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基于CoO的催化剂的活性电子密度调制增强了它们的析氧性能。

Active Electron Density Modulation of Co O -Based Catalysts Enhances their Oxygen Evolution Performance.

作者信息

He Dong, Song Xianyin, Li Wenqing, Tang Chongyang, Liu Jiangchao, Ke Zunjian, Jiang Changzhong, Xiao Xiangheng

机构信息

Department of Physics, Key Laboratory of Artificial Micro- and Nano-structures of Ministry of Education, Hubei Nuclear Solid Physics Key Laboratory, Wuhan University, Wuhan, 430072, P. R. China.

出版信息

Angew Chem Int Ed Engl. 2020 Apr 20;59(17):6929-6935. doi: 10.1002/anie.202001681. Epub 2020 Mar 19.

Abstract

Despite the fact that many strategies have been developed to improve the efficiency of the oxygen evolution reaction (OER), the precise modulation of the surface electronic properties of catalysts to improve their catalytic activity is still challenging. Herein, we demonstrate that the surface active electron density of Co O can be effectively regulated by an argon-ion irradiation method. X-ray photoelectron and synchrotron x-ray absorption spectroscopy, UV photoelectron spectrometry, and DFT calculations show that the surface active electron density band center of Co O has been upshifted, leading to a significantly enhanced absorption capability of the oxo group. The optimized Co O -based catalysts exhibit an excellent overpotential of 260 mV at 10 mA cm and Tafel slope of 54 mV dec , superior to the capability of the benchmark RuO , representing one of the best Co-based OER catalysts. This approach could guide the future rational design and discovery of ideal electrocatalysts.

摘要

尽管已经开发出许多策略来提高析氧反应(OER)的效率,但精确调节催化剂的表面电子性质以提高其催化活性仍然具有挑战性。在此,我们证明了通过氩离子辐照方法可以有效地调节CoO的表面活性电子密度。X射线光电子能谱和同步辐射X射线吸收光谱、紫外光电子能谱以及密度泛函理论计算表明,CoO的表面活性电子密度带中心已经上移,导致氧代基团的吸收能力显著增强。优化后的CoO基催化剂在10 mA cm时表现出260 mV的优异过电位和54 mV dec的塔菲尔斜率,优于基准RuO的性能,代表了最佳的Co基OER催化剂之一。这种方法可以指导未来理想电催化剂的合理设计和发现。

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