The Study Of The Dissociative Photoionization Of Ethyl Acrylate And The Reaction Of CH₂OO Radical With O₃

This paper describes the application of vacuum ultraviolet synchrotron radiation single-photon ionization method to the research of the photoionization dissociation of ethyl acrylate and the pre-study of the ozonolysis reaction of CH2OO.First we can get the mass spectrometry under different energieswith TOF technology, the appearance energies (AE) of different peaks can also be achieved by scanning photoionization efficiencies of different ions, and then the chemical composition of the main peaks of the ions and their molecular structures can be obtained combined with the quantum chemical calculation method, the different dissociation pathways that the parent ions experienced are also determined. Finally, the studies of Criegee radicals is reviewed and the tendency of it’s study in the future is also discussed, as well as the preparation of our laboratory for the research of this kind of free radicals.In this thesis, there are four chapters in total, the contents of each chapter as follows:In the first chapter, the synchrotron radiation and our experiment station(atomic and molecular physics) are introduced. Including the principle and the development process of synchrotron radiation, advantages and features. The system performance of HLS, as well as the beam line (both the structure of atomic and molecular physics beamline and the application of filter) for the completion of this article is also presented.The second chapter shows an overview of the theoretical calculation of quantum chemistry methods. Including ab initio methods, semi-empirical molecular orbital method, density functional theory methods and electron correlation, additionally, each type of calculation method is given in detail. What’s more, a brief review of the development process of the theoretical calculation methods is presented. And the calculation method used herein is explained in detail.In the third chapter, the study of ethyl acrylate (EA) by the VUV ionization is discussed. With the application of photoionization mass spectrometry (PIMS), in the energy range of9.0-20.0eV, we carry out a research on the photoionization dissociation of EA. The ionization energy of EA and the AE of major fragment ions can be obtained by their PIE curves. Based on the experimental results, the dissociation photoionization channels are put forward.The fourth chapter describes the research progress of the Criegee radicals, especially the previous researches of the ozonolysis reaction of CH2OO. Firstly,making a brief summary on the formation mechanism of Criegee intermediates, secondly, the generation process and the related reactions involved in the experiments are also reviewed, and the theoretical studieson the reactions of this kind of intermediate are also introduced. We also make an introduction of the equipment of our laboratory for the study of free radicals. Finally, the tendency of the study of CI in the future is also discussed.