期刊文献+

Ni(Ⅱ)-硫醇盐配合物中Ni—S键的反应多样性及模拟含镍生物酶活性部位金属有机化合物的合成

Reaction diversity of Ni—S bonds in nickel(Ⅱ)-thiolate complexes and synthesis of organometallic compounds to mimick the active site of nickel containing enzymes
下载PDF
导出
摘要 报道了利用镍(Ⅱ)-硫醇阴离子配合物[Ni—(S)4]和Fe3(CO)12反应制备有机硫配体桥联的多核Ni—Fe2配合物[Ni{(C6H4S2)2(CH2)3}(μ-S,S')Fe2(CO)6]和[Ni{(CH3C6H3S2)2(C3OH)}(μ-S,S')Fe2(CO)6]。其中后者中引入了羟基功能化基团,以便将其负载到改性的电极材料上研究其还原产物的电催化性能。通过核磁共振、红外、质谱和晶体结构测定等手段对相关化合物进行了表征。 The syntheses of thiolate bridged multinuclear [ Ni'Fe21 complexes, [ Ni{ ( C6H4S2 )2 ( CH2 )3 } ( μ-S, S') Fe2(CO)6] and [Ni{(CH3C6H3S2)2(C3OH)} (μ-S,S') Fe2 (CO) 6 ] were reported from the reaction of Ni ( Ⅱ ) -thio- late complexes with Fe3 (CO)12. Functional OH group was in- troduced into [ Ni{ (CH3C6H3S2)5 (C3OH) I ( μ-S, S') Fe2 (CO) 6 ] so that it can be grafted onto modified electrodes to investigate the electro-catalytic property of reduced species of [Ni/(CH3C6H3S2)2(C3OH)} (μ-S,S')Fe2(CO)6].The new compounds were confirmed by NMR, IR, MS and X-ray crystallography.
出处 《化学试剂》 CAS CSCD 北大核心 2013年第5期399-404,共6页 Chemical Reagents
基金 教育部留学回国人员科研启动基金资助项目 湖北省自然科学基金资助项目(2008CDB038) 湖北省教育厅科学技术研究计划项目(D20091703)
关键词 氢化酶 镍(Ⅱ)-硫醇配合物 活性中心 金属有机化合物 hydrogenase nickel ( Ⅱ ) -thiolate complex activesite organometallic compound
  • 相关文献

参考文献14

  • 1YEUNG L L,YIP Y C,LUH T Y. Transition metal promo- ted reactions. 28. tungsten hexacarbonyl mediated desul- furdimerization of dithioacetals, evidence for a thione in- termediate[ J]. Y. Org. Chem. , 1990, 55 ( 6 ) : 1 874- 1 881.
  • 2LINDAHL P A. Metal-metal bonds in biology [ J ]. J. In- org. Biochem. ,2012,106( 1 ) : 172-178.
  • 3FONTECILLA-CAMPS J C,VOLBEDA A,GAVAZZA C, et al. Structure/function relationships of [ NiFe ] and [ FeFe ] -hydrogenases [ J ]. Chem. Rev. , 2007,107 ( 10 ) : 4 273-4 303.
  • 4WANG Qiang,MARR A C,BLAKE A J,et al. Formation of nickel-thiolate aggregates via reaction with CH2CI2 [ J ]. Chem. Commun. ,2003, (22) :2 776-2 777.
  • 5WANG Qiang, BARCLAY J E, BLAKE A J, et al. The synthesis and electronic structure of a novel [ NiS4Fe2- (CO) 6 ] radical cluster:implications for the active site of the [ NiFe ] hydrogenases [ J ]. Chem. Eur. J. , 2004,10 (14) :3 384-3 396.
  • 6PERRA A, DAVIES E S, HYDE J R, et al. Electrocataly- tic production of hydrogen by a synthetic model of [ NiFe ] hydrogenases [J]. Chem. Commun. ,2006, ( 10 ) : 1 103-1 105.
  • 7SELLMANN D, FUNFGELDER S, POHLMANN G, et al. Transition-metal complexes with sulfur ligands. Nickel complexes with thiolato-thioether ligands including nitro- gen and oxygen donors in S6, S5 , OS4, NS4, and S4 donor sets. syntheses, properties, and X-ray structure determina- tions of [Ni(‘ S6 ’) ], [ Ni(‘ S5 ’) ], [ Ni(‘ 0S4 ’ ] 2, [Ni(‘S4-C5')]2, and [Ni(‘ S4-C3 ')] [J]. lnorg. Chem. ,1990,29(23) :4 772-4 778.
  • 8SELLMANN D, BAIL P, KNOCH F, et al. Transition me- tal complexes with sulfur ligands CXI. skeletal rearrange- ment of 2,3-dibromo-l-propanol in the template alkyla- tion of [Ni( ‘S2C6H4’ )]2- (‘ S2C6H4 ’^n- = 1,2- benzeneditiotale( 2 - ) ). syntheses of [ M ( t S4 -C3 OH ') ] complexes ( M = Ni Ⅱ , Pt Ⅱ ;‘ S4-C3 OH ^n - = 1,3-bis ( 2- mecaptophenylthio) -2-propanol (2-) ) [ J ]. Inorg. Chim. Acta, 1995,237 (1/2) : 137-141.
  • 9NAMETKIN N S,TYURIN V D,KUKINA M A. Synthesis and some properties of sulfur-containing iron tricarbonyl complexes[ J] . J. Organomet. Chem. , 1978,149(3) :355- 370.
  • 10ZHU Wen-feng, MARR A C, WANG Qiang, et al. Modu- lation of the electronic structure and the Ni-Fe dis- tance in eterobimetallie models for the active site in [ NiFe ] hydrogenase [ J ]. Pro. Natl. Acad. Sci. USA, 2005,102(51) :18 280-18 285.

相关作者

内容加载中请稍等...

相关机构

内容加载中请稍等...

相关主题

内容加载中请稍等...

浏览历史

内容加载中请稍等...
;
使用帮助 返回顶部