Solubility of actinide surrogates in nuclear glasses

This paper discusses the results of a study of actinide surrogates in a nuclear borosilicate glass to understand the effect of processing conditions (temperature and oxidizing versus reducing conditions) on the solubility limits of these elements. The incorporation of cerium oxide, hafnium oxide, and neodymium oxide in this borosilicate glass was investigated. Cerium is a possible surrogate for tetravalent and trivalent actinides, hafnium for tetravalent actinides, and neodymium for trivalent actinides. The material homogeneity was studied by optical, scanning electron microscopy. Cerium L_III XANES spectroscopy showed that the Ce³⁺/Ce_total ratio increased from about 0.5 to 0.9 as the processing temperature increased from 1100 to 1400 °C. Cerium L_III XANES spectroscopy also confirmed that the increased Ce solubility in glasses melted under reducing conditions was due to complete reduction of all the cerium in the glass. The most significant results pointed out in the current study are that the solubility limits of the actinide surrogates increases with the processing temperature and that Ce³⁺ is shown to be more soluble than Ce⁴⁺ in this borosilicate glass.