光催化产氢双助催化剂: 类别、合成和设计策略

doi:10.1016/S1872-2067(23)64542-5

催化学报 ›› 2023, Vol. 54: 137-160.DOI: 10.1016/S1872-2067(23)64542-5

光催化产氢双助催化剂: 类别、合成和设计策略

伍超^a, 吕康乐^a, 李鑫^b^,^*(), 李覃^a^,^*()

^a中南民族大学, 催化与能源材料化学教育部重点实验室, 催化与材料科学湖北省重点实验室, 国家民委分析化学重点实验室, 湖北武汉430074
^b华南农业大学, 生物质工程研究所, 农业农村部能源植物资源与利用重点实验室, 广东广州510642

收稿日期:2023-08-20 接受日期:2023-09-27 出版日期:2023-11-18 发布日期:2023-11-15
通讯作者: *电子信箱: liqin0518@mail.scuec.edu.cn (李覃), xinli@scau.edu.cn (李鑫).
基金资助:
国家自然科学基金(21972171);中南民族大学中央高校基本研究经费(CZQ23037);湖北省自然科学基金(2021CFA022)

Dual cocatalysts for photocatalytic hydrogen evolution: Categories, synthesis, and design considerations

Chao Wu^a, Kangle Lv^a, Xin Li^b^,^*(), Qin Li^a^,^*()

^aKey Laboratory of Catalysis and Energy Materials Chemistry of Ministry of Education & Hubei Key Laboratory of Catalysis and Materials Science & Key Laboratory of Analytical Chemistry of the State Ethnic Affairs Commission, South-Central Minzu University, Wuhan 430074, Hubei, China
^bInstitute of Biomass Engineering, Key Laboratory of Energy Plants Resource and Utilization, Ministry of Agriculture and Rural Affairs, South China Agricultural University, Guangzhou 510642, Guangdong, China

Received:2023-08-20 Accepted:2023-09-27 Online:2023-11-18 Published:2023-11-15
Contact: *E-mail: liqin0518@mail.scuec.edu.cn (Q. Li), xinli@scau.edu.cn (X. Li).
About author:Xin Li (South China Agricultural University) received his B.S. and Ph.D. degrees in chemical engineering from Zhengzhou University in 2002 and the South China University of Technology in 2007, respectively. Then, he joined the South China Agricultural University as a faculty staff member, and became a professor in 2017. During 2012 and 2019, he worked as a visiting scholar at the Electrochemistry Center, the University of Texas at Austin, and the Department of Chemistry, the University of Utah, respectively. His research interests include photocatalysis, photoelectrochemistry, adsorption, biomass engineering and related materials, and device development (see http://www.researcherid.com/rid/A-2698-2011).
Qin Li (School of Chemistry and Materials Science, South Central Minzu University) received her B.S. in 2009 and Ph.D degree in 2014 from Wuhan University of Technology. She was co-trained as a graduate student in 2010-2011 at the National Nanoscience Center. At the end of 2014, she joined the faculty of School of Chemistry and Materials Science, South Central Minzu University in Wuhan, and became an associate professor in 2020. Over the last 10 years, her research has focused on photocatalytic hydrogen production from water splitting over metal sulfide based composite materials. She has been ranked among the top 100000 scientists in the world in 2022.
Supported by:
National Natural Science Foundation of China(21972171);Fundamental Research Funds for the Central Universities, South- Central MinZu University(CZQ23037);Hubei Provincial Natural Science Foundation, China(2021CFA022)

摘要/Abstract

摘要：

在低碳经济背景下, 开发以氢能为代表的清洁可再生能源至关重要. 利用太阳能驱动半导体进行光催化分解水, 是未来可持续制取氢气的有效方法之一. 然而, 光催化制氢技术产业化受限于半导体表面光生载流子复合效率高和量子效率低. 解决上述问题的办法是在半导体中引入双元助催化剂, 这不仅可以促使三相界面的形成, 促进界面电荷的有效转移, 而且不同种类的双助催化剂可以为半导体提供各自的积极作用, 协同提高光催化产氢效率和稳定性. 因此, 需要密切关注双助催化剂的开发, 以建立一个集优异的光活性和光稳定性于一体的光催化产氢体系.

本文系统地介绍了光催化产氢双助催化剂的类别、优势、合成方法和设计策略. 首先, 双助催化剂被分为双还原型(Red-Red)和还原-氧化型(Red-Ox)两类, 详细概述了在光催化产氢领域中还原型和氧化型助催化剂相互匹配后形成的双助催化剂的实例及其协同效应. 总结了在制氢体系中双助催化剂相对于单一助催化剂的五大优势: 促进载流子快速迁移、实现电子-空穴空间分离、提高产氢吸附/脱附动力学、提高催化剂光稳定性和阻断可逆反应. 随后, 概括了双助催化剂-半导体光催化剂的合成策略, 基于通常报道的水/溶剂热处理、煅烧、光沉积、自组装和化学沉积等助催化剂的合成方法, 可以采用一步法和两步法将两种助催化剂加载到半导体上, 获得三元复合材料. 探讨了双助催化剂-半导体光催化体系的设计策略, 详细总结了如何设计具有优化电子传递路径的Red-Red助催化剂体系和具有空间分离电荷的Red-Ox助催化剂体系. 其中, 为了优化电子传递路径, 两种还原型助催化剂的位置关系可分为三类: 核壳包裹结构、分散分布结构和相邻结构; 为了实现氧化/还原位点空间分离, 氧化-还原型双助催化剂在半导体表面可设计为三种结构: 内外结构、晶面相关结构和端侧结构. 最后, 提出了双助催化剂在光催化制氢领域中的现状、挑战及未来发展方向.

在未来, 可以继续开发新型无贵金属助催化剂来降低催化剂体系总成本, 真正达到经济实用目标; 需要继续发展利于规模化生产的双助催化剂三元复合材料的合成策略; 需要通过实验表征, 结合同位素标记法、分子模拟和密度泛函理论计算, 深入研究助催化剂的性质和作用机理. 希望本文能够为构建高效实用的双助催化剂三元析氢光催化体系提供借鉴.

关键词: 双助催化剂, 异质结, 电荷载流子动力学, 光催化, 产氢

Abstract:

To enable a low-carbon economy, it is vital to develop clean and renewable energy sources such as hydrogen energy. One promising strategy is to sustainably generate H₂ by solar-driven photocatalytic water splitting using semiconductors. However, the bottleneck in the industrialization of photocatalysis technology lies in the high recombination rate of photogenerated charge carriers in the semiconductors. Fortunately, introducing dual cocatalysts into the semiconductor can promote the development of three-phase interfaces that enable the efficient transfer of interfacial charges, thereby enhancing the photocatalytic H₂-evolution efficiency. In this review, we provide a detailed and systematic description of the development of ternary composite photocatalysts with high H₂-evolution efficiencies by loading dual cocatalysts onto semiconductors. First, we categorize dual cocatalysts into two types: dual-reductive pairs and reductive-oxidative pairs, and then summarize four advantages of the dual-cocatalyst-based systems for H₂ production. Subsequently, the synthesis strategies for dual cocatalyst-semiconductor photocatalysts and their design considerations are presented in detail. Finally, the current status, challenges, and future developmental directions of dual cocatalysts for photocatalytic H₂ production are summarized.

Key words: Dual co-catalyst, Heterojunctions, Charge carrier dynamics, Photocatalysis, Hydrogen evolution

伍超, 吕康乐, 李鑫, 李覃. 光催化产氢双助催化剂: 类别、合成和设计策略[J]. 催化学报, 2023, 54: 137-160.

Chao Wu, Kangle Lv, Xin Li, Qin Li. Dual cocatalysts for photocatalytic hydrogen evolution: Categories, synthesis, and design considerations[J]. Chinese Journal of Catalysis, 2023, 54: 137-160.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(23)64542-5

https://www.cjcatal.com/CN/Y2023/V54/I11/137

图/表 31

Fig. 1. Schematic illustration of semiconductor-based photocatalytic H2 evolution.

Fig. 2. Schematic summarizing the content in this review.

Fig. 3. Schematic illustration of the categories of dual cocatalysts for H2 evolution.

Table 1 Summary of the photocatalyst systems with Red-Red cocatalysts for H2 evolution.

Semiconductor	Red (I)-Red (II) cocatalyst	Synthesis strategy		H₂ evolution							Ref. (year)
Semiconductor	Red (I)-Red (II) cocatalyst	Synthesis strategy		Light source	Sacrificial reagent	Mass (mg)	R_H2 (μmol·h^-1·g^-1)	Enhancement factor	AQY (%)	Stability	Ref. (year)
TiO₂	I: Pd	two steps	chemical deposition	<400 nm (Xe)	—	15	602	301	NG	NG	[109] (2015)
TiO₂	II : Pt	two steps	hydrothermal	<400 nm (Xe)	—	15	602	301	NG	NG	[109] (2015)
TiO₂	I: Pd	two steps	chemical deposition	420-780 nm (Xe)	TEOA	15	52	NP	0.2 (530 nm)	20 h	[75] (2019)
TiO₂	II : Au	two steps	chemical deposition	420-780 nm (Xe)	TEOA	15	52	NP	0.2 (530 nm)	20 h	[75] (2019)
TiO₂	I: Ti₃C₂	one step	hydrothermal	UV-Vis (Xe)	Na₂S/Na₂SO₃	25	319	4	NG	30 h	[110] (2021)
TiO₂	II: MoS₂	one step	hydrothermal	UV-Vis (Xe)	Na₂S/Na₂SO₃	25	319	4	NG	30 h	[110] (2021)
TiO₂	I: rGO	one step	impregnation	420-780 nm (Xe)	Methanol	15	0.53	NG	NG	16 h	[66] (2018)
TiO₂	II: Ag	one step	impregnation	420-780 nm (Xe)	Methanol	15	0.53	NG	NG	16 h	[66] (2018)
TiO₂	I: Ti₃C₂	two steps	hydrothermal	AM 1.5 (Xe)	Acetone/TEOA	10	10506	193	7.5 (365 nm)	24 h	[41] (2020)
TiO₂	II: MoS₂	two steps	hydrothermal	AM 1.5 (Xe)	Acetone/TEOA	10	10506	193	7.5 (365 nm)	24 h	[41] (2020)
TiO₂	I: Ti₃C₂	two steps	hydrothermal	AM 1.5 (Xe)	Acetone/TEOA	10	3410	50	2.4 (365 nm)	24 h	[111] (2020)
TiO₂	II: WS₂	two steps	hydrothermal	AM 1.5 (Xe)	Acetone/TEOA	10	3410	50	2.4 (365 nm)	24 h	[111] (2020)
TiO₂	I: Ti₃C₂	two steps	hydrothermal	AM 1.5 (Xe)	Acetone/TEOA	10	9738	132	6.8 (365 nm)	24 h	[61] (2019)
TiO₂	II: MoS₂	two steps	hydrothermal	AM 1.5 (Xe)	Acetone/TEOA	10	9738	132	6.8 (365 nm)	24 h	[61] (2019)
TiO₂	I: Ti₃C₂	two steps	hydrothermal	AM 1.5 (Xe)	Acetone/TEOA	10	6426	87	4.2 (365 nm)	24 h	[29] (2019)
TiO₂	II: MoS₂	two steps	hydrothermal	AM 1.5 (Xe)	Acetone/TEOA	10	6426	87	4.2 (365 nm)	24 h	[29] (2019)
TiO₂	I: Au	two steps	photodeposition	356 nm (LED)	Ethanol	50	9616	291	46 (365 nm)	36 h	[112] (2022)
TiO₂	II: NiS₁₊_x	two steps	photodeposition	356 nm (LED)	Ethanol	50	9616	291	46 (365 nm)	36 h	[112] (2022)
TiO₂	I: N-doped carbon	two steps	photodeposition	AM 1.5 (Xe)	TEOA	10	24800	10	0.8 (365 nm)	50 h	[113] (2020)
TiO₂	II: Au	two steps	calcination	AM 1.5 (Xe)	TEOA	10	24800	10	0.8 (365 nm)	50 h	[113] (2020)
TiO₂	I: Au	one step	chemical deposition	UV-Vis (Xe)	Methanol	50	23666	10	NG	NG	[60] (2015)
TiO₂	II: Pt	one step	chemical deposition	UV-Vis (Xe)	Methanol	50	23666	10	NG	NG	[60] (2015)
TiO₂	I: MoS₂	two steps	hydrothermal	UV(Xe)	Na₂S/Na₂SO₃	20	129	4	NG	NG	[114] (2021)
TiO₂	II: TiN	two steps	calcination	UV(Xe)	Na₂S/Na₂SO₃	20	129	4	NG	NG	[114] (2021)
TiO₂	I: rGO	two steps	impregnation	365 nm (LED)	Methanol	50	207	30	5.9 (365 nm)	20 h	[98] (2018)
TiO₂	II: MoS_x	two steps	photodeposition	365 nm (LED)	Methanol	50	207	30	5.9 (365 nm)	20 h	[98] (2018)
TiO₂	I: Ag	two steps	photodeposition	365 nm (LED)	Methanol	50	2380	52	9.8 (365 nm)	NG	[115] (2018)
TiO₂	II: Ag₂S	two steps	chemical deposition	365 nm (LED)	Methanol	50	2380	52	9.8 (365 nm)	NG	[115] (2018)
TiO₂	I: Au nanorod	two steps	ultrasonication	≥420 nm (Xe)	TEOA	20	9115	NG	9.1 (420 nm)	20 h	[116] (2019)
g-C₃N₄	II: Pt	two steps	photodeposition	≥420 nm (Xe)	TEOA	20	9115	NG	9.1 (420 nm)	20 h	[116] (2019)
CdS	I: Ni	one step	ultrasonication	≥420 nm (Xe)	TEOA	10	5900	4	NG	NG	[117] (2020)
CdS	II: graphene	one step	ultrasonication	≥420 nm (Xe)	TEOA	10	5900	4	NG	NG	[117] (2020)
CdS	I: Au	two steps	chemical deposition	≥400 nm (Xe)	Na₂S/Na₂SO₃	50	16350	112	41 (420 nm)	20 h	[64] (2020)
CdS	II: PdS	two steps	chemical deposition	≥400 nm (Xe)	Na₂S/Na₂SO₃	50	16350	112	41 (420 nm)	20 h	[64] (2020)
CdS	I: NiS₂	two steps	impregnation	≥420 nm (Xe)	Na₂S/Na₂SO₃	50	3334	5	NG	12 h	[118] (2017)
CdS	II: carbon black	two steps	ultrasonication	≥420 nm (Xe)	Na₂S/Na₂SO₃	50	3334	5	NG	12 h	[118] (2017)
CdS	I: MoS₂	One step	ultrasonication	AM 1.5	LA	1	168930	67	NG	25 h	[119] (2021)
CdS	II: SeS₂	One step	ultrasonication	AM 1.5	LA	1	168930	67	NG	25 h	[119] (2021)
CdS	I: MoS₂	two steps	hydrothermal	≥420 nm (Xe)	LA	100	2525	13	NG	18 h	[120] (2019)
	II: NiS		hydrothermal
	II: Co_1.4Ni_0.6P		chemical deposition
g-C₃N₄	I: acetylene black	two steps	ultrasonication	≥420 nm (Xe)	TEOA	50	240	320	NG	12 h		[121] (2016)
g-C₃N₄	II: Ni(OH)₂	two steps	chemical deposition	≥420 nm (Xe)	TEOA	50	240	320	NG	12 h		[121] (2016)
g-C₃N₄	I: Ni	two steps	calcination	≥420 nm (Xe)	TEOA	50	515	406	NG	12 h		[84] (2017)
g-C₃N₄	II: NiS	two steps	impregnation	≥420 nm (Xe)	TEOA	50	515	406	NG	12 h		[84] (2017)
g-C₃N₄	I: Ti₃C₂	two steps	impregnation	AM 1.5	TEOA	30	5100	15	3.1 (420 nm)	6 h		[122] (2018)
g-C₃N₄	II: Pt	two steps	photodeposition	AM 1.5	TEOA	30	5100	15	3.1 (420 nm)	6 h		[122] (2018)
g-C₃N₄	I: NiS	one step	ultrasonication	UV-Vis (Xe)	TEOA	10	6893	41	NG	NG		[123] (2022)
g-C₃N₄	II: Ni₂P	one step	ultrasonication	UV-Vis (Xe)	TEOA	10	6893	41	NG	NG		[123] (2022)
g-C₃N₄	I: Au	two steps	photodeposition	≥420 nm (Xe)	TEOA	80	239	NG	NG	35 h		[124] (2015)
g-C₃N₄	II: Pt	two steps	photodeposition	≥420 nm (Xe)	TEOA	80	239	NG	NG	35 h		[124] (2015)
g-C₃N₄	I: Ni₃C	two steps	ultrasonication	≥420 nm (Xe)	TEOA	10	1128	NG	1.5 (420 nm)	12 h		[125] (2021)
g-C₃N₄	II: Ni	two steps	calcination	≥420 nm (Xe)	TEOA	10	1128	NG	1.5 (420 nm)	12 h		[125] (2021)
g-C₃N₄	I: Carbon black	two steps	ultrasonication	≥420 nm (Xe)	TEOA	50	405	810	NG	12 h		[100] (2019)
g-C₃N₄	II: Co_1.4Ni_0.6P	two steps	chemical deposition	≥420 nm (Xe)	TEOA	50	405	810	NG	12 h		[100] (2019)
ZnIn₂S₄	I: Au	one step	self-assembly	≥420 nm (Xe)	Na₂S/Na₂SO₃	10	4175	10	6.2 (420 nm)	20 h		[65] (2021)
ZnIn₂S₄	II: Pt	one step	self-assembly	≥420 nm (Xe)	Na₂S/Na₂SO₃	10	4175	10	6.2 (420 nm)	20 h		[65] (2021)
ZnIn₂S₄	I: WN-QDs	one step	hydrothermal	≥400 nm (Xe)	LA	20	196	61	NP	NP		[126] (2021)
ZnIn₂S₄	II: Graphene	one step	hydrothermal	≥400 nm (Xe)	LA	20	196	61	NP	NP		[126] (2021)
Zn_0.5Cd_0.5S	I: rGO	one step	photodeposition	≥420 nm (Xe)	LA	30	77000	82	NP	50 h		[68] (2016)
Zn_0.5Cd_0.5S	II: MoS₂	one step	photodeposition	≥420 nm (Xe)	LA	30	77000	82	NP	50 h		[68] (2016)
Mn_0.5Cd_0.5S	I: rGO	one step	hydrothermal	≥420 nm (Xe)	Na₂S/Na₂SO₃	50	12843	4	36.4 (420 nm)	16 h		[69] (2020)
Mn_0.5Cd_0.5S	II: MoS₂	one step	hydrothermal	≥420 nm (Xe)	Na₂S/Na₂SO₃	50	12843	4	36.4 (420 nm)	16 h		[69] (2020)
CuSe	I: Au	two steps	chemical deposition	≥420 nm (Xe)	Na₂S/Na₂SO₃	50	4180	44	0.6 (600 nm)	24 h		[127] (2020)
CuSe	Ⅱ: Pt	two steps	chemical deposition	≥420 nm (Xe)	Na₂S/Na₂SO₃	50	4180	44	0.6 (600 nm)	24 h		[127] (2020)
Nb₂O₅	I: Nb₂CT_x	two steps	hydrothermal	UV-Vis (Xe)	Methanol	20	682	NG	1.6 (313 nm)	15 h		[73] (2021)
Nb₂O₅	II: Ag	two steps	photodeposition	UV-Vis (Xe)	Methanol	20	682	NG	1.6 (313 nm)	15 h		[73] (2021)
SiC	I: Au	two steps	photodeposition	≥420 nm (Xe)	Na₂S/Na₂SO₃	30	100	NG	2.2 (420 nm)	25 h		[128] (2022)
SiC	II: Pt	two steps	photodeposition	≥420 nm (Xe)	Na₂S/Na₂SO₃	30	100	NG	2.2 (420 nm)	25 h		[128] (2022)

Table 1 Summary of the photocatalyst systems with Red-Red cocatalysts for H2 evolution.

Semiconductor	Red (I)-Red (II) cocatalyst	Synthesis strategy		H₂ evolution							Ref. (year)
Semiconductor	Red (I)-Red (II) cocatalyst	Synthesis strategy		Light source	Sacrificial reagent	Mass (mg)	R_H2 (μmol·h^-1·g^-1)	Enhancement factor	AQY (%)	Stability	Ref. (year)
TiO₂	I: Pd	two steps	chemical deposition	<400 nm (Xe)	—	15	602	301	NG	NG	[109] (2015)
TiO₂	II : Pt	two steps	hydrothermal	<400 nm (Xe)	—	15	602	301	NG	NG	[109] (2015)
TiO₂	I: Pd	two steps	chemical deposition	420-780 nm (Xe)	TEOA	15	52	NP	0.2 (530 nm)	20 h	[75] (2019)
TiO₂	II : Au	two steps	chemical deposition	420-780 nm (Xe)	TEOA	15	52	NP	0.2 (530 nm)	20 h	[75] (2019)
TiO₂	I: Ti₃C₂	one step	hydrothermal	UV-Vis (Xe)	Na₂S/Na₂SO₃	25	319	4	NG	30 h	[110] (2021)
TiO₂	II: MoS₂	one step	hydrothermal	UV-Vis (Xe)	Na₂S/Na₂SO₃	25	319	4	NG	30 h	[110] (2021)
TiO₂	I: rGO	one step	impregnation	420-780 nm (Xe)	Methanol	15	0.53	NG	NG	16 h	[66] (2018)
TiO₂	II: Ag	one step	impregnation	420-780 nm (Xe)	Methanol	15	0.53	NG	NG	16 h	[66] (2018)
TiO₂	I: Ti₃C₂	two steps	hydrothermal	AM 1.5 (Xe)	Acetone/TEOA	10	10506	193	7.5 (365 nm)	24 h	[41] (2020)
TiO₂	II: MoS₂	two steps	hydrothermal	AM 1.5 (Xe)	Acetone/TEOA	10	10506	193	7.5 (365 nm)	24 h	[41] (2020)
TiO₂	I: Ti₃C₂	two steps	hydrothermal	AM 1.5 (Xe)	Acetone/TEOA	10	3410	50	2.4 (365 nm)	24 h	[111] (2020)
TiO₂	II: WS₂	two steps	hydrothermal	AM 1.5 (Xe)	Acetone/TEOA	10	3410	50	2.4 (365 nm)	24 h	[111] (2020)
TiO₂	I: Ti₃C₂	two steps	hydrothermal	AM 1.5 (Xe)	Acetone/TEOA	10	9738	132	6.8 (365 nm)	24 h	[61] (2019)
TiO₂	II: MoS₂	two steps	hydrothermal	AM 1.5 (Xe)	Acetone/TEOA	10	9738	132	6.8 (365 nm)	24 h	[61] (2019)
TiO₂	I: Ti₃C₂	two steps	hydrothermal	AM 1.5 (Xe)	Acetone/TEOA	10	6426	87	4.2 (365 nm)	24 h	[29] (2019)
TiO₂	II: MoS₂	two steps	hydrothermal	AM 1.5 (Xe)	Acetone/TEOA	10	6426	87	4.2 (365 nm)	24 h	[29] (2019)
TiO₂	I: Au	two steps	photodeposition	356 nm (LED)	Ethanol	50	9616	291	46 (365 nm)	36 h	[112] (2022)
TiO₂	II: NiS₁₊_x	two steps	photodeposition	356 nm (LED)	Ethanol	50	9616	291	46 (365 nm)	36 h	[112] (2022)
TiO₂	I: N-doped carbon	two steps	photodeposition	AM 1.5 (Xe)	TEOA	10	24800	10	0.8 (365 nm)	50 h	[113] (2020)
TiO₂	II: Au	two steps	calcination	AM 1.5 (Xe)	TEOA	10	24800	10	0.8 (365 nm)	50 h	[113] (2020)
TiO₂	I: Au	one step	chemical deposition	UV-Vis (Xe)	Methanol	50	23666	10	NG	NG	[60] (2015)
TiO₂	II: Pt	one step	chemical deposition	UV-Vis (Xe)	Methanol	50	23666	10	NG	NG	[60] (2015)
TiO₂	I: MoS₂	two steps	hydrothermal	UV(Xe)	Na₂S/Na₂SO₃	20	129	4	NG	NG	[114] (2021)
TiO₂	II: TiN	two steps	calcination	UV(Xe)	Na₂S/Na₂SO₃	20	129	4	NG	NG	[114] (2021)
TiO₂	I: rGO	two steps	impregnation	365 nm (LED)	Methanol	50	207	30	5.9 (365 nm)	20 h	[98] (2018)
TiO₂	II: MoS_x	two steps	photodeposition	365 nm (LED)	Methanol	50	207	30	5.9 (365 nm)	20 h	[98] (2018)
TiO₂	I: Ag	two steps	photodeposition	365 nm (LED)	Methanol	50	2380	52	9.8 (365 nm)	NG	[115] (2018)
TiO₂	II: Ag₂S	two steps	chemical deposition	365 nm (LED)	Methanol	50	2380	52	9.8 (365 nm)	NG	[115] (2018)
TiO₂	I: Au nanorod	two steps	ultrasonication	≥420 nm (Xe)	TEOA	20	9115	NG	9.1 (420 nm)	20 h	[116] (2019)
g-C₃N₄	II: Pt	two steps	photodeposition	≥420 nm (Xe)	TEOA	20	9115	NG	9.1 (420 nm)	20 h	[116] (2019)
CdS	I: Ni	one step	ultrasonication	≥420 nm (Xe)	TEOA	10	5900	4	NG	NG	[117] (2020)
CdS	II: graphene	one step	ultrasonication	≥420 nm (Xe)	TEOA	10	5900	4	NG	NG	[117] (2020)
CdS	I: Au	two steps	chemical deposition	≥400 nm (Xe)	Na₂S/Na₂SO₃	50	16350	112	41 (420 nm)	20 h	[64] (2020)
CdS	II: PdS	two steps	chemical deposition	≥400 nm (Xe)	Na₂S/Na₂SO₃	50	16350	112	41 (420 nm)	20 h	[64] (2020)
CdS	I: NiS₂	two steps	impregnation	≥420 nm (Xe)	Na₂S/Na₂SO₃	50	3334	5	NG	12 h	[118] (2017)
CdS	II: carbon black	two steps	ultrasonication	≥420 nm (Xe)	Na₂S/Na₂SO₃	50	3334	5	NG	12 h	[118] (2017)
CdS	I: MoS₂	One step	ultrasonication	AM 1.5	LA	1	168930	67	NG	25 h	[119] (2021)
CdS	II: SeS₂	One step	ultrasonication	AM 1.5	LA	1	168930	67	NG	25 h	[119] (2021)
CdS	I: MoS₂	two steps	hydrothermal	≥420 nm (Xe)	LA	100	2525	13	NG	18 h	[120] (2019)
	II: NiS		hydrothermal
	II: Co_1.4Ni_0.6P		chemical deposition
g-C₃N₄	I: acetylene black	two steps	ultrasonication	≥420 nm (Xe)	TEOA	50	240	320	NG	12 h		[121] (2016)
g-C₃N₄	II: Ni(OH)₂	two steps	chemical deposition	≥420 nm (Xe)	TEOA	50	240	320	NG	12 h		[121] (2016)
g-C₃N₄	I: Ni	two steps	calcination	≥420 nm (Xe)	TEOA	50	515	406	NG	12 h		[84] (2017)
g-C₃N₄	II: NiS	two steps	impregnation	≥420 nm (Xe)	TEOA	50	515	406	NG	12 h		[84] (2017)
g-C₃N₄	I: Ti₃C₂	two steps	impregnation	AM 1.5	TEOA	30	5100	15	3.1 (420 nm)	6 h		[122] (2018)
g-C₃N₄	II: Pt	two steps	photodeposition	AM 1.5	TEOA	30	5100	15	3.1 (420 nm)	6 h		[122] (2018)
g-C₃N₄	I: NiS	one step	ultrasonication	UV-Vis (Xe)	TEOA	10	6893	41	NG	NG		[123] (2022)
g-C₃N₄	II: Ni₂P	one step	ultrasonication	UV-Vis (Xe)	TEOA	10	6893	41	NG	NG		[123] (2022)
g-C₃N₄	I: Au	two steps	photodeposition	≥420 nm (Xe)	TEOA	80	239	NG	NG	35 h		[124] (2015)
g-C₃N₄	II: Pt	two steps	photodeposition	≥420 nm (Xe)	TEOA	80	239	NG	NG	35 h		[124] (2015)
g-C₃N₄	I: Ni₃C	two steps	ultrasonication	≥420 nm (Xe)	TEOA	10	1128	NG	1.5 (420 nm)	12 h		[125] (2021)
g-C₃N₄	II: Ni	two steps	calcination	≥420 nm (Xe)	TEOA	10	1128	NG	1.5 (420 nm)	12 h		[125] (2021)
g-C₃N₄	I: Carbon black	two steps	ultrasonication	≥420 nm (Xe)	TEOA	50	405	810	NG	12 h		[100] (2019)
g-C₃N₄	II: Co_1.4Ni_0.6P	two steps	chemical deposition	≥420 nm (Xe)	TEOA	50	405	810	NG	12 h		[100] (2019)
ZnIn₂S₄	I: Au	one step	self-assembly	≥420 nm (Xe)	Na₂S/Na₂SO₃	10	4175	10	6.2 (420 nm)	20 h		[65] (2021)
ZnIn₂S₄	II: Pt	one step	self-assembly	≥420 nm (Xe)	Na₂S/Na₂SO₃	10	4175	10	6.2 (420 nm)	20 h		[65] (2021)
ZnIn₂S₄	I: WN-QDs	one step	hydrothermal	≥400 nm (Xe)	LA	20	196	61	NP	NP		[126] (2021)
ZnIn₂S₄	II: Graphene	one step	hydrothermal	≥400 nm (Xe)	LA	20	196	61	NP	NP		[126] (2021)
Zn_0.5Cd_0.5S	I: rGO	one step	photodeposition	≥420 nm (Xe)	LA	30	77000	82	NP	50 h		[68] (2016)
Zn_0.5Cd_0.5S	II: MoS₂	one step	photodeposition	≥420 nm (Xe)	LA	30	77000	82	NP	50 h		[68] (2016)
Mn_0.5Cd_0.5S	I: rGO	one step	hydrothermal	≥420 nm (Xe)	Na₂S/Na₂SO₃	50	12843	4	36.4 (420 nm)	16 h		[69] (2020)
Mn_0.5Cd_0.5S	II: MoS₂	one step	hydrothermal	≥420 nm (Xe)	Na₂S/Na₂SO₃	50	12843	4	36.4 (420 nm)	16 h		[69] (2020)
CuSe	I: Au	two steps	chemical deposition	≥420 nm (Xe)	Na₂S/Na₂SO₃	50	4180	44	0.6 (600 nm)	24 h		[127] (2020)
CuSe	Ⅱ: Pt	two steps	chemical deposition	≥420 nm (Xe)	Na₂S/Na₂SO₃	50	4180	44	0.6 (600 nm)	24 h		[127] (2020)
Nb₂O₅	I: Nb₂CT_x	two steps	hydrothermal	UV-Vis (Xe)	Methanol	20	682	NG	1.6 (313 nm)	15 h		[73] (2021)
Nb₂O₅	II: Ag	two steps	photodeposition	UV-Vis (Xe)	Methanol	20	682	NG	1.6 (313 nm)	15 h		[73] (2021)
SiC	I: Au	two steps	photodeposition	≥420 nm (Xe)	Na₂S/Na₂SO₃	30	100	NG	2.2 (420 nm)	25 h		[128] (2022)
SiC	II: Pt	two steps	photodeposition	≥420 nm (Xe)	Na₂S/Na₂SO₃	30	100	NG	2.2 (420 nm)	25 h		[128] (2022)

Table 2 Summary of photocatalyst systems with Red-Ox cocatalysts for H2 evolution.

Semiconductor	Red (I)-Ox (II) cocatalysts	Synthesis strategy		H₂ evolution								Ref. (year)
Semiconductor	Red (I)-Ox (II) cocatalysts	Synthesis strategy		Light source	Sacrificial reagent	Mass (mg)	R_H2 (μmol h^-1 g^-1)		Enhancement factor	AQY (%)	Stability	Ref. (year)
TiO₂	I: Pt	two steps	chemical deposition	365 nm (LED)	methanol	50	4200		42	NG	NG	[129] (2016)
TiO₂	II: RuO₂	two steps	calcination	365 nm (LED)	methanol	50	4200		42	NG	NG	[129] (2016)
TiO₂	I: Pd	two steps	impregnation	UV-Vis (Xe)	methanol	100	7740		NG	NG	NG	[108] (2014)
TiO₂	II: IrO_x	two steps	photodeposition	UV-Vis (Xe)	methanol	100	7740		NG	NG	NG	[108] (2014)
TiO₂	I: Pt	two steps	photodeposition	UV-Vis (Xe)	methanol	50	5280		NG	11.3 (365 nm)	9 h	[130] (2016)
TiO₂	II: Co₃O₄	two steps	photodeposition	UV-Vis (Xe)	methanol	50	5280		NG	11.3 (365 nm)	9 h	[130] (2016)
TiO₂	I: Cu	two steps	photodeposition	AM 1.5	methanol	20	764		NG	NG	25 h	[131] (2018)
TiO₂	II: Ti₃C₂T_x	two steps	hydrothermal	AM 1.5	methanol	20	764		NG	NG	25 h	[131] (2018)
TiO₂	I: Pt	two steps	photodeposition	AM 1.5	methanol	10	45357		187	NG	NG	[132] (2020)
TiO₂	II: PdO_x	two steps	calcination	AM 1.5	methanol	10	45357		187	NG	NG	[132] (2020)
TiO₂	I: CuO	one step	ball-milling	UV-Vis (Xe)	methanol	20	14300		NG	NG	NG	[86] (2017)
TiO₂	II: Co₃O₄	one step	ball-milling	UV-Vis (Xe)	methanol	20	14300		NG	NG	NG	[86] (2017)
TiO₂	I: Pt	two steps	AL deposition	UV (Xe)	methanol	35	5518		5	NG	NG	[133] (2017)
TiO₂	II: Au	two steps	calcination	UV (Xe)	methanol	35	5518		5	NG	NG	[133] (2017)
CdS	I: rGO	two steps	calcination	≥420 nm (Xe)	Na₂S/Na₂SO₃	50	5450		7	2.4 (420 nm)	16 h	[134] (2019)
CdS	II: MnO_x	two steps	self-assembly	≥420 nm (Xe)	Na₂S/Na₂SO₃	50	5450		7	2.4 (420 nm)	16 h	[134] (2019)
CdS	I: MoS₂	one step	calcination	400-800 nm (Xe)	LA	20	1200		8	11.3 (420 nm)	12 h	[135] (2022)
CdS	II: Ni(OH)₂	one step	calcination	400-800 nm (Xe)	LA	20	1200		8	11.3 (420 nm)	12 h	[135] (2022)
CdS	I: MoS₂	two steps	photodeposition	≥420 nm (Xe)	TEOA	20	7400		6	7.6 (420 nm)	NP	[136] (2022)
CdS	II: CoO_x	two steps	photodeposition	≥420 nm (Xe)	TEOA	20	7400		6	7.6 (420 nm)	NP	[136] (2022)
CdS	I: MoS₂	two steps	photodeposition	≥420 nm (Xe)	LA	20	40500		27	36 (420 nm)	20 h	[137] (2019)
CdS	II: Co-Pi	two steps	photodeposition	≥420 nm (Xe)	LA	20	40500		27	36 (420 nm)	20 h	[137] (2019)
CdS	I: MoS₂	two steps	hydrothermal	AM 1.5	—	100	52		NG	0.3 (365 nm)	25 h	[83] (2020)
CdS	II: RuO₂	two steps	hydrothermal	AM 1.5	—	100	52		NG	0.3 (365 nm)	25 h	[83] (2020)
CdS	I: carbon dots	two steps	ultrasonication	≥420 nm (Xe)	Na₂S/Na₂SO₃	100	1444		5	NG	15 h	[105] (2018)
CdS	II: NiS	two steps	hydrothermal	≥420 nm (Xe)	Na₂S/Na₂SO₃	100	1444		5	NG	15 h	[105] (2018)
CdS	I: MoS₂	two steps	chemical deposition	≥420 nm (Xe)	LA	20	14888		7	NG	12 h	[138] (2023)
CdS	II: Ti₃C₂	two steps	hydrothermal	≥420 nm (Xe)	LA	20	14888		7	NG	12 h	[138] (2023)
CdS	I: Ni(II)	two steps	impregnation	≥420 nm (Xe)	Na₂S/Na₂SO₃	50	3438		2	NG	20 h	[139] (2016)
CdS	II: PdS	two steps	chemical deposition	≥420 nm (Xe)	Na₂S/Na₂SO₃	50	3438		2	NG	20 h	[139] (2016)
P-doped CdS	I: Ag₂S	two steps	photodeposition	≥420 nm (Xe)	LA	20	4828		45	49.5 (420 nm)	12 h	[10] (2021)
P-doped CdS	Ⅱ: NiS	two steps	hydrothermal	≥420 nm (Xe)	LA	20	4828		45	49.5 (420 nm)	12 h	[10] (2021)
CdSe	I: Pt	two steps	photodeposition	≥420 nm (Xe)	Na₂S/Na₂SO₃	100	5300		20	45 (420 nm)	16 h	[103] (2019)
CdSe	II: CoO_x	two steps	photodeposition	≥420 nm (Xe)	Na₂S/Na₂SO₃	100	5300		20	45 (420 nm)	16 h	[103] (2019)
g-C₃N₄	I: Au	two steps	impregnation	≥420 nm (Xe)	methanol	50	1533		12	8.61 (420 nm)	20 h	[140] (2021)
g-C₃N₄	II: CoO_x	two steps	calcination	≥420 nm (Xe)	methanol	50	1533		12	8.61 (420 nm)	20 h	[140] (2021)
g-C₃N₄	I: MoS₂	two steps	hydrothermal	UV-Vis (Xe)	methanol	20	3400	366		6.4 (420 nm)	30 h	[67] (2020)
g-C₃N₄	II: Ni(OH)₂	two steps	chemical deposition	UV-Vis (Xe)	methanol	20	3400	366		6.4 (420 nm)	30 h	[67] (2020)
Zn_0.5Cd_0.5S	I: Pt	two steps	photodeposition	≥420 nm (Xe)	Na₂S/Na₂SO₃	10	7300	36		89.0 (420 nm)	16 h	[141] (2020)
Zn_0.5Cd_0.5S	II: PdS	two steps	photodeposition	≥420 nm (Xe)	Na₂S/Na₂SO₃	10	7300	36		89.0 (420 nm)	16 h	[141] (2020)
Mn_0.5Cd_0.5S	I: MoS₂	two steps	chemical deposition	≥420 nm (Xe)	Na₂S/Na₂SO₃	50	1375	22		16.1 (420 nm)	12 h	[142] (2018)
Mn_0.5Cd_0.5S	II: Cu_2-_xS	two steps	photodeposition	≥420 nm (Xe)	Na₂S/Na₂SO₃	50	1375	22		16.1 (420 nm)	12 h	[142] (2018)
ZnCdS	I: graphene QDs	two steps	hydrothermal	≥420 nm (Xe)	Na₂S/Na₂SO₃	50	10340	15		22.4 (420 nm)	25 h	[143] (2018)
ZnCdS	II: PdS	two steps	chemical deposition	≥420 nm (Xe)	Na₂S/Na₂SO₃	50	10340	15		22.4 (420 nm)	25 h	[143] (2018)
La₂Ti₂O₇	I: rGO	two steps	hydrothermal	AM 1.5	TEOA	20	532	9		NG	NG	[144] (2018)
La₂Ti₂O₇	II: NiFe-LDH	two steps	self-assembly	AM 1.5	TEOA	20	532	9		NG	NG	[144] (2018)
PbTiO₃	I: Pt	two steps	photodeposition	UV-Vis (Xe)	TEOA	100	350	NG		NG	NG	[145] (2014)
PbTiO₃	II: MnO_x	two steps	photodeposition	UV-Vis (Xe)	TEOA	100	350	NG		NG	NG	[145] (2014)

Table 2 Summary of photocatalyst systems with Red-Ox cocatalysts for H2 evolution.

Semiconductor	Red (I)-Ox (II) cocatalysts	Synthesis strategy		H₂ evolution								Ref. (year)
Semiconductor	Red (I)-Ox (II) cocatalysts	Synthesis strategy		Light source	Sacrificial reagent	Mass (mg)	R_H2 (μmol h^-1 g^-1)		Enhancement factor	AQY (%)	Stability	Ref. (year)
TiO₂	I: Pt	two steps	chemical deposition	365 nm (LED)	methanol	50	4200		42	NG	NG	[129] (2016)
TiO₂	II: RuO₂	two steps	calcination	365 nm (LED)	methanol	50	4200		42	NG	NG	[129] (2016)
TiO₂	I: Pd	two steps	impregnation	UV-Vis (Xe)	methanol	100	7740		NG	NG	NG	[108] (2014)
TiO₂	II: IrO_x	two steps	photodeposition	UV-Vis (Xe)	methanol	100	7740		NG	NG	NG	[108] (2014)
TiO₂	I: Pt	two steps	photodeposition	UV-Vis (Xe)	methanol	50	5280		NG	11.3 (365 nm)	9 h	[130] (2016)
TiO₂	II: Co₃O₄	two steps	photodeposition	UV-Vis (Xe)	methanol	50	5280		NG	11.3 (365 nm)	9 h	[130] (2016)
TiO₂	I: Cu	two steps	photodeposition	AM 1.5	methanol	20	764		NG	NG	25 h	[131] (2018)
TiO₂	II: Ti₃C₂T_x	two steps	hydrothermal	AM 1.5	methanol	20	764		NG	NG	25 h	[131] (2018)
TiO₂	I: Pt	two steps	photodeposition	AM 1.5	methanol	10	45357		187	NG	NG	[132] (2020)
TiO₂	II: PdO_x	two steps	calcination	AM 1.5	methanol	10	45357		187	NG	NG	[132] (2020)
TiO₂	I: CuO	one step	ball-milling	UV-Vis (Xe)	methanol	20	14300		NG	NG	NG	[86] (2017)
TiO₂	II: Co₃O₄	one step	ball-milling	UV-Vis (Xe)	methanol	20	14300		NG	NG	NG	[86] (2017)
TiO₂	I: Pt	two steps	AL deposition	UV (Xe)	methanol	35	5518		5	NG	NG	[133] (2017)
TiO₂	II: Au	two steps	calcination	UV (Xe)	methanol	35	5518		5	NG	NG	[133] (2017)
CdS	I: rGO	two steps	calcination	≥420 nm (Xe)	Na₂S/Na₂SO₃	50	5450		7	2.4 (420 nm)	16 h	[134] (2019)
CdS	II: MnO_x	two steps	self-assembly	≥420 nm (Xe)	Na₂S/Na₂SO₃	50	5450		7	2.4 (420 nm)	16 h	[134] (2019)
CdS	I: MoS₂	one step	calcination	400-800 nm (Xe)	LA	20	1200		8	11.3 (420 nm)	12 h	[135] (2022)
CdS	II: Ni(OH)₂	one step	calcination	400-800 nm (Xe)	LA	20	1200		8	11.3 (420 nm)	12 h	[135] (2022)
CdS	I: MoS₂	two steps	photodeposition	≥420 nm (Xe)	TEOA	20	7400		6	7.6 (420 nm)	NP	[136] (2022)
CdS	II: CoO_x	two steps	photodeposition	≥420 nm (Xe)	TEOA	20	7400		6	7.6 (420 nm)	NP	[136] (2022)
CdS	I: MoS₂	two steps	photodeposition	≥420 nm (Xe)	LA	20	40500		27	36 (420 nm)	20 h	[137] (2019)
CdS	II: Co-Pi	two steps	photodeposition	≥420 nm (Xe)	LA	20	40500		27	36 (420 nm)	20 h	[137] (2019)
CdS	I: MoS₂	two steps	hydrothermal	AM 1.5	—	100	52		NG	0.3 (365 nm)	25 h	[83] (2020)
CdS	II: RuO₂	two steps	hydrothermal	AM 1.5	—	100	52		NG	0.3 (365 nm)	25 h	[83] (2020)
CdS	I: carbon dots	two steps	ultrasonication	≥420 nm (Xe)	Na₂S/Na₂SO₃	100	1444		5	NG	15 h	[105] (2018)
CdS	II: NiS	two steps	hydrothermal	≥420 nm (Xe)	Na₂S/Na₂SO₃	100	1444		5	NG	15 h	[105] (2018)
CdS	I: MoS₂	two steps	chemical deposition	≥420 nm (Xe)	LA	20	14888		7	NG	12 h	[138] (2023)
CdS	II: Ti₃C₂	two steps	hydrothermal	≥420 nm (Xe)	LA	20	14888		7	NG	12 h	[138] (2023)
CdS	I: Ni(II)	two steps	impregnation	≥420 nm (Xe)	Na₂S/Na₂SO₃	50	3438		2	NG	20 h	[139] (2016)
CdS	II: PdS	two steps	chemical deposition	≥420 nm (Xe)	Na₂S/Na₂SO₃	50	3438		2	NG	20 h	[139] (2016)
P-doped CdS	I: Ag₂S	two steps	photodeposition	≥420 nm (Xe)	LA	20	4828		45	49.5 (420 nm)	12 h	[10] (2021)
P-doped CdS	Ⅱ: NiS	two steps	hydrothermal	≥420 nm (Xe)	LA	20	4828		45	49.5 (420 nm)	12 h	[10] (2021)
CdSe	I: Pt	two steps	photodeposition	≥420 nm (Xe)	Na₂S/Na₂SO₃	100	5300		20	45 (420 nm)	16 h	[103] (2019)
CdSe	II: CoO_x	two steps	photodeposition	≥420 nm (Xe)	Na₂S/Na₂SO₃	100	5300		20	45 (420 nm)	16 h	[103] (2019)
g-C₃N₄	I: Au	two steps	impregnation	≥420 nm (Xe)	methanol	50	1533		12	8.61 (420 nm)	20 h	[140] (2021)
g-C₃N₄	II: CoO_x	two steps	calcination	≥420 nm (Xe)	methanol	50	1533		12	8.61 (420 nm)	20 h	[140] (2021)
g-C₃N₄	I: MoS₂	two steps	hydrothermal	UV-Vis (Xe)	methanol	20	3400	366		6.4 (420 nm)	30 h	[67] (2020)
g-C₃N₄	II: Ni(OH)₂	two steps	chemical deposition	UV-Vis (Xe)	methanol	20	3400	366		6.4 (420 nm)	30 h	[67] (2020)
Zn_0.5Cd_0.5S	I: Pt	two steps	photodeposition	≥420 nm (Xe)	Na₂S/Na₂SO₃	10	7300	36		89.0 (420 nm)	16 h	[141] (2020)
Zn_0.5Cd_0.5S	II: PdS	two steps	photodeposition	≥420 nm (Xe)	Na₂S/Na₂SO₃	10	7300	36		89.0 (420 nm)	16 h	[141] (2020)
Mn_0.5Cd_0.5S	I: MoS₂	two steps	chemical deposition	≥420 nm (Xe)	Na₂S/Na₂SO₃	50	1375	22		16.1 (420 nm)	12 h	[142] (2018)
Mn_0.5Cd_0.5S	II: Cu_2-_xS	two steps	photodeposition	≥420 nm (Xe)	Na₂S/Na₂SO₃	50	1375	22		16.1 (420 nm)	12 h	[142] (2018)
ZnCdS	I: graphene QDs	two steps	hydrothermal	≥420 nm (Xe)	Na₂S/Na₂SO₃	50	10340	15		22.4 (420 nm)	25 h	[143] (2018)
ZnCdS	II: PdS	two steps	chemical deposition	≥420 nm (Xe)	Na₂S/Na₂SO₃	50	10340	15		22.4 (420 nm)	25 h	[143] (2018)
La₂Ti₂O₇	I: rGO	two steps	hydrothermal	AM 1.5	TEOA	20	532	9		NG	NG	[144] (2018)
La₂Ti₂O₇	II: NiFe-LDH	two steps	self-assembly	AM 1.5	TEOA	20	532	9		NG	NG	[144] (2018)
PbTiO₃	I: Pt	two steps	photodeposition	UV-Vis (Xe)	TEOA	100	350	NG		NG	NG	[145] (2014)
PbTiO₃	II: MnO_x	two steps	photodeposition	UV-Vis (Xe)	TEOA	100	350	NG		NG	NG	[145] (2014)

Fig. 4. TEM (inset: partial enlargement) (a), HRTEM (b), and HAADF-STEM (c) images and corresponding EDS maps of Au and Pt for the Pt/Au NR769/CNNT650 sample. Photocatalytic H2 evolution rates of CNNT650 deposited with different Pt and/or Au NRs under visible-light irradiation (d) and >590 nm irradiation (e). (f) Photocatalytic mechanism of Pt/Au NR769/CNNT650 with LSPR enhancement. Reprinted with permission from Ref. [116]. Copyright 2019, John Wiley and Sons.

Fig. 5. (a) Schematic illustration of Au-induced self-redox deposition formation of core-shell Au@MoS2+x-loaded TiO2 photocatalysts. (b) Production mechanism of Au@MoS2+x. TEM (c) and HRTEM (d) images of TiO2/Au@MoS2+x. (e,f) Schematic diagrams of the enhanced interfacial transfer of photogenerated electrons on the Au@MoS2+x cocatalyst that enables fast photocatalytic H2 evolution. Reprinted with permission from Ref. [163]. Copyright 2023, John Wiley and Sons.

Fig. 6. TEM (a) and HR-TEM (b) images of a typical ZCS@MoS2/rGO. (c) Schematic diagram of ZCS@MoS2/rGO under solar light irradiation. Reprinted with permission from Ref. [68]. Copyright 2016, American Chemical Society.

Fig. 7. TEM image (a), HRTEM image (b), and Corresponding SAED pattern (c) of PdOx@TiO2@Pt. (d-i) EDS maps of PdOx@TiO2@Pt, where the (e) shows the overlaid images of Ti, O, Pd, and Pt. (j) Schematic illustration of the photocatalytic H2-evolution mechanism over the MOx@TiO2@Pt photocatalyst. Reprinted with permission from Ref. [132]. Copyright 2020, American Chemical Society.

Fig. 8. Schematic representation of the five advantages of dual cocatalysts for H2 evolution.

Fig. 9. Time-dependent amount (a) and average rate (b) of photocatalytic H2 production over different photocatalysts. Proposed photocatalytic H2 production mechanisms over g-C3N4-1.0%NiS (c), g-C3N4-0.5%Ni (d), and ternary g-C3N4-Ni-NiS (e) composites under visible-light irradiation. Reprinted with permission from Ref. [84]. Copyright 2017, American Chemical Society.

Fig. 10. (a) Comparison of the H2-production rate of Au/CuSe/Pt, Au/CuSe, and Pt/CuSe hybrids. (b) Normalized ΔI probed at 560 and 900 nm for Au, Au/CuSe, and Au/CuSe/Pt. (c) Schematic diagrams of the possible electron-transfer processes in the Au/CuSe/Pt tangential hybrid during the photocatalytic HER. Reprinted with permission from Ref. [127]. Copyright 2020, John Wiley and Sons.

Fig. 11. (a) Comparison of the HER performance of g-C3N4 and g-C3N4-MoS2 with and without M(OH)x, where A is g-C3N4-Ni(OH)2, B is g-C3N4-Co(OH)2, and C is g-C3N4-Fe(OH)3. (b) TRPL spectra of pristine g-C3N4, g-C3N4-MoS2, and its heterostructures with M(OH)x. (c) Schematic illustration of photo-excited charge-carrier separation and the photocatalytic reaction of the ternary g-C3N4-MoS2-Ni(OH)2 photocatalyst. Reprinted with permission from Ref. [67]. Copyright 2020, RSC Pub.

Fig. 12. (a) Calculated Gibbs free energy diagram of the HER on different sites of WO3/C3N4@C. (b) Linear sweep voltammetry plots of ZnIn2S4 and 2 wt% WO3/C3N4@C/ZnIn2S4 in 0.2 mol L-1 Na2SO4 solution measured at a scan rate of 50 mV s-1. (c) Temperature dependence of the reaction rate of ZnIn2S4 and 2 wt% WO3/C3N4@C/ZnIn2S4. (d) Schematic diagram of the Ea difference between ZnIn2S4 and 2 wt% WO3/C3N4@C/ZnIn2S4. Reprinted with permission from Ref. [126]. Copyright 2021, Elsevier.

Fig. 13. (a) Cycling activity results for CdS, CdS@Ti3C2, and CdS@MoS2/Ti3C2. (b) Time-dependent photocatalytic H2 production profile of CdS@MoS2/Ti3C2. (c) Photographs of initial H2-production solutions containing CdS, CdS@Ti3C2, and CdS@MoS2/Ti3C2 and those after 4 h of illumination. (d) Proposed mechanism of charge transfer over ternary CdS@MoS2/Ti3C2 photocatalysts during the photocatalytic HER, where lactic acid (LA) was used as the sacrificial agent. Reprinted with permission from Ref. [138]. Copyright 2023, Elsevier.

Fig. 15. (a) Schematic of the preparation of Ti3C2-TiO2-MoS2 catalysts. SEM images of Ti3C2 (b) and Ti3C2-TiO2-MoS2 (c) samples. (d) EDS map of Ti3C2-TiO2-MoS2. Reprinted with permission from Ref. [110]. Copyright 2021, John Wiley and Sons.

Fig. 16. (a) Schematic representation for the formation process of Au@Pt/ZIS. (b,c) TEM image of Au16@Pt/ZIS. (d) STEM-HAADF images and EDS maps of Au16@Pt NPs. Reprinted with permission from Ref. [65]. Copyright 2021, Elsevier.

Fig. 17. (a) Schematic of the preparation of CdS@MoS2/Ti3C2 composites. TEM images ofTi3C2 (b) and MoS2/Ti3C2 (c). TEM (d) and HRTEM (e) images of CdS@MoS2/Ti3C2. Reprinted with permission from Ref. [138]. Copyright 2023, Elsevier.

Fig. 18. (a) Schematic diagram of the preparation of CdS@MoS2@Co-Pi composite photocatalysts. (b) Typical TEM image of as-prepared blank CdS NWs. (c,d) Typical TEM images of CdS@MoS2@Co-Pi composite. Reprinted with permission from Ref. [137]. Copyright 2019, American Chemical Society.

Fig. 21. Three configurations of dual reductive cocatalyst-semiconductor systems with optimal electron-transport paths: core-shell (a), dispersed (b), and the adjacent (c) structures.

Fig. 22. (a) TEM and HRTEM images of CN08-2. (b) Schematic of Ni3C@Ni/g-C3N4 photocatalysts. (c) Average H2-evolution rate over g-C3N4-8-Ni3C, CN08-0.5, CN08-1, CN08-2, CN08-3, and g-C3N4-1Pt systems. (d) Schematic of the photo-induced charge separation process in the Ni3C/g-C3N4 composite photocatalysts. Reprinted with permission from Ref. [125]. Copyright 2021, Elsevier.

Fig. 23. Fig. 23. TEM (a,b) and HRTEM (c) images of a TiO2/Ag-Ag2S photocatalyst. (d) The energy-band structures of TiO2, Ag and Ag2S. (e) Schematic diagram illustrating the photocatalytic H2-evolution mechanism of TiO2/Ag-Ag2S. Reprinted with permission from Ref. [115]. Copyright 2018, Elsevier.

Fig. 24. (a) HAADF-STEM images and corresponding EDS maps of Au/Pd-TiO2. Average H2 production rates of TiO2-based photocatalysts (15 mg) under broad-spectrum irradiation (b) and schematics of the corresponding charge kinetics (c). Reprinted with permission from Ref. [75]. Copyright 2019, John Wiley and Sons.

Fig. 25. Three configurations of oxidative and reductive co-catalyst-semiconductor systems promoting spatial segregation of electron-hole pairs: internal-external distribution using hollow structures (a), crystallographically determined distributions based on different facet types (b), and tip-side distribution using nanorods (c).

Fig. 26. (a) Architecture of PdS@CdS@MoS2. (b) HAADF-STEM image of a quarter of a PdS@CdS@MoS2 nanosphere and the corresponding EDS maps. (c) Cross-sectional view of a chloroplast structure. (d) Diagrams of photoinduced charge carrier migration on a PdS@CdS@MoS2 hollow sphere. Reprinted with permission from Ref. [184]. Copyright 2022, John Wiley and Sons.

Fig. 27. (a) TEM images of TiO2-Co3O4-Pt samples. (b) Schematics of selective deposition of Pt and Co3O4 on {101} and {001} crystal surfaces of TiO2, respectively, and the related hydrogen production mechanism of TiO2-Co3O4-Pt. Reprinted with permission from Ref. [130]. Copyright 2016, Elsevier. (c,d) SEM images of Pt/{001}PbTiO3 and MnOx/{001}PbTiO3 (insets show corresponding structural schematics. (e) Schematic of the process of loading redox cocatalysts on single-domain ferroelectric crystals where A is the electron acceptor and D is the electron donor. Reprinted with permission from Ref. [145]. Copyright 2014, Royal Society of Chemistry.

Fig. 28. (a) Schematic of SrTiO3 nanocrystals changing from a 6-facet to 18-facet structure. (b) Morphology of 6-facet SrTiO3 nanocrystals. (c) Morphology of 18-facet SrTiO3 nanocrystals. SEM images of 18-facet and 6-facet SrTiO3 nanocrystals with simultaneous photodeposition of Pt and Co3O4 as cocatalysts: Pt-Co3O4/18-facet SrTiO3 (d) and Pt-Co3O4/6-facet SrTiO3 (e). Reprinted with permission from Ref. [188]. Copyright 2016, RSC Publishing.

Fig. 29. TEM images of (RuO2/CdS)@MoS2 (a) and RuO2/CdS/MoS2 (b,c). (d) Hydrogen and oxygen production under illumination over time. (e) Schematic of charge-transfer routes. Reprinted with permission from Ref. [83]. Copyright 2020, John Wiley and Sons.

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光催化产氢双助催化剂: 类别、合成和设计策略

Dual cocatalysts for photocatalytic hydrogen evolution: Categories, synthesis, and design considerations

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