Supercharging Metal-Organic Frameworks (SuperMOF)

电荷载流子的产生、传输和寿命是所有清洁能源技术中材料应用的基础。固体的氧化和还原行为决定了电子和空穴是否可以在太阳能电池中分离和收集，是否会发生给定的太阳能燃料反应，或者电荷是否可以在电池或超级电容器中存储并随后释放。虽然无机和有机化合物的氧化还原特性的工程规则已经建立，但混合有机-无机固体代表了本项目将探索的新前沿。在混合材料中组合两种不同组分的灵活性提供了无限数量的化学和结构可能性。然而，还没有建立系统的方法来设计与特定电子标准相匹配的组合物和配置。我将专注于金属有机框架（MOFs）的基础上有序的，往往是多孔的，结构。MOF构建块和拓扑结构的多样性为跨多个维度设计电荷转移途径提供了巨大的化学空间。SuperMOF将牢固地建立MOF的氧化还原化学。我将采用尖端的材料建模技术，包括大规模框架的电子结构模拟，以：（i）开发一种新的氧化还原理论，描述MOFs的独特行为;（ii）构建工程电子迁移率和电导率的设计原则;（iii）模型MOF光化学，包括太阳能设备中的异质界面。与正在进行的实验活动有着密切的联系，以确保我的预测得到快速验证和测试。其结果将是对材料化学新领域的深刻理解，为氧化还原活性框架的新家族开发工程原理，以及支持计算材料化学前沿的研究小组。

The generation, transport, and lifetime of charge carriers is fundamental to the application of materials across all clean energy technologies. The oxidation and reduction behaviour of solids determines whether electrons and holes can be separated and collected in a solar cell, if a given solar fuel reaction will occur, or whether charge can be stored and later released in a battery or supercapacitor. While the rules for engineering the redox properties of inorganic and organic compounds are well established, hybrid organic-inorganic solids represent a new frontier that this project will explore. The flexibility of combining two distinct components in hybrid materials provides an infinite number of chemical and structural possibilities. However, there is no systematic approach established for designing compositions and configurations that match specific electronic criteria. I will focus on metal-organic frameworks (MOFs) based on ordered, and often porous, structures. The diversity of MOF building blocks and topologies provides access to an immense chemical space for engineering charge transfer pathways across multiple dimensions. SuperMOF will firmly establish the redox chemistry of MOFs. I will employ cutting-edge materials modelling techniques, including electronic structure simulations of massive frameworks, to: (i) develop a new redox theory that describes the unique behaviour of MOFs; (ii) construct design principles for engineering electron mobility and conductivity; (iii) model MOF photochemistry including heterointerfaces in solar energy devices. There are strong links with ongoing experimental activity to ensure rapid validation and testing of my predictions. The outcome will be a deep understanding of a new field of materials chemistry, the development of engineering principles for novel families of redox-active frameworks, and the support of a research group at the forefront of computational materials chemistry.