Photoinduced monooxygenation involving NAD(P)H-FAD sequential single-electron transfer

Simon Ernst, Stefano Rovida, Andrea Mattevi, Susanne Fetzner and Steffen L. Drees ()
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Simon Ernst: University of Münster
Stefano Rovida: University of Pavia
Andrea Mattevi: University of Pavia
Susanne Fetzner: University of Münster
Steffen L. Drees: University of Münster

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

Abstract: Abstract Light-dependent or light-stimulated catalysis provides a multitude of perspectives for implementation in technological or biomedical applications. Despite substantial progress made in the field of photobiocatalysis, the number of usable light-responsive enzymes is still very limited. Flavoproteins have exceptional potential for photocatalytic applications because the name-giving cofactor intrinsically features light-dependent reactivity, undergoing photoreduction with a variety of organic electron donors. However, in the vast majority of these enzymes, photoreactivity of the enzyme-bound flavin is limited or even suppressed. Here, we present a flavoprotein monooxygenase in which catalytic activity is controllable by blue light illumination. The reaction depends on the presence of nicotinamide nucleotide-type electron donors, which do not support the reaction in the absence of light. Employing various experimental approaches, we demonstrate that catalysis depends on a protein-mediated photoreduction of the flavin cofactor, which proceeds via a radical mechanism and a transient semiquinone intermediate.

Date: 2020
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Persistent link: https://EconPapers.repec.org/RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-16450-y

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DOI: 10.1038/s41467-020-16450-y

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