PNNL

Abstract

Sodium and aluminum rich high level nuclear waste glasses are prone to nepheline (NaAlSiO4) crystallization. Since nepheline removes three moles of glass forming oxides (Al2O3 and SiO2) per each mole of Na2O, its formation can result in sever deterioration of the chemical durability. The present study aims at investigating the relationships between the molecular-level structure of sodium alumino-borosilicate based simulated high-level nuclear waste glasses and their crystallization behavior by infrared spectroscopy (FTIR) and x-ray diffraction, respectively. The molecular structure of most of the investigated glasses comprises of a mixture of Q2 and Q3 (Si) units while aluminum and boron are predominantly present in tetrahedral and trigonal coordination, respectively. The increasing boron content has been shown to suppress the nepheline formation in the glasses. The structural influence of various glass components on nepheline crystallization has been discussed.