Molecular metal siloxides as models for functional units of oxidic frameworks and surfaces

该项目的目标是分子化合物的合成和研究，这些化合物可以模拟在具有高丰度和应用相关性的氧化物表面上发生的结构单元;具体地说，氧化铝/氢氧化物，氧化铁和铝硅酸盐是重点，在铝硅酸盐的情况下，特别注意金属改性变体。用于构建分子的硅氧配体将适合氧化物/氢氧化物聚集体的捕获和稳定以及硅酸盐环境的模拟。一方面，对这些化合物的研究应该有助于对相应单元的行为（例如与水接触）进行基本的原子尺度的理解。水普遍存在于上述材料的合成、溶解和应用过程中，阐明其作用机理具有重要的基础意义。另一方面，设想使作为硅酸盐材料（特别是金属改性的沸石）的一部分表现出令人感兴趣的反应性的功能单元可接近并可用于溶液中的化学研究和应用。在开发相应的表面激发分子之后，将测试激活双氧或O原子转移试剂的潜力，以最终实现烃的氧官能化;因此，另一个目标是开发新型功能分子。在沸石类反应性的情况下，分子化学固有的方法的应用也可以揭示机制信息，促进对在固态材料的情况下观察到的反应性的理解。根据选择的材料选择为分子合成的指导，该项目将处理铝，铜，镍和铁的氧化物。

The target of this project is the synthesis and investigation of molecular compounds, which can mimic structural units occurring on the surfaces of oxides with high abundance and application relevance; concretely, aluminium oxides/hydroxides, iron oxides and aluminosilicates are in the focus, in case of the aluminosilicates special attention is on metal-modified variants. The siloxide ligands used for the construction of the molecules will suit the trapping and stabilization of oxide/hydroxide aggregates as well as the simulation of silicate environments. The investigation of such compounds on the one hand is supposed to contribute to a fundamental, atomic-scale understanding of the behavior of corresponding units, for instance in contact with water. Water is ubiquitous during the synthesis, dissolution and application of the mentioned materials and the elucidation of the corresponding mechanisms is of basic significance. On the other hand it is envisaged to make functional units, which exhibit interesting reactivities as part of silicate materials (in particular metal-modified zeolites), accessible and utilizable for chemical investigations and applications in solution. Subsequent to the development of corresponding surface-inspired molecules the potential to activate dioxygen or O-atom transfer reagents will be tested to finally achieve the oxyfunctionalisation of hydrocarbons; accordingly, a further goal is the development of novel functional molecules. In case of zeolite-like reactivities the application of the methods inherent to molecular chemistry can also reveal mechanistic information that advances the understanding of reactivities observed in case of the solid-state materials. According to the selection of materials chosen as guides for molecular synthesis the project will deal with aluminium, copper, nickel, and iron siloxides.