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Nano Research 2022, 15(9): 8001-8009 https://doi.org/10.1007/s12274-022-4629-3
Research Article | Issue | Published: 23 June 2022

Spatial confinement of copper single atoms into covalent triazine-based frameworks for highly efficient and selective photocatalytic CO2 reduction

Show Author's Information Guocheng Huang1,  Qing Niu1,  Yuxin He1,  Jinjin Tian1,  Mingbin Gao4( ),  Chaoyang Li5,  Ning An5,  Jinhong Bi1,3( ),  Jiangwei Zhang2,4,5( )
Department of Environmental Science and Engineering, Fuzhou University, Fuzhou 350108, China
Advanced Chemical Engineering and Energy Materials Research Center, China University of Petroleum (East China), Qingdao 266580, China
State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University, Fuzhou 350108, China
National Engineering Laboratory for Methanol to Olefins, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China
Anhui Chuangpu Instrument Technology Co., LTD., Hefei 230088, China
Keywords:
selectivity, visible light, covalent triazine-based frameworks, Cu single atoms, photocatalytic CO2 reduction
Topics:
Photocatalysis
Cite this article:
Huang G, Niu Q, He Y, et al. Spatial confinement of copper single atoms into covalent triazine-based frameworks for highly efficient and selective photocatalytic CO2 reduction. Nano Research, 2022, 15(9): 8001-8009. https://doi.org/10.1007/s12274-022-4629-3
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Abstract Full text Electronic supplementary material About this article

Converting CO2 into carbonaceous fuels via photocatalysis represents an appealing strategy to simultaneously alleviate the energy crisis and associated environmental problems, yet designing with high photoreduction activity catalysts remains a compelling challenge. Here, combining the merits of highly porous structure and maximum atomic efficiency, we rationally constructed covalent triazine-based frameworks (CTFs) anchoring copper single atoms (Cu-SA/CTF) photocatalysts for efficient CO2 conversion. The Cu single atoms were visualized by high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) images and coordination structure of Cu-N-C2 sites was revealed by extended X-ray absorption fine structure (EXAFS) analyses. The as-prepared Cu-SA/CTF photocatalysts exhibited superior photocatalytic CO2 conversion to CH4 performance associated with a high selectivity of 98.31%. Significantly, the introduction of Cu single atoms endowed the Cu-SA/CTF catalysts with increased CO2 adsorption capacity, strengthened visible light responsive ability, and improved the photogenerated carriers separation efficiency, thus enhancing the photocatalytic activity. This work provides useful guidelines for designing robust visible light responsive photoreduction CO2 catalysts on the atomic scale.


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About this article

Spatial confinement of copper single atoms into covalent triazine-based frameworks for highly efficient and selective photocatalytic CO2 reduction

Show Author's information Guocheng Huang1, Qing Niu1, Yuxin He1, Jinjin Tian1, Mingbin Gao4( ), Chaoyang Li5, Ning An5, Jinhong Bi1,3( ), Jiangwei Zhang2,4,5( )
Department of Environmental Science and Engineering, Fuzhou University, Fuzhou 350108, China
Advanced Chemical Engineering and Energy Materials Research Center, China University of Petroleum (East China), Qingdao 266580, China
State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University, Fuzhou 350108, China
National Engineering Laboratory for Methanol to Olefins, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China
Anhui Chuangpu Instrument Technology Co., LTD., Hefei 230088, China

Abstract

Converting CO2 into carbonaceous fuels via photocatalysis represents an appealing strategy to simultaneously alleviate the energy crisis and associated environmental problems, yet designing with high photoreduction activity catalysts remains a compelling challenge. Here, combining the merits of highly porous structure and maximum atomic efficiency, we rationally constructed covalent triazine-based frameworks (CTFs) anchoring copper single atoms (Cu-SA/CTF) photocatalysts for efficient CO2 conversion. The Cu single atoms were visualized by high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) images and coordination structure of Cu-N-C2 sites was revealed by extended X-ray absorption fine structure (EXAFS) analyses. The as-prepared Cu-SA/CTF photocatalysts exhibited superior photocatalytic CO2 conversion to CH4 performance associated with a high selectivity of 98.31%. Significantly, the introduction of Cu single atoms endowed the Cu-SA/CTF catalysts with increased CO2 adsorption capacity, strengthened visible light responsive ability, and improved the photogenerated carriers separation efficiency, thus enhancing the photocatalytic activity. This work provides useful guidelines for designing robust visible light responsive photoreduction CO2 catalysts on the atomic scale.

Keywords: selectivity, visible light, covalent triazine-based frameworks, Cu single atoms, photocatalytic CO2 reduction

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Publication history
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Acknowledgements

Publication history

Received: 02 May 2022
Revised: 03 June 2022
Accepted: 05 June 2022
Published: 23 June 2022
Issue date: September 2022

Copyright

© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

We gratefully acknowledge BL14W1 beamline of Shanghai Synchrotron Radiation Facility (SSRF) Shanghai, China for providing the beam time. This work was financially supported by the National Natural Science Foundation of China (Nos. 51672047, 21707173, and 21701168), Dalian high level talent innovation project (No. 2019RQ063), the National Natural Science Foundation of Fujian Province (Nos. 2019J01648 and 2019J01226), Open project Foundation of State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences (No. 20200021), and the Youth Talent Support Program of Fujian Province (No. 00387077).

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