pH-Dependent isotope exchange and hydrogenation catalysed by water-soluble NiRu complexes as functional models for [NiFe]hydrogenases

Dalton Transactions : an International Journal of Inorganic Chemistry
Bunsho KureSeiji Ogo

Abstract

The pH-dependent hydrogen isotope exchange reaction between gaseous isotopes and medium isotopes and hydrogenation of the carbonyl compounds have been investigated with water-soluble bis(mu-thiolate)(mu-hydride)NiRu complexes, Ni(II)(mu-SR)(2)(mu-H)Ru(II) {(mu-SR)(2) = N,N'-dimethyl-N,N'-bis(2-mercaptoethyl)-1,3-propanediamine}, as functional models for [NiFe]hydrogenases. In acidic media (at pH 4-6), the mu-H ligand of the Ni(II)(mu-SR)(2)(mu-H)Ru(II) complexes has H(+) properties, and the complexes catalyse the hydrogen isotope exchange reaction between gaseous isotopes and medium isotopes. A mechanism of the hydrogen isotope exchange reaction between gaseous isotopes and medium isotopes through a low-valent Ni(I)(mu-SR)(2)Ru(I) complex is proposed. In contrast, in neutral-basic media (at pH 7-10), the mu-H ligand of the Ni(II)(mu-SR)(2)(mu-H)Ru(II) complexes acts as H(-), and the complexes catalyse the hydrogenation of carbonyl compounds.

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Citations

Jun 9, 2009·Chemical Communications : Chem Comm·Seiji Ogo
Jan 16, 2013·Proceedings of the Japan Academy. Series B, Physical and Biological Sciences·Tatsuhiko Yagi, Yoshiki Higuchi
Jun 30, 2016·Chemical Reviews·David SchilterThomas B Rauchfuss
Jul 21, 2016·Chemical Reviews·Nathan A Eberhardt, Hairong Guan
Sep 14, 2011·Angewandte Chemie·Takahiro MatsumotoSeiji Ogo
Aug 8, 2009·Dalton Transactions : an International Journal of Inorganic Chemistry·Koji IchikawaSeiji Ogo
Aug 6, 2009·Dalton Transactions : an International Journal of Inorganic Chemistry·Yuichiro HimedaKazuyuki Kasuga
Feb 18, 2010·Dalton Transactions : an International Journal of Inorganic Chemistry·Chunbai ZhengSeiji Ogo
Mar 12, 2010·Dalton Transactions : an International Journal of Inorganic Chemistry·Koji IchikawaSeiji Ogo
May 23, 2014·Dalton Transactions : an International Journal of Inorganic Chemistry·Sandeep Kaur-Ghumaan, Matthias Stein
Nov 13, 2010·Chemical Communications : Chem Comm·Tsuyoshi MatsumotoKazuyuki Tatsumi
Mar 12, 2010·Dalton Transactions : an International Journal of Inorganic Chemistry·Loredana VaccaroMartin J Field
Sep 18, 2009·Dalton Transactions : an International Journal of Inorganic Chemistry·Hideaki OgataYoshiki Higuchi

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