双通道氧化还原反应用于光催化析氢耦合废弃物光重整氧化

doi:10.1016/S1872-2067(24)60118-X

催化学报 ›› 2024, Vol. 65: 1-39.DOI: 10.1016/S1872-2067(24)60118-X

• 综述 • 下一篇

双通道氧化还原反应用于光催化析氢耦合废弃物光重整氧化

刘欢^a^,¹, 何少雄^b^,¹, 曲家福^a, 蔡亚辉^c, 杨晓刚^a, 李长明^a^,^*(), 胡俊蝶^a^,^b^,^*()

^a苏州科技大学材料科学与工程学院, 江苏苏州215009, 中国
^b新加坡国立大学化学与生物分子工程系, 新加坡
^c南京林业大学材料科学与工程学院, 江苏南京210037, 中国

收稿日期:2024-06-03 接受日期:2024-08-19 出版日期:2024-10-18 发布日期:2024-10-15
通讯作者: *电子信箱: ecmli@swu.edu.cn (李长明), hjd@usts.edu.cn (胡俊蝶).
作者简介:¹共同第一作者.
基金资助:
江苏省自然科学基金项目(BK20231342);江苏省自然科学基金项目(BK20210867);国家自然科学基金项目(22008163);能源与环境光催化国家重点实验室开放项目(SKLPEE-KF202309);江苏省高校自然科学研究项目(21KJB150038)

Dual-channel redox reactions for photocatalytic H₂-evolution coupled with photoreforming oxidation of waste materials

Huan Liu^a^,¹, Shaoxiong He^b^,¹, Jiafu Qu^a, Yahui Cai^c, Xiaogang Yang^a, Chang Ming Li^a^,^*(), Jundie Hu^a^,^b^,^*()

^aSchool of Materials Science and Engineering, Suzhou University of Science and Technology, Suzhou 215009, Jiangsu, China
^bDepartment of Chemical and Biomolecular Engineering, National University of Singapore, Singapore 117585, Singapore
^cCollege of Materials Science and Engineering, Nanjing Forestry University, Nanjing 210037, Jiangsu, China

Received:2024-06-03 Accepted:2024-08-19 Online:2024-10-18 Published:2024-10-15
Contact: *E-mail: ecmli@swu.edu.cn (C. M. Li), hjd@usts.edu.cn (J. Hu).
About author:Chang Ming Li (School of Materials Science and Engineering, Suzhou University of Science and Technology) received his B.S. degree from University of Science and Technology of China in 1970, and Ph.D. degree from Wuhan University in 1987. He worked at Nanyang Technological University (from 2003 to 2012) and Southwest University (from 2012 to 2016). Since 2017, he has been working in Suzhou University of Science and Technology. His research interests mainly focus on cross-field sciences including functional nanomaterials and green energies. He has published 800 more peer-reviewed journal papers and H-index of 107 as well as 240 patents. He is the Chief Editor of Mater. Rep.: Energy.
Jundie Hu (School of Materials Science and Engineering, Suzhou University of Science and Technology) received her Ph.D degree in 2019 from Soochow University. In June 2019, she joined the School of Materials Science and Engineering, Suzhou University of Science and Technology. Since March 2024, she has been a visiting scholar (1 year) at the Department of Chemical and Biomolecular Engineering, National University of Singapore. Her research interests currently focus on the applications of nanomaterials in photocatalysis, including water splitting, carbon dioxide conversion, plastic recycling and upcycling, environmental remediation, etc. She has published more than 70 peer-reviewed papers. She was invited as a Community Board member of Nanoscale Horiz. Science 2020, and became a young member of the editorial board of Mater. Rep.: Energy Since 2024.
¹ Contributed equally to this work.
Supported by:
Natural Science Foundation of Jiangsu Province(BK20231342);Natural Science Foundation of Jiangsu Province(BK20210867);National Natural Science Foundation of China(22008163);Open Project Program of the State Key Laboratory of Photocatalysis on Energy and Environment(SKLPEE-KF202309);Natural Science Research Project of Higher Education Institutions in Jiangsu Province(21KJB150038)

摘要/Abstract

摘要：

双通道氧化还原系统在光催化析氢耦合废弃物光重整氧化方面展现出热力学和动力学上的双重优势. 然而, 现有综述聚焦于某些特定的氧化反应, 例如有机合成､水修复等, 往往忽视了塑料升级､生物质转化和过氧化氢生产方面的最新进展, 也缺乏对催化机制的深入探讨. 本综述通过全面概述双通道光催化制氢耦合高价值废弃物光重整氧化的最新进展来弥补这些空白. 重点介绍“变废为宝”的设计理念, 强调双通道光催化反应的挑战､优势和各类应用, 包括生物质､酒精､胺类､塑料废物､有机污染物的光重整, 以及过氧化氢的生产. 本文重点讨论改进策略和催化机制探索, 包括先进的原位表征､自旋捕获实验和密度泛函理论计算 (DFT). 通过对该领域的挑战和未来发展方向的分析, 本文旨在为设计创新的双通道光催化系统提供有价值的见解.

本文系统介绍了双通道光催化制氢耦合高值氧化反应的最新研究进展, 包括生物质转化､醇转化､胺转化､塑料废物光重整､废水中有机污染物降解和过氧化氢生产. 首先概述了光催化制氢的基本知识, 分析了水分解过程中遇到的挑战, 如析氧反应动力学缓慢､电荷重组快速､逆反应和对牺牲剂的依赖, 强调了双通道光催化反应系统的优势, 如抑制电荷重组､消除牺牲剂､高效利用光生载流子. 重点讨论双通道光催化反应的各种应用, 及提高反应效率的策略, 如氧化还原中心的空间分离､调整电子结构､构筑内建电场､发挥协同催化效应. 最后, 本文指出了该领域的挑战和未来发展方向: (1)生物质和废塑料等有机基质的成分复杂, 往往导致光催化转换效率较低; (2)反应过程中, 通过调节氧化物种类型和控制氧化途径, 可以提高产物的选择性和光催化反应效率; (3)优化反应条件和光催化系统防止有机底物的过度氧化; (4)采用先进表征技术和DFT理论计算深入探究催化协同机制和复杂的氧化过程; (5)实现产物有效分离, 促进该双通道反应体系的实际工业化应用; (6)借助双通道反应体系在热力学和动力学上的双重优势减少能量消耗､降低工业应用成本.

综上, 本文总结了空间分离的双通道光催化析氢耦合废弃物光重整氧化的研究进展, 旨在为创新双通道光催化系统的设计提供有见地的参考.

关键词: 光催化, 双通道, 析氢, 光重整氧化, 原位表征

Abstract:

Dual-channel redox reaction system is advantageous for photocatalytic hydrogen (H₂) production when coupled with photoreforming oxidation of waste materials, benefiting both thermodynamically and kinetically. However, existing reviews primarily focus on specific oxidation reactions, such as oxidative organic synthesis and water remediation, often neglecting recent advancements in plastic upgrading, biomass conversion, and H₂O₂ production, and failing to provide an in-depth discussion of catalytic mechanisms. This review addresses these gaps by offering a comprehensive overview of recent advancements in dual-channel redox reactions for photocatalytic H₂-evolution and waste photoreforming. It highlights waste-to-wealth design concepts, examines the challenges, advantages and diverse applications of dual-channel photocatalytic reactions, including photoreforming of biomass, alcohol, amine, plastic waste, organic pollutants, and H₂O₂ production. Emphasizing improvement strategies and exploration of catalytic mechanisms, it includes advanced in-situ characterization, spin capture experiments, and DFT calculations. By identifying challenges and future directions in this field, this review provides valuable insights for designing innovative dual-channel photocatalytic systems.

Key words: Photocatalysis, Dual-channel, Hydrogen evolution, Photoreforming oxidation, In situ characterization

刘欢, 何少雄, 曲家福, 蔡亚辉, 杨晓刚, 李长明, 胡俊蝶. 双通道氧化还原反应用于光催化析氢耦合废弃物光重整氧化[J]. 催化学报, 2024, 65: 1-39.

Huan Liu, Shaoxiong He, Jiafu Qu, Yahui Cai, Xiaogang Yang, Chang Ming Li, Jundie Hu. Dual-channel redox reactions for photocatalytic H₂-evolution coupled with photoreforming oxidation of waste materials[J]. Chinese Journal of Catalysis, 2024, 65: 1-39.

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图/表 33

Fig. 1. Important milestones in the development of dual-channel photocatalytic H2-evolution coupled with high-value oxidation reactions.

Fig. 2. Overview of recent advances of dual-channel photocatalytic H2-evolution coupled high-value oxidation reactions.

Fig. 3. Schematic depicting the evolutionary journey of water splitting photocatalysts for H2 evolution. (a) Reprinted with permission from Ref. [35]. Copyright 2022, Elsevier. (b) Reprinted with permission from Ref. [26]. Copyright 2008, Springer Nature. (c) Reprinted with permission from Ref. [36]. Copyright 2024, John Wiley and Sons. (d) Reprinted with permission from Ref. [28]. Copyright 2014, Royal Society of Chemistry. (e) Reprinted with permission from Ref. [29]. Copyright 2015, Royal Society of Chemistry. (f) Reprinted with permission from Ref. [30]. Copyright 2018, John Wiley and Sons. (g) Reprinted with permission from Ref. [31]. Copyright 2019, Elsevier. (h) Reprinted with permission from Ref. [32]. Copyright 2021, Springer Nature. (i) Reprinted with permission from Ref. [33]. Copyright 2022, Springer Nature. (j) Reprinted with permission from Ref. [34]. Copyright 2023, Springer Nature.

Fig. 4. Photocatalytic mechanism of water splitting for H2-evolution on semiconductors.

Fig. 5. Challenges of photocatalytic water splitting for H2-evolution.

Fig. 6. Advantages of dual-channel photocatalytic H2-evolution coupled high-value oxidation reactions.

Fig. 7. Schematic diagram of dual-channel photocatalytic H2-evolution coupled high-value oxidation reactions.

Table 1 Recent research advancements in photocatalytic H2-evolution coupled with biomass conversion.

No.	Photocatalyst	Substrate	Oxidation product	H₂ yield (μmol g^-1 h^-1)	Oxidation product yield (μmol g^-1 h^-1)	Light source	Ref.
1	TiO₂-NiO	lignin	fatty acid	23500	30	Xe lamp	[45]
2	h-ZnSe/Pt@TiO₂	cellulose	HCOOH	1858	372	Xe lamp	[46]
3	0.2-NiS/CdS	lactic acid, lignin	ethanol formic acid oxalic acid	1512.4	—	Xe lamp	[47]
4	Zn_0.3Cd_0.7S	glucose	lactic acid	13640	76.8	Xe lamp	[48]
5	CQDs/TiO₂	glucose	arabinose glycolic acid	2430	—	Xe lamp	[49]
6	O-ZIS-120	HMF	DFF	1522	1624	Xe lamp	[50]
7	Znln₂S₄/Nb₂O₅	HMF	DFF	1286	—	Xe lamp λ > 420 nm	[51]
8	Pt-SGCN	HMF	DFF	1200	130	LED > 420 nm	[52]
9	UCNT	HMF	DFF	92	950	Xe lamp λ ≥ 420 nm	[12]
10	Zn_0.5Cd_0.5S-P	HMF	DFF	419	—	LED (30 × 3 W)	[53]
11	CoP/ZCS	HMF	DFF	2440	1610	Xe lamp	[54]
12	NiS/Ni-CdS	ethanol	acetaldehyde	7980	7330	Xe lamp	[55]
13	CdS/MoO₂/MoS₂	lactic acid	pyruvic acid	9600	—	Xe lamp λ > 420 nm	[56]

Fig. 8. (a) Diagram of photocatalytic cellulose reforming on h-ZnSe/Pt@TiO2. Reprinted with permission from Ref. [46]. Copyright 2023, John Wiley and Sons. (b) Diagram of photocatalytic lignocellulosic oxidation on PtSA-CdS. Reprinted with permission from Ref. [57]. Copyright 2024, John Wiley and Sons. (c) Reaction mechanism of glucose photoreforming. Reprinted with permission from Ref. [49]. Copyright 2021, Elsevier. (d) Mechanism of photocatalytic oxidation of HMF. Reprinted with permission from Ref. [52]. Copyright 2013, Royal Society of Chemistry (e) Photocatalytic performance in H2 evolution and HMF oxidation. (f) Photocatalytic HMF conversion on CoP/ZCS. Reprinted with permission from Ref. [54]. Copyright 2022, American Chemical Society.

Table 2 Recent research advancements in photocatalytic H2-evolution coupled with alcohol conversion.

No.	Photocatalyst	Substrate	Oxidation products	H₂ yield (μmol g^-1 h^-1)	Oxidation product yield (μmol g^-1 h^-1)	Light source	Ref.
1	MoS₂/ZIS	FA	FAL	2752	2832	Xe lamp λ > 420 nm	[59]
2	Ti₃C₂T_x/CdS	FA	FAL	193.25	194.25	Xe lamp λ > 420 nm	[60]
3	LaVO₄/g-C₃N₄	FA	FAL	1440	950	Xe lamp 250 mW cm^-2	[61]
4	ZnIn₂S₄/Tp-Tta COF	FA	FAL	9730	12100	Xe lamp λ ≥ 350 nm	[62]
5	CoTiO₃/Zn_0.5Cd_0.5S	FA	FAL	1929	3197.12	White LEDs λ ≥ 420 nm	[63]
6	ZCS/Pt	FA	FAL	1045	807.6	Xe lamp	[64]
7	ReS₂/ZIS	FA	FAL	3092.90	710	LED λ > 420 nm	[65]
8	Ti₃C₂T_x/g-C₃N₄	FA	FAL	1170	1220	Xe lamp	[66]
9	ReS₂/ZnIn₂S₄-S_v	FA	FAL	1080	710	Xe lamp	[67]
10	Pt-g-C₃N₄	BA	BAD	2856.7	198.28	Xe lamp λ > 420 nm	[68]
11	CdS/BiVO₄	BA	BAD	4558	4396	Xe lamp λ > 420 nm	[69]
12	CN/BP@Ni	BA	BAD	8590	9390	LED lamp	[70]
13	VC/CdS	BA	BAD	20500	71280	Xe lamp λ = 420 nm	[71]
14	CdS(ZB)/CdS (WZ)/Ni-BTC	BA	BAD	2891	—	Xe lamp λ > 420 nm	[72]
15	CdS/MIL-53(Fe)	BA	BAD	2334	2825	Xe lamp λ > 420 nm	[73]
16	Ru_SA-RuO₂/TiO₂	BA	BAD	2910	1420	Xe lamp	[74]
17	CIZS/NiPcCDs	BA	BAD	4100	—	Xe lamp	[11]
18	NiS/CdS	BA	BAD	10390	8190	Xe lamp	[75]
19	SCNHMS	BA	BAD	3760	3870	Xe lamp	[76]

Fig. 9. (a) Transient photocurrent signals. Reprinted with permission from Ref. [64]. Copyright 2021, John Wiley and Sons. (b) Yield of H2 evolution coupled with FA oxidation. (c) Proposed reaction mechanism for FA conversion and H2 evolution over MoS2-ZIS. Reprinted with permission from Ref. [59]. Copyright 2021, Elsevier. (d) Schematic diagram of photocatalysis mechanism on TC/CN. (e) Electron density distribution on TC/CN. (f) Free energy profiles of FAL oxidation. Reprinted with permission from Ref. [66]. Copyright 2023, Royal Society of Chemistry. (g) Schematic illustration for photocatalytic H2 evolution coupled with FA production on LaVO4/CN. Reprinted with permission from Ref. [61]. Copyright 2021, Elsevier. (h) Schematic diagram of synthesis route of ReS2/ZnIn2S4-Sv heterojunction. Reprinted with permission from Ref. [67]. Copyright 2022, Elsevier.

Fig. 10. (a) Synthesis of RuSA-RuO2/TiO2. Reprinted with permission from Ref. [74]. Copyright 2023, Elsevier. (b) Schematic diagram of the ternary CIZS/NiPc-CDs composite. (c) Comparison of H2 production rates. Reprinted with permission from Ref. [11]. Copyright 2023, John Wiley and Sons. (d) 1H NMR spectra of the solvent. Reprinted with permission from Ref. [75]. Copyright 2021, Elsevier. (e) Mechanism of photocatalyzed alcohol oxidation. Reprinted with permission from Ref. [72]. Copyright 2021, Elsevier.

Table 3 Recent research advancements in photocatalytic H2-evolution coupled with amine conversion.

No.	Photocatalyst	Oxidation product	H₂ evolution (μmol g^-1 h^-1)	Oxidation product yield (μmol g^-1 h^-1)	Light source	Ref.
1	Pd_SA+C/TiO₂-V_O	NBLL	585.4	257.3	Xe lamp	[83]
2	CdS/Fe₂O₃	NBLL	39400	10114.4	Xe lamp λ = 420 nm	[14]
3	PdSA-ZIS	NBLL	11100	10200	Xe lamp	[13]
4	MOF-808	NBLL	1.7	128	Xe lamp	[84]
5	DZIS	NBLL	93002	147734	Xe lamp λ > 420 nm	[85]
6	Pd@TiO₂@ZnIn₂S₄	NBLL	5350	11430	Xe lamp	[86]
7	CoCN	NBLL	3979	147734	Xe lamp λ > 420nm	[87]
8	CN-NS/TO-NW(40)	NBLL	5100	93	Xe lamp λ > 400 nm	[88]
9	TCOF-Pt SA3	NBLL	501.8	477.3	Xe lamp	[89]
10	NiCoFe-LDH@ZIS	NBLL	113570	97.78	Xe lamp	[90]
11	Pt@UiO-66-NH₂@ZIS)	Imine	850	78	Xe lamp λ > 420 nm	[91]
12	PdO_x@HCdS@ZIS@Pt	NBLL	86380	164750	Xe lamp λ = 350-780 nm	[92]

Fig. 11. (a) Possible photocatalytic mechanisms on Pt/CdS/Fe2O3. (b) The capture experiments. (c) Energy band positions of CdS and Fe2O3. Reprinted with permission from Ref. [14]. Copyright 2022, American Chemical Society. (d) FT-EXAFS spectra. (e) Mechanism diagram of photocatalytic H2 evolution coupled with benzylamine oxidation. Reprinted with permission from Ref. [83]. Copyright 2020, John Wiley and Sons. (f) Production for the N-benzylidenebenzylamine and H2 of as-prepared metal single atom-ZIS. (g) Charge density difference mapping between InS2 layer and PdSA-ZnS layer in PdSA-ZIS side view and (h) top view. Reprinted with permission from Ref. [13]. Copyright 2022, Elsevier.

Table 4 Recent research advancements in photocatalytic H2-evolution coupled with reforming of waste plastics.

No.	Photocatalyst	Substrate	Photoreforming	H₂ evolution (mmol g^-1 h^-1)	Light source	Ref.
1	CdS/CdO_x	PLA	polylactic acid, polyethylene, terephthalate polyurethane	64.3	simulated solar light AM 1.5G	[93]
2	CN_x\|Ni₂P	PLA	acetate formate	0.17	simulated solar light AM 1.5G	[16]
3	O-CuIn₅S₈	PET	formate, acetate, glycolate	2.57	Xe lamp	[94]
4	Pt/TiO_2-_x/Ti	plastic wastes	acetate, CH₄, CO	399.2	Xe lamp 400-800 nm	[95]
5	MCN	PET	aormate, lyoxal, acetate	7.33	Xe lamp 100 mW cm^-2	[96]
6	d-NiPS₃/CdS	PET	carbonate	121.04	Xe lamp λ > 400 nm	[15]
7	MoS₂/CdS	PLA	formate, lactate	379.35	Xe lamp	[97]
8	M-2/Z_0.6C_0.4S	PET	glycolate, acetate, ethanol	14.2	Xe lamp λ > 420 nm	[98]
9	CN-CNTs-NiMo	PLA	glyoxal, carboxylate	0.09	Xe lamp	[99]
10	Pt-CdO_x/CdS/SiC	PET	glycolate	0.025	Xe lamp	[100]
11	5.6LS-CZS	PET	glycolate, ethanol	13.83	Xe lamp	[101]
12	Ni₂P/ZnIn₂S₄	PLA	pyruvic acid	0.7813	LED λ > 420 nm (4 × 25 W)	[102]
13	Ag₂O/Fe-MOF	PET	formic acid, acetic acid	1.9	Xe lamp	[103]
14	MoS₂/Cd_0.5Zn_0.5S	PET	formate, methanol, actate ethanol	15.9	Xe lamp	[104]

Fig. 12. (a) Schematic diagram of photoreforming of plastic on MoS2/CdS. Reprinted with permission from Ref. [97]. Copyright 2022, American Chemical Society. (b) Photoreforming of PET bottle over CN-CNTs-NM. (c) Schematic diagram of the process of photoreforming of PET on CN-CNTs-NM. Reprinted with permission from Ref. [99]. Copyright 2022, Elsevier. (d) Schematic diagram of the polymer photoreforming on CNx|Ni2P. Reprinted with permission from Ref. [16]. Copyright 2019, American Chemical Society. (e) Schematic diagram of photoreforming waste plastic. Reprinted with permission from Ref. [98]. Copyright 2021, Elsevier. (f) 1H NMR spectra of PLA cups and PET bottles following photoreforming. (g) Photograph of H2 evolution without and with illumination on d-NiPS3/CdS. (h) Schematic for charge transfer on d-NiPS3/CdS. Reprinted with permission from Ref. [15]. Copyright 2023, American Chemical Society.

Table 5 Recent research advancements in photocatalytic H2-evolution coupled with organic pollutants degradation in wastewater.

No.	Photocatalyst	Pollutant	Light source	H₂ evolution (μmol g^-1 h^-1)	Removal efficiency	Ref.
1	Ag₃PO₄/CABBQDs/rGH	tetracycline hydrochloride	Xe lamp λ ≥ 420 nm	994.30	89	[105]
2	g-C₃N₄/Mn_0.25Cd_0.75S	tetracycline	Xe lamp	3140	—	[106]
3	RGO/Pt/ZnIn₂S₄	organic amines	Xe lamp λ ≥ 420 nm	1597	—	[107]
4	MOS₂/SiO₂/GO	CPBL	Xe lamp	778	84.2	[108]
5	MoS₂@CdS	amoxicillin	Xe lamp λ ≥ 420 nm	87	16.4	[109]
6	Bi/C₃N₄	amoxicillin	Xe lamp λ ≥ 420 nm	718	5.3	[110]
7	ZIS/RGO/BiVO₄	formaldehyde	Xe lamp λ ≥ 420 nm	1687	22.9	[111]
8	MoS₂/ZnIn₂S₄	bisphenol A	Xe lamp λ > 420 nm	672.7	53	[112]
9	ACN-550	bisphenol A	Xe lamp λ = 190-1100 nm	761.8 ± 4.3	89	[113]
10	TOA-30	rhodamine B	Xe lamp	2370	—	[114]
11	CeO₂/CueI-bpy-2.0	rhodamine B	Xe lamp	145	—	[115]
12	ZnIn₂S₄-WO₃-4	crystal violet	Xe lamp λ > 420 nm	737.75	>99.99	[116]
13	UiO-66@Zn_0.5Cd_0.5S	ciprofloxacin	Xe lamp	224	83.6	[117]

Fig. 13. (a) Proposed photocatalytic mechanism of RGO/ZnIn2S4. Reprinted with permission from Ref. [107]. Copyright 2019, American Chemical Society. (b) HPLC results of photocatalytic H2 evolution at different irradiation intervals. Reprinted with permission from Ref. [110]. Copyright 2018, Elsevier. (c) Mechanism of photocatalytic degradation of PHE and TC. (d) Time courses of PHE activity. (e) Photocatalytic degradation of TC. Reprinted with permission from Ref. [105]. Copyright 2022, Elsevier. (f) Mechanism of photocatalytic degradation of CPBL and H2 on MoS2/SiO2/GO. Reprinted with permission from Ref. [108]. Copyright 2022, American Chemical Society. (g,h) Schematic diagram of e- transfer. (i) Possible photocatalytic mechanisms. Reprinted with permission from Ref. [116]. Copyright 2023, Elsevier.

Table 6 Recent research advancements in photocatalytic H2-evolution coupled with H2O2 production.

No.	Photocatalyst	H₂ evolution (μmol g^-1 h^-1)	H₂O₂ production (μmol g^-1 h^-1)	Light source	Ref.
1	PCN-10-CP-10	15.26	15.26	Xe lamp	[121]
2	Few-layer C₆₀	91	116	Xe lamp	[122]
3	C-N-g-C₃N₄	0.84	0.98	420 nm ≤ λ ≤ 720nm	[123]
4	ISQDs-2.25	42.17	36.85	Xe lamp	[124]
5	Pt-NaCN(6)	900	880	Xe lamp 400 < λ < 800 nm	[125]
6	PAA/CoO-NC	48.4	20.4	AM 1.5 G	[126]
7	ZCS/PO/Ni₃Pi₂	1464	1375	Xe lamp λ ≥ 420 nm	[127]
8	Ni₂P/CDs	258.6	1281.4	λ > 420 nm	[119]

Fig. 14. (a) The band alignment diagram of the prepared samples. (b) Schematic diagram of charge transfer mechanism. (c) Detailed transmission channels for electron transfer. Reprinted with permission from Ref. [121]. Copyright 2022, Elsevier. (d) Diagram of possible mechanism of H2 evolution and H2O2 production. Reprinted with permission from Ref. [123]. Copyright 2018, John Wiley and Sons. (e) Schematic diagram of overall water splitting on In2S3 and In2S3 QDs. Reprinted with permission from Ref. [124]. Copyright 2023, Elsevier. (f) Diagram of charge transfer. Reprinted with permission from Ref. [122]. Copyright 2023, John Wiley and Sons.

Fig. 15. (a) The sulfuration of Co/Cd-MOF into Co9S8/CdS heterostructure. (b) The mechanism over Co9S8/CdS. Reprinted with permission from Ref. [131] Copyright 2020 Elsevier B.V. (c) Rates of photocatalytic dehydrogenation of PhCH2OH for H2 evolution and PhCHO production. (d) Time-resolved PL decay plots. Reprinted with permission from Ref. [132]. Copyright 2020, Elsevier. (e) Transient photocurrent-time (I-t) curves. (f) EPR spectra of the prepared samples. (g) Band structure and possible reaction mechanism of CdS/BiVO4 hybrid products. Reprinted with permission from Ref. [69]. Copyright 2022, American Chemical Society.

Fig. 16. (a) Time courses of photocatalytic H2 evolution. (b) Band structures for pure g-C3N4. (c) Band structures for W doped g-C3N4. Reprinted with permission from Ref. [140]. Copyright 2021, Elsevier. (d) The UV-vis spectra. Reprinted with permission from Ref. [139]. Copyright 2017, Elsevier.

Fig. 17. (a) Illustration of synthesizing the Pd/HNb3O8 photocatalyst. (b) Production rates of H2 and benzaldehyde over photocatalysts. Reprinted with permission from Ref. [147]. Copyright 2021, Elsevier. (c) TEM images of FNS@ZIS-2. (d) N2 adsorption-desorption isotherms of ZIS. (e) N2 adsorption-desorption isotherms of FNS@ZIS-2. Reprinted with permission from Ref. [148]. Copyright 2020, Elsevier.

Fig. 18. (a) Comparison of photocatalytic H2 and PhCHO production rates of different photocatalyst. (b) The I-IEF formation by band bending and the charge transfer path at the NP/ZIS-O interface. (c) Schematic illustration for the photocatalytic mechanism of NP/ZIS-O. Reprinted with permission from Ref. [154]. Copyright 2022, John Wiley and Sons. (d) H2 evolution in the aqueous solution of FA. (e) TR-PL spectroscopy of samples. (f) Schematic diagram of ZnIn2S4 and Tp-Tta COF before/after contact and IEF formation and band bending. Reprinted with permission from Ref. [62]. Copyright 2012, Royal Society of Chemistry.

Fig. 19. (a) Synthesis process of Pt/TiO2-x/Ti. (b) H2 evolution rates of samples. (c) Diagram of reforming plastics for H2 evolution. The illustration is the finite-difference top domain (FDTD) result of a near-field electromagnetic field distribution at 785 nm. Reprinted with permission from Ref. [95]. Copyright 2023, Elsevier. (d) Piezotron effect that promotes light generation of e- and h+ separation. (e) Photocatalytic selective oxidation of aniline and H2 evolution. Reprinted with permission from Ref. [155]. Copyright 2021, Elsevier. (f) Schematic diagram of charge transfer on F-BiVO4@NiFe-LDH. Reprinted with permission from Ref. [156]. Copyright 2020, Elsevier. (g) Strategies for constructing TAPP-[2Fe2S]-CMP and possible structures of its functional sites. Reprinted with permission from Ref. [157]. Copyright 2023, Elsevier.

Fig. 20. (a) FTIR spectra of the Sn0.24-Ru0.68/TiO2 photocatalyst. (b) The EPR spectra. Reprinted with permission from Ref. [159]. Copyright 2013, Elsevier. (c) Composite diagram of RuO2@TiO2@Pt hollow sphere. (d) Charge transfer over RuO2@TiO2@Pt. Reprinted with permission from Ref. [160]. Copyright 2016, Elsevier.

Fig. 21. (a) UV-vis diffuse reflectance spectra of the samples. (b) The calculated band structures and partial densities. Reprinted with permission from Ref. [161]. Copyright 2019, Elsevier B.V. (c) ATR-FTIR spectra of SA-TiO2 and free SA. (d) The ESR spectra of 5-CH3O-SA-TiO2. Reprinted with permission from Ref. [163]. Copyright 2018, Elsevier B.V.

Fig. 22. (a) In situ DRIFTS measurement. Reprinted with permission from Ref. [83]. Copyright 2020, Wiley-VCH GmbH. (b) In situ FTIR spectra. Reprinted with permission from Ref. [92]. Copyright 2024, Elsevier Inc. (c) The schematic of the photoelectrochemical system with LSV-Raman analysis. (d) In situ Raman spectra. Reprinted with permission from Ref. [164]. Copyright 2020, Wiley-VCH Verlag GmbH. In situ irradiation XPS of (e) Zn 2p and (f) Ti 2p. Reprinted with permission from Ref. [46]. Copyright 2023, Wiley-VCH GmbH.

Fig. 23. (a) Cu2O structure change under irradiation. (b-d) In-situ TEM observation of Cu2O during photocatalytic H2 evolution process. Reprinted with permission from Ref. [165]. Copyright 2020, Elsevier B.V. (e) KPFM images of TF10 in darkness. (f) KPFM image of TF10 with 365-nm UV light illumination. Reprinted with permission from Ref. [4]. Copyright 2022, Wiley-VCH GmbH. (g) In situ XRD. Reprinted with permission from Ref. [166]. Copyright 2022, Wiley-VCH GmbH. (h) In-situ XANES spectra. (i) Least-squares curve-fitting analysis. Reprinted with permission from Ref. [167]. Copyright 2023, Springer Nature.

Fig. 24. (a) DMPO ESR spin-trapping for •O2-. (b) DMPO ESR spin-trapping for •OH. Reprinted with permission from Ref. [49]. Copyright 2021, Elsevier. (c) TEMPO ESR spectrum of h+. Reprinted with permission from Ref. [48]. Copyright 2022, Elsevier. (d) In situ ESR spectra for UCNT. Reprinted with permission from Ref. [12]. Copyright 2022, American Chemical Society. (e) Detected EPR signals. Reprinted with permission from Ref. [18]. Copyright 2024, American Chemical Society (f) In situ EPR spectra for CoP/CdS. Reprinted with permission from Ref. [168]. Copyright 2024, Wiley-VCH GmbH.

Fig. 25. (a) Charge density difference for NiCoFe-LDH@ZIS. Reprinted with permission from Ref. [90]. Copyright 2023, Elsevier. (b) Electron density difference and bader electron transfer on CdS/MoS2. Reprinted with permission from Ref. [56]. Copyright 2022, Wiley-VCH. (c) Calculated work functions of ZIS. Reprinted with permission from Ref. [169]. Copyright 2023, Elsevier B.V. (d) DFT simulated frontier orbitals of PCN-777. Reprinted with permission from Ref. [84]. Copyright 2018, Wiley-VCH. (e) Possible cyclic process and active site of the samples. Reprinted with permission from Ref. [170]. Copyright 2023, Springer Nature. (f) DFT-calculated energy diagram. Reprinted with permission from Ref. [171]. Copyright 2022, Elsevier B.V.

Fig. 26. (a) Photocatalytic reaction mechanism of RS/ZIS-Sv heterojunction. Reprinted with permission from Ref. [67]. Copyright 2022, Elsevier B.V. (b) The proposed mechanism for CdS(ZB)/CdS(WZ)/Ni-BTC. Reprinted with permission from Ref. [72]. Copyright 2021, Elsevier B.V. (c) The photocatalytic mechanism in ZnCo2S4/Zn0.2Cd0.8S heterojunction. Reprinted with permission from Ref. [130]. Copyright 2022, Elsevier Ltd. (d) Type-II transfer mechanism. (e) S-scheme transfer mechanism over Zn0.1Cd0.9S/MoO3-x. Reprinted with permission from Ref. [172]. Copyright 2022, Elsevier. B.V.

Fig. 27. Challenges and outlooks in dual-channel H2-evolution coupled with photoreforming oxidation of waste materials.

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双通道氧化还原反应用于光催化析氢耦合废弃物光重整氧化

Dual-channel redox reactions for photocatalytic H₂-evolution coupled with photoreforming oxidation of waste materials

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双通道氧化还原反应用于光催化析氢耦合废弃物光重整氧化

Dual-channel redox reactions for photocatalytic H2-evolution coupled with photoreforming oxidation of waste materials

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Dual-channel redox reactions for photocatalytic H₂-evolution coupled with photoreforming oxidation of waste materials