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Synthesis and applications of ruthenium(II)quaterpyridinium complexes and poly-N-isopropylacrylamide/acrylic acid copolymers.

机译：钌（II）四吡啶鎓配合物和聚-N-异丙基丙烯酰胺/丙烯酸共聚物的合成和应用。

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摘要

Tris-homoleptic ruthenium(II)-quaterpyridyl and quaterpyridinium complexes, with +8 and +14 charge were synthesized by utilizing high pressure reaction pathway. These complexes have diameters ranging from 1.82 to 4.55 nm according to the molecular modeling calculations. These ruthenium complexes are highly luminescent and contain long excited state life times. The novel ruthenium(II)-quaterpyridinium complexes exhibit superior reactivity as sensitizer-relay-assemblies (SRA's) in sacrificial systems for water and carbon dioxide reductions, while harvesting the ultraviolet- and most of the visible fraction of the incident solar spectrum. Ru(II)-quaterpyridinium complexes and Pd/TiO2 catalysts were successfully used as the catalytic system for the photo catalytic reduction of water and carbon dioxide to hydrogen and methane respectively. Phosphonate-tethered Ru(II)-quaterpyridinium complexes were synthesized from Ru(II)-tris-quaterpyridyl complexes. These complexes form stable adhesive layers on indium tin oxide (ITO) electrodes. A series of differential pulse voltammetry experiments were carried out to measure the ground state and excited state redox potentials of all the Ru(II)quaterpyridinium complexes. The reductive potentials obtained were compared with the reductive potentials of CO2 to CH4 and H2O to H2 reductions. The measurements obtained from the experiments confirmed that it is possible to thermodynamically oxidize water and reduce CO2 by using phosphonate-tethered Ru(II)-quaterpyridinium complexes.;These complexes are successfully utilized as prototypes for mycobacterial channel blockers. The Ru(II) complexes show distinct changes in their luminescence spectra when bound to the porin MspA from M. smegmatis, which is a non-pathogenic relative of M. tuberculosis. By using HPLC, we have determined binding constants of the Ru(II)-complexes to MspA in phosphate buffer (0.05 M, pH = 6.8) ranging from 5.2 x 109 M-1 (Ru-C2) to 1.8 x 109 M-1 (Ru-C4). Our findings indicate that channel blocking is a promising treatment strategy for mycobacterial infections.;Poly-N-isopropyl-acrylamide/acetic acid copolymers were synthesized and characterized by elemental analysis and gel permeation chromatography. The average composition of the copolymers determined from CHN analysis is in excellent correlation with the feed composition indicating that the radical polymerization process is indeed statistical. Crosslinking of individual polymer chains permitted the generation of ultraflat layers on Mica surfaces by a simple spin-casting procedure, which are able to host the mycobacterial channel protein MspA, while retaining its channel function.
机译：利用高压反应途径合成了具有+8和+14电荷的三同位钌（II）-四吡啶基和四吡啶鎓配合物。根据分子模型计算，这些配合物的直径范围为1.82至4.55 nm。这些钌配合物具有高发光性，并具有较长的激发态寿命。新型钌（II）-四吡啶鎓络合物在牺牲系统中表现出优异的反应性，可作为增敏剂-继电器组件（SRA）用于减少水和二氧化碳，同时收获了入射太阳光谱的紫外线和大部分可见光。 Ru（II）-季铵盐配合物和Pd / TiO2催化剂已成功用作催化体系，用于将水和二氧化碳分别光催化还原为氢气和甲烷。由Ru（II）-三-季吡啶基配合物合成了膦酸酯系的Ru（II）-四吡啶鎓配合物。这些络合物在铟锡氧化物（ITO）电极上形成稳定的粘合剂层。进行了一系列差分脉冲伏安法实验，以测量所有Ru（II）四吡啶鎓络合物的基态和激发态氧化还原电势。将获得的还原电势与CO2还原为CH4以及H2O还原为H2的还原电势进行了比较。从实验中获得的测量结果证实，通过使用膦酸酯束缚的Ru（II）-季吡啶鎓配合物可以热力学氧化水并减少CO2。这些配合物已成功用作分枝杆菌通道阻滞剂的原型。当与耻垢分枝杆菌的孔蛋白MspA结合时，Ru（II）配合物在其发光光谱中显示出明显的变化，这是结核分枝杆菌的非致病性亲戚。通过HPLC，我们确定了Ru（II）复合物与磷酸盐缓冲液（0.05 M，pH = 6.8）中MspA的结合常数，范围为5.2 x 109 M-1（Ru-C2）至1.8 x 109 M-1 （Ru-C4）。我们的研究结果表明，通道阻断是一种针对分枝杆菌感染的有前途的治疗策略。;合成了聚-N-异丙基-丙烯酰胺/乙酸共聚物，并通过元素分析和凝胶渗透色谱进行了表征。由CHN分析确定的共聚物的平均组成与进料组成具有极好的相关性，表明自由基聚合过程确实是统计的。单个聚合物链的交联允许通过简单的旋转浇铸程序在云母表面生成超平层，该层能够容纳分枝杆菌通道蛋白MspA，同时保留其通道功能。

著录项

  • 作者

    Siyambalagoda Gamage, Pubudu Hasanka.;

  • 作者单位

    Kansas State University.;

  • 授予单位 Kansas State University.;
  • 学科 Chemistry Organic.
  • 学位 Ph.D.
  • 年度 2009
  • 页码 187 p.
  • 总页数 187
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

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