Using first principles simulations to develop catalysts for the next generation of clean energy technologies

催化是许多现代清洁能源技术的核心，如燃料电池和汽车催化剂，贵金属中的金属纳米颗粒被用作催化剂。一个主要的研究挑战是找到减少每个设备中使用的贵金属重量的方法，同时最大限度地提高其活性和寿命。计算化学在这个领域扮演着重要的角色。诸如第一性原理量子力学计算之类的方法可以用来模拟纳米粒子的电子特性和结构，以及它们表面发生的化学反应。这样的模拟可以在电子和原子层面上提供独特的见解，可以用来理解如何开发更好的催化剂。工业上相关的金属纳米颗粒由数百到数千个原子组成。随着计算量子理论的最新进展，如Skylaris教授小组开发的ONETEP计划中的方法，在超级计算机上模拟如此大量的金属原子开始成为可能。使用这种方法，我们将有机会首次在1-10nm的重要纳米颗粒尺寸范围内建立化学反应模型，从“纳米颗粒”到“大块金属”的转变发生。这个博士项目将包括使用模拟来研究和理解金属纳米颗粒的大小、形状和表面如何影响关键催化过程中涉及的小分子的吸附。随后，在工业上重要的催化循环中，纳米颗粒表面的化学反应，如燃料电池中的氧还原反应，将被研究。这将使我们了解反应物与纳米粒子的电子相互作用如何导致特定的反应机制，并获得可用于设计更好的催化剂的信息。环境，如纳米粒子固定的表面，溶剂，对纳米粒子的电子特性有很强的影响，也需要使用合适的多尺度模拟方法进行研究。本项目还将涉及一些方法开发，以增强将要使用的模拟技术。

Catalysis is at the core of many modern clean energy technologies such as fuel cells and automotive (car) catalysts, and metallic nanoparticles from precious metals are used as catalysts. A major research challenge is to find ways to reduce the weight of precious metal used in each device while at the same time maximising its activity and lifetime. Computational chemistry has a big role to play in this area. Methods such as first principles quantum mechanical calculations can be used to simulate the electronic properties and structure of nanoparticles and the chemical reactions that take place on their surfaces. Such simulations can provide unique insights at the level of electrons and atoms which can be used to understand how to develop better catalysts. Industrially relevant metallic nanoparticles consist of hundreds to thousands of atoms. Such large numbers of metal atoms are beginning to be possible to simulate on supercomputers with recent advances in computational quantum theory such as the methods within the ONETEP program which is developed in the group of Professor Skylaris. Using this approach we will have the opportunity to model for the first time chemical reactions in the important nanoparticle size regime of 1-10nm where the transition from "nanoparticle" to "bulk metal" occurs. This PhD project will involve using simulations to investigate and understand how the size, shape, and surface of metallic nanoparticles affect the adsorption of small molecules that are involved in key catalytic processes. Subsequently chemical reactions on the surface of the nanoparticles in industrially important catalytic cycles, such as the oxygen reduction reaction in fuel cells, will be investigated. This will allow us to understand how the electronic interaction of the reactants with the nanoparticle results in particular reaction mechanisms, and to obtain information that can be used to design better catalysts. The environment, such as the surface on which the nanoparticle is anchored, and the solvent, has a strong effect on the electronic properties of the nanoparticle and will also need to be investigated using suitable multiscale simulation approaches. Some method development will also be involved in this project to enhance the simulation techniques that will be used.