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Absence of CO2 electroreduction on copper, gold and silver electrodes without metal cations in solution
Nature Catalysis ( IF 37.8 ) Pub Date : 2021-07-26 , DOI: 10.1038/s41929-021-00655-5
Mariana C. O. Monteiro 1 , Bellenod Hagedoorn 1 , Marc T. M. Koper 1 , Federico Dattila 2 , Rodrigo García-Muelas 2 , Núria López 2
Affiliation  

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.



中文翻译:

溶液中没有金属阳离子的铜、金和银电极上不存在 CO2 电还原

二氧化碳的电催化还原被广泛研究用于燃料和化学品的可持续生产。电解质中的金属离子会影响反应性能,尽管它们的主要作用正在讨论中。在这里,我们通过循环伏安法研究了金电极上的 CO 2还原,结果表明,在没有金属阳离子的情况下,反应不会在纯 1 mM H 2 SO 4电解质中发生。我们使用扫描电化学显微镜在表面生成尖端收集模式下使用铂超微电极作为 CO 和 H 2进一步研究了溶液中有和没有金属阳离子的 CO 2还原传感器。只有在电解液中加入金属阳离子时,才会在金、银或铜上产生 CO。密度泛函理论模拟证实,部分去溶剂化的金属阳离子通过短程静电相互作用稳定了 CO 2中间体,从而使其得以还原。总体而言,我们的结果重新定义了反应机制,并提供了明确的证据,证明来自电解质的带正电物质是稳定关键反应中间体的关键。

更新日期:2021-07-26
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