| The dissertation mainly consists of three parts:the study about stability and pyrolysis mechanism of KFn-, KFn and KFnn+series, CaFn-, CaFn and CaFn+series fluorine compounds separately, and the comparison between these two series fluorine compounds.In the first chapter, the current research of hyperhalogens, the application and development of41Ca-AMS (accelerator mass spectrometry) technology were summarized and introduced. The theoretical methods and principles were introduced in this dissertation concisely. At last, the research contents in this dissertation were introduced briefly.In chapter two, the stable geometries of KFn-, KFn+fluorine compounds and their neutral counterparts KFn (n=1-4) were optimized firstly. Then the VDE (vertical detachment energies) of KFn-and the EAvert (vertical electron affinities), EAad (adiabatic electron affinities) of KFn, KFn+were calculated at the same level. The thermodynamics energy changes of all the possible pyrolysis reactions of these compounds were calculated, and obtained the lowest energy pathways finally. Moreover, the ionization dissociation energy changes of KFn-compounds were calculated and analyzed. In order to research the isotope effect, the VDE, EAvert, EAad and thermodynamics energy changes of41KFn-,41KFn and41KFn+(n=1-4) were calculated at the same time. The properties of dynamic about these fluorine compounds were investigated at last.In the third chapter, the equilibrium geometries of CaFn-, CaFn and CaFn+(n=1-4) series fluorine compounds were optimized at first. Then the VDE, EAvert and EAad were calculated. Meanwhile, the thermodynamics energy changes of all the possible pyrolysis reactions of these compounds were calculated. And the ionization dissociation energy changes of CaFn-fluorine compounds were also calculated and analyzed. In addition, the VDE, EAvert and EAad of41CaFn-,41CaFn and41CaFn+(n=1-4) were calculated, and the results were compared with the thermodynamics energy changes of CaFn-, CaFn and CaFn+series of compounds. Finally, the properties of dynamic about these fluorine compounds were also researched and analyzed.The last chapter mainly about the calculation and analysis of the thermodynamics properties of K and Ca series fluorine compounds. First, the energy changes between the pyrolysis and ionization dissociation of KFn-and KFn (n=1-4) series compounds were calculated and analyzed. Then the energy changes between the pyrolysis and ionization dissociation of CaFn-and CaFn (n=1-4) series compounds were calculated samely. At last, the pyrolysis and ionization dissociation energy changes of KFn-, KFn, KFn+and CaFn-, CaFn, CaFn+series compounds were compared and analyzed respectively. |
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