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    題名: On the Activity/Selectivity and Phase Stability of Thermally Grown Copper Oxides during the Electrocatalytic Reduction of CO2
    作者: 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
    關鍵詞: cathodic CO2 reduction reaction;oxide derived copper;electrocatalysis
    日期: 2020-09-09
    上傳時間: 2021-05-05 12:11:55 (UTC+8)
    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.
    關聯: ACS Catalysis 10(19), p.11510-11518
    DOI: 10.1021/acscatal.0c03484
    顯示於類別:[電機工程學系暨研究所] 期刊論文

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