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氢氧化镍铁晶格拉伸应变:增强对含氧中间体的吸附以实现高效水氧化催化

NiFe Hydroxide Lattice Tensile Strain: Enhancement of Adsorption of Oxygenated Intermediates for Efficient Water Oxidation Catalysis.

作者信息

Zhou Daojin, Wang Shiyuan, Jia Yin, Xiong Xuya, Yang Hongbin, Liu Song, Tang Jialun, Zhang Junming, Liu Dong, Zheng Lirong, Kuang Yun, Sun Xiaoming, Liu Bin

机构信息

State Key Laboratory of Chemical Resource Engineering, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029, China.

School of Chemical and Biomedical Engineering, Nanyang Technological University, Singapore, 637459, Singapore), E-mail: Bin Liu.

出版信息

Angew Chem Int Ed Engl. 2019 Jan 14;58(3):736-740. doi: 10.1002/anie.201809689. Epub 2018 Dec 17.

Abstract

The binding strength of reactive intermediates with catalytically active sites plays a crucial role in governing catalytic performance of electrocatalysts. NiFe hydroxide offers efficient oxygen evolution reaction (OER) catalysis in alkaline electrolyte, however weak binding of oxygenated intermediates on NiFe hydroxide still badly limits its catalytic activity. Now, a facile ball-milling method was developed to enhance binding strength of NiFe hydroxide to oxygenated intermediates via generating tensile strain, which reduced the anti-bonding filling states in the d orbital and thus facilitated oxygenated intermediates adsorption. The NiFe hydroxide with tensile strain increasing after ball-milling exhibits an OER onset potential as low as 1.44 V (vs. reversible hydrogen electrode) and requires only a 270 mV overpotential to reach a water oxidation current density of 10 mA cm .

摘要

反应中间体与催化活性位点的结合强度在决定电催化剂的催化性能方面起着关键作用。氢氧化镍铁在碱性电解质中提供高效的析氧反应(OER)催化,然而,含氧中间体在氢氧化镍铁上的弱结合仍然严重限制了其催化活性。现在,人们开发了一种简便的球磨方法,通过产生拉伸应变来增强氢氧化镍铁与含氧中间体的结合强度,这减少了d轨道中的反键填充态,从而促进了含氧中间体的吸附。球磨后拉伸应变增加的氢氧化镍铁表现出低至1.44 V(相对于可逆氢电极)的OER起始电位,并且仅需要270 mV的过电位就能达到10 mA cm 的水氧化电流密度。

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