Dynamically Adaptive Metal-organic Nanopores

我们建议制备和研究一类新的基于动态金属-有机络合物的合成离子通道，它拥有一个孔状的中心通道，允许底物通过脂质双层进行运输。这些配合物是通过在八面体金属离子模板周围凝聚简单的有机构筑块而得到的。这些络合物的模块化性质及其亚胺键的动态性质将使我们能够调整组装，以赋予它们不同的物理性质，同时保持它们的整体结构。通过调整，我们将确定可以插入到脂质双层中的复合体的关键特征。这个项目建立在初步研究的基础上，这些研究表明，含庚基链的衍生物允许氯离子通过膜，为我们的研究提供了一个出发点。在其他关键的先例工作中，我们建立了在不同模板阴离子存在的情况下，有可能诱导络合物重组为完全不同的结构。我们将研究如何利用这一现象作为一种控制跨膜通量的方法，方法是可逆地触发重组，形成不具有中心通道的复合体，从而抑制离子传输。这些可调节的选通离子通道的开发将为新的工业工艺铺平道路，这些工艺由有效地将高价值化合物从不纯混合物中分离出来，以及涉及在泡状反应室之间选择性地选通中间物种的新的化学转化。在未来，我们的技术还可能为那些患有经络病的人提供新的治疗方法。

We propose to prepare and study a new class of synthetic ion channels based on dynamic metal-organic complexes that possess a pore-like central channel that will allow for substrate transport across a lipid bilayer. These complexes are obtained through the condensation of simple organic building blocks around octahedral metal ion templates. The modular nature of these complexes and the dynamic nature of their imine bonds will allow us to tune the assemblies to confer different physical properties upon them, while retaining their overall structures. Through tuning we will identify the key characteristics of complexes that can be inserted into lipid bilayers. This project builds upon preliminary investigations that have shown that heptyl-chain-bearing derivatives allowed chloride ions to pass across a membrane, providing a point of departure for our investigations.In other key precedent work we established that it is possible to induce reconstitution of the complexes into entirely different structures in the presence of different templating anions. We will investigate ways to exploit this phenomenon as an approach to controlling flux across a membrane by reversibly triggering reconstitution to form complexes that do not possess central channels, thus inhibiting ion transport. Development of these tuneable, gating ion channels will pave the way to new industrial processes that are driven by the effective separation of high value compounds from impure mixtures, and new chemical transformations involving the selective gating of intermediate species between vesicular reaction chambers. In future, our technologies may also facilitate new treatments for those who suffer from forms of channelopathy.