Insights into the mechanism of coreactant electrochemiluminescence facilitating enhanced bioanalytical performance

Alessandra Zanut, Andrea Fiorani, Sofia Canola, Toshiro Saito, Nicole Ziebart, Stefania Rapino, Sara Rebeccani, Antonio Barbon, Takashi Irie, Hans-Peter Josel, Fabrizia Negri, Massimo Marcaccio, Michaela Windfuhr, Kyoko Imai, Giovanni Valenti () and Francesco Paolucci ()
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Alessandra Zanut: University of Bologna
Andrea Fiorani: University of Bologna
Sofia Canola: University of Bologna
Toshiro Saito: Hitachi High-Tech Corporation
Nicole Ziebart: Roche Diagnostics GmbH
Stefania Rapino: University of Bologna
Sara Rebeccani: University of Bologna
Antonio Barbon: University of Padova
Takashi Irie: Hitachi High-Tech Corporation
Hans-Peter Josel: Roche Diagnostics GmbH
Fabrizia Negri: University of Bologna
Massimo Marcaccio: University of Bologna
Michaela Windfuhr: Roche Diagnostics GmbH
Kyoko Imai: Hitachi High-Tech Corporation
Giovanni Valenti: University of Bologna
Francesco Paolucci: University of Bologna

Nature Communications, 2020, vol. 11, issue 1, 1-9

Abstract: Abstract Electrochemiluminescence (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.

Date: 2020
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DOI: 10.1038/s41467-020-16476-2

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