Metallic Single‐Unit‐Cell Orthorhombic Cobalt Diselenide Atomic Layers: Robust Water‐Electrolysis Catalysts
2015
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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