Electrons from hydrogen.
The growing need for hydrogen-based fuel cells has driven research into hydrogenase (H(2)ase)-a natural enzyme that catalyses the extraction of electrons from H(2) in water under ambient conditions. Unfortunately, the exact mechanism by which H(2)ase achieves this feat has remained a matter of some controversy until now, with many mechanisms being inconsistent with experimental data. Recently, however, we have been able to produce a successful catalytic mimic of H(2)ase that replicates key aspects of it. This paper begins with an overview of the research from many groups that preceded this discovery, followed by a detailed analysis of the key points that set our unique functional model apart-that is to say a proton-like "hydride" species, a surprisingly low-valent Ni(I)Ru(I) complex and the key insight that two molecules of H(2) are required for electron extraction.
Ogo
Seiji
S
Center for Future Chemistry, Kyushu University, 744, Moto-oka, Nishi-ku, Fukuoka, 819-0395, Japan. ogo-tcm@mbox.nc.kyushu-u.ac.jp
D055162:Biocatalysis; D020134:Catalytic Domain; D004583:Electrons; D006859:Hydrogen / Q000737:chemistry* / Q000378:metabolism; D006863:Hydrogen-Ion Concentration; D006864:Hydrogenase / Q000737:chemistry / Q000378:metabolism; D007501:Iron / Q000737:chemistry; D007506:Iron-Sulfur Proteins / Q000737:chemistry / Q000378:metabolism; D007554:Isotopes / Q000737:chemistry; D008958:Models, Molecular; D012428:Ruthenium / Q000737:chemistry; D013438:Sulfhydryl Compounds / Q000737:chemistry; D014867:Water / Q000737:chemistry
D007506:Iron-Sulfur Proteins; D007554:Isotopes; D013438:Sulfhydryl Compounds; D014867:Water; D012428:Ruthenium; D006859:Hydrogen; D007501:Iron; C118830:iron hydrogenase; C043296:nickel-iron hydrogenase; D006864:Hydrogenase