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    题名: The Role of the Copper Oxidation State in the Electrocatalytic Reduction of CO2 into Valuable Hydrocarbons
    其它题名: 氧化銅價態與二氧化碳電還原之碳氫產物間研究
    作者: Juan-Jesús Velasco-Vélez;Travis Jones;Dunfeng Gao;Emilia Carbonio;Rosa Arrigo;Cheng-Jhih Hsu;Yu-Cheng Huang;Chung-Li Dong;Jin-Ming Chen;Jyh-Fu Lee;Peter Strasser;Beatriz Roldan Cuenya;Robert Schlögl;Axel Knop-Gericke;Cheng-Hao Chuang
    关键词: Charge transport limitation;CO2RR;Copper carbonate passivation layer;DFT calculations;Electrocatalytically active reduced copper oxides;Electrodeposited prepared copper oxides;In situ X-ray spectroscopy
    日期: 2018-11-29
    上传时间: 2019-05-08 12:10:18 (UTC+8)
    出版者: American Chemical Society
    摘要: Redox-active copper catalysts with accurately prepared oxidation states (Cu0, Cu+, and Cu2+) and high selectivity to C2 hydrocarbon formation, from electrocatalytic cathodic reduction of CO2, were fabricated and characterized. The electrochemically prepared copper-redox electro-cathodes yield higher activity for the production of hydrocarbons at lower oxidation state. By combining advanced X-ray spectroscopy and in situ microreactors, it was possible to unambiguously reveal the variation in the complex electronic structure that the catalysts undergo at different stages (i.e., during fabrication and electrocatalytic reactions). It was found that the surface, subsurface, and bulk properties of the electrochemically prepared catalysts are dominated by the formation of copper carbonates on the surface of cupric-like oxides, which prompts catalyst deactivation by restraining effective charge transport. Furthermore, the formation of reduced or partially reduced copper catalysts yields the key dissociative proton-consuming reactive adsorption of CO2 to produce CO, allowing the subsequent hydrogenation into C2 and C1 products by dimerization and protonation. These results yield valuable information on the variations in the electronic structure that redox-active copper catalysts undergo in the course of the electrochemical reaction, which, under extreme conditions, are mediated by thermodynamics, but critically, kinetics dominate near the oxide/metal phase transitions.
    關聯: ACS Sustainable Chemistry & Engineering 7(1), p.1485-1492
    DOI: 10.1021/acssuschemeng.8b05106
    显示于类别:[電機工程學系暨研究所] 期刊論文

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