https://scholars.lib.ntu.edu.tw/handle/123456789/575726
標題: | Mechanism of Oxygen Evolution Catalyzed by Cobalt Oxyhydroxide: Cobalt Superoxide Species as a Key Intermediate and Dioxygen Release as a Rate-Determining Step | 作者: | Moysiadou A Lee S Hsu C.-S Chen H.M Hu X. HAO MING CHEN |
關鍵字: | Absorption spectroscopy; Catalysts; Cobalt metallography; Hydrogen fuels; Oxygen evolution reaction; Reaction intermediates; Spectroscopic analysis; Transition metal oxides; Transition metals; X ray absorption; Active intermediates; Cobalt oxyhydroxide; Oxygen evolution; Oxygen evolution reaction (oer); Oxygen isotope exchange; Rate determining step; Renewable energies; Spectroscopic method; Cobalt compounds; cobalt derivative; cobalt oxyhydroxide; cobalt superoxide species; hydrogen; hydroxide; oxygen; superoxide; unclassified drug; Article; catalysis; catalyst; chemical analysis; chemical reaction; chemical structure; electrochemical analysis; experimental study; kinetics; oxygen evolution; Raman spectrometry; spectroscopy; X ray absorption spectroscopy | 公開日期: | 2020 | 卷: | 142 | 期: | 27 | 起(迄)頁: | 11901-11914 | 來源出版物: | Journal of the American Chemical Society | 摘要: | The oxygen evolution reaction (OER) is the performance-limiting half reaction of water splitting, which can be used to produce hydrogen fuel using renewable energies. Whereas a number of transition metal oxides and oxyhydroxides have been developed as promising OER catalysts in alkaline medium, the mechanisms of OER on these catalysts are not well understood. Here we combine electrochemical and in situ spectroscopic methods, particularly operando X-ray absorption and Raman spectroscopy, to study the mechanism of OER on cobalt oxyhydroxide (CoOOH), an archetypical unary OER catalyst. We find the dominating resting state of the catalyst as a Co(IV) species CoO2. Through oxygen isotope exchange experiments, we discover a cobalt superoxide species as an active intermediate in the OER. This intermediate is formed concurrently to the oxidation of CoOOH to CoO2. Combing spectroscopic and electrokinetic data, we identify the rate-determining step of the OER as the release of dioxygen from the superoxide intermediate. The work provides important experimental fingerprints and new mechanistic perspectives for OER catalysts. ? 2020 American Chemical Society. |
URI: | https://www.scopus.com/inward/record.uri?eid=2-s2.0-85088208094&doi=10.1021%2fjacs.0c04867&partnerID=40&md5=ca288bcf8442a888656d4d9ffa659ad6 https://scholars.lib.ntu.edu.tw/handle/123456789/575726 |
ISSN: | 27863 | DOI: | 10.1021/jacs.0c04867 | SDG/關鍵字: | Absorption spectroscopy; Catalysts; Cobalt metallography; Hydrogen fuels; Oxygen evolution reaction; Reaction intermediates; Spectroscopic analysis; Transition metal oxides; Transition metals; X ray absorption; Active intermediates; Cobalt oxyhydroxide; Oxygen evolution; Oxygen evolution reaction (oer); Oxygen isotope exchange; Rate determining step; Renewable energies; Spectroscopic method; Cobalt compounds; cobalt derivative; cobalt oxyhydroxide; cobalt superoxide species; hydrogen; hydroxide; oxygen; superoxide; unclassified drug; Article; catalysis; catalyst; chemical analysis; chemical reaction; chemical structure; electrochemical analysis; experimental study; kinetics; oxygen evolution; Raman spectrometry; spectroscopy; X ray absorption spectroscopy |
顯示於: | 化學系 |
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