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Cascade Reaction Regulated Electrochemiluminescence via Dual-Atomic-Site Catalysts. | LitMetric

Cascade Reaction Regulated Electrochemiluminescence via Dual-Atomic-Site Catalysts.

Anal Chem

Institute of Nanochemistry and Nanobiology School of Environmental and Chemical Engineering, Shanghai University, Shanghai 200444, P. R. China.

Published: August 2023

Single-atom catalysts (SACs), a novel kind of electrocatalysts with full metal utilization, have been developed as unique signal amplifiers in several sensing platforms. Herein, based on theoretical prediction of the oxygen reduction reaction (ORR) mechanism on different atom sites, we constructed dual-atomic-site catalysts (DACs), Fe/Mn-N-C, to catalyze luminol-dissolved oxygen electrochemiluminescence (ECL). Computational simulation indicated that the weak adsorption of OH* on a single Fe site was overcome by introducing Mn as the secondary metallic active site, resulting in a synergic dual-site cascade mechanism. The superior catalytic activity of Fe/Mn-N-C DACs for the ORR was proven by the highly efficient cathodic luminol ECL, surpassing the performance of single-site catalysts (SACs), Fe-N-C and Mn-N-C. Furthermore, the ECL system, enhanced by a cascade reaction, exhibited remarkable sensitivity to ascorbic acid, with a detection limit of 0.02 nM. This research opens up opportunities for enhancing both the ECL efficiency and sensing performance by employing a rational atomic-scale design for DACs.

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Source
http://dx.doi.org/10.1021/acs.analchem.3c00891DOI Listing

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