Binuclear iron-sulfur complexes with bidentate phosphine ligands as active site models of Fe-hydrogenase and their catalytic proton reduction
文献类型：期刊论文
| 作者 | W. M. Gao ; J. Ekstrom ; J. H. Liu ; C. N. Chen ; L. Eriksson ; L. H. Weng ; B. Akermark ; L. H. Sun |
| 刊名 | Inorganic Chemistry
 |
| 出版日期 | 2007-03 |
| 卷号 | 46期号:6页码:1981-1991 |
| 关键词 | only hydrogenases electrochemical properties ruthenium photosensitizer electron-transfer chemistry dinuclear exchange |
| ISSN号 | 0020-1669 |
| 中文摘要 | The displacement of CO in a few simple Fe(I)-Fe(I) hydrogenase model complexes by bisphosphine ligands Ph(2)P-(CH(2))(n)-PPh(2) [with n = 1 (dppm) or n = 2 (dppe)] is described. The reaction of [{mu-(SCH(2))(2)CH(2)}Fe(2)(CO)(6)] (1) and [{mu-(SCH(2))(2)N(CH(2)CH(2)CH(3))}Fe(2)(CO)(6)] (2) with dppe gave double butterfly complexes [{mu-(SCH(2))(2)CH(2)}Fe(2)(CO)(5)(Ph(2)PCH(2))](2) (3) and [{mu-(SCH(2))(2)N(CH(2)CH(2)CH(3))}Fe(2)(CO)(5)(Ph(2)PCH(2))](2) (4), where two Fe(2)S(2) units are linked by the bisphosphine. In addition, an unexpected byproduct, [{mu-(SCH(2))(2)N(CH(2)CH(2)CH(3))}Fe(2)(CO)(5){Ph(2)PCH(2)CH(2)(Ph(2)PS)}] (5), was isolated when 2 was used as a substrate, where only one phosphorus atom of dppe is coordinated, while the other has been converted to PS, presumably by nucleophilic attack on bridging sulfur. By contrast, the reaction of 1 and 2 with dppm under mild conditions gave only complexes [{mu-(SCH(2))(2)CH(2)}Fe(2)(CO)(5)(Ph(2)PCH(2)PPh(2))] (6) and [{mu-(SCH(2))(2)N(CH(2)CH(2)CH(3))}Fe(2)(CO)(5)(Ph(2)PCH(2)PPh(2))] (8), where one ligand coordinated in a monodentate fashion to one Fe(2)S(2) unit. Furthermore, under forcing conditions, the complexes [{mu-(SCH(2))(2)CH(2)}Fe(2)(CO)(4){mu-(Ph(2)P)(2)CH(2)}] (7) and [{mu-(SCH(2))(2)N(CH(2)CH(2)CH(3))}Fe(2)(CO)(4){mu-(Ph(2)P)(2)CH(2)}] (9) were formed, where the phosphine acts as a bidentate ligand, binding to both the iron atoms in the same molecular unit. Electrochemical studies show that the complexes 3, 4, and 9 catalyze the reduction of protons to molecular hydrogen, with 4 electrolyzed already at -1.40 V versus Ag/AgNO(3) (-1.0 V vs NHE). |
| 语种 | 英语 |
| 公开日期 | 2013-04-01 |
| 源URL | [http://ir.fjirsm.ac.cn/handle/350002/6262]  |
| 专题 | 福建物质结构研究所_中科院福建物质结构研究所_期刊论文 |
| 推荐引用方式 GB/T 7714 | W. M. Gao,J. Ekstrom,J. H. Liu,et al. Binuclear iron-sulfur complexes with bidentate phosphine ligands as active site models of Fe-hydrogenase and their catalytic proton reduction[J]. Inorganic Chemistry,2007,46(6):1981-1991. |
| APA | W. M. Gao.,J. Ekstrom.,J. H. Liu.,C. N. Chen.,L. Eriksson.,...&L. H. Sun.(2007).Binuclear iron-sulfur complexes with bidentate phosphine ligands as active site models of Fe-hydrogenase and their catalytic proton reduction.Inorganic Chemistry,46(6),1981-1991. |
| MLA | W. M. Gao,et al."Binuclear iron-sulfur complexes with bidentate phosphine ligands as active site models of Fe-hydrogenase and their catalytic proton reduction".Inorganic Chemistry 46.6(2007):1981-1991. |
入库方式： OAI收割
来源：福建物质结构研究所
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