Supramolecular Bioinspired Responsive Materials: Exploiting Polyproline Helices

该项目将率先使用一类独特的刺激反应生物相容性超分子构建块，聚脯氨酸螺旋，用于合成新型超分子生物激发反应材料。我们将创造独特的智能生物相容性结构，能够执行发散绿色催化，化学传感，化学分离和药物输送。利用超分子相互作用（动态的、“非永久的”和可逆的相互作用），科学家们可以创造出具有前所未有的性能的材料，比如自我修复。使用生物聚合物，如DNA和RNA，来创建复杂的3D结构（DNA折纸）是将超分子化学与可编程和周期性生物聚合物相结合时可实现的独特结果的一个主要例子。多肽是一种不同类型的生物聚合物，作为生物启发超分子化学的潜在构建块而受到越来越多的关注。这些类型的生物聚合物可以大量获得，并且可以使用强大的合成方法与非天然氨基酸功能化。它们作为超分子化学基石的行为是一个正在进行和活跃的研究领域。在这个研究项目中，我们将使用一种具有明确二级结构的特殊类型的肽：聚脯氨酸螺旋。这些手性螺旋是稳定的（即使是在短序列中），通用的（即它们可以在不干扰其构象的情况下在其主链上承受广泛的功能），并对外部刺激（如温度，pH值，溶剂性质）有反应。这些特性的结合将使我们能够对肽进行编程，使其以各种方式组装，从而产生不同的结构，每种结构都将执行独特的任务（例如主客体化学，催化，可编程组装和拆卸结构）。该项目旨在了解这些肽作为超分子构建块的行为，以便合理设计独特的智能生物材料，能够以绿色和生物相容性的方式进行化学催化，化学传感，化学分离和药物输送。我们有条不紊和理性的方法将导致生物启发超分子化学领域的重大进步，使英国处于这一令人兴奋的研究领域的前沿。

This project will pioneer the use of a unique class of stimuli responsive biocompatible supramolecular building blocks, polyproline helices, for the synthesis of novel supramolecular bioinspired responsive materials. We will create unique smart biocompatible constructs capable of performing divergent green catalysis, chemical sensing, chemical separation and drug delivery. The use of supramolecular interactions (dynamic, "non-permanent" and reversible interactions) allow scientists to create materials with unprecedented properties such as self-healing. The use of biopolymers, such as DNA and RNA, to create complex 3D structures (DNA origami) is a prime example of the unique results achievable when combining supramolecular chemistry with programmable and periodic biopolymers. Peptides are a different type of biopolymer which are receiving increasing interest as potential building blocks in bioinspired supramolecular chemistry. These types of biopolymers can be accessed in large quantities and can be functionalised with non-natural amino acids using robust synthetic methods. Their behaviour as building blocks in supramolecular chemistry is an ongoing and active area of research. In this research project we will be using a specific type of peptide with a well-defined secondary structure: polyproline helices. These chiral helices are stable (even in short sequences), versatile (ie they can tolerate a wide range of functionalities on their backbone without perturbation of their conformation) and are responsive to external stimuli (eg temperature, pH, nature of the solvent). These properties combined will allow us to programme the peptides to assemble in a variety of ways giving rise to different constructs, each of which will perform a unique task (eg host-guest chemistry, catalysis, programmable assembly and disassembly of a construct). This project aims to understand the behaviour of these peptides as supramolecular building blocks in order to rationally design unique smart biomaterials capable of performing chemical catalysis, chemical sensing, chemical separation and drug delivery in a green and biocompatible manner. Our methodical and rational approach will lead to a significant advancement in the field of bioinspired supramolecular chemistry placing the UK at the forefront of this exciting research area.