Computational chemistry studies of actinide complexes

NUCL 17

David A. Dixon, dadixon@bama.ua.edu, Keith E. Gutowski, gutow001@bama.ua.edu, Shenggang Li, sli@bama.ua.edu, Raluca Craciun, raluca.craciun@gmail.com, Virgil Jackson, vejackson@gmail.com, and Kathryn Tippey. Department of Chemistry, The University of Alabama, Box 870336, Shelby Hall, Tuscaloosa, AL 35487-0336
We will describe the calculation of the properties of complexes containing actinides by using density functional theory with the B3LYP functional and molecular orbital theory with a correlation treatment at the MP2 level. The prediction of the equilibrium constant for the reaction UO2(H2O)42+ + H2O °ê UO2(H2O)52+ in aqueous solution will be described. The calculations were done at the MP2 level including part of the second solvent shell and a continuum model for the rest of the solution. The calculated value of -2.0 kcal/mol is in good agreement with the experimental value of -1.2 1.2 ± 0.4 kcal/mol. We will describe the calculation of the number of H2O molecules in the 1st solvation shell for Th4+. We will describe calculations of the interaction of UO22+ with imidazole as a model for binding to amino acids. We will describe the interaction of UO22+ with phosphate and silicate groups with differing charges.