Investigation of the thermal decomposition of Pu(IV) oxalate: a transmission electron microscopy study

Buck, Edgar C.; Reilly, Dallas D.; Sweet, Luke E.; Nicholas, Aaron D.; Heller, Forrest D.; Hall, Gabriel B.; Clark, Richard A.; Casella, Amanda J.

doi:10.3389/fnuen.2024.1380137

Title: Investigation of the thermal decomposition of Pu(IV) oxalate: a transmission electron microscopy study

Journal Article · 21 May 2024 · Frontiers in Nuclear Engineering

DOI: https://doi.org/10.3389/fnuen.2024.1380137 · OSTI ID:2352793

Buck, Edgar C.; Reilly, Dallas D.; Sweet, Luke E.; Nicholas, Aaron D.; Heller, Forrest D.; Hall, Gabriel B.; Clark, Richard A.; Casella, Amanda J.

The degradation of the internal structure of plutonium (IV) oxalate during calcination was investigated with Transmission Electron Microscopy (TEM), electron diffraction, Electron Energy-Loss Spectroscopy (EELS), and 4D Scanning TEM (STEM). TEM lift-outs were prepared from samples that had been calcined at 300°C, 450°C, 650°C and 950°C. The resulting phase at all calcination temperatures was identified as PuO ₂ with electron diffraction. The grain size range was obtained with high-resolution TEM. In addition, 4D STEM images were analyzed to provide grain size distributions. In the 300°C calcined sample, the grains were <10 nm in diameter, at 650°C, the grains ranged from 10 to 20 nm, and by 950°C, the grains were 95–175 nm across. Using the Kolmogorov-Smirnov (K-S) two sample test, it was shown that morphological measurements obtained from 4D-STEM provided statistically significant distributions to distinguish samples at the different calcination conditions. Using STEM-EELS, carbon was shown to be present in the low temperature calcined samples associated with oxalate but had formed carbon (possibly graphite) deposits in the 950°C calcined sample. This work highlights the new methods of STEM-EELS and 4D-STEM for studying the internal structure of special nuclear materials (SNM).

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Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

OSTI ID:: 2352793

Alternate ID(s):: OSTI ID: 2367450

Journal Information:: Frontiers in Nuclear Engineering, Journal Name: Frontiers in Nuclear Engineering Vol. 3; ISSN 2813-3412

Publisher:: Frontiers Media SACopyright Statement

Country of Publication:: Switzerland

Language:: English

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