期刊
NATURE COMMUNICATIONS
卷 5, 期 -, 页码 -出版社
NATURE PUBLISHING GROUP
DOI: 10.1038/ncomms5374
关键词
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资金
- School of Engineering and the Precourt Institute for Energy at Stanford University
- Gordon and Betty Moore Foundation [GBMF2573]
- National Science Foundation [1336835]
- US Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES), Division of Materials and Engineering Sciences [DE-AC04-94AL85000, DE-AC02-05CH11231]
- Stanford Graduate Fellowship
- Directorate For Engineering
- Div Of Chem, Bioeng, Env, & Transp Sys [1336835] Funding Source: National Science Foundation
Electrochemical incorporation reactions are ubiquitous in energy storage and conversion devices based on mixed ionic and electronic conductors, such as lithium-ion batteries, solid-oxide fuel cells and water-splitting membranes. The two-way traffic of ions and electrons across the electrochemical interface, coupled with the bulk transport of mass and charge, has been challenging to understand. Here we report an investigation of the oxygen-ion incorporation pathway in CeO2-delta (ceria), one of the most recognized oxygen-deficient compounds, during hydrogen oxidation and water splitting. We probe the response of surface oxygen vacancies, electrons and adsorbates to the electrochemical polarization at the ceria-gas interface. We show that surface oxygen-ion transfer, mediated by oxygen vacancies, is fast. Furthermore, we infer that the electron transfer between cerium cations and hydroxyl ions is the rate-determining step. Our in operando observations reveal the precise roles of surface oxygen vacancy and electron defects in determining the rate of surface incorporation reactions.
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