AMICI: Amorphous Microstructure Imaging at Composite Interfaces in Metal-Organic Frameworks

减少排放需要在分离（取代能源密集型蒸馏）、燃料电池（使用耐用、低成本的膜）和高效照明（封装卤化物钙钛矿）方面取得进展，所有这些都依赖于对化学传输的有效控制。金属有机框架（MOFs）由有机分子在特征多孔网络中连接的金属节点组成，如果我们能够利用它们的结构和化学选择性，它将有望加速节能。然而，设备集成具有挑战性。大多数情况下制备为结晶粉末，将MOFs与由其他MOFs制成的聚合物或玻璃融合，形成与设备兼容的形式。反过来，界面相互作用促进气体吸收、质子传导性和发光。然而，定义非周期性结构仍然没有得到解决。该项目将通过确定无定形组分的原子结构、晶体的畸变和界面的变化来揭示MOF复合材料的微观结构多样性。我雄心勃勃的研究计划将建立一种纳米级版本的技术，即使用扫描透射电子显微镜对MOF/MOF、MOF/聚合物和MOF/钙钛矿复合材料进行电子对分布函数分析。现在，我将结合低温、低剂量显微镜和旋进电子光学，进行直接的显微镜观察，以回答有关MOF如何熔化和形成玻璃、客体分子如何穿过MOF以及分子如何穿过MOF/聚合物膜的问题。再加上动态和多尺度显微镜，我将联合收割机这些工具来跟踪模型燃料电池膜中的水传输。只有通过开发非晶微结构的纳米分辨成像（界面上的域大小，形状，组成和原子结构描述符），才有可能确定精确的结构-功能关系，并合理设计主客体和基质-填料相互作用，以实现MOF技术的潜力。

Reducing emissions requires advances in separations (replace energy-intensive distillations), fuel cells (use robust, low-cost membranes), and high-efficiency lighting (encapsulate halide perovskites), all relying on efficient control of chemical transport. Metal-organic frameworks (MOFs), consisting of metal nodes linked by organic molecules in characteristically porous networks, are poised to accelerate energy savings if we can harness their structural and chemical selectivity. Yet device integration is challenging. Most often prepared as crystalline powders, fusing MOFs with polymers or glasses made from other MOFs creates device-compatible forms. In turn, interfacial interactions boost gas uptake, proton conductivity, and luminescence. However, the defining non-periodic structures remain unresolved. This project will unveil the microscopic structural variety in MOF composites by determining the atomic structure of amorphous components, distortions in crystals, and changes at interfaces.My ambitious research programme will build a nanoscale version of the technique known as electron pair distribution function analysis for MOF/MOF, MOF/polymer, and MOF/perovskite composites using scanning transmission electron microscopy. Now uniting cryogenic, low-dose microscopy and precession electron optics, I will make direct microscopic observations to answer questions on how MOFs melt and form glasses, how guest molecules move through MOFs, and how molecules traverse MOF/polymer membranes. Together with dynamic and multi-scale microscopies, I will combine these tools to track water transport in a model fuel cell membrane. Only through developing nanometre-resolved imaging of amorphous microstructure (domain size, shape, composition, and atomic structure descriptors across interfaces) will it be possible to determine precise structure-function relationships and rationally design host-guest and matrix-filler interactions to realise the potential of MOF technologies.