Electron transfer and hydrogen generation from a molecular dyad: platinum(ii) alkynyl complex anchored to [FeFe] hydrogenase subsite mimic

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Abstract
A PS–Fe2S2 molecular dyad 1a directly anchoring a platinum(II) alkynyl complex to a Fe2S2 active site of a [FeFe] H2ase mimic, and an intermolecular system of its reference complexes 1b and 2, have been successfully constructed. Time-dependence of H2 evolution shows that PS–Fe2S21a as well as complex 2 with 1b can produce H2 in the presence of a proton source and sacrificial donor under visible light irradiation. Spectroscopic and electrochemical studies on the electron transfer event reveal that the reduced FeIFe0 species generated by the first electron transfer from the excited platinum(II) complex to the Fe2S2 active site in PS–Fe2S21a and complex 2 with 1b is essential for photochemical H2 evolution, while the second electron transfer from the excited platinum(II) complex to the protonated FeIFe0 species is thermodynamically unfeasible, which might be an obstacle for the relatively small amount of H2 obtained by PS–Fe2S2 molecular dyads reported so far.

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