A Functional Model of [Fe]-Hydrogenase

[Fe]-Hydrogenase
catalyzes the hydrogenation of a biological substrate
via the heterolytic splitting of molecular hydrogen. While many synthetic
models of [Fe]-hydrogenase have been prepared, none yet are capable
of activating H2 on their own. Here, we report the first
Fe-based functional mimic of the active site of [Fe]-hydrogenase,
which was developed based on a mechanistic understanding. The activity
of this iron model complex is enabled by its unique ligand environment,
consisting of biomimetic pyridinylacyl and carbonyl ligands, as well
as a bioinspired diphosphine ligand with a pendant amine moiety. The
model complex activates H2 and mediates hydrogenation of
an aldehyde.