催化作用
反应性(心理学)
原位
材料科学
遗传算法
电化学
拉曼光谱
氧化还原
化学
无机化学
纳米技术
组合化学
化学工程
物理化学
电极
有机化学
病理
工程类
物理
光学
生物
进化生物学
替代医学
医学
作者
Chunsong Li,Haocheng Xiong,Ming He,Bingjun Xu,Qi Lü
出处
期刊:ACS Catalysis
日期:2021-09-14
卷期号:11 (19): 12029-12037
被引量:27
标识
DOI:10.1021/acscatal.1c02852
摘要
Ag and Au are efficient monometallic electrocatalysts for the CO2 reduction reaction (CO2RR) to CO. Recent preoxidation treatments on Ag and Au have been shown to effectively improve their reactivity in CO production. However, the mechanism underlying the improvements remains controversial. The challenges in probing the surface speciation under reaction conditions hinder the efforts to be made for correlating the catalyst surface speciation with its performance. Herein, we combine in situ surface-enhanced Raman spectroscopy and reactivity measurements to investigate the coelectrolysis of CO2 and O2 demonstrating that the in-situ-formed surface oxyhydroxyl species on Ag can significantly enhance the CO production rate (>80 fold). In contrast, no surface oxyhydroxyl species was observed on Au in coelectrolysis with O2, which was accompanied by much less significant enhancement in the CO activity (<3-fold). Our work highlights the impact of catalyst surface speciation on the CO2RR performance and opens up a promising route for designing efficient CO2RR catalysts. We believe the findings presented in our work point out a fruitful strategy to design an advanced catalyst and reaction scheme to achieve efficient CO2RR.
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