光电催化析氧和CO2还原反应催化剂的研究进展

doi:10.1016/S1872-2067(24)60053-7

催化学报 ›› 2024, Vol. 62: 53-107.DOI: 10.1016/S1872-2067(24)60053-7

光电催化析氧和CO₂还原反应催化剂的研究进展

朱鸿睿, 徐慧民, 黄陈金, 张志杰, 詹麒尼, 帅婷玉, 李高仁^*()

四川大学材料科学与工程学院, 四川成都 610065

收稿日期:2024-03-08 接受日期:2024-05-06 出版日期:2024-07-18 发布日期:2024-07-10
通讯作者: *电子信箱: ligaoren@scu.edu.cn (李高仁).
基金资助:
国家自然科学基金(52373215);四川科技项目(2023NSFSC0086);中央高校基本研究经费(YJ2021156)

Recent advances of the catalysts for photoelectrocatalytic oxygen evolution and CO₂ reduction reactions

Hong-Rui Zhu, Hui-Min Xu, Chen-Jin Huang, Zhi-Jie Zhang, Qi-Ni Zhan, Ting-Yu Shuai, Gao-Ren Li^*()

College of Materials Science and Engineering, Sichuan University, Chengdu 610065, Sichuan, China

Received:2024-03-08 Accepted:2024-05-06 Online:2024-07-18 Published:2024-07-10
Contact: *E-mail: ligaoren@scu.edu.cn (G.-R. Li).
About author:Gao-Ren Li (College of Materials Science and Engineering, Sichuan University). Prof. Gao-Ren Li received his B.A. degree from East China University of Technology (China) in 2000, and Ph.D. degree from Sun Yat-sen University (China) in 2005. From September 2005 to September 2021, he worked in School of Chemistry, Sun Yat-sen University. Since October 2021, he has been working in College of Materials Science and Engineering, Sichuan University. His current research interests mainly focus on electrocatalysis, especially water splitting and electrochemical conversion of CO₂.
Supported by:
National Natural Science Foundation of China(52373215);Sichuan Science and Technology Program(2023NSFSC0086);Fundamental Research Funds for the Central Universities(YJ2021156)

摘要/Abstract

摘要：

随着日益增加的化石能源消耗和环境污染, 新能源和环境友好型技术的应用对工业发展发挥着重要作用. 利用太阳能及电能进行各种催化反应的光电催化(PEC)是一种有应用前景的技术, 与传统催化技术相比, 具有环保节能、效率高的优势. 析氧反应(OER)和CO₂还原反应(CO₂RR)是两种具有能源及环境应用潜力的催化反应. PEC OER对基于水氧化和其他相关氧化反应的可再生能源技术具有重要作用. PEC CO₂RR可以将CO₂转化为高附加值化学品, 实现CO₂的合理利用. 上述两种技术均具有较大的研究价值和应用前景.

本综述首先阐述了电催化和光催化技术的优缺点. 由于工业上使用电催化技术会消耗煤和石油等化石能源, 有污染环境的风险, 且长期的用电成本会影响最终的盈利; 而使用光催化技术又面临着反应效率不理想、稳定性差和可见光吸收率低等缺点. 一方面, PEC技术可以解决光催化中光生电子-空穴对复合速度快、反应时间长的缺点; 另一方面, PEC技术可以降低电催化过程中在高电流密度下反应所需的过电位, 在节省电能的同时提高反应效率. 此外, 系统地介绍了光电催化产氧和CO₂RR的机理和参数、催化剂类型、评价标准以及近年来的研究进展. 对于反应条件, 光电催化和电催化所使用的基础仪器基本相同, 而光电催化是在电催化的基础之上施加外部光源, 利用光能进一步提高反应效率和稳定性. 光电催化和电催化的反应机理也基本一致, 不同的是光电催化的评价标准与电催化有所不同. 在光照作用下, 除了关注特定电压下的电流密度、选择性和稳定性外, 研究者们更关注应用偏压光子电流转换效率(ABPE)和入射光子对电流的效率(IPCE)的影响. 同时, 介绍了用于PEC OER和CO₂RR催化剂的类别、优势、合成方法、设计原则和改性策略. 就目前研究而言, 光电催化性能优异的催化剂一般都具有导电性良好、光吸收效率高和载流子分离速率快等特点. 随着对光电催化技术研究地深入, 通过掺杂、制造缺陷、设计异质结、负载单/双原子和改变反应微环境等方法有效地提升了催化效率和稳定性. 在上述研究基础上, 还扩展性地阐述光热催化、光酶催化等近几年的热点技术, 这些技术均具有反应条件温和、过程简单和效率高等特点, 在未来具有较大的研究价值. 最后, 展望了PEC技术的未来发展趋势和前景, 重点关注了它在工业上的应用前景和价值.

在未来, PEC技术将朝着智能化、创新和环保的方向发展. 通过先进的理论技术(如理论计算、机器学习、分子动力学模拟等)和原位表征探索反应机理, 实现低成本、绿色和智能化的技术以迎接未来实现大规模工业化的挑战, 从而在盈利和环保两者之间实现“双赢”. 希望本文能帮助读者更快及更全面地了解PEC技术的基本原理、常用催化剂、改性策略、拓展技术、应用前景和发展趋势, 从而为读者提供可借鉴的研究思路.

关键词: 光电催化, 催化剂设计, 催化剂制备, 析氧反应, 二氧化碳还原反应

Abstract:

Increasing global energy consumption and environmental pollution make the use of new energy sources and environmentally friendly technologies essential to meet the diverse needs of industries. Photoelectrocatalysis is a promising method of utilising solar and electrical energy for various catalytic reactions with significant environmental and energy saving benefits. And photoelectrocatalytic (PEC) oxygen evolution reaction (OER) and CO₂ reduction reaction (CO₂RR) are two catalytic reactions with great potential for energy and environmental applications. PEC OER is critical for renewable energy technologies for water oxidation and other related oxidation reactions. PEC CO₂RR converts carbon dioxide into high-value products via a catalyst, enabling the rational use of carbon dioxide and the reduction of greenhouse gas emissions. Both technologies are efficient, environmentally friendly, and sustainable. However, further research and optimisation are needed to promote the industrial application of both technologies for energy conversion and environmental protection. This paper reviews the research progress of PEC CO₂RR and OER catalysts in recent years, including detailed descriptions of catalyst types, reaction mechanisms and performance tests. Finally, the paper considers the future trends and prospects of PEC technology, providing new insights into the technology and research directions for PEC OER and CO₂RR catalysts.

Key words: Photoelectrocatalysis, Catalyst design, Catalyst fabrication, Oxygen evolution reaction, CO₂ reduction reaction

朱鸿睿, 徐慧民, 黄陈金, 张志杰, 詹麒尼, 帅婷玉, 李高仁. 光电催化析氧和CO₂还原反应催化剂的研究进展[J]. 催化学报, 2024, 62: 53-107.

Hong-Rui Zhu, Hui-Min Xu, Chen-Jin Huang, Zhi-Jie Zhang, Qi-Ni Zhan, Ting-Yu Shuai, Gao-Ren Li. Recent advances of the catalysts for photoelectrocatalytic oxygen evolution and CO₂ reduction reactions[J]. Chinese Journal of Catalysis, 2024, 62: 53-107.

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图/表 50

Scheme 1. Advantages and disadvantages of photocatalysis and electrocatalysis. Realization of PEC by avoiding the disadvantages and integrating the advantages.

Table 1 Pathways of PEC OER (under alkaline conditions) [93??????-100].

Number	Reaction
1	4OH⁻ → O₂ + 2H₂O + 4e⁻
2	M + OH⁻ → MOH + e⁻
3	MOH + OH⁻ → MO + H₂O + e⁻
4	MO + OH⁻→ MOOH + e⁻
5	MOOH + OH⁻ → M + O₂ + H₂O + e⁻

Scheme 2. Classification of PEC catalysts for OER.

Fig. 1. Classification of PEC catalysts for OER.

Fig. 2. BiVO4-based catalysts for PEC OER. (a) Schematic diagram of PEC OER installation. (b,c) Chopped J-V curves of different photoanodes. (d) ABPE values of different photoanodes. (e) ABPE values of the NiFeOOH/MoOx/MQD/BiVO4 with other BiVO4-based photoanodes. (f,?g) Illustrations of the charge transfer process for BiVO4 and NiFeOOH/MoOx/MQD/BiVO4. Reprinted with permission from Ref. [139]. Copyright 2022, John Wiley and Sons. (h) Schematic diagram of the preparation of photoanodes. (i) Chopped LSV curves of Co-agZIF-62/BiVO4 photoanodes with different cobalt-contents. (j) LSV curves of different photoanodes. (k) ABPE values, (l) IPCE values. (m,n) Mechanistic diagram of the charge transfer process occurring at different photoanodes. Reprinted with permission from Ref. [140]. Copyright 2023, John Wiley and Sons.

Fig. 3. Fe2O3-based catalysts for PEC OER. (a) Schematic representation of the operando XAS experiment during PEC OER. (b) LSV of several FTO/Ni0.8Fe0.2OOH catalysts prepared with different number of cycles. (c) LSV of different photoanodes. The inset in each panel shows schematics of the working electrodes. Reprinted with permission from Ref. [141]. Copyright 2021, American Chemical Society. (d) Schematic illustration for the synthesis of SAs Pt: Fe2O3. (e) SEM image. (f) J-V curves of different samples. (g) ABPE value of SAs Pt: Fe2O3-Ov. Reprinted with permission from Ref. [142]. Copyright 2023, Nature Publishing Group.

Fig. 4. Metal oxide-based catalysts for PEC OER. (a) Schematic illustration of the TQ-NiFe grown on the carbon cloth. (b) EDS maps. (c) PEC OER performance of the TQ-NiFe under dark and illumination. (d) Increased current densities for TQ-NiFe under irradiation. (e) Tafel plots for TQ-NiFe under dark. (f) Reaction activation energy of PEC OER for TQ-NiFe. Reprinted with permission from Ref. [143]. Copyright 2023, Springer Nature. (g) Preparation process of different photoanodes. (h) LSV curves of different photoanodes under illumination in different solutions. (i) Charge separation efficiencies. (j) The formation energy for Sn-doping, Ge-doping, and Ge:Sn co-doping in Fe2O3. (k) DFT calculations of the atomic arrangement of Fe2O3 in different structures. (l) Gibbs free energy diagram for the formation of reaction intermediates from pure Fe2O3 and Ge-Fe2O3. Reprinted with permission from Ref. [144]. Copyright 2021, Springer Nature.

Fig. 5. Ta3N5-based catalysts for PEC OER. SEM images of raw-Ta3N5 (a), TaCl5-Ta3N5 (b). Current-potential (j-E) curves of raw-Ta3N5, TaCl5-Ta3N, heated-Ta3N5, necked-Ta3N5 (c) and CoPi/necked-Ta3N5 electrode (d). Reprinted with permission from Ref. [152]. Copyright 2016, Royal Society of Chemistry. (e) HRTEM image of Ta3N5. (f) HRTEM image of the post treated Ta3N5(P). (g) LSV curves of pure Ta3N5, Ta3N5(P) photoanodes and the Ta3N5(P) photoanode under illumination. (h) Schematic structure of the synthesized Ta3N5 photoanodes system. (i) LSV curves of different samples; inset Figure illustrates the saturated photocurrent curve. Reprinted with permission from Ref. [153]. Copyright 2016, Royal Society of Chemistry.

Fig. 6. Ta3N5-based catalysts for PEC OER. (a,b) HRTEM images of NiCoFe-Bi/gradient-Mg:Ta3N5/Nb. (c) J-V curves of different catalysts. (d) IPCE spectrum of the NiCoFe-Bi/gradient-Mg:Ta3N5/Nb photoanode. (e) ABPE of the photoanodes. Reprinted with permission from Ref. [154]. Copyright 2020, Springer Nature. (f) SEM image of Ta3N5-NRs/Ta3N5-thin film/GaN. (g,h) HRTEM images of FeNiCoOx/Ta3N5-NRs. (i) Schematic diagram of the prepared device and reaction mechanism. (j) J-Va curves of bis-CuInSe2 (dashed line: independent; solid line: behind the photoanode) and Ta3N5-NR. (k) Stochiometric (2:1) production of hydrogen and oxygen gases. Reprinted with permission from Ref. [155]. Copyright 2023, John Wiley and Sons.

Fig. 7. Ta3N5-based catalysts for PEC OER. Photographic image (a), SEM image (b) of Ta3N5/GaN/Al2O3 thin film. (c) i-E curve obtained from NiFeOx/Ta3N5/GaN/Al2O3 photoanode. (d) Half-cell solar-to-hydrogen energy conversion efficiency of NiFeOx/Ta3N5/GaN/Al2O3 photoanode as a function of potential. (e) Half-cell solar-to-hydrogen energy conversion efficiency of NiFeOx/Ta3N5/GaN/Al2O3 photoanode as a function of potential. (f) Relationship between STH values and reaction times. Reprinted with permission from Ref. [156]. Copyright 2019, John Wiley and Sons. Structures and morphological properties of the Ta3N5-NRs and Ba:Ta3N5-NRs specimens. (g) XRD spectrum. SEM images of the Ba: Ta3N5-NRs (h-k). (l) J-V curves. (m) Half-cell solar-to-hydrogen (HC-STH) curves. (n) IPCE spectra. (o) Integrated photocurrent densities. Reprinted with permission from Ref. [157]. Copyright 2021, Royal Society of Chemistry.

Fig. 8. CdIn2S4-based catalysts for PEC OER. (a) Schematic representation of the synthesis of VS-CdIn2S4. (b) SEM image of Vs-CIS-500. (c) J-V plots measured under dark and illumination. (d) APBE values under dark and light conditions. (e) IPCE spectra under single wavelength reaction conditions. Reprinted with permission from Ref. [158]. Copyright 2020, Springer Nature. (f) SEM images of nanoflakes. (g) LSV curves of modified SnS2 under backlighting conditions. (h) IPCE curves of SnS2 with front and back lighting conditions. Reprinted with permission from Ref. [159]. Copyright 2019, John Wiley and Sons.

Fig. 9. CdS-based catalysts for PEC OER. (a) Schematic representation of the conversion of CdS nfa to CdS@CdIn2S4 nfa. (b,c) SEM images of CdS@CdIn2S4 NFAs. (d) LSV under illumination. (e) Photoelectric conversion efficiencies of CdS NFAs and CdS@CdIn2S4 NFAs. Reprinted with permission from Ref. [160]. Copyright 2017, Royal Society of Chemistry. (f) Schematic illustration of TiO2/CdS/MoS2 synthesis. (g,h) SEM images of TiO2/CdS/MoS2 (i) LSV curves for different samples. (j) Stability testing of photoanodes. IPCE curves (k) and UV-vis absorbance spectra (l) of different samples. Reprinted with permission from Ref. [161]. Copyright 2019, Elsevier.

Fig. 10. Polymers-based catalysts for PEC OER. (a) Chemical structures of PNDITCVT (PA) and PBDTTTPD (PD). (b) Energy levels of PA and PD, sacrificial oxidation potential and OER potential. (c) Schematic of FTO/mZnO/BHJ composite for PEC OER. (d) LSV scans (under intermittent illumination). (e) IPCE spectrum of FTO/mZnO/BHJ/PTAA/LI. (f) CA curve of FTO/mZnO/BHJ/LIO and FTO/mZnO/BHJ/PTAA/LI for PEC OER. Reprinted with permission from Ref. [170]. Copyright 2021, Springer Nature.

Fig. 11. Polymers-based catalysts for PEC OER. (a) Schematic diagram of a PEC cell with an IO-TiO2|dpp|Pos-PSII photoanode connected to an IO-ITO|H2ase cathode (right). SEM image of the IO-TiO2 photoanode structure (left). (b) Solution UV-vis spectra of dpp and PSII. (c) The mode of carrier transfer between different materials and the associated redox potentials. (d) Chronoamperometry for the determination of the onset potential (Eonset) and limiting photocurrent for the IO-TiO2|dpp|Pos-PSII photoanode. (e) Photocurrent density (J) plotted as a function of Eapp determined by the stepped potential chronoamperometry in (d). Reprinted with permission from Ref. [171]. Copyright 2018, Springer Nature.

Fig. 12. LDH-based catalysts for PEC OER. (a) SEM image of the InN/PM6. (b) XRD spectrum of InN and InN/PM6. (c) FT-IR spectrum of PM6 and InN/PM6. LSV curves (d) and ABPE curves (e) of different photoanodes. (f) EIS spectra of all photoanodes. Reprinted with permission from Ref. [172]. Copyright 2023, Royal Society of Chemistry. (g) Schematic representation of the synthesis of BV/P3HT-CuPc/LDH. (h,i) LSV curves of different photoanode under illumination in (h) KBi and (i) 0.5 mol L?1 Na2SO3. IPCE (j) and ABPE curves (k) of the different photoanode. Reprinted with permission from Ref. [174]. Copyright 2022, Elsevier.

Fig. 13. Carbon-based catalysts for PEC OER. (a) Schematic representation of the synthesis of undoped and N, S co-doped GQDs. TEM (b) and HRTEM image (c). (d) HER and OER LSV curves of NS-GQD/graphene. Cathodic (e) and anodic electrochemical properties (f) of NS-GQD/ graphene in ethanol. (g) Electrocatalytic activity of HER and OER of NS-GQD/graphene. Reprinted with permission from Ref. [179]. Copyright 2020, American Chemical Society. (h) Schematic representation of the PEC OER of the material synthesised. (i) Energy band spectra of InSe/Gr. (j) PEC OER model for DFT simulation of InSe/Gr. (k) LSV curves of InSe/Gr after different illumination times. (l) Optical current density under dark and light conditions. Reprinted with permission from Ref. [180]. Copyright 2021, Springer Nature.

Fig. 14. Carbon-based catalysts for PEC OER. (a) Schematic synthesis of n-Si/TiO2/NiOx/pGr. (b) Raman spectra for different samples. (c) Current density-potential (J-V) curves of the different photoanode. (d) Von and J1.23 values for different photoanodes. (e) Representative OER polarization plots in 1 mol L-1 KOH of different samples. (f) Typical Nyquist plots measured for different photoanodes. Reprinted with permission from Ref. [181]. Copyright 2023, John Wiley and Sons. (g) Schematic procedure for the photoanode preparation. (h-j) SEM images of the representative n-Si/TiO2/NiOx/SLG/Ni photoanode. (k) J-V curves of different samples. (l) ABPE values of n-Si/TiO2/NiOx/SLG/Ni and n-Si/TiO2/NiOx/SLG/Ni without SLG. Reprinted with permission from Ref. [182]. Copyright 2022, John Wiley and Sons.

Fig. 15. MOF-based catalysts for PEC OER. (a) The synthesis of core-shell Ov-BiVO4@NiFe-MOFs. J-V curves (b), ABPEs (c), IPCE (d) and EIS spectrum (e) of different photoanodes. Reprinted with permission from Ref.[187]. Copyright 2021, John Wiley and Sons. (f) Schematic flow diagram of the synthesis of different photoanodes. (g,h) LSV curves under light and dark conditions. ABPE values (i) and IPCE spectrum (j) (inset shows the APCE spectra) of different samples. Reprinted with permission from Ref. [188]. Copyright 2023, John Wiley and Sons.

Fig. 16. MOF-based catalysts for PEC OER. (a) Schematic of TiO2 NR growth on FTO and photographs of different lengths of TiO2 NR grown by controlling the reaction time. (b) J-V curves of TiO2 NRs and MIL(125)-NH2/TiO2 NRs. (c) Photocurrent density of different samples. IPCE (d) and EIS spectrum (e) of TiO2 NRs and MIL(125)-NH2-TiO2 NRs. Reprinted with permission from Ref. [189]. Copyright 2019, Elsevier. (f) Schematic of the synthesis of core-shell Ti: analysis Fe2O3@CoFe-cMOFs photoanode. (g) LSV curves (1 mol L?1 KOH, pH 13.6), (h) ABPE, IPCE (i) and LSV curves (j) (0.2 mol L?1 Na2SO3) of different samples. Reprinted with permission from Ref. [59]. Copyright 2022, Elsevier.

Table 2 Half reactions of CO2 reduction for possible processes along with the corresponding standard redox potential (25 °C, 1 atmosphere of gases and 1 mol L?1 solutes in aqueous solution) [173???????????-185].

Number	Reaction	E^θ/V (vs. SHE)
1	CO₂ + e⁻ → CO₂⁻	-1.900
2	CO₂ + 2H⁺ + 2e⁻ → CO + H₂O	-0.530
3	CO₂ + H₂O + 2e⁻ → CO + 2OH⁻	-1.347
4	CO₂ + 2H⁺ + 2e⁻ → HCOOH	-0.610
5	CO₂ + H₂O + 2e⁻ → HCOO⁻ + OH⁻	-1.491
6	CO₂ + 4H⁺+ 4e⁻ → HCOH + H₂O	-0.480
7	CO₂ + 3H₂O + 4e⁻ → HCOH + 4OH⁻	-1.311
8	CO₂ + 6H⁺ + 6e⁻ → CH₃OH + H₂O	-0.380
9	CO₂ + 5H₂O + 6e⁻ →CH₃OH + 6OH⁻	-1.225
10	CO₂ + 6H₂O + 8e⁻ → CH₄ + 8OH⁻	-1.072
11	2CO₂ + 12H⁺ + 12e⁻ → C₂H₄ + 4H₂O	-0.340
12	2CO₂ + 8H₂O + 12e⁻ → C₂H₄ + 12OH⁻	-1.177
13	2CO₂ + 14H⁺ + 14e⁻ → C₂H₆ + 4H₂O	-0.270

Table 3 Onset potentials, photocurrent densities, electrolytes, ABPE and IPCE values for different catalysts.

Catalyst	Onset potential (V_RHE)	J_photo at 1.23 V (mA cm⁻²)	Electrolyte	ABPE (%)	IPCE (%)	Ref.
b-BiVO₄/TiO_2-_x	—	6.12	1 mol L^‒1 Na2_SO₃	2.5	94.7	[135⇓⇓-138]
NiFeOOH/MoO_x/MQD/BiVO₄	—	5.85	pH9.3-KBi	2.43	90	[139]
Co-agZIF-62/NiO/MO	—	5.34	pH9.5-KBi	1.67	90.8	[140]
SAs Pt: Fe₂O₃	0.627	3.65	1 mol L^‒1 KOH	0.68	38	[142]
CdS-CdSe/MoS₂/NiFe-LDH	0.243	10 at 1.229 V_RHE	1 mol L^‒1 KOH	—	40	[143]
NiFeO_x@Ge-PH/PSC	0.39	4.6	1 mol L^‒1 NaOH	—	—	[144]
necked-Ta₃N₅	—	6.1	1 mol L^‒1 NaOH	—	50	[152]
Ni(OH)_x/Fh/Ta₃N₅ (P)	0.55	6.8	1 mol L^‒1 NaOH	2.5	90-100	[153]
NiCoFe-bi/gradient-Mg: Ta₃N₅/Nb	0.4	7	1 mol L^‒1 KOH	3.25 ± 0.05	85	[154]
Ta₃N₅-TF/GaN/Al₂O₃	0.75	10.8	1 mol L^‒1 KOH	1.5	90	[155]
NiFeO_x/Ta₃N₅/GaN/Al₂O₃	0.65	6.3	0.2 mol L^‒1 KPi	1.15	66	[156]
Ba: Ta₃N₅-NRs	0.6	5.5	0.5 mol L^‒1 KH₂PO₄	0.76	48	[157]
V_s-CdIn₂S₄	0.14	2.49	0.25 mol L^‒1 Na₂S	5.73	60	[158]
SnS₂	—	4.5	0.1 mol L^‒1 KI + 1 mol L^‒1 H₂SO₄	—	~100	[159]
CdS@CdIn₂S₄ NFA	0.49	5.5	0.25 mol L^‒1 Na₂S/0.35 mol L^‒1 Na₂SO₃	0.45	—	[160]
TiO₂/CdS/MoS₂	-0.09	3.25 at 1.229 V_RHE	0.35 mol L^‒1 Na₂SO₃, 0.25 mol L^‒1 Na₂S	—	45	[161]
FTO/mZnO/BHJ	0.7	3	0.1 mol L^‒1 NaBi	—	>25	[170]
InN/PM6/NiFe LDH	—	3.21	0.1 mol L^‒1 KOH	0.66	—	[172]
BV/P3HT-CuPc/LDH	0.23	5.54	0.5 mol L^‒1 Na₂SO₃	1.36	60	[174]
InSe/Gr	0.42	>10	0.2 mol L^‒1 NaOH	—	—	[180]
n-Si/TiO₂/NiO_x/pGr	1.13 ± 0.01	8.08 ± 1.0	1 mol L^‒1 KOH	—	—	[181]
n-Si/TiO₂/NiO_x/SLG	1.03 ± 0.01	21.1±0.96	1 mol L^‒1 KOH	1.0	—	[182]
Ov-BiVO₄@NiFe-MOFs	—	5.3 ± 0.15	0.5 mol L^‒1 KBi	1.62	72.9	[187]
BiVO₄/CoFe MOF	0.79	3.92	1 mol L^‒1 KPi	1.09	89	[188]
MIL(125)-NH₂/TiO₂	~0.4	1.63	1 mol L^‒1 NaOH	—	84.4	[189]

Fig. 17. The schematic diagram of the electrolysis device.

Fig. 18. Classification of PEC catalysts for CO2RR.

Fig. 19. (a) Schematic for the photoelectrochemical deposition of Cu onto n+p-Si. (b) n+p-Si μW and planar n+p-Si in the Jph-E curve, before (solid line) and after (dashed line) passing ?1.00 C cm-2. LSV curves were recorded at ?200 mV s-1. An electropolished Cu film (c), and a n+p-Si μW/Cu photocathode (d) under illumination. Reprinted with permission from Ref. [90]. Copyright 2020, American Chemical Society. (e) The array has a nanowire diameter of 400 nm and a length of 21 μm. (f) Schematic illustration showing the dopant layer and charge separation. (g) Diagram of the custom cell. (h) Mass loading dependence. Comparison of FE (i) and semilog plots (j) of jC2H4 between 40 μg cm?2 CuNPs on illuminated SiNWs and 69 μg cm?2 CuNPs. Reprinted with permission from Ref. [215]. Copyright 2022, American Chemical Society.

Fig. 20. Cu-based catalysts for PEC CO2RR. (a) Charge transfer processes on the Cu2+-OH (aq) surface. (b) Schematic representation of the charge transfer within the system in the absence of Cu2+-OH (aq) catalyst in the reaction environment. (c) Chronoamperometry of Cu2O and Ag/Cu2O photocathodes. (d) J-t curves of Cu2O and Ag/Cu2O. (e) LSV curves for different photocathodes. (f) FE on Ag/Cu2O/ZS/FTO photocathode for PEC CO2RR. Reprinted with permission from Ref. [94]. Copyright 2021, Springer Nature. (g) Schematic of Cu-MOF/Cu2O in acetonitrile solution for PEC CO2RR. (h) FE of CO production for PEC CO2RR in dark and (i) solar-to-CO (STC) efficiencies. Reprinted with permission from Ref. [216]. Copyright 2019, American Chemical Society.

Fig. 21. GaN-based catalysts for PEC CO2RR. (a) Molecular structure of n-GaN nanowires and composites on silicon substrates. (b) SEM images of n-GaN nanowires grown on the substrate. (c) Relative energy levels in the composites, red arrows indicate the electron transfer paths under light conditions. (d) Schematic representation of Si|mesoTiO2|CotpyP photocathode. (e) Bias photocurrent densities of different samples in phosphate buffer after argon degassing under illumination conditions. (f) PEC CO2RR stability performance test, the small graph shows the FE efficiency for different products. Reprinted with permission from Ref. [217]. Copyright 2019, Springer Nature. (g) SEM images of Ag-modified GaN NWs grow on n-p silicon wafers and schematic representation of the synthesis process with AgX co-catalysts (X = Cl, Br, I). (h) Energy band diagram of AgX/GaN/Si photocathode. (i) TEM images of Ag/GaN NWs. (j) FE efficiencies and ratios of different gas products measured over 12 h at different potentials and light conditions. Reprinted with permission from Ref. [218]. Copyright 2022, American Chemical Society.

Fig. 22. GaN-based catalysts for PEC CO2RR. (a) Schematic representation of the synthesis of CuS/GaN/Si on n+-p silicon wafers. LSV curves (b), FEHCOOH (c), and jHCOOH (d) of different catalysts. (e) PEC CO2 RR performance of CuS/GaN/Si in different reaction environments. Reprinted with permission from Ref. [219]. Copyright 2021, American Chemical Society. (f) Schematic diagram of a plant to produce formate from biomass material and CO2. (g) Schematic of Bi/GaN/Si for HCOO? production by PEC CO2RR. (h) SEM image and photograph of Bi/GaN/Si. (i) LSV curves, (j) FEs and jHCOO? at varied applied potentials over Bi/GaN/Si. Reprinted with permission from Ref. [220]. Copyright 2023, Springer Nature.

Fig. 23. GaN-based catalysts for PEC CO2RR. (a) Schematic illustration of the structure. (b) SEM images display GaN nanowires vertically grown on a Pt-TiO2/GaN/n-p Si silicon substrate. (c) J-V curves of different samples. (d) FEs for CO and H2. Reprinted with permission from Ref. [221]. Copyright 2018, American Chemical Society. Schematic (e,f) and energy diagram (g) of Sn NP/GaN NW/Si for PEC CO2RR with different solutions. (h) The black curve is the J-V curve of Sn NP/GaN NW/Si measured under dark conditions. (i) FEs of different products of Sn-, Co-, and Ni-decorated GaN NW/Si. Reprinted with permission from Ref. [14]. Copyright 2019, Royal Society of Chemistry.

Fig. 24. TiO2-based catalysts for PEC CO2RR. (a) Schematic representation of Si|mesoTiO2|CotpyP photocathode. TON for the CO2 reduction products (b) and Faradaic efficiencies for all products (c). (d) CPPE (J-t) traces of different photocathodes under continuous illumination and an hourly 2min dark chop. (e) LSVs of Si|mesoTiO2 and Si|mesoTiO2|CotpyP with chopped illumination. (f) Si|mesoTiO2|CotpyP and products of control experiments. Reprinted with permission from Ref. [97]. Copyright 2019, Springer Nature. (g) Schematic diagram of energy bands of amorphous silicon composites for PEC CO2RR. (h) PEC J-V curves of different photocathodes. Different product FEs after PEC CO2RR (i) a-Si/TiO2, (j) ST-4Au and (k) ST-7Au. Reprinted with permission from Ref. [222]. Copyright 2019, Royal Society of Chemistry.

Fig. 25. Porphyrin-based catalysts for PEC CO2RR. (a) Schematic representation of photosynthesis and PEC CO2RR for chlorophyll and HNTM-Au-SA, respectively. (b) TEM image. (c) STEM image. (d) FT-EXAFS spectra of different samples, and Au foil at Au L3 edge. (e) The FT-EXAFS space-fitting curve of HNTM-Au-SA. (f) FEmax and product observed on each catalyst. (g) Calculated by DFT free energy of CO2 to CO. Reprinted with permission from Ref. [225]. Copyright 2019, Springer Nature. (h) Schematic representation of the synthesis process of Cu@porphyrin-COFs nanorods. FEs of total carbon-based products of PEC CO2 reduction on (i) [OH]-H2P-COF/CF; (j) Cu@[OH]-H2P-COF/CF. (k) Different photocathodes at -1.0 V. (l) Different reaction condition of CO2 reduction of Cu@[OH]-H2P-COF/CF photocathode. Reprinted with permission from Ref. [226]. Copyright 2020, Elsevier.

Fig. 26. Porphyrin-based catalysts for PEC CO2RR. (a) Schematic diagram of different photocathodes. LSV curves (b), CO FEs (c) of different electrodes. (d) Chronoamperometric stability tests on Si/rGO-Co at ?0.1 V vs. RHE. (e) The photocurrent densities and reaction stability in this work are compared to similar work that has been reported previously. Reprinted with permission from Ref. [227]. Copyright 2023, John Wiley and Sons. (f) Schematic illustration of the construction of Co-Bpy-COF and its Postsynthetic Modification to Co-Bpy-COF-Rux. (g) LSV curves of different samples. (h) LSV curves of Co-Bpy-COF and Co-Bpy-COF-Ru1/2. Comparison of the PEC CO2RR performance: FECO (i), and TOF (j) at different potentials. Reprinted with permission from Ref. [164]. Copyright 2023, American Chemical Society.

Fig. 27. Doping modification strategies for catalysts in PEC OER. (a) Schematic image of the synthetic Si-ZnAl-LDH process. (b) TEM image of Si-ZnAl-LDH nanosheet. (c,d) AFM results of ZnAl-LDH and Si-ZnAl-LDH. LSV curves (e), cdl results (f) and EIS curves (g) of different samples. (h) Long-term stability test of Si-ZnAl-LDH. Reprinted with permission from Ref. [239]. Copyright 2024, Elsevier. (i) Schematic diagram of the Mn-FeBTC/NIF synthesis process. (j) Schematic representation of the competitive reactions that occur on the substrate surface during electrosynthesis. LSV curves (k), Tafel slope (l), EIS curves (m), and Cdl results (n) of different samples under different reaction conditions. Reprinted with permission from Ref. [240]. Copyright 2023, Elsevier.

Fig. 28. Manufacturing defects for catalysts in PEC OER. (a1-a6) AC-STEM images of the BVO (a1-a3) and B(VO)1-δ (a4-a6) films. (b,c) Schematic illustration of the DMF post-treatment induced VO4 vacancy gradient in B(VO)1-δ and its gradient band structure. LSV curves (d), ABPE curves (e), IPCE curves (f) of BVO and B(VO)1-δ photoanodes. Reprinted with permission from Ref. [247]. Copyright 2024, John Wiley and Sons. (g) Surface photovoltage images different VO concentration of PbCrO4. The surface photovoltage images were calculated using contact potential difference (CPD) under dark and light conditions (CPDlight-CPDdark). (h) Wavelength-dependent surface photovoltage spectra. (i) Open-circuit potential (OCP) of O-rich and O-poor PbCrO4 under chopped light illumination. (j) Photovoltage (OCPdark-OCPlight) was determined from open-circuit potential tests. (k) LSV curves of optimal PbCrO4 photoanodes. (l) Statistics of photocurrent density from different VO concentrations. Reprinted with permission from Ref. [71]. Copyright 2023, John Wiley and Sons.

Fig. 29. Single or diatomic strategies for catalysts in PEC OER. (a) HAADF-STEM image of Co-C3N4. (b) Co K-edge XANES spectra of Co-C3N4 and Co foils. LSV curves (c), IPCE curves (d), ABPE curves (e) and EIS results (f) of different photoanodes. Reprinted with permission from Ref. [257]. Copyright 2023, John Wiley and Sons. (g) Schematic illustration of the synthesis procedure for FeOOH/Ni-N4-O/BiVO4. J-V curves (h), ABPE curves (i), IPCE curves (j) of different photonodes. (k) Comparison of ABPE values in this work with previously reported research. Reprinted with permission from Ref. [258]. Copyright 2021, American Chemical Society.

Fig. 30. Doping modification strategies for catalysts in PEC CO2RR. (a) Top and side views of the basic unit of the CoPor-N3 polymer structure. TEM image (b), High magnification AC-HAADF-STEM (c), HAADF-STEM (d1) and TEM-EDS (d2-d4) images of CoPor-N3 polymer. (e) FE(CO)/FE(H2) values of the CoPor-N3 polymer at different potentials. (f) FE(CO)/FE(H2) values of the CoPor-N3 polymer at different potentials with illumination. (g) Structural sketch and photoelectrocatalytic CO2RR and OER mechanisms of the CoPor-N3||NiCo-LDH/CuPc/BiVO4 (Double) cell. (h) FE(CO) of the CoPor-N3||NiCo-LDH/CuPc/BiVO4 (Double) cell at different potentials under illumination. Reprinted with permission from Ref. [259]. Copyright 2021, John Wiley and Sons. (i) Schematic illustration of the preparation of dual-atom catalyst. (j) Aberration-corrected HAADF-STEM image. The orange ellipse highlighted the Ir-Pd diatom. (k) The linear scanning profile along the region of the marked orange rectangles and the corresponding intensity of the atoms. (l) CO2 conversion and product selectivity of IrPd-In2O3 catalysts synthesised by different methods. (m) Effect of metal loading on the space-time yield (STY) of methanol over Ir1Pd1-In2O3 (CP-PD). Reprinted with permission from Ref. [260]. Copyright 2024, John Wiley and Sons

Fig. 31. Heterojunction modification strategies for catalysts in PEC OER and CO2RR. (a) Schematic of the synthesis. HR-TEM images (b), and elemental mapping (c) of NiFeOx/BVO/BiVO4 photoanodes. (d) J-V curves with and without Na2SO3 (the dotted line is with 0.5 mol L?1 Na2SO3 solution). ABPE curves (e), and IPCE (f) of four BiVO4-based photoanodes. Reprinted with permission from Ref. [265]. Copyright 2023, Elsevier. (g) Schematic depiction of the assembly method of CoPc molecules on GO. (h) Selectivity of different products at different potentials under dark condition of CFP-GO/CoPc. (i) Selectivity of different products at different potentials under light illumination of STA-GO/CoPc. Reprinted with permission from Ref. [266]. Copyright 2023, John Wiley and Sons.

Fig. 32. Microenvironmental modulation modification strategies for catalysts in PEC OER and CO2RR. (a) Schematic diagram of the Co-Sil/CTF-BTh/Gd-Fe2O3 catalyst by modulating the microenvironment to improve the catalytic activity of the system. Calculated charge transfer rate constant (Kct) (b), surface recombination rate constant (Krec) (c) of different Photoanodes at different applied potentials. LSV curves (d), chronoamperometry curves (e), ABPE curves (f) and IPCE curves (g) of of different Photoanodes. Reprinted with permission from Ref. [273]. Copyright 2022, American Chemical Society. (h) SMA fabrication and CFx coating. (i) Total photocurrent and product distribution at ?0.7 V. CO and H2 were sampled every 10 min. (j) Reaction stability was tested at a constant photocurrent of 15 mA cm-2. (k) Performance comparison of different photocathodes for PEC CO2RR. Reprinted with permission from Ref. [274]. Copyright 2024, American Chemical Society.

Fig. 33. Reaction step analysis of PEC OER based on theoretical analysis. Chemisorption models (a) and corresponding Gibbs free energies of BiVO4 (b), MQD/BiVO4 (c) and MoOx/MQD/BiVO4 (d). Reprinted with permission from Ref. [139]. Copyright 2022, John Wiley and Sons. (e) Charge density difference of Co-agZIF-62/NiO/BiVO4. Gibbs free energies of NiO/BiVO4 (f), Zn-agZIF-62/NiO/BiVO4 (g) and Co-agZIF-62/NiO/BiVO4 (h). Reprinted with permission from Ref. [140]. Copyright 2023, John Wiley and Sons.

Fig. 34. Reaction step analysis of PEC CO2RR based on theoretical analysis. Free energies of PEC OER steps for CdIn2S4 (a) and for Vs-CdIn2S4 (b). (c) Density of states of Vs-CdIn2S4 at different bias voltages. (d) Trend of charge transfer of Vs-CdIn2S4 under light conditions, yellow areas represent electron accumulation. Reprinted with permission from Ref. [158]. Copyright 2020, Springer Nature. (e) Free energies of PEC OER reaction steps occurring on Pt-O or Pt-O-Fe active sites in SAs Pt: Fe2O3. Reprinted with permission from Ref. [142]. Copyright 2023, Springer Nature.

Fig. 35. Reaction step analysis of PEC CO2RR based on theoretical analysis. Key steps in the photocatalytic reduction of CO2 to CH4 by VS-CuIn5S8 (a) and pure CuIn5S8 (b). Reprinted with permission from Ref. [285]. Copyright 2019, Springer Nature. (c) Transition orbital of T1 state under illumination. (d) Schematic representation of the excited states of porphyrin-Au. (e) Electron transfer pathways under light (left) and dark (right) conditions. Reprinted with permission from Ref. [225]. Copyright 2019, Springer Nature. Side view of the optimised structures after CO2 adsorption on Pt(111) (f) and Ti3O6H6/Pt(111) (g) surfaces. (h) Differential charge density after adsorption of CO2 at the Ti3O6H6/Pt(111) interface. (i) Gibbs free energy diagrams for the reduction of CO2 on the surfaces of Pt(111) and Ti3O6H6/Pt(111) at 0 V. Reprinted with permission from Ref. [221]. Copyright 2018, American Chemical Society.

Fig. 36. Reaction step analysis of PEC CO2RR based on theoretical analysis. (a) Free energy for CO2RR to CO of different samples. (b) PDOS plots of surface catalytic Ag sites Reprinted with permission from Ref. [218]. Copyright 2022, American Chemical Society. (c) Mechanistic diagram of the possible occurrence of PEC CO2RR on Co-Bpy-COF-Ru1/2. (d) Free energy curves for the conversion of CO2 to CO occurring on the surface of Co-Bpy-COF-Ru1/2 under darkness and light. Reprinted with permission from Ref. [227]. Copyright 2023, John Wiley and Sons. Differential charge density for the Sn13O26/GaN(101-0) system (e) and the *CO/Sn13O26/GaN(101-0) system (f). (g) The energy barrier for PEC CO2RR to make HCOOH at the interface of GaN NWs and Sn NPs. Reprinted with permission from Ref. [14]. Copyright 2019, Royal Society of Chemistry.

Fig. 37. Reaction step analysis of PEC OER and CO2RR based on COMSOL simulations. COMSOL simulations on c-TiO2 (a), a-TiO2 (b) and a-B-TiO2 (c) under the field of electric force poling. The orange arrow indicates the polarization direction of the sample from un-poled to poling to fully poled. Reprinted with permission from Ref. [286]. Copyright 2023, Elsevier. Effect of the inverse opal structure on light absorption of io-CBO 200, io-CBO 400, and Planar-CBO at 550 nm (d-f) and 750 nm (g-i) simulated by the COMSOL software, and all average electric field intensities at different wavelengths at x = 1.6 μm are summed up in (j). (d,g) io-CBO 200, (e,h) io-CBO 400, and (f,i) Planar-CBO. Reprinted with permission from Ref. [287]. Copyright 2022, American Chemical Society.

Fig. 38. Reaction step analysis of PEC OER based on machine learning. (a) The introduction of AI and machine learning in materials science. Reprinted with permission from Ref. [295]. Copyright 2021, John Wiley and Sons. (b) The schematic illustration of the machine learning guided dopant selection towards efficient PEC process. Reprinted with permission from Ref. [296]. Copyright 2022, John Wiley and Sons.

Fig. 39. In-situ characterizations of PEC OER and PEC CO2RR. (a) Schematic of the device used for Operando PEC-ATR-FTIR. (b) In situ IR spectra of the BiVO4/electrolyte interface measured during photocharging (electrolyte is borate buffer). (c) Comparison of in situ IR spectra after photocharging in borate buffered electrolyte and ultrapure water. Reprinted with permission from Ref. [297]. Copyright 2021, American Chemical Society. (d) In situ Raman spectroscopy of Ag/Cu2O electrodes during PEC CO2RR. (e) SERS spectra for the CO stretching. (f) The relationship between CO frequency and potential for different variations of open-circuit voltage. (g) In situ Raman spectroscopy of Ag/Cu2O/pentanethiol electrodes during PEC CO2RR. Reprinted with permission from Ref. [298]. Copyright 2023, American Chemical Society.

Fig. 40. In-situ characterizations of PEC OER and PEC CO2RR. (a) Operando UV-vis spectra of ZnFe2O4 at different potentials. Reprinted with permission from Ref. [299]. Copyright 2021, John Wiley and Sons. (b) In-situ FTIR spectra of NiFe/CA/Fe-BiVO4. Reprinted with permission from Ref. [300]. Copyright 2024, Elsevier. In situ ATR-FTIR spectra measured on different photoanode surfaces in [H2O] 8 mol L?1 (c) and [D2O] 8 mol L?1 (d) conditions. Reprinted with permission from Ref. [301]. Copyright 2023, American Chemical Society.

Fig. 41. Photothermal catalysis. (a) Schematic representation of CoFex catalysts synthesised at different temperatures. Reprinted with permission from Ref. [318]. Copyright 2018, John Wiley and Sons. (b) Designed interfacial photothermal catalytic esterification principle. Reprinted with permission from Ref. [319]. Copyright 2022, Springer Nature. (c) Schematic diagram of the recovery process of spent LCO and photothermal catalytic polyester recycling. Reprinted with permission from Ref. [320]. Copyright 2024, Springer Nature. (d) Catalysts prepared from ZnCoAl-LDH nanosheets at different temperatures and CO hydrogenation selectivity in different wavelength ranges. Reprinted with permission from Ref. [321]. Copyright 2018, John Wiley and Sons.

Fig. 43. Photoenzymatic catalysis. (a) Strategies for biocatalyst development. Reprinted with permission from Ref. [350]. Copyright 2023, Springer Nature. (b) Synergistic photoredox and pyridoxal radical biocatalysis. (c) Diastereo- and enantioselective biocatalytic synthesis of ncAAs with up to three contiguous stereogenic centers. (d) Enantiodivergent synthesis of L- and D-amino acids using an orthogonal set of engineered PLP enzymes. Reprinted with permission from Ref. [351]. Copyright 2023, Science Publishing Group. (e) RAP-catalysed diastereo- and enantiodivergent decarboxylative radical cyclization. Reprinted with permission from Ref. [352]. Copyright 2024, Springer Nature. (f) Comparison of enantio-induction of excited-state reactions with that of ground-state reactions. Reprinted with permission from Ref. [353]. Copyright 2022, Springer Nature.

Table 4 Product selectivity and other performance parameters of different catalysts in PEC CO2RR.

Catalyst	Electrolyte	Potential	Main carbon product	FE (%)	Ref.
Ag/Cu₂O/ZS/FTO	0.1 mol L^‒1 KHCO₃	−1.2 V vs. Fc+/Fc	C₂H₄	60	[94]
Cu₂O-Derived Cu electrode	0.1 mol L^‒1 KHCO₃	0.35 V vs. RHE	CO	45	[208]
Cu₂O-Derived Cu-In electrode	0.1 mol L^‒1 KHCO₃	−0.6 V vs. RHE	CO	85	[209]
CuNPs/SiNWs	0.1 mol L^‒1 KHCO₃	−0.55 V vs. RHE	C₂H₄	25 ± 6	[215]
Cu₃(BTC)₂/Cu₂O/ITO	MeCN/TBAPF6	−1.97 V vs. Fc+/Fc	CO	95	[216]
Si\|n-GaN\|-NPhN-Ru(CP)2+ 2-RuCt	50 mmol L^‒1 NaHCO₃	−0.25 V vs. RHE	Formate	64	[217]
AgBr/GaN/Si	0.1 mol L^‒1 KHCO₃	−0.4 V vs. RHE	CO	>80	[218]
Cu/GaN/Si	0.1 mol L^‒1 KHCO₃	−1.0 V vs. RHE	Formate	20.7	[219]
NiOOH/α-Fe₂O₃	1 mol L^‒1 KOH	0.8 V vs. RHE	Formate	85	[220]
Pt-TiO₂/GaN/n-p Si	0.5 mol L^‒1 KHCO₃	0.47 V vs. RHE	CO	78	[221]
a-Si/TiO₂/Au	0.1 mol L^‒1 KHCO₃	0.4 V vs. RHE	CO	40	[222]
HNTM-Au-SA	0.1 mol L^‒1 KHCO₃	−0.9 V vs. RHE	CO	94.2	[225]
Si/rGO-Co	0.1 mol L^‒1 KHCO₃	−0.1 V vs. RHE	CO	82.8	[227]

Fig. 44. Industrialised applications and future development trends of PEC OER and PEC CO2RR.

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光电催化析氧和CO₂还原反应催化剂的研究进展

Recent advances of the catalysts for photoelectrocatalytic oxygen evolution and CO₂ reduction reactions

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