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 Communjournal_title
Nature communicationsauthors
Willistein M,Bechtel DF,Müller CS,Demmer U,Heimann L,Kayastha K,Schünemann V,Pierik AJ,Ullmann GM,Ermler U,Boll Mdoi
10.1038/s41467-019-10078-3subject
Has Abstractpub_date
2019-05-06 00:00:00pages
2074issue
1issn
2041-1723pii
10.1038/s41467-019-10078-3journal_volume
10pub_type
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