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Metallic Single‐Unit‐Cell Orthorhombic Cobalt Diselenide Atomic Layers: Robust Water‐Electrolysis Catalysts
Authors:Liang Liang  Dr Hao Cheng  Fengcai Lei  Dr Jun Han  Shan Gao  Dr Chengming Wang  Prof Yongfu Sun  Shaista Qamar  Prof Shiqiang Wei  Prof Yi Xie
Institution:1. Hefei National Laboratory for Physical Sciences at Microscale, Collaborative Innovation Center of Chemistry for Energy Materials, University of Science & Technology of China, Hefei, Anhui 230026 (P.R. China);2. National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui 230029 (P.R. China);3. Paul Scherrer Institut, 5232 Villigen PSI (Switzerland)
Abstract: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.
Keywords:atomic layers  cobalt diselenide  electrocatalysis  water splitting
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