The contribution is focused on chemical, geochemical and mineralogical research of bentonite stability with the aim to determine
the effect of saturation medium composition and loading by heat on bentonite stability. The main part of the research is directed
to the experimental results of bentonite and bentonite leachate samples obtained for the bentonite interaction under laboratory
experiments. Computer-modeling methods were used to calculate equilibrium thermodynamic principles, the distributions of predominant
aqueous species, and potential solubility controls for the environmentally important oxidation states of each investigated
radioactive contaminants. The Eh–pH diagrams of individual chemical species of the tested radionuclides were calculated by
the geochemical software tool Geochemist’s Workbench that included the actual chemical compositions of the solid–liquid systems
under the given experimental conditions. It was confirmed that smectites are transformed to more stable silicate phases, such
as illite/smectite mixed layers, illite. The data obtained from the model calculations conform with experimental results.
The effect of the variable aqueous phase composition on bentonite stability using Ca–Mg and Na–Ca bentonites for the experiments
was studied. The synthetic granitic waters with the higher concentration of the K+ and Mg2+ cations were applied for the study of bentonite stability.