Quantitative Understanding of Cation Effects on the Electrochemical Reduction of CO2 and H+ in Acidic Solution
Conducting electrochemical reduction of CO2 in acidic media can effectively increase the utilization efficiency of CO2. Alkali cations (M+) are indispensable for CO2 reduction in acidic media, while the high concentration of M+ results in bicarbonate precipitation in a gas diffusion electrode. To develop selective and sustainable CO2 reduction techniques in acidic media, quantitative understandings of cation effects on reduction rates of CO2 and H+ are demanded. Previous study shows that M+ in acidic media can modulate the electric field distribution in a double layer, which suppresses H+ migration and stabilizes the intermediate of CO2 reduction. In this work, we conducted a more quantitative study through the combination of electrochemical experiments and generalized modified Poisson–Nernst–Planck (GMPNP) simulations. When the concentration of M+ is higher than that of H+, the migration of H+ is substantially suppressed. The diffusion rate of H+ is also influenced by the concentration of M+. Furthermore, the concentration and identity of M+ affect the electric field within the Stern layer, which is the driving force of the electron transfer from the cathode to CO2. Only in M+-containing solutions, the electric field strength within the Stern layer increases as the potential moves negatively, and CO2 reduction can be accelerated by applying a larger overpotential. These aspects together determine the selectivity of CO2 reduction in acidic solution.
First ; Corresponding
|WOS Accession No|
Cited Times [WOS]:0
|Document Type||Journal Article|
|Department||Department of Chemistry|
1.Department of Chemistry, Southern University of Science and Technology, Shenzhen, Guangdong518055, China
2.Department of Mechanical and Energy Engineering, Southern University of Science and Technology, Shenzhen, Guangdong518055, China
|First Author Affilication||Department of Chemistry|
|Corresponding Author Affilication||Department of Chemistry|
|First Author's First Affilication||Department of Chemistry|
Hai-Gang,Qin,Fu-Zhi,Li,Yun-Fan,Du,et al. Quantitative Understanding of Cation Effects on the Electrochemical Reduction of CO2 and H+ in Acidic Solution[J]. ACS Catalysis,2022,13(2):916-926.
Hai-Gang,Qin.,Fu-Zhi,Li.,Yun-Fan,Du.,Lin-Feng,Yang.,Hao,Wang.,...&Jun,Gu.(2022).Quantitative Understanding of Cation Effects on the Electrochemical Reduction of CO2 and H+ in Acidic Solution.ACS Catalysis,13(2),916-926.
Hai-Gang,Qin,et al."Quantitative Understanding of Cation Effects on the Electrochemical Reduction of CO2 and H+ in Acidic Solution".ACS Catalysis 13.2(2022):916-926.
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