Electroactive MOF Networks

电活性MOF网络

• 批准号: 316670871
• 负责人: Professor Dr. Thomas Bein
• 金额: --
• 依托单位: Computer-Chemie-Centrum (CCC)
• 依托单位国家: 德国
• 项目类别: Priority Programmes
• 资助国家: 德国
• 项目状态: 未结题
• 来源: https://gepris.dfg.de/gepris/projekt/316670871?language=en
• 关键词: Electroactive; MOF; Networks

Here, we aim to develop metalorganic frameworks with periodic, interpenetrating networks of electron donor- and acceptor-phases that give maximum control over the nature of the molecular building blocks with specific electronic properties, their sequence of assembly, their spatial orientation relative to each other, their wall-thickness, and their overall orientation relative to a substrate. We build such highly defined model systems based on MOF structures, to enhance our understanding of the relationship between the electronic and structural parameters and the resulting optoelectronic properties, including charge-carrier dynamics. In one line of research, we wish to synthesize MOFs with different stacked (hetero)aromatic electron donor- and acceptor moieties, thus forming highly ordered (interpenetrating) networks for light-induced charge separation and photodetection. A second line of research is based on the structural paradigm of the MOF-74 topology, in which linear building blocks are connected into honeycomb-like structures through coordination of divalent metal ions. Here, we will vary both the structural and electronic properties of the metal coordination sphere and of the linear building blocks. Moreover, we introduce a strategy to partition the electronically coupled pore systems through Kagome-like tiling in order to protect charge carriers from recombination and to increase their lifetimes. Complementary charge-carrier phases will be introduced into the MOF host structures through inclusion chemistry. Building blocks include extended heterocyclic chromophores with push-pull elements to tune optoelectronic properties, and twisted systems with potential singlet/triplet conversion control for MOF-based light-emitting diodes. Furthermore, we aim to develop film-growth techniques based on different deposition strategies for oriented MOF- and heteroepitaxial MOF-MOF structures, ultimately to be integrated into model photovoltaic devices, photodetectors and MOF-LEDs, and to study their detailed charge-carrier dynamics with a wide range of techniques and in collaboration with other research groups. The work will be complemented with powerful theoretical modeling, addressing optimized structure and packing of the molecular building blocks, advanced electronic property calculations of the MOFs, charge transport calculations and conductance-path searches to determine limiting factors and optimization strategies, as well as morphology prediction for the growth of thin films.

在这里，我们的目标是开发具有周期性的、由电子给体和受体相组成的互穿网络的金属有机骨架，这些骨架可以最大限度地控制具有特定电子性质的分子构建块的性质、它们的组装顺序、它们相互之间的空间取向、它们的壁厚以及它们相对于底物的整体取向。我们建立了基于MOF结构的高度定义的模型系统，以加强我们对电子参数和结构参数与由此产生的光电性质之间的关系的理解，包括电荷-载流子动力学。在一系列研究中，我们希望合成具有不同堆积(杂化)芳香族电子给体和受体基团的MOF，从而形成用于光诱导电荷分离和光检测的高度有序(互穿)网络。第二条线是基于MOF-74拓扑的结构范式，其中线性积木通过二价金属离子的配位连接成蜂窝状结构。在这里，我们将改变金属配位球和线性积木的结构和电子性质。此外，我们引入了一种策略，通过Kagome类瓦片来划分电子耦合的孔道系统，以保护电荷载流子不会复合，从而延长它们的寿命。互补载流子相将通过包裹体化学引入MOF主体结构中。构建块包括扩展的杂环发色团，具有推挽元件以调整光电性能，以及具有潜在的单态/三态转换控制的扭曲系统，用于基于MOF的发光二极管。此外，我们的目标是开发基于不同沉积策略的定向MOF和异质外延MOF-MOF结构的薄膜生长技术，最终集成到模型光伏器件、光电探测器和MOF-LED中，并通过广泛的技术和与其他研究小组的合作来研究它们的详细电荷-载流子动力学。这项工作将辅之以强大的理论建模，解决分子构建块的优化结构和堆积，先进的MOF电子性质计算，电荷传输计算和电导路径搜索，以确定限制因素和优化策略，以及薄膜生长的形态预测。