An electrochemical study of carbon dioxide electroreduction on gold-based nanoparticle catalysts
An electrochemical study of carbon dioxide electroreduction on gold-based nanoparticle catalysts
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DOI：
10.1016/j.electacta.2013.10.162
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发表时间：
2014-05-10
影响因子：
6.6
通讯作者：
Kriek, R. J.
中科院分区：
文献类型：
--
作者：
Lates, V.;Falch, A.;Kriek, R. J.
我们在这里报告的电化学研究二氧化碳电还原（CO2 ER）采用电化学阻抗谱（EIS）和旋转环盘电极（RRDE）不同的金基催化剂，即散装多晶金，金纳米粒子（Au NPs）和Au@Ag核壳纳米粒子。RRDE测量允许CO2到CO的还原电位的鉴定和NP的表征基于它们对CO2 ER相对于析氢的选择性。发现金-银组合催化剂比Au NPs具有更高的选择性，尽管过电位更高。一种金-银催化剂在很宽的电位范围内表现出恒定的选择性。首次，EIS数据显示，存在两个电荷转移过程中的CO2还原。这些都归因于两个表面局限的反应，涉及吸附的中间体，这是与建议的机制。这些反应的电势范围对于每种催化剂是特定的，其中金-银催化剂表现出比Au NP、Au和Ag多晶电极更慢的电子转移。(C)2013爱思唯尔有限公司版权所有。
We report here on an electrochemical study of carbon dioxide electroreduction (CO2ER) employing electrochemical impedance spectroscopy (EIS) and a rotating ring-disk electrode (RRDE) on different gold based catalysts, namely bulk polycrystalline gold, gold nanoparticles (Au NPs) and Au@Ag core-shell nanoparticles. RRDE measurements allowed the identification of the reduction potential of CO2 to CO and the characterisation of NPs based on their selectivity for CO2ER with respect to hydrogen evolution. Gold-silver combined catalysts were found to be more selective than Au NPs although at higher overpotential. One gold-silver catalyst exhibits a constant selectivity over a wide potential range. For the first time, EIS data showed the existence of two charge transfers during the reduction of CO2. These are attributed to two surface confined reactions that involve an adsorbed intermediate which is correlated with a proposed mechanism. The potential range of these reactions is specific for each catalyst with gold-silver catalysts exhibiting a slower electron transfer than Au NPs, Au and Ag polycrystalline electrodes. (C) 2013 Elsevier Ltd. All rights reserved.