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。本研究旨在开发一种新的固体催化剂系列，我们打算用它来产生环加成反应的环状化合物。我们的催化剂是金属-有机框架（简称MOFs），它由金属原子和有机连接剂组成的网格状组装。mof是一种相对较新的材料，用它们来催化反应是非常罕见的。然而，它们有很大的希望，因为它们含有发生反应的孔，这些孔的大小和形状可以通过改变有机连接剂来控制，从而改变孔中的反应条件。许多天然和合成的化合物都是手性的，这意味着它们可以以左手和右手的形式存在，它们互为镜像。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。我们将研究是否通过使用手性MOF催化剂，我们可以产生手性的反应产物，即只有左手或右手。为了进行这些研究，我们打算从不同的角度来解决这个问题：1)在实验室中使用合成化学来生产MOF催化剂，并随后测试其手性环加成反应的可行性；2)利用计算机模拟来预测这些催化剂如何在分子水平上起作用；3)测量催化剂的扩散和吸附性能，了解试剂如何进入孔隙以及分子如何与催化剂相互作用。通过结合这三种方法，我们希望生产出更有效的催化剂，在纯状态下产生环加成产物，并且具有“左”或“右”手性。

Catalysts 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 cycloaddition reactions. Our catalysts are metal-organic frameworks (abbreviated to MOFs) which are comprised of a grid-like assembly of metal atoms and organic linkers. 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 thus altering the reaction conditions in the pores.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 will investigate 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 different points of view: 1) using synthetic chemistry to produce MOF catalysts in the laboratory and subsequently testing their viability for chiral cycloaddition reactions; 2) using computer simulations to predict how these catalysts could work at a molecular level; and 3) measuring the diffusion and adsorption properties of the catalysts to find out how the reagents move into the pores and how the molecules interact with the catalyst. By combining these three approaches we hope to produce more efficient catalysts that produce cycloaddition products in a pure state and as one chirality, either 'left' or 'right'.