Understanding Liquid Phase Heterogeneous Catalysis to Develop Catalytic Processes

该项目与对液相反应的非均相催化剂的理解有关。特别是，我们的目标是开发一些技术，通过这些技术来探测的非均相催化剂的孔内的反应，以关联的活性-选择性的催化剂与特定的表面和液相相互作用。这项研究将弥合理解典型的非均相催化剂的孔中限制的液体的性质之间的知识差距，和它们的应用。对支撑这些复杂系统的化学功效的多相相互作用的这种缺乏理解是限制许多涉及复杂的固/液和固/液/气界面的可持续催化过程的发展的主要因素之一。例如，扩散过程以及吸附在确定这些多相反应的选择性方面是至关重要的。然而，在液相反应中的催化剂的孔内，很难评估它们的相对贡献，因为观察到的全局动力学是表面反应动力学和质量传递的组合。一系列的互补NMR和中子散射技术将建立，例如，从其中，扩散特性，孔液相结构和吸附模式将在反应条件下阐明。这些新技术的信息将与X射线吸收和红外光谱数据以及密度泛函理论计算和动力学建模相结合，以获得反应条件下多孔多相催化剂系统内的气/液反应的完整描述。为了开发该技术，将使用两类示例性选择性氢化反应。苯乙炔加氢制苯乙烯和乙苯为这一要求低温低压的连续反应工艺提供了试验平台。一旦建立，将开发更高压力和温度的电池，以使芳香酸氢化的研究成为可能。用于该反应的催化剂可以定制以有利于许多产物，包括芳族醇、环氢化醇或甲苯胺基衍生物，并且呈现具有多个途径但在工业上非常相关的更具挑战性的方法。该项目将由贝尔法斯特女王大学、剑桥大学、ISIS和约翰逊万泰密切合作开展。

This project is associated with the understanding of heterogeneous catalysts for liquid phase reactions. In particular, we aim to develop a number of techniques by which to probe the reactions within the pores of the heterogeneous catalysts in order to correlate the activity-selectivity of the catalyst with the specific surface and liquid phase interactions. This research will bridge the knowledge gap between understanding the properties of liquids confined in the pores of typical heterogeneous catalysts, and their applications. This lack of understanding of the multiphase interactions underpinning the chemical efficacy of these complex systems is one of the major factors restraining the advancement of many sustainable catalytic processes which involve complex solid/liquid and solid/liquid/gas interfaces. For example, diffusion processes as well as adsorption are critically important in determining the selectivity of these multiphase reactions. However, within the pores of the catalyst in liquid phase reactions it is difficult to evaluate their relative contributions as the observed global kinetics observed are a combination of surface reaction kinetics as well as mass transport. A range of complementary NMR and neutron scattering techniques will be established from which, for example, the diffusion characteristics, pore liquid phase structure and adsorption modes will be elucidated under reaction conditions. The information from these new techniques will be combined with X-ray absorption and infra-red spectroscopy data as well as Density Functional Theory calculations and kinetic modelling in order to obtain a complete description of a gas/liquid reaction within a porous heterogeneous catalyst system under reaction conditions. In order to develop the techniques two families of exemplar selective hydrogenation reactions will be used. The hydrogenation of phenylacetylene to styrene and ethylbenzene will provide a test bed for the techniques which requires low pressures and temperatures and is a sequential reaction. Once established, higher pressure and temperature cells will be developed to enable the study of aromatic acid hydrogenation. The catalyst for this reaction can be tailored to favour a number of products including the aromatic alcohol, ring hydrogenated alcohol or toluidyl derivatives and presents a more challenging process with multiple pathways but one which is industrially very relevant. The project will be undertaken by the Queen's University of Belfast, University of Cambridge, ISIS and Johnson Matthey in close collaboration.