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

Yi-Man Wang, Fang-Qin Yan, Qian-You Wang, Chen-Xia Du, Li-Ya Wang, Bo Li, Shan Wang () and Shuang-Quan Zang ()
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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

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: 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.

Date: 2024
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DOI: 10.1038/s41467-024-46098-x

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