Identifying the active sites in unequal iron-nitrogen single-atom catalysts

Liang Huang, Qiong Liu, Weiwei Wu, Ge Gao, Xiliang Zheng, Jin Wang () and Shaojun Dong ()
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Liang Huang: Chinese Academy of Sciences
Qiong Liu: Chinese Academy of Sciences
Weiwei Wu: Chinese Academy of Sciences
Ge Gao: Chinese Academy of Sciences
Xiliang Zheng: Chinese Academy of Sciences
Jin Wang: University of Chinese Academy of Sciences
Shaojun Dong: Chinese Academy of Sciences

Nature Communications, 2023, vol. 14, issue 1, 1-8

Abstract: Abstract Single-atom catalysts (SACs) have become one of the most attractive frontier research fields in catalysis and energy conversion. However, due to the atomic heterogeneity of SACs and limitations of ensemble-averaged measurements, the essential active sites responsible for governing specific catalytic properties and mechanisms remain largely concealed. In this study, we develop a quantitative method of single-atom catalysis–fluorescence correlation spectroscopy (SAC-FCS), leveraging the atomic structure-dependent catalysis kinetics and single-turnover resolution of single-molecule fluorescence microscopy. This method enables us to investigate the oxidase-like single-molecule catalysis on unidentical iron-nitrogen (Fe-N) coordinated SACs, quantifying the active sites and their kinetic parameters. The findings reveal the significant differences of single sites from the average behaviors and corroborate the oxidase-like catalytic mechanism of the Fe-N active sites. We anticipate that the method will give essential insights into the rational design and application of SACs.

Date: 2023
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DOI: 10.1038/s41467-023-41311-9

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