电子转移
催化作用
循环伏安法
化学
伏安法
电化学
玻璃碳
氧化还原
分析化学(期刊)
锡
质子化
傅里叶变换红外光谱
旋转圆盘电极
无机化学
电极
物理化学
化学工程
离子
有机化学
工程类
作者
Jie Zhang,Lu Chen,Fengwang Li,Christopher D. Easton,Jiezhen Li,Alan M. Bond
标识
DOI:10.1021/acscatal.7b01305
摘要
Two underlying electron transfer processes that directly underpin the catalytic reduction of carbon dioxide (CO2) to HCOO -and CO at Sn electrodes have been detected using the higher order harmonic components available in Fourier-transformed large amplitude ac voltammetry.Both closely spaced electron transfer processes are undetectable by dc voltammetry and associated with the direct reduction of CO2 species and have reversible potentials of approximately -1.27 and -1.40 V vs. Ag/AgCl.A mechanism involving a reversible inner-sphere one-electron reduction of CO2 followed by a rate determining CO2 .-protonationstep is proposed.Molecular CO2 has been identified as the dominant electro-active species that undergoes a series of coupling electron transfer and chemical reactions to form the final products.The substantial difference in the catalytic responses of Sn(SnOx) modified glassy carbon and Sn foil electrodes are attributed to their strongly preferred Sn (200) orientation and polycrystalline states, respectively.The Fourier transformed ac technique should be generally applicable for predicting the performance of Sn catalysts.
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