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Water-Soluble Silver(I) Complexes Featuring the Hemilabile 3,7-Dimethyl-1,3,5-triaza-7-phosphabicyclo[3.3.1]nonane Ligand: Synthesis, Characterization, and Antimicrobial Activity
Inorganic Chemistry ( IF 4.6 ) Pub Date : 2018-05-23 00:00:00 , DOI: 10.1021/acs.inorgchem.8b00227
Declan Armstrong , Sarah M. Kirk , Cormac Murphy , Antonella Guerriero 1 , Maurizio Peruzzini 1, 2 , Luca Gonsalvi 1 , Andrew D. Phillips 1
Affiliation  

This paper describes the preparation and comprehensive characterization of a series of water-soluble cationic silver(I)-centered complexes featuring the hemilabile P,N-ligand known as 3,7-dimethyl-1,3,5-triaza-7-phosphabicyclo[3.3.1]nonane (herein abbreviated as PTN(Me)) and differing types of monoanionic counterions including known biologically active sulfadiazine and triclosan. The complexes primarily differed though the number of coordinating PTN(Me) ligands. The bis-substituted Ag(I) complexes revealed P,N bidentate coordination, while the only P-monocoordination of the metal center was observed for the tris-substituted systems. The bis-ligated silver compounds were observed to quickly degrade upon photoexposure or in contact with air. In contrast, the tris-ligated complexes demonstrated greater stability, in particular, a high resistance to photo-decomposition. Calculated geometry optimized models using the density functional theory method (BP86) revealed for the bis-substituted PTN(Me) Ag(I) species that the total enthalpy of the tetrahedral C2-symmetric structure is marginally lower by −0.6 kcal mol–1 compared to the planar C2h structure, which is analogous for the corresponding [Au(PTN(Me))2]+ complex with ΔH = −0.5 kcal mol–1. Hence both types of complexes feature free rotation of the PTN ligand about the M–P bond axis. This series of Ag(I) and bis-PTN(Me) Au(I) complexes were evaluated using the agar well diffusion test for potential antimicrobial and antifungal activity. The nature of the counterion was found to have a strong correlation with the area of microbiological growth inhibition. Silver(I) complexes bearing the deprotonated triclosan as the counterion demonstrated the greatest activity, with large zones of growth inhibition, with the tris-ligated triclosan complex obtaining of a high clearance of 42 mm against the Gram-negative Escherichia coli. In contrast, the previously reported [Au(PTN(Me))2]Cl complex demonstrated activity only against E. coli, which is lower than that observed for the silver(I) PTN(Me) species.

中文翻译:

具有半不稳定的3,7-二甲基-1,3,5-三氮杂-7-磷杂双环[3.3.1]壬烷配体的水溶性银(I)配合物:合成,表征和抗菌活性。

本文描述了一系列水溶性阳离子银(I)中心的配合物的制备和全面表征,这些配合物具有半不稳定的PN-配体,称为3,7-二甲基-1,3,5-三氮杂-7-磷杂双环[3.3.1]壬烷(在此缩写为PTN(Me))和不同类型的单阴离子抗衡离子,包括已知的生物活性磺胺嘧啶和三氯生。配合物的主要区别在于配体PTN(Me)配体的数量。双取代的Ag(I)配合物显示PN的双齿配位,而唯一的P对于三取代的体系,观察到金属中心的单配位。观察到双连接的银化合物在曝光或与空气接触时迅速降解。相反,tris-连接的复合物显示出更高的稳定性,特别是对光分解的高抗性。使用密度泛函理论方法(BP86)计算的几何优化模型显示,对于双取代的PTN(Me)Ag(I)物种,四面体C 2对称结构的总焓略低-0.6 kcal mol –1与平面C 2 h结构相比,这类似于相应的[Au(PTN(Me))2 ] +ΔH = −0.5 kcal mol –1的复合物。因此,两种类型的复合物都具有PTN配体绕M–P键轴自由旋转的特征。使用琼脂井扩散测试评估了该系列的Ag(I)和bis-PTN(Me)Au(I)复合物的潜在抗微生物和抗真菌活性。发现抗衡离子的性质与微生物生长抑制区域有很强的相关性。带有去质子化的三氯生作为抗衡离子的银(I)配合物表现出最大的活性,具有较大的生长抑制区域,而三连接的三氯生配合物对革兰氏阴性大肠杆菌具有42毫米的高清除率。相反,先前报道的[Au(PTN(Me))2] Cl复合物仅对E具有活性。大肠杆菌,低于银(I)PTN(Me)物种所观察到的。
更新日期:2018-05-23
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