The alteration of illite by Bad Nauheim and Gerolstein brine; Implications on fluid permeability in geothermal systems

Illite is one of the most abundant clay minerals on earth, yet its structure remains not fully solved. In hydrothermal reservoir sandstones, illites can display a fibrous growth within the pores and pore throats. The network created by them and the particles trapped therein during fluid flow lead to a dramatic decrease in permeability, which should be prevented if the reservoirs were to be used for geothermal energy extraction. In order to determine possible changes in structure, stacking or shape of the illite fibers, the interaction of a sandstone with two different brines was compared to an unaltered sandstone via environmental scanning electron microscopy and transmission electron microscopy. Moreover, three-dimensional electron diffraction experiments were performed using automated diffraction tomography. The 1M_tv structure of illite could be solved based on a single dataset of a 50 nm illite fiber. Illites that were altered with synthetic Gerolstein brine showed one-dimensional diffuse scattering, indicating a disorder in the stacking of the illite layers. The degree of disorder is dependent on the potassium content of the fluid, since the K⁺ ions of the interlayer can be released via the (010) facet. This causes a stability reduction of the structure, resulting in a high fragmentation and detachment of individual illite layers. Fluids interacting with the sandstone can then transport such mobile layer fragments, leading to entangling and interweaving of illite fibers. These new insights into the structure of illite fibers show a significant dependence of the arrangement of the fibers in the pores on the potassium content of the fluid. The increased migration and interweaving of illite fibers associated with a low potassium content can lead to severe clogging of the pores and thus to a reduction in fluid permeability. Altered sandstones with illitic pore filling are therefore less suitable for long-term geothermal projects.