Catalytic applications of metal-organic frameworks

催化剂在不改变自身的情况下提高反应速度。本研究旨在开发一系列新的固体催化剂，我们打算用它来生产环状化合物，使用一种称为环加成反应。我们的催化剂由金属原子和有机连接体的网格状组装体组成，这些材料被称为金属有机框架（缩写为MOFs）。MOFs是相对较新的材料，将其用于催化反应非常罕见。然而，它们有很大的希望，因为它们含有反应发生的孔，这些孔的大小和形状可以通过改变有机连接体来控制。许多天然和合成化合物是手性的，这意味着它们可以以左手和右手的形式存在，彼此是镜像。手性在药物生产中很重要，因为通常两种可能的左手或右手药物分子中只有一种具有生物活性。我们打算看看通过使用手性MOF催化剂，我们是否可以产生本身是手性的反应产物，即只有左手或右手。为了进行这些研究，我们打算从两个角度来解决这个问题：一个是使用合成化学和在实验室中生产MOF催化剂;另一个是基于计算机模拟，预测这些催化剂如何在分子水平上工作。通过结合这两种方法，我们希望将这两个过程“融合”在一起，并产生更有效的MOF催化剂，这些催化剂在纯状态下产生环加成产物，并且作为一种手性，无论是“左”还是“右”。我们还将测量催化剂的扩散和吸附特性，以便了解试剂如何进入孔隙以及分子如何与催化剂相互作用。

SummaryCatalysts increase the speed of reactions without themselves being changed. This research aims to develop a new series of solid catalysts that we intend to use to produce cyclic compounds using a reaction called cycloaddition. Our catalysts are comprised of a grid-like assembly of metal atoms and organic linkers, and these materials are called metal-organic frameworks (abbreviated to MOFs). MOFs are relatively new materials and use of them for catalysing reactions is very rare. They have, however, great promise as they contain pores in which the reactions occur, and the size and shapes of these pores can be controlled by altering the organic linkers.Many natural and synthetic compounds are chiral, which means they can exist in left-handed and right-handed forms that are mirror images of each other. Chirality is important in the production of drugs as usually only one of the two possible left- or right-handed drug molecules is biologically active. We intend to see if by using chiral MOF catalysts we can produce reaction products that are themselves chiral i.e. only left or right-handed.To undertake these studies we intend to attack the problem from two points of view: One of these uses synthetic chemistry and the production of MOF catalysts in the laboratory; the other is based on computer simulations, predicting how these catalysts could work at a molecular level. By combining these two approaches we hope to 'fuse' these two processes together and produce more efficient MOF catalysts that produce cycloaddition products in a pure state and as one chirality, either 'left' or 'right'. We will also measure the diffusion and adsorption properties of the catalysts so we find out how the reagents move into the pores and how the molecules interact with the catalyst.