From Criegee-Intermediates to particle size distributions. Precursor chemistry and aggregation kinetics of sulfuric acid containing clusters in experiment and simulation

Criegee中间体或羰基氧化物与二氧化硫反应形成三氧化硫和羰基化合物是硫酸的重要大气来源。Criegee中间体在烯烃臭氧化过程中通过初级臭氧化物的分解而产生。在这个项目中遵循的方法可以允许检测的原则上所有Criegee中间体在气相中通过红外光谱在时间分辨实验与高反应物浓度。到目前为止，替代方法仅限于低压和小物种。 在我们的研究框架内，应提供动力学数据，这是评估Criegee反应与二氧化硫的大气影响所需的。在二氧化硫存在下的2-丁烯臭氧分解允许在动力学控制实验中产生高浓度的硫酸。我们将利用这一特性来研究硫酸诱导新粒子形成的动力学。

The reaction of Criegee intermediates or carbonyl oxides with sulphur dioxide forming sulphur trioxide and a carbonyl compound is an important atmospheric source of sulphuric acid. Criegee intermediates are produced during alkene ozonolysis by the decomposition of the primary ozonide. The approach followed in this project may allow the detection of in principle all Criegee intermediates in the gas-phase by infrared spectroscopy in time resolved experiments with high reactant concentrations. Alternative methods have been so far restricted to low pressure and small species. In the framework of our studies the kinetic data shall be provided, which are needed to assess the atmospheric influence of the Criegee reaction wit sulphur dioxide. The 2-butene ozonolysis in the presence of sulphur dioxide allows producing high sulphuric acid concentrations in a kinetically controlled experiment. This property we will exploit to study the dynamics of sulphuric acid induced new particle formation.