High End Computing for the Characterisation of Structure and Reactivity of Complex Oxide Catalysts

我们建议继续开发和优化用于嵌入式集群(混合量子/经典)计算的计算机代码。这些发展提出了针对高端计算平台的建议，并涉及到充分利用拥有数百或数千个处理器的机器所需的优化和算法改变。其结果将是能够对凝聚相体系的结构和反应性进行更准确计算的代码，例如执行多相催化的体系的活性表面位置。这类体系通常是混合金属氧化物材料，通常由额外的过渡金属原子或团簇提供反应中心。所提出的发展将使高精度量子方法应用于系统的更大部分，处理更大和更复杂的反应中心，并允许更先进的理论方法，例如从依赖密度泛函理论(DFT)转向多组态方法(MCSCF)，微扰理论(MP2)和耦合团簇(CCSD(T))。我们将测试一些工业上感兴趣的催化体系的发展，例如(I)氧化锌和二氧化钛(乙醇水蒸气重整制氢催化剂)的表面，(Ii)MoS21Al203界面-用于汽油加氢脱硫的界面(Iii)基于微孔硅酸盐和硅酸铝材料(包括沸石)的催化剂，用于链和芳香烃的部分氧化、羟基化和环氧化。该项目将适合同时有望完成高性能计算硕士学位的博士生。这门课程将在实习期间作为一系列模块教授，提供基础技术方面的培训，例如软件开发所需的并行计算机的MPI编程。

We propose to continue the development and optimisation of computer codes for embedded cluster (mixed quantum/classical) calculations. The developments proposed target High End Computing platforms, and involve optimisations an algorithm changes needed to make full use of machines with hundreds or thousands of processors. The result will be codes capable of performing more accurate calculations of the structure and reactivity of condensed phase systems, such as the active surface sites of systems which perform heterogeneous catalysis. Such systems are often mixed metal oxide materials, often with additional transition metal atoms or clusters providing the reaction site.The proposed developments will allow high accuracy quantum methods to be applied to a larger part of the system, deal with larger and more complex reacting sites, and also to allow more advanced theoretical methods, for example moving from reliance on Density Functional Theory (DFT) to multiconfiguration methods (MCSCF), perturbation theory (MP2) and coupled cluster (CCSD(T)).We will test out the developments on a number of catalytic systems of industrial interest, such as(i) the surfaces of ZnO and TiO2 (catalysts for the production of hydrogen by ethanol steam reforming), (ii) the interface between MoS21AI203 interface - for hydrodesulphurisation of gas oils(iii) catalysts based on microporous siliceous and aluminium silicate materials (including zeolites) for partial oxidation, hydroxylation and epoxidation of chain and aromatic hydrocarbonsThe project will be suitable for a PhD student who is also expected to complete an MSc in High Performance Computing. This course wll be taught as a series of modules during the studentship, providing training in the underlying technology, e.g. MPI programming of parallel computers that is needed for the software developments.