Single-atom tailored atomically-precise nanoclusters for enhanced electrochemical reduction of CO<sub>2</sub>-to-CO activity.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 38418496.
- Also identified by DOI 10.1038/s41467-024-46098-x and PMC identifier 10901820.
- Licence recorded as CC BY.
- The licence permits redistribution, so the abstract is shown in full and the full text is available from the publisher.
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 Au<sub>8</sub> 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 Au<sub>8</sub> clusters, which amplifies their electrocatalytic reduction of CO<sub>2</sub> to CO activity by ~18.07 fold compared to isolated Au<sub>8</sub> 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 CO<sub>2</sub> 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.