Ab Initio Molecular Dynamics Study, the Reaction Mechanism and Topological Properties of the Microscopic Interaction of PuO2 and H2O

Abstract

AbstractDensity functional theory (DFT) and transition state theory(TST) were used to study the interaction between PuO2 and H2O. Firstly, we considered all possible spin states. The wave function was tested and optimized to get a stable configuration, and a minimal energy path(MEP) was derived so that the internuclear separations and interaction energy can be reasonably evaluated. Moreover, various topological analysis methods were used to investigate the changes in bonds during the interaction process. The localized orbital bonding analysis (LOBA) method was used to study the changes in the valence state of the product. The density of states diagram was drawn to analyze the contribution of 5 f orbital in the reaction process. And with the help of natural bond orbit (NBO) analysis, the bond orbit information was described. Finally, the reaction rate constant was calculated using the variational transition state theory (VTST). The current research provides necessary theoretical data support for the follow‐up related theoretical experimental research.