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Nano Research 2023, 16(4): 4812-4820 https://doi.org/10.1007/s12274-023-5432-5
Research Article | Issue | Published: 23 January 2023

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

Show Author's Information Kun Zhao1,§( ),  Weiying Pang1,§,  Shuaiyu Jiang3,§,  Canyu Hu4,  Porun Liu3,  Dandan Cui5,  Xuefei An1,  Baojuan Tian1,  Chao Gao4,  Pan Zhang1,  Meng 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.

Keywords:
surface reconstruction, photocatalytic CO2 reduction, balanced relationship, unsaturated Co-Ox catalytic site
Topics:
Photocatalysis
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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Abstract Full text Electronic supplementary material About this article

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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Electronic supplementary material
About this article

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

Show Author's information Kun Zhao1,§( ), Weiying Pang1,§, Shuaiyu Jiang3,§, Canyu Hu4, Porun Liu3, Dandan Cui5, Xuefei An1, Baojuan Tian1, Chao Gao4, Pan Zhang1, Meng 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.

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.

Keywords: surface reconstruction, photocatalytic CO2 reduction, balanced relationship, unsaturated Co-Ox catalytic site

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Publication history
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Acknowledgements

Publication history

Received: 05 November 2022
Revised: 19 December 2022
Accepted: 20 December 2022
Published: 23 January 2023
Issue date: April 2023

Copyright

© Tsinghua University Press 2023

Acknowledgements

Acknowledgements

The authors appreciate the financial support from the National Natural Science Foundation of China (Nos. 51776072, 42007327, and 41731279), the Fundamental Research Funds for the Central Universities (No. 2021MS098), the Natural Science Foundation of Hebei Province (No. B2022502005), and the Natural Science Foundation of Jiangsu Province (No. BK20220930). The authors acknowledge that the XAS measurements were performed using [AS183/XAS/14123] beamline of Australian Synchrotron facility. We also thank Zumin Wang’s constructive suggestion and kind help with the manuscript revision.

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