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首页> 外文学位 >Properties and applications of tetrahedral organic molecules; new tripodal titanium dioxide sensitizers.
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Properties and applications of tetrahedral organic molecules; new tripodal titanium dioxide sensitizers.

机译：四面体有机分子的性质和应用；新的三脚架二氧化钛敏化剂。

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摘要

This thesis includes three chapters related to two projects. The first chapter describes a new approach for studying fixed distance electron transfer at molecule-nanoparticle interface. The general strategy is to utilize a tripod-shaped organic molecule as a rigid, three-point anchor that positions a sensitizer at fixed distance with respect to the surface of semiconductor nanoparticles. The tripods are unsymmetrical adamantane derivatives with three rigid-rod arms terminating with ester groups and a fourth arm terminating with a Ru II-polypyridine complex as a sensitizer. The synthetic methodology that we have developed allowed us to synthesize a variety of tripods. These were anchored to TiO2 nanoparticles by the formation of an ester bond. High binding constants and high surface coverages on TiO2 surface were observed for all tripods. The absorption difference spectra of the TiO2 bound tripods indicate rapid interfacial electron transfer (kcs > 108 s−1 and fast charge recombination (200 μs). A specific application of Ru(II) sensitizers is as photoanodes in regenerative solar cells, and we have demonstrated that the tripods can be employed to prepare cells that convert light into electricity as efficiently as other Ru(II) complexes.; The second chapter describes a study of the motif-forming characteristics of weak intermolecular interactions (Br &cdots; Br, C≡CH &cdots; C≡C and C≡CBr &cdots; C≡C) in the crystals of tetraphenylmethane and 1,3,5,7-tetraphenyladamantane derivatives substituted at the four vertices with bromo, ethynyl and bromoethynyl groups. The crystals of the bromo- and ethynyl-substituted tetraphenylmethane derivatives exhibited diamondoid lattices sustained by weak interactions between the bromo- and ethynyl substituents. It was observed that when the bromo- and ethynyl groups were interchanged in these compounds, their solid-state structures did not change significantly. The crystals of tetrakis(4-bromoethynyphenyl)methane, as well as 1,4- and 1,3,5-bromoethynylbenzene, were sustained by rare, T-shaped C≡CBr &cdots; C≡C contacts, but a comparison between these solid-state structures showed significant differences in the ways bromoethynyl groups interact.
机译：本文包括与两个项目相关的三章。第一章介绍了一种研究分子-纳米粒子界面上固定距离电子转移的新方法。一般的策略是利用三脚架形状的有机分子作为刚性的三点固定点，该固定点将敏化剂相对于半导体纳米粒子的表面固定地定位。三脚架是不对称的金刚烷衍生物，其三个刚性杆臂以酯基为末端，而第四臂以Ru II -聚吡啶配合物为敏化剂。我们开发的合成方法使我们能够合成各种三脚架。它们通过形成酯键固定在TiO 2 纳米颗粒上。在所有三脚架上都观察到了TiO 2 表面的高结合常数和高表面覆盖率。 TiO 2 结合的三脚架的吸收差谱表明界面电子转移迅速（ k c s 8 s −1 和快速电荷重组（200μs）。Ru（II）敏化剂的具体应用是作为可再生太阳能电池中的光阳极，我们已经证明三脚架可用于制备能第二章描述了弱分子间相互作用（Br ＆cdots; Br ，C≡CH ＆cdots; C≡C和C≡CBr ＆cdots; C≡C）在四个顶点上被溴，乙炔基和溴乙炔基取代的四苯基甲烷和1,3,5,7-四苯基金刚烷衍生物的结构溴和乙炔基取代的四苯基甲烷衍生物的晶体表现出由弱整数支撑的类金刚石晶格溴和乙炔基取代基之间的区别。观察到当这些化合物中的溴和乙炔基互换时，它们的固态结构没有明显改变。四（4-溴乙炔基苯基）甲烷，1,4-和1,3,5-溴乙炔基苯的晶体由稀有的T形C≡CBr ＆cdots支撑。 C≡C接触，但是这些固态结构之间的比较显示溴乙炔基相互作用的方式存在显着差异。

著录项

  • 作者

    Guo, Wenzhuo.;

  • 作者单位

    Rutgers The State University of New Jersey - Newark.;

  • 授予单位 Rutgers The State University of New Jersey - Newark.;
  • 学科 Chemistry Organic.
  • 学位 Ph.D.
  • 年度 2001
  • 页码 p.1395
  • 总页数 169
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 有机化学;
  • 关键词

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