少层氮化碳光催化剂合成太阳燃料和高附加值化学品: 现状与展望

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

催化学报 ›› 2022, Vol. 43 ›› Issue (5): 1216-1229.DOI: 10.1016/S1872-2067(21)63985-2

少层氮化碳光催化剂合成太阳燃料和高附加值化学品: 现状与展望

陈方帅^a, 吴崇备^a, 郑耿锋^c(), 曲良体^b(), 韩庆^a()

^a北京理工大学化学与化工学院, 原子分子簇科学教育部重点实验室, 光电转换材料北京市重点实验室, 北京100081
^b清华大学化学系, 有机光电与分子工程教育部重点实验室, 北京100084
^c先进材料实验室, 复旦大学化学与材料学院, 上海市分子催化和功能材料重点实验室, 上海200438

收稿日期:2021-10-01 接受日期:2021-11-24 出版日期:2022-05-18 发布日期:2022-03-23
通讯作者: 郑耿锋,曲良体,韩庆
基金资助:
国家重点研发计划(2018YFA0209401);国家自然科学基金(21905025);国家自然科学基金(22025502);国家自然科学基金(21975051);国家自然科学基金(22175022)

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

Fangshuai Chen^a, Chongbei Wu^a, Gengfeng Zheng^c(), Liangti Qu^b(), Qing Han^a()

^aKey Laboratory of Cluster Science Ministry of Education of China, Key Laboratory of Photoelectronic/Electrophotonic Conversion Materials, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 100081, China
^bKey Laboratory of Organic Optoelectronics & Molecular Engineering of Ministry of Education, Department of Chemistry, Tsinghua University, Beijing 100084, China
^cLaboratory of Advanced Materials, Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Faculty of Chemistry and Materials Science, Fudan University, Shanghai 200438, China

Received:2021-10-01 Accepted:2021-11-24 Online:2022-05-18 Published:2022-03-23
Contact: Gengfeng Zheng, Liangti Qu, Qing Han
Supported by:
National Key Research and Development Program of China(2018YFA0209401);National Natural Science Foundation of China(21905025);National Natural Science Foundation of China(22025502);National Natural Science Foundation of China(21975051);National Natural Science Foundation of China(22175022)

摘要/Abstract

摘要：

将太阳能直接转化为燃料和高附加值化学品是存储可再生能源非常有前景的策略. 少层氮化碳材料因其比表面积大、电荷传输距离短、活性位点暴露多等优点, 在合成太阳燃料和高附加值化学品方面展示出巨大潜力, 而成为光催化领域的研究热点.

本文总结了近年来少层氮化碳基光催化剂的合成、结构调控及其在合成太阳燃料和高附加值化学品领域的研究成果. 首先简要介绍了用于少层氮化碳材料的合成方法, 包括剥离、热氧化刻蚀、真空冷冻干燥、分子自组装、球磨以及化学气相沉积技术, 并讨论了不同方法的优缺点. 其次, 深入分析了少层氮化碳的化学改性(杂原子掺杂、缺陷工程、异质结构)、微结构调控(零维量子点、一维纳米带、二维纳米网片、三维纳米组装体)对其电子结构、光学性质、电荷分离和迁移的影响. 针对不同的改性策略, 分别从光催化反应三个过程(光的捕集、光生电荷分离和迁移及表面催化反应)讨论其对于少层氮化碳基材光催化活性的促进作用以及存在的不足, 涉及的反应包括光催化分解水、CO₂还原、氮气还原合成氨、光合成过氧化氢和光催化有机小分子合成. 最后, 从光催化剂设计、光催化反应体系、反应机理和反应器四个方面讨论了少层氮化碳基光催化剂在合成太阳燃料和高附加值化学品领域面临的挑战和发展前景.

对于催化剂设计, 其表面态决定光催化性能. 目前定量研究催化剂表面缺陷和光催化活性之间的关系是一个巨大的挑战, 未来在精确控制少层氮化碳基光催化剂的表面态方面需要更多的研究工作; 另外, 目前报道的助催化剂大多是大颗粒或者纳米粒子, 未来应将具有高活性的单原子或单活性位点与少层氮化碳结合, 以提高其光催化活性. 对于光催化反应体系, 目前报道的研究工作大部分需要利用使用牺牲剂消耗掉空穴, 以实现高效分解水产氢、CO₂还原、合成氨, 从而导致成本较高. 将原本消耗牺牲剂端的氧化半反应替换为附加值更高的化学品同时产氢、CO₂还原或者N₂还原则可以充分利用光生电子和空穴, 减少浪费. 目前报道的大部分反应机理和反应路径依赖于假设, 缺少确凿的证据, 可以利用先进的原位技术如时间分辨光谱、瞬态和稳态光谱应该用来研究少层氮化碳的激发态载流子动力学和反应中间物种, 进而阐明反应路径. 对于反应器, 目前反应采用的都是罐子反应器, 但存在传质受限和催化剂分离与回收成本问题, 结合工业化需求, 未来可开发流动反应器来解决上述问题. 此外, 大数据、机器学习、人工智能对于繁琐的催化剂筛选以及预测提供了快捷路径, 这将是未来的研究重点.

关键词: 少层氮化碳, 光催化剂, 合成技术, 结构调控, 太阳燃料和化学品

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

陈方帅, 吴崇备, 郑耿锋, 曲良体, 韩庆. 少层氮化碳光催化剂合成太阳燃料和高附加值化学品: 现状与展望[J]. 催化学报, 2022, 43(5): 1216-1229.

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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图/表 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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少层氮化碳光催化剂合成太阳燃料和高附加值化学品: 现状与展望

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

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