Insights into the mechanism of coreactant electrochemiluminescence facilitating enhanced bioanalytical performance

Author:

Zanut Alessandra,Fiorani AndreaORCID,Canola SofiaORCID,Saito Toshiro,Ziebart Nicole,Rapino StefaniaORCID,Rebeccani SaraORCID,Barbon AntonioORCID,Irie Takashi,Josel Hans-Peter,Negri FabriziaORCID,Marcaccio MassimoORCID,Windfuhr Michaela,Imai Kyoko,Valenti GiovanniORCID,Paolucci FrancescoORCID

Abstract

AbstractElectrochemiluminescence (ECL) is a powerful transduction technique with a leading role in the biosensing field due to its high sensitivity and low background signal. Although the intrinsic analytical strength of ECL depends critically on the overall efficiency of the mechanisms of its generation, studies aimed at enhancing the ECL signal have mostly focused on the investigation of materials, either luminophores or coreactants, while fundamental mechanistic studies are relatively scarce. Here, we discover an unexpected but highly efficient mechanistic path for ECL generation close to the electrode surface (signal enhancement, 128%) using an innovative combination of ECL imaging techniques and electrochemical mapping of radical generation. Our findings, which are also supported by quantum chemical calculations and spin trapping methods, led to the identification of a family of alternative branched amine coreactants, which raises the analytical strength of ECL well beyond that of present state-of-the-art immunoassays, thus creating potential ECL applications in ultrasensitive bioanalysis.

Funder

Ministero dell'Istruzione, dell'Università e della Ricerca

Publisher

Springer Science and Business Media LLC

Subject

General Physics and Astronomy,General Biochemistry, Genetics and Molecular Biology,General Chemistry

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