过电位
析氧
分解水
催化作用
密度泛函理论
化学
制氢
材料科学
物理化学
化学物理
化学工程
计算化学
电化学
有机化学
电极
光催化
工程类
作者
Yanan Zhou,Lanlan Chen,Li Sheng,Qiquan Luo,Wenhua Zhang,Jinlong Yang
出处
期刊:Nano Research
[Springer Nature]
日期:2022-06-21
卷期号:15 (9): 7994-8000
被引量:36
标识
DOI:10.1007/s12274-022-4510-4
摘要
The electrochemical oxygen evolution reaction (OER) is a half-reaction of water-splitting for hydrogen generation, yet suffers from its sluggish kinetics and large overpotential. It is highly desirable to develop efficient and stable OER electrocatalysts for the advancement of water-splitting. Herein, by means of density functional theory (DFT) calculations, we systematically investigated a series of two-dimensional (2D) dual-atom catalysts (DACs) on a novel synthesized covalent organic framework (COF) material as potential efficient catalysts toward the OER. The designed 6 homonuclear (2TM-COF) and 15 heteronuclear (TM1TM2-COF) DACs all exhibit good stability. There is a strong scaling relationship between the adsorption Gibbs free energies of HO* and HOO* intermediates, and the OER overpotential (ηOER) volcano curve can be plotted as a function of ∆GO* − ∆GHO*. RhIr-COF shows the best OER catalytic activity with a ηOER value of 0.29 V, followed by CoNi-COF (0.33 V), RuRh-COF (0.34 V), and Nilr-COF (0.37 V). These four OER DACs exhibit lower onset potential and higher current density than that of the IrO2(110) benchmark catalyst. Aided by the descriptor identification study, the Bader charge that correlated with the Pauling electronegativity of the embedded dual-metal atoms was found to be the most important factor governing the catalytic activity of the OER. Our work highlights a potentially efficient class of 2D COF-based DACs toward the OER.
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