Few-layer carbon nitride photocatalysts for solar fuels and chemicals: Current status and prospects

doi:10.1016/S1872-2067(21)63985-2

Abstract

Abstract:

Converting sunlight directly to fuels and chemicals is a great latent capacity for storing renewable energy. Due to the advantages of large surface area, short diffusion paths for electrons, and more exposed active sites, few-layer carbon nitride (FLCN) materials present great potential for production of solar fuels and chemicals and set off a new wave of research in the last few years. Herein, the recent progress in synthesis and regulation of FLCN-based photocatalysts, and their applications in the conversion of sunlight into fuels and chemicals, is summarized. More importantly, the regulation strategies from chemical modification to microstructure control toward the production of solar fuels and chemicals has been deeply analyzed, aiming to inspire critical thinking about the effective approaches for photocatalyst modification rather than developing new materials. At the end, the key scientific challenges and some future trend of FLCN-based materials as advanced photocatalysts are also discussed.

Key words: Few-layer carbon nitride, Photocatalyst, Synthesis technique, Structure regulation, Solar fuels and chemicals

Fangshuai Chen, Chongbei Wu, Gengfeng Zheng, Liangti Qu, Qing Han. Few-layer carbon nitride photocatalysts for solar fuels and chemicals: Current status and prospects[J]. Chinese Journal of Catalysis, 2022, 43(5): 1216-1229.

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Figures/Tables 12

Fig. 1. The overview diagram of FLCN-based architectures including chemically modified and microstructure-tailored nanosheets, as well as their applications in converting sunlight into fuels and chemicals.

Fig. 2. (a) Schematic illustration of liquid-exfoliation process from bulk CN to CN nanosheets. (b) Nyquist plots of CN nanosheets and bulk CN. Reprinted with permission from Ref. [35]. Copyright 2013, American Chemical Society. (c) Atomic force microscopy (AFM) of CN nanosheets. Inset: the Tyndall effect of the CN nanosheets aqueous dispersion. Reprinted with permission from Ref. [43]. Copyright 2019, Elsevier Inc. (d) The displacement-voltage curve and phase curve of U-T-CN. Reprinted with permission from Ref. [45]. Copyright 2015, Wiley-VCH. (e) Schematic of the formation process of CN nanosheets by the thermal oxidation etching method. Reprinted with permission from Ref. [44]. Copyright 2012, Wiley-VCH. (f) The dipole moment of CN monolayer with different numbers of tri-s-triazine units. Reprinted with permission from Ref. [45]. Copyright 2015, Wiley-VCH.

Fig. 3. (a) Vacuum freeze-drying process for the preparing FLCN seaweed architecture. Reprinted with permission from Ref. [47]. Copyright 2015, Wiley-VCH. (b) Schematic representation of FLCN. Reprinted with permission from Ref. [30]. Copyright 2019, American Chemical Society. SEM images of the pristine DCDA (c), the nanostructured DCDA (d). Inset in (c): Photograph of DCDA solution; inset in (d): Photograph of nanostructured DCDA. TEM images of the mesoporous CN bulk (e) and monolayer CN nanomesh (f). (g) AFM image of monolayer CN nanomesh; (h) Height profiles along the lines in (g). (c?h) Reprinted with permission from Ref. [52]. Copyright 2016, American Chemical Society.

Fig. 4. (a) Schematic of ball-milling process of bulk CN and iodine resulting in the formation of ICNs. (b) AFM image of ICNs. (a,b) Reprinted with permission from Ref. [2]. Copyright 2015, Royal Society of Chemistry. (c) Illustration showing the growth of ultrathin carbon nitride film by CVD onto the surface of quartz substrate. (d) Quartz substrate before and after the film polymerization. Scale bar: 1 cm. (e) TEM image of CN thin film. (c-e) Reprinted with permission from Ref. [56]. Copyright 2020, Wiley-VCH.

Fig. 5. Scheme of heteroatom doped FLCN (a), defect-rich FLCN (b), FLCN/polymer or graphene hybrids (c) and FLCN/metal hybrids (d); (e) TEM image of ICNs. (a?e) Reprinted with permission from Ref. [2]. Copyright 2015, Royal Society of Chemistry. (f) TEM image of nitrogen defects-rich CN nanosheets. Reprinted with permission from Ref. [7]. Copyright 2018, American Chemical Society. (g) TEM images of 2D mesoporous CN on 2D mesoporous graphene sheets(CN@GM). Reprinted with permission from Ref. [101]. Copyright 2017, Wiley-VCH. (h) TEM image of Ag nanoparticle decorated FLCN hybrids. Reprinted with permission from Ref. [3]. Copyright 2019, Wiley-VCH.

Fig. 6. (a) UV-Vis absorption spectra of bulk CN and ICNs-x (x represents I atomic percentage). Inset in (a): PL spectra of bulk CN, I-free CNSs and ICNs-0.34. (b) Photocatalytic H2 production rate of bulk CN, I-free CNs, ICNs-0.76, ICNs-0.34, ICNs-0.19 and ICNs-0.08 under λ > 420 nm. (a,b) Reprinted with permission from Ref. [2]. Copyright 2015, Royal Society of Chemistry. (c) The nitrogen temperature programmed desorption (N2-TPD) curves of BCN and pristine CN; (d) The photocatalytic NH3 yield rates of BCN and pristine CN in N2-saturated Na2SO3 solution under visible-light irradiation. (c,d) Reprinted with permission from Ref. [70]. Copyright 2020, Wiley-VCH.

Fig. 7. (a) UV-Vis spectra of NVs-CN and pristine CN. Inset: schematic diagram of the possible molecular structure of NVs-CN. (b) Photocatalytic activities of CN and NVs-CN under visible light irradiation. Inset in (b): EPR spectra of CN and NVs-CN. TEM images of NVs-CN (c) and CN (d) after photocatalytic reaction. (e) Time-resolved PL decay spectra of BCN and pristine CN. (a?e) Reprinted with permission from Ref. [7]. Copyright 2018, American Chemical Society. (f) Schematic diagram of the possible molecular structure of CN-O. (g) The highest occupied molecular orbitals (VB) and lowest unoccupied molecular orbitals (CB) of CN-O and pristine CN. (h) Mott-Schottky plots for CN-O and pristine CN. (i) EPR spectra (left) and the relative variation of the number of spins (Nx/NCTHP30, right) for pristine CN, CHP, THP, and CTHP30, respectively. (j) H2 evolution and O2 evolution rate of the pristine CN, THP, CHP, and CTHPx, respectively. (f?j) Reprinted with permission from Ref. [26]. Copyright 2021, Royal Society of Chemistry.

Fig. 8. (a) UV-vis absorption curves of CN-Au(111), pristine CN, AuNP. Inset in (a): Transient photocurrent responses of CN-Au(111) and pristine CN, λ > 420 nm. Reproduced with permission [83]. Copyright 2018, American Chemical Society. (b) TEM image of In2O3-cube/FLCN, respectively; inset of (b): statistic edge length of In2O3-cube. (c) Nanosecond transient absorption kinetic analysis at 670 nm and exponential function fitted curves of pristine CN and In2O3-cube/FLCN. (b,c) Reprinted with permission from Ref. [84]. Copyright 2021, Wiley-VCH.

Fig. 9. (a) Schematic illustration of photocatalytic CO2 reduction on FLCN photocatalyst coloaded with reduction and oxidation cocatalysts for solar fuel production. Reproduced with permission [88]. Copyright 2018, Wiley-VCH. (b) Optimized adsorption modes for CO2 over BIF-20 with exposed B-H bonding sites (the top) and the calculated charge distribution over the framework in the neutral state or in the one-electron charged state (the bottom). (c) CO2 adsorption-desorption isotherms of the CNNs, BIF-20/CNNs, and ZIF-8/CNNs at 23 °C. (d) Time course of production evolution in different reaction conditions. (b?d) Reproduced with permission [89]. Copyright 2020, American Chemical Society. (e) TEM image of the resulting 15CN/BVNS heterojunction; (f) The mechanism of the photocatalytic activities for CO2 reduction under UV-visible light using 15CN/BVNS. (g) Illustration of energy band structures of the heterojunction. (e?g) Reproduced with permission [80]. Copyright 2021, Wiley-VCH.

Fig. 10. Scheme of FLCN QDs (a), FLCN nanoribbon (b), FLCN nanomeshes (c), and FLCN assembly (d); (e) TEM image of FLCN QDs. Reproduced with permission [54]. Copyright 2015, Springer Nature. (f) TEM image of FLCN nanoribbon. Reprinted with permission from Ref. [96]. Copyright 2020, Royal Society of Chemistry. (g) TEM image of FLCN nanomesh. Reprinted with permission from Ref. [52]. Copyright 2016, American Chemical Society. (h) TEM image of FLCN assembly. Reprinted with permission from Ref. [47]. Copyright 2015, Wiley-VCH.

Fig. 11. (a) Schematic illustration of band structures of bulk CN and FLCN QDs, and their corresponding Photographs of the solutions in water with concentrations of 0.1 mg·mL-1 after one week. (a) Reprinted with permission from Ref. [54]. Copyright 2015, Springer Nature. (b) A-D motifs in TOH-CN. Inset: the differences in hydrophilicity between bulk CN (the top) and TOH-CN (the bottom); (c) Energy schematic of the TOH-CN for water splitting. (b,c) Reprinted with permission from Ref. [96]. Copyright 2020, Royal Society of Chemistry. (d) Proposed reaction mechanism of oxidative coupling of benzylamine over FLCN. (d) Reprinted with permission from Ref. [30]. Copyright 2019, American Chemical Society. (e) TEM image of G@CN MMs. The pore size of several nanometers in diameter originates from GM, and the hole size larger than 10 nm corresponds to CNM. (e) Reprinted with permission from Ref. [101]. Copyright 2017, Wiley-VCH. (f) H2O2 production is accomplished by photocatalysis. (f) Reprinted with permission from Ref. [3]. Copyright 2019, Wiley-VCH. (g) Transient photocurrents of CN seaweed (1), and CN nanomesh (2), and CN bulk (3) under visible light illumination. (g) Reprinted with permission from Ref. [47]. Copyright 2015, Wiley-VCH. (h) Photocatalytic H2 yield rates of Pt/bulk CN, CN fiber@N-carbon, Pt/CN fiber, and CN/N-carbon fiber; (i) The mechanism of the photocatalytic activities for H2 evolution using CN/N-carbon fiber. (h,i) Reprinted with permission from Ref. [110]. Copyright 2016, Wiley-VCH.

Table 1 Summary of the typical FLCN-based photocatalysts for solar fuels and chemicals.

Photocatalyst	Synthesis method	Regulation strategy	Badgap (eV)	CB (eV)	VB (eV)	Performance improvement	Photocatalytic performance	Ref.
I-doped CN nanosheets	Ball milling	Heteroatom doping	2.37	-1.01	1.36	(1), (3)	HER = 890 μmol g^-1 h^-1 AQE = 3.0% at 420 nm	[2]
Ag@FLCN	Exfoliation	Microstructure mediation	2.7	-1.3	1.4	(1), (2), (3)	H₂O₂ yield rate = 1185 μmol g^-1 h^-1	[3]
NVs-CN	Molecular self-assembly	Defect engineering	1.78	-0.6	1.18	(1), (2), (3)	HER = 37680 μmol g^-1 h^-1AQE = 34.4% at 400 nm	[7]
Porous P-doped FLCN	Thermal oxidation etching	Heteroatom doping	2.93	-0.83	2.08	(1), (2), (3)	HER = 1590 μmol g^-1 h^-1AQE = 3.65% at 420 nm	[20]
CN-O	Molecular self-assembly Vacuum freeze-drying	Microstructure Mediation, hybrid structures	2.23	N/A	N/A	(1), (2), (3)	HER = 10379 μmol g^-1 h^-1AQE = 29.4% at 400 nm	[26]
BDCN/FLCN	Exfoliation	Hybrid structures, defect engineering, heteroatom doping	2.73	-0.31	2.42	(1), (2), (3)	HER = 658.8 μmol g^-1 h^-1 OER = 328.4 μmol g^-1 h^-1	[27]
Porous FLCN	Molecular self-assembly	Microstructure mediation	2.75	-0.97	1.78	(1), (2)	HER = 79900 μmol g^-1 h^-1 AQE = 9.8% at 400 nm	[30]
Atomically-thin porous CN	Thermal oxidation etching	Defect engineering	2.96	-0.73	1.69	(2), (3)	HER = 1233.5 μmol g^-1 h^-1	[31]
Ultrathin CN nanosheets	Thermal oxidation etching	Microstructure mediation	2.94	-1.17	1.77	(2)	HER = 12016 μmol g^-1 h^-1	[46]
CN seaweed	Vacuum freeze-drying	Microstructure mediation	2.72	N/A	N/A	(2), (3)	HER = 9900 μmol g^-1 h^-1 AQE = 7.8% at 400 nm	[47]
Atomically Thin CN nanomesh	Exfoliation Vacuum freeze-drying	Microstructure mediation	2.75	-1.25	1.50	(1), (2), (3)	HER = 8510 μmol g^-1 h^-1AQE = 5.1% at 420 nm	[52]
3D porous CN	Ball milling	Microstructure mediation	2.49	-0.63	1.86	(2), (3)	HER = 598 μmol g^-1 h^-1 AQE = 3.31% at 420 nm	[53]
FLCN QDs	Ball milling	Microstructure mediation	2.69	-1.55	1.14	(2), (3)	HER = 1365 μmol g^-1 h^-1AQE = 3.6% at 420 nm	[54]
FLCN nanosheets	Thermal oxidation etching	Defect engineering	2.30	-0.77	1.85	(2), (3)	HER = 5375 μmol g^-1 h^-1	[72]
CTHP₃₀	Vacuum freeze-drying	Defect engineering	2.65	-1.2	1.45	(1), (2), (3)	HER = 12723 μmol g^-1 h^-1 AQE = 11.97% at 400 nm OER = 221 μmol g^-1 h^-1	[78]
FLCN/BiVO₄ nanosheets	Exfoliation	Hybrid structures	2.7	-1.15	1.55	(1), (3)	CO₂ reduction into CO rate =5.18 μmol g^-1 h^-1	[80]
BIF-20@CN nanosheets	Exfoliation	Hybrid structures	2.37	-0.72	1.65	(2)	CO₂ reduction into CO rate = 2693 μmol g^-1 h^-1 CO₂ reduction into CH₄ rate = 776 μmol g^-1 h^-1	[89]
TOH-CN	Vacuum freeze-drying	Microstructure mediation, hybrid structures	2.35 1.91	N/A	N/A	(1), (2)	HER = 2027.9 μmol g^-1 h^-1 AQE = 7.9% at 420 nm OER = 142.5 μmol g^-1 h^-1	[96]
CN nanosheets	Exfoliation	Microstructure mediation	2.35	-1.4	0.95	(1), (2)	HER = 3100 μmol g^-1 h^-1	[105]
CN nanosheets	Thermal oxidation etching	Microstructure mediation	2.77	N/A	N/A	(2)	HER = 19000 μmol g^-1 h^-1AQE = 3.65% at 420 nm	[106]
Ultrathin CN nanosheets	Thermal oxidation etching	Microstructure mediation	2.86	N/A	N/A	(2), (3)	HER = 2560 μmol g^-1 h^-1	[107]
C-rich CN nanosheets	Thermal oxidation etching	Defect engineering	2.73	-0.35	2.28	(2), (3)	HER = 3960 μmol g^-1 h^-1	[108]
Ultrathin CN/ MoS₂ nanosheet	Ball milling	Hybrid structures	1.44	-0.34	1.78	(2)	HER = 385.04 μmol g^-1 h^-1	[109]
CN/N-carbon fiber	Vacuum freeze-drying	Microstructure mediation, hybrid structures	2.2	-0.73	1.47	(1), (2), (3)	HER = 16885 μmol g^-1 h^-1 AQE = 14.3% at 420 nm	[110]

Table 1 Summary of the typical FLCN-based photocatalysts for solar fuels and chemicals.

Photocatalyst	Synthesis method	Regulation strategy	Badgap (eV)	CB (eV)	VB (eV)	Performance improvement	Photocatalytic performance	Ref.
I-doped CN nanosheets	Ball milling	Heteroatom doping	2.37	-1.01	1.36	(1), (3)	HER = 890 μmol g^-1 h^-1 AQE = 3.0% at 420 nm	[2]
Ag@FLCN	Exfoliation	Microstructure mediation	2.7	-1.3	1.4	(1), (2), (3)	H₂O₂ yield rate = 1185 μmol g^-1 h^-1	[3]
NVs-CN	Molecular self-assembly	Defect engineering	1.78	-0.6	1.18	(1), (2), (3)	HER = 37680 μmol g^-1 h^-1AQE = 34.4% at 400 nm	[7]
Porous P-doped FLCN	Thermal oxidation etching	Heteroatom doping	2.93	-0.83	2.08	(1), (2), (3)	HER = 1590 μmol g^-1 h^-1AQE = 3.65% at 420 nm	[20]
CN-O	Molecular self-assembly Vacuum freeze-drying	Microstructure Mediation, hybrid structures	2.23	N/A	N/A	(1), (2), (3)	HER = 10379 μmol g^-1 h^-1AQE = 29.4% at 400 nm	[26]
BDCN/FLCN	Exfoliation	Hybrid structures, defect engineering, heteroatom doping	2.73	-0.31	2.42	(1), (2), (3)	HER = 658.8 μmol g^-1 h^-1 OER = 328.4 μmol g^-1 h^-1	[27]
Porous FLCN	Molecular self-assembly	Microstructure mediation	2.75	-0.97	1.78	(1), (2)	HER = 79900 μmol g^-1 h^-1 AQE = 9.8% at 400 nm	[30]
Atomically-thin porous CN	Thermal oxidation etching	Defect engineering	2.96	-0.73	1.69	(2), (3)	HER = 1233.5 μmol g^-1 h^-1	[31]
Ultrathin CN nanosheets	Thermal oxidation etching	Microstructure mediation	2.94	-1.17	1.77	(2)	HER = 12016 μmol g^-1 h^-1	[46]
CN seaweed	Vacuum freeze-drying	Microstructure mediation	2.72	N/A	N/A	(2), (3)	HER = 9900 μmol g^-1 h^-1 AQE = 7.8% at 400 nm	[47]
Atomically Thin CN nanomesh	Exfoliation Vacuum freeze-drying	Microstructure mediation	2.75	-1.25	1.50	(1), (2), (3)	HER = 8510 μmol g^-1 h^-1AQE = 5.1% at 420 nm	[52]
3D porous CN	Ball milling	Microstructure mediation	2.49	-0.63	1.86	(2), (3)	HER = 598 μmol g^-1 h^-1 AQE = 3.31% at 420 nm	[53]
FLCN QDs	Ball milling	Microstructure mediation	2.69	-1.55	1.14	(2), (3)	HER = 1365 μmol g^-1 h^-1AQE = 3.6% at 420 nm	[54]
FLCN nanosheets	Thermal oxidation etching	Defect engineering	2.30	-0.77	1.85	(2), (3)	HER = 5375 μmol g^-1 h^-1	[72]
CTHP₃₀	Vacuum freeze-drying	Defect engineering	2.65	-1.2	1.45	(1), (2), (3)	HER = 12723 μmol g^-1 h^-1 AQE = 11.97% at 400 nm OER = 221 μmol g^-1 h^-1	[78]
FLCN/BiVO₄ nanosheets	Exfoliation	Hybrid structures	2.7	-1.15	1.55	(1), (3)	CO₂ reduction into CO rate =5.18 μmol g^-1 h^-1	[80]
BIF-20@CN nanosheets	Exfoliation	Hybrid structures	2.37	-0.72	1.65	(2)	CO₂ reduction into CO rate = 2693 μmol g^-1 h^-1 CO₂ reduction into CH₄ rate = 776 μmol g^-1 h^-1	[89]
TOH-CN	Vacuum freeze-drying	Microstructure mediation, hybrid structures	2.35 1.91	N/A	N/A	(1), (2)	HER = 2027.9 μmol g^-1 h^-1 AQE = 7.9% at 420 nm OER = 142.5 μmol g^-1 h^-1	[96]
CN nanosheets	Exfoliation	Microstructure mediation	2.35	-1.4	0.95	(1), (2)	HER = 3100 μmol g^-1 h^-1	[105]
CN nanosheets	Thermal oxidation etching	Microstructure mediation	2.77	N/A	N/A	(2)	HER = 19000 μmol g^-1 h^-1AQE = 3.65% at 420 nm	[106]
Ultrathin CN nanosheets	Thermal oxidation etching	Microstructure mediation	2.86	N/A	N/A	(2), (3)	HER = 2560 μmol g^-1 h^-1	[107]
C-rich CN nanosheets	Thermal oxidation etching	Defect engineering	2.73	-0.35	2.28	(2), (3)	HER = 3960 μmol g^-1 h^-1	[108]
Ultrathin CN/ MoS₂ nanosheet	Ball milling	Hybrid structures	1.44	-0.34	1.78	(2)	HER = 385.04 μmol g^-1 h^-1	[109]
CN/N-carbon fiber	Vacuum freeze-drying	Microstructure mediation, hybrid structures	2.2	-0.73	1.47	(1), (2), (3)	HER = 16885 μmol g^-1 h^-1 AQE = 14.3% at 420 nm	[110]

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