期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 140, 期 47, 页码 16237-16244出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.8b09743
关键词
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资金
- Office of Basic Energy Sciences (BES), Division of Materials Sciences and Engineering, of the U.S. Department of Energy (DOE) through the Structure and Dynamics of Materials Interfaces program [DE-AC02-05CH11231, FWP KC31SM]
- DOE
- Office of Science of the U.S. Department of Energy
Knowledge of the molecular composition and electronic structure of electrified solid-liquid interfaces is key to understanding elemental processes in heterogeneous reactions. Using X-ray absorption spectroscopy in the interface sensitive electron yield mode (EY-XAS), first-principles electronic structure calculations, and multiscale simulations, we determined the chemical composition of the interfacial region of a polycrystalline platinum electrode in contact with aqueous sulfuric acid solution at potentials between the hydrogen and oxygen evolution reactions. We found that between 0.7 and 1.3 V vs Ag/AgCl the electrical double layer (EDL) region comprises adsorbed sulfate ions with hydrated hydronium ions in the next layer. No evidence was found for bisulfate or Pt-O/Pt-OH species, which have very distinctive spectral signatures. In addition to resolving the long-standing issue of the EDL structure, our work establishes interface- and element-sensitive EY-XAS as a powerful spectroscopic tool for studying condensed phase, buried solid-liquid interfaces relevant to various electrochemical processes and devices.
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