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首页> 外文期刊>Chemistry: A European journal >Formation of the distinct redox-interrelated forms of nitric oxide from reaction of dinitrosyl iron complexes (DNICs) and substitution ligands
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Formation of the distinct redox-interrelated forms of nitric oxide from reaction of dinitrosyl iron complexes (DNICs) and substitution ligands

机译：由二亚硝酰基铁配合物（DNIC）与取代配体反应形成独特的氧化还原相关形式的一氧化氮

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摘要

Release of the distinct NO redox-interrelated forms (NO~+, NO, and HNO/NO~-), derived from reaction of the dinitrosyl iron complex (DNIC) [(NO)_2Fe(C_(12)HaN)_2]~- (1) (C_(12)H_8N = carbazolate) and the substitution Iigands (S_2CNMe_2)_2, [SC_6H _4-O-NHC(O)(C_5H_4N)]_2, ((PyPepS) _2), and P(C_6H_3,-3SiMe_3-2-SH) _3 ([P(SH)_3]), respectively, was demonstrated. In contrast to the reaction of (PyPepS)_2 and DNIC 1 in a 1:1 stoichiometry that induces the release of an NO radical and the formation of complex [PPN][Fe(PyPepS)_2] (4), the incoming substitution ligand (S _2CNMe_2)_2 triggered the transformation of DNIC 1 into complex [(NO)Fe(S_2CNMe_2J_2] (2) along with N-nitrosocarbazole (3). The subsequent nitrosation of N-acetylpenicillamine (NAP) by N-nitrosocarbazole (3) to produce S-nitroso-A-acetylpenicillamine (SNAP) may signify the possible formation pathway of S-nitrosothiols from DNICs by means of transnitrosation of N-nitrosamines. Protonation of DNIC 1 by [P(SH)_3] triggers the release of HNO and the generation of complex [PPN][Fe(NO)P(C_6H_3-3-SiMe_3-2-S)_3] (5). In a similar fashion, the nucleophilic attack of the chelating ligand P(C_6H_3,-3-SiMe_3,-2-SNa)_3 ([P(SNa)_3]) on DNIC 1 resulted in the direct release of [NO] ~- captured by [(~(15)NO)Fe(SPh)_3]~-, thus leading to [(~(15)NO)~- (~(14)NO)Fe(SPh) _2]~-. These results illustrate one aspect of how the incoming substitution ligands ((S_2CNMe_2)_2 vs. (PyPepS)_2 vs. [P(SH)_3]/[P(SNa)_3]) in cooperation with the carbazolate-coordinated ligands of DNIC 1 function to control the release of NO_+, NO, or [NO]~- from DNIC 1 upon reaction of complex 1 and the substitution ligands. Also, these results signify that DNICs may act as an intermediary of NO in the redox signaling processes by providing the distinct redox-interrelated forms of NO to interact with different NO-responsive targets in biological systems.
机译：释放源自二亚硝基铁络合物（DNIC）[（NO）_2Fe（C_（12）HaN）_2]〜的独特的NO氧化还原相关形式（NO〜+，NO和HNO / NO〜-） -（1）（C_（12）H_8N =咔唑酸酯）和取代配体（S_2CNMe_2）_2，[SC_6H _4-O-NHC（O）（C_5H_4N）] _ 2，（（（PyPepS）_2）和P（C_6H_3，分别说明了-3SiMe_3-2-SH）_3（[P（SH）_3]）。与（PyPepS）_2和DNIC 1的化学计量比为1：1的反应相反，该反应诱导NO自由基的释放和复合物[PPN] [Fe（PyPepS）_2]的形成（4），即将出现的取代配体（S _2CNMe_2）_2触发DNIC 1与N-亚硝基咔唑（3）一起转变为复合物[（NO）Fe（S_2CNMe_2J_2]（2）。随后N-亚硝基咔唑（3）将N-乙酰青霉胺（NAP）亚硝化产生S-亚硝基-A-乙酰青霉胺（SNAP）可能意味着通过D-亚硝胺的亚硝化作用，可能从DNIC中形成S-亚硝基硫醇的途径。[P（SH）_3]使DNIC 1的质子化触发HNO的释放并生成复杂的[PPN] [Fe（NO）P（C_6H_3-3-SiMe_3-2-S）_3]（5）。螯合配体P（C_6H_3，-3- DNIC 1上的SiMe_3，-2-SNa）_3（[P（SNa）_3]）导致[[]（15NO）Fe（SPh）_3]〜-捕获的[NO]〜-的直接释放，因此导致[（〜（15）NO）〜-（〜（14）NO）Fe（SPh）_2]〜-。传入取代配体（（S_2CNMe_2）_2对（PyPepS）_2对[P（SH）_3] / [P（SNa）_3]）与DNIC 1的氨基甲酸配位配体协同作用的一方面以控制配合物1与取代配体反应后从DNIC 1中释放NO _ +，NO或[NO]〜-。而且，这些结果表明，DNIC通过提供不同的氧化还原相关形式的NO与生物系统中不同的NO响应靶标相互作用，可以在氧化还原信号传导过程中充当NO的中介。

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