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

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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.

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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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Authors and Affiliations

  1. Department of Environmental Science and Engineering, Fuzhou University, Fuzhou, 350108, China

    Guocheng Huang, Qing Niu, Yuxin He, Jinjin Tian & Jinhong Bi

  2. Advanced Chemical Engineering and Energy Materials Research Center, China University of Petroleum (East China), Qingdao, 266580, China

    Jiangwei Zhang

  3. State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University, Fuzhou, 350108, China

    Jinhong Bi

  4. National Engineering Laboratory for Methanol to Olefins, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China

    Mingbin Gao & Jiangwei Zhang

  5. Anhui Chuangpu Instrument Technology Co., LTD., Hefei, 230088, China

    Chaoyang Li, Ning An & Jiangwei Zhang

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  1. Guocheng Huang
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Correspondence to Mingbin Gao, Jinhong Bi or Jiangwei Zhang.

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

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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 Res. 15, 8001–8009 (2022). https://doi.org/10.1007/s12274-022-4629-3

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