Iron Single-Atom Catalyst-Enabled Peroxydisulfate Activation Enhances Cathodic Electrochemiluminescence of Tris(bipyridine)ruthenium(II)

Zhen Luo; Weiqing Xu; Zhichao Wu; Lei Jiao; Xin Luo; Mengzhen Xi; Rina Su; Liuyong Hu; Wenling Gu; Chengzhou Zhu

doi:10.1021/acs.analchem.3c01822

Iron Single-Atom Catalyst-Enabled Peroxydisulfate Activation Enhances Cathodic Electrochemiluminescence of Tris(bipyridine)ruthenium(II)

Anal Chem. 2023 Jul 18;95(28):10762-10768. doi: 10.1021/acs.analchem.3c01822. Epub 2023 Jul 8.

Authors

Zhen Luo¹, Weiqing Xu¹, Zhichao Wu¹, Lei Jiao¹, Xin Luo¹, Mengzhen Xi¹, Rina Su¹, Liuyong Hu², Wenling Gu¹, Chengzhou Zhu¹

Affiliations

¹ National Key Laboratory of Green Pesticide, International Joint Research Center for Intelligent Biosensing Technology and Health, College of Chemistry, Central China Normal University, Wuhan 430079, P. R. China.
² Hubei Key Laboratory of Plasma Chemistry and Advanced Materials, Hubei Engineering Technology Research Center of Optoelectronic and New Energy Materials, Wuhan Institute of Technology, Wuhan 430205, P. R. China.

PMID: 37421333
DOI: 10.1021/acs.analchem.3c01822

Abstract

The tris(bipyridine)ruthenium(II) (Ru(bpy)₃²⁺)-tripropylamine anodic electrochemiluminescence (ECL) system has been widely applied in commercial bioanalysis. However, the presence of amine compounds in the biological environment results in unavoidable anodic interference signals, which hinder further extensive use of the system. In contrast, the cathodic Ru(bpy)₃²⁺ ECL system can overcome these limitations. The Ru(bpy)₃²⁺/peroxydisulfate (S₂O₈^2-, PDS) ECL system has been extensively employed due to its ability to produce a sulfate radical anion (SO₄^•-) with strong oxidation ability, which enhances the ECL signal. However, the symmetrical molecular structure of PDS makes it challenging to be activated and causes low luminescence efficiency. To address this issue, we propose an efficient Ru(bpy)₃²⁺-based ternary ECL system that uses the iron-nitrogen-carbon single-atom catalyst (Fe-N-C SAC) as an advanced accelerator. Fe-N-C SAC can efficiently activate PDS into reactive oxygen species at a lower voltage, which significantly boosts the cathodic ECL emission of Ru(bpy)₃²⁺. Benefiting from the outstanding catalytic activity of Fe-N-C SAC, we successfully established an ECL biosensor that detects alkaline phosphatase activity with high sensitivity, demonstrating the feasibility of practical application.