Estimating the Gibbs Hydration Energies of Actinium and Trans-Plutonium Actinides.

The use of actinides for medical, scientific and technological purposes has gained momentum in the recent years. This creates a need to understand their interactions with biomolecules, both at the interface and as they become complexed. Calculation of the Gibbs binding energies of the ions to biomolecules, i. e., the Gibbs energy change associated with a transfer of an ion from the water phase to its binding site, could help to understand the actinides' toxicities and to design agents that bind them with high affinities. To this end, there is a need to obtain accurate reference values for actinide hydration, that for most actinides are not available from experiment. In this study, a set of ionic radii is developed that enables future calculations of binding energies for Pu 3+ and five actinides with renewed scientific and technological interest: Ac 3+ , Am 3+ , Cm 3+ , Bk 3+ and Cf 3+ . Reference hydration energies were calculated using quantum chemistry and ion solvation theory and agree well for all ions except Ac 3+ , where ion solvation theory seems to underestimate the magnitude of the Gibbs hydration energy. The set of radii and reference energies that are presented here provide means to calculate binding energies for actinides and biomolecules.