Transformation of Dinitrosyl Iron Complexes [(NO)[sub2]Fe(SR)[sub2]] (R = Et, Ph) into [4Fe-4S] Clusters [Fe[sub4]S[sub4](SPh)[sub4]][sup2-]: Relevance to the Repair of the Nitric Oxide-Modified Ferredoxin [4Fe-4S] Clusters.
Transformation of dinitrosyl iron complexes (DNICs) [(NO)[sub2]Fe(SR)[sub2]] (R = Et, Ph) into [4Fe-4S] clusters [Fe[sub4]S[sub4](SPh)[sub4]][sup2-] in the presence of [Fe(SPh)[sub4]][sup2-/1-] and S-donor species S[sub8] via the reassembling process ([(NO)[sub2]Fe(SR)[sub2]][sup-] → [Fe[sub4]S[sub3...
| Publicado en: | Journal of the American Chemical Society Vol. 130; no. 50; pp. 17154 - 17161 |
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| Autores principales: | , , , |
| Formato: | Artículo |
| Publicado: |
American Chemical Society
12/17/2008
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| Materias: | |
| Acceso en línea: | Ver este registro en EBSCOhost |
| fields | @attributes: recordID: 1 pdfLink: plink: https://search.ebscohost.com/login.aspx?direct=true&db=hlh&AN=35847000&site=ehost-live header: @attributes: shortDbName: hlh uiTerm: 35847000 longDbName: Humanities International Complete uiTag: AN controlInfo: bkinfo: jinfo: jid: 00027863 ACS jtl: Journal of the American Chemical Society issn: 00027863 maglogo: N pubinfo: dt: 12/17/2008 vid: 130 iid: 50 pid: 997 pub: American Chemical Society artinfo: ui: 35847000 10.1021/ja806050x ppf: 17154 ppct: 7 formats: tig: atl: Transformation of Dinitrosyl Iron Complexes [(NO)[sub2]Fe(SR)[sub2]] (R = Et, Ph) into [4Fe-4S] Clusters [Fe[sub4]S[sub4](SPh)[sub4]][sup2-]: Relevance to the Repair of the Nitric Oxide-Modified Ferredoxin [4Fe-4S] Clusters. aug: au: Chih-Chin Tsou Zong-Sian Lin Tsai-Te Lu Wen-Feng Liaw affil: Department of Chemistry, National Tsing Hua University, Hsinchu 30013, Taiwan, Republic of China su: Nitric oxide Iron ions Ferredoxin-NADP reductase Cysteine proteinases Optical diffraction Biomimetic chemicals sug: subj: Nitric oxide Iron ions Ferredoxin-NADP reductase Cysteine proteinases Optical diffraction Biomimetic chemicals ab: Transformation of dinitrosyl iron complexes (DNICs) [(NO)[sub2]Fe(SR)[sub2]] (R = Et, Ph) into [4Fe-4S] clusters [Fe[sub4]S[sub4](SPh)[sub4]][sup2-] in the presence of [Fe(SPh)[sub4]][sup2-/1-] and S-donor species S[sub8] via the reassembling process ([(NO)[sub2]Fe(SR)[sub2]][sup-] → [Fe[sub4]S[sub3](NO)[sub7]][sup-] (1)/[Fe[sub4]S[sub3](NO)[sub7]][sup2-] (2) → [Fe[sub4]S[sub4](NO)[sub4]][sup2-] (3) → [Fe[sub4]S[sub4](SPh)[sub4]][sup2-] (5)) was demonstrated. Reaction of [(NO)[sub2]Fe(SR)[sub2]] (R = Et, Ph) with S[sub8] in THF, followed by the addition of HBF[sub4] into the mixture solution, yielded complex [Fe[sub4]S[sub3](NO)[sub7]] (1). Complex [Fe[sub4]S[sub3](NO)[sub7]][sup2-] (2), obtained from reduction of complex 1 by [Na][biphenyl], was converted into complex [Fe[sub4]S[sub4](NO)[sub4]][sup2-] (3) along with byproduct [(NO)[sub2]Fe(SR)[sub2]][sup-] via the proposed [Fe[sub4]S[sub3](SPh)(NO)[sub4]][sup2-] intermediate upon treating complex 2 with 1.5 equiv of [Fe(SPh)[sub4]][sup2-] and the subsequent addition of 1/8 equiv of S[sub8] in CH[sub3]CN at ambient temperature. Complex 3 was characterized by IR, UV-vis, and single-crystal X-ray diffraction. Upon addition of complex 3 to the CH[sub3]CN solution of [Fe(SPh)[sub4]][sup-] in a 1:2 molar ratio at ambient temperature, the rapid NO radical-thiyl radical exchange reaction between complex 3 and the biomimetic oxidized form of rubredoxin [Fe(SPh)[sub4]][sup-] occurred, leading to the simultaneous formation of [4Fe-4S] cluster [Fe[sub4]S[sub4](SPh)[sub4]][sup2-] (5) and DNIC [(NO)[sub2]Fe(SPh)[sub2]][sup-]. This result demonstrates a successful biomimetic reassembly of [4Fe-4S] cluster [Fe[sub4]S[sub4](SPh)[sub4]][sup2-] from NO-modified [Fe-S] clusters, relevant to the repair of DNICs derived from nitrosylation of [4Fe-4S] clusters of endonuclease Ill back to [4Fe-45] clusters upon addition of ferrous ion, cysteine, and lscS. pubtype: Academic Journal doctype: Article src: R language: English refInfo: copyright: @attributes: flag: Y dt: @attributes: year: 2008 holdings: @attributes: islocal: N |
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