气候变化领域集成服务门户(CCPortal): Time-resolved observation of C-C coupling intermediates on Cu electrodes for selective electrochemical CO2reduction

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DOI	10.1039/d0ee01690j
	Time-resolved observation of C-C coupling intermediates on Cu electrodes for selective electrochemical CO2reduction
	Kim Y.; Park S.; Shin S.-J.; Choi W.; Min B.K.; Kim H.; Kim W.; Hwang Y.J.
发表日期	2020
ISSN	17545692
起始页码	4301
结束页码	4311
卷号	13 期号:11
英文摘要	In the electrochemical CO2 reduction reaction (CO2RR), Cu has been spotlighted as the only electro-catalyst that can produce multi-carbon molecules, but the mechanism of the selective C2+ production reaction remains elusive. Here, we directly monitored CO2RR intermediates by employing time-resolved attenuated total reflection-surface enhanced infrared absorption spectroscopy (ATR-SEIRAS), with particular attention to the C1 and C2+ pathways beyond the formation of ∗CO. Electrodeposited Cu and Cu(OH)2-derived Cu were synthesized, and subsequently employed as a C1 and C2+ activating catalyst and C2+ activating catalyst, respectively. For the first time, a kinetically linked dimer intermediate (∗OCCO) was observed and identified as the C2+ path triggering intermediate. The ATR-SEIRAS results suggest that C-C coupling occurs exclusively by CO dimerization toward ∗OCCO, without the participation of ∗CHO, which is an intermediate for CH4 production. In the real-time measurements, CO dimerization occurred concurrently with CO adsorption (∼5 s), while proton-coupled reduction toward ∗CHO has slower kinetics (∼30 s). We demonstrated that the sites showing a high vibrational frequency of ∗CO on the fragmented Cu surface are the potential active sites for the fast dimerization of CO. This work provides mechanistic insights into the CO2RR pathways and enables the design of efficient C2+-producing catalysts. © The Royal Society of Chemistry.
英文关键词	Absorption spectroscopy; Catalysts; Chemical activation; Dimerization; Dimers; Electrodes; Light absorption; Reduction; Attenuated total reflections; Carbon molecules; CO adsorption; CO2 reduction; Cu electrode; Real time measurements; Surface enhanced infrared absorption spectroscopy; Time-resolved; Copper; adsorption; carbon dioxide; catalyst; copper; electrochemical method; electrode; reaction kinetics; reduction
语种	英语
来源期刊	Energy & Environmental Science
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/189480
作者单位	Clean Energy Research Center, Korea Institute of Science and Technology, 5 Hwarang-ro 14-gil Seongbuk-gu, Seoul, 02792, South Korea; Department of Chemical and Biological Engineering, Sookmyung Women's University, Seoul, 04310, South Korea; Department of Chemistry, Korea Advanced Institute of Science and Technology (KAIST), Daejeon, 34141, South Korea; Graduate School of Energy and Environment, 145 Anam-ro Seongbuk-gu, Seoul, 02841, South Korea; Department of Chemical and Biomolecular Engineering, Yonsei-KIST Convergence Research Institute, Yonsei University, Seoul, 03722, South Korea; Division of Energy and Environmental Technology, Kist School, Korea University of Science and Technology (UST), Seoul, 02792, South Korea
推荐引用方式 GB/T 7714	Kim Y.,Park S.,Shin S.-J.,et al. Time-resolved observation of C-C coupling intermediates on Cu electrodes for selective electrochemical CO2reduction[J],2020,13(11).
APA	Kim Y..,Park S..,Shin S.-J..,Choi W..,Min B.K..,...&Hwang Y.J..(2020).Time-resolved observation of C-C coupling intermediates on Cu electrodes for selective electrochemical CO2reduction.Energy & Environmental Science,13(11).
MLA	Kim Y.,et al."Time-resolved observation of C-C coupling intermediates on Cu electrodes for selective electrochemical CO2reduction".Energy & Environmental Science 13.11(2020).