AUTHOR=Villa-Aleman Eliel , Darvin Jason R. , Dick Don D. , Maxwell Michael C. , Swindle Ashlee R. , Foley Bryan J. 

TITLE=Spectroscopic analysis of Pu-bearing compounds in double-walled cells

JOURNAL=Frontiers in Nuclear Engineering

VOLUME=3

YEAR=2024

URL=https://www.frontiersin.org/journals/nuclear-engineering/articles/10.3389/fnuen.2024.1355374

DOI=10.3389/fnuen.2024.1355374

ISSN=2813-3412

ABSTRACT=<p>Spectroscopic analysis of radiological materials has been historically limited to radiological labs with older or less advanced scientific instrumentation. The development of double-walled cells (DWCs) at the Savannah River National Laboratory (SRNL) has enabled Pu-bearing compounds to be removed from radiological laboratories and studied in our radiologically clean spectroscopy laboratory with state-of-the-art instrumentation. In this manuscript, we discuss the contributions of DWCs that have allowed the application of Raman spectroscopy, diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), diffuse reflectance spectroscopy (DRS) in the shortwave infrared, and gamma spectroscopy at SRNL. Significant advances have been made in the understanding of the thermal decomposition of Pu(III) and Pu(IV) oxalates, alpha-induced damage to the PuO<sub>2</sub> crystal lattice, and the effect of calcination temperatures on the quality of PuO<sub>2</sub>. These techniques have enabled methods to conduct PuO<sub>2</sub> age dating since last calcination and estimate the calcination temperature with Raman spectroscopy and DRS. Additional spectroscopic information measured with DRIFTS has enabled the observation of the evolution of carbon species with calcination temperature, while gamma spectroscopy provides information on age dating since last purification.</p>