Abstract
AbstractSingle-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.
Publisher
Springer Science and Business Media LLC
Subject
General Physics and Astronomy,General Biochemistry, Genetics and Molecular Biology,General Chemistry,Multidisciplinary