We utilized first-principles density-functional-theory (DFT) calculations to evaluate the thermodynamic feasibility of a pyroprocessing methodology for reducing the volume of high-level radioactive materials and recycling spent nuclear fuels. The thermodynamic properties of transuranium elements (Pu, Np and Cm) were obtained in electrochemical equilibrium with a LiCl-KCl molten salt as ionic phases and as adsorbates on a W(110) surface. To accomplish the goal, we rigorously calculated the double layer interface structures on an atomic resolution, on the thermodynamically most stable configurations on W(110) surfaces and the chemical activities of the transuranium elements for various coverages of those elements. Our results indicated that the electrodeposition process was very sensitive to the atomic level structures of Cl ions at the double-layer interface. Our studies are easily expandable to general electrochemical applications involving strong redox reactions of transition metals in non-aqueous solutions.
Bibliographical noteFunding Information:
The Nuclear R & D Program funded by the Ministry of Science, ICT & Future Planning (2011-0031839) supported this research. This work was supported by the Global Frontier R&D Program (2013-2013078882) on the Center for Hybrid Interface Materials (HIM) funded by the Ministry of Science, ICT & Future Planning. The Authors also thank the Leading Foreign Research Institute Recruitment Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Education, Science and Technology (MEST) (2012K1A4A3053565).
All Science Journal Classification (ASJC) codes
- Physics and Astronomy(all)