Copper Electrode Fabricated via Pulse Electrodeposition: Toward High Methane Selectivity and Activity for CO2 Electroreduction

选择性 电极 材料科学 电化学 甲烷 法拉第效率 化学工程 催化作用 限制电流 电流密度 无机化学 化学 冶金 有机化学 物理化学 工程类 物理 量子力学
作者
Yanling Qiu,Hexiang Zhong,Taotao Zhang,Wenbin Xu,Xianfeng Li,Huamin Zhang
出处
期刊:ACS Catalysis [American Chemical Society]
卷期号:7 (9): 6302-6310 被引量:88
标识
DOI:10.1021/acscatal.7b00571
摘要

Electrochemical reduction of CO2 (ERC) to methane has significant economic benefits and represents one promising solution for energy and environmental sustainability. However, traditional metal electrodes suffer from higher overpotentials, low activities, and poor selectivity. In this article, the pulse electrodeposition (P-ED) method is employed to prepare a copper electrode for ERC. The P-ED method can easily create Cu coatings on carbon paper with a much rougher surface and extended surface area, which is highly beneficial for improving their activity and selectivity. As a result, the prepared Cu electrodes exhibit high faradaic efficiency (of 85% at −2.8 V) and enhanced partial current density (jCH4 = 38 mA cm–2) for methane, which is by far the highest value ever reported at room temperature and ambient pressure. The enhanced activity is attributed to the extended reactive areas with rough morphology and loosened coating structure to ensure CO2 access the reaction sites located at the sublayers of the deposited Cu coatings. The prominent selectivity for CH4 is likely due to the presence of a stepped surface, which is formed by introduction of Cu (100) step into Cu (111) and Cu (220) terraces during the P-ED processes. The lower resistance to the one-electron transfer to CO2, which is a pre-equilibrium step prior to the rate-limiting nonelectrochemical step, is another positive factor to improve the ERC activity for CH4. Furthermore, we surprisingly find that the activity and selectivity of the Cu electrode can be easily recovered through continuous CO2 bubbling. This paper provides a facile method to prepare highly effective electrodes for electrochemical conversion of CO2.
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