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Photoinduced Biphasic Hydrogen Evolution: Decamethylosmocene as a Light-Driven Electron Donor
(WILEY-V C H VERLAG GMBH, 2013) Ge, Peiyu; Olaya, Astrid J.; Scanlon, Micheal D.; Patir, Imren Hatay; Vrubel, Heron; Girault, Hubert H.
Excitation of the weak electron donor decamethylosmocene on illumination with white light produces an excited-state species capable of reducing organically solubilized protons under biphasic conditions. Insight into the mechanism and kinetics of light-driven biphasic hydrogen evolution are obtained by analysis with gas chromatography, cyclic voltammetry, and UV/Vis and H-1 NMR spectroscopy. Formation of decamethylosmocenium hydride, which occurs prior to hydrogen evolution, is a rapid step relative to hydrogen release and takes place independently of light activation. Remarkably, hydride formation occurs with greater efficiency (ca. 90% conversion) under biphasic conditions than when the reaction is carried out in an acidified single organic phase (ca. 20% conversion). Cyclic voltammetry studies reveal that decamethylosmocene has a higher proton affinity than either decamethylferrocene or osmocene.