Review on g-C3N4-based S-scheme heterojunction photocatalysts

doi:10.1016/j.jmst.2022.02.035

Abstract

Abstract:

With the rapid development of economy and modern industry, serious environmental pollution and energy shortage have become major urgent challenges to the human society. Photocatalysis is a promising technology to provide green energy. As a typical metal-free polymer photocatalyst, g-C₃N₄ has attracted more and more attention due to its excellent performance. Unfortunately, the fast recombination of photo-induced charges, limited light response range as well as weak oxidation ability are still the key drawback that restrict the photocatalytic performance of g-C₃N₄. These problems can be effectively addressed by constructing g-C₃N₄-based heterojunctions with two or more semiconductor materials, during which the respective advantages can be integrated. Up to now, the various oxidation semiconductor photocatalysts have been tried to construct the novel S-scheme heterojunction photocatalysts with g-C₃N₄. Thus, this review provides a comprehensive introduction of g-C₃N₄-based S-scheme heterojunctions, including the main characteristics of the S-scheme heterojunction, photocatalytic mechanisms, design rules and preparation methods of g-C₃N₄-based S-scheme heterojunction photocatalysts. Moreover, this review summarizes recently reported works on the potential applications of g-C₃N₄-based S-scheme photocatalysts in various important photocatalytic reactions, including photocatalytic hydrogen production, photocatalytic degradation of contaminants, photo-reduction of CO₂ into fuels, and photocatalytic sterilization. Finally, based on the current research progress, we propose some shortages in the preparation methods and applications of g-C₃N₄-based S-scheme heterojunctions, which are to be further investigated and resolved in this promising and creative research field.

Key words: Photocatalysis, Semiconductor, g-C₃N₄, Heterojunction, S-scheme

Yunfeng Li, Zhiling Xia, Qing Yang, Linxi Wang, Yan Xing. Review on g-C₃N₄-based S-scheme heterojunction photocatalysts[J]. J. Mater. Sci. Technol., 2022, 125: 128-144.

Figures/Tables 22

Fig. 1. The main steps of photocatalytic reactions over g-C3N4 semiconductor photocatalysts.

Fig. 2. Schematic diagram of charge transfer for various typical g-C3N4-based heterojunctions.

Fig. 3. Two possible charges transfer paths for (A,C) traditional Z-scheme heterojunction and (B,D) all-solid-state Z-scheme heterojunction. The labels D and A stand for electron donor and acceptor, respectively.

Fig. 4. Energy band structure diagram of typical oxidation photocatalyst and reduction photocatalyst for constructing S-scheme heterojunction.

Fig. 5. Charges transfer path and mechanism of novel S-scheme heterojunction photocatalyst.

Fig. 6. Schematic diagram for the fabrication of all organic PDI-Ala/S-C3N4 S-scheme heterojunction photocatalysts. Reproduced with permission from Ref. [86]. Copyright 2021, Acta Physico-Chimica Sinica.

Fig. 7. (A) Transient photocurrent response, (B) electrochemical impedance spectroscopy and (C) photocatalytic reaction mechanism of defect-functionalized WO3/g-C3N4 S-scheme heterojunction. Reproduced with permission from Ref. [98]. Copyright 2021, Royal Society of Chemistry.

Fig. 8. (A) Transient photocurrent response, (B) linear sweep voltammetry, (C) electrochemical impedance spectroscopy and (D) photoluminescence spectrum of the samples. Reproduced with permission from Ref. [99]. Copyright 2021, American Chemical Society.

Fig. 9. (A) Calculated charges density difference within the composite system. Photocatalytic mechanism of S-scheme (B) g-C3N4/SnS2 and (C) O-C3N4/SnS2 heterojunctions. Reproduced with permission from Ref. [100]. Copyright 2021, Elsevier.

Table 1. Various g-C3N4-based S-scheme heterojunctions for photocatalytic hydrogen production reported in recent years.

S-scheme heterojunction	Mass of sample	Light source (wavelength/nm)	Hydrogen (μmol/h)	Enhancement factor versus g-C₃N₄	AQY (%)	Refs.
WO₃/g-C₃N₄	50	350 W Xe lamp (λ>420 nm)	982	1.7	—	[53]
BiVO₃/g-C₃N₄	50	350 W Xe lamp	6800	10	—	[76]
N-MoS₂/S-g-C₃N₄	50	300 W Xe lamp	658.5	23	—	[78]
Bi₂S₃/g-C₃N₄	30	300 W Xe lamp	3394.1	2.6	—	[79]
WO₃/g-C₃N₄	30	300 W Xe lamp	1034	4.5	7.4	[98]
g-C₃N₄/α-Fe₂O₃/Co₃S₄	10	5 W LED white light	191.41	1007.4	—	[99]
O-g-C₃N₄/SnS₂	20	350 W Xe lamp	154	—	—	[100]
(TiO₂NT)/TiO₂/g-C₃N₄	30	300 W mercury lamp	7.97	—	—	[101]
W₁₈O₄₉/g-C₃N₄	25	300 W Xe lamp (λ>420 nm)	892	3.4	6.21	[102]
CdS/g-C₃N₄	5	300 W Xe lamp (λ>420 nm)	15300	3060	6.86	[103]
g-C₃N₄/g-C₃N₄	50	300 W Xe lamp (λ>420 nm)	29.9	1.8	—	104
BiOBr/g-C₃N₄	30	300 W Xe lamp (λ>420 nm)	106.63	—	—	[105]
g-C₃N₄/Bi₂MoO₆	50	300 W Xe lamp (λ>420 nm)	5.63	2.5	—	[106]
Ni₂P/g-C₃N₄/CdZnSe	20	300 W Xe lamp (λ>420 nm)	12627	105.23	—	[107]
pg-C₃N₄/CdS-DETA	50	300 W Xe lamp (λ>420 nm)	9738	12.2	—	[108]
S/Cl-g-C₃N₄/CdSe-D	20	300 W Xe lamp (λ>420 nm)	18800	391.67	—	[109]
MoO₃/g-C₃N₄	50	300 W Xe lamp (λ>420 nm)	512500	13.9	—	[110]
g-C₃N₄/Zn_0.2Cd_0.8S-DETA	50	300 W Xe lamp (λ>420 nm)	6690	16.7	—	[111]
CuInS₂/g-C₃N₄	50	350 W Xe lamp (λ>420 nm)	375	1.57	—	[112]
CuI-GD/g-C₃N₄	10	5 W LED white light	49.8	9.8	—	[113]
CdS/g-C₃N₄	50	300 W Xe lamp (λ>400 nm)	262.6	26.8	—	[114]
Ag/g-C₃N₄-g-C₃N₄	10	400 W metal halide lamp	10100	8	—	[115]

Fig. 11. Photocatalytic CO production rates over prepared samples in (A) acetonitrile/H2O and (B) ethyl acetate/H2O solvent systems. (C) Stability test and (D) CO production rates under various conditions. Reproduced with permission form Ref. [129]. Copyright 2021, American Chemical Society.

Fig. 12. (A) CO and CH4 yields and (B) H2, CO, CH4 yields with CO2 selectivity of the samples. (C) N2 adsorption-desorption isotherms and (D) CO2 adsorption capacity on the TiO2/MoS2/g-C3N4 S-scheme heterojunctions. Reproduced with permission form Ref. [130]. Copyright 2021, Elsevier.

Table 2. g-C3N4-based S-scheme heterojunctions for photocatalytic CO2 reduction reported in recent years.

S-scheme heterojunction	Mass of sample	Light source (wavelength/nm)	Reduction products	Yield (μmol g^-1)	Enhancement factor versus g-C₃N₄	Refs.
BiOBr/g-C₃N₄	20	100 W Xe lamp	CH₃OH	1068.07	—	[42]
g-C₃N₄/CdSe-DETA	50	300 W Xe lamp (λ>420 nm)	CO	25.87	—	[61]
g-C₃N₄/Bi/BiVO₄	100	300 W Xe lamp (λ>420 nm)	CO	0.63	—	[65]
g-C₃N₄/TiO₂/C	30	Xe lamp (PLS-SXE300)	CO+CH₄	9030	2.88	[84]
TiO₂/C₃N₄/Ti₃C₂MXene	30	350 W Xe lamp	CO+CH₄	5.59	3	[128]
us-Cu₃P\|S/g-C₃N₄	5	300 W Xe lamp	CO	137	8	[129]
TiO₂/MoS₂/g-C₃N₄	20	300 W Xe lamp (λ>420 nm)	CO+CH₄	67.41	3.1	[130]

Fig. 13. (A) Photocatalytic degradation of RhB over CdS-g-C3N4-GA with and without addition of scavengers. (B, C) EPR spectra of the prepared samples. (D-F) Calculated work functions of GA, g-C3N4 and CdS. (D) The charges transfer mechanism of CdS-g-C3N4-GA S-scheme heterojunctions. Reproduced with permission from Ref. [134]. Copyright 2021, Elsevier.

Fig. 14. Mott-Schottky plots of (A) MoS2/g-C3N4 sample prepared by calcination at 600 °C, (B) g-C3N4 sample prepared by calcination at 500 °C and (C) MoS2/g-C3N4 sample prepared by calcination at 500 °C. (D) The schematic diagram of band alignment of heterojunction and S-scheme charge transfer mechanism at interface of MoS2 and g-C3N4. Reproduced with permission from Ref. [135].

Fig. 15. (A,B) Photocatalytic degradation of tetracycline on prepared samples and fitted kinetic data assuming 1st-order reactions. (C) The k value of the fitted kinetic data. (D) Stability test of S-doped g-C3N4/WO2.72 S-scheme heterojunction. Reproduced with permission from Ref. [136]. Copyright 2021, Elsevier.

Table 3. g-C3N4-based S-scheme heterojunctions for photocatalytic degradation of pollutants reported in recent years.

S-scheme heterojunction	Light source (wavelength/nm)	Application	Removal rate	Enhancement factor versus g-C₃N₄	Refs.
ZnFe₂O₄/g-C₃N₄	8 W LED light	Uranium (VI)	94.62%	—	[21]
Bi₂WO₆/g-C₃N₄	300 W Xe lamp (λ>400 nm)	Ammonium dinitramide	98.93%	7.17	[38]
WO₃/g-C₃N₄	300 W Xe lamp	Tetracycline	90.54%	2.25	[44]
ZnO/g-C₃N₄	350 W Xe lamp (λ>420 nm)	MB	92.5%	8.5	[47]
g-C₃N₄/ZrO₂	300 W Xe lamp	Acid orange II	98%	—	[59]
Bi₂O₃/P-C₃N₄	500 W Xe lamp	Levofloxacin	89.2%	1.33	[60]
Bi₂MoO₆/g-C₃N₄	300 W Xe lamp (λ>420 nm)	RhB	97.6%	13.1	[64]
Cd_0.5Zn_0.5S/ g-C₃N₄	350 W Xe lamp (λ>420 nm)	RhB	97.8%	13	[71]
g-C₃N₄/AgBr/BP	PL-X300D xenon light	MO	98.0%	—	[75]
S-g-C₃N₄/TiO₂	300 W Xe lamp	Congo Red	96.2%	8.2	[77]
g-C₃N₄/Bi₂WO₆	300 W Xe lamp (λ>420 nm)	Tetracycline	81.4%	2.85	[80]
g-C₃N₄/Si-Fe₂O₃	150 W Xe lamp	2-chlorophenol	96.6%	—	[82]
Bi₂O₂CO₃/g-C₃N₄	300 W Xe lamp (λ>400 nm)	Tetracycline	96%	3.96	[85]
PDI-Ala/S-C₃N₄	350 W Xe lamp (λ>420 nm)	Tetracycline	90%	2.14	[86]

Fig. 16. (A) Photocatalytic activities of HCHO removal under full spectrum light. (B) Pseudo second-order reaction kinetic fits and (C) HCHO conversion, CO2 and CO selectivity on as-synthesized samples. (D) The cycle tests of the sample under full spectrum light. Reproduced with permission from Ref. [143]. Copyright 2021, Elsevier.

Fig. 17. The antibacterial effects without illumination, under illumination and corresponding fluorescent dye mapping images over (A-C) the blank experiment, (D-F) g-C3N4, (G-I) CeO2, and (J-L) CeO2/g-C3N4 composite, respectively. Reproduced with permission from Ref. [144]. Copyright 2020, Wiley-VCH.

Fig. 18. (A) Photocatalytic NO oxidation and (B) stability tests of the as-prepared samples. (C) In situ DRIFT spectra of the photocatalytic reaction of NO over the prepared sample. Reproduced with permission from Ref. [145]. Copyright 2021, Elsevier.

Fig. 19. Some special concerns to be further studied and clarified for g-C3N4-based S-scheme heterojunctions.

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Review on g-C₃N₄-based S-scheme heterojunction photocatalysts

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