Journal
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
Volume 2021, Issue 32, Pages 3277-3291Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/ejic.202100511
Keywords
Aging study; Nanostructures; Nuclear chemistry; Plutonium; Structure elucidation
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Funding
- Laboratory Directed Research and Development (LDRD) Program
- Nuclear Process Science Initiative (NPSI) at Pacific Northwest National Laboratory (PNNL)
- U.S. Department of Energy (DOE) [DE-AC05-76RL01830]
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This study presents a comprehensive analysis of time-resolved powder X-ray diffraction experiments, solid-state optical spectroscopy, and electron microscopy of aged plutonium oxalate powders. The data provide new insights into the chemical and structural changes that occur in these solids over time at room temperature, suggesting the auto-decomposition of plutonium oxalates to form nanocrystalline plutonium oxide.
It has been known since the 1950s that plutonium oxalate powders change color and lose mass over time when stored at room temperature in air. Despite several studies monitoring these changes, there are still discrepancies in the literature regarding the speciation of intermediate and final products that result from this decomposition. Presented here for the first time is a comprehensive series of time-resolved powder X-ray diffraction experiments coupled with solid-state optical spectroscopy and electron microscopy of aged plutonium (III) and (IV) oxalate powders. These data provide fresh insight into the chemical and structural changes that occur in these solids over time at room temperature and represent new evidence suggesting both plutonium (III) and plutonium (IV) oxalates auto-decompose to form nanocrystalline plutonium oxide in the solid state.
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