Cation effects in electrocatalytic reduction reactions: Recent advances

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

Chinese Journal of Catalysis ›› 2024, Vol. 63: 16-32.DOI: 10.1016/S1872-2067(24)60080-X

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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)

Abstract

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

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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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(24)60080-X

https://www.cjcatal.com/EN/Y2024/V63/I8/16

Figures/Tables 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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Cation effects in electrocatalytic reduction reactions: Recent advances

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