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Peptides and polypeptides as scaffolds for optoelectronics and biomaterials applications.

机译：肽和多肽作为光电子和生物材料应用的支架。

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摘要

Peptides and polypeptides are emerging as a new class of biomaterials due to their unique structural, physiochemical, mechanical, and biological properties. The development of peptide and protein-based biomaterials is driven by the convergence of convenient techniques for peptide/protein engineering and its importance in applications as smart biomaterials. The thesis is divided in two parts; the first part highlights the importance of incorporation of non-natural amino acids into peptides and proteins. In particular, incorporation on p-bromophenylalanine in short alpha-helical peptide templates to control the association of chromophores is discussed. In the second part, design of a multi-component, biocompatible polypeptide with superior elasticity is discussed.;Part1. Novel peptide templates to control association of chromophores.;Tailor made peptide and protein materials have many versatile applications, as both conformation and functional group position can be controlled. Such control may have intriguing applications in the development of hybrid materials for electroactive applications. A critical need in fabricating devices from organic semiconducting materials is to achieve control over the conformation and distance between two conjugated chains. Controlling chromophore spacing and orientation with required precision over nanometer length scale poses a greater challenge. Here we propose a peptide based template to control the alignment of the methylstilbene and Oxa-PPV chromophores with desired orientations and spacing. The hybrid peptides were characterized via CD, exciton coupled CD, 1H NMR and photoluminescence experiments. It is observed that slight change in the orientation of molecules has pronounced effect on the photo-physical behavior of the molecules. Characterization of the hybrid peptides via circular dichroism (CD) confirmed the helical character of the designed peptides and indicated that inclusion of non-natural amino acids has significant effects on peptide conformation. pi-orbital interactions at the molecular level were observed to be very sensitive to intermolecular distance and orientation of the chromophores attached to the alpha-helical peptide templates. When the methylstilbene or Oxa-PPV molecules were arranged on the same side of the helix with intermolecular spacing of 6A, the chromophores interacted strongly with each other forming excimers. Such interactions were absent when the molecules were arranged on the opposite side of the helix. These peptide-templated systems therefore offer enormous opportunities for the elucidation of complex photophysical phenomena that occur in relatively aggregated morphologies of conjugated species, but under dilute solution conditions in which the number of chromphores in the aggregate can be manipulated.;Part 2. Synthesis and characterization of biocompatible polypeptide elastomer.;Lately, the significance of mechanical forces and biological cues involved in tissue remodeling are highly valued; thus the capacity of a biomaterial to present a fitting mechanical and biological environment for optimal tissue generation has become a key parameter for biomaterial design. In addition to having suitable mechanical properties, materials used for these applications need to be biologically active, i.e. trigger dynamic interactions with cells and stimulate explicit cell and tissue responses. Thus, we have designed a resilin-based modular biomaterial incorporating both mechanically and biologically active domains to sense and aptly respond to the bio-mechanical demand or changes in their environment. The use of resilin-like polypeptides offers access to a class of hydrophilic elastomers with excellent resilience and high frequency responsiveness, which can be used for encapsulating hydrophilic drugs like proteins for drug delivery, and provides hydrophilic extracellular matrix mimicking cell adhesive and enzyme degradable substrate for tissue engineering. Hence, we have designed a multi-component elastomeric polypeptide scaffold containing a resilin mimetic flexible domain that governs the mechanical properties, a cell adhesion domain, a proteolytic degradation site and a growth factor binding domain for applications in tissue regeneration. The modular protein was synthesized in an E. coli host and the purified protein, as analyzed via CD and FTIR exhibited mainly unordered conformation with slight contribution from type II beta-turns. The crosslinked protein is highly elastic in nature and support cell attachment. There materials could be used for tissue repair where high frequency responsiveness and superior fatigue resistance are important, such as scaffolds for vocal fold regenerations and as cardiovascular patches.
机译：肽和多肽由于其独特的结构，物理化学，机械和生物学特性而成为一类新型的生物材料。肽和蛋白质基生物材料的发展受到肽/蛋白质工程方便技术的融合及其在作为智能生物材料的应用中的重要性的推动。论文分为两个部分。第一部分强调将非天然氨基酸掺入肽和蛋白质的重要​​性。特别地，讨论了在短的α-螺旋肽模板中掺入对溴苯丙氨酸以控制生色团的缔合。在第二部分中，讨论了具有高弹性的多组分生物相容性多肽的设计。新型肽模板可控制发色团的缔合；量身定制的肽和蛋白质材料具有多种用途，因为可以同时控制构象和官能团位置。在用于电活性应用的混合材料的开发中，这种控制可能具有吸引人的应用。由有机半导体材料制造装置的关键需求是实现对两条共轭链之间的构象和距离的控制。在纳米长度范围内以所需的精度控制发色团的间距和取向提出了更大的挑战。在这里，我们提出了一种基于肽的模板，以控制甲基二苯乙烯和Oxa-PPV发色团以所需的方向和间距进行比对。通过CD，激子偶联的CD，1 H NMR和光致发光实验对杂合肽进行了表征。观察到分子方向的轻微变化对分子的光物理行为具有显着影响。通过圆二色性（CD）对杂合肽进行表征，证实了所设计肽的螺旋特征，并表明包含非天然氨基酸对肽构象有重要影响。观察到在分子水平上的π-轨道相互作用对与α-螺旋肽模板连接的生色团的分子间距离和方向非常敏感。当甲基sti或Oxa-PPV分子以6A的分子间间距排列在螺旋的同一侧时，发色团之间会强烈相互作用，形成受激准分子。当分子排列在螺旋的相反侧时，这种相互作用是不存在的。因此，这些以肽为模板的系统为阐明复杂的光物理现象提供了巨大的机会，这些现象发生在共轭物种的相对聚集形态中，但是在稀溶液条件下，可以控制聚集体中的染色体数目。；第二部分。合成和生物相容性多肽弹性体的表征。最近，涉及组织重构的机械力和生物学线索的重要性受到高度重视。因此，生物材料呈现合适的机械和生物环境以实现最佳组织生成的能力已成为生物材料设计的关键参数。除了具有合适的机械性能外，用于这些应用的材料还必须具有生物活性，即触发与细胞的动态相互作用并刺激明显的细胞和组织反应。因此，我们设计了一种结合了机械和生物活性域的基于弹性蛋白的模块化生物材料，以感知并适当地响应生物力学的需求或环境的变化。使用弹性蛋白样多肽可提供一类具有出色回弹性和高频响应性的亲水性弹性体，可用于封装亲水性药物（如蛋白质）以进行药物递送，并为细胞外基质提供亲水性模仿细胞黏附剂和酶可降解底物，组织工程。因此，我们设计了一种多组分弹性体多肽支架，其中包含可调控机械性能的弹性蛋白模拟结构域，细胞粘附结构域，蛋白水解降解位点和生长因子结合结构域，可用于组织再生。模块化蛋白质是在大肠杆菌宿主中合成的，纯化的蛋白质（通过CD和FTIR分析）主要表现出无序构象，而II型β-转角的贡献很小。交联的蛋白质本质上具有高度弹性，并支持细胞附着。那里的材料可用于组织修复，在这些组织中，高频响应性和出色的抗疲劳性很重要，例如用于声带再生的支架和心血管斑块。

著录项

  • 作者

    Charati, Manoj B.;

  • 作者单位

    University of Delaware.;

  • 授予单位 University of Delaware.;
  • 学科 Engineering Materials Science.
  • 学位 Ph.D.
  • 年度 2009
  • 页码 199 p.
  • 总页数 199
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 工程材料学;
  • 关键词

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