The effect of high pH alkaline solutions on the mineral stability of the Boom Clay – Batch experiments at 60°C

Abstract

Boom Clay is currently viewed as a reference host formation for studies on deep geological disposal of radioactive waste in Belgium. The interactions between bulk rock Boom Clay and 0.1 M KOH, 0.1 M NaOH, 0.1 M Ca(OH)2, young cement water and evolved cement water solutions, ranging in pH from 12.5 to 13.2, were examined as static batch experiments at 60 °C to simulate alkaline plume perturbations, which are expected to occur in the repository due to the presence of concrete. Both liquids and solids were investigated at specific times between 90 and 510 days in order to control the elemental budget and to search for potential mineralogical alterations. Also, the clay fraction was separated from the whole-rock Boom Clay at the end of each run and characterized for its mineralogical composition. Thereby, the importance of the mineral matrix to buffer the alkaline attack and the role of organic matter to protect clay minerals were also addressed. The results indicate that the degree of geochemical perturbation in Boom Clay is dependent on the initial pH of the applied solution together with the nature of the major cation in the reactant fluids. The higher the initial pH of the media, the stronger its interaction with Boom Clay. No major non-clay mineralogical alteration of the Boom Clay was detected, but dissolution of kaolinite, smectite and illite occurred within the studied experimental conditions. The dissolution of clays is accompanied by the decrease in the layer charge, followed by a decrease in the cation-exchange capacity. The highest TOC values coincide with the highest total elemental concentrations in the leachates, and correspondingly, the highest dissolution degree. However, no quantitative link could be established between the degree of organic matter decomposition and clay dissolution.