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Single-atom tailored atomically-precise nanoclusters for enhanced electrochemical reduction of CO2-to-CO activity

Author

Listed:
  • Yi-Man Wang

    (Zhengzhou University)

  • Fang-Qin Yan

    (Zhengzhou University)

  • Qian-You Wang

    (Zhengzhou University)

  • Chen-Xia Du

    (Zhengzhou University)

  • Li-Ya Wang

    (Nanyang Normal University)

  • Bo Li

    (Nanyang Normal University)

  • Shan Wang

    (Zhengzhou University)

  • Shuang-Quan Zang

    (Zhengzhou University)

Abstract

The development of facile tailoring approach to adjust the intrinsic activity and stability of atomically-precise metal nanoclusters catalysts is of great interest but remians challenging. Herein, the well-defined Au8 nanoclusters modified by single-atom sites are rationally synthesized via a co-eletropolymerization strategy, in which uniformly dispersed metal nanocluster and single-atom co-entrenched on the poly-carbazole matrix. Systematic characterization and theoretical modeling reveal that functionalizing single-atoms enable altering the electronic structures of Au8 clusters, which amplifies their electrocatalytic reduction of CO2 to CO activity by ~18.07 fold compared to isolated Au8 metal clusters. The rearrangements of the electronic structure not only strengthen the adsorption of the key intermediates *COOH, but also establish a favorable reaction pathway for the CO2 reduction reaction. Moreover, this strategy fixing nanoclusters and single-atoms on cross-linked polymer networks efficiently deduce the performance deactivation caused by agglomeration during the catalytic process. This work contribute to explore the intrinsic activity and stability improvement of metal clusters.

Suggested Citation

  • Yi-Man Wang & Fang-Qin Yan & Qian-You Wang & Chen-Xia Du & Li-Ya Wang & Bo Li & Shan Wang & Shuang-Quan Zang, 2024. "Single-atom tailored atomically-precise nanoclusters for enhanced electrochemical reduction of CO2-to-CO activity," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-46098-x
    DOI: 10.1038/s41467-024-46098-x
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    References listed on IDEAS

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    1. Zongyao Zhou & Xiang Li & Dong Guo & Digambar B. Shinde & Dongwei Lu & Long Chen & Xiaowei Liu & Li Cao & Ammar M. Aboalsaud & Yunxia Hu & Zhiping Lai, 2020. "Electropolymerization of robust conjugated microporous polymer membranes for rapid solvent transport and narrow molecular sieving," Nature Communications, Nature, vol. 11(1), pages 1-9, December.
    2. Meng Zhou & Chenjie Zeng & Yuxiang Chen & Shuo Zhao & Matthew Y. Sfeir & Manzhou Zhu & Rongchao Jin, 2016. "Evolution from the plasmon to exciton state in ligand-protected atomically precise gold nanoparticles," Nature Communications, Nature, vol. 7(1), pages 1-7, December.
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