Absence of CO2 electroreduction on copper, gold and silver electrodes without metal cations in solution

超微电极 电解质 无机化学 化学 循环伏安法 金属 铂金 电极 电化学 反应机理 支撑电解质 氧化还原 催化作用 物理化学 有机化学
作者
Mariana C. O. Monteiro,Federico Dattila,Bellenod J. L. Hagedoorn,Rodrigo Garcı́a-Muelas,Núria López,Marc T. M. Koper
出处
期刊:Nature Catalysis [Nature Portfolio]
卷期号:4 (8): 654-662 被引量:701
标识
DOI:10.1038/s41929-021-00655-5
摘要

The electrocatalytic reduction of carbon dioxide is widely studied for the sustainable production of fuels and chemicals. Metal ions in the electrolyte influence the reaction performance, although their main role is under discussion. Here we studied CO2 reduction on gold electrodes through cyclic voltammetry and showed that, without a metal cation, the reaction does not take place in a pure 1 mM H2SO4 electrolyte. We further investigated the CO2 reduction with and without metal cations in solution using scanning electrochemical microscopy in the surface-generation tip-collection mode with a platinum ultramicroelectrode as a CO and H2 sensor. CO is only produced on gold, silver or copper if a metal cation is added to the electrolyte. Density functional theory simulations confirmed that partially desolvated metal cations stabilize the CO2– intermediate via a short-range electrostatic interaction, which enables its reduction. Overall, our results redefine the reaction mechanism and provide definitive evidence that positively charged species from the electrolyte are key to stabilize the crucial reaction intermediate. Metal cations present in the electrolyte are known to influence the performance in CO2 electroreduction, but their specific role remains under discussion. Now, it is shown that the reaction can only take place in the presence of such cations, which are required to stabilize negatively charged reaction intermediates.
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