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

被引：41

作者：

Kure, Bunsho ^{[1
]}

Matsumoto, Takahiro ^{[1
]}

Ichikawa, Koji ^{[1
]}

Fukuzumi, Shunichi ^{[2
]}

Higuchi, Yoshiki ^{[3
]}

Yagi, Tatsuhiko ^{[4
]}

Ogo, Seiji ^{[1
]}

机构：

[1] Kyushu Univ, Ctr Future Chem, Fukuoka 8190395, Japan

[2] Osaka Univ, Grad Sch Engn, Div Adv Sci & Biotechnol, Dept Mat & Life Sci,Japan Sci & Technol Agcy, Suita, Osaka 5650871, Japan

[3] Univ Hyogo, Grad Sch Life Sci, Dept Life Sci, Kamigori, Hyogo 6781297, Japan

[4] Shizuoka Univ, Shizuoka 4228529, Japan

来源：

DALTON TRANSACTIONS | 2008年 / 35卷 / 35期

关键词：

D O I：

10.1039/b807555g

中图分类号：

O61 [无机化学];

学科分类号：

070301 ; 081704 ;

摘要：

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.

引用

页码：4747 / 4755

页数：9

共 73 条

[1] Isolation and characterization of methanophenazine and function of phenazines in membrane-bound electron transport of Methanosarcina mazei Gol [J].