3d过渡金属氧化物/氢氧化物氧析出电催化DFT研究进展

Progress in DFT study on 3d transition metal oxide/hydroxide electrocatalyst for oxygen evolution

氧析出(OER)是电解水、空气电池充电等电化学能量转换与储存过程中的关键反应.从原子尺度上认识反应机理和构效关系是高效OER电催化剂设计与应用的基础.本文概述密度泛函理论(DFT)在3d过渡金属(Mn、Fe、Co、Ni)氧化物及氢氧化物OER电催化材料中的研究进展,介绍DFT+U方法研究晶体结构变化、元素掺杂、缺陷形成及基底装载对催化性能的影响,总结催化剂性能提升策略,并讨论DFT+U方法在3d金属氧化物催化剂的设计和改良中的研究发展方向.

Oxygen evolution reaction(OER) is a key reaction in electrochemical energy conversion and storage devices such as water electrolyzer and rechargeable metal-air battery. The design and application of efficient OER electrocatalysts rely largely on understanding of the mechanism and structure-activity relationship at the atomic scale. In this article, we briefly overview recent progress made in density functional theory(DFT) studies on 3 d transition metal(e.g., Mn, Fe, Co and Ni) oxide/hydroxide electrocatalysts for the OER. Using DFT correlated by on-site coulomb interactions(DFT+U), much insight can be gained in elucidating the effect of crystal structure, element doping, defect formation and substrate loading on the catalytic activity. Furthermore, representative examples and discussions are provided on the efficient strategies to improve the performance of 3 d transition metal-based electrocatalysts.