First-principles calculations of the thermodynamic properties of transuranium elements in a molten salt medium

• Published in: Journal of the Korean Physical Society Vol. 64; no. 6; pp. 806 - 812
• Main Authors: Noh, Seunghyo, Kwak, Dohyun, Lee, Juseung, Kang, Joonhee, Han, Byungchan
• Format: Journal Article
• Language: English
• Published: Seoul The Korean Physical Society 01.03.2014; 한국물리학회
• Subjects: Mathematical and Computational Physics; Particle and Nuclear Physics; Physics; Physics and Astronomy; Theoretical; 물리학; Recycling spent nuclear fuels; Density functional theory; First principles; Pyroprocess; Molten salt
• ISSN: 0374-4884; 1976-8524
• DOI: 10.3938/jkps.64.806

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.