Thermodynamic studies of studtite thermal decomposition pathways via amorphous intermediates UO3, U2O7, and UO4

Xiaofeng Guo, Di Wu, Hongwu Xu, Peter C. Burns, Alexandra Navrotsky

Research output: Contribution to journalArticlepeer-review

22 Scopus citations

Abstract

The thermal decomposition of studtite (UO2)O2(H2O)2·2H2O results in a series of intermediate X-ray amorphous materials with general composition UO3+x (x = 0, 0.5, 1). As an extension of a structural study on U2O7, this work provides detailed calorimetric data on these amorphous oxygen-rich materials since their energetics and thermal stability are unknown. These were characterized in situ by thermogravimetry, and mass spectrometry. Ex situ X-ray diffraction and infrared spectroscopy characterized their chemical bonding and local structures. This detailed characterization formed the basis for obtaining formation enthalpies by high temperature oxide melt solution calorimetry. The thermodynamic data demonstrate the metastability of the amorphous UO3+x materials, and explain their irreversible and spontaneous reactions to generate oxygen and form metaschoepite. Thus, formation of studtite in the nuclear fuel cycle, followed by heat treatment, can produce metastable amorphous UO3+x materials that pose the risk of significant O2 gas. Quantitative knowledge of the energy landscape of amorphous UO3+x was provided for stability analysis and assessment of conditions for decomposition.

Original languageEnglish (US)
Pages (from-to)158-163
Number of pages6
JournalJournal of Nuclear Materials
Volume478
DOIs
StatePublished - Sep 1 2016
Externally publishedYes

Keywords

  • Calorimetry
  • Enthalpy of formation
  • Nuclear fuel alteration
  • Studtite
  • UO

ASJC Scopus subject areas

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

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