Journal
NATURE CATALYSIS
Volume 4, Issue 1, Pages 36-45Publisher
NATURE PORTFOLIO
DOI: 10.1038/s41929-020-00550-5
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Funding
- US National Science Foundation [CBET-1805022, CBET-2004808, CBET-2005250]
- US DOE [DE-AC02-06CH11357]
- Canadian Light Source
- US DOE Office of Science Facility, at Brookhaven National Laboratory [DE-SC0012704]
- US DOE Office of Science User Facility [DE-AC02-05CH11231]
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Efficient single-site Co catalysts supported on well-defined TiO2 nanorods were found to exhibit excellent performance in the oxygen evolution reaction (OER), with turnover frequencies among the highest reported for Co-based catalysts. Computational and experimental results showed good agreement in describing the catalytic reaction kinetics and mechanisms.
Efficient electrocatalysts for the oxygen evolution reaction (OER) are paramount to the development of electrochemical devices for clean energy and fuel conversion. However, the structural complexity of heterogeneous electrocatalysts makes it a great challenge to elucidate the surface catalytic sites and OER mechanisms. Here, we report that catalytic single-site Co in a well-defined brookite TiO2 nanorod (210) surface (Co-TiO2) presents turnover frequencies that are among the highest for Co-based heterogeneous catalysts reported to date, reaching 6.6 +/- 1.2 and 181.4 +/- 28 s(-1) at 300 and 400 mV overpotentials, respectively. Based on grand canonical quantum mechanics calculations and the single-site Co atomic structure validated by in situ and ex situ spectroscopic probes, we have established a full description of the catalytic reaction kinetics for Co-TiO2 as a function of applied potential, revealing an adsorbate evolution mechanism for the OER. The computationally predicted Tafel slope and turnover frequencies exhibit exceedingly good agreement with experiment.
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