先进的光电催化耦合反应

doi:10.1016/S1872-2067(25)64697-3

催化学报 ›› 2025, Vol. 73: 99-145.DOI: 10.1016/S1872-2067(25)64697-3

先进的光电催化耦合反应

潘嘉宁^a, 李敏^a(), 王瑛琦^a, 谢文富^a, 张天雨^b, 王强^a^,^b()

^a北京林业大学环境科学与工程学院, 水体污染源控制技术北京市重点实验室, 水污染源头控制与生态修复工程研究中心, 北京 100083
^b北京林业大学森林资源高效生产国家重点实验室, 北京 100083

收稿日期:2025-01-07 接受日期:2025-03-18 出版日期:2025-06-18 发布日期:2025-06-12
通讯作者: *电子信箱: limin2022@bjfu.edu.cn (李敏),qiangwang@bjfu.edu.cn (王强).
基金资助:
国家自然科学基金(52225003);国家自然科学基金(52300125);国家自然科学基金(52470113);北京林业大学5·5工程研究创新团队项目(BLRC2023B04)

Advanced photoelectrocatalytic coupling reactions

Jianing Pan^a, Min Li^a(), Yingqi Wang^a, Wenfu Xie^a, Tianyu Zhang^b, Qiang Wang^a^,^b()

^aBeijing Key Laboratory for Source Control Technology of Water Pollution, Engineering Research Center for Water Pollution Source Control & Eco-remediation, College of Environmental Science and Engineering, Beijing Forestry University, Beijing 100083, China
^bState Key Laboratory of Efficient Production of Forest Resources, Beijing Forestry University, Beijing 100083, China

Received:2025-01-07 Accepted:2025-03-18 Online:2025-06-18 Published:2025-06-12
Contact: *E-mail: limin2022@bjfu.edu.cn (M. Li),qiangwang@bjfu.edu.cn (Q. Wang).
About author:Dr. Min Li received her B.S. in 2015 and Ph.D degree in 2020 from School of Materials Science and Technology, China University of Geosciences (Beijing). She carried out postdoctoral research at Department of Chemistry, Tsinghua University from 2020 to 2022. Since the end of 2022, she joined the faculty of College of Environmental Science and Engineering, Beijing Forestry University. Her current research mainly focuses on the design and modification of environmental functional materials and photo/photoelectro-catalytic CO₂ conversion.
Professor Qiang Wang received his BSc (2003) and MSc (2005) from Harbin Institute of Technology in China, and PhD (2009) from POSTECH in South Korea. In 2009-2011, he worked as a research fellow at the Institute of Chemical and Engineering Sciences under ASTAR, Singapore. In 2011-2012, he worked as a postdoctoral associate at the Department of Chemistry, University of Oxford. Since 2012, he holds a full professor position at the College of Environmental Science and Engineering, Beijing Forestry University. He serves as the section editor (capture, storage, and chemical conversion of carbon dioxide) of the Journal of Energy Chemistry and the editorial boards of several scientific journals. His current research interests include environmental functional nanomaterials for air pollution control and CO₂ capture and utilizations (CCU).
Supported by:
National Natural Science Foundation of China(52225003);National Natural Science Foundation of China(52300125);National Natural Science Foundation of China(52470113);5·5 Engineering Research & Innovation Team Project of Beijing Forestry University(BLRC2023B04)

摘要/Abstract

摘要：

光电催化(PEC)作为一种新兴的技术, 在多种氧化还原反应中展现出广泛的应用前景, 尤其在能源转化和环境修复领域具有巨大的潜力. 然而, 传统的PEC反应主要在阳极进行析氧反应, 受限于较高的热力学能垒和缓慢的动力学过程, 导致能量消耗过大. 此外, 析出的氧气经济价值有限, 进一步制约了PEC技术的实际应用. 为了克服这一瓶颈, 研究人员提出了先进的阴极−阳极耦合反应系统, 通过用较低电位、具有较高经济价值的氧化反应代替传统的析氧反应, 显著提高能量转化效率, 同时合成高价值的化学品, 实现能量利用的优化, 并有效降低环境污染. 更重要的是, 通过合理设计和优化光电极材料, 该系统可以在光照下产生足够的光电压, 以满足整体反应的热力学和动力学需求. 此外, 通过精准调控电压, 实现阴极和阳极的电流密度匹配, 从而在无偏压条件下驱动耦合反应的高效进行.

本综述总结了PEC耦合反应机理, 并与其它光驱动催化反应体系(如光伏、光热、光酶催化)进行了对比分析. 详细归纳了光电耦合反应体系中光阴极与光阳极催化剂的设计策略及其合成方法, 进一步从组分调控(单原子、双原子、高熵合金与高熵氧化物)、结构调控(限域效应、动态缺陷调控)、异质结构筑(范德华异质结、电子极化异质结)、电子轨道调控(d轨道调控、电子自旋极化调控)、微环境调控(表面修饰、pH调控、极化电场调控)等方面探讨了先进的催化剂改性策略. 重点介绍了PEC耦合系统的最新进展, 包括光阴极CO₂还原、硝酸盐还原、氧还原、酶活化与光阳极有机氧化、生物质氧化和污染物降解等反应的耦合. 此外, 归纳了当前用于阐明反应机理的先进原位表征技术, 如原位X射线吸收精细结构、拉曼、红外、电子顺磁共振、X射线衍射、X射线光电子能谱和电化学质谱. 最后, 探讨了光电极材料设计、光电催化反应系统优化及大规模应用所面临的挑战, 并对PEC耦合系统的未来发展进行了展望.

本综述强调了PEC耦合系统在提升能源利用效率、降低反应能耗及促进绿色化学转化方面的巨大潜力, 为未来此类体系的合理设计提供了重要的研究思路和技术指导.

关键词: 光电催化, 耦合反应, 光阳极, 光阴极

Abstract:

Photoelectrocatalysis (PEC) is extensively applied in diverse redox reactions. However, the traditional oxygen evolution reaction (OER) occurring at the (photo)anode is hindered by high thermodynamic demands and sluggish kinetics, resulting in excessive energy consumption and limited economic value of the O₂ produced, thereby impeding the practical application of PEC reactions. To overcome these limitations, advanced anodic-cathodic coupling systems, as an emerging energy conversion technology, have garnered significant research interest. These systems substitute OER with lower potential, valuable oxidation reactions, significantly enhancing energy conversion efficiency, yielding high-value chemicals, while reducing energy consumption and environmental pollution. More importantly, by designing and optimizing photoelectrodes to generate sufficient photovoltage under illumination, meeting the thermodynamic and kinetic potential requirements of the reactions, and by tuning the voltage to match the current densities of the cathode and anode, coupling reactions can be achieved under bias-free conditions. In this review, we provide an overview of the mechanisms of PEC coupling reactions and summarize photoelectrode catalysts along with their synthesis methods. We further explore advanced catalyst modification strategies and highlight the latest development in advanced PEC coupling systems, including photocathodic CO₂ reduction, nitrate reduction, oxygen reduction, enzyme activation, coupled with photoanodic organic oxidation, biomass oxidation, and pollutant degradation. Additionally, advanced in situ characterization techniques for elucidating reaction mechanisms are discussed. Finally, we propose the challenges in catalyst design, reaction systems, and large-scale applications, while offering future perspectives for PEC coupling system. This work underscores the tremendous potential of PEC coupling systems in energy conversion and environmental remediation, and provides valuable insights for the future design of such coupling systems.

Key words: Photoelectrocatalysis, Coupling reaction, (Photo)cathode, (Photo)anode

潘嘉宁, 李敏, 王瑛琦, 谢文富, 张天雨, 王强. 先进的光电催化耦合反应[J]. 催化学报, 2025, 73: 99-145.

Jianing Pan, Min Li, Yingqi Wang, Wenfu Xie, Tianyu Zhang, Qiang Wang. Advanced photoelectrocatalytic coupling reactions[J]. Chinese Journal of Catalysis, 2025, 73: 99-145.

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图/表 26

Fig. 1. Timeline of PEC coupling reactions in recent years.

Fig. 2. Schematic diagram of cathodic and anodic reactions in PEC coupling systems.

Fig. 3. Schematic diagrams of PEC systems. (a) bias-assisted photoanode PEC cell. (b) bias-assisted photocathode PEC cell. (c) bias-free tandem PEC cell. (d) The bandgaps and band positions of p-type and n-type semiconductors. Reprinted with permission from Ref. [33]. Copyright 2025, Royal Society of Chemistry.

Fig. 4. (a) The illustration to prepare In2S3/MnIn2S4 catalyst. Reprinted with permission from Ref. [82]. Copyright 2024, Elsevier B.V. (b) Detailed prepared diagram for NCDs/Co3O4/Ti mesh photocathode. Reprinted with permission from Ref. [85]. Copyright 2023, Elsevier B.V. (c) Schematic illustration for the synthesis of the b-TiO2-x nanocones photoanode. Reprinted with permission from Ref. [86]. Copyright 2024, Elsevier B.V.

Fig. 5. (a) Schematic diagram of coating. (b) Schematic diagram of impregnation. (c) Schematic illustration for the synthesis of the Pt/TiO2/SiNW photoanode.

Fig. 6. The schematic of advanced modification strategies for catalysts.

Fig. 7. (a) Schematic diagram of the synthesis of Ni-SAC by the confinement synthesis strategy. (b) HAADF-STEM images of Ni-SAC sample. (c) Mechanism diagram. Reprinted with permission from Ref. [103]. Copyright 2024, Springer Nature Limited. (d) HAADF-STEM image of FeSn-C2N, showing the dual atoms (yellow ellipse) and single atom (blue circle). (e) The dimer structure of active FeSn dual atom sites derived from the EXAFS result. (f) Gibbs free energy of ORR intermediates absorbed on FeSn-C2N, Fe-C2N, and Sn-C2N. Reprinted with permission from Ref. [106]. Copyright 2024, American Chemical Society.

Fig. 8. (a) FE-SEM image of the MnFeCoNiCu HEA. (b) Bader charge analysis of the MnFeCoNiCu HEA. (c) Electron density of the MnFeCoNiCu HEA. Reprinted with permission from Ref. [111]. Copyright 2025, Wiley-VCH. (d) TEM of ZnFeNiCuCoRu-O. (e) i-t test of ZnFeNiCuCoRu-O||Pt/C for overall water splitting. Reprinted with permission from Ref. [112]. Copyright 2023, Wiley-VCH.

Fig. 9. (a?c) HAADF-STEM images. (d) Energy difference between the β-C association intermediate and the β-pentacyclic association intermediate. Reprinted with permission from Ref. [116]. Copyright 2024, American Chemical Society. (e) EPR spectra of the samples. (f) Formation energy of oxygen vacancy over ZO-OV, CZO-OV, and CZO-OV-adding electrons. Reprinted with permission from Ref. [119]. Copyright 2024, National Academy of Sciences.

Fig. 10. (a) HRTEM images of 3CoPc/0.6P-WS2. (b) The model of 3CoPc/0.6P-WS2 with side view and top view. (c) Photocatalytic stability [122]. Copyright 2023, Wiley-VCH. (d) HRTEM image of PtSe2/PtCo heterojunctions with the inset FFT pattern of PtSe2/PtCo heterojunctions. (e) Charge density difference plot at the PtSe2/PtCo interface; The yellow and cyan regions represent electron aggregation and electron depletion respectively. (f) ΔGH* diagram for HER [124]. Copyright 2024, Wiley-VCH.

Fig. 11. (a) d-band center and G OH*. Computed projected density of states of Fe5N mC (b) and Fe5Cu N mC (c) after OH* adsorption [127]. Copyright 2023, Wiley-VCH. (d) Scheme depicting the synthesis of Co3O4 with Co vacancies. (e) Co L-edge XANES of Co3O4 and Co3?xO4 samples. (f) Calculated free energy diagrams of photoreduction of CO2 to CO on Co3O4 and Co3?xO4 with and without consideration of spin polarization in the calculation [130]. Copyright 2024, American Chemical Society.

Fig. 12. (a) With CTAB. Interfacial water molecules are repelled away from electrode-electrolyte interface, which favors racemates generation. Production distribution over carbon paper (b) and CTAB-modified carbon paper (c) [135]. Copyright 2023, Springer Nature Limited. (d) Schematic illustration for fabrication of La-Cu HS. (e) From left to right are the pH distribution in electrolyte near surface of solid sphere, hollow sphere, and within channels of hollow sphere at ?900 mA [137]. Copyright 2024, Springer Nature Limited. (f) HAADF-STEM images of BTOPAu. (g) Electric hysteresis loops of BTO, BTOP, BTOAu3, and BTOPAu (at 10 kV·cm?1) [139]. Copyright 2024, Springer Nature Limited.

Fig. 13. (A): (a) The schematic illustration of photothermal-assisted co-electrolysis of CO2 and methanol; (b) FE for CO at different applied potentials of Ni-Bpy-COF and Ni-2CBpy2+-COF; (c) Faradaic efficiency of MOR product at different applied potentials for Ni-Bpy-COF and Ni-2CBpy2+-COF; (d) Cycling tests of temperature changes of Ni-2CBpy2+-COF and Ni-Bpy-COF under irradiation (insert images are the photothermal images of Ni-2CBpy2+-COF). (e) jCO as a function of the cell voltage; (f) Radar chart of the performances for co-electrolysis of CO2 and methanol in two-electrode system [83]. Copyright 2022, Wiley-VCH. (B): (a) Schematic representation of a fully assembled two-electrode PEC cell; (b) LSV of a three-electrode cell that comprised a mTiO2|STEMPO/DPP-CA working electrode and a cyclic voltammogram of a three-electrode cell that comprised a mITO|FDH working electrode with a Ag/AgCl(KClsat) reference and Pt mesh counter electrodes; (c) Comparison of mTiO2|STEMPO/dye electrodes for 4-MBA oxidation; (d) CPPE of the two-electrode cell at an applied voltage of 0?V [148]. Copyright 2022, Springer Nature Limited.

Fig. 14. (A): (a) LSV curves of Si,GaN/Si and Bi/GaN/Si at light and dark; (b) FEs and jHCOO? at varied applied potentials over Bi/GaN/Si; (c) LSV curves of α-Fe2O3 with different co-catalysts; (d) FEs and TOFs for HCOO? production at varied potentials over NiOOH/ α-Fe2O3; (e) LSV curves of the tandem PEC cell with and without biomass addition; (f) Comparisons of the bias required to achieve varied current densities with and without biomass addition [73]. Copyright 2023, Springer Nature Limited. (B): (a) Representative photocurrent density versus bias for SiNW photocathodes prepared with (biotic) and without (abiotic) methanol-adapted S. ovata; (b) Schematic of a bias-free photochemical diode device; (c) Overlap of the J-V curves of the biophotocathode and the photoanode on the RHE scale; (d) Photocurrent density versus applied bias for biophotochemical diodes combining the S. ovata/Pt/TiO2/n+ p-SiNW photocathode and Pt-Au/TiO2/p+ n-SiNW photoanode; (e) Faradaic efficiencies of the cathodic product (blue), all of the anodic products (pink) and each anodic product under bias-free operation of the biophotochemical diode [98]. Copyright 2024, Springer Nature Limited. (C): (a) Yields of CH3OH and CO (μmol/L, cm2) over various catalysts; (b) LSV curves of bare (Au/α-Fe2O3/RGO/ITO//Ru/RGP/Pt) and Au/α-Fe2O3/RGO/ITO//Ru/RGP/Pt with the presence of CO2 in the cathodic chamber and 30 mmol FF in the anodic chamber; (c) Simultaneous reduction of CO2 over the Au/α-Fe2O3/RGO/ITO photocathode and oxidation of FF over the Ru/RGO/Pt anode; (d) Effect of FF amount vs. conversion and yields of 2-FA and 5-HFA from the anode chamber and the effect of FF amount vs. the yields of CH3OH and CO from the cathode chamber; (e) Proposed mechanisms for the simultaneous reduction of CO2 and oxidation of FF via a paired electrode system using an H-cell [158]. Copyright 2021, Elsevier B.V.

Fig. 15. (a) Curves of linear voltammetry obtained for TiO2Nt under dark (curve I) and irradiated by UV-Vis light (curve II) and TiO2Nt-ZrO2 irradiated by UV-Vis light (curve III); (b) Photocurrent response curves obtained by chronoamperometry for TiO2Nt (curve I) and TiO2Nt-ZrO2 (curve II); (c) Representative scheme of the full cell with two compartments used in the experiments of organic compound oxidation and CO2 reduction; (d) Scheme of a photoanode-driven system of two electrodes [74]. Copyright 2019, Elsevier Ltd.

Fig. 16. (a) Schematic of the PEC cell used for NH3 production. (b) CV curves of various Pt-based electrocatalysts for GOR. (c) LSV curves of the Ru@TiNS/Ni/perovskite photocathode overlapped with OER and GOR. (d) Amount of NH3 generated at the photocathode and the corresponding FE. (e) FE of GOR products in the bias-free system under continuous operation [89]. Copyright 2024, Springer Nature Limited.

Fig. 17. (a) Illustration of two-compartment artificial PEC cell for simultaneous PEC oxidation and nitrite-ammonia conversion. (b) FE and selectivity of BAD on CdS/CdIn2S4 in the presence of various radical scavengers. (c) Photocurrent-time curves at 1.1 V versus CE of two-electrode configuration [84]. Copyright 2022, Wiley-VCH.

Fig. 18. (A): (a) Schematic illustrating the flow-through system; (b) H2O2 production and SMX removal under different filters and photoelectric modes in a phosphate buffer solution. Filters I-IV are for MXene, Fe-NC/MXene, Sb-SA/MXene and Sb-Fe/Mxene; (c) Schematic of the Sb-SA/MXene photocatalytic surface with H2O2 generation and the Fe-NC/MXene electrocatalytic surface with ?OH production concurrently; (d) The removal efficiency of Sb (III) and SMX by pure MXene at the feed-side and Fe-NC/MXene at the permeate-side simultaneously; (e) Repeatability of Sb-Fe/MXene filter for H2O2 production and SMX degradation [170]. Copyright 2023, Elsevier B.V. (B): (a) Schematic illustration of the PEC cell for degradation of 4-FP; (b) Concentration of residual 4-FP by direct photolytic, photocatalytic, electrocatalytic, and PEC process; (c) Concentration of residual 4-FP as well as corresponding defluorination and TOC removal efficiencies in the PEC system; (d) Plausible coexisting degradation pathways of 4-FP for the synchronous defluorination-oxidation process [174]. Copyright 2023, Elsevier B.V. (C): (a) Schematic illustration of PEC water purification on b-TiO2-x photoanode and H2O2 production on NADE; (b) ?OH quantitative concentration over b-TiO2-x and TiO2; (c) Degradation and reaction rate constant of SMT; (d) H2O2 production in b-TiO2-x/NADE and b-TiO2-x/Pt PEC systems; (e) Performance of the b-TiO2-x/NADE system for contaminant SMT degradation under EC, PC, and PEC conditions; (f) Comparison of water purification performance under applied bias voltage with the last five years reported PEC water purification literatures [86]. Copyright 2024, Elsevier B.V.

Fig. 19. (A): (a) Schematic diagram of nanozyme-coupled PEC degradation of 3-CP; (b) PEC degradation curves of 3-CP curves using WO3 photoanode and different cathodes; (c) The removal of 3-CP by different processes [176]. Copyright 2024, Elsevier Ltd. (B): (a) Degradation of SDZ in different system; (b) Energy consumption (EEO) of TiO2 NNs-NCDs/Co3O4 and single photoelectrode PEC system for SDZ removal; (c) Schematic illustration of SDZ degradation by TiO2 NNs-NCDs/Co3O4 PEC system [85]. Copyright 2023, Elsevier B.V. (C): (a) Schematic diagram of H2O2 and HClO were produced simultaneously at the cathode and anode; (b) the S-scheme charge transfer mechanism between In2S3 and MnIn2S4; (c) LSV plots of the ORR||ClOR and ORR||OER systems by In2S3/MnIn2S4/PVDF/NF||In2S3/MnIn2S4/CP; (d) The effect of bia potentials on the generation of H2O2 and HClO and current density and cell voltage versus time curves of this PEC cascade production system at 1.2 V vs. Ag/AgCl; (e) Degradation efficiency of MB in H2O2 alone system, HClO alone system, H2O2-HClO coupling system [82]. Copyright 2024, Elsevier B.V. (D): (a) The reaction mechanism of PEC degradation of TC by MgO/g-C3N4 photoanode coupled with MCF cathode system; (b) Degradation efficiency of TC in different systems [90]. Copyright 2024, Elsevier B.V. (E): (a) Reaction schemes of the Blue-TNTs PEC-PEF process; (b) 2,4-D degradation in different processes; (c) Effect of different cathodes on 2,4-D removal [76]. Copyright 2020, Elsevier Ltd.

Table 1 Pollutant concentration and degradation performance.

Types of pollutant	Concentration	Degradation efficiency	Ref.
2,4-D MB SDZ SMT TC BPA SMX 4-FP 3-CP	10.0 mg/L 10.0 mg/L 10.0 mg/L 10.0 mg/L 20.0 mg/L 10.0 mg/L 10.0 mg/L 20.0 ppm 10.0 mg/L	100% 100% 98.54% 98.32% 100% 92% 94.7% 14.4 g h^‒1 m^‒2 91.1%	[76] [82] [85] [86] [90] [95] [170] [174] [176]

Fig. 20. (a) Schematic diagram of solar-powered photoelectrochemical biosynthetic reactions using non-recyclable real-world PET microplastics; (b) Time profiles of electrocatalytic production of H2O2; (c) Linear sweep voltammograms for NAD+ reduction; (d) Electrochemical production of NADH from NAD+ using CFP cathode; (e) Potential-dependent production rates of formate and acetate driven by α-Fe2O3 and Zr:α-Fe2O3 photoanodes [183]. Copyright 2024, Springer Nature Limited.

Table 2 Summary of (photo)cathode and (photo)anode catalysts, reaction conditions, and performances in PEC coupling reactions.

Types of coupling reaction			Photoelectrode catalyst		Reaction condition		Performance		Ref.
-	+	+	-	+	-	+	-	+	Ref.
CO₂ reduction	alcohol oxidation	methanol	Ni-2CBpy²⁺-COF	Ni-2CBpy²⁺-COF	0.5 mol L^-1 KHCO₃ (pH = 7.2), −0.9 V vs. RHE	1 mol L^-1 KOH, 1 mol L^-1 methanol, 1.4 V vs. RHE	FE_CO: 98%	FE_HCOOH: 92%	[83]
	biomass oxidation	4-methylbenzylalcohol	mITO/FDH	mTiO₂/ STEMPO/ DPP-CA	0.05 mol L^-1 NaHCO₃ (pH = 6.4), 0 V	0.1 mol L^-1 Na₂B₄O₇ (pH = 8.0), AM 1.5G, λ > 420 nm, 0 V	yield_4-MBAd: 3.1± 0.31 µmol cm^-2, FE: 108 ± 18%	yield_formate: 2.16 ± 0.26 µmol cm^-2, FE: 7 ± 17%	[148]
		glucose	Bi/GaN/Si	NiOOH/ α-Fe₂O₃	0.5 mol L^-1 KHCO₃ (pH = 7.5), AM 1.5G, −0.2 V vs. RHE	1 mol L^-1 KOH (pH = 13.6), AM 1.5G, 1.0 V vs. RHE	FE_HCOO−: 85.2%	FE_HCOO−: 96%	[73]
		glycerol	Pt/TiO₂/ n⁺p-SiNW loaded with S.ovata	Pt-Au/TiO₂/p⁺n-SiNW	bacterial medium with 50 mmol L^-1, MES (pH = 6.2), red light (740 nm), 20 mW cm⁻², −0.4 V vs. RHE	1 mol L^-1 KOH, 0.1 mol L^-1 glycerol, red light (740 nm), 20 mW cm⁻², 0.45 V vs. RHE	FE_acetate: 86.8 ± 14.0%	FE: 79.3 ± 9.1%	[98]
		glycerol	Ag	Ni/Si	1 mol L^-1 CsOH and 0.5 mol L^-1 glycerol	1 mol L^-1 CsOH, 0.5 mol L^-1 glycerol, 1000 mW cm^-2, AM 1.5G, 1.0 V vs. Ag/AgCl	FE_CO: 95%	FE: 85%	[156]
		glycerol	PVK/CuNF	Si/TiO₂/ PtAu	0.1 mol L^-1 KHCO₃ (pH = 6.8), AM 1.5G, 0 V vs. RHE	1 mol L^-1 KOH with 0.1 mol L^-1 glycerol (pH = 6.8), AM1.5G, 0 V vs. RHE	faradaic yield (FY)_C2: 5%-7%	FY: glycerate (53±1%), formate (18±4%), lactate (8±1%), acetate (7±2%)	[78]
		furfural	Au/α-Fe₂O₃/ RGO	Ru/RGO/Pt	0.1 mol L^-1 KOH, −0.6 V vs. SCE, λ = 400-450 nm	0.1 mol L^-1 KOH, 10 mmol FF, −0.6 V vs. SCE	yield_CH3OH: 51 μmol L^-1 cm^-2, yield_CO: 2 μmol L^-1 cm^-2	yield_2-FA: 59%, yield_5-HFA: 19%	[158]
	degradation of organic pollutants	benzyl alcohol	GDL-Cu₂O	TiO₂Nt-ZrO₂	0.1 mol L^-1 KHCO₃ (pH = 7)	0.1 mol L^-1 Na₂SO₄, 1.0 mmol L^-1 benzyl alcohol (pH = 7), 125W high-pressure mercury lamp, 1.5 V vs. Ag/AgCl	yield_CH3OH: 3.8 mmol/L, yield_CH3CH2OH: 0.96 mmol/L	degradation rate:68%	[74]
Nitrate or nitrite reduction	glycerol oxidation		Ru@TiNS/Ni/perovskite	Pt@TiNS	0.5 mol L^-1 KNO₃, 1.0 mol L^-1 KOH, AM 1.5G, 0.0 V vs. CE	0.5 mol L^-1 glycerol and 1.0 mol L^-1 KOH, 0.0 V vs. CE	FE_NH3: 99.5 ± 0.8%, SAP: 1744.9±20.6 µg_NH3 cm^-2 h^-1	FE: 98.1±2.4%	[89]
Nitrate or nitrite reduction	benzyl alcohol oxidation		TiO₂/AZO/ Cu₂O/Au	CdS/CdIn₂S₄	MeCN with 1 mol L^-1 KOH, AM 1.5G	MeCN with 0.2 mol L^-1 TBAHFP, AM 1.5G, 0.67 V vs. RHE	FE_NH3: 98.1%	FE_BAD: >99% selectivity: >98%	[84]
	cyclohexane oxidation		R-TiO₂	R-TiO₂	0.5 mol L^-1 Na₂CO₃-NaHCO₃ (pH = 9) with 0.1 mol L^-1 CYC and 1.8 mol L^-1 KNO₃, AM 1.5G, 1.6 V	0.5 mol L^-1 Na₂CO₃-NaHCO₃ (pH = 10) with 50 mmol L^-1 CYC, 1.6 V	Yield_CHO: 21.0 μmol cm^‒2 h^‒1	Yield_CYC: 0.43 μmol cm^‒2 h^‒1	[166]
Oxygen reduction	Degradation of pollutants	SMX	Sb-SA/Mxene	Fe-NC/Mxene	phosphate buffer solution (pH = 6.8), with 10.0 mg L^-1 SMX AM 1.5G, cell potential = 0.9 V	Phosphate, buffer solution (pH = 6.8), with 10.0 mg L^-1 SMX cell potential = 0.9 V	yield_H2O2: 343.4 μmol L^-1	removal efficiency: 94.7%	[170]
		4-FP	graphite plate	TiO₂ nanopillar	0.1 mol L^-1 Na₂SO₄, 20 ppm of 4-FP (pH = 6.0)	0.1 mol L^-1 Na₂SO₄, 20 ppm of 4-FP (pH = 6.0), 400 mW cm^-2, 1.0 V vs. RHE	—	degradation rate: 14.4 g h^‒1 m^‒2	[174]
		SMT	NADE	b-TiO_2-_x	0.1 mol L^-1 Na₂SO₄, 0.5 V	0.1 mol L^-1 Na₂SO₄ with 10 mg L^-1 SMT, 50 W LED lamp, 0.5 V	yield_H2O2: 6.83 μmol h^-1 cm^-2	degradation efficiency: 98.32%	[86]
		BPA	CF-DPA	WO₃	200 mmol L^-1 NaCl, pH = 5, -0.5 V vs. Ag/AgCl	200 mmol L^-1 NaCl with 10 mg L^-1 BPA, pH = 10.8, 1 sun illumination	yield_H2O2: 5.4 mmol L^-1	degradation efficiency: 92%	[95]
		CECs(TMP, SMX, CBZ DFC)	GDE	WO₃	simulated wastewater effluent or 7.5 mmol L^-1 Na₂SO₄, cell potential = 1.5 V	simulated wastewater effluent or 7.5 mmol L^-1 Na₂SO₄, concentration of each CEC (100 µg L^-1), λ = 200-480 nm, 86 W m^-2, cell potential = 1.5 V	FE_H2O2: 55%	degradation rate constants: TMP (5.67 × 10⁻³ min⁻¹), SMX (5.35 × 10⁻³ min⁻¹), CBZ (2.9 × 10⁻³ min⁻¹), DFC (4.35 × 10⁻³ min⁻¹)	[175]
		3-CP	BiOI	WO₃	0.1 mol L^-1 Na₂SO₄ with 10 mg L^-1 3-CP,1.8 V	0.1 mol L^-1 Na₂SO₄ with 10 mg L^-1 3-CP, 200 mW cm⁻²,1.8 V	—	degradation efficiency: 91.1%	[176]
		SDZ	NCDs/ Co₃O₄/ Ti mesh	TiO₂ NNs/Ti mesh	0.05 mol L^-1 Na₂SO₄ with 10 mg L^-1 SDZ, LED light, 0.4 V	0.05 mol L^-1 Na₂SO₄ with 10 mg L^-1 SDZ, LED light, 0.4 V	0.05 mol L^-1 Na₂SO₄, 10 mg L^-1 SDZ, LED light, 0.4 V	degradation efficiency: 98.54%	[85]
		MB	In₂S₃/ MnIn₂S₄/PVDF/ NF	In₂S₃/MnIn₂S₄/CP	0.1 mol L^-1 Na₂SO₄ with 10 mg L^-1 MB, (pH = 3), 300 W Xenon lamp, λ > 420 nm, −0.6 V vs. Ag/AgCl	35 g L^-1 NaCl 10 mg L^-1 MB 300 W Xenon lamp, λ > 420 nm, 1.3 V vs. Ag/AgCl	yield_H2O2: 2107.8 μmol L^-1, degradation efficiency: 95.1%	yield_HClO: 28.5 μmol L^-1, degradation efficiency: 98.5%	[82]
		TC	MCF	MgO/g- C₃N₄	0.1 mol L^-1 Na₂SO₄ with 20 mg L^-1 TC (pH = 5.6), −0.5 V vs. Ag/AgCl	0.1 mol L^-1 Na₂SO₄ with 20 mg L^-1 TC (pH = 5.6), LED lamp (380 nm < λ < 840 nm)	yield_H2O2: 10.19 mg L^-1	degradation efficiency: 100%	[90]
		2,4-D	modified carbon felt	Blue-TNTs	0.05 mol L^-1 Na₂SO₄with 10 mg L^-1 2,4-D, 0.2 mmol L^-1 FeSO₄, 2.4 V	0.05 mol L^-1 Na₂SO₄with 10 mg L^-1 2,4-D, 0.2 mmol L^-1 FeSO₄, 200 W, Xenon lamp (λ = 300- 900 nm), 80 mW cm^-2, 2.4 V	yield_H2O2: 9.7 mg L^-1	degradation efficiency: 100%	[76]
Enzymes activation	PET microplastics conversion		AQC/ CFP	Zr:α-Fe₂O₃	100 mmol L^-1 KPi buffer (pH = 6.0), 0.16 V vs. RHE	50 mg mL^-1 PET microplastics, 5 mol L^-1 NaOH, AM 1.5G, 1.0 V vs. RHE	formate and acetate produced by Zr:α-Fe₂O₃	yield_H2O2: 1.85 ± 0.07 mmol L^-1 h^-1, yield_{(R)-1- phenylethanol}: 1.63 ± 0.08 mmol L^-1 h^-1, TOF_rAaeUPO: 32700±1500 h⁻¹	[183]
Enzymes activation	PET microplastics conversion				100 mmol L^-1 NaPi buffer (pH = 7.5), −0.2 V vs. RHE			yield_NADH: 1.19± 0.07 mol L^-1 h^-1, yield_L-glutamate: 2.74 ± 0.11 mmol L^-1 h^-1, TOF_GDH: 5500 ± 200 h⁻¹, yield_{(R)-2-methylcyclohexanone}: 1.16 ± 0.16 mol L^-1 h^-1, TOF_TsOYE: 230 ± 30 h⁻¹

Table 2 Summary of (photo)cathode and (photo)anode catalysts, reaction conditions, and performances in PEC coupling reactions.

Types of coupling reaction			Photoelectrode catalyst		Reaction condition		Performance		Ref.
-	+	+	-	+	-	+	-	+	Ref.
CO₂ reduction	alcohol oxidation	methanol	Ni-2CBpy²⁺-COF	Ni-2CBpy²⁺-COF	0.5 mol L^-1 KHCO₃ (pH = 7.2), −0.9 V vs. RHE	1 mol L^-1 KOH, 1 mol L^-1 methanol, 1.4 V vs. RHE	FE_CO: 98%	FE_HCOOH: 92%	[83]
	biomass oxidation	4-methylbenzylalcohol	mITO/FDH	mTiO₂/ STEMPO/ DPP-CA	0.05 mol L^-1 NaHCO₃ (pH = 6.4), 0 V	0.1 mol L^-1 Na₂B₄O₇ (pH = 8.0), AM 1.5G, λ > 420 nm, 0 V	yield_4-MBAd: 3.1± 0.31 µmol cm^-2, FE: 108 ± 18%	yield_formate: 2.16 ± 0.26 µmol cm^-2, FE: 7 ± 17%	[148]
		glucose	Bi/GaN/Si	NiOOH/ α-Fe₂O₃	0.5 mol L^-1 KHCO₃ (pH = 7.5), AM 1.5G, −0.2 V vs. RHE	1 mol L^-1 KOH (pH = 13.6), AM 1.5G, 1.0 V vs. RHE	FE_HCOO−: 85.2%	FE_HCOO−: 96%	[73]
		glycerol	Pt/TiO₂/ n⁺p-SiNW loaded with S.ovata	Pt-Au/TiO₂/p⁺n-SiNW	bacterial medium with 50 mmol L^-1, MES (pH = 6.2), red light (740 nm), 20 mW cm⁻², −0.4 V vs. RHE	1 mol L^-1 KOH, 0.1 mol L^-1 glycerol, red light (740 nm), 20 mW cm⁻², 0.45 V vs. RHE	FE_acetate: 86.8 ± 14.0%	FE: 79.3 ± 9.1%	[98]
		glycerol	Ag	Ni/Si	1 mol L^-1 CsOH and 0.5 mol L^-1 glycerol	1 mol L^-1 CsOH, 0.5 mol L^-1 glycerol, 1000 mW cm^-2, AM 1.5G, 1.0 V vs. Ag/AgCl	FE_CO: 95%	FE: 85%	[156]
		glycerol	PVK/CuNF	Si/TiO₂/ PtAu	0.1 mol L^-1 KHCO₃ (pH = 6.8), AM 1.5G, 0 V vs. RHE	1 mol L^-1 KOH with 0.1 mol L^-1 glycerol (pH = 6.8), AM1.5G, 0 V vs. RHE	faradaic yield (FY)_C2: 5%-7%	FY: glycerate (53±1%), formate (18±4%), lactate (8±1%), acetate (7±2%)	[78]
		furfural	Au/α-Fe₂O₃/ RGO	Ru/RGO/Pt	0.1 mol L^-1 KOH, −0.6 V vs. SCE, λ = 400-450 nm	0.1 mol L^-1 KOH, 10 mmol FF, −0.6 V vs. SCE	yield_CH3OH: 51 μmol L^-1 cm^-2, yield_CO: 2 μmol L^-1 cm^-2	yield_2-FA: 59%, yield_5-HFA: 19%	[158]
	degradation of organic pollutants	benzyl alcohol	GDL-Cu₂O	TiO₂Nt-ZrO₂	0.1 mol L^-1 KHCO₃ (pH = 7)	0.1 mol L^-1 Na₂SO₄, 1.0 mmol L^-1 benzyl alcohol (pH = 7), 125W high-pressure mercury lamp, 1.5 V vs. Ag/AgCl	yield_CH3OH: 3.8 mmol/L, yield_CH3CH2OH: 0.96 mmol/L	degradation rate:68%	[74]
Nitrate or nitrite reduction	glycerol oxidation		Ru@TiNS/Ni/perovskite	Pt@TiNS	0.5 mol L^-1 KNO₃, 1.0 mol L^-1 KOH, AM 1.5G, 0.0 V vs. CE	0.5 mol L^-1 glycerol and 1.0 mol L^-1 KOH, 0.0 V vs. CE	FE_NH3: 99.5 ± 0.8%, SAP: 1744.9±20.6 µg_NH3 cm^-2 h^-1	FE: 98.1±2.4%	[89]
Nitrate or nitrite reduction	benzyl alcohol oxidation		TiO₂/AZO/ Cu₂O/Au	CdS/CdIn₂S₄	MeCN with 1 mol L^-1 KOH, AM 1.5G	MeCN with 0.2 mol L^-1 TBAHFP, AM 1.5G, 0.67 V vs. RHE	FE_NH3: 98.1%	FE_BAD: >99% selectivity: >98%	[84]
	cyclohexane oxidation		R-TiO₂	R-TiO₂	0.5 mol L^-1 Na₂CO₃-NaHCO₃ (pH = 9) with 0.1 mol L^-1 CYC and 1.8 mol L^-1 KNO₃, AM 1.5G, 1.6 V	0.5 mol L^-1 Na₂CO₃-NaHCO₃ (pH = 10) with 50 mmol L^-1 CYC, 1.6 V	Yield_CHO: 21.0 μmol cm^‒2 h^‒1	Yield_CYC: 0.43 μmol cm^‒2 h^‒1	[166]
Oxygen reduction	Degradation of pollutants	SMX	Sb-SA/Mxene	Fe-NC/Mxene	phosphate buffer solution (pH = 6.8), with 10.0 mg L^-1 SMX AM 1.5G, cell potential = 0.9 V	Phosphate, buffer solution (pH = 6.8), with 10.0 mg L^-1 SMX cell potential = 0.9 V	yield_H2O2: 343.4 μmol L^-1	removal efficiency: 94.7%	[170]
		4-FP	graphite plate	TiO₂ nanopillar	0.1 mol L^-1 Na₂SO₄, 20 ppm of 4-FP (pH = 6.0)	0.1 mol L^-1 Na₂SO₄, 20 ppm of 4-FP (pH = 6.0), 400 mW cm^-2, 1.0 V vs. RHE	—	degradation rate: 14.4 g h^‒1 m^‒2	[174]
		SMT	NADE	b-TiO_2-_x	0.1 mol L^-1 Na₂SO₄, 0.5 V	0.1 mol L^-1 Na₂SO₄ with 10 mg L^-1 SMT, 50 W LED lamp, 0.5 V	yield_H2O2: 6.83 μmol h^-1 cm^-2	degradation efficiency: 98.32%	[86]
		BPA	CF-DPA	WO₃	200 mmol L^-1 NaCl, pH = 5, -0.5 V vs. Ag/AgCl	200 mmol L^-1 NaCl with 10 mg L^-1 BPA, pH = 10.8, 1 sun illumination	yield_H2O2: 5.4 mmol L^-1	degradation efficiency: 92%	[95]
		CECs(TMP, SMX, CBZ DFC)	GDE	WO₃	simulated wastewater effluent or 7.5 mmol L^-1 Na₂SO₄, cell potential = 1.5 V	simulated wastewater effluent or 7.5 mmol L^-1 Na₂SO₄, concentration of each CEC (100 µg L^-1), λ = 200-480 nm, 86 W m^-2, cell potential = 1.5 V	FE_H2O2: 55%	degradation rate constants: TMP (5.67 × 10⁻³ min⁻¹), SMX (5.35 × 10⁻³ min⁻¹), CBZ (2.9 × 10⁻³ min⁻¹), DFC (4.35 × 10⁻³ min⁻¹)	[175]
		3-CP	BiOI	WO₃	0.1 mol L^-1 Na₂SO₄ with 10 mg L^-1 3-CP,1.8 V	0.1 mol L^-1 Na₂SO₄ with 10 mg L^-1 3-CP, 200 mW cm⁻²,1.8 V	—	degradation efficiency: 91.1%	[176]
		SDZ	NCDs/ Co₃O₄/ Ti mesh	TiO₂ NNs/Ti mesh	0.05 mol L^-1 Na₂SO₄ with 10 mg L^-1 SDZ, LED light, 0.4 V	0.05 mol L^-1 Na₂SO₄ with 10 mg L^-1 SDZ, LED light, 0.4 V	0.05 mol L^-1 Na₂SO₄, 10 mg L^-1 SDZ, LED light, 0.4 V	degradation efficiency: 98.54%	[85]
		MB	In₂S₃/ MnIn₂S₄/PVDF/ NF	In₂S₃/MnIn₂S₄/CP	0.1 mol L^-1 Na₂SO₄ with 10 mg L^-1 MB, (pH = 3), 300 W Xenon lamp, λ > 420 nm, −0.6 V vs. Ag/AgCl	35 g L^-1 NaCl 10 mg L^-1 MB 300 W Xenon lamp, λ > 420 nm, 1.3 V vs. Ag/AgCl	yield_H2O2: 2107.8 μmol L^-1, degradation efficiency: 95.1%	yield_HClO: 28.5 μmol L^-1, degradation efficiency: 98.5%	[82]
		TC	MCF	MgO/g- C₃N₄	0.1 mol L^-1 Na₂SO₄ with 20 mg L^-1 TC (pH = 5.6), −0.5 V vs. Ag/AgCl	0.1 mol L^-1 Na₂SO₄ with 20 mg L^-1 TC (pH = 5.6), LED lamp (380 nm < λ < 840 nm)	yield_H2O2: 10.19 mg L^-1	degradation efficiency: 100%	[90]
		2,4-D	modified carbon felt	Blue-TNTs	0.05 mol L^-1 Na₂SO₄with 10 mg L^-1 2,4-D, 0.2 mmol L^-1 FeSO₄, 2.4 V	0.05 mol L^-1 Na₂SO₄with 10 mg L^-1 2,4-D, 0.2 mmol L^-1 FeSO₄, 200 W, Xenon lamp (λ = 300- 900 nm), 80 mW cm^-2, 2.4 V	yield_H2O2: 9.7 mg L^-1	degradation efficiency: 100%	[76]
Enzymes activation	PET microplastics conversion		AQC/ CFP	Zr:α-Fe₂O₃	100 mmol L^-1 KPi buffer (pH = 6.0), 0.16 V vs. RHE	50 mg mL^-1 PET microplastics, 5 mol L^-1 NaOH, AM 1.5G, 1.0 V vs. RHE	formate and acetate produced by Zr:α-Fe₂O₃	yield_H2O2: 1.85 ± 0.07 mmol L^-1 h^-1, yield_{(R)-1- phenylethanol}: 1.63 ± 0.08 mmol L^-1 h^-1, TOF_rAaeUPO: 32700±1500 h⁻¹	[183]
Enzymes activation	PET microplastics conversion				100 mmol L^-1 NaPi buffer (pH = 7.5), −0.2 V vs. RHE			yield_NADH: 1.19± 0.07 mol L^-1 h^-1, yield_L-glutamate: 2.74 ± 0.11 mmol L^-1 h^-1, TOF_GDH: 5500 ± 200 h⁻¹, yield_{(R)-2-methylcyclohexanone}: 1.16 ± 0.16 mol L^-1 h^-1, TOF_TsOYE: 230 ± 30 h⁻¹

Fig. 21. (a) Optimum reaction potentials of (photo)athode, (photo)anode and coupling systems. (b) The standard electrochemical potential of most reviewed reactions.

Fig. 22. Potential dependence of in situ first-order derivatives of the XANES spectra (a) and EXAFS spectra (b) of the CuSiOx under CO2RR using chronoamperometry [188]. Copyright 2023, American Chemical Society. In situ Raman spectra of ZIF-CoNi (c) and ZIF-CoNi(g) (d) during electrochemical reconstruction [191]. Copyright 2024, Wiley-VCH. (e) In situ Raman spectra of Bi2S3/CP as a function of the applied potentials [192]. Copyright 2024, Wiley-VCH. In situ FTIR spectra of isopropanol (f) and n-propanol (g) adsorbed on TiO2, Bi2O3, and Bi2O3/TiO2 [195]. Copyright 2022, American Chemical Society.

Fig. 23. (a) In situ EPR spectrum detected from the photolysis of TiO2-Ov-400; [167] Copyright 2021, Springer Nature Limited. (b) In situ XRD patterns at ?0.4 V for various time points [203]. Copyright 2023, Wiley-VCH. In situ XPS spectra of Pd-ZIS and ZIS: S 2p (c) and Pd 3d (d) [206]. Copyright 2023, American Chemical Society.

Fig. 24. Schematic illustration of challenges and future perspectives for PEC coupling reactions.

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先进的光电催化耦合反应

Advanced photoelectrocatalytic coupling reactions

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