Enthalpies of formation and phase stability relations of USi, U3Si5 and U3Si2

Cheng Kai Chung, Xiaofeng Guo, Gaoxue Wang, Tashiema L. Wilson, Joshua T. White, Andrew T. Nelson, Anna Shelyug, Hakim Boukhalfa, Ping Yang, Enrique R. Batista, Artaches A. Migdisov, Robert C. Roback, Alexandra Navrotsky, Hongwu Xu

Research output: Contribution to journalArticlepeer-review

7 Scopus citations

Abstract

U–Si intermetallic compounds have drawn great attention due to their potential application as nuclear fuels. However, the thermodynamic properties and phase equilibria of this binary system from ambient to high temperature conditions are not fully understood. Via high temperature oxidative drop calorimetry and detailed characterization of the initial and final phases, we have experimentally determined the standard enthalpies of formation of USi and U3Si5.07 at 298 K to be −43.2 ± 6.2 and −43.8 ± 9.0 kJ/mol·atom, respectively. The energetics of the tetragonal USi (t-USi, space group I4/mmm) phase has also been calculated with Density Functional Theory (DFT) for the first time. Combining the obtained formation enthalpies with the heat capacities measured previously, we assessed the thermodynamic stability of t-USi relative to a phase assemblage of two other U–Si phases, U3Si5.07 and U3Si2, from ambient temperature to 1200 K. The tetragonal USi is thermodynamically more stable than U3Si5.07 + U3Si2, which supports previously published phase diagram (H. Okamoto and T. Massalski, 1990 [1]): specifically, at least one stable USi phase exists when the U content is 50 at.%. Further thermodynamic and phase equilibrium studies are needed for a more comprehensive understanding of the U–Si system across broader compositional and temperature ranges.

Original languageEnglish (US)
Pages (from-to)101-110
Number of pages10
JournalJournal of Nuclear Materials
Volume523
DOIs
StatePublished - Sep 2019
Externally publishedYes

Keywords

  • Calorimetry
  • Density functional theory
  • Intermetallics
  • Nuclear reactor fuel
  • Phase stability
  • Thermodynamic properties

ASJC Scopus subject areas

  • Nuclear and High Energy Physics
  • Materials Science(all)
  • Nuclear Energy and Engineering

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