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Direct 12-Electron Oxidation of Ethanol on a Ternary Au(core)-PtIr(Shell) Electrocatalyst

Liang, Zhixiu, Song, Liang, Deng, Shiqing, Zhu, Yimei, Stavitski, Eli, Adzic, Radoslav R., Chen, Jingyi, Wang, Jia X.·2019·Journal of the American Chemical Society

Abstract

Understanding the roles of metals and atomic structures in activating various elementary steps of electrocatalytic reactions can help rational design of binary or ternary catalysts for promoting activity toward desirable products via favorable pathways. Here we report on a newly developed ternary [email protected] core–shell catalyst for ethanol oxidation reaction (EOR) in alkaline solutions, which exhibits an activity enhancement of 6 orders of magnitude compared to AuPtIr alloy catalysts. Analysis of in situ infrared reflection absorption spectra for [email protected] and its bimetallic subsets, [email protected] and PtIr alloy, found that monatomic steps and Au-induced tensile strain on PtIr facilitate C–C bond splitting via ethanol dissociative adsorption and Ir promotes dehydrogenation at low potentials. As evidenced by the CO band being observed only for the PtIr alloy that is rather inactive for ethanol dissociative adsorption, we propose that splitting the C–C bond at the earliest stage of EOR activates a direct 12-electron full oxidation pathway because hydrogen-rich fragments can be fully oxidized without CO as a poisoning intermediate. The resulting synergy of complementary effects of Au core and surface Ir leads to an outstanding performance of [email protected] for EOR as characterized by a low onset potential of 0.3 V and 8.3 A mg –1 all-metals peak current with 57% currents generated via full ethanol oxidation.

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Crossref · 10.1021/jacs.9b03474

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Metadata

Authors
Liang, Z., Song, L., Deng, S., Zhu, Y., Stavitski, E., Adzic, R. R., Chen, J., & Wang, J. X.
Venue
Journal of the American Chemical Society
Published
2019-05-26
Volume
141
Issue
24
Pages
9629-9636
ISSN
  • 0002-7863 (ISSN-L)
  • 1520-5126
OpenAlex
W2945768880
Cited by
209
References
1
FWCI
4.95
Type
journal article
Language
en
Open access
closed

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