期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 54, 期 41, 页码 12004-12008出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201505245
关键词
atomic layers; cobalt diselenide; electrocatalysis; water splitting
资金
- National Basic Research Program of China [2015CB932302]
- National Nature Science Foundation [21331005, 21422107, 21201157, 91422303, 11321503]
- Program for New Century Excellent Talents in University [NCET-13-0546]
- Youth Innovation Promotion Association of CAS [CX2340000100]
- Fundamental Research Funds for Central Universities [WK2340000063]
The bottleneck in water electrolysis lies in the kinetically sluggish oxygen evolution reaction (OER). Herein, conceptually new metallic non-metal atomic layers are proposed to overcome this drawback. Metallic single-unit-cell CoSe2 sheets with an orthorhombic phase are synthesized by thermally exfoliating a lamellar CoSe2-DETA hybrid. The metallic character of orthorhombic CoSe2 atomic layers, verified by DFT calculations and temperature-dependent resistivities, allows fast oxygen evolution kinetics with a lowered overpotential of 0.27 V. The single-unit-cell thickness means 66.7% of the Co2+ ions are exposed on the surface and serve as the catalytically active sites. The lowered Co2+ coordination number down to 1.3 and 2.6, gives a lower Tafel slope of 64 mV dec(-1) and higher turnover frequency of 745 h(-1). Thus, the single-unit-cell CoSe2 sheets have around 2 and 4.5 times higher catalytic activity compared with the lamellar CoSe2-DETA hybrid and bulk CoSe2.
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