Computational investigations of the chemical mechanism of the enzyme nitrogenase.

Computational investigations of the chemical mechanism of the enzyme nitrogenase.
Chembiochem. 2019 Dec 05;:
Authors: Dance IG
Abstract
The chemical mechanism of nitrogenase, catalyzing N2 + 8e- + 8H+  ® 2NH3 + H2, occurs at a large multi-metal cluster (FeMo-co) with composition CFe7MoS9(homocitrate).  This requires more than 20 steps.  Experimental elucidation of this mechanism is thwarted, for various reasons, and computational approaches have a valuable role.   This review critically surveys recent density functional calculations of the coordination chemistry and relevant reactions of FeMo-co, within the protein surrounds.  Topics covered include the accuracies and validation of the density functionals used, the treatment of electronic structure, and the chemical models used.  The components of mechanism, including the input of N2, proton supply, the egress of NH3, and the roles of surrounding protein are described.  This leads to descriptions and evaluations of the overall mechanistic cycles proposed on the basis of density functional calculations.  Finally I discuss some current issues, and consider the outlook for further work.
PMID: 31803989 [PubMed - as supplied by publisher]

Source: Chembiochem - December 4, 2019 Category: Biochemistry Authors: Dance IG Tags: Chembiochem Source Type: research