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

本项目的目的是利用原位分析从根本上描述机械力化学反应和合成的机理、热力学和动力学。我们想要比以前更好地了解有机和有机金属化合物的机械力化学反应和合成。我们的实验方法的基础是一个原位装置，它允许我们使用X射线粉末衍射和拉曼光谱相结合的方法来研究真实条件下的机械力化学反应。这种分析提供了对反应过程的洞察，并通过改变相关的实验条件(研磨频率、材料和研磨球的数量等)。可以确定影响因素。可以检测到晶态和非晶态中间体，并对其进行了结构表征。对于静态和暂态反应物的定量，应建立拉曼光谱数据的多变量分析。由于结构和热信息的结合有待开发，我们预计知识将显著增加。这将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。另一个方面是实现机械化学色谱计直接测定反应热，如果根据所获得的结果，机械力化学作为一种绿色和可持续的合成方法可以得到更广泛的应用，这与化学、制药、环境科学和农业直接相关。

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.