Exceptional Dendrimer-Based Mimics of Diiron Hydrogenase for the Photochemical Production of Hydrogen

A three‐component homogeneous catalyst system has been prepared with an IrIII complex as the photosensitizer, artificial hydrogenases bearing a diiron core and dendritic frameworks as the proton reduction catalyst, and triethylamine as the sacrificial electron donor. An initial turnover frequency of over 7240 h−1 and a quantum yield of up to 28 % were determined for the photocatalytic evolution of hydrogen.