Polymer Mechanochemistry Enhanced with Mechanically Interlocked Molecules

通过机械联锁分子增强聚合物机械化学

• 批准号: EP/X023788/1
• 负责人: Guillaume De Bo
• 金额: $ 219.57万
• 依托单位: University of Manchester
• 依托单位国家: 英国
• 项目类别: Research Grant
• 财政年份: 2023
• 资助国家: 英国
• 起止时间: 2023 至 无数据
• 项目状态: 未结题
• 来源: https://gtr.ukri.org/projects?ref=EP%2FX023788%2F1
• 关键词: Polymer; Mechanochemistry; Enhanced; Mechanically; Interlocked

Mechanical force is a formidable source of energy that, with its ability to distort, bend and stretch chemical bonds, is unique in the way it activates chemical reactions. In polymer mechanochemistry, polymers are used to transduce mechanical force towards a mechanoresponsive functional group (a "mechanophore") that then undergoes a mechanochemical transformation. Although mechanical force is exceptional in its ability to promote reaction pathways that are otherwise inaccessible, it has so far been limited to transformations involving bond cleavage or rearrangements. The origin of these limitations is due to the fact that the actuating polymers have to be linked to the mechanophore to activate it, which has so far made impossible to: repetitively activate scissile mechanophores or to build molecules. A solution to that problem would be to find a way for the polymer to 'grab' the mechanophore without being covalently attached to it. Interlocked molecules, which have been instrumental in the development of molecular machines, are ideally suited for that task because their subcomponents are entangled in space but not covalently linked. As a result, they can undergo large amplitude internal displacements, such as a macrocycle shuttling along the axle of a rotaxane, which makes them attractive force actuators. In this programme, we want to demonstrate how a rotaxane architecture can be used to repetitively activate scissile mechanophores and to build molecules.

机械力是一种强大的能源，其扭曲，弯曲和拉伸化学键的能力在激活化学反应的方式上是独一无二的。在聚合物机械化学中，聚合物用于将机械力转向机械官能团（一种“机械电池”），然后进行机械化学转换。尽管机械力在促进反应途径的能力方面是不可访问的，但迄今为止，它仅限于涉及键裂解或重排的转化。这些局限性的起源是由于必须将致动聚合物与机械电池相关的事实以激活它，这到目前为止，这已经无法重复激活剪刀机械粒或构建分子。解决该问题的一种解决方案是找到一种方法，可以使聚合物“抓住”机械学，而无需共价附着在其上。互锁的分子在分子机器的开发中发挥了作用，非常适合该任务，因为它们的子组件纠缠在太空中，但没有共价连接。结果，它们可以经历大幅度的内部位移，例如沿着旋转烷的轴的大环班车，这使它们成为吸引力的力执行器。在此程序中，我们要演示如何使用轮济烷结构重复激活剪刀机械团并构建分子。