Operando Identification of the Dynamic Behavior of Oxygen Vacancy-Rich Co3O4 for Oxygen Evolution Reaction

化学 析氧 电催化剂 X射线光电子能谱 氧气 价(化学) 循环伏安法 X射线吸收精细结构 介电谱 催化作用 电化学 氧化还原 氧气储存 空位缺陷 反应机理 无机化学 化学工程 光谱学 物理化学 结晶学 电极 有机化学 工程类 物理 量子力学
作者
Zhaohui Xiao,Yucheng Huang,Chung‐Li Dong,Chao Xie,Zhijuan Liu,Shiqian Du,Wei Chen,Dafeng Yan,Tao Li,Zhiwen Shu,Guanhua Zhang,Huigao Duan,Yanyong Wang,Yuqin Zou,Ru Chen,Shuangyin Wang
出处
期刊:Journal of the American Chemical Society [American Chemical Society]
卷期号:142 (28): 12087-12095 被引量:1074
标识
DOI:10.1021/jacs.0c00257
摘要

The exact role of a defect structure on transition metal compounds for electrocatalytic oxygen evolution reaction (OER), which is a very dynamic process, remains unclear. Studying the structure-activity relationship of defective electrocatalysts under operando conditions is crucial for understanding their intrinsic reaction mechanism and dynamic behavior of defect sites. Co3O4 with rich oxygen vacancy (VO) has been reported to efficiently catalyze OER. Herein, we constructed pure spinel Co3O4 and VO-rich Co3O4 as catalyst models to study the defect mechanism and investigate the dynamic behavior of defect sites during the electrocatalytic OER process by various operando characterizations. Operando electrochemical impedance spectroscopy (EIS) and cyclic voltammetry (CV) implied that the VO could facilitate the pre-oxidation of the low-valence Co (Co2+, part of which was induced by the VO to balance the charge) at a relatively lower applied potential. This observation confirmed that the VO could initialize the surface reconstruction of VO-Co3O4 prior to the occurrence of the OER process. The quasi-operando X-ray photoelectron spectroscopy (XPS) and operando X-ray absorption fine structure (XAFS) results further demonstrated the oxygen vacancies were filled with OH• first for VO-Co3O4 and facilitated pre-oxidation of low-valence Co and promoted reconstruction/deprotonation of intermediate Co-OOH•. This work provides insight into the defect mechanism in Co3O4 for OER in a dynamic way by observing the surface dynamic evolution process of defective electrocatalysts and identifying the real active sites during the electrocatalysis process. The current finding would motivate the community to focus more on the dynamic behavior of defect electrocatalysts.
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