Production of mixed element actinide reference particulates to support nuclear safeguards using THESEUS, an aerosol-based particulate synthetic methodology

Abstract

The THermally Evaporated Spray for Engineered Uniform particulateS (THESEUS) production platform was developed to generate highly uniform mixed actinide oxide particles. The particulate synthesis platform builds on previous efforts and utilizes an aerosol-based technology to generate, calcine, characterize, and aggregate a monodisperse oxide phase particle product. In this study, particles comprised of uranium oxide, incorporated with varying compositions of thorium, were produced. Th/U test materials with ²³²Th concentrations between 1 ppm and 10%, ratioed to ²³⁸U, were successfully generated with in situ calcination at 600 °C and characterized by in situ aerodynamic particle size spectrometry and ex situ microanalytical methods. Populations of monodisperse particulates (geometric standard deviation – GSD < 1.15) with an average diameter near 1 μm were generatated and micro-Raman spectroscopy of individual particles identified U₃O₈ as the primary material phase for the range of Th/U samples analyzed. Single particle measurements and automated particle analyses by secondary ion mass spectrometry (SIMS) were performed. Uniform inter-particle elemental and isotopic homogeneity for uranium and thorium isotopes was characterized by SIMS, and a ²³²Th/²³⁸U relative sensitivity factor of 0.53 was determined. SIMS results demonstrated differences in the ²³²Th/²³⁸U profiling behavior for Th/U particulates with increased Th content (>1%). Despite the observed profiling behavior, single particle measurements of the 10% Th sample indicate inter-particle homogeneity. This work represents the first systematic study of Th/U microparticulate reference materials generated and intended for nuclear safeguards applications and serves as a demonstration of THESEUS to support a sustained capability for the production mixed-element particulate reference materials.