Journal Article

·2016 OPEN ACCESS

Modeling Superionic Behavior of Plutonium Dioxide

Seçkin D. Günay YTU , Berna Akgenç YTU , Çetin Taşseven YTU

High Temperature Materials and Processes

Abstract

Abstract The Bredig transition to the superionic phase indicated with the $$\lambda $$ -peak in $${C_p}$$ was highly expected for plutonium dioxide ( $${\rm{Pu}}{{\rm{O}}_2}$$ ) as other actinide dioxides. However, least-square fit and local smoothing techniques applied to the experimental enthalpy data of PuO 2 in 1980s could not detect a $$\lambda $$ -peak in specific heat that might be due to too scattered and insufficient experimental data. Therefore, this issue has not been yet put beyond the doubts. In the current article, a superionic model of $${\rm{Pu}}{{\rm{O}}_2}$$ is developed with partially ionic model of a rigid ion potential. Thermophysical properties were calculated in constant pressure–temperature ensemble using molecular dynamics simulation. The Bredig transition with vicinity of a $$\lambda $$ -peak in specific heat was successfully observed for the model system at about 2,100 K. Moreover, the experimental enthalpy change was well reproduced before and after the estimated transition temperature.

Keywords

Thermodynamics Enthalpy Ionic bonding Lambda Phase transition Plutonium Diffusion Actinide Ion Chemistry Heat capacity Materials science Physics Inorganic chemistry Quantum mechanics

Subject Areas

Nuclear Materials and Properties ·Materials Chemistry ·Physical Sciences
Radioactive element chemistry and processing ·Inorganic Chemistry ·Physical Sciences
Nuclear reactor physics and engineering ·Aerospace Engineering ·Physical Sciences

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