光催化制氢研究进展

doi:10.3866/PKU.WHXB201905068

物理化学学报 >> 2020, Vol. 36 >> Issue (3): 1905068.doi: 10.3866/PKU.WHXB201905068

所属专题：光催化剂

光催化制氢研究进展

潘金波¹,申升¹,周威¹,唐杰¹,丁洪志¹,王进博¹,陈浪¹,区泽堂¹,尹双凤^2,*()

¹ 湖南大学化学化工学院，化学/生物传感与化学计量学国家重点实验室，湖南省化石燃料高效利用重点实验室(降低二氧化碳排放)，长沙 410082
² 湖南工程学院化学与化学工程学院，湖南湘潭 411104

收稿日期:2019-05-21 录用日期:2019-07-08 发布日期:2019-07-11
通讯作者: 尹双凤 E-mail:sf_yin@hnu.edu.cn
作者简介:Shuang-Feng Yin obtained his Bachelor Degree in 1996 from Beijing University of Chemical Technology. He subsequently received his Ph.D. from Tsinghua University in 2003. He was promoted to full Professor in Hunan University in 2006. He has been a senior visiting scholar in the Hong Kong Baptist University and Japan Institute of Integrated Industrial Technology from 2008 to 2009. His research interests focus on photocatalytic energy conversion and C―H bond activation
基金资助:
国家自然科学基金(21725602);国家自然科学基金(21476065);国家自然科学基金(21671062);国家自然科学基金(21776064);湖南省创新研究群体(2019JJ10001);湖南省研究生科研创新项目(CX2018B193)

Recent Progress in Photocatalytic Hydrogen Evolution

Jinbo Pan¹,Sheng Shen¹,Wei Zhou¹,Jie Tang¹,Hongzhi Ding¹,Jinbo Wang¹,Lang Chen¹,Chak-Tong Au¹,Shuang-Feng Yin^2,*()

¹ College of Chemistry and Chemical Engineering, State Key Laboratory of Chemo/Biosensing and Chemometrics, Provincial Hunan Key Laboratory for Cost-effective Utilization of Fossil Fuel Aimed at Reducing Carbon-dioxide Emissions, Hunan University, Changsha 410082, P. R. China
² College of Chemistry and Chemical Engineering, Hunan Institute of Engineering, Xiangtan 411104, Hunan Province, P. R. China

Received:2019-05-21 Accepted:2019-07-08 Published:2019-07-11
Contact: Shuang-Feng Yin E-mail:sf_yin@hnu.edu.cn
Supported by:
the National Natural Science Foundation of China(21725602);the National Natural Science Foundation of China(21476065);the National Natural Science Foundation of China(21671062);the National Natural Science Foundation of China(21776064);the Innovative Research Groups of Hunan Province(2019JJ10001);Hunan Provincial Innovation Foundation for Postgraduate(CX2018B193)

摘要/Abstract

摘要：

光催化制氢作为一种具有前景的能源转化方式，受到了广泛关注。但是光催化过程中的三个步骤(光吸收、载流子分离、表面反应)效率较低，目前难以实现工业应用。研究者们对光催化的机理进行了深入研究，并提出了多种策略来调节半导体光催化剂的物理化学性质，以期有效提高光催化剂对可见光的吸收，降低光生载流子的复合，加速表面反应。上述策略包括：制造缺陷、局域表面等离子体共振、元素掺杂、异质结构建、助催化剂负载等。深入研究上述改性策略能够为设计制备高效稳定的光催化剂提供指导。因此，本综述聚焦于优化光吸收、载流子分离、表面反应的机理和改性光催化剂的制氢应用，并对构建高效制氢光催化剂的趋势做出了展望。

关键词: 光催化, 制氢, 光吸收, 载流子分离, 表面反应

Abstract:

The photocatalytic hydrogen evolution reaction (PHER) has gained much attention as a promising strategy for the generation of clean energy. As opposed to conventional hydrogen evolution strategies (steam methane reforming, electrocatalytic hydrogen evolution, etc.), the PHER is an environmentally friendly and sustainable method for converting solar energy into H₂ energy. However, the PHER remains unsuitable for industrial applications because of efficiency losses in three critical steps: light absorption, carrier separation, and surface reaction. In the past four decades, the processes responsible for these efficiency losses have been extensively studied. First, light absorption is the principal factor deciding the performance of most photocatalysts, and it is closely related to band-gap structure of photocatalysts. However, most of the existing photocatalysts have a wide bandgap, indicating a narrow light absorption range, which restricts the photocatalytic efficiency. Therefore, searching for novel semiconductors with a narrow bandgap and broadening the light absorption range of known photocatalysts is an important research direction. Second, only the photogenerated electrons and holes that migrate to the photocatalyst surface can participate in the reaction with H₂O, whereas most of the photogenerated electrons and holes readily recombine with one another in the bulk phase of the photocatalysts. Hence, tremendous effort has been undertaken to shorten the charge transfer distance and enhance the electric conductivity of photocatalysts for improving the separation and transfer efficiency of photogenerated carriers. Third, the surface redox reaction is also an important process. Because water oxidation is a four-electron process, sluggish O₂ evolution is the bottleneck in photocatalytic water splitting. The unreacted holes can easily recombine with electrons. Sacrificial agents are widely used in most catalytic systems to suppress charge carrier recombination by scavenging the photogenerated holes. Moreover, the low H₂ evolution efficiency of most photocatalysts has encouraged researchers to introduce highly active sites on the photocatalyst surface. Based on the abovementioned three steps, multifarious strategies have been applied to modulate the physicochemical properties of semiconductor photocatalysts with the aim of improving the light absorption efficiency, suppressing carrier recombination, and accelerating the kinetics of surface reactions. The strategies include defect generation, localized surface plasmon resonance (LSPR), element doping, heterojunction fabrication, and cocatalyst loading. An in-depth study of these strategies provides guidance for the design of efficient photocatalysts. In this review, we focus on the mechanism and application of these strategies for optimizing light absorption, carrier separation and transport, and surface reactions. Furthermore, we provide a critical view on the promising trends toward the construction of advanced catalysts for H₂ evolution.

Key words: Photocatalysis, Hydrogen evolution, Light absorption, Carriers separation, Surface reaction

MSC2000:

O643

潘金波,申升,周威,唐杰,丁洪志,王进博,陈浪,区泽堂,尹双凤. 光催化制氢研究进展[J]. 物理化学学报, 2020, 36(3): 1905068.

Jinbo Pan,Sheng Shen,Wei Zhou,Jie Tang,Hongzhi Ding,Jinbo Wang,Lang Chen,Chak-Tong Au,Shuang-Feng Yin. Recent Progress in Photocatalytic Hydrogen Evolution[J]. Acta Physico-Chimica Sinica, 2020, 36(3): 1905068.

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Strategy	Photocatalyst	Sacrificial agent	Light source	H₂ evolution rate/(μmol·h⁻¹·g⁻¹)	Ref.
Ov	Vo-γ-Ga₂O₃	CH₃OH	125 W mercury lamp	25600	17
Ov	Vo-TiO₂	–	300 W Xenon lamp, AM 1.5	160	35
Ov/HF	C@TiO₂₋_x/g-C₃N₄	triethanolamine	300 W xenon lamp, λ > 420 nm	417.24	36
Ov/HF	Zn_0.3Cd_0.7S/WO_3–x	Na₂S/Na₂SO₃	300 W xenon lamp, λ > 420 nm	3521	37
LSPR	Ag/g-C₃N₄	triethanolamine	300 W xenon lamp, λ > 420 nm	625	38
LSPR/HF	TiO₂/WO₃/Au	CH₃OH	300 W Xenon lamp	3476.8	39
LSPR/HF	Cu@Cu₂O/ZnO	Na₂S/Na₂SO₃	300 W Xenon lamp	1472.2	40
ED	O-doped C₃N₄	TEOA	300 W xenon lamp, λ > 420 nm	1690	41
ED	F-TiO₂	CH₃OH	300 W xenon lamp, λ > 405 nm	18270	42
ED	P-doped CdS	–	90W LED, λ > 420 nm	231	43
HF	WS₂/CdS	lactic acid	300 W xenon lamp, λ > 420 nm	61100	44
HF	Cu₂O/C₃N₄	TEOA	300 W xenon lamp, λ > 420 nm	241.3	45
HF	α-Fe₂O₃/g-C₃N₄	TEOA	300 W xenon lamp, λ > 400 nm	31400	46
HF	CdS/CdWO₄	Na₂S/Na₂SO₃	300 W xenon lamp, λ > 420 nm	2400	47
CL	Pt/TiO₂ nanotubes	glycerol	Solar light	173.3	48
CL/LSPR	Pt@MIL-125/Au	TEOA	300 W xenon lamp, λ > 380 nm	1743	49
CL	MoS₂/Co-C₃N₄	TEOA	200 W xenon lamp, λ > 400 nm	1990	50
CL	Ni-P/g-C₃N₄	TEOA	350 W xenon lamp	1051	51

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光催化制氢研究进展

Recent Progress in Photocatalytic Hydrogen Evolution

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