A Six-Year Hydration Evaluation of Cs-Bearing Materials at Room Temperature and 55% Relative Humidity Simulating Radioactive Waste with Different Crystallinities

Radioactive wastes often contain amorphous and crystalline phases, and vapor hydration
can affect their durability. In this study, Cs-clinoptilolite was heated (at 1100 °C and for 2–36 h) to prepare the samples that were composed mainly of an amorphous phase (AmP) and CsAlSi5O12 (≥94%) with minor CsAlSi2O6. Six samples with an AmP/CsAlSi5O12 ratio from 26.5 to 0.1 were kept at 21 ◦C and 55% relative humidity, and their hydration was measured via thermogravimetry (TG) over a period of almost six years. The hydration that resulted was directly related to the AmP quantity. The increase in water content followed a logarithmic trend over time. It reached 1.95% in the AmP-richest material, while it attained only 0.07% in the most crystalline sample. The hydrolysis of the AmP led to an increase over time in the tightly bound water. Samples with an AmP of ≤19% demonstrated slightly higher durability due to the lower Cs content in the AmP.