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Research Article

Operando reconstruction-induced CO2 reduction activity and selectivity for cobalt-based photocatalysis

Kun Zhao1,§( )Weiying Pang1,§Shuaiyu Jiang3,§Canyu Hu4Porun Liu3Dandan Cui5Xuefei An1Baojuan Tian1Chao Gao4Pan Zhang1Meng Tian2( )Dong Fu1( )Huijun Zhao3( )
Hebei Key Lab of Power Plant Flue Gas Multi-Pollutants Control, School of Environmental Science and Engineering, North China Electric Power University, Baoding 071003, China
Interdisciplinary Center for Fundamental and Frontier Sciences, Nanjing University of Science and Technology, Jiangyin 214443, China
Centre for Catalysis and Clean Energy, Griffith University Gold Coast Campus, LD 4222, Australia
Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovative Center of Chemistry for Energy Materials, School of Chemistry and Materials Science, and National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei 230026, China
School of Physics and BUAA-UOW Joint Research Centre, Beihang University, Beijing 100191, China

§ Kun Zhao, Weiying Pang, and Shuaiyu Jiang contributed equally to this work.

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Graphical Abstract

The oxygen atom coordination inducing the structure reconstruction of the catalytic sites would lead to an enhanced activity and selectivity for photocatalytic CO2 reduction into CO.

Abstract

The oxygen atom coordination inducing the structure reconstruction of the catalytic site is identified and recognized ambiguously, which is related to accurately declare the mechanism in a dynamic catalytic process. Herein, we demonstrated that the reconstructed catalytic sites would lead to a remarkable performance for photocatalytic CO2 reduction. At the initial 4-cycles testing, the in-situ formation of CoOx active sites on the Co (CoP) surface performed an increasing transient activity and selectivity toward CO evolution. The formation of reconstructive Co-O bond and the appearance of intermediate specie CO were simultaneously observed by the pre-operando Raman, revealing the dynamic relationship between catalytic site structure and the photocatalytic properties. Moreover, density functional theory calculations showed that the electronic structure of the reconstructive surface sites could modulate the ability of CO2 adsorption and CO desorption. The reduced barrier energy for the rate-determining step finally improved the activity and selectivity of CO2 reduction.

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Nano Research
Pages 4812-4820
Cite this article:
Zhao K, Pang W, Jiang S, et al. Operando reconstruction-induced CO2 reduction activity and selectivity for cobalt-based photocatalysis. Nano Research, 2023, 16(4): 4812-4820. https://doi.org/10.1007/s12274-023-5432-5
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Received: 05 November 2022
Revised: 19 December 2022
Accepted: 20 December 2022
Published: 23 January 2023
© Tsinghua University Press 2023
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