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Surface modification and controlled assembly of molecular materials.

机译：分子材料的表面改性和受控组装。

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摘要

Organic materials were prepared to gain an understanding of how to control the surface and bulk properties of molecular materials. Surfaces were modified by growing thin films of electronically relevant phenylene vinylene hyperbranched polymers from silicon using the Heck reaction with triiodobenzene and divinylbenzene monomers. Hyperbranched polymers enabled continued film growth regardless of random chain termination. Films were grown by reacting one monomer with the surface at a time and washing the unreacted monomer away. Films grown from patterned surfaces indicated monomers reacted with chemisorbed initiator molecules on the surface and did not physisorb onto unpatterned regions. Films were characterized using XPS, ellipsometry, SEM, and AFM.; Bulk organization of molecular materials was studied using oligomers and single crystals. A series of oligo(m-phenylene ethynylene)s having triethylene glycol ester-linked side chains were studied with regard to their supramolecular organization in the solid-state. Small angle X-ray diffraction indicated that the oligomers with a chain length of eight or more monomers organized longitudinally with a d-spacing linearly dependent on the chain length, suggestive of lamellar packing. This is in contrast to the helical conformation observed in acetonitrile.; Single crystal molecular organization was investigated using coordination network crystals. Crystals that had molecules arranged as chains, such as catena-poly[dicyanobenzene-silver(I)]-triflate, were exposed to inhibitors specifically designed to bind at the growing surface. It was found that inhibitors had qualitative effects on the morphology and on the surface composition of the crystals and that the surface and bulk properties had potential to be modified independently. Copper-pyridine crystals were studied to determine how the steric bulk on pyridine influenced the pyridine coordination to copper. It was found that as the steric bulk of the pyridine increased, the probability that all the copper coordination sites were occupied with pyridine decreased, and that solvent molecules and ancillary ligands also coordinated to copper. A single crystal of 4'-undecyloxy-4-biphenyl carbonitrile revealed that the molecules in the crystalline form had similar organization as the molecules in the smectic phase.
机译：准备有机材料以了解如何控制分子材料的表面和体积特性。通过与三碘代苯和二乙烯基苯单体的Heck反应，从硅上生长出电子相关的亚苯基亚乙烯基超支化聚合物的薄膜来修饰表面。超支化聚合物可实现连续的膜生长，而与无规链终止无关。通过一次使一种单体与表面反应并洗去未反应的单体来生长薄膜。从形成图案的表面生长的膜表明单体与表面上化学吸附的引发剂分子反应，没有物理吸附到未形成图案的区域上。使用XPS，椭偏仪，SEM和AFM对膜进行表征。使用低聚物和单晶研究了分子材料的整体组织。研究了具有三乙二醇酯连接的侧链的一系列低聚（间亚苯基亚乙炔基）的固态超分子结构。小角度X射线衍射表明，链长为八个或更多的单体的低聚物纵向排列，d-间距线性地取决于链长，暗示了层状堆积。这与在乙腈中观察到的螺旋构象相反。使用配位网络晶体研究了单晶分子组织。将具有链状排列的分子的晶体（例如链烯-聚[二氰基苯-银（I）]-三氟甲磺酸盐）暴露于专门设计用于在生长表面结合的抑制剂。发现抑制剂对晶体的形态和表面组成具有定性作用，并且表面和整体性质具有独立改性的潜力。研究了铜-吡啶晶体，以确定吡啶上的空间体积如何影响吡啶与铜的配位。发现随着吡啶的空间体积的增加，所有铜配位位点被吡啶占据的可能性降低，并且溶剂分子和辅助配体也与铜配位。 4'-十一烷氧基-4-联苯腈的单晶表明，该结晶形式的分子与近晶相分子具有相似的组织。

著录项

  • 作者

    Prest, Peggy-Jean.;

  • 作者单位

    University of Illinois at Urbana-Champaign.;

  • 授予单位 University of Illinois at Urbana-Champaign.;
  • 学科 Chemistry Organic.; Engineering Materials Science.; Chemistry Polymer.
  • 学位 Ph.D.
  • 年度 1999
  • 页码 126 p.
  • 总页数 126
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 有机化学;工程材料学;高分子化学（高聚物）;
  • 关键词

  • 入库时间 2022-08-17 11:48:14

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