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Article history:
Received 23 May 2016
Received in revised form 2 July 2016
Accepted 3 July 2016
Available online xxx
Keywords:
Carbon nitride (g-C3 N4 )
Composite photocatalysts
Co-catalysts
Articial photosynthesis
Z-scheme heterojunction
Nanocarbons
a b s t r a c t
As one of the most appealing and attractive technologies, heterogeneous photocatalysis has been utilized
to directly harvest, convert and store renewable solar energy for producing sustainable and green solar
fuels and a broad range of environmental applications. Due to their unique physicochemical, optical and
electrical properties, a wide variety of g-C3 N4 -based photocatalysts have been designed to drive various reduction and oxidation reactions under light irradiation with suitable wavelengths. In this review,
we have systematically summarized the photocatalytic fundamentals of g-C3 N4 -based photocatalysts,
including fundamental mechanism of heterogeneous photocatalysis, advantages, challenges and the
design considerations of g-C3 N4 -based photocatalysts. The versatile properties of g-C3 N4 -based photocatalysts are highlighted, including their crystal structural, surface phisicochemical, stability, optical,
adsorption, electrochemical, photoelectrochemical and electronic properties. Various design strategies
are also thoroughly reviewed, including band-gap engineering, defect control, dimensionality tuning,
pore texture tailoring, surface sensitization, heterojunction construction, co-catalyst and nanocarbon
loading. Many important applications are also addressed, such as photocatalytic water splitting (H2
evolution and overall water splitting), degradation of pollutants, carbon dioxide reduction, selective
organic transformations and disinfection. Through reviewing the important state-of-the-art advances
on this topic, it may provide new opportunities for designing and constructing highly effective g-C3 N4 based photocatalysts for various applications in photocatalysis and other related elds, such as solar
cell, photoelectrocatalysis, electrocatalysis, lithium battery, supercapacitor, fuel cell and separation and
purication.
2016 Elsevier B.V. All rights reserved.
1. Introduction
Nowadays, among the various possibilities for exploring attractive sustainable energy sources and technologies, photocatalytic
technology is considered as one of the most appealing and promising technologies to directly harvest, convert and store renewable
solar energy for generating sustainable and green energy and
a broad range of environmental applications. In 1972, the pioneering work of photoelectrochemical (PEC) H2 production from
water splitting using a Pt-attached n-TiO2 cell was rstly reported
by Fujishima and Honda [1]. Subsequently, Bard extended the
basic principle of PEC water splitting system to the heterogeneous photocatalytic systems with illuminated semiconductor
particles suspended in water as photocatalysts [25]. Since then,
Corresponding authors.
E-mail addresses: chenxiaobo@umkc.edu (X. Chen), Xinliscau@yahoo.com
(X. Li).
the heterogeneous photocatalysis occurring on powdered semiconductors has been widely used in the different elds, such
as water splitting [610], environmental remediation [9,1115],
CO2 reduction [1620], disinfection [21] and selective organic
transformations[2224]. It is noteworthy that there has been a
growing interest in the use of semiconductors as photocatalysts
for various applications (the red columns in Fig. 1a). In 2015, more
than 5500 papers about the photocatalytic applications have been
published, further indicating the high importance and tremendous research interests in heterogeneous photocatalysis. Clearly,
the presence of efcient photocatalysts plays an essential role
in determining the overall quantum efciency of all these photocatalytic reaction systems. During the past 40 years, various
available semiconductor materials such as TiO2 , SrTiO3 , CdS, BiVO4 ,
Ta3 N5 , TaON, g-C3 N4 , Ag3 PO4 , and their nanostructured assemblies
have been extensively employed as photocatalysts to directly harness solar energy for different redox reactions [7,2530]. As the
most widely employed golden photocatalyst, TiO2 has dominated
the published work on heterogeneous photocatalysis owing to its
http://dx.doi.org/10.1016/j.apsusc.2016.07.030
0169-4332/ 2016 Elsevier B.V. All rights reserved.
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Fig. 1. (a) The annual number of publications containing the word graphene* (TiO2 *, g-C3 N4 * or carbon nitride*) in the title and photocataly* in the topic since 2009. (b)
The annual number of citations for Wangs pioneering paper published on Nature Materials in 2009. (Using Web of Science, date of search: Jul 2, 2016).
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Table 1
Band gap structures of several typical photocatalysts.
Semiconductor
TiO2
Cu2 O
CdS
g-C3 N4
g-C3 N4
Ta3 N5
TaON
BiVO4
WO3
Ag3 PO4
a
Crystal structure
Anatase
cubic
Ref.
CB
VB
Eg /eV
0.5
1.16
0.9
1.3
1.53
0.75
0.75
0.3
0.1
0.04
2.7
0.85
1. 5
1.4
1.16
1.35
1.75
2.1
2.7
2.49
3.2
2.0
2.4
2.7
2.7
2.1
2.5
2.4
2.8
2.45
[90]
[91]
[92]
[44,84]
[93]a
[94]
[94]
[95]
[96]
[97]
Measurement by the valence band X-ray photoelectron spectroscopy (VB XPS) spectrum.
Table 2
Standard redox potentials for some typical species [83,98].
Reaction
E0 (V) vs NHE at pH 0
2H+ + 2e H2 (g)
O2 (g) + e O2 (aq)
O2 (g) + H+ + e HO2 (aq)
O2 (g) + 2H+ + 2e H2 O2 (aq)
2H2 O (aq) + 4 h+ O2 (g) + 4H +
OH + h+ OH
O3 (g) + 2 H+ + 2 e O2 (g) + H2 O
CO2 + e CO2
2 CO2 (g) + 2 H+ + 2 e HOOCCOOH(aq)
CO2 (g) + 2H+ + 2e HCOOH(aq)
CO2 (g) + 2 H+ + 2e CO(g) + H2 O
CO2 (g) + 4H+ + 4e C(s) + 2H2 O
CO2 (g) + 4H+ + 4e HCHO(aq) + H2 O
CO2 (g) + 6H+ + 6e CH3 OH(aq) + H2 O
CO2 (g) + 8H+ + 8e CH4 (g) + 2H2 O
2CO2 (g) + 8H2 O + 12e C2 H4 (g) + 12OH
2CO2 (g) + 9H2 O + 12e C2 H5 OH(aq) + 12OH
3CO2 (g) + 13H2 O + 18e C3 H7 OH(aq) + 18OH
H2 O2 (aq) + H+ + e H2 O + OH
HO2 + H+ + e H2 O2 (aq)
H2 O2 (aq) + 2H+ + 2e 2H2 O
0
0.33
0.046
0.695
1.229
2.69
2.075
1.9
0.481
0.199
0.11
0.206
0.07
0.03
0.169
0.07
0.08
0.09
1.14
1.44
1.763
surface active sites or co-catalysts, and further stimulate the elctrocatalytic reduction (stage 6) and oxidation (stage 7) reactions of the
reactants adsorbed on the semiconductor, respectively. It should
be noted that the surface reactions possibly occur only when the
reduction and oxidation potentials are more positive and negative
than CB and VB levels, respectively. Some typical standard redox
potentials have been listed in Table 2. Notably, almost all reactions in Table 2 exhibit the same linear pH dependence with a
slope of 0.059 V, apart from E0 (O2 /O2 ) which is pH-independent
[83,87]. Furthermore, for the surface electrocatalytic reactions (surface charge utilization), the large onset overpotential and sluggish
kinetics are two key factors limiting the surface photocatalytic
efciency of reduction and oxidation reactions. Principally, these
two restrictive factors can be overcome by loading suitable cocatalysts (electrocatalysts) simultaneously [88]. More importantly,
the co-catalysts (electro-catalysts) can play the additional roles in
improving the photostability and charge separation of semiconductors [89]. The complicated co-catalyst effects will be thoroughly
discussed in the section 4.7.
However, it should be noteworthy that the photocatalytic quantum efciency (c ) is strongly determined by the cumulative effect
of the efciency in all four-step processes, including light harvesting efciency (abs ), charge separation efciency (cs ), charge
migration and transport efciency (cmt ), and charge utilization
efciency (cu ) for H2 generation. The relationship between them
could be expressed according to Eq. (1) [7]:
c = abs cs cmt cu
(1)
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Fig. 3. The redox potentials of the relevant reactions with respect to the estimated position of the g-C3 N4 band edges at pH 7.
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Table 3
Structural parameters and total energies for different C3 N4 phases [131].
C3 N4 phases
Space group
Lattice parameter ()
Alpha
Beta
Cubic
Pseudocubic
g-h-triazine
g-h-heptazine
g-o-triazine
P31 c (159)
P3 (143)
I-43d (220)
P42 m (111)
P-6m2 (187)
Cmc21 (36)
P2 mm (25)
a = 6.465, c = 4.709
a = 6.406, c = 2.406
a = 5.411
a = 3.426
a = 4.746, c = 6.586
a = 7.083, b = 12.269, c = 6.871
a = 4.147, b = 4.754, c = 6.474
4
2
2
1
2
4
2
5.49
4.85
4.30
4.13
2.97
2.88
0.93
3.76
3.12
2.87
2.53
1.16
0.89
composition, structures and properties. More denitely speaking, hetero-junction construction [120,121], dimensionality tuning
(nano-templating [122,123]) and nanocarbon loading have been
widely applied in promoting the charge transfer, mobility and
separation respectively. Furthermore, suitable co-catalyst loading
[44,124127] and defect control have been available in accelerating
the surface reaction kinetics (charge utilization). In addition, pore
texture tailoring, surface sensitization, and band-gap engineering (non-metal doping [128] and co-polymerization [84,129,130]
strategies) were utilized to create highly mesoporous g-C3 N4 with
high surface area and to increase the light harvesting and visible absorption through the red-shift of its optical absorption edge,
respectively. In future, it is expected more and more engineering
modication strategies will be developed to improve the photocatalytic performances of g-C3 N4 -based photocatalysts. More
importantly, all different photocatalytic stages such as light harvesting, charge excitation, charge transfer, mobility and separation,
and surface charge utilization should be simultaneously considered and optimized [7]. In other words, the synergy and integration
effect of these different strategies should be paid more attention.
In the following sections, the versatile properties, design strategies
and potential applications will be thoroughly summarized.
Fig. 5. Design considerations of g-C3 N4 -based photocatalysts based on the different
photocatalytic stages.
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Fig. 6. The stacked 2D layered structure of g-C3 N4 (a); structures of s-triazine (b) and tri-s-triazine (c) as the primary building blocks of g-C3 N4 .
Fig. 7. XRD patterns of (a) the tubular carbon nitride and (b) the bulky g-C3 N4
synthesized by directly heating melamine at 520 C for 2 h [138].
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Fig. 10. Comparison between the Raman spectra of coplanar bulk and 1-layer gC3 N4 samples (780 nm laser) [154].
means of chemical oxidation, thus greatly favoring their good dispersion in the aqueous solutions and further enhanced interfacial
coupling and photocatalytic activities [140145].
Commonly, these functional groups and networks (C N ) could
be further identied by the Fourier transform infrared (FT-IR) spectra, X-ray photoelectron spectroscopy (XPS) measurements, Raman
spectra, and Boehm titration analysis. Generally, the chemical composition and bonding information of g-C3 N4 could be partially
identied by FT-IR measurement. Fig. 9 depicts typical FTIR spectra
of g-C3 N4 powders obtained by heating melamine (MCN), thiourea
(TCN), and urea (UCN) [146]. As shown, the main characteristic
peaks observed in the region from 900 to 1700 cm1 were usually
assigned to stretching vibration signals of aromatic heptazinederived repeating units, including the typical sp2 C N stretching
modes and out-of-plane bending vibrations of the sp3 C N
bonds [130,147150], while the sharp absorption peak centered
at approximately 810 cm1 was attributed to the characteristic
breathing mode of tri-s-triazine cycles [150152]. Meanwhile, the
absorption band at 883 cm1 were indexed as the deformation
mode of N H in amino groups [153], whereas the broadened
peaks between 3000 and 3500 cm1 were related to the stretching vibration [146,149,150,153] of residual free N H in the bridging
C NH C units and O H originated from physically adsorbed water
species on g-C3 N4 surface, respectively. In the recorded Raman
spectra, several characteristic peaks of g-C3 N4 can be observed
at 1616, 1555, 1481, 1234, 751, 705, 543, and 479 cm1 , further
conrming the vibration modes of CN heterocycles [151,154]. It
should be noted that the peak at 1234 cm1 , corresponding to
the N C (sp2 ) bending vibration, exhibits signicant blue shift
(1250 cm1 for 1-layer g-C3 N4 ), due to the phonon connement
and strong quantum connement effect [154]. Moreover, it has also
been experimentally and theoretically demonstrated that the ratios
of peak heights of 751705 cm1 (I751 /I705 ) and 543479 cm1
(I543 /I479 ), corresponding to layerlayer deformation vibrations or
the correlation vibrations, obviously increased with decreasing the
layer number of g-C3 N4 [154]. Additionally, the nitrogen containing species can be further quantitatively analyzed by the element
analysis and Boehm titration. For the element analysis, X-ray photoelectron spectroscopy (XPS) can not only reveal the atom ratio
of carbon to nitrogen, but also identify the carbon and nitrogen
species in g-C3 N4 . For example, the main peak at 288.2 eV in the
high-resolution C 1s XPS spectra of the 1.0 wt% RGO/g-C3 N4 sample, indicates the existence of the N C N2 coordination [151]. The
N 1 s binding energies at about 398.6, 399.8, and 401.5 eV in the
high-resolutionN1 s XPS spectra of the 1.0 wt% RGO/g-C3 N4 sample can be assigned to sp2 -hybridized nitrogen (C N C), tertiary
nitrogen (N (C)3 ) and amino functional groups having a hydrogen
atom (C N H), respectively [146,151,155,156]. For Boehm titration analysis, it was found that the content of basic group per unit
area of g-C3 N4 generally decreased with increasing the calcination
temperature [157]. In a word, the combination of Raman vibration properties, FTIR, XPS spectra and Boehm titration analysis can
fully reveal the surface functional groups of g-C3 N4 nanomaterials
(Figs. 9,10 and 11).
Interestingly, the basic surface functionalities can be further
evidenced by the isoelectric point (IEP) and the zeta potentials of
g-C3 N4 dispersions [146]. It is known that the IEP is an important
physicochemical parameter of many compounds, such as oxides,
suldes, hydroxides, and nitrides, which has been widely used
to estimate the surface charges of compound particles at various pH conditions. In general, the solid particles are positively
Fig. 11. High-resolution XPS spectra of C 1s (A) for the 1.0 wt% RGO/g-C3 N4 sample (a) and GO (b) and N 1s (B) for the 1.0 wt% RGO/g-C3 N4 sample [151].
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Fig. 12. Zeta potentials of MCN, TCN, and UCN powders as functions of the pH value
of the suspensions (as shown in Fig. 12) [146].
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Fig. 13. The TG-DSC analysis for heating the melamine (a) and the g-C3 N4 (b) obtained by heat polymerization of melamine at 520 C [149].
Fig. 14. Reaction path for the formation of g-C3 N4 starting from cyanamide.
Fig. 15. Electronic structure of g-C3 N4 . (a) DFT band structure for g-C3 N4 calculated
along the X and Y directions. The potentials for H+ to H2 and H2 O to O2 are
displayed by the blue and red dashed lines, respectively; the KohnSham orbitals
for the valence band (b) and conduction band (c) of g-C3 N4 . The C, N and H atoms are
gray, blue and white, respectively. The isodensity surfaces are drawn for a charge
density of 0.01qe A3 [44]. (For interpretation of the references to colour in this
gure legend, the reader is referred to the web version of this article.)
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Fig. 16. Schematic illustration of the band structures of different types of g-C3 N4 samples: g-C3 N4 [84], Feg-C3 N4 [54,181], Sg-C3 N4 [182], Pg-C3 N4 [183], Og-C3 N4 [184],
Cg-C3 N4 [185], Ig-C3 N4 [186] and Bg-C3 N4 [84]. VB-XPS: valence band X-ray photoelectron spectroscopy; MS: electrochemical analysis by MottSchottky plots.
Fig. 17. (a), time-resolved PL spectrum monitored at 525 nm under 420 nm excitation at 298 K for bulk g-C3 N4 (black) and mpg-C3 N4 (red) [123];(b), time-resolved PL spectra
monitored at 480 nm under 420 nm excitation at 77 K for CN and CNSCN [121]. (For interpretation of the references to colour in this gure legend, the reader is referred to
the web version of this article.)
In addition, the underlying electronic properties and charge carrier dynamics, including the microscopic dynamic process of the
charge generation, recombination, separation, and transfer, play
crucial roles in determining the photocatalytic performance [7,58].
Thus, the in-depth understanding of the electrical properties and
charge carrier dynamics is, therefore, fundamentally important
to help us to design and construct the more efcient and stable
g-C3 N4 -based composite photocatalysts. To date, many different
advanced techniques, such as femtosecond transient absorption
(TA) spectroscopy [188,189], time-resolved uorescence spectroscopy, transient photocurrent decay, Nyquist impedance plots
and the transient photovoltage (TPV) technique [190195] have
been available in studying the charge carrier dynamics of g-C3 N4 based composite photocatalysts. For instance, Wang et. al measured
the time-resolved PL spectrum of bulk g-C3 N4 and revealed that the
photoinduced charge carriers in bulk g-C3 N4 showed a lifetime of
5 ns even at 298 K, indicating the fast recombination rate (Fig. 17a)
[123]. The greatly suppressed PL signal of mpg-C3 N4 further indicated that the surface terminal sites of mpg-C3 N4 can promote the
electron relocalization, thus accelerating the catalytic functions of
mpg-C3 N4 for surface redox reactions. Similarly, the isotype heterojunctions between g-C3 N4 and S-doped g-C3 N4 have been found to
exhibit a matched band alignment, which can signicantly promote
the charge separation between them, thus resulting in prolonging
the lifetime of photo-excited charge carriers by about 2.15 ns [121].
It is believed that the prolonged lifetime of photo-generated charge
carriers could further increase their utilization efciency in driving
surface photoredox reactions. Recently, the TA spectra of g-C3 N4
also revealed that the existence of silica templates can prolong the
lifetime of excited charge carriers by about hundreds of picoseconds, thereby achieving the high photocatalytic activities (Fig. 17b)
[188]. More recently, it was demonstrated that the charge separate
efciency in g-C3 N4 -based photocatalysts could be also revealed
by the SPV measurement, as an advanced and facile technology. As
shown in Fig. 18, the obviously increased SPV signal in the range
Fig. 18. SPV of g-C3 N4 (Ni0) and Ni@g-C3 N4 (Ni10). The inset shows the schematic
setup of SPV measurements [192].
of 300450 nm could be achieved through loading Ni nanoparticles on g-C3 N4 as co-catalysts, suggesting the greatly accelerated
charge separation efciency [192,193].
3.5. Optical properties
For various kinds of photochemistry-related applications of gC3 N4 , the decisive optical properties, including Ultravioletvisible
(UV/Vis) absorption, photoluminescence (PL) and electrochemiluminescence (ECL), have been readily further revealed by means
of the theoretical calculations or experimental characterizations
[47,55,187]. The typical UV/Vis absorption spectrum of g-C3 N4 prepared at different temperature were displayed in Fig. 19a [44].
Indeed, the absorption edge of conventional g-C3 N4 shows an
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Fig. 19. (a) UV/Vis absorption spectra of g-C3 N4 prepared at different temperature. Inset: photograph of the photocatalyst [44]; (b) the room-temperature PL spectrum
of g-C3 N4 solid powder ( = 365 nm, top gure) and the ECL spectrum of g-C3 N4 -modied electrode in 0.10 M K2 SO4 and 3.0 mM K2 S2 O8 solution by cycling the potential
between 0.00 and 1.30 V (vs. Ag/AgCl) with a scan rate of 100 mV/s and step potential of 1 mV (bottom gure) [78].
detection of trace metal ions, such as Cu2+ . Therefore, it is naturally expected that the metal-free and non-toxic g-C3 N4 could be
extensively utilized as a multifunctional optical material for light
emitting devices [62,63], bioimaging, [100,142,204,205] ECL sensing probe [76,78,206,207] and uorescent probes [208210].
3.6. Adsorption properties
Generally speaking, adsorption property of a given adsorbent
is strongly dependent by both its porous microtexture and surface chemical property [211215]. Similar to the 2D graphene or
graphene oxide materials, a wide variety of targeted adsorbates
can be adsorpted on the multiple different functional groups (e.g.,
amino groups) and defect sites on g-C3 N4 through different types
of interactions such as physical adsorption (- stacking interaction), electrostatic attraction, or chemical interaction (surface
complexation or acid-base interactions) [216]. Due to the weaker
- stacking interaction in the physical adsorption, the stronger
electrostatic attraction and chemical interaction have been proposed to the improved adsorption properties of g-C3 N4 , which will
be thoroughly discussed in this section.
Based on the electrostatic attraction, it has been demonstrated
that the selective photodecomposition of anionic methyl orange
(MO) or cationic methyl violet (MV) and methylene blue (MB) could
be achieved over positively or negatively charged TiO2 -based semiconductors, respectively [217219]. Similarly, the electrostatic
attraction between the negatively charged g-C3 N4 and positively
charged adsorbate molecules, such as cationic MV and MB have
been proposed to achieve the selective adsorption and photocatalysis in many studies. For example, Yu and his coworkers
demonstrated that the negatively charged g-C3 N4 particles exhibited extraordinaryly higher adsorption capacity towards a cationic
MB dye than anionic MO dye in aqueous suspension [146]. Further results showed that the adsorption kinetics of MB on three
different kinds of g-C3 N4 (Fig. 20a) could be well depicted by a
pseudo-second-order kinetic equation as follows [220]:
dqt /dt = k2 (qe qt )2
(2)
(3)
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Fig. 20. Adsorption kinetics (a) and adsorption isotherms (b) of methylene blue on MCN, TCN, and UCN [146].
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Fig. 21. (a) CO2 -capture capacities of g-C3 N4 (CN) and amine-functionalized g-C3 N4 (3CN) [227]; (b) CO2 adsorption isotherms of the mesoporous g-C3 N4 microspheres at
25 and 75 C [229].
Fig. 22. (A), (a) Free energy plots of ORR on g-C3 N4 with 0e , 2e , and 4e paths (corresponding to paths I, II, and III). (bd), Schemes of ORRs pathway on pristine g-C3 N4
with 0e , 2e or 4e participation, respectively (red areas represent the active sites facilitating ORR). (B) ORR polarization curves for various electrocatalysts on rotating
electrode at 1500 rpm in O2 -saturated 0.1 M KOH solution [69]. (For interpretation of the references to colour in this gure legend, the reader is referred to the web version
of this article.)
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Fig. 23. (a) The HER polarization curves of g-C3 N4 , NG, g-C3 N4 /NG mixture, 33 wt% of g-C3 N4 @NG and referenced 20% Pt/C smaples (electrolyte: 0.5 M H2 SO4 , scan rate:
5 mV s1 ). (b) The calculated Gibbs free-energy for chemical adsorption of H* on three metal-free catalysts and Pt reference at the equilibrium potential. (c) Volcano plots of i0
as a function of the GH for the C3 N4 @NG (red triangle), various metals (open symbols) and a nanostructured MoS2 electrocatalyst (closed symbol) [239]. (For interpretation
of the references to colour in this gure legend, the reader is referred to the web version of this article.)
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Fig. 24. (a) Variation of photocurrent density versus applied voltage. Number lables (3), (2), and (1) data represent the hybrid 3D WO3 /C3 N4 //CoOx , WO3 /C3 N4 , and WO3 ,
respectively. (b) Energy diagram and expected charge ow of WO3 /C3 N4 [285].
of g-C3 N4 , thus resulting in enhanced separation and immigration of photo-generated carriers under visible light [305]. More
recently, Dong and coworkers revealed that K atoms could achieve
an interlayer doping (as shown in Fig. 26b), instead of the cave
doping of Na atoms in g-C3 N4 [306]. It is believed that K atoms can
bridge the two adjacent g-C3 N4 layers, which lead to the narrowed
band gap, extended conjugated systems, and positive-shifted
valence band position, thus achieving the increased visible-light
harvesting, efcient charge separation, and strong oxidation capability, respectively. In contrary, despite of the increased in-planar
electron density and visible-light absorption, the cave doping of
Na atoms still exhibits high recombination rate of carriers in the
g-C3 N4 planes, thus resulting in the reduced photocatalytic performance [306]. This work might provide new insights into the deep
understanding on the metal doping of g-C3 N4 and the design of
electronically optimized layered photocatalysts for enhanced solar
energy conversion.
Apart from metal doping, the non-metal doping of g-C3 N4 has
been majorly realized through the chemically substituted doping.
As displayed in Fig. 16, almost all the non-metal doping, such as
S [118,182,307311], P [183,312316], B [114,317320], O [184],
C [185], and I [128,186], could narrow the bandgap of g-C3 N4 and
enhance its light harvesting capability. In general, the C self-doping
can substitute the bridging N atoms [185], whereas the O [184,321],
S [307,309,322] and I [128,186] doping could achieve the replacement of N atoms in the aromatic triazine rings (as shown in Fig. 27).
Interestingly, the doping of these different elements can promote
the delocalization of the -conjugated electrons, which is fundamentally important for improving the conductivity, mobility and
separation of photo-generated electrons, thus greatly enhancing
the photocatalytic performances of doped g-C3 N4 . In the contrary, the substituted doping of P [183,315,316,323326] and B
[327,328] atoms preferentially occur on the C atoms, thus leading to the formation of strong Lewis acid sites (P+ ) on the basic
surface (from amine or imine groups) of g-C3 N4 , due to the intrinsic polarization of PN bond and delocalization of one extra lone
electron in electron-rich P atom [324]. Most recently, Qiaos group
demonstrated that the P-doping of porous g-C3 N4 nanosheets can
drastically narrow the intrinsic band gap from 2.98 to 2.66 eV and
promote the photo-excitation of electrons from the VB of P-doped
g-C3 N4 , due to the formation of vacant midgap states below the
CB minimum of g-C3 N4 through the hybridization of C 2s2p, N
2s2p and P 3s3p, thus enhancing visible light absorption [326].
Meanwhile, it was also demonstrated that the (NH4 )2 HPO4 as phosphorus precursor could achieve the cave doping (in the interstitial
sites, as shown in Fig. 27). Furthermore, it is well known that S
atoms have been found to preferentially substitute N atoms with a
larger electronegativity (3.04), thus leading to the decreased VB/CB
levels and band gap [118,182,199,307,310,329]. Nevertheless, as
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Fig. 26. Two kinds of metal ion doping of g-C3 N4 framework: (a) cave doping, the incorporation of metal ions (Mn + ) through the coordination interactions, Color scheme:
C, red; N, yellow [27]; (b) interlayer doping (the interlayer bridging pattern for K) [306]. (For interpretation of the references to colour in this gure legend, the reader is
referred to the web version of this article.)
Fig. 27. Possible substituted sites of non-metal doping in the single layer of g-C3 N4 .
special cases, in situ sulfur and boron doping of g-C3 N4 has also
been found to replace the C and N atoms in the rings, respectively [182,330]. In addition, the F doping (NH4 F as a cheap uorine
source) can achieve the formation of the C F bonding in g-C3 N4
(as shown in Fig. 27), thus lowering the electronic band gaps [331].
However, it should be point out that excessive doping of nonmetal
and metal is found to be detrimental to enhance the photocatalysis,
because the more defects can also act as the recombination centers
of electronhole pairs. In future, the co-doping of different metals
and/or nonmetals, such as Fe/P [332] S/Co/O [333], S/P [334], P/O
[335], K/Na [336] and C/Fe [337] deserves more attention, due to
their positive synergetic effects on the visible-light absorption and
photocatalytic properties.
In addition, copolymerization at molecular level was also widely
employed to strongly enhance the photocatalytic activity of g-C3 N4 ,
via simultaneously modulating its band gap, electronic structures
and physical and chemical properties. Commonly, it is believed
that the copolymerization modication with structure-matching
aromatic compounds or organic additives could increase the
desired delocalization of -conjugated electrons and improve the
intrinsic drawbacks in g-C3 N4 , thus maximizing the photochemical activities [54,338341]. For example, Wang and co-workers
demonstrated that the tunable bandgaps of tri-striazine-based
g-C3 N4 ranging from 2.67 to 1.58 eV could be obtained (as
shown in Fig. 28a) through the copolymerization of dicyandiamide (monomer) and different amounts of barbituric acid (BA,
comonomer) [84]. More interestingly, 2D g-C3 N4 nanosheets fabricated by the one-pot condensation of urea and electron-rich
thiophene co-monomers could achieve the highest quantum efciency of 8.8% at 420 nm for H2 generation, (Fig. 28b) owing to
the narrowed band gap, improved electron migration and through
the formation of surface dyadic structures [129,342]. In contrary,
the molecular doping by an electron-decient pyromellitic dianhydride could thereby enhance the strong photooxidation capability
of g-C3 N4 , due to greatly decreased both the CB and VB positions [343]. To sum up, as a unique bottom-up way for tailoring
the bandgap of g-C3 N4 , the copolymerization approach provides
more opportunities for designing highly effective polymeric photocatalysts with desired electrical properties and band gap through
incorporating structure-matching organic moleculars, which also
provides insights into the mechanism of heterogeneous photocatalysis of organic semiconductors at molecular levels.
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Fig. 28. (a) UVvis absoprtion spectra of g-C3 N4 and CNBx (arrow direction, x = 0.05, 0.1, 0.2, 0.5, 1, 2), where x refers to the weight ration of barbituric acid [84]. (b) H2
evolution over different g-C3 N4 copolymerized by urea and various monomers (3wt%Pt as co-catalyst) [129].
Fig. 29. (a) UVvis absorption spectra g-C3 N4 (GCN) and amorphous g-C3 N4 (ACN). Inset: Schematic of monolayer crystalline GCN and ACN; (b) The detailed band structures
of GCN and CAN, as well as the redox potentials of water splitting [348].
Fig. 30. (a) Lateral view and (b) vertical view for the interactions between water and a layer of defect g-C3 N4 sheet. Red, white, gray and white spheres represent O, H, C
and N atoms, respectively. (c) Spatial distribution functions of O and H atoms projected onto the defect g-C3 N4 sheet within the rst layer [353]. (For interpretation of the
references to colour in this gure legend, the reader is referred to the web version of this article.)
from 460 to 682 nm (as shown in Fig. 29a). The further valence
band XPS analysis reveals that the levels of VB and CB could be
reduced by 0.31 and 0.61 eV, respectively, without affecting the
thermodynamic requirements for O2 evolution and water reduction (as shown in Fig. 29b). These results could open up new ways
to develop visible light-driven amorphous or defective g-C3 N4 photocatalysts.
Apart from Ar-atmosphere heat treatment, the hightemperature treatment of pristine g-C3 N4 in a H2 , NH3 or
vacuum atmosphere could also create nitrogen or carbon vacancies in carbon nitrides, thus achieving the narrowed band gap
and improved photocatalytic performances [347,349351]. For
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example, a novel g-C3 N4 photocatalyst with N-vacancy structures and a bandgap of 2.03 eV could be fabricated by heating
the melon in a H2 atmosphere [347], which exhibits promising
photocatalytic activities towards generating OH radicals and
decomposing the organic pollutant Rhodamine B. It is believed
that the nitrogen-vacancy defects could greatly widen visible light
absorption range and suppress the unexpected fast recombination
of photo-excited carriers, thus achieving the improved photoactivity. Similarly, it was also demonstrated that the introduction of
hydrogenated defects in g-C3 N4 nanosheets could greatly enhance
the photocatalytic hydrogen evolution [349,352]. Furthermore, a
simple thermal treatment under an NH3 atmosphere can not only
develop highly porous g-C3 N4 nanosheets with plenary carbon
vacancies through etching their lattice carbon sites by the reactive
radicals from the NH3 decomposition [350,351], but also can
enhance the surface area, porosity and crystallinity of condensed
g-C3 N4 , due to the greatly reduced N defects in the -conjugated
network [346]. More interestingly, through employing both DFT
and molecular dynamics calculations, Wu et al. indicated that
the defect within g-C3 N4 played a key role in the adsorption
and dissociation of water, whereas, water does not dissociate on
the perfect g-C3 N4 sheet (as shown in Fig. 30) [353]. However,
it should be noted that the excessive nitrogen vacancies as the
recombination centers could be also harmful for the photocatalysis
[354]. To demonstrate this point, Osterloh and co-workers found
that surface structure defects in g-C3 N4 , with energy levels at
+0.97 V and 0.38 V (vs.NHE), limit visible light driven hydrogen
evolution and photovoltage [191]. More interestingly, it was also
demonstrated that the vacuum heat-treatment at 500 C could
obtain the highest photoactivity for H2 evolution due to the
increased content of the tri-s-triazine phase and suitable N defects
in the tri-s-triazine ring building blocks [355], which are similar
to the previous report about the vacuum-treated titanium dioxide
[356]. Consequently, the controlled defect concentration in g-C3 N4
is crucial for achieving the ideal photoactivity.
4.3. Pore texture tailoring
Another attractive design strategy is to tailor the porous structures/texture of g-C3 N4 materials, which can signicantly increase
their exposed surface area and accessible channels(porosity) and
active sites in g-C3 N4 , thus facilitating the molecular mass transfer/transport, charge migration and separation, surface reactions
and light harvesting [83]. All these advantageous features can
benet the enhancement of photocatalytic efciency. So far, a
variety of highly porous g-C3 N4 with diverse nanoarchitectures
and morphology have been widely fabricated through several
typical pathways, such as hard templating (nanocasting), soft
templating (self-assembly along the structure directing agents),
self-templating (supramolecular self-assembly) and template-free
methods [27,48,54,357], which have been thoroughly summarized
in Table 4. The detailed comparison and discussion between them
will be highlighted in this section.
As observed in Table 4, it is clear that the hard templating
(nanocasting) strategy is deemed to be one of the most simple and
effective methods to construct mesoporous g-C3 N4 photocatalysts
with superior high surface area (up to 517623 m2 /g) [69,229,360].
In theory, various kinds of macro/mesoporous materials with super
high surface area can be employed as hard templates to construct porous g-C3 N4 . To date, various kinds of hard templates
such as porous anodic Al2 O3 [358,359], CaCO3 [370], graphene
oxide nanosheets, [151] CMK-3 mesoporous carbon [69], mesoporous silica (nanospheres, [123,361,363] foams, [229] SBA-15,
[122,170,362] chiral silica, [365,366] silica KIT-6, [368] and KCC1 [369]) have been available in developing highly porous g-C3 N4 .
Absolutely, the mesoporous silica materials have been demon-
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Table 4
Summarization of different fabrication methods for mesoporous g-C3 N4 .
Morphology
Templates
Precursor
EDA, CTC
CA
CA
CA
CA
EDA, CTC
CA
SBA-15
12-nm SiO2 particles
Monodisperse silica@ mesoporous
silica
Chiral mesoporous silica
Chiral silica
nanorods
7 nm colloidal silica particles
ATC
ATC
CA
2.78
CA
CA
2.75
2.7
MA
CA
CA
CA
DCDA
DCDA
Urea
Ionic liquids(BmimBF4 )
BmimBF4
BMIM-PF6
BmimDCN
Pluronic P123
DCDA
Urea
DCDA
DCDA
MA
Pluronic P123
Triton X-100
Triton X-100
Triton X-100
Bubble (urea)
Bubble (thiourea)
Bubble (water vapor)
Ammonium alginate or gelatin
Bubble (sublimed sulfur)
Bubble (sucrose)
Bubble (water)
Diatomite
DCDA
DCDA
MA, GA
MA sulfate
DCDA
DCDA
Urea
DCDA
MA
MA
urea
CA
Ordered mesoporous
Hierarchical mesostructures
Inverse opal
structures
Mesoporous
nanorods
Ordered mesoporous
Mesoporous
Hollow nanospheres
Helical rodlike
Porous nanorod
Mesoporous
sphere
Porous composite
g-C3 N4 @CMK-3 composite
Cubic mesoporous
Nanosheet-based nanospheres
Porous
Porous
Macroscopic 3D Porous monolith
Soft templating methods
Sponge-like mesopore
Porous nanosheets
Nanoporous
Worm-like
porous
Nanoporous
Nanoporous
Bimodal mesoporous
Nanoporous
Nanoporous
Porous
Sponge-like
Mesopore
Mesopore
Honeycomb-like
Diatom-structure
Template-free methods
Nanobelts
Porous
Porous
Hierarchical structure
Nanoporous
Nanosheets
Seaweed-like architecture
Monolayer mesoporous
Porous microspheres
Nanosheets
Nanorod-network superstructures
MA
MA hydrochloride
DCDA
MA
MA
urea
DCDA
DCDA
CAC/MA
Urea, Ph4 BNa
CAC/MA
BJH pore
size (nm)
Pore
volume
(cm3 g1 )
5.3
0.34
8.3
3.4
4/43
20
70
3.9
0.41
0.49
0.9
0.79
1.7
5.3
0.34
0.77
2.7
2.86
[365] (2014)
[366] (2014)
224
[367] (2012)
0.08
0.76
26.6
623
208
160
38.6
46
78
[151] (2011)
[69] (2011)
[368] (2010)
[369] (2014)
[370] (2015)
[371] (2015)
[372] (2015)
25.0 23.4
0.32
0.40 0.51
444
73
5.6
0.179
81
90
0.128
0.284
299
116
17.6
3.0
3.6
3.8
0.09
0.49
0.4
0.4
2.472.57
3.7
18.2
0.321
2.49
50
13.2
2.65
0.355
0.68
3040
0.4
0.3
12.84
0.31
2.79
2.7
2.75
2.42
2.83
1.92
[360] (2013)
[229] (2010)
[361]
(2011)
[362] (2012)
56
52
3.8
3.8/1040
2.83
2.72
2.74
2.75
2.78
[358] (2009)
[359] (2011)
[122] (2009)
[123] (2009)
3.8/10.7
1.55
2.73
2.25
25
239
373
126
517
550
230
140
110200
Ref. (year)
[170] (2011)
[363] (2012)
[364] (2012)
2.89
2.72
BET surface
area
[m2 g1 ]
239
176
79
2.9
Urea
CAA/MA
MA/CAA
MA/CAA
CAA/MA
MA, urea, CAA
CA, MA, DPT
CAA, MA, BA
MA, TAP
CAA/MA
2.9
2.74
2.7
CA
Band gap
[eV]
15.8
0.50
0.15
1.41
<20
<20
16.2
0.62
90
[114] (2010)
[373] (2014)
[312] (2010)
[374] (2010)
[375] (2012)
50135
60
46.4
69.6
63
46
121
106
5
[374] (2010)
[374] (2010)
[376] (2011)
[377] (2014)
[378] (2014)
[379] (2013)
[380] (2012)
[279] (2013)
[381] (2015)
[382] (2015)
[383] (2015)
[384] (2013)
45
77
66
41
97.4
75 5
6070
119
77
[110] (2013)
[107] (2013)
[385] (2013)
[386] (2015)
[387] (2014)
[111] (2014)
[388] (2014)
[108] (2014)
[389] (2014)
69
201
35.6
30.9
288
130
331
8.5
144
30
[390] (2011)
[391] (2012)
[392] (2013)
[393] (2014)
[394] (2015)
[153] (2013)
[395] (2015)
[396] (2016)
[397] (2015)
[328] (2013)
[398] (2012)
BmimBF4 : 1-butyl-3methylimidazolium tetrauoroborate; BMIM-PF6: 1-butyl3-methylimidazolium hexauorophosphate; BmimDCN Ph4 BNa: sodium tetraphenylboron;
CA: cyanamide; MA: melamine; DCDA: Dicyandiamide; CAA: cyanuric acid; CAC: Cyanuric chloride; DPT: 2,4-diamino-6-phenyl-1,3,5-triazine; BA: barbituric acid; ATC:
ammonium thiocyanate; EDA: ethylenediamine; CTC: carbon tetrachloride; GA: glutaraldehyde, TAP: 2,4,6-triaminopyrimidine.
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semiconductors with high surface area and unique nanostructures in a low-temperature solution in future research [54]. In
addition, it is also expected that the two strategies of in situ
template-sacricial dissolution [401] and chemically induced selftransformation [217,402408] could be applied in developing
highly porous g-C3 N4 -based semiconductors.
4.4. Dimensionality tuning
Generally, compared with the bulk counterparts, nanostructured g-C3 N4 semiconductors with unique dimensions and
congurations could exhibit several obvious advantages for solar
photocatalysis, such as the higher surface area, shorter charge
migration length, higher solubility and tunable electronic structure [37]. Detailedly speaking, the charge carriers generated in
the ultrathin g-C3 N4 nanosheets can readily reach their surface
for redox reactions through the very short paths, as compared
to traditional 3D bulk g-C3 N4 semiconductors, thus achieving
the rapid charge separation. More importantly, through controlling the layer number without changing the atomic structure,
the energy band structure of g-C3 N4 could be effectively tailored due to the quantum connement effects, thus leading to
improved activity and selectivity for various reactions, such as CO2
reduction [409] and O2 reduction [410]. In addition, the nanostructured g-C3 N4 with different dimensions also exhibited signicantly
enhanced opened-up surface areas and highly exposed active
sites, thereby greatly facilitating the photocatalytic enhancements.
All these advanced features endow the nanostructured g-C3 N4
with attractive structure-dependent, morphology-dependent and
thickness-dependent applications ranging from photocatalysis to
other emerging elds. Thus, as a simple way, tuning physical
dimensions of g-C3 N4 has become a popular strategy to manipulate the optical, electrical, and redox properties, thus achieving the
desired catalytic activity, selectivity, and long-term stability. So far,
nanostructured g-C3 N4 with various different dimensionality, such
as 0D quantum dots [411414], 1D nanowires/nanorods/nanotubes
[138,277,359,395,400], 2D nanosheets [100,415,416], 3D hierarchical structures [393,417419] have been widely exploited and
applied in the photocatalysis [55]. Among them, the 2D ultrathin
g-C3 N4 nanosheets have proven to be more promising for various
photocatalytic applications [27,52,56], whose fabrication strategies
will be highlighted in this section.
Generally, the free-standing ultrathin g-C3 N4 nanosheets could
be obtained via two distinct synthetic strategies, including the
top-down exfoliation of layered bulk g-C3 N4 materials and bottomup assembly of precursors (molecular building blocks) in a 2D
manner [52,56]. Typically, these two fabrication strategies can
be further classied into ve detailed categories: ultrasonicationassisted liquid exfoliation, chemical exfoliation, thermal oxidation
etching, combined and other approaches. In order to facilitate
further comparison, various different fabrication methods for gC3 N4 nanosheets have been thoroughly summarized in Table 5. As
observed in Table 5, it is clear that the 2D single-layer and few-layer
g-C3 N4 nanosheets could exhibit much higher surface areas in the
range from 50 to 384 m2 g1 , which are several times larger than
that of bulk layered g-C3 N4 (10 m2 g1 ), thus signicantly favoring
the photocatalytic enhancement.
Inspired by the formation of graphene/metal dichalcogenide/double hydroxide nanosheets by liquid exfoliation of
layered bulk counterparts [463469], it is highly expected that the
mono- or few-layer C3 N4 nanosheets could be obtained through
a simple liquid exfoliation of bulk layered g-C3 N4 by sonication.
Clearly, the well matched surface energy between a liquid solvent
and g-C3 N4 (115 mJ m2 ) could effectively reduce their enthalpy of
mixing, thus leading to the enhanced exfoliation efciency of bulk
g-C3 N4 into 2D nanosheets [426,465]. Thus, the ultrasonication
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Table 5
Summarization of different fabrication methods for g-C3 N4 nanosheets.
Bulk g-C3 N4
Water, 100/200, 16 h
MA (P, 600 C)
MA (P, 550 C)
Water, 50/50, 2 h
Water/organic solvents, 500/150, 10 h
MA (P, 550 C)
Isopropanol, 30/10, 10 h
Commercial g-C3 N4
(Carbodeon Ltd)
CA (P, 550 C)
Ethanol, 50/50, 2 h
1,3-butanediol, 60/25, 24 h
DCDA (P, 600 C)
MA (P, 550 C)
30 wt% isopropanol + water, 4/1, 10 h
Water, 100/200, 16 h
MA (P, 600 C)
DMF, 50/200, 2h(80 C)+ melamine
DCDA (P, 520 C)
Ethanolamine/1,3-butanediol/3Commercial g-C3 N4
(Carbodeon Ltd)
pyridinemethanol,30/10,4h
Chemical exfoliation
MA (P, 550 C)
MA + LiCl(P, 380 + 550 C)
DCDA (P, 550 C)
MA (P, 550 C)
DCDA (P, 550 C)
DCDA (P, 550 C)
MA (P, 550 C)
MA (P, 550 C)
MA (P, 520 C)
MA (P, 600 C)
Thermal oxidation etching
DCDA (P, 550 C)
DCDA(P, 550 C)
Urea (P, 550 C)
MA (P, 550 C)
MA (P, 550 C)
MA (P, 520 + 540 C)
MA (P, 500 + 520 C)
MA (P, 500 + 550 C)
MA (P, 600 C)
DCDA (P, 520 C)
Commercial g-C3 N4
(Carbodeon Ltd)
DCDA(P, 550 C)
Mixed DCDA/NH4 Cl
Mixed DCDA/NH4 Cl
Mixed MA/KCl
Mixed MA/KBH4
Guanidinium cyanurate
Guanidinium chloride
DCDA (P, 600 C)
Combined approaches
MA (P, 520 C)
MA (P, 500 + 530 C)
MA (P, 500 + 530 C)
MA (P, 520 C)
MA (P, 550 C)
MA (P, 520 C)
DCDA (P, 550 C)
DCDA/2-aminobenzonitrile (P,
550 C)
Urea (P, 600 C)
0.15/
0.2/
2.70/
/14.5
/14.5
/8.6
2.5/7
12/36
1.8/56
1.2/4
1.0/3
2.6/
3/
1.2/<5
0.38/1
2/ < 9
2.79/59.4
2.65/384
0.35/
23/58
0.92.1/36
2/6
2.73/112.5
2.79/32.54
2.70/
23/69
7
2.75/116.76
/8.6
1/
[100] (2013)
[103] (2014)
[410] (2013)
[299,420](2013)
[421] (2013)
[422] (2013)
[423] (2014)
[424] (2015)
[416] (2013)
[425] (2014)
[426] (2014)
[427] (2014)
[422] (2013)
[428] (2015)
[429] (2015)
/85%
2.5/8
23/69
2.78/22.5
2.82/186
[430] (2014)
[431] (2016)
/30%
0.4/1
2.92/205.8
[178] (2013)
/70%
300/
/2530%
2.5
/1
24/610
2.93/86.29
3.28/
2.75/305
/109.3
/65
[432] (2015)
[180] (2015)
[82] (2014)
[433] (2014)
[164] (2013)
/2530%
9.0/30
3.42/
2.7/179.5
[82] (2014)
[434] (2015)
Air, 500 C, 2 h
Air, 500 C, 2 h
Air, 550 C, 2 h
Air, 500 C, 2 h
Air, 500 C, 2 h
Air, 540 C, 2 h
Air, 520 C, 4 h
Air, 500 C, 2 h
Air, 500 C, 4 h
Air, 400 C, 4 h
H2 , 400 C, 4 h
/<6%
/<6%
/8.0
1.622.62/47
1.622.62/47
16/
2.97/306
2.97306
2.86/151
3.06/165.66
2.91/122.6
2.93/210
2.82/153.32
2.97/150.1
[415] (2012)
[409] (2014)
[435] (2015)
[436] (2014)
[326] (2015)
[437] (2015)
[438] (2016)
[439] (2014)
[440] (2015)
[441] (2013)
[442] (2015)
58/1020
/0.35%
2.7/8
1.9/6
0.9/3
2/6
NH3 , 510 C, 1 h
Air, 550 C, 2 h
Air, 550 C, 4 h
Air, 550 C, 4 h
Air, 550 C, 4 h
Air, 550 C, 4 h
Air, 600 C, 4 h
Air, 350 C, 2 h (NH4 Cl intercalation, N2 )
20/50
3.1/8
1.0/3
1.56.3
1.5/4
0.61.5/13
0.5/1
0.40.5/1
0.81.2/23
0.5/1
MA (P, 550 C)
Other approaches
MA (P, 550 C)
MA and carbon bre
MA (P, 550 C)
23/69
0.6/1
510/1520
0.64/210
2.89/
/260
2.95/196
2.83/52.9
2.77/77.7
2.71/
2.87/133.8
2.44/109.9
2.85/30.1
3.03/
3.0/380
2.95/109.30
3.0/140
2.89/
/10.5
[350] (2015)
[443] (2014)
[444] (2015)
[445] (2014)
[446] (2014)
[447] (2015)
[448] (2014)
[449] (2014)
[450] (2014)
[451] (2014)
[452] (2015)
[453] (2014)
[454] (2014)
[455] (2015)
[456] (2015)
[457] (2016)
[458] (2016)
2.5/7
2.88/80
[459] (2015)
0.81.4/34
2.79/54.3
[460] (2016)
/12
1.6/5
2.98/
2.88/239
[461] (2015)
[462] (2016)
Please cite this article in press as: J. Wen, et al., A review on g-C3 N4 -based photocatalysts, Appl. Surf. Sci. (2016),
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Fig. 31. (a) Schematic illustration for the synthesis process of ultrathin g-C3 N4 nanosheets via liquid exfoliation. (b) AFM image of the synthetic g-C3 N4 nanosheets. (d) The
corresponding height image of two random nanosheets [100].
Fig. 32. Schematic illustration for fabricting the ultrathin nanosheets of g-C3 N4
through a dicyandiamide-blowing method [443].
In general, there are ve typical strategies to increase the visiblelight absorbance of wide band gap semiconductors: band-gap
engineering (impurity doping and solid solution), defect control, surface plasmon resonance (SPR) effect, sensitization by dye
and quantum dot [16]. Although the aforementioned two strategies of band-gap engineering and defect control can partially
extend their visible-light absorption, the moderate band gaps
(2.7 eV) of g-C3 N4 -based semiconductors are still the main bottlenecks affecting the highly effective generation of photo-generated
charge carriers, which thereby play the crucial roles in determining the visible-light photocatalytic performances of g-C3 N4 -based
semiconductors. Thus, other three strategies, including loading
plasmonic metals, sensitization by quantum dots (QDs) and organic
dyes (the corresponding mechanisms shown in Fig. 33), have been
also widely applied in enhancing the visible-light absorbance of gC3 N4 -based semiconductors, which will be thoroughly discussed
in this section.
Firstly, the famous SPR effects of noble metals, such as
Au [77,200,479482] and Ag [433,455,479,483492], have been
widely employed to improve the visible-light absorbance and
charge separation of g-C3 N4 . In general, it is well accepted that
the deposited plasmonic metals could function as electron sink,
reduction co-catalyst and photosensitizers to enhance the visiblelight absorption of a given semiconductor [493]. For example, Bai
et al. fabricated the coreshell nanostructured Ag@C3 N4 photocatalysts through the simple methanol-reux treatment of g-C3 N4
nanosheets deposited by Ag nanoparticles (as shown in Fig. 34)
[488]. The combination of LSPR effect of Ag nanoparticles and their
hybrid effect with C3 N4 could achieve 1.8- and 30-time enhancements in the photocatalytic MB degradation and H2 evolution,
respectively. In another example, Wei et al. constructed the type-II
2D-1D C3 N4 /TiO2 hybrid nanobers and further decorated plasmonic noble metal nanoparticles (Au, Ag, or Pt) with sizes from 5
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Fig. 33. Mechanisms for g-C3 N4 photocatalysts sensitized by (a) plasmonic metals, (b) quantum dots (QDs), (c) organic dyes.
Fig. 34. Synthetic route and charge-separation mechanism for C3 N4 and coreshell
nanostructured Ag@C3 N4 photocatalysts under light irradiation [488].
to 10 nm on them [479]. The resulting SPR sensitized heterostructures could achieve highly efcient photocatalytic H2 evolution
due to the simultaneous implementation of improved light absorption, charge separation and utilization. In future, it is expected that
the plasmonic alloys [494,495], Cu [496498] and Bi [499501]
nanoparticles could be deposited onto g-C3 N4 to boost their visiblelight photocatalytic activity.
Secondly, the quantum dots modied g-C3 N4 photocatalytic
systems are still very interesting and promising [502505]. For
example, Ge et al. rst demonstrated that the deposition of 30 wt%
CdS QDs onto the bulk g-C3 N4 could achieve a 9-fold enhancement
in the visible-light photocatalytic H2 -evolution activity, due to the
increased the absorbance of visible light and promoted charge separation [502]. Since then, CdS QDs have been widely used to improve
the visible-light activity of bulk g-C3 N4 for various kinds of applications [284,405,502,503,506508]. In future, it is expected that
more efcient CdS/g-C3 N4 composite photocatalysts with earthabundant co-catalysts should be further exploited.
Thirdly, various kinds of low-cost organic dyes, such as magnesium phthalocyanine (MgPc) [509], zinc phthalocyanine [510515],
Xanthene [516], Erythrosin B (ErB) [473,517] and Eosin Y (EY) [518],
have been readily coupled with different nanostructured g-C3 N4
to fabricate the highly efcient organic semiconductor heterojunctions. For example, Domen and his coworkers deposited an organic
MgPc dye (with a band gap of 1.8 eV) on the Pt/mpg-C3 N4 composite semiconductors and achieve the enhanced photocatalytic
H2 evolution under long-wavelength irradiation (>600 nm) [509].
The results indicated that the monolayer dye could achieve the
highest photocatalytic H2 -evolution performance due to promoted
charge generation, transfer and utilization, whereas excess thickness of the dye layer will cover the co-catalyst sites, thus reducing
the photocatalytic activity [509]. Similarly, Lu and coworkers
successfully demonstrated that the sensitization of mesoporous
g-C3 N4 with a EY dye could achieve an H2 -evolution AQE of
19.4% under 550 nm irradiation [519]. It is suggested that the
high surface area and nanoporous structure of mpg-C3 N4 are
greatly favorable for deposition of EY molecules on its surface,
thus promoting the signicantly increased and extended light
harvesting in the visible-light response region and further improving H2 -evolution activity. More surprisingly, Xu and coworkers
demonstrated that the deposition of ErB dye onto Pt/g-C3 N4 sample exhibited a remarkably enhanced H2 evolution rate (652.5 or
162.5 mol h1 ) from an aqueous solution of TEOA under visible
light irradiation ( > 420 nm or > 550 nm), with an AQY of 33.4%
at 460 nm [473]. The resulting ternary Pt/g-C3 N4 /ErB photocatalyst also showed the stability and good recyclability, remaining
90% of the activity after 5 runs [473]. Most recently, it has been
demonstrated that the promising earth-abundant Co(OH)2 and
MoS2 could be utilized as co-catalysts to boost the photocatlytic H2 evolution activity over these dye-sensitized g-C3 N4 photocatalysts
[517,520,521]. More interestingly, the g-C3 N4 -based photocatalytic
systems co-sensitized by two organic dyes or inorganic photosensitizers (plasmonic metals and QDs) are also highly desirable in
future studies [510,512,521,522]. However, the apparent quantum
effciency and stabilities of these systems are still needed to be further enhanced.
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Fig. 35. Spatial charge-separation mechanisms for four different types of semiconductor heterojunctions: (A) Schottky junction, (B) Type I, (C) Type II, and (D) Type III
heterojunctions.
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Fig. 36. Schematic illustration of spatial charge separation in CdS/g-C3 N4 (a) and g-C3 N4 /S-g-C3 N4 (b).
Fig. 37. Schematic illustration of spatial charge separation in the all-solid-state g-C3 N4 -based Z-scheme photocatalytic systems with (a) and without (b) mediators.
Fig. 38. Schematic illustration for the charge transfer and separation in g-C3 N4 -TiO2 Z-scheme photocatalysts under UV light irradiation [523].
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In addition, it should be also noted that the interfacial contact/coupling performances could be further improved by several
strategies, such as, increasing the contact areas, improving the
tightness of interfaces [621624] and introducing the highlyconductive interfacial mediator [625627]. Clearly, larger contact
area can provide sufcient charge transfer and trapping channels for achieving their fast separation. As compared with other
types of composite pohotocatalysts with 1D (i.e. 0D/1D and
1D/1D) or 2D (i.e. 0D/2D and 1D/2D) contact interfaces, the
unique 2D2D layered nano-junctions possess the much larger
contact surface between the two adjacent sheets (as shown in
Fig. 39), thus favoring more efcient interfacial charge separation and photo-activity enhancement [476]. More fortunately,
g-C3 N4 itself possesses a unique 2D layered structure, which holds
great promise for potential applications in constructing 2D layered
composite photocatalysts. In 2011, Xiang et al. rst constructed
graphene/g-C3 N4 composite photocatalysts with the larger 2D-2D
coupling interfaces (as shown in Fig. 40a) [151], demonstrating a
more than 3.07-time enhancement of photocatalytic H2 -evolution
activity (using Pt and methanol as cocatalyst and sacricial
agent, respectively). Subsequently, a series of 2D g-C3 N4 -based
layered heterojunctions (e.g. MoS2 [120,290,292,628633], SnS2
[634636], WS2 [637,638], graphene [482,639], SnNb2 O6 [640],
WO3 [287], BiOBr [641], layered double hydroxide [288,642,643],
Bi4 O5 I2 [644] and Bi2 O2 CO3 [645]) have been widely fabricated for
different photocatalytic applications. Among them, g-C3 N4 /MoS2
2D-2D coupling systems have attracted much attention since the
rst report about concept of layered nanojunctions by Hou et al. in
2003 (as shown in Fig. 40b) [120]. It is believed that 2D layered MoS2
can function as co-catalysts [646], stable semiconductor sensitizers
[647] or electron trapper [648,649] in these systems. More inter-
of CO2 /CO(0.51 V), H + /H2 (0.41 V), and O2 /O2 (0.33 V),
respectively (As shown in Fig. 41). Thermodynamically, the photogenerated electrons on the CB of g-C3 N4 have much stronger
driving force (or over-potentials) for these three typical kinds of
reduction reactions, as compared to those in TiO2 [28,657,658].
However, the obvious structure defects in bulk g-C3 N4 generally
lead to their fast recombination with the photo-excited holes.
More importantly, the photocatalytic H2 evolution and CO2 reduction are typical up-hill reactions, thus resulting in the sluggish
kinetics on the surface of bulk g-C3 N4 . Fortunately, these disadvantageous factors could be simultaneously overcome by loading
suitable reduction co-catalysts onto the surface of g-C3 N4 , which
could lower the reaction activation energy (or electrochemical
overpotentials), improve the charge separation and transport,
increase stability of photocatalyts, and accelerate the sluggish reaction kinetics of various surface reduction reactions, thus greatly
enhancing the photocatlytic activity [88,124]. Essentially speaking, the single-electron or multi-electron O2 -reduction reactions
(as shown in Table 2) are of signicant importance for photocatalytic degradation [83,410,657], selective organic transformations
[119,244] and disinfection [659,660]. More interestingly, the cocatalysts can also achieve the selective photoreduction products
of CO2 [16,661]. In addition, it is also necessary to deposit suitable hole co-catalysts to accelerate the difcult water oxidation
reactions, due to the lower overpotential of g-C3 N4 for water oxidation (0.59 V), as well as the inherent challenges of four-electron
water oxidation [7,662]. Thus, it is obvious that all these reduction and oxidation co-catalysts play decisive roles in achieving
highly efcient and selective photocatalytic reactions. These four
Fig. 40. Schematic illustration of 2D-2D coupling of g-C3 N4 /graphene (a) and g-C3 N4 /MoS2 (b).
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Noble-metal co-catalysts
H2 evolution
Hole co-catalysts
CO2 reduction
O2 reduction (degradation)
Pt, Au [590], Ag
[433,483,485,488,506,710723],
Ag2 O [724728], Pd [729732],
bimetallic Au/Pt [481], Ag
Quantum Cluster[733]
Graphene/LDH [288]
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Fig. 42. Roles of carbon materials in enhancing the performance of g-C3 N4 -based
composite photocatalysts [781].
Fig. 43. The proposed mechanism for photocatalytic water splitting over the gC3 N4 (electron sink and H2 -evolution site)/RGO-3 composite [773].
in the RGO (Fig. 43) [773]. The ndings pave the way for developing RGO-based composites for photocatalytic applications. At this
point, the semiconductor properties of RGO are more promising
in constructing composite photocatalysts [740], which deserves
more attention in future studies. In addition, doping or co-doping
of RGO materials with heteroatoms has also been demonstrated
to exhibit the signicantly enhanced electrocatalytic performances
[791], which are also highly expected to be utilized in constructing
g-C3 N4 /doped RGO composite photocatalysts.
5. Potential applications of g-C3 N4 -based composite
photocatalysts
5.1. Photocatalytic water splitting
Since the pioneering works by Honda and Fujishima in 1972 [1],
various heterogeneous photocatalysts have been widely applied
in the attracted photocatalytic hydrogen production from water
reduction [7]. Normally, photocatalytic water splitting systems
can be divided into half-reaction water splitting (for H2 and O2 )
and overall water splitting systems [7]. Interestingly, g-C3 N4 has
been extensively applied in these two systems to boost their photocatalytic activity for water splitting. Table 7 summarizes the
photocatalytic activities of g-C3 N4 based photocatalysts for H2
generation on various conditions, including the amount of photocatalysts, the sacricial reagents, H2 generation rate, and the
corresponding quantum efciency in this review. As shown in
Table 7, co-catalysts and sacricial reagents are crucial for achieving the highly efcient photocatalytic H2 evolution, which will be
discussed in detail.
As observed in Table 7, it is clear that the high H2 -evolution
activity over nanostructured g-C3 N4 -based semiconductors is generally obtained via loading the shape-dependent noble-metal Pt
nanoparticles as co-catalysts [315,321,348,445,562,809,819,823].
In the pioneering work, Wang and co-workers found that the
loading 3 wt% Pt as co-catalysts on g-C3 N4 could achieve the H2 evolvtion amount of 770 mol after 72 h in the TEOA aqueous
solution, whereas the bare g-C3 N4 exhibits the negligible H2 production activity. This is due to the rapid recombination of CB
electrons and VB holes, and the large H2 -evolution overpoten-
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http://dx.doi.org/10.1016/j.apsusc.2016.07.030
structure
synthetic method
co-catal./mass ratio
mass (g)
light source
incident light
aqueous
reaction
cocatal./activity
(mol h1 )
Ni@/g-C3 N4
NiS/g-C3 N4
particles/lamellar
nanoparticles/lamellar
solvothermal method
hydrothermal method
Ni/10 wt.%
NiS/1.25 wt.%
0.05
0.1
quartz reactor
Pyrex reactor
10 vol.% TEOA
15 vol.% TEOA
Ni/8.41
NiS/46
NiS/g-C3 N4
nanoparticles/lamellar
NiS/1.5 mol%
0.1
10 vol.% TEOA
NiS/44.77
[670] (2014)
NiS/e-C3 N4
ultrathin
nanosheets/nanoparticles
NiS/1.0 wt.%
0.05
quartz reactor
10 vol.% TEOA
NiS/4.2
[671] (2015)
Ni(OH)2 /gC3 N4
Ni/NiO/g-C3 N4
nanoparticles/lamellar
liquid
exfoliation-hydrothermal
method
precipitation method
500 W Xe lamp
300 W Xe lamp,
> 420 nm
300 W Xe lamp,
> 420 nm
150 W Xe lamp,
> 400 nm
0.05
Pyrex reactor
10 vol.% TEOA
Ni(OH)2 /7.6
core-shell/lamellar
Ni/NiO/2 wt.%
0.05
Pyrex reactor
10 vol.% TEOA
Ni/NiO/10
[792] (2015)
NiS/CNT/mpgC3 N4
NiS/CB/g-C3 N4
nanoparticles/nanotubes/lamellar
sol-gel-precipitation method
NiS/1 wt.%
0.05
quartz reactor
10 vol.% TEOA
NiS/26.05
[198] (2015)
nanoparticles/lamellar
quartz reactor
15 vol.% TEOA
CB, NiS/49.6
[156] (2015)
sub-mircowires/lamellar
CB/0.5 wt.%,
NiS/1.0 wt.%
Ni(dmgH)2 /3.5 wt.%
0.05
Ni(dmgH)2 /gC3 N4
g-C3 N4
physical mixing-chemical
deposition
chemical deposition
0.005
quartz reactor
15 vol.% TEOA
Ni(dmgH)2 /1.18
[677] (2014)
Pt/3 wt.%
0.05
Pyrex reactor
10 vol.% TEOA
Pt/28.55
[793] (2016)
pm-g-C3 N4
porous
co-polymerization-surface
activation-exfoliation
sintering
Pt/3 wt.%
0.1
10 vol.% TEOA
Pt/41.7
[159] (2017)
g-C3 N4
microsphere
solvothermal method
Pt/3 wt.%
15 vol.% TEOA
Pt/1.80
g-C3 N4
lamellar
Pt/1 wt.%
0.1
Pyrex reactor
10 vol.% TEOA
Pt/34
g-C3 N4
ower-like nanorods
Pt/3 wt.%
0.05
quartz reactor
10 vol.% TEOA
Pt/261.8
Pt/0.6 wt.%
0.1
10 vol.% TEOA
Pt/89.28
[794]
(2015)
[795]
(2015)
[428] (2015)
Pt/3 wt.%
0.05
Pyrex reactor
10 vol.% TEOA
Pt/272
[796] (2015)
0.1
Pyrex reactor
10 vol.% TEOA
Pt/502
10 vol.% TEOA
Pt/39.4
quasi-2D-C3 N4 lamellar
mg-C3 N4
mesoporous
melamine-assisted exfoliation
method
calcinating-dissolving method
CNIC
nanotubes
molten salt
Pt/3 wt.%
CNT/g-C3 N4
nanotubes/lamellar
calcinating method
MVNTs/g-C3 N4 nanotubes/particles
calcinating method
MVNTs/2.0 wt.%
0.1
C/g-C3 N4
ber/lamellar
Pt/1.0 wt.%
0.05
C/g-C3 N4
mixing-calcinating method
0.1
C-dots/g-C3 N4
nanoparticles/rectangular
nanotube
dots/lamellar
electrospinning and
calcinations method
molten salt method
0.05
CQDs/g-C3 N4
quantum dots/lamellar
hydrothermal method
0.05
C-dots/g-C3 N4
hydrothermal method
thermal condensation
C-dots/0.2 wt.%,
Pt/0.2 wt.%
C-ZIF/1 wt.%
0.05
C-ZIF/g-C3 N4
nanodots/ultrathin
nanosheets
nanoparticles/lamellar
0.1
N/g-C3 N4
nanosheet
calcinating method
N-doped,Pt/3 wt.%
0.05
C3 N4+x
lamellar
co-thermal condensation
N-doped,Pt/3 wt.%
0.08
[126] (2013)
[397] (2015)
[106] (2013)
[147] (2014)
quartz reactor
[681] (2012)
Pyrex reactor
10 vol.% TEOA
[682] (2015)
quartz reactor
[779] (2014)
Pyrex reactor
[797] (2015)
Pyrex reactor
10 vol.% TEOA
Pt/5.805
[680] (2016)
5 vol.% CH3 OH
Pt/88.1
0 vol.% TEOA
C-ZIF/32.58
[777]
(2016)
[683] (2016)
10 vol.% TEOA
Pt/64
[798] (2016)
10 vol.% TEOA
Pt/44.28
[799] (2015)
Pyrex reactor
Pt/54
29
4 UV-LEDs (3 W,
= 420 nm)
400 W Xe lamp,
> 420 nm
300 W Xe lamp,
> 420 nm
300 W Xe lamp,
> 400 nm
300 W Xe lamp,
> 420 nm
300 W Xe lamp,
> 400 nm
[192] (2015)
[125] (2013)
ARTICLE IN PRESS
ultrathin nanosheets
reference
(year)
G Model
QY (%)
photocatalyst
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Table 7
Summary of the photocatalytic H2 evolution on g-C3 N4 -based photocatalysts.
structure
synthetic method
co-catal./mass ratio
mass (g)
light source
incident light
aqueous
reaction
cocatal./activity
(mol h1 )
P/g-C3 N4
calcinating method
0.05
10 vol.% TEOA
Pt/104.1
[315] (2015)
copolymerization
P-doped
0.1
Pyrex reactor
10 vol.% TEOA
Pt/50.6
Br/g-C3 N4
lamellar
calcinating method
10 vol.% TEOA
Pt/48
[324]
(2015)
[800] (2016)
g-C3 N4
calcinating method
0.05
Pyrex reactor
10 vol.% TEOA
Pt/60.2
S/g-C3 N4
calcinating method
0.1
quartz reactor
[307] (2013)
K-g-C3 N4
lamellar
KCl-template method
K, Pt/0.5 wt.%
0.01
Pyrex reactor
10 vol.% TEOA
[445] (2014)
Zn/g-C3 N4
lamellar
calcinating method
0.2
Pyrex reactor
Co-Pi/g-C3 N4
in situ photodepositions
0.1
Au/g-C3 N4
nanoparticles/aggregated
sheets
nanoparticles/lamellar
Pt/59.5
18.5 vol.%
CH3 OH
25 vol.% CH3 OH Pt/19.48
0.05 M AgNO3
10 vol.% TEOA Au/177.4
AuPd/g-C3 N4
nanoparticles/lamellar
0.05
Pyrex reactor
P/g-C3 N4
owers of in-plane
mespores
lamellar
0.1
photodeposition method
0.05
impregnaton method
CsTaWO6 /Au/g- gathered
C3 N4
block/nanoparticles/lamellar
Cd0.5 Zn0.5 S/gnanoparticles/lamellar
hydrothermal method
C3 N4
Au/0.33 wt.%,
Pt/0.40 wt.%
Au/0.5 wt.%
0.08
[194] (2015)
Pyrex reactor
Pt-Au/17
[350] (2015)
Pyrex reactor
[200] (2016)
quartz reactor
[667] (2015)
Pyrex reactor
20.8 mL/h
300 W Xe lamp,
> 420 nm
300 W Xe lamp,
> 420 nm
300 W Xe lamp,
> 420 nm
300 W Xe lamp,
> 400 nm
300 W Xe lamp,
> 420 nm
350 W Xe arc lamp,
420 nm
Pyrex reactor
0.35 M Na2 S
and 0.25 M
Na2 SO3
0.1 M Na2 S and
0.1 M Na2 SO3
0.1 M Na2 S and
0.5 M Na2 SO3
0.1 M
L-ascorbic acid
25% vol.%
CH3 OH
10 vol.% TEOA
0.35 M Na2 S
and 0.25 M
Na2 SO3
0.35 M Na2 S
and 0.25 M
Na2 SO3
10 vol.% TEOA
Pt/265.15
[348] (2015)
Pt/207.6
[562] (2013)
NiS/128.2
[197] (2015)
[669]
(2016)
MoS2 /2.52
[632] (2015)
37 (425 nm)
[801] (2015)
299.24
Pt/22.47
8 (420 nm)
[802]
(2015)
[803]
(2016)
[503] (2013)
0.05
particles/lamellar
hydrothermal method
0.05
QDs/lamellar
Pt/0.5 wt.%
0.005
QDs/lamellar
chemical impregnation
method
Pt/1.0 wt.%
0.1
Pt/3 wt.%
0.02
particles/particles
in situ self-transformation
method
Pt/1.0 wt.%
0.05
CdS/g-C3 N4
core/cell nanowires
solvothermal-chemisorption
method
Pt/0.6 wt.%
0.05
Pyrex reactor
nanoparticles/nanorodes/lamellar
in situ hydrothermal method
NiS/CdS/gC3 N4
Ni(OH)2 /CdS/g- core/shell nanorodes
hydrothermal method
C3 N4
NiS/9 wt.%
0.05
quartz reactor
Ni(OH)2 /4.76
0.001
300 W Xe lamp,
420 nm
300 W Xe lamp,
> 420 nm
300 W Xe lamp,
> 400 nm
300 W Xe arc lamp,
> 400 nm
Pyrex reactor
0.25 M Na2 S
and 0.35 M
Na2 SO3
10 vol.% TEOA
quartz reactor
0.01
MoS2 /g-C3 N4
nanoparticles/lamellar
mixing-calcinating method
0.1
[666] (2014)
AuPd/16.3
hydrothermal method
ower-like/lamellar
[690] (2013)
10 vol.% TEOA
nanoparticles/lamellar
MoS2 /g-C3 N4
[300] (2011)
quartz reactor
QDs/hollow
quartz reactor
quartz reactor
quartz reactor
Pyrex reactor
Pyrex reactor
quartz reactor
208.8
Pt/17.27
[502] (2012)
Pt/601
[804] (2015)
[628] (2013)
ARTICLE IN PRESS
Au/PtO/g-C3 N4 nanoparticles/lamellar
0.02
Pt/102.8
[321] (2015)
0.05
Au/1 wt.%
deposition-precipitation
method
chemical reduction-calcinating AuPd/0.5 wt.%
method
photodeposition method
Pt, Au
quartz reactor
reference
(year)
G Model
QY (%)
photocatalyst
30
Please cite this article in press as: J. Wen, et al., A review on g-C3 N4 -based photocatalysts, Appl. Surf. Sci. (2016),
http://dx.doi.org/10.1016/j.apsusc.2016.07.030
Table 7 (Continued)
synthetic method
MoS2 /CN-Py
ower-like/lamellar
ZnS/g-C3 N4
WS2 /g-C3 N4
QY (%)
mass (g)
light source
incident light
aqueous
reaction
cocatal./activity
(mol h1 )
0.05
Pyrex reactor
10 vol.% TEOA
25
[805] (2016)
microsphere/lamellar
precipitation method
0.05
Pyrex reactor
[806] (2014)
slabs/porous sheet-like
gas-solid reaction
0.05
Pyrex reactor
[638] (2015)
0.05
Pyrex reactor
10 vol.% TEOA
WS2 /6.12
[637] (2014)
impregnation-suldation
method
hydrothermal method
Pt/1.0 wt.%
0.05
Pyrex reactor
nanoparticles/lamellar
H2 reduction
Cu
0.05
[807] (2015)
Cu/g-C3 N4
300 W Xe lamp,
> 420 nm
4 UV-LEDs (3 W,
= 420 nm)
300 W Xe lamp,
> 420 nm
300 W Xe lamp,
> 420 nm
4 UV-LEDs (3 W,
= 420 nm)
Xe lamp, > 400 nm
CuO/g-C3 N4
mono-dispersed
wet impregnation-calcination
sphere/lamellar
method
clusters/spherical particles precipitation method
Pt/1.0 wt.%
0.1
Cu(OH)2 /0.34mol%
0.1
nanoparticles/lamellar
Pt/3 wt.%
0.1
CuO2 @g-C3 N4
core@shell octahedra
Pt/3 wt.%
0.3
g-C3 N4 /InVO4
lamellar/nanoparticles
solvothermal and
chemisorption method
hydrothermal method
Pt/0.6 wt.%
0.05
ZnFe2 O4 /gC3 N4
CuFe2 O4 /gC3 N4
FeOX /g-C3 N4
akes/lamellar
calcinating method
Pt/1 wt.%
0.1
nanoparticles/lamellar
calcinating method
Pt/3 wt.%
0.1
granular-like
calcinating method
Ag2 O/g-C3 N4
nanaosheets
hydrothermal method
0.01
Ag2 S/g-C3 N4
particle/mesopores sheets
precipitation method
0.05
TiO2 /g-C3 N4
0.05
g-C3 N4 /B-TiO2
0.1
CoTiO3 /g-C3 N4
C,
NTiO2 /g-C3 N4
N,STiO2 /gC3 N4
nanoparticles/ultrathin
nanosheets
semi-spherical
nanoparticles/lamellar
Pt/3 wt.%
0.02
0.1
0.05
1% wt.%Pt/TiO2
chemical
g-C3 N4 /PtTiO2 nanoparticles/nanoparticles/lamellar
adsorption-calcinating method
lamellar/nanosheets/nanorodes
hydrothermal method
gC3 N4 /MoS2 /TiO2
hydrothermal method
Pt/1 wt.%
C3 N4 /rGO/WO3 nanosheets/nanosheets/nanoparticles
0.1
0.005
solvothermal method
Pt/3 wt.%
0.1
0.02
300 W Xe lamp,
> 420 nm
300 W Xe arc lamp,
> 400 nm
300 W Xe lamp,
> 420 nm
300 W Xe lamp,
> 420 nm
300 W Xe arc lamp,
> 420 nm
300 W Xe arc lamp,
> 430 nm
300 W Xe lamp,
680 nm > > 420 nm
300 W Xe lamp, 780
nm > > 420 nm
300 W Xe lamp,
> 420 nm
300 W Xe lamp,
> 420 nm
4 UV-LEDs (3 W,
= 420 nm)
4 UV-LEDs (3 W,
= 420 nm)
300 W Xe arc lamp,
> 400 nm
300 W Xe lamp
300 W Xe lamp,
> 400 nm
125 W medium
pressure Hg lamp,
400 nm
300 W Xe lamp,
420 nm
300 W Xe arc lamp,
> 400 nm
250 W iron doped
metal halid UVvis
lamp ( > 420 nm)
300 W Xe arc lamp,
> 420 nm
10 vol.% TEOA
Pt/93.7
reference
(year)
[674]
(2016)
[808] (2016)
Pyrex reactor
[809] (2014)
Pyrex reactor
10 vol.% TEOA
Pt/24.13
[525] (2014)
Pyrex reactor
10 vol.% TEOA
Pt/79.5
[802] (2015)
[351] (2015)
Pyrex reactor
10 vol.% TEOA
Pt/20
[439] (2014)
quartz reactor
10 vol.% TEOA
Pt/76
[810] (2016)
quartz reactor
10 vol.% TEOA
FeOX , Pt/108
[811] (2016)
Pyrex reactor
10 vol.% TEOA
Pt/14.62
[812] (2015)
Pyrex reactor
10 vol.% TEOA
33.04
[813] (2015)
Pyrex reactor
20 vol.% CH3 OH 10
[665] (2014)
Pyrex reactor
[814] (2016)
Pyrex reactor
[815] (2016)
quartz reactor
10 vol.%
C2 H5 OH
10 vol.% TEOA
3.92
[817] (2015)
10 vol.% TEOA
317
[818]
(2015)
Pyrex reactor
10 vol.% TEOA
Pt/178
[819] (2012)
Pyrex reactor
Pyrex reactor
deionized
water
Pt/2.84
[820]
(2016)
[821] (2015)
quartz reactor
10 vol.% TEOA
Pt/3.69
[822] (2016)
[816] (2016)
31
Co-Pi: cobalt-phosphate; MVNTS: multi-walled carbon nanotubes; py:pyridine; CNIC: carbon nitride intercalation compound; C-ZIF: ZIF-8 derived.
Pt/11.7
ARTICLE IN PRESS
Cu(OH)2 /gC3 N4
CuO2 /g-C3 N4
co-catal./mass ratio
G Model
structure
Please cite this article in press as: J. Wen, et al., A review on g-C3 N4 -based photocatalysts, Appl. Surf. Sci. (2016),
http://dx.doi.org/10.1016/j.apsusc.2016.07.030
photocatalyst
Table 7 (Continued)
G Model
APSUSC-33598; No. of Pages 52
32
ARTICLE IN PRESS
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Fig. 44. The photocatalytic H2 -evolution rate over g-C3 N4 modied by Pt cocatalysts with different shapes [823].
Please cite this article in press as: J. Wen, et al., A review on g-C3 N4 -based photocatalysts, Appl. Surf. Sci. (2016),
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G Model
APSUSC-33598; No. of Pages 52
ARTICLE IN PRESS
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33
Fig. 45. (a) Comparison of the photocatalytic H2 -production activity of the Nix (x, Ni(OH)2 to (g-C3 N4 + Ni(OH)2 ) was 0, 0.1, 0.5, 1.0, 1.6, and 10 (mol%))and Pt-deposited
g-C3 N4 samples in triethanolamine aqueous solution. (b) Charge separation mechanisms in the Ni(OH)2 /g-C3 N4 system under visible light [126].
Fig. 46. (A) Time courses and (B) the average rate of photocatalytic H2 evolution over the photocatalysts: (a) g-C3 N4 ; (b) g-C3 N4 -CdS; (c) g-C3 N4 -9%NiS; (d) CdS-9%NiS; (e)
g-C3 N4 -CdS-3%NiS; (f) g-C3 N4 -CdS-6%NiS; (g) g-C3 N4 -CdS-9%NiS; (h) g-C3 N4 -CdS-12%NiS; (i) g-C3 N4 -CdS-15%NiS [197].
Fig. 47. (A) The average rate of H2 evolution and (B) proposed charge transfer mechanisms in the g-C3 N4 /CB/NiS composite under visible light irradiation: A g-C3 N4 , B
g-C3 N4 -0.5% CB, C g-C3 N4 -1.5% NiS, D g-C3 N4 -0.5%CB-1.5%NiS, E g-C3 N4 -1.0% CB-1.5% NiS, F g-C3 N4 -1.5% CB-1.5% NiS, G g-C3 N4 -1.5% NiS-0.5% CB [156].
Fig. 48. (a) In situ EPR studies of a suspension of Cat-1 in TEOA solution under continuous visible-light irradiation with increasing the time. (b) Charge separation in sg-CN
and the formation of Ni0 nanoparticles during photocatalysis [676].
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G Model
APSUSC-33598; No. of Pages 52
34
ARTICLE IN PRESS
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H2 and O2 evolution are still the major bottleneck for achieving the
practical H2 evolution or overall water splitting on g-C3 N4 .
5.2. Photocatalytic degradation of pollutants
With rapid growth of population and accelerating industrialization, the environmental contamination has become a major
threat to public health all over the world. Since the rst report
on heterogeneous photocatalytic remediation of environmental
pollutants (CN in water) on titania by Frank and Bard in 1977
[829], the heterogeneous photocatalysis has been widely used
in widespread environmental purication such as air and water
purication [309,830839]. Furthermore, a variety of ways for
increasing the photodecomposition efciency of pollutants over
g-C3 N4 -based semiconductors have been exploited [9,11,20,840],
which have been summarized in Table 8.
As observed in Table 8, constructing the g-C3 N4 -based semiconductor heterojunction and loading suitable O2 -reduction
co-catalysts are the general two strategies to achieve the improved
photocatalytic degradation activity, which will be discussed in this
section. It is clear that the OH radicals in g-C3 N4 -based photocatalysts mainly originated from multi-electron O2 reduction reactions
driven by photo-generated electrons on the CB of g-C3 N4 , because
the photo-generated holes exhibited much negative potentials
(1.4 V) than that of OH/OH (+2.29 V, vs NHE, pH = 7), leading to the
failure in driving the oxidation reaction of adsorbed OH groups to
OH radicals [83,410]. Thus, for improving the photocatalytic activity of g-C3 N4 , more efforts have been devoted to strengthening the
decisive O2 -reduction reactions.
On the one hand, the photocatalytic degradation of gas-phase
pollutants over g-C3 N4 -based photocatalysts has been extensively
investigated, such as NOx [144,883,884], formaldehyde [523],
acetaldehyde [539,885] and so forth. For example, Dong and
coworkers deposited the monodispersed plasmonic Ag nanoparticles onto g-C3 N4 nanosheets to extend visible-light absorption,
increase the generation of O2 and enhance the charge separation, thus achieving the enhanced the photocatalytic activity of
g-C3 N4 nanosheets towards oxidation of NO to nal products [884].
Katsumata et al. demonstrated that WO3 /g-C3 N4 heterojunction
photocatalysts showed a 1.4 times enhancement in photodegradation of acetaldehyde gas, as compared to pristine g-C3 N4 [539]. In
another paper by Yu et al., a direct TiO2 /g-C3 N4 Z-scheme photocatalyst without an electron mediator (as shown in Fig. 38) exhibited
a high photocatalytic performance in the oxidation decomposition
of formaldehyde in air [523]. In these studies, the enhancement
in photoactivity was primarily accredited to the improved transfer
and separation of photogenerated charge carriers and promoted O2
reduction. A mechanically mixed g-C3 N4 and TiO2 sample with similar content did not remarkably improve the conversion of NOx , thus
conrming that the interaction between g-C3 N4 and P25 is vital
for the enhanced activity. EPR measurements once again indicated
that O2 was the main active species involved in the oxidation
of NO under both visible and UV light irradiation [886]. In addition, it should be noted that the adsorption of gas-phase pollutants
on the g-C3 N4 should be carefully optimized to achieve the ideal
photocatalytic degradation efciency.
On the other hand, the g-C3 N4 -based photocatalysts have
been widely used in the photocatalytic degradation of liquidphase pollutants, such as MB [319,506,734,843,887893],
MO
[314,330,576,580,617,688,894898],
RhB
[324,330,742,857,858,872,899906] and so forth. As observed
in Table 8, in pure g-C3 N4 -based visible-light systems, the two
main reactive species, O2 and h+ species, are generally involved
in the degradation of pollutants. Interestingly, besides the aforementioned two species, the presence of OH radicals in Ag/g-C3 N4
systems further provides the direct evidence for its increased
Please cite this article in press as: J. Wen, et al., A review on g-C3 N4 -based photocatalysts, Appl. Surf. Sci. (2016),
http://dx.doi.org/10.1016/j.apsusc.2016.07.030
Degradation
time/
efciency
calcinating method
0.1
40 min/99%
solvothermal method
0.08
RhB/0.01 g L1 /80 mL
60 min/100%
hydrothermal method
0.05
MO/0.01 g L1 /100 mL
SiO2 /g-C3 N4
core-shell nanosphere
calcinating method
0.07
g-C3 N4 /TiO2
lamellar/particles
sol-gel method
0.1
TiO2 /g-C3 N4
core-cell
self-assembly method
0.05
TiO2 /g-C3 N4
mesoporous
melt-inltrating-calcinating
spheres/lamellar
method
yolk-shell spheres/lamellar solvothermal method
Synthetic method
In2 O3 /g-C3 N4
particles/lamellar
TiO2 /g-C3 N4
g-C3 N4 /TiO2
lamellar/nanoparticles
g-C3 N4 /TiO2
g-C3 N4 /TiO2
g-C3 N4 /F-TiO2 lamellar
Co-catal./optimized
mass ratio
0.05
0.01
calcinating method
0.1
0.04
hydrothermal-calcination
method
hydrothermal method
gC3 N4 /Ag/TiO2
K-Na/g-C3 N4
lamellarparticles/microspheres
lamellar
photodeposition-Physical
mixing method
calcinating method
mg-C3 N4
mesopores
calcinating-dissolving method
0.03
0.1
Ag/2 wt.%
0.03
K-Na co-doped
0.05
0.05
g-C3 N4
lamellar
thermal condensation
0.02
mg-C3 N4
mesoporous
0.05
C60 /mg-C3 N4
particles/lamellar
calcinating method
0.025
CDs/g-C3 N4
dots/lamellar
mixing-calcinating method
0.05
C-dots/g-C3 N4 dots/lamellar
mixing-calcinating method
C-dots/0.25 wt.%
0.1
Pd/mpg-C3 N4
particles/mesoporous
chemical reduction
Pd-doped/1.5 wt.%
Pt/C3 N4
nanoparticles/nanotubes
hydrothermal method
Pt/2 wt.%
0.1
Au/Pt/g-C3 N4
particles/lamellar
photodeposition method
0.1
Au/g-C3 N4 /Fe2 O3
particles/lamellar/
rhombohedral-like
hydrothermal and
ultrasonication method
Au
0.05
300 W halogen
tungsten lamp,
> 400 nm
350 W xenon arc lamp,
> 420 nm
500 W tungsten lamp,
> 400 nm
300 W xenon lamp,
400 nm
500 W xenon lamp,
> 420 nm
500 W xenon lamp,
UVvis light
500 W xenon lamp,
> 400 nm
350 W xenon arc lamp,
> 420 nm
2 150 W tungsten
lamp, > 420 nm
400 W halide lamp,
> 400 nm
300 W xenon lamp,
> 420 nm
50 W LED light,
= 410 nm
300 W xenon lamp,
> 420 nm
250 W high-pressure
sodium lamp,
420 < < 800 nm
300 W xenon lamp,
> 420 nm
300 W xenon lamp,
> 420 nm
300 W xenon lamp,
> 400 nm
500 W xenon lamp,
> 420 nm
300 W xenon lamp,
> 420 nm
3 W LED lamp,
= 365 5 nm
350 W xenon lamp,
> 420 nm
300 W xenon lamp,
> 420 nm
500 W xenon lamp,
> 400 nm
halogen lamp
Kapp
[102 min1 ]
Main active
species
Ref. (year)
O2 , OH
[841] (2014)
OH
[797] (2015)
120 min/90%
O2 , h+
[807] (2015)
RhB/0.01 g L1 /70 mL
150 min/94.3%
OH, h+
[842] (2015)
MB/0.01 g L1 /100 mL
360 min/92%
h+
RhB/10 ppm/200 mL
80 min/82%
RhB/0.01 g L1 /50 mL
140 min/100%
RhB/0.01 g L1 /80 mL
60 min/95%
150 min/100%
h+
[436] (2014)
h+
[847]
(2016)
[655] (2014)
ciprooxacin//0.01 g L
100 mL
RhB/0.01 g L1 /40 mL
4.6
[843] (2016)
4.4
[844] (2015)
[845] (2016)
acyclovir/10 ppm/100 mL
90 min/100%
1.57
MB/0.01 g L1 /100 mL
60 min/89%
3.74
O2 , h+
+
[814] (2016)
OH, h , e
MO/0.0135 g L /30 mL
240 min/94%
phenol/0.0166 g L1 /30 mL 240 min/96%
RhB/1 105 M/200 mL
120 min/90%
RhB/0.005 g L1 /100 mL
4
2,4,6-TCP/10
M/20 mL
[846] (2015)
[848] (2014)
0.86
O2 , OH
20 min/95%
[336] (2015)
[849] (2015)
O2 , OOH
[850] (2013)
MO/0.01 g L1 /100 mL
120 min/90%
60 min/84%
O2
[745] (2016)
BPA/0.02 g L1 /50 mL
360 min/100% 1
O2
[729] (2013)
PCP/0.02 g L1 /100 mL
420 min/98%
TC-HCl/0.02 g L
/100 mL
RhB/0.004 g L1 /250 mL
180 min/93%
15.13
1.3
[796] (2015)
OH, h+
[753] (2014)
[851] (2016)
[852] (2015)
42.86
[481] (2015)
3.16
[853] (2015)
ARTICLE IN PRESS
Targe pollutant/
concentration/volume
Structure
G Model
Photocatalyst
Please cite this article in press as: J. Wen, et al., A review on g-C3 N4 -based photocatalysts, Appl. Surf. Sci. (2016),
http://dx.doi.org/10.1016/j.apsusc.2016.07.030
Table 8
Summary of the photocatalytic degradation of pollutants over g-C3 N4 -based photocatalysts.
0.025
0.05
13.5
0.02
0.1
90 min/98.3%
270 min/99%
1.54
OH
particles/lamellar
hydrothermal method
precipitation and reuxing
method
mixing-calcinating method
RhB/0.01 g L1 /100 mL
120 min/97%
3.8
O2 , h+
particles/lamellar
mixing-calcinating method
0.05
[854] (2015)
[535]
(2015)
[855] (2015)
RhB/0.01 g L1 /100 mL
60 min/95.5%
4.91
O2 , h+
[616] (2016)
RhB/0.01 g L1 /300 mL
O2 , h+
[856]
(2015)
[857] (2013)
RhB/0.01 g L1 /300 mL
[858] (2013)
MO/10 ppm/100 mL
180 min/73%
0.78
[859] (2014)
MB/0.01 g L1 /80 mL
240 min/99%
1.73
MO/0.01 g L1 /100 mL
PNP/0.01 g L1 /100 mL
RhB/0.01 g L1 /100 mL
120 min/100%
120 min/100%
120 min/96%
2.52
atrazine/100 ppm/500 mL
60 min/99%
RhB/0.005 g L1 /100 mL
MO/0.02 g L1 /50 mL
phenol/0.02 g L1 /50 mL
RhB/0.005 g L1 /100 mL
30 min/90%
180 min/82%
40 min/100%
10.53
1.4
h+
19.54
BF/0.02 g L1 /50 mL
90 min/100%
Bisphenol/0.02 g L1 /50 mL 90 min/85%
1
MO/0.02 g L /40 mL
60 min/100%
5.52
2.08
4
90 min/88%
tetracycline/0.02 g L1 /100 mL
2.18
O2 , h+
[865] (2016)
180 min/90.45%
OH, h+
[506] (2014)
/100 mL
90 min/88.2%
O2 , h
[866] (2016)
240 min/46%
OH, h+
[867] (2015)
RhB/0.01 g L1 /50 mL
phenol/0.01 g L1 /50 mL
MO/0.02 g L1 /100 mL
80 min/95.8%
180 min/76.1%
120 min/100% 0.77
ZnO@mpgC3 N4
core-shell
ZnO/g-C3 N4
gC3 N4 /ZnO/AgCl
Zn2 SnO4 /gC3 N4
V2 O5 /g-C3 N4
owerlike/lamellar
lamellar/particles
g-C3 N4 /V2 O5
lamellar/nanoparticles
Co-catal./optimized
mass ratio
0.2
one-pot method
0.05
0.3
mixing-calcinating method
0.3
mixing-calcinating method
0.1
SnNb2 O6 /gC3 N4
Ag/g-C3 N4
nanosheets/lamellar
mixing-calcinating method
0.02
particles/lamellar
photodeposition method
AgI@ g-C3 N4
0.1
precipitation method
0.1
AgCl@pg-C3 N4 nanoparticles/lamellar
0.2
deposition-precipitation
method
precipitation method
0.05
g-C3 N4 /Ag2 O
core-shell
Ag/2 wt.%
particles/lamellar
Ag2 O/g-C3 N4
nanoparticles/lamellar
coprecipitation method
Ag@g-C3 N4
core-shell
reuxing method
0.02
0.1
Ag/0.5 wt.%
0.025
0.025
0.05
0.02
particles/nanoclusters/lamellar
hydrothermal-photodeposition Ag/3 wt.%, Fe3 O4 /9 wt.% 0.05
method
lamellar/nanotube
precipitation method
0.08
QDs/lamellar
CdS
QDs/npg-C3 N4
CdWO4 /g-C3 N4 nanorods/lamellar
mixing-calcinating method
0.1
mixing-calcinating method
0.05
hydrothermal method
0.05
in situ method
0.1
RhB/0.01 g L
/50 mL
MB/0.025 g L1 /200 mL
1
RhB/0.01 g L
Main active
species
Ref. (year)
[533] (2014)
80 min/100%
Kapp
[102 min1 ]
30 min/100%
O2 , h+
[640] (2016)
[489] (2013)
O2 , h+
O2 , h+ , OH [860] (2015)
[861] (2015)
O2 , h+ , OH [862] (2015)
[728] (2013)
0.27
O2 , h
[726] (2014)
[488] (2014)
O2 , h+
OH, h+
OH, h+
h+
[433] (2014)
[863] (2015)
[864] (2014)
[802] (2015)
[868] (2014)
ARTICLE IN PRESS
Degradation
time/
efciency
Synthetic method
G Model
Targe pollutant/
concentration/volume
Structure
Photocatalyst
36
Please cite this article in press as: J. Wen, et al., A review on g-C3 N4 -based photocatalysts, Appl. Surf. Sci. (2016),
http://dx.doi.org/10.1016/j.apsusc.2016.07.030
Table 8 (Continued)
Structure
Synthetic method
BiOCl/C3 N4
owerlike/amorphous
solvothermal method
g-C3 N4 /BiOBr
lamellar/nanosheets
BiOx Iy /g-C3 N4
Targe pollutant/
concentration/volume
Degradation
time/
efciency
0.2
MO/0.01 g L1 /500 mL
80 min/95%
RhB/0.06 g L1 /40 mL
2,4-DCP/0.01 g L1 /40 mL
CV/10 ppm/100 mL
100 min/98%
180 min/80%
36 h/99%
4.01
3.91
0.283
240 min/56%
17
O2 , h+
MO/0.01 g L1 /200 mL
180 min/94.82%1.66
deposition-precipitation
method
square thin-plates/lamellar controlled hydrothermal
0.02
0.04
0.01
lamellar/plates
mixing-calcinating method
0.05
lamellar/nanosheets
hydrothermal method
0.4
QDS-lamellar
in situ method
0.05
agglomeration
mixing-calcinating method
0.15
lamellar-hollow sphere
hydrothermal method
0.02
lamellar-akelike
hydrothermal method
0.1
lamellar/particles
ball milling
2gL
CuTCPP/g-C3 N4 rodlike/lamellar
0.3
lamellar/nanoparticles
gC3 N4 /Bi2 MoO6
MoS2 /g-C3 N4 nanosheets/lamellar
calcinating method
0.025
0.01
0.2
[WO4 ]2 doped
0.1
mixing-calcinating method
hydrothermal method
0.05
0.2
mixing-calcinating method
0.1
solvothermal method
0.03
0.04
Ce-doped
0.05
0.1
Ce/g-C3 N4
lamellar
CoO4 /g-C3 N4
lamellar
NiO/g-C3 N4
nanoparticles/lamellar
calcinating method
0.05
RhB/0.01 g L
/50 mL
30 min/100%
Kapp
[102 min1 ]
16.8
MO/0.01 g L1 /50 mL
RhB/0.01 g L1 /50 mL
70 min/98%
Main active
species
Ref. (year)
h+
[869] (2013)
h+
OH
O2
[870] (2013)
[580] (2014)
+
O2 , h , OH [505] (2015)
[576] (2011)
5.15
O2
MO/0.005 g L1 /100 mL
120 min/93%
2,4-DCP/0.02 g L1 /100 mL 300 min/92%
1
acid orange II/0.05 g L
0.856
4.1
O2
O2 , h
RhB/0.015 g L1 /100 mL
1.41
240 min/90%
phenol/5 ppm/50 mL
1
[871]
(2016)
[872] (2014)
[873] (2014)
[874] (2013)
+
O2
[875]
(2016)
[876] (2015)
0.04
O2 , h+
[877] (2015)
MO/0.02 g L /50 mL
MO/0.01 g L1 /160 mL
70 min/83.3%
240 min/86%
2.05
0.88
O2 , h
O2 , OH
[878] (2016)
[587] (2016)
RhB/10 ppm/100 mL
90 min/87%
2.2
O2 , OH
[879] (2015)
RhB/0.005 g L1 /100 mL
MO/0.01 g L1 /100 mL
DEP/0.01 g L1 /100 mL
MB/0.01 g L1 /100 mL
90 min/91%
2.61
240 min/99%
1440 min/85%
180 min/93%
1.47
[544] (2015)
[880] (2014)
MB/0.01 g L1 /30 mL
40 min/90%
6.88
RhB/0.01 g L1 /50 mL
MO/0.01 g L1 /50 mL
RhB/10 ppm/200 mL
20 min/96%
180 min/95%
120 min/90%
15.2
1.61
1.55
[604]
(2015)
[633] (2016)
MO/0.01 g L1 /100 mL
120 min/100%
MB/0.005 g L1 /100 mL
40 min/100%
[881] (2013)
h+
h+
O2
5.1
O2
[882] (2015)
[688] (2014)
[734] (2014)
ARTICLE IN PRESS
Co-catal./optimized
mass ratio
G Model
Photocatalyst
Please cite this article in press as: J. Wen, et al., A review on g-C3 N4 -based photocatalysts, Appl. Surf. Sci. (2016),
http://dx.doi.org/10.1016/j.apsusc.2016.07.030
Table 8 (Continued)
Morphologies and
microstructures
g-C3 N4 /NaNbO3
NaNbO3 nanowires/g-C3 N4
nanosheets
TiO2 nanoparticles/g-C3 N4
nanosheets
worm-like mesostructures
direct thermolysis
in-situ deposition
in situ hydrothermal approach
hard-template route
ultrasonic dispersion followed
by heat treatment method
directly calcining
simple calcination of g-C3 N4
and Sn6 O4 (OH) 4
calcination
2 wt% Pt
S-doped g-C3 N4
AgX/g-C3 N4 (X = Cl and
Br)
AgCl/C3 N4
AgCl nanoparticles/C3 N4
nanosheet
GO-g-C3 N4
sandwich-like
RGO/p-C3 N4
sandwich-like
g-C3 N4 /ZnO
[608] (2015)
[927] (2016)
CH4 (2.5)
[693] (2015)
CO(19.2) CH4(1.4)
CH3 OH(3.1)
[928] (2015)
0.05/CO2 and H2 O
vapor/230 mL
0.1/CO2 and H2 O
vapor/780 mL
0.1/CO2 and H2 O
vapor/2700 mL
/
0.006/CO2 and H2 O
vapor/100 mL
CH4 (6.4)
[929] (2014)
CO(12.25)
[930] (2014)
[931] (2016)
CH3 CHO(8)
CH4 (0.85)
[932] (2015)
[933] (2016)
CH4 (1.302)
[692] (2015)
CH3 CHO(0.37)
[199] (2015)
CO(39) CH3OH(10)
CH4(4) C2H5OH(1.5)
CH3 OH(0.6)
[536] (2015)
CH4 (1.393)
[934] (2015)
[614] (2016)
CH4(0.3) HCHO(0.075)
CH3OH(0.24)
[691] (2014)
/
300 W Xenon short arc
lamp
405 nm < < 723 nm
15 W energy-saving
daylight bulb
300-W simulated solar
Xe arc lamp
500 W Xe lamp
nanoparticles/lamellar
g-C3 N4 Pt
300 W Hg lamp
Pt/g-C3 N4
BiOI/g-C3 N4
300 W Xe lamp,
420 nm
300 W Xe lamp,
420 nm
300 W of Xenon-arc
lamp
300 W Xe lamp,
420 nm
500 W Xe lamp
/
/
0.8%wt Pt
RGO/g-C3 N4
Ref. (year)
hard-template synthesis
solvent evaporation
method
ZnO microcrystals/g-C3 N4
nanosheets
sandwich-Like Hybrid
Nanosheets
BiOI particles/g-C3N4
nanosheets
two-dimensional lamellar
structure and numerous
randomly organized
nanosheets
irregular spheres of
AgX/g-C3N4 nanosheets
Selective products
(activity) [M h1 g1 ]
sponge-like structure
B4 C particles/g-C3 N4
nanosheets
g-C3 N4 /ZnO
Mass [g]/systems/Volume
[mL]
C3 N4 MCF
B4 C/C3 N4
ZnO/g-C3 N4
Light source
1 wt% Pt
sonication-assisted
deposition-precipitation
approach
in situ
depositionprecipitation
approach.
a facile one-pot
impregnationthermal
reduction strategy
a novel combined ultrasonic
dispersion and electrostatic
self-assembly strategy
a one-step facile calcination
method
15 wt% RGO
1 wt% Pt
0.1/CO2 and
H2 O vapor/500 mL
0.05/CO2 and
H2 O vapor/500 mL
0.1/CO2 and H2 O vapor
0.1/CO2 and H2 O
vapor/180 mL
0.1/CO2 and H2 O
vapor/200 mL
[926] (2015)
[220] (2015)
30%AgBr/g-C3 N4
CH4 (1.092)
[935] (2016)
15 W energy-saving
daylight lamp
CH4 (0.95)
[936] (2016)
15 wt% GO
15 W energy-saving
daylight bulb
CH4 (5.87)
[702] (2015)
15 wt% rGO
15 W energy-saving
daylight lamp
CH4 (1.393)
[160] (2015)
CH3 OH(0.6)
[601] (2015)
ARTICLE IN PRESS
Mo-doped g-C3 N4
g-C3 N4 nanosheets/layered
structure KNbO3
SnO2-x nanoparticles/g-C3N4
sheets are
Cocatalyst
g-C3 N4 -N-TiO2
Synthesis method
G Model
Material
38
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http://dx.doi.org/10.1016/j.apsusc.2016.07.030
Table 9
Summary of the photocatalytic CO2 reduction over g-C3 N4 -based photocatalysts.
G Model
ARTICLE IN PRESS
[939] (2016)
250 W lamp,
= 365 nm
nanospheres/aky morphology
CdS/g-C3 N4
polycondensation and
hydrothermal methods
/
a facile one-pot chemical
condensation of urea
dense and stacked particles
and sheets
CNUBAX
300 W Xe lamp,
> 420 nm
0.03/CO2 saturated
solution of CoCl2 ,
2,2-bipyridine,
triethanolamine
0.02/CO2 saturated
methanol solution/20 mL
HCOOH (1352.07)
[938] (2015)
[620] (2014)
Ag/g-C3 N4 + WO3 :
CH3 OH(24.05)
Au/g-C3 N4 + WO3
CH3 OH(34.02)
CO(469)
0.003/CO2 and H2 O
0.5%wt Au,
0.5%wt Ag
WO3 /
g-C3 N4 (P-CW)
planetary mill
photodeposition method
amine-functionalized
g-C3 N4
CO(9.9)
/
thermal condensation
of melamine
facile electrostatic
self-assembly method
thin nanosheets
2D hydroxyl-rich C3 N4
nanosheets
UiO-66/10%CNNS
light-emitting diode
(LED), = 435 nm
[227] (2015)
CH4 (0.34)
CH3 OH(0.28)
[708] (2015)
[937] (2015)
CH4 (0.75)
[697] (2016)
HCOOH(7.8)
0.005/CO2 and MeCN/TEOA
mixture (4:1, v/v) 4 mL
400 W high
pressure Hg lamp with
a NaNO2 solution lter
300 W Xe lamp,
> 420 nm
300 W xenon arclamp,
400 nm< < 800 nm
RuP
adsorption
Suspension systems for CO2 photoreduction
mesoporous structure
RuP/g-C3 N4
Material
Table 9 (Continued)
Morphologies and
microstructures
Synthesis method
Cocatalyst
Light source
Mass [g]/systems/Volume
[mL]
Selective products
(activity) [M h1 g1 ]
Ref. (year)
39
highest apparent quantum yield of 5.7% at 400 nm for the photocatalytic reduction of CO2 into formic acid under visible-light
irradiation (as shown in Fig. 50) [695]. Surprisingly, the ternary
hybrid of plasmonic Ag nanoparticles and g-C3 N4 /binuclear Ru(II)
complex could achieve a very high turnover number of > 33,000
with a high selectivity of 8799% for HCOOH production, due to the
combination effects of plasmonic Ag and Z-Scheme charge transfer (as shown in Fig. 51) [700]. These are the best values that have
been reported for heterogeneous photocatalysts for CO2 reduction
under visible-light irradiation to date. The present study clearly
highlighted the great potential of complex molecular co-catalyst
on carbon nitride in photocatalytic CO2 reduction under visible
light. Thus, it is expected that the multi coupling of complex molecular co-catalyst, g-C3 N4 and other photosensitizers may provide
exciting opportunities for promising CO2 photoreduction over gC3 N4 -based photocatalysts. In addition, it is also noted from Table 9
that there are few earth-abundant co-catalysts reported to accelerate the CO2 photoreduction over g-C3 N4 -based photocatalysts,
which should be urgently developed in the near future. At this
point, the nano-carbons, such as RGO and CNTs, are highly expected
to coupling with the g-C3 N4 to obtain highly efcient metal-free
g-C3 N4 -based photocatalysts for CO2 photoreduction [934].
Besides co-catalysts, doping and nanostructured heterojunction
were also extensively used to enhance the visible light absorption and photocatalytic CO2 reduction activity of g-C3 N4 -based
photocatalysts. Wang et al. fabricated sulfur-doped g-C3 N4 photocatalysts by employing thiourea as the sulfur precursor for the
reduction of CO2 to CH3 OH [199]. The DFT studies conrmed that
the electrons can be easily excited from the VB to the impurity
state, and then to the CB of sulfur-doped g-C3 N4 owing to the
impurity sulfur doping (as shown in Fig. 52a), which induced additional electrons, resulting in the spin polarization. As the band
gap was narrowed from 2.7 to 2.63 eV, the light absorption was
broadened in the sulfur-doped g-C3 N4 , generating more electrons and holes under the light irradiation. Thus, the CH3 OH yield
(1.12 mol g1 ) was 1.5 times higher than that the unmodied gC3 N4 (0.81 mol g1 ) (as shown in Fig. 52b). In another example,
Yu et al. constructed a binary g-C3 N4 /ZnO photocatalyst with an
intimate contact interface via a one-step facile calcination method
[220]. The results showed that the as-prepared g-C3 N4 /ZnO photocatalytic system exhibited enhanced photocatalytic activity for
CO 2 reduction by a factor of 2.3 compared with pure g-C3 N4 (as
shown in Fig. 53a). The better performances of the g-C3 N4 /ZnO
binary composite photocatalytic system could be well explained
by the direct Z-scheme mechanism rather than the conventional
heterojunction-type mechanism (as shown in Fig. 53b and c), which
was achieved due to the highly efcient ZnO-to-g-C3 N4 electron
transfer occurring at the intimate contact interface between the gC3 N4 phase and ZnO phase. This work highlighted that the rational
construction of direct Z-scheme g-C3 N4 -based photocatalytic system without an electron mediator should be promising strategy for
the applications in the photocatalytic CO2 reduction.
On the other hand, the product selectivity of photocatalytic CO2
reduction should be also a major consideration in designing semiconductor photocatalysts [942]. For example, Liu and coworkers
obtained the g-C3 N4 nanosheets by the thermal delamination of
bulk g-C3 N4 in air. It was shown that g-C3 N4 nanosheets with a band
gap of 2.97 eV yielded the major product of CH4 , whereas bulk gC3 N4 with a smaller band gap of 2.77 eV formed the main product of
CH3 CHO (Fig. 54a) [409]. This elucidated that the nanosheets had a
larger band gap by 0.2 eV, leading to a lower VB edge by 80 meV and
a higher CB edge by 120 meV. Therefore, the nanosheets provided a
larger thermodynamic diving force for the hole and electron transfer by means of a greater difference in energy level between redox
potentials of the reactants and band edges (Fig. 54b). This indirectly led to a larger proportion of long-lived charge carriers for the
Please cite this article in press as: J. Wen, et al., A review on g-C3 N4 -based photocatalysts, Appl. Surf. Sci. (2016),
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J. Wen et al. / Applied Surface Science xxx (2016) xxxxxx
Fig. 49. (a) Photoconversion of CO2 into CH4 , CH3 OH and HCHO over PtX -loaded g-C3 N4 (x, the weight percentage ratios of Pt against g-C3 N4 were 0, 0.25, 0.5, 0.75, 1.0 and
2.0 wt%); (b) Charge separation mechanisms in the Pt/g-C3 N4 systems [691].
Fig. 50. Scheme illustration for CO2 reduction using a Ru complex/C3 N4 hybrid
photocatalyst.
Fig. 51. Scheme illustration for Z-Scheme CO2 reduction using a ternary Hybrid of
Ag/g-C3 N4 /Binuclear Ru(II) Complex [700].
Please cite this article in press as: J. Wen, et al., A review on g-C3 N4 -based photocatalysts, Appl. Surf. Sci. (2016),
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41
Fig. 52. (a) Schematic of band structure of pure g-C3 N4 (left) and S-doped g-C3 N4 (right); (b) Comparison of photocatalytic CH3 OH production over S-doped g-C3 N4 (TCN)
and un-doped g-C3 N4 (MCN) at 3 h under UVvis light irradiation [199].
Fig. 53. Comparison of photocatalytic CH3 OH production rates of cm-ZnO, pure ZnO, G10, and pure g-C3 N4 . Schematic illustration of two different mechanisms for charge
carrier separation: (b) conventional heterojunction-type and (c) direct Z-scheme mechanisms [220].
Fig. 54. (a) Schematic illustration of the photoreduction CO2 to CH3 CHO and CH4 on bulk g-C3 N4 and g-C3 N4 nanosheets. (b) Band structures of g-C3 N4 nanosheets (left) and
bulk g-C3 N4 (right) and the redox potentials of the reactions [409].
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Fig. 56. Schematic illustration of the visible-light-driven photocatalytic bacterial inactivation mechanisms of (a) CNRGOS8 ; (b) RGOCNS8 in aerobic condition; (c) CNRGOS8 ;
(d) RGOCNS8 in anaerobic condition [660].
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