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taozhikai½ð³æ (ÖøÃûдÊÖ)
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| Reduction of acids to molecular hydrogen as a means of storing energy is catalyzed byplatinum, but its low abundance and high cost are problematic. Precisely controlled deliveryof protons is critical in hydrogenase enzymes in nature that catalyze hydrogen (H2) productionusing earth-abundant metals (iron and nickel). Here, we report that a synthetic nickel complex,[Ni(PPh2NPh)2](BF4)2, (PPh2NPh = 1,3,6-triphenyl-1-aza-3,6-diphosphacycloheptane), catalyzesthe production of H2 using protonated dimethylformamide as the proton source, with turnoverfrequencies of 33,000 per second (s−1) in dry acetonitrile and 106,000 s−1 in the presence of1.2 M of water, at a potential of ¨C1.13 volt (versus the ferrocenium/ferrocene couple). Themechanistic implications of these remarkably fast catalysts point to a key role of pendantamines that function as proton relays.[ Last edited by taozhikai on 2011-8-12 at 21:54 ] |
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