Quantitative Microstructural Characterization of Plutonium Oxalate Auto‐Degradation and Evidence for PuO 2 Nanocrystal Formation

Corbey, Jordan F.; Sweet, Lucas E.; Sinkov, Sergey I.; Reilly, Dallas D.; Parker, Cyrena M.; Lonergan, Jason M.; Johnson, Timothy J.

doi:10.1002/ejic.202100511

Quantitative Microstructural Characterization of Plutonium Oxalate Auto‐Degradation and Evidence for PuO ₂ Nanocrystal Formation

Journal Article · Wed Jul 21 00:00:00 EDT 2021 · European Journal of Inorganic Chemistry

DOI:https://doi.org/10.1002/ejic.202100511· OSTI ID:1808901

^[1]; Sweet, Lucas E. ^[1]; Sinkov, Sergey I. ^[1]; Reilly, Dallas D. ^[1]; Parker, Cyrena M. ^[1]; Lonergan, Jason M. ^[1]; Johnson, Timothy J. ^[1]

Pacific Northwest National Laboratory 902 Battelle Boulevard Richland, WA 99352 USA

Abstract

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.

View Accepted Manuscript (Publisher)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1808901

Alternate ID(s):: OSTI ID: 1820043

Journal Information:: European Journal of Inorganic Chemistry, Journal Name: European Journal of Inorganic Chemistry Journal Issue: 32 Vol. 2021; ISSN 1434-1948

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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Quantitative Microstructural Characterization of Plutonium Oxalate Auto‐Degradation and Evidence for PuO ₂ Nanocrystal Formation