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Coupling H2 to Electron Transfer with a 17-Electron Heterobimetallic Hydride: A “Redox Switch” Model for the H2-Activating Center of Hydrogenase
A meta-stable heterobimetallic mixed-valence ion, , is formed by the one-electron oxidation of Cp*(dppf)RuH <1, dppf = 1,1'-bis(diphenylphosphino)ferrocene, Cp* = pentamethylcyclopentadienide>.A remarkable stability toward one-electron oxidation is revealed by the cyclic voltammetry of 1 which contains two reversible oxidations at +0.073 and +0.541 V and a quasireversible oxidation at +0.975 V (vs NHE assigned to Ru(III/II), Ru(IV/III), and Fe(III/II), respectively.The isolable Ru(III) metal hydride, PF6 (1+), is characterized by a NIR absorption at 912 nm (epsilon = 486 M-1A cm-1) assigned to an intervalence transfer band and a series of atom transfer reactions yielding the even electron derivatives PF6 (X = H, Cl, Br, I).A crystallographically determined Fe-Ru distance of 4.383(1) Angstroem in 1 is consonant with the classification of 1+ as a weakly coupled.Type II mixed-valence ion (Hab = 627 cm-1, alpha2 = 3.3×10-3).This is the first reported example of a mixed-valence bimetallic complex containing the widely used dppf ligand.The ability of 1 to serve as a heterobimetallic catalyst for the reduction of methyl viologen with H2 makes it a unique functional model of hydrogenase enzymes.
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Reference£º
Highly efficient and robust molecular ruthenium catalysts for water oxidation,
Catalysts | Special Issue : Ruthenium Catalysts – MDPI