首页|Unveiling the geometric site dependent activity of spinel Co3O4 for electrocatalytic chlorine evolution reaction

Unveiling the geometric site dependent activity of spinel Co3O4 for electrocatalytic chlorine evolution reaction

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Spinel cobalt oxide(Co3O4),consisting of tetrahedral Co2+(CoTd)and octahedral Co3+(CoOh),is considered as promising earth-abundant electrocatalyst for chlorine evolution reaction(CER).Identifying the cat-alytic contribution of geometric Co site in the electrocatalytic CER plays a pivotal role to precisely mod-ulate electronic configuration of active Co sites to boost CER.Herein,combining density functional theory calculations and experiment results assisted with operando analysis,we found that the CoOh site acts as the main active site for CER in spinel Co3O4,which shows better Cl-adsorption and more moderate inter-mediate adsorption toward CER than CoTd site,and does not undergo redox transition under CER condi-tion at applied potentials.Guided by above findings,the oxygen vacancies were further introduced into the Co3O4 to precisely manipulate the electronic configuration of Cooh to boost Cl-adsorption and opti-mize the reaction path of CER and thus to enhance the intrinsic CER activity significantly.Our work fig-ures out the importance of geometric configuration dependent CER activity,shedding light on the rational design of advanced electrocatalysts from geometric configuration optimization at the atomic level.

Chlorine evolution reactionGeometry effectsActive chlorineElectronic configuration optimizationSpinel oxides

Linke Cai、Yao Liu、Jingfang Zhang、Qiqi Jia、Jiacheng Guan、Hongwei Sun、Yu Yu、Yi Huang

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Key Laboratory of Pesticide & Chemical Biology of Ministry of Education,Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction of Ministry of Education,College of Chemistry,Central China Normal University,Wuhan 430079,Hubei,China

College of Materials Science and Engineering,Fuzhou University,Fuzhou 350108,Fujian,China

Key Laboratory of Green Chemical Engineering Process of Ministry of Education,Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of Education,Hubei Key Laboratory of Novel Reactor and Green Chemical Technology,School of Chemical Engineering & Pharmacy,Wuhan Institute of Technology,Wuhan 430205,Hubei,China

School of Chemistry and Chemical Engineering,Anhui University,Hefei 230601,Anhui,China

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National Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNatural Science Foundation of HubeiFundamental Research Funds for the Central China Normal University(CCNU)

U21A2028622206054218050692021CFB094

2024

10.1016/j.jechem.2023.12.002

能源化学
中国科学院大连化学物理研究所 中国科学院成都有机化学研究所

能源化学

CSTPCDEI
影响因子：0.654
ISSN：2095-4956
年,卷(期)：2024.92(5)