Operando Insight into the Correlation between the Structure and Composition of CuZn Nanoparticles and Their Selectivity for the Electrochemical CO2 Reduction

选择性 化学 X射线吸收精细结构 双金属片 X射线光电子能谱 电化学 催化作用 法拉第效率 纳米颗粒 X射线吸收光谱法 氧化还原 合金 无机化学 吸收光谱法 化学工程 光谱学 电极 物理化学 工程类 物理 有机化学 量子力学 生物化学
作者
Hyo Sang Jeon,Janis Timoshenko,Fabian Scholten,Ilya Sinev,Antonia Herzog,Felix T. Haase,Beatriz Roldán Cuenya
出处
期刊:Journal of the American Chemical Society [American Chemical Society]
卷期号:141 (50): 19879-19887 被引量:192
标识
DOI:10.1021/jacs.9b10709
摘要

Bimetallic CuZn catalysts have been recently proposed as alternatives in order to achieve selectivity control during the electrochemical reduction of CO2 (CO2RR). However, fundamental understanding of the underlying reaction mechanism and parameters determining the CO2RR performance is still missing. In this study, we have employed size-controlled (∼5 nm) Cu100–xZnx nanoparticles (NPs) supported on carbon to investigate the correlation between their structure and composition and catalytic performance. By tuning the concentration of Zn, a drastic increase in CH4 selectivity [∼70% Faradaic efficiency (F.E.)] could be achieved for Zn contents from 10 to 50, which was accompanied by a suppression of the H2 production. Samples containing a higher Zn concentration displayed significantly lower CH4 production and an abrupt switch in the selectivity to CO. Lack of metal leaching was observed based on quasi in situ X-ray photoelectron spectroscopy (XPS). Operando X-ray absorption fine structure (XAFS) spectroscopy measurements revealed that the alloying of Cu atoms with Zn atoms takes place under reaction conditions and plays a determining role in the product selectivity. Time-dependent XAFS analysis showed that the local structure and chemical environment around the Cu atoms continuously evolve during CO2RR for several hours. In particular, cationic Zn species initially present were found to get reduced as the reaction proceeded, leading to the formation of a CuZn alloy (brass). The evolution of the Cu–Zn interaction with time during CO2RR was found to be responsible for the change in the selectivity from CH4 over Cu-ZnO NPs to CO over CuZn alloy NPs. This study highlights the importance of having access to in depth information on the interplay between the different atomic species in bimetallic NP electrocatalysts under operando reaction conditions in order to understand and ultimately tune their reactivity.
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