2. Academic Validation
  3. Luciferase-free Luciferin Electrochemiluminescence

Luciferase-free Luciferin Electrochemiluminescence

  • Angew Chem Int Ed Engl. 2022 Nov 14;61(46):e202209670. doi: 10.1002/anie.202209670.
Mattia Belotti 1,  Mohsen M T El-Tahawy 2 3,  Li-Juan Yu 4,  Isabella C Russell 4,  Nadim Darwish 1,  Michelle L Coote 5,  Marco Garavelli 2,  Simone Ciampi 1
Affiliations

Affiliations

  • 1 School of Molecular and Life Sciences, Curtin University, Bentley, 6102, Western Australia, Australia.
  • 2 Dipartimento di Chimica Industriale "Toso Montanari", Università di Bologna, Bologna, 40136, Emilia Romagna, Italy.
  • 3 Chemistry Department, Faculty of Science, Damanhour University, Damanhour, 22511, Egypt.
  • 4 Research School of Chemistry, Australian National University, Canberra, 2601, Australian Capital Territory, Australia.
  • 5 Institute for Nanoscale Science and Technology, College of Science and Engineering, Flinders University, Bedford Park, 5042, South Australia, Australia.
PMID: 36169114 DOI: 10.1002/anie.202209670
Abstract

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.

Keywords

Electrochemiluminescence; Electrochemistry; Electrostatic Interactions; Profluorescence; Quantum Chemistry.

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