Supercharging Metal-Organic Frameworks (SuperMOF)

电荷载流子的产生、传输和寿命是材料在所有清洁能源技术中应用的基础。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，或者电荷是否可以存储并稍后在电池或超级电容器中释放。虽然设计无机和有机化合物的氧化还原性能的规则已经确立，但有机-无机杂化固体代表了这个项目将探索的一个新的前沿。在混合材料中结合两种不同成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符合特定电子标准的成分和配置。我将专注于金属有机骨架(MOF)，它基于有序的、通常是多孔的结构。MOF构建块和拓扑的多样性为跨越多个维度的工程电荷转移路径提供了巨大的化学空间。超级MOF将牢固地建立MOF的氧化还原化学。我将使用尖端材料模拟技术，包括大规模框架的电子结构模拟，以：(I)开发描述MOF独特行为的新的氧化还原理论；(Ii)构建工程电子迁移率和导电性的设计原则；(Iii)模型MOF光化学，包括太阳能器件中的异质界面。这与正在进行的实验活动有很强的联系，以确保我的预测得到快速验证和测试。其成果将是对材料化学的一个新领域的深刻理解，为氧化还原活性骨架的新家族开发工程原理，以及一个处于计算材料化学前沿的研究小组的支持。

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.