g-C3N4表面改性及其光催化制H2与CO2还原研究进展

doi:10.3866/PKU.WHXB202009030

物理化学学报 >> 2021, Vol. 37 >> Issue (6): 2009030.doi: 10.3866/PKU.WHXB202009030

所属专题：先进光催化剂设计与制备

g-C₃N₄表面改性及其光催化制H₂与CO₂还原研究进展

李云锋¹^,*(), 张敏¹, 周亮¹, 杨思佳¹, 武占省¹^,*(), 马玉花²^,*()

¹ 西安工程大学环境与化学工程学院，西安 71004
² 新疆师范大学化学化工学院，乌鲁木齐 830054

收稿日期:2020-09-07 录用日期:2020-10-08 发布日期:2020-10-19
通讯作者: 李云锋,武占省,马玉花 E-mail:liyf377@nenu.edu.cn;wuzhans@126.com;15199141253@163.com
作者简介:Yunfeng Li received his Ph.D. from Northeast Normal University in 2018. He then joined College of Environmental and Chemical Engineering in Xi'an Polytechnic University as Assistant Professor. His research interests focus on environment and energy photocatalysis
Zhansheng Wu, received his Ph.D. from Beijing Institute of Technology in 2011. He then joined School of Environmental and Chemical Engineering in Xi'an Polytechnic University as Professor. His research interests focus on environmental chemical engineering
Yuhua Ma obtained her Ph.D. degree from Xinjiang University in 2017. She then became a lecturer at Xinjiang Normal University. Her main research background lies in the area of nanostructured semiconductor photocatalyst for energy and environmental applications
基金资助:
国家自然科学基金(22008185);国家自然科学基金(52063028);陕西省教育厅科研项目(19JK0376);陕西省自然科学基础研究项目(2019JQ-841);国家级大学生创新创业训练计划项目(S202010709004)

Recent Advances in Surface-Modified g-C₃N₄-Based Photocatalysts for H₂ Production and CO₂ Reduction

Yunfeng Li¹^,*(), Min Zhang¹, Liang Zhou¹, Sijia Yang¹, Zhansheng Wu¹^,*(), Ma Yuhua²^,*()

¹ College of Environmental and Chemical Engineering, Xi'an Polytechnic University, Xi'an 710000, China
² College of Chemistry and Chemical Engineering, Xinjiang Normal University, Urumqi 830054, China

Received:2020-09-07 Accepted:2020-10-08 Published:2020-10-19
Contact: Yunfeng Li,Zhansheng Wu,Ma Yuhua E-mail:liyf377@nenu.edu.cn;wuzhans@126.com;15199141253@163.com
About author:Emails: 15199141253@163.com (Y.M)
Emails: wuzhans@126.com (Z.W)
Emails: liyf377@nenu.edu.cn (Y.L), Tel.: +86-13134451412 (Y.L)
Supported by:
the National Natural Science Foundation of China(22008185);the National Natural Science Foundation of China(52063028);Scientific Research Program Funded by Shaanxi Provincial Education Department(19JK0376);Natural Science Basic Research Program of Shaanxi(2019JQ-841);National Training Program of Innovation and Entrepreneurship for Undergraduates(S202010709004)

摘要/Abstract

摘要：

石墨相氮化碳(g-C₃N₄)作为一种不含金属的有机高分子材料，因独特的能带结构、易于制备以及成本低廉而备受关注。但一些瓶颈问题仍然制约着其光催化活性。截至目前，人们已经尝试了许多方法来优化g-C₃N₄的光电性能，例如：元素掺杂、官能团改性以及构筑异质结等，而这些改性策略均与g-C₃N₄的表面行为密切相关。所以，g-C₃N₄的表面行为对其光催化性能起着关键作用。因此，本文对典型表面改性方法(表面功能化和构建异质结)制备的g-C₃N₄基光催化剂进行了全面综述，阐述了其光激发和响应机制，详细介绍了其可见光照射下光生载流子的转移路线和表面催化反应。此外，本文总结了表面改性g-C₃N₄基光催化剂在光催化制氢与CO₂还原方面的潜在应用。最后，根据已有研究，我们提出了今后有待进一步探索与解决的几方面问题。

关键词: 光催化, 制氢, CO₂还原, 表面改性, 异质结

Abstract:

Solar energy is the largest renewable energy source in the world and the primary energy source of wind energy, tidal energy, biomass energy, and fossil fuel. Photocatalysis technology is a sunlight-driven chemical reaction process on the surface of photocatalysts that can generate H₂ from water, decompose organic contaminants, and reduce CO₂ into organic fuels. As a metal-free polymeric material, graphite-like carbon nitride (g-C₃N₄) has attracted significant attention because of its special band structure, easy fabrication, and low costs. However, some bottlenecks still limit its photocatalytic performance. To date, numerous strategies have been employed to optimize the photoelectric properties of g-C₃N₄, such as element doping, functional group modification, and construction of heterojunctions. Remarkably, these modification strategies are strongly associated with the surface behavior of g-C₃N₄, which plays a key role in efficient photocatalytic performance. In this review, we endeavor to provide a comprehensive summary of g-C₃N₄-based photocatalysts prepared through typical surface modification strategies (surface functionalization and construction of heterojunctions) and elaborate their special light-excitation and response mechanism, photo-generated carrier transfer route, and surface catalytic reaction in detail under visible-light irradiation. Moreover, the potential applications of the surface-modified g-C₃N₄-based photocatalysts for photocatalytic H₂ generation and reduction of CO₂ into fuels are summarized. Finally, based on the current research, the key challenges that should be further studied and overcome are highlighted. The following are the objectives that future studies need to focus on: (1) Although considerable effort has been made to develop a surface modification strategy for g-C₃N₄, its photocatalytic efficiency is still too low to meet industrial application standards. The currently obtained solar-to‑hydrogen (STH) conversion efficiency of g-C₃N₄ for H₂ generation is approximately 2%, which is considerably lower than the commercial standards of 10%. Thus, the regulation of the surface/textural properties and electronic band structure of g-C₃N₄ should be further elucidated to improve its photocatalytic performance. (2) Significant challenges remain in the design and construction of g-C₃N₄-based S-scheme heterojunction photocatalysts by facile, low-cost, and reliable methods. To overcome the limitations of conventional heterojunctions thoroughly, a promising S-scheme heterojunction photocatalytic system was recently reported. The study further clarifies the charge transfer route and mechanism during the catalytic process. Thus, the rational design and synthesis of g-C₃N₄-based S-scheme heterojunctions will attract extensive scientific interest in the next few years in this field. (3) First-principle calculation is an effective strategy to study the optical, electrical, magnetic, and other physicochemical properties of surface strategy modified g-C₃N₄, providing important information to reveal the charge transfer path and intrinsic catalytic mechanism. As a result, density functional theory (DFT) computation will be paid increasing attention and widely applied in surface-modified g-C₃N₄-based photocatalysts.

Key words: Photocatalysis, H₂ generation, CO₂ reduction, Surface modification, Heterojunction

李云锋, 张敏, 周亮, 杨思佳, 武占省, 马玉花. g-C₃N₄表面改性及其光催化制H₂与CO₂还原研究进展[J]. 物理化学学报, 2021, 37(6), 2009030. doi: 10.3866/PKU.WHXB202009030

Yunfeng Li, Min Zhang, Liang Zhou, Sijia Yang, Zhansheng Wu, Ma Yuhua. Recent Advances in Surface-Modified g-C₃N₄-Based Photocatalysts for H₂ Production and CO₂ Reduction[J]. Acta Phys. -Chim. Sin. 2021, 37(6), 2009030. doi: 10.3866/PKU.WHXB202009030

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB202009030

https://www.whxb.pku.edu.cn/CN/Y2021/V37/I6/2009030

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Photocatalysts	Mass of samples	Light source (wavelength)	Cocatalyst	Sacrifice agent	Application	Enhancement factor	Refs.
In₂O₃/g-C₃N₄	20 mg	300 W Xe lamp (λ > 420 nm)	–	TEOA	H₂ evolution	2.3	99
g-C₃N₄/CdS	10 mg	300 W Xe lamp (AM 1.5G)	Pt	TEOA	H₂ evolution	3.3	100
ZnIn₂S₄/g-C₃N₄	50 mg	300 W Xe lamp (λ > 420 nm)	Pt	TEOA	H₂ evolution	11.6	101
CaTiO₃/g-C₃N₄	50 mg	300 W Xe lamp (100 mW∙cm^-2)	–	Methanol	H₂ evolution	19.6	102
InVO₄-g-C₃N₄/rGO	5 mg	Solar light irradiation	–	TEOA	H₂ evolution	45.0	103
CoO/g-C₃N₄	50 mg	LED lamp (λ>400 nm)	–	-	Overall water splitting	243.6	104
ZnS/g-C₃N₄	50 mg	300 W Xe lamp (λ > 420 nm)	–	Na2S/Na2SO3	H₂ evolution	30.0	105
Co₃(PO₄)₂/g-C₃N₄	50 mg	300 W Xe lamp (λ > 400 nm)	–	–	Overall water splitting	74.8	106
UNiMOF/g-C₃N₄	50 mg	300 W Xe lamp (λ > 420 nm)	–	TEOA	H₂ evolution	50.1	107
NiCo₂O₄/g-C₃N₄	50 mg	300 W Xe lamp(AM 1.5G)	Pt	Methanol	H₂ evolution	2.2	108
Ag₂NCN/g-C₃N₄	70 mg	300 W Xe lamp(Simulated sunlight)	–	TEOA	H₂ evolution	117.7	109
MoS₂/g-C₃N₄	10 mg	450 W Xe lamp (AM 1.5G)	MoS₂	Lactic acid	H₂ evolution	9.5	110
Ti₃C₂/g-C₃N₄	20 mg	300 W Xe lamp (λ > 420 nm)	–	–	CO₂reduction	8.1	111
g-C₃N₄/NiAl-LDH	50 mg	300 W Xe lamp (λ > 420 nm)	–	–	CO₂reduction	9.0	112
Bi₄NbO₈Cl/g-C₃N₄	50 mg	300 W Xe lamp (λ > 420 nm)	–	–	CO₂reduction	3.5	113
LaPO₄/g-C₃N₄	30 mg	300 W Xe lamp (λ > 420 nm)	–	–	CO₂reduction	8.1	114
g-C₃N₄@CeO₂	50 mg	300 W Xe lamp (λ > 420 nm)	–	–	CO₂reduction	–	115
CsPbBr₃/g-C₃N₄	8 mg	300 W Xe lamp (λ > 420 nm)	–	–	CO₂reduction	3.0	116

Photocatalysts	Light source(wavelength)	Cocatalyst	Sacrifice agent	Application	System	Enhanced factor	Refs.
Ag₂CrO₄/g-C₃N₄/GO	300 W Xe lamp (λ > 420 nm)	–	–	CO₂ reduction	Z-scheme	2.3	117
CdS/g-C₃N₄	300 W Xe lamp (λ > 420 nm)	Pt	Na₂S/Na₂SO₃	H₂ evolution	Z-scheme	87.5	118
g-C₃N₄/Bi4NbO8Cl	300 W Xe lamp (λ > 420 nm)	Pt	Lactic acid	H₂ evolution	Z-scheme	6.9	119
NiMoO₄/g-C₃N₄	30WDuhalledbulb	–	–	CO₂ reduction	Z-scheme	–	123
Sb₂MoO₆/g-C₃N₄	300 W Xe lamp (λ > 420 nm)	–	Methanol	H₂ evolution	Z-scheme	5.4	124
Co₃O₄/g-C₃N₄	300 W Xe lamp (λ > 400 nm)	Pt	TEOA	H₂ evolution	Z-scheme	9.3	125
ZnO/ZnWO₄/g-C₃N₄	300 W Xe lamp (0.95 mW•cm^-2)	–	–	CO₂ reduction	Z-scheme	3.9	126
SnS₂/g-C₃N₄	300 W Xe lamp (λ > 400 nm)	-	TEOA	H₂ evolution	Z-scheme	2.7	6
α-Fe₂O₃/g-C₃N₄	300 W Xe lamp (λ > 420 nm)	–	–	CO₂ reduction	Z-scheme	3.0	8
WO₃/g-C₃N₄	350 W Xe lamp (Full spectrum)	Pt	Lactic acid	H₂ evolution	S-scheme	1.68	127
g-C₃N₄/g-C₃N₄	300 W Xe lamp (λ > 420 nm)	Pt	TEOA	H₂ evolution	S-scheme	3.1/2.5	130
CuInS₂/g-C₃N₄	350 W Xe lamp (λ > 420 nm)	Pt	Na₂S/Na₂SO₃	H₂ evolution	S-scheme	1.6	135
g-C₃N₄/Zn0.2Cd0.8S	300 W Xe lamp (λ > 420 nm)	Pt	Na₂S/Na₂SO₃	H₂ evolution	S-scheme	16.7	136
CdS/g-C₃N₄	300 W Xe lamp (λ > 420 nm)	–	Na₂S/Na₂SO₃	H₂ evolution	S-scheme	3060.0	137
TiO₂/C₃N₄/Ti₃C₂	350 W Xe lamp (λ > 420 nm)	–	–	CO₂ reduction	S-scheme	3.0/8.0	138

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g-C₃N₄表面改性及其光催化制H₂与CO₂还原研究进展

Recent Advances in Surface-Modified g-C₃N₄-Based Photocatalysts for H₂ Production and CO₂ Reduction

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