Nations using borosilicate glass as an immobilization material for radioactive waste have reinforced the importance of scientific collaboration to obtain a consensus on the mechanisms controlling the long-term dissolution rate of glass. This goal is deemed to be crucial for the development of reliable performance assessment models for geological disposal. The collaborating laboratories all conduct fundamental and/or applied research using modern materials science techniques. This paper briefly reviews the radioactive waste vitrification programs of the six participant nations and summarizes the current state of glass corrosion science, emphasizing the common scientific needs and justifications for on-going initiatives
Understanding the long-term release
of radionuclides from nuclear
waste to the environment is critical for public acceptance and sustainability
of nuclear energy. Iodoapatite, a synthetic material similar to mineral
vanadinite proposed for radioactive iodine-129 immobilization, is
employed in this study as a model system for iodine waste forms and
ceramic waste forms in general to understand its long-term chemical
durability. Semidynamic leaching experiments were performed in cap-sealed
Teflon vessels to evaluate the chemical durability at temperatures
from 20 to 90 °C and pH values from 4 to 9 using deionized water
and pH buffer solutions. The leachates were analyzed using inductively
coupled plasma-mass spectrometry. The leached surfaces were examined
by X-ray diffraction, scanning electron microscopy, and Raman spectroscopy.
Effects of test variables including surface-to-volume ratio, leachant
replacement interval, and environmental variables including temperature
and pH on the dissolution rate were systematically investigated. The
activation energy of the dissolution was 16.9 ± 1.5 kJ/mol for
the matrix elements and 34.4 ± 3.9 kJ/mol for the diffusive iodine
release. The order of the pH effect on the dissolution rate as a power
law exponent was 0.87 ± 0.08. The effect of the surface-to-volume
ratio and replacement interval was approximated by a single exponential
function rise to maximum. Fully parametrized models were then combined
to predict iodine release rate under various conditions. The result
suggests that the long-term iodine release is controlled by iodide
diffusion when the matrix dissolution rate is very low in near neutral
pH solutions and by matrix dissolution when the dissolution rate is
high at low pH. The present study demonstrates a mechanistic approach
to parametrize models that can be used to evaluate the performance
of nuclear waste forms under various disposal environments.
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