In situ mechanochemistry: structure, thermodynamics, kinetics, and mechanisms

这个项目的目的是用原位分析从根本上描述机械化学反应和合成的机制、热力学和动力学。我们希望比以前更好地了解有机和有机体-滑石化合物的机械化学反应和合成。然后，机械化学反应可以被专门优化并有效地用于合成新的和已知的化合物。我们的实验方法的基础是一个原位设置，使我们能够在实际条件下使用组合x射线粉末衍射和拉曼光谱研究机械化学反应。通过分析可以了解反应的过程，并通过改变相关的实验条件（研磨频率、材料、磨球数等）来确定影响因素。晶体和非晶体中间体可以被检测和结构表征。为了定量测定稳态和瞬态反应物，需要建立拉曼光谱数据的多元分析。由于结构和热信息的结合有待开发，我们期望在知识方面有显著的收获。这是通过同时吸收斯托克斯线和反斯托克斯线来直接检测反应物的温度来实现的。另一方面是实现了直接测定反应焓的机械化学光度计。如果根据所获得的发现，机械化学可以作为一种绿色和可持续的合成方法得到更广泛的应用，这与化学、制药、环境科学和农业工业直接相关。

The aim of this project is to fundamentally describe the mechanisms, the thermodynamics and the kinetics of mechanochemical reactions and syntheses using in situ analytics. We want to gain a better understanding of the mechanochemical reactions and syntheses of organic and organome-tallic compounds than previously possible. Mechanochemical reactions can then be specifically optimized and efficiently used to synthesize new and known compounds.The basis of our experimental approach is an in situ setup that allows us to study mechanochemical reactions under real conditions using combined X-ray powder diffraction and Raman spectroscopy. This analysis provides insights into the course of the reaction and by altering relevant experimental conditions (grinding frequency, material and number of grinding balls, etc.) influencing factors can be identified. Crystalline and non-crystalline intermediates can be detected and structurally charac-terized. For the quantification of stationary and transient reactants the multivariate analysis of the Raman spectroscopic data shall be established. Due to the combination of structural and thermal information to be developed, we expect a significant gain in knowledge. This is to be achieved via the direct detection of the temperature of the reactants by the simultaneous uptake of the Stokes and anti-Stokes lines. Another aspect is the realization of a mechanochemical clarorimeter for the direct determination of the reaction enthalpy.If, based on the findings obtained, mechanochemistry can be used more broadly as a green and sustainable synthetic method this is directly relevant for chemistry, pharmacy, environmental sci-ences and the agricultural industry.