Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 142, Issue 43, Pages 18378-18386Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.0c05050
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Funding
- National Natural Science Foundation of China [21931001, 21922105, 51771085, 51801088]
- Special Fund Project of Guiding Scientific and Technological Innovation Development of Gansu Province [2019ZX-04]
- 111 Project [B20027]
- Natural Science Foundation of China (NSFC) [21771156]
- Early Career Scheme (ECS) fund from the Research Grant Council (RGC) in Hong Kong [PolyU 253026/16P]
- National Postdoctoral Program for Innovative Talents [BX20200157]
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Simultaneous realization of improved activity, enhanced stability, and reduced cost remains a desirable yet challenging goal in the search of electrocatalysis oxygen evolution reaction (OER) in acid. Herein, we report a novel strategy to prepare iridium single-atoms (Ir-SAs) on ultrathin NiCo2O4 porous nanosheets (Ir-NiCo2O4 NSs) by the co-electrodeposition method. The surface-exposed Ir-SAs couplings with oxygen vacancies (V-o) exhibit boosting the catalysts OER activity and stability in acid media. They display superior OER performance with an ultralow overpotential of 240 mV at j = 10 mA cm(-2) and long-term stability of 70 h in acid media. The TOFs of 1.13 and 6.70 s(-1) at an overpotential of 300 and 370 mV also confirm their remarkable performance. Density functional theory (DFT) calculations reveal that the prominent OER performance arises from the surface electronic exchange-andtransfer activities contributed by atomic Ir incorporation on the intrinsic V-o existed NiCo2O4 surface. The atomic Ir sites substantially elevate the electronic activity of surface lower coordinated Co sites nearby V-o, which facilitate the surface electronic exchange-and-transfer capabilities. With this trend, the preferred H2O activation and stabilized *O have been reached toward competitively lower overpotential. This is a generalized key for optimally boosting OER performance.
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