Origin and evolution of cup-shaped structures on leached nuclear waste containment glass surfaces

Abstract

A three-dimensional surface microanalysis system equipped with a sensitive topographical probe was used to quantify the evolution of cup-shaped structures formed by aqueous leaching of nuclear waste containment glass. A model of the dissolution phenomenon provides satisfactory correlation between calculated and measured cup radius and depth. Dissolution cups form from cracks on the initially cut glass surface. Large cracks control the phenomenon by forming the largest cups, which gradually absorb smaller ones. The evolution of the size and shape of the dissolution cups was described by a model that assumes a constant dissolution rate on the surface, diminishing with crack depth. The best fit with the experimental data was obtained with a dissolution rate one hundred times lower at the bottom of the crack than at the surface. Moreover, it is predictable that all the cups will gradually disappear as they grow larger and flatter over a leaching period of some 2 years, for the glass composition and experimental leaching procedures used in this work.