Study On The Functional Theory Of The Isoelectronic System Of The Binding Of Actinides With Multi-chalcogenides

The molecular simulation and theoretical calculation of actinide complexes have been calculated by the quantum chemical calculation.Some of the molecular systems and their corresponding structural parameters which difficult received by experiments were obtained.The study of isoelectronic systems combining lanthanides with polychalcogens has become a hot topic in the moment.For example,the exploration of the highest oxidation number of lanthanides is also one of the current hot spots,and the kinetics of the peroxide form of actinides in organisms have also received much attention.In this paper,we first considered and selected a series of ground state structures of metal tetraoxides from energy,and found that the trends of different central metals under different defined charges were similar.Through the bond frequency analysis and LBO analysis,we found that the trends of the two kind parameters were consistent.The relationship of the 1s orbital energy between the oxidation state of each series of tetraoxides and the O atoms of ligands was also found by NAO analysis.In the series of molecules,when the lanthanide was in the high oxidation state,the bonding was no longer dependent on the 5f valence layer to lose electrons,but lost by the 6p orbital.To date,researches on the synthesis and functional application of uranyl-salophen have received much attention,while the studies on the independent chalcogen-substituted uranyl isoelectronic species and their complexes with salophen were still blank.In this paper,the existence of independent chalcogen-substituted uranyl isoelectronic species were explored by using DFT method and HF method of Guassian09 software,and the ground state structure of these molecules were found.The electronic structure,bond strength and type were discussed through natural population analysis,ELF analysis and NBO analysis.It was found that in these systems,U atoms formed covalent bonds with each chalcogen element,but with atomic number increased,the bond strength in these systems were lower.The LOBA method were also used to determine the oxidation state of each atom in independent chalcogen-substituted uranyl isoelectronic species,where in the U atom exhibits a positive hexavalent.It has also been found that the law of the electrophilic index obtained by orbit energy could be:UO₂²⁺<OUS²⁺<US₂²⁺<OUSe²⁺<SUSe²⁺?USe₂²⁺.From this series of results,it was found that the higher the total atomic number of the electrons of independent chalcogen-substituted uranyl isoelectronic species,the more difficult it was to exist alone.The relative changes in the overall structure of complexes formed by salophen and independent chalcogen-substituted uranyl isoelectronic species were measured using the root mean square deviation,and it was found that SUSe²⁺-salophen changed the most.Some quantitative properties of these molecules could be derived from molecular orbitals in order to explore a basis for drug identification.