Unraveling Sequential Oxidation Kinetics and Determining Roles of Multi-Cobalt Active Sites on Co3O4 Catalyst for Water Oxidation

被引:90
|
作者
Kang, Wanchao [1 ,2 ]
Wei, Ruifang [2 ]
Yin, Heng [2 ]
Li, Dongfeng [2 ,3 ]
Chen, Zheng [2 ]
Huang, Qinge [2 ]
Zhang, Pengfei [2 ]
Jing, Huanwang [1 ]
Wang, Xiuli [2 ]
Li, Can [1 ,2 ,3 ]
机构
[1] Lanzhou Univ, Coll Chem & Chem Engn, State Key Lab Appl Organ Chem, Key Lab Adv Catalysis, Lanzhou 730000, Gansu, Peoples R China
[2] Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
[3] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
基金
中国国家自然科学基金;
关键词
OXYGEN EVOLUTION REACTION; ELECTROCATALYSTS; IDENTIFICATION; MECHANISM; SURFACE; PLANET; OXIDES; STATES;
D O I
10.1021/jacs.2c11508
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The multi-redox mechanism involving multi-sites has great implications to dictate the catalytic water oxidation. Understanding the sequential dynamics of multi-steps in oxygen evolution reaction (OER) cycles on working catalysts is a highly important but challenging issue. Here, using quasi-operando transient absorption (TA) spectroscopy and a typical photo-sensitization strategy, we succeeded in resolving the sequential oxidation kinetics involving multi-active sites for water oxidation in OER catalytic cycle, with Co3O4 nanoparticles as model catalysts. When OER initiates from fast oxidation of surface Co2+ ions, both surface Co2+ and Co3+ ions are active sites of the multi-cobalt centers for water oxidation. In the sequential kinetics (Co2+-* Co3+-* Co4+), the key characteristic is fast oxidation and slow consumption for all the cobalt species. Due to this characteristic, the Co4+ intermediate distribution plays a determining role in OER activity and results in the slow overall OER kinetics. These insights shed light on the kinetic understanding of water oxidation on heterogeneous catalysts with multi-sites.
引用
收藏
页码:3470 / 3477
页数:8
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