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DOI10.1126/science.aba5005
Water-promoted interfacial pathways in methane oxidation to methanol on a CeO2-Cu2O catalyst
Liu Z.; Huang E.; Orozco I.; Liao W.; Palomino R.M.; Rui N.; Duchoň T.; Nemšák S.; Grinter D.C.; Mahapatra M.; Liu P.; Rodriguez J.A.; Senanayake S.D.
发表日期2020
ISSN0036-8075
起始页码513
结束页码517
卷号368期号:6490
英文摘要Highly selective oxidation of methane to methanol has long been challenging in catalysis. Here, we reveal key steps for the promotion of this reaction by water when tuning the selectivity of a well-defined CeO2/Cu2O/Cu(111) catalyst from carbon monoxide and carbon dioxide to methanol under a reaction environment with methane, oxygen, and water. Ambient-pressure x-ray photoelectron spectroscopy showed that water added to methane and oxygen led to surface methoxy groups and accelerated methanol production. These results were consistent with density functional theory calculations and kinetic Monte Carlo simulations, which showed that water preferentially dissociates over the active cerium ions at the CeO2–Cu2O/Cu(111) interface. The adsorbed hydroxyl species blocked O-O bond cleavage that would dehydrogenate methoxy groups to carbon monoxide and carbon dioxide, and it directly converted this species to methanol, while oxygen reoxidized the reduced surface. Water adsorption also displaced the produced methanol into the gas phase. © 2020 American Association for the Advancement of Science. All rights reserved.
关键词carbon dioxidecarbon monoxidecerium oxidecopper oxidemethanemethanoloxygenwateradsorptioncarbon dioxidecarbon monoxidecatalysiscatalystchemical bondinginorganic compoundmethaneoxidationadsorptionArticlecatalysischemical bondchemical reactiondehydrogenationdissociationenvironmentoxidationpriority journalX ray photoemission spectroscopy
语种英语
来源机构Science
文献类型期刊论文
条目标识符http://gcip.llas.ac.cn/handle/2XKMVOVA/133533
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GB/T 7714
Liu Z.,Huang E.,Orozco I.,et al. Water-promoted interfacial pathways in methane oxidation to methanol on a CeO2-Cu2O catalyst[J]. Science,2020,368(6490).
APA Liu Z..,Huang E..,Orozco I..,Liao W..,Palomino R.M..,...&Senanayake S.D..(2020).Water-promoted interfacial pathways in methane oxidation to methanol on a CeO2-Cu2O catalyst.,368(6490).
MLA Liu Z.,et al."Water-promoted interfacial pathways in methane oxidation to methanol on a CeO2-Cu2O catalyst".368.6490(2020).
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