Hydrogenase efficiently and rapidly produces and oxidizes hydrogen in biological systems.  We have demonstrated that the outer coordination sphere, in addition to the first and second coordination spheres, plays an important role in the rate of hydrogen production in [Ni(P2PhN2Ph)2](BF4)2 complexes.  Recently, we have reported that a nickel catalyst, [Ni(7PPh2NPh)2](BF4)2, (7PPh2NPh = 1,3,6-triphenyl-1-aza-3,6-diphosphacycloheptane) catalyzes the H2 production using [(DMF)H]+OTf- as the proton source, with turnover frequencies of 33,000 s-1 in dry acetonitrile and 106,000 s-1 in the presence of H2O  (1.2 M), with overpotential of 625 mV. Herein, we will report the synthesis, structural characterization, and catalytic activity of a series of peptide coupled Ni-based complexes for hydrogen production built on the framework of [Ni(7P2PhNPh-AA)2]2+.

Peptide coupled hydrogen production electrocatalysts

243rd National Meeting (2012)

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