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方便合成氰尿酸衍生的 NHC 配体、它们的 Ag(I)和 Au(I)配合物及其抗菌活性。

Convenient syntheses of cyanuric chloride-derived NHC ligands, their Ag(I) and Au(I) complexes and antimicrobial activity.

机构信息

School of Chemistry, Cardiff University, Main Building, Park Place, Cardiff, CF10 3AT, UK.

出版信息

Dalton Trans. 2013 Sep 14;42(34):12370-80. doi: 10.1039/c3dt51400e. Epub 2013 Jul 16.

Abstract

Convenient syntheses of mono- and bis-imidazolium 1,3,5-triazine derivatives bearing piperidine and morpholine substituents are reported. In situ deprotonation of the mono-imidazolium salts and reaction with Ag2O or Au(tht)Cl (tht = tetrahydrothiophene) precursors affords the corresponding Ag(NHC)Cl and Au(NHC)Cl carbene complexes. In the presence of Ag(I) or Au(I) salts the bis-imidazolium pincers eliminate the imidazolium group to afford -OMe or -NMe2 substituted triazines depending on the solvent used. In solution, the Ag(I) and Au(I) complexes show a barrier to rotation about the Ctriazine-Namine bonds, with calculated ΔG(≠) barriers in the region of 70 kJ mol(-1). Single crystal X-ray structures of several of the proligands and their corresponding Ag(I) and Au(I) complexes were obtained. These universally reveal an extended, rigidly planar π-conjugated network between the triazine core, imidazolium/imidazolylidene substituents and exocyclic amine functions, to which the origin of the rotational barrier observed in solution is attributed. Only very weak Ntriazine-metal interactions are observed in the solid state, as indicated by small deviations of the CNHC-Ag-Cl bond angles from 180° and also supported by DFT calculations on the Ag(NHC)Cl complex (NHC = 4,6-dipiperidinyl-2-methylimidazolylidene triazine). Preliminary antimicrobial susceptibility studies against five microorganisms (methicillin resistant Staphylococcus aureus NCTC 13277, S. aureus NCTC 6571, Pseudomonas aeruginosa NCTC 10662, Proteus mirabilis NCTC 11938 and Candida albicans ATCC 90028) show that the above triazine-based Ag-NHC complexes are active antimicrobial and antifungal agents.

摘要

报道了一系列含哌啶基和吗啉基取代基的单-和双-咪唑啉 1,3,5-三嗪衍生物的简便合成方法。通过对单-咪唑啉盐进行原位去质子化,并与 Ag2O 或 Au(tht)Cl(tht = 四氢噻吩)前体反应,得到相应的 Ag(NHC)Cl 和 Au(NHC)Cl 卡宾配合物。在 Ag(I)或 Au(I)盐的存在下,双-咪唑啉夹具消除咪唑啉基团,根据所用溶剂的不同,可得到-OCH3 或-NMe2 取代的三嗪。在溶液中,Ag(I)和 Au(I)配合物在三嗪-Namine 键旋转时存在能垒,计算出的ΔG(≠)能垒约为 70 kJ mol(-1)。获得了几个前配体及其相应的 Ag(I)和 Au(I)配合物的单晶 X 射线结构。这些结构普遍揭示了三嗪核、咪唑啉/咪唑啉基取代基和外环胺官能团之间的扩展、刚性平面π共轭网络,这归因于在溶液中观察到的旋转能垒的起源。在固态中只观察到非常弱的 Ntriazine-金属相互作用,这由 CNHC-Ag-Cl 键角偏离 180°的小偏差表明,也得到了 Ag(NHC)Cl 配合物(NHC = 4,6-二哌啶基-2-甲基咪唑啉基三嗪)的 DFT 计算支持。对五种微生物(耐甲氧西林金黄色葡萄球菌 NCTC 13277、金黄色葡萄球菌 NCTC 6571、铜绿假单胞菌 NCTC 10662、奇异变形杆菌 NCTC 11938 和白色念珠菌 ATCC 90028)的初步抗菌药敏研究表明,上述基于三嗪的 Ag-NHC 配合物是有效的抗菌和抗真菌剂。

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