On the Activity/Selectivity and Phase Stability of Thermally Grown Copper Oxides during the Electrocatalytic Reduction of CO2
學年 109
學期 1
出版（發表）日期 2020-10-02
作品名稱 On the Activity/Selectivity and Phase Stability of Thermally Grown Copper Oxides during the Electrocatalytic Reduction of CO2
作品名稱（其他語言）
著者 Juan-Jesús Velasco-Vélez; Cheng-Hao Chuang; Dunfeng Gao; Qingjun Zhu; Danail Ivanov; Hyo Sang Jeon; Rosa Arrigo; Rik Valentijn Mom; Eugen Stotz; Heng-Liang Wu; Travis E. Jones; Beatriz Roldan Cuenya; Axel Knop-Gericke; Robert Schlögl
單位
出版者
著錄名稱、卷期、頁數 ACS Catalysis 10(19), p.11510-11518
摘要 Revealing the active nature of oxide-derived copper is of key importance to understand its remarkable catalytic performance during the cathodic CO2 reduction reaction (CO2RR) to produce valuable hydrocarbons. Using advanced spectroscopy, electron microscopy, and electrochemically active surface area characterization techniques, the electronic structure and the changes in the morphology/roughness of thermally oxidized copper thin films were revealed during CO2RR. For this purpose, we developed an in situ cell for X-ray spectroscopy that could be operated accurately in the presence of gases or liquids to clarify the role of the initial thermal oxide phase and its active phase during the electrocatalytic reduction of CO2. It was found that the Cu(I) species formed during the thermal treatment are readily reduced to Cu0 during the CO2RR, whereas Cu(II) species are hardly reduced. In addition, Cu(II) oxide electrode dissolution was found to yield a porous/void structure, where the lack of electrical connection between isolated islands prohibits the CO2RR. Therefore, the active/stable phase for CO2RR is metallic copper, independent of its initial phase, with a significant change in its morphology upon its reduction yielding the formation of a rougher surface with a higher number of underco-ordinated sites. Thus, the initial thermal oxidation of copper in air controls the reaction activity/selectivity because of the changes induced in the electrode surface morphology/roughness and the presence of more undercoordinated sites during the CO2RR.
關鍵字 cathodic CO2 reduction reaction;oxide derived copper;electrocatalysis
語言 en_US
ISSN 2155-5435
期刊性質 國外
收錄於 SCI Scopus
產學合作
通訊作者
審稿制度 是
國別 USA
公開徵稿
出版型式 ,電子版
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