Activating Lattice Oxygen in Spinel ZnCo2O4 through Filling Oxygen Vacancies with Fluorine for Electrocatalytic Oxygen Evolution

被引:228
作者
Xiao, Kang [1 ]
Wang, Yifan [2 ]
Wu, Peiyuan [1 ]
Hou, Liping [2 ]
Liu, Zhao-Qing [1 ]
机构
[1] Guangzhou Univ, Sch Chem & Chem Engn, Inst Clean Energy & Mat, Minist Educ,Guangzhou Key Lab Clean Energy & Mat,K, Guangzhou 510006, Peoples R China
[2] Guangzhou Univ, Sch Life Sci, Guangzhou 510006, Peoples R China
基金
中国国家自然科学基金;
关键词
Absorbate Evolution Mechanism; Lattice Oxidation Mechanism; Oxygen Evolution; Spinel; ZnCo2O4; WATER OXIDATION; BIFUNCTIONAL ELECTROCATALYST; CATALYTIC-ACTIVITY; OXIDE CATALYSTS; RECENT PROGRESS; PEROVSKITE; SITES; REDOX; NANOPARTICLES; PERFORMANCE;
D O I
10.1002/anie.202301408
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The development of productive catalysts for the oxygen evolution reaction (OER) remains a major challenge requiring significant progress in both mechanism and material design. Conventionally, the thermodynamic barrier of lattice oxidation mechanism (LOM) is lower than that of absorbate evolution mechanism (AEM) because the former can overcome certain limitations. However, controlling the OER pathway from the AEM to the LOM by exploiting the intrinsic properties of the catalyst remains challenging. Herein, we incorporated F anions into the oxygen vacancies of spinel ZnCo2O4 and established a link between the electronic structure and the OER catalytic mechanism. Theoretical density calculations revealed that F upshifts the O 2p center and activates the redox capability of lattice O, successfully triggering the LOM pathway. Moreover, the high electronegativity of F anions is favourable for balancing the residual protonation, which can stabilize the structure of the catalyst.
引用
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页数:10
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