Low potential enzymatic hydride transfer via highly cooperative and inversely functionalized flavin cofactors.

Abstract:

:Hydride transfers play a crucial role in a multitude of biological redox reactions and are mediated by flavin, deazaflavin or nicotinamide adenine dinucleotide cofactors at standard redox potentials ranging from 0 to -340 mV. 2-Naphthoyl-CoA reductase, a key enzyme of oxygen-independent bacterial naphthalene degradation, uses a low-potential one-electron donor for the two-electron dearomatization of its substrate below the redox limit of known biological hydride transfer processes at E°' = -493 mV. Here we demonstrate by X-ray structural analyses, QM/MM computational studies, and multiple spectroscopy/activity based titrations that highly cooperative electron transfer (n = 3) from a low-potential one-electron (FAD) to a two-electron (FMN) transferring flavin cofactor is the key to overcome the resonance stabilized aromatic system by hydride transfer in a highly hydrophobic pocket. The results evidence how the protein environment inversely functionalizes two flavins to switch from low-potential one-electron to hydride transfer at the thermodynamic limit of flavin redox chemistry.

journal_name

Nat Commun

journal_title

Nature communications

authors

Willistein M,Bechtel DF,Müller CS,Demmer U,Heimann L,Kayastha K,Schünemann V,Pierik AJ,Ullmann GM,Ermler U,Boll M

doi

10.1038/s41467-019-10078-3

subject

Has Abstract

pub_date

2019-05-06 00:00:00

pages

2074

issue

1

issn

2041-1723

pii

10.1038/s41467-019-10078-3

journal_volume

10

pub_type

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