Luciferase-free Luciferin Electrochemiluminescence.

Autor: Belotti M; School of Molecular and Life Sciences, Curtin University, Bentley, 6102, Western Australia, Australia., El-Tahawy MMT; Dipartimento di Chimica Industriale 'Toso Montanari', Università di Bologna, Bologna, 40136, Emilia Romagna, Italy.; Chemistry Department, Faculty of Science, Damanhour University, Damanhour, 22511, Egypt., Yu LJ; Research School of Chemistry, Australian National University, Canberra, 2601, Australian Capital Territory, Australia., Russell IC; Research School of Chemistry, Australian National University, Canberra, 2601, Australian Capital Territory, Australia., Darwish N; School of Molecular and Life Sciences, Curtin University, Bentley, 6102, Western Australia, Australia., Coote ML; Institute for Nanoscale Science and Technology, College of Science and Engineering, Flinders University, Bedford Park, 5042, South Australia, Australia., Garavelli M; Dipartimento di Chimica Industriale 'Toso Montanari', Università di Bologna, Bologna, 40136, Emilia Romagna, Italy., Ciampi S; School of Molecular and Life Sciences, Curtin University, Bentley, 6102, Western Australia, Australia.
Jazyk: angličtina
Zdroj: Angewandte Chemie (International ed. in English) [Angew Chem Int Ed Engl] 2022 Nov 14; Vol. 61 (46), pp. e202209670. Date of Electronic Publication: 2022 Oct 25.
DOI: 10.1002/anie.202209670
Abstrakt: Luciferin is one of Nature's most widespread luminophores, and enzymes that catalyze luciferin luminescence are the basis of successful commercial "glow" assays for gene expression and metabolic ATP formation. Herein we report an electrochemical method to promote firefly's luciferin luminescence in the absence of its natural biocatalyst-luciferase. We have gained experimental and computational insights on the mechanism of the enzyme-free luciferin electrochemiluminescence, demonstrated its spectral tuning from green to red by means of electrolyte engineering, proven that the colour change does not require, as still debated, a keto/enol isomerization of the light emitter, and gained evidence of the electrostatic-assisted stabilization of the charge-transfer excited state by double layer electric fields. Luciferin's electrochemiluminescence, as well as the in situ generation of fluorescent oxyluciferin, are applied towards an optical measurement of diffusion coefficients.
(© 2022 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.)
Databáze: MEDLINE
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