气候变化领域集成服务门户(CCPortal): CO2 reduction on pure Cu produces only H2 after subsurface O is depleted: Theory and experiment

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DOI	10.1073/pnas.2012649118
	CO2 reduction on pure Cu produces only H2 after subsurface O is depleted: Theory and experiment
	Liu G.; Lee M.; Kwon S.; Zeng G.; Eichhorn J.; Buckley A.K.; Toste F.D.; Goddard W.A.; III; Toma F.M.
发表日期	2021
ISSN	0027-8424
卷号	118 期号:23
英文摘要	We elucidate the role of subsurface oxygen on the production of C2 products from CO2 reduction over Cu electrocatalysts using the newly developed grand canonical potential kinetics density functional theory method, which predicts that the rate of C2 production on pure Cu with no O is ∼500 times slower than H2 evolution. In contrast, starting with Cu2O, the rate of C2 production is >5,000 times faster than pure Cu(111) and comparable to H2 production. To validate these predictions experimentally, we combined time-dependent product detection with multiple characterization techniques to show that ethylene production decreases substantially with time and that a sufficiently prolonged reaction time (up to 20 h) leads only to H2 evolution with ethylene production ∼1,000 times slower, in agreement with theory. This result shows that maintaining substantial subsurface oxygen is essential for long-term C2 production with Cu catalysts. © 2021 National Academy of Sciences. All rights reserved.
英文关键词	DFT; Electrocatalysis; Ethylene evolution; Grand canonical potential kinetics; Hydrogen evolution reaction
语种	英语
来源期刊	Proceedings of the National Academy of Sciences of the United States of America
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/238534
作者单位	Joint Center for Artificial Photosynthesis, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, United States; Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, United States; Liquid Sunlight Alliance, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, United States; Department of Chemistry and Chemical Biology, Cornell University, Ithaca, NY 14853, United States; Materials and Process Simulation Center, California Institute of Technology, Pasadena, CA 91125, United States; Joint Center for Artificial Photosynthesis, California Institute of Technology, Pasadena, CA 91125, United States; Liquid Sunlight Alliance, California Institute of Technology, Pasadena, CA 91125, United States; Walter Schottky Institut, Technische Universität München, Garching, 85748, Germany; Physik Department, Technische Universität München, Garching, 85748, Germany; Department of Chemistry, University of California, Berkeley, CA 94720, United States
推荐引用方式 GB/T 7714	Liu G.,Lee M.,Kwon S.,et al. CO2 reduction on pure Cu produces only H2 after subsurface O is depleted: Theory and experiment[J],2021,118(23).
APA	Liu G..,Lee M..,Kwon S..,Zeng G..,Eichhorn J..,...&Toma F.M..(2021).CO2 reduction on pure Cu produces only H2 after subsurface O is depleted: Theory and experiment.Proceedings of the National Academy of Sciences of the United States of America,118(23).
MLA	Liu G.,et al."CO2 reduction on pure Cu produces only H2 after subsurface O is depleted: Theory and experiment".Proceedings of the National Academy of Sciences of the United States of America 118.23(2021).