Toward Hydrogenase mimicry : subjecting the problem to three different approaches

Abstract

In this work, the challenging task of modelling Hydrogenase is subjected to three different approaches. The first strategy used here is bioorganometallic. A wide range of sulfur containing ferrocene-peptide derivatives were synthesized and fully characterized. As a second approach, organic self-assembled oligoquinoline were designed and synthesized. These two kind of structures were further used a scaffold for Hydrogenase mimics. In the third approach, a theoretical computational study of the ferrocene-peptide derivatives is led. In order to investigate a wider range of ferrocene-peptide as a molecular scaffold, a molecular force field was successfully implemented and validated for CHARMM. After the deprotection of the thiol group in the bioorganometallic approach, the free SH groups were coordinated with iron-carbonyl, so as to mimic the Fe-only Hydrogenase active site. The complexes thus obtained were comprehensively characterized and their electronic and electrochemical properties were extensively studied.