Analysis of neptunium oxides produced through modified direct denitration

Abstract

Production of neptunium-237 (²³⁷Np) target materials for plutonium-238 (²³⁸Pu) radioisotope thermoelectric generators (RTGs) for deep space exploration requires advanced chemistry and engineering development. Currently, the domestic Pu-238 Supply Program at Oak Ridge National Laboratory produces neptunium dioxide (NpO₂) for target material using a modified direct denitration (MDD) flowsheet. Although the chemistry, reaction mechanisms, and product characteristics of MDD are well understood for uranium, corresponding studies of the neptunium system are still needed to continue optimization of target material properties, production equipment design, and production flowsheets. The objective of this work is to characterize crystalline phases, morphology, surface texture, and particle size of NpO₂ produced via MDD reactions. Solid-phase characterization techniques, including powder X-ray diffraction (pXRD) and scanning electron microscopy with energy-dispersive spectroscopy (SEM-EDS), were employed to achieve this objective. Subsequent data processing using the Morphological Analysis for Material Attribution (MAMA) software was performed to analyze particle morphology and size. Broadly, the powders were found to contain a mixture of NpO₂ and Np₂O₅ after denitration with a variety of morphologies. After high-firing, the product was found to be NpO₂ with a typical polycrystalline oxide morphology and a grain size ranging from 0.72 to 0.94 µm. These analyses provide knowledge on the reaction pathway for a non-traditional NpO₂ synthesis method and offer additional unique insight into production-scale environments for transuranic materials.