Nitrogen Reduction to Ammonia on a Biomimetic Mononuclear Iron Centre: Insights into the Nitrogenase Enzyme.

ABSTRACT: Nitrogenases catalyse nitrogen fixation to ammonia on a multinuclear Fe-Mo centre, but their mechanism and particularly the order of proton and electron transfer processes that happen during the catalytic cycle is still unresolved. Recently, a unique biomimetic mononuclear iron model was developed using tris(phosphine)borate (TPB) ligands that was shown to convert N₂ into NH₃ . Herein, we present a computational study on the [(TPB)FeN₂ ]^- complex and describe its conversion into ammonia through the addition of electrons and protons. In particular, we tested the consecutive proton transfer on only the distal nitrogen atom or alternated protonation of the distal/proximal nitrogen. It is found that the lowest energy pathway is consecutive addition o

SUBMITTER: Kaczmarek MA 

PROVIDER: S-EPMC5915742 | biostudies-literature | 2018 Apr

REPOSITORIES: biostudies-literature