Effect of hydrogen on oxidative dissolution of epsilon particles-doped UO2 pellets under carbonate condition with hydrogen peroxide

Abstract

The epsilon particles that result from nuclear fission of UO₂ fuel possess both advantages and disadvantages from a spent nuclear fuel (SNF) management perspective. In this study, the effect of epsilon particles, namely Ru, Mo, and Pd, inherent in simulated UO₂ pellets is examined. Various analytical methods have been used to explore the changes in the structural, surface, and electrochemical properties of which contain epsilon particles. A notable finding is that the epsilon particles are not evenly distributed and tend to clump together, transforming into a metallic state after sintering, as detailed in the X-ray diffraction analyses. Energy-dispersive X-ray spectroscopy analyses highlight interesting aspects of the distribution of elements, especially the disappearance of Pd during sintering, which is likely due to its high vapor pressure. Although the lattice structure of UO₂ remains unchanged, the sizes of the grains and pores visibly change, which may influence the tendency of UO₂ pellet-cracking. Despite the addition of the epsilon particles, the electrical conductivity analyses show no significant changes, suggesting that they act as minor impurities without affecting the structural lattice. However, their possible role as catalysts in electrochemical reactions opens new and interesting areas that require thorough investigation. Moreover, examining the anodic dissolution under various conditions provides detailed insights into UO₂ dissolution and oxidation, revealing how epsilon particles subtly influence the oxidative dissolution process. This study clarifies the basic interactions and effects of epsilon particles in UO₂ pellets and broadens the path for a deeper understanding and improvement of nuclear fuel matrices and steering advancements in the safe and effective use of nuclear energy.