期刊
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
卷 13, 期 13, 页码 3047-3052出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.1c04187
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资金
- National Science Foundation (NSF) through the NSF CAREER award [CBET-1941204]
- Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231]
- Holland Computing Center at the University of Nebraska-Lincoln
Cathodic corrosion of metals, discovered over 120 years ago, still remains poorly understood. This study uses density-functional-theory calculations to elucidate the identity of reaction intermediates and their reactivity at the Pt(111)/electrolyte interface, providing new insights into this process.
Cathodic corrosion of metals discovered more than 120 yearsago remains a poorly understood electrochemical process. It is believed thatthe corrosion intermediates formed during cathodic polarization areextremely short-lived species because of their high reactivity. Togetherwith the concurrent vigorous hydrogen evolution, this makes it challengingto investigate the reaction mechanism and detect the intermediatesexperimentally. From a computational standpoint, the process also presentsa serious challenge as it occurs at rather low negative potentials inconcentrated alkaline solutions. Here, we use density-functional-theorycalculations to elucidate the identity of reaction intermediates and theirreactivity at the Pt(111)/electrolyte interface. By controlling the electrodepotential in an experimentally relevant region through constant Fermi-level molecular dynamics, we reveal the formation of alkalication-stabilized Pt hydrides as intermediates of cathodic corrosion. The results also suggest that the found Pt anions could dischargeat the interface to produce H2by reacting with either surface-bound hydrogen species or solution water molecules
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