期刊
ACS CATALYSIS
卷 10, 期 3, 页码 1855-+出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.9b05170
关键词
oxygen evolution reaction; cobalt sulfides; operando Raman spectroscopy; operando X-ray absorption spectroscopy; active species transformation
资金
- National Natural Science Foundation of China [51961165103, 51672210]
- National Key Research and Development Program of China [2018YFB1502003, 2017YFE0193900]
- National Program for Support of Top-notch Young Professionals
In-depth understanding of electrocatalytically active species transformation during oxygen evolution reaction (OER) is highly guidable to design effective electrocatalysts for water splitting. Herein, cobalt sulfide (CoSx) nanovesicles decorated with iron sulfide (FeSx) heterophases were successfully synthesized by using a metal-organic framework precursor through a solvothermal method. The obtained CoSx/FeSx exhibited much elevated OER activity as compared to pristine CoSx and even most previously reported cobalt-based electrocatalysts, with the overpotential of 304 mV at 10 mA cm(-2) in 1 M KOH. As revealed by operando Raman and X-ray absorption spectroscopy measurements, the electrocatalytically active species transformation in CoSx nanovesicles could be stimulated by the incorporated FeSx heterophases due to the increased average valence state of cobalt and lowered coordination of cobalt sites. As a result, the electrocatalytically active cobalt oxyhydroxides could be more easily formed on the catalyst surface during OER and thus contributed to the highly improved performance. This real-time spectral and electrochemical insight into the electrocatalytically active species transformation may guide the rational design of highly efficient electrocatalysts for water splitting from the viewpoint of electronic structure-electrocatalytic activity relationship.
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