A Model of the [FeFe] Hydrogenase Active Site with a Biologically Relevant Azadithiolate Bridge: A Spectroscopic and Theoretical Investigation

Abstract

Convincing evidence for the presence of a nitrogen atom in the dithiolate bridge of the active site of native [FeFe] hydrogenases (B) is provided by a spectroscopic, electrochemical, and theoretical study of a well-characterized structural mimic of the [FeFe] hydrogenase subcluster (picture: 14N matched-HYSCORE spectrum of the model compound A). This result should help to understand the mechanism of dihydrogen conversion and production.