). Even though TiO2 has the advantages of long-
term stability and excellent results in combination with AOPs, its
wide band gap, low utilization of solar energy, and fast electron-
hole recombination limit its practical application. Many subsequent
studies have been conducted to improve these properties, includ-
ing by photocatalyst modification (decoration with metals, metal
doping or heterojunction construction), technical improvements,
and combination with other processes (Rocha et al., 2011; Vilar
et al., 2011a, a; Vilar et al., 2011b, b). Moreover, exploring alter-
native semiconductor photocatalysts is another important way to
improve photocatalytic leachate treatment.
g-C3 N4 has attracted wide interest as a promising photo-catalyst
because it is inexpensive, easily available, robust, and has wide
visible-light activity. The known photodegradation processes per-
formed by g-C3 N4 are shown in Fig. 3, and provide theoretical
evidences that g-C3 N4 can generate free radicals and potentially
efficiently treat leachate. As shown, during photocatalysis g-C3 N4 is
excited by absorbing photons, generating photo-induced electron-
hole pairs due to the transfer of an electron from the valence band
(VB) to the conduction band (CB) (Ge et al., 2011; Zhang et al.,
2019b). The absorbed energy (h) must be larger than the band
gap (Eg) of g-C3 N4 (∼2.7 eV) (Wen et al., 2017; Zhang et al., 2010b).
In general, during the electron transfer process, the surface elec-
trons (e− ) and holes (h+ ) serve as electron donors and acceptors for
producing strongly oxidizing or reducing radical species which can
directly degrade the various organic contaminants in leachate into
CO2 , H2 O and other small molecule products. Take phenol removal
by the Fe-g-C3 N4 graphene hydrogel (rGH/Fe-g-C3 N4 ) 3D struc-
ture as an example, in the presence of visible light, electrons and
holes could be generated by rGH/Fe-g-C3 N4 . Partial electrons would
quickly transfer to Fe3+ for Fe2+ formation, while other electrons
could transfer to graphene via ␲-␲ conjugation, and thus directly
decompose H2 O2 to form ·OH. Generated Fe2+ can further react with
H2 O2 to produce ·OH, which can firstly attack the ortho and para-
carbons within benzene ring to form catechol and hydroquinone,
subsequently open the ring to form the chain compounds and are
finally mineralized into CO2 and H2 O (Hu et al., 2020).
The application of g-C3 N4 -based materials in leachate treatment
is currently under development and there are only a limited num-
ber of reported studies. We will do our best to summarize the
existing studies and the potential of C3 N4 -induced AOPs. Although
there have been no specific studies of the practical application of
g-C3 N4 in leachate treatment, there are sufficient available mech-
anisms to eliminate the contaminants that are present in leachate.
Employing g-C3 N4 as a photocatalyst results in high degradation
performance for the recalcitrant organic pollutants in leachate
under visible light (Wang et al., 2009). Further combining fungal
degradation (using white rot fungi) with photocatalytic g-C3 N4
produced superior performance for the degradation of organic
compounds in leachate under visible light (Hu et al., 2017). The
white rot fungi that were used efficiently on pre-biodegradation
of natural lignocellulosic substrates and various organic pollutants
by secreting extracellular enzymes, and their spatial structure pro-
vided a large number of tiny interspaces and active reaction sites
for degradation reactions. Ultimately, this combination not only
achieved 74.99 % organic carbon (TOC) removal (the initial TOC con-
centration was 100 mg L−1 ), but also showed excellent degradation
potential for almost all the organic compounds present in leachate
(Hu et al., 2017). Other studies have also shown that the microbial
degradation of dye-containing wastewater by photosynthetic bac-
teria was improved significantly due to a synergistic effect between
the C16 alkane degradation performed by JLS1 bacteria and simul-
236 M. Han et al. / Process Safety and Environmental Protection 139 (2020) 230–240

Fig. 3. Schematic illustration of the photodegradation processes performed by g-C3 N4 for leachate treatment.

taneous photocatalysis by g-C3 N4 , (Xu et al., 2017; Zhang et al.,
2017).
In addition, the microbial contaminations as well as the
highly-concerned Novel Coronavirus (SARS-CoV-2) or other viruses
appeared in landfill leachate may pose severe pathogenic risks to
humans. Water disinfection and microbial control (e.g. of bacte-
ria, viruses, and microalgae) using g-C3 N4 -based photocatalysts
provide complementary treatment for leachate in addition to tra-
ditional water disinfection techniques. Previous studies showed
that g-C3 N4 possessed both excellent antibacterial and antiviral
activities (Zhang et al., 2019a), which may provide a low-cost
and environmental-friendly alternative for the sustainable leachate
treatment (Ong et al., 2016). Yu et al. displayed that the high
inactivation efficiency of antibiotic-resistant bacteria (tetracycline-
resistant Escherichia coli, TC-E. coli) in secondary effluents could be
achieved by using Ag/AgBr/g-C3 N4 as the photocatalyst (Yu et al.,
2020). In addition, Zhang et al. also found a water-surface-floating
photocatalytic g-C3 N4 composites (g-C3 N4 /EP-520) can exhibit an
excellent antibacterial/ antiviral activity under visible-light irradi-
ation, extending the application of g-C3 N4 -based material for water
disinfection (Zhang et al., 2018). To better meet the real demand,
further studies toward an in-depth understanding of the microbial
inactivation process are encouraged, while the researches about
lethal action of photocatalysts and the vulnerable components
of microbes for maximizing the inactivation efficiency are also
required. Several studies have demonstrated the theoretical and
technical feasibility of the application of g-C3 N4 in combination
with AOPS in leachate treatment. More related studies are still
required to improve the understanding of the application of AOPs
to leachate treatment. Table 2 presents in detail the relevant studies
of the potential application of g-C3 N4 in leachate treatment.
The high nitrogen load of landfill leachate increases environ-
mental stress on rivers and streams. Photocatalytic denitrification
of leachate by g-C3 N4 has become an available option. The
photocatalytically generated electrons and holes can be used
for reduction and oxidation, respectively. Photocatalytic den-
itrification using g-C3 N4 also can avoid the limitations of
applying biological denitrification, due to insufficient electron
donors. TiO2 /g-C3 N4 photocatalysts coupled with in-situ culti-
vated biofilms have been shown to enhance nitrate reduction
in water, with 40.3 % removal of the nitrate after 16 h. This
approach provides a new strategy for enhancing nitrate reduc-
tion in leachate and insights into the reduction mechanism (Zhang
et al., 2020). Moreover, the hazards of releasing large molecu-

Table 2
Relevant studies of the potential application of g-C3 N4 to the treatment of substances in leachate.

Categories Substances Photocatalysts Efficiency Ref. (Year)

Organics all organic compounds in leachate, a combination of 74.99 % TOC removal efficiency (Hu et al., 2017)
especially volatile fatty acids and Phanerochaete chrysosporium (72 h, initial concentration of
long-chain hydrocarbons and photocatalysis with g-C3 N4 100 mg L−1 )
Heavy metals and Cr(VI) Ti3+ -TiO2 /g-C3 N4 65 %/39 % (Lu et al., 2015)
salts
As(III) urea-derived g-C3 N4 70 % (Kim et al., 2018)
nitrate reduction TiO2 /g-C3 N4 40.3 % (16 h) (Zhang et al., 2020)
High molecular amoxicillin (AMX) A magnetic fluorinated 90 % (Mirzaei et al., 2019)
weight mesoporous g-C3 N4
compounds
bisphenol A (BPA) Pd/g-C3 N4 nanoparticles 91 % BPA with an initial (Wang et al., 2017)
concentration of 20 mg L−1 in
60 min
trace polychlorinated biphenyls magnetic carbon nitride – (Li et al., 2017)
(PCBs) nanocomposites
degradation of 2-chlorophenol Cr2 O3 /g-C3 N4 94 % (Anjum et al., 2018)
tetracycline hydrochloride Polymeric carbon 18.9 % (pharmaceutical (Wang et al., 2018)
(TC-HCl) nitride foam (CNF) wastewater) to 78.9 % (natural
seawater)
Other disinfection and microbial control g-C3 N4 bacteria were broken in 12 h; virus (Zhang et al., 2019a) (Ong
died after 6 h; all microalgae et al., 2016)
ruptured after 6 h
 M. Han et al. / Process Safety and Environmental Protection 139 (2020) 230–240
lar weight organic compounds into the environment are also an
important issue in leachate treatment. A magnetic fluorinated
mesoporous g-C3 N4 has been employed for the photocatalytic
degradation of the antibiotic amoxicillin (AMX) in leachate, and
achieved a higher degree of mineralization with a lower accu-
mulation of toxic by-products (Mirzaei et al., 2019). Moreover,
•
AOPs based on sulfate radicals (SO4 –), which have a high oxi-
dation potential, can be combined with g-C3 N4 . Sulfate radicals
are usually generated by the activation of persulfate (PS) through
heating, UV irradiation, bases, or transition metals. g-C3 N4 dis-
played high catalytic activity for the activation of persulfate in
persulfate-based AOPs. The results reported by Wang et al. indi-
cated that Pd nanoparticles anchored on g-C3 N4 were very active
for the degradation of bisphenol A (BPA) by efficiently activating
PMS (Wang et al., 2017). The composite photocatalyst Cr2 O3 /C3 N4
achieved the rapid photodegradation of 2-chlorophenol under visi-
ble light with a removal rate of 94 % at the optimal pH (Anjum et al.,
2018).
4. Conclusion
In this review, current development and progress on the appli-
cation of g-C3 N4 to leachate treatment have been showcased. The
application of g-C3 N4 as a photocatalyst in AOPs for the treatment
of landfill leachate has been comprehensively reviewed, provid-
ing theoretical and technical possibilities for the wide application
of g-C3 N4 -based AOPs for leachate treatment. Notably, although
there have been a large number of studies dedicated to the applica-
tion of g-C3 N4 -based photocatalysts in the evolution of H2 and the
degradation of pollutants, direct practical applications to landfill
leachate have received less attention. Most studies have dealt with
the degradation of single components in leachate. The development
of a high-performance g-C3 N4 catalyst would be key for the reme-
diation of complex wastewater using AOPs. Based on laboratory
tests and theoretical studies, and considering the characteristics of
waste leachate like its complex, high concentration components,
high ammonia nitrogen content, and the presence of unknown
interfering substances, it is necessary to expand this application
to resolve the practical issues of leachate pollution. Coupling AOPs
with other methods and technologies should be actively explored
and applied in practical problem solving. Furthermore, leachate
treatment using g-C3 N4 should also be extended to the remediation
of secondary sites, such as leachate sediment and the surround-
ing soil. Hopefully, this review will encourage more research into
applying the robust and inexpensive g-C3 N4 in photocatalytic AOPs
for leachate treatment.
Declaration of Competing Interest
The authors declare that they have no known competing finan-
cial interests or personal relationships that could have appeared to
influence the work reported in this paper.
Acknowledgements
This work was finically supported by the National Natural Sci-
ence Foundation of China (No. 51961165104) and the Project of
Thousand Youth Talents (No. AUGA2160100917).
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