电催化还原反应中的阳离子效应:最新进展

doi:10.1016/S1872-2067(24)60080-X

催化学报 ›› 2024, Vol. 63: 16-32.DOI: 10.1016/S1872-2067(24)60080-X

电催化还原反应中的阳离子效应:最新进展

任清汇^a, 徐亮^b^,^*(), 吕梦雨^a, 张秩远^c, 栗振华^a^,^c^,^*(), 邵明飞^a^,^c^,^*(), 段雪^a^,^c

^a北京化工大学化学学院化工资源有效利用国家重点实验室, 北京 100029
^b北京化工大学化学工程学院, 北京 100029
^c衢州资源化工创新研究院, 浙江衢州 324000

收稿日期:2024-03-06 接受日期:2024-06-05 出版日期:2024-08-18 发布日期:2024-08-19
通讯作者: *电子信箱: XL@buct.edu.cn (徐亮),LZH0307@mail.buct.edu.cn (栗振华),shaomf@mail.buct.edu.cn (邵明飞).
基金资助:
国家自然科学基金(22090031);国家自然科学基金(22108008);国家自然科学基金(22302006);国家自然科学基金(22288102);青年人才托举工程项目(2021QNRC001);中央高校基本科研业务费(buctrc202011);国家资助博士后基金(GZB20230049)

Cation effects in electrocatalytic reduction reactions: Recent advances

Qinghui Ren^a, Liang Xu^b^,^*(), Mengyu Lv^a, Zhiyuan Zhang^c, Zhenhua Li^a^,^c^,^*(), Mingfei Shao^a^,^c^,^*(), Xue Duan^a^,^c

^aState Key Laboratory of Chemical Resource Engineering, College of Chemistry, Beijing University of Chemical Technology, Beijing 100029, China
^bCollege of Chemical Engineering, Beijing University of Chemical Technology, Beijing 100029, China
^cQuzhou Institute for Innovation in Resource Chemical Engineering, Quzhou 324000, Zhejiang, China

Received:2024-03-06 Accepted:2024-06-05 Online:2024-08-18 Published:2024-08-19
Contact: *E-mail: XL@buct.edu.cn to (L. Xu), LZH0307@mail.buct.edu.cn (Z. Li), shaomf@mail.buct.edu.cn (M. Shao).
About author:Liang Xu received her PhD degree in Chemical Engineering and Technology from Beijing University of Chemical Technology (BUCT) (China) in 2019. She did postdoctoral research at the Institute of Chemistry, Chinese Academy of Sciences from 2020 to 2023. Then she served as a lecturer at BUCT. Her research interests mainly focus on the electrocatalytic conversion of CO₂/NOx into high value-added chemicals.
Zhenhua Li (College of Chemistry, Beijing University of Chemical Technology), received his B.S. in 2014 and Ph.D degree in 2019 from Beijing University of Chemical Technology. In 2017, he completed a joint doctoral training program at Nanyang Technological University in Singapore; From 2019 to 2023, he served as an associate professor at Beijing University of Chemical Technology, and promoted to professor from 2024. His research interests lie in the field of water electrolysis for hydrogen production couple with organic synthesis. He has published over 70 SCI papers, with more than 5800 citations, 11 ESI highly cited papers, and an H-index of 41. In the last five years, he has led a National Key R&D Program (Hydrogen Special)-Young Scientist Project, a National Natural Science Foundation of China-Youth Program, a Beijing Natural Science Foundation-Youth Program, and participated in two National Natural Science Foundation of China Major Programs.
Mingfei Shao (State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology) received his Ph.D. degree from Beijing University of Chemical Technology (BUCT) in 2014, after which he joined the staff of BUCT and was promoted to professor in 2018. He was also a visiting student at the University of Oxford in 2013. His research interests mainly include electrochemical energy related chemistry, materials and engineering. He proposed the idea of the water electrolysis coupled with green electrosynthesis (e.g., hydrogen generation coupled with organic oxidation). He also proposed a new method of integrated electrode design based on layered double hydroxides, which is a platform for construct various energy materials and devices. He has been published more than 130 papers, which have been cited >13000 times (H index = 62). In addition, He has obtained and awarded from the National Natural Science Foundation of China-Outstanding Youth Foundation in 2019 and the Chinese Catalytic Rookie Award.
Supported by:
National Natural Science Foundation of China(22090031);National Natural Science Foundation of China(22108008);National Natural Science Foundation of China(22302006);National Natural Science Foundation of China(22288102);Young Elite Scientist Sponsorship Program by CAST(2021QNRC001);Fundamental Research Funds for the Central Universities(buctrc202011);National Funded Postdoctoral Researchers Program(GZB20230049)

摘要/Abstract

摘要：

近年来, 全球对于清洁能源技术的需求日益增长, 利用太阳能和风能等可再生能源驱动的电化学还原反应成为实现可持续化学生产的重要途径. 将廉价原料(如CO₂, N₂/NO_x, 有机物, O₂)升级为高附加值的化学品或燃料, 为能源转换和化学品生产提供了新的可能. 在过去几十年里, 为提高电化学还原反应活性, 研究人员开发和改良了许多种类的电催化剂. 然而, 仅依赖催化剂的优化提高催化性能仍存在局限性. 研究表明, 在电化学还原反应中, 电解质中阳离子的种类和浓度对反应活性和产物选择性有重要影响. 因此, 深入探讨阳离子效应在电催化还原反应中的作用机理及其应用对于推动清洁能源和绿色化学领域的电化学研究具有重要意义.

本文对阳离子效应在调控电化学还原反应活性和产物选择性的反应机理、表征手段、计算方法以及应用范围进行讨论, 并对该领域面临的挑战和未来发展进行了展望. 首先, 详细概括了阳离子效应在电化学还原反应过程中的机理, 包括促进反应物的吸附/稳定反应中间体、局部电场和界面pH的调控以及对氢析出对反应的影响. 其次, 全面总结了阳离子效应在电化学还原反应中的应用, 包括电催化二氧化碳还原反应、电催化氮气/硝酸根还原反应、电催化有机化合物还原反应以及氧还原反应. 通过上述反应展示了阳离子效应如何通过调节电催化反应的局部环境和反应路径, 有效地提升了电催化还原反应的活性和产物选择性, 进一步证明了在电催化还原领域深入研究和应用阳离子效应的重要性和潜力. 随后介绍了一系列针对阳离子效应研究的原位和非原位表征手段以及理论计算模拟的方法. 最后, 概述了阳离子效应在电催化反应中所面临的挑战, 并对未来的研究方向进行了展望, 主要挑战包括: (1) 在阳离子反应机理方面, 可以利用先进的技术手段更准确地揭示界面电场效应; (2) 在表征技术方面, 开发新的技术手段以识别特定反应/阳离子系统在操作条件下的主要机制; (3) 催化剂稳定性方面, 应开发新的方法和策略来优化电催化剂; (4) 催化剂设计策略方面, 应深入探索和发展先进的修饰策略(如非晶态单原子或双原子研究、范德华异质结、微环境调节、自旋态调节以及非晶态二维层状材料耦合等); (5) 开发阳离子效应在其他催化领域中的应用; (6) 发展阳离子效应在电催化氧化反应中的研究; (7) 深入研究电催化剂体相结构因阳离子插入而发生的动态变化.

综上所述, 本文深入系统地总结了阳离子效应对电催化还原反应的机理和应用, 并对该领域目前存在的挑战和未来的研究方向进行了展望, 以期为阳离子效应的应用提供基础认知和设计参考, 进而推动阳离子效应的快速发展.

关键词: 电催化, 还原反应, 阳离子效应, 机理, 应用

Abstract:

Electrocatalytic reduction reactions, powered by clean energy sources such as solar energy and wind, offer a sustainable method for converting inexpensive feedstocks (e.g., CO₂, N₂/NO_x, organics, and O₂) into high-value-added chemicals or fuels. The design and modification of electrocatalysts have been widely implemented to improve their performance in these reactions. However, bottlenecks are encountered, making it challenging to further improve performance through catalyst development alone. Recently, cations in the electrolyte have emerged as critical factors for tuning both the activity and product selectivity of reduction reactions. This review summarizes recent advances in understanding the role of cation effects in electrocatalytic reduction reactions. First, we introduce the mechanisms underlying cation effects. We then provide a comprehensive overview of their application in electroreduction reactions. Characterization techniques and theoretical calculation methods for studying cation effects are also discussed. Finally, we address remaining challenges and future perspectives in this field. We hope that this review offers fundamental insights and design guidance for utilizing cation effects, thereby advancing their development.

Key words: Electrocatalysis, Reduction reaction, Cation effect, Mechanism, Application

任清汇, 徐亮, 吕梦雨, 张秩远, 栗振华, 邵明飞, 段雪. 电催化还原反应中的阳离子效应:最新进展[J]. 催化学报, 2024, 63: 16-32.

Qinghui Ren, Liang Xu, Mengyu Lv, Zhiyuan Zhang, Zhenhua Li, Mingfei Shao, Xue Duan. Cation effects in electrocatalytic reduction reactions: Recent advances[J]. Chinese Journal of Catalysis, 2024, 63: 16-32.

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图/表 15

Fig. 1. Development timeline of cation effects.

Fig. 2. Schematic of the main components of this review (M+: cations; R: reactant or intermediate).

Fig. 3. Relationship between the four mechanisms.

Fig. 4. (a) CO2RR in a medium containing alkali metal cations (AM+). (b) DFT-MD simulations of CO2 and electrode distances in different electrolytes. Reprinted with permission from Ref. [75], Copyright 2023, Springer Nature. (c) CO2RR product Faradaic efficiency (FE) and total current densities of Cu(OH)2 nanoparticles at -1.0 vs. RHE under various cations conditions. (d) Observation of *CO dynamics in Li+ through TR-SERS. Reprinted with permission from Ref. [76] Copyright 2023, American Chemical Society.

Fig. 5. (a) Free energy profile for the electroreduction of CO2 to CO on the Ag (111) electrode surfaces. (b) CO2 adsorption energy as a function of the field. Reprinted with permission from Ref. [57] Copyright 2016 American Chemical Society. (c) A higher hydrated Cs+ concentration on the outer Helmholtz plane induces a stronger interfacial electric field. (d) Normalized (to Li+) CO partial current density on Ag (110), Ag (111), and polycrystalline Ag (pc-Ag) at -1.0 V vs. RHE) in the presence of different alkali metal cations. Reprinted with permission from Refs. [56] Copyright 2019, Royal Society of Chemistry.

Fig. 6. (a) Effect of the cation radius on the local pH and pKa of cation hydrolysis. (b) The FE for CO increased and that for H2 decreased with increasing cation size owing to decreased polarization. Reprinted with permission from Ref. [77]. Copyright 2016, American Chemical Society. (c) Schematic of the pH test at the Au-electrolyte interface in situ using ATR-SEIRAS. (d) Steady-state pH at the metal-electrolyte interface during the electroreduction of CO2. Reprinted with permission from Ref. [82]. Copyright 2017, American Chemical Society.

Fig. 7. (a) Impact of multivalent cations on HER. (b) Relationship between the performance of CO2RR and HER and the ionic radius and acidity of the cations at high potentials. Reprinted with permission from Ref. [86]. Copyright 2021, American Chemical Society. (c) Schematic of the double layer near cathode in the electrolyte. (d) FE of formic acid on SnO2/C catalyst with different cations. Reprinted with permission from Ref. [79]. Copyright 2022, Springer Nature.

Table 1 The impact of cation species and concentration on electroreduction reactions activity.

Catalyst	Reaction	\|Current density (mA cm^-2)\|/Selectivity (%)/FE (%)					Ref.
Catalyst	Reaction	No added cations	Li⁺	Na⁺	K⁺	Cs⁺	Ref.
Ag GDE	CO₂ to CO	5.5/8	22/30	27/62	28/65	32/75	[93]
Ag	CO₂ to CO	-	-	97/85	276/94	315/98	[10]
Cu	CO₂ to C₂	-	4.7	5.1	6.6	8.5	[59]
Au	CO₂ to CO	-	0.11	0.25	0.58	0.82	[86]
Au	CO₂ to CO	-	0.76	0.9	0.98	1.6	[82]
Ag	CO₂ to CO	-	3.8	4.9	6.6	8.3	[77]
Cu	CO to C₂	-	2.9/37	5.7/50	9.2/58	13/55	[60]
Au	CO₂ to CO	-	0.03/3.1	0.79/19.5	1.02/50.2	1.04/49.1	[94]
Ag	CO₂ to CO	-	3.5/81	8.6/91	12.1/97	12.5/98	[95]
SnO₂/C	CO₂ to formic acid	-	25.2	40.5	59.9	81.0	[79]
Sn	NO₃^- to NH₃	-	15	21	22	39	[12]
Heat-carbon black	O₂ to H₂O₂	-	0.53/76	-	0.74/90	1.27/93	[96]
Pt	O₂ to H₂O₂	-	0.64	0.79	0.90	0.56	[81]
Carbon nanotube	O₂ to H₂O₂	0.6/4.1	-	0.89/36.6	-	-	[97]
Reduced graphene oxide	O₂ to H₂O₂	5.7/10	-	150/41.4	-	-	[97]
Pt₅Gd	O₂ to H₂O₂	-	4.8	2.7	2.5	2.0	[98]
Pt (111)	O₂ to H₂O₂	-	1.1	3.3	4.7	5.0	[86]
TiO₂^a	Oxalic acid to glycollic acid	100/63.7	190/84.8 (Al³⁺)	69.8	69.0	66.0 (Mg²⁺)	[88]

Table 2 Effect of cation concentration on electroreduction reaction activity.

Catalyst	Reaction	\|Current density (mA cm^-2)\|/Selectivity (%)/FE (%)		Ref.
Catalyst	Reaction	Low concentration of M⁺	High concentration of M⁺	Ref.
Ag	CO₂ to CO/formate	6.2 (CO, 0.5 mol L^‒1 KAc) 92.3 (formate, 0.5 mol L^‒1 KAc)	31.8 (CO, 10 mol L^‒1 KAc) 66.4 (formate, 10 mol L^‒1 KAc)	[74]
Cu	CO₂ to CO/formate	70.8 (CO, 0.5 mol L^‒1 KAc) 8.7 (formate, 0.5 mol L^‒1 KAc)	28.7 (CO, 10 mol L^‒1 KAc) 39.3 (formate, 10 mol L^‒1 KAc)	[74]
Cu	CO₂ to CO/C₂H₄	46.6 (CO, 0.05 mol L^‒1 KOH) 8.7 (C₂H₄, 0.05 mol L^‒1 KOH)	2.5 (CO, 1 mol L^‒1 KOH) 10.7 (C₂H₄, 1 mol L^‒1 KOH)	[99]
CuNNAs CuNNs ^a	CO₂ to C₂	20.0 (CuNNAs as catalyst)	59.0 (CuNNs as catalyst)	[100]
Au needle/Au particles ^a	CO₂ to CO	15.0 (Au needle as catalyst)	98.6 (Au particles as catalyst)	[58]
Pd NTs/Pd@ArS-Pd₄S NTs ^a	Alkyne to alkene	51.7/70.6 (Pd NTs as catalyst)	65.7/89.6 (Pd@ArS-Pd₄S NTs as catalyst)	[101]
BiNCs	N₂ to NH₃	9.8 (0.2 mol L^‒1 K⁺)	66.5 (1.2 mol L^‒1 K⁺)	[102]
heat-treated carbon black	O₂ to H₂O₂	1.16 (0.1 mol L^‒1 KCl)	3.75 (0.5 mol L^‒1 KCl)	[96]
Pt (111)	O₂ to H₂O₂	4.3 (0.02 mol L^‒1 methanesulfonic acid)	0.8 (0.2 mol L^‒1 methanesulfonic acid)	[103]

Fig. 8. (a) Relationship between adsorption K+ and reaction current density, and tip electric field intensity. (b) Current on different catalysts with a thin TiO2 insulator layer at a bias of -1 V. Reprinted with permission from Ref. [58]. Copyright 2016, Springer Nature. (c) Concentration of K+ and electric field at the tips of different nanoneedles. (d) The performance of CuNNs and CuNNAs. Reprinted with permission from Refs. [100]. Copyright 2022, American Chemical Society. (e) Mechanism of the CO2RR over the F-modified Cu catalyst. Reprinted with permission from Ref. [115]. Copyright 2020, Springer Nature.

Fig. 9. (a) ΔG*NNH on Bi (012), (110), and (104) facets with and without K+ cations. (b) Nitrogen reduction current density (jN), HER current density (jH), and total current density (jT) at different c(K+) values. (c) FE of NRR with different c(K+) values. Reprinted with permission from Ref. [102]. Copyright 2019. Springer Nature. Influence of different electrolytes on concentration of N species (d) and selectivity (e). Reprinted with permission from Ref. [12]. Copyright 2023, Elsevier B.V.

Fig. 10. (a) Conversions of 4-ethynylaniline and selectivity of 4-vinylaniline at -1.1 V vs. Hg/HgO. (b) ECSA-normalized linear sweep voltammetry (LSV) curves. (c) EPR trapping of hydrogen (*) and carbon (#) radicals. Reprinted with permission from Ref. [101]. Copyright 2022, American Association for the Advancement of Science. (d) Productivities and FEs of GA over TiO2 in 0.2 mol L-1 OX with different metal salts. (e) The adsorption of OX and GO over pure TiO2 and TiO2-Al3+ by electrochemical adsorbate-stripping measurements. (f) EPR trapping of hydrogen (#) radicals. Reprinted with permission from Ref. [88]. Copyright 2023, American Chemical Society.

Fig. 11. (a) Schematic of noncovalent bonding between hydrated alkali metal cations and surface-bound OH species. Reprinted with permission from Ref. [123]. Copyright 2009, Springer Nature. (b) Schematic of H+ repulsion by Na+. (c) Polarization curve of ORR for Pt/C supported on a glassy carbon electrode in O2-saturated 0.1 and 0.2 mol L?1 NaOH. Reprinted with permission from Ref. [125]. Copyright 2016 American Chemical Society. (d) The long-term galvanostatic charge-discharge profile of zinc-air cells assembled with different electrolytes. Reprinted with permission from Ref. [130]. Copyright 2021, American Chemical Society.

Fig. 12. Schematic of SHINERS. (a,b) Electromagnetic field distribution of SHINs on a Pd/Au substrate. Reprinted with permission from Ref. [135] Copyright 2021, Springer Nature. (c,d) Schematic illustration of ATR-SEIRAS. Reprinted with permission from Ref. [94]. Copyright 2020, American Chemical Society. Reprinted with permission from Ref. [111]. Copyright 2019, Elsevier Ltd. (e) Schematic illustration of the LICT. Reprinted with permission from Ref. [139]. Copyright 2022, John Wiley and Sons.

Fig. 13. Schematic of the main outlook.

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电催化还原反应中的阳离子效应:最新进展

Cation effects in electrocatalytic reduction reactions: Recent advances

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