期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 142, 期 27, 页码 11901-11914出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.0c04867
关键词
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资金
- European Research Council [681292]
- Marie Sklodowska-Curie Fellowship under the European Union's Horizon 2020 research and innovation program [838367]
- Ministry of Science and Technology, Taiwan [MOST 108-2628-M-002-004-RSP]
- Marie Curie Actions (MSCA) [838367] Funding Source: Marie Curie Actions (MSCA)
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 onco 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.
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