Clay minerals are widely used to treat groundwater and surface water containing radionuclides. In our study, the method of mechanochemical activation for increasing the sorption capacity of the natural clay mineral montmorillonite was used. By adjusting the grinding time, the increasing sorption parameters of mechanochemically activated montmorillonite were determined. X-ray diffraction method, scanning electron microscopy, and the determination of the specific surface by low-temperature adsorption–desorption of nitrogen to characterize the natural and mechanochemical-activated montmorillonites were used. It was established that the maximal sorption of uranium, strontium, and cesium is found for montmorillonite after mechanochemical treatment for 2 h. It is shown that the filling of the surface of montmorillonite with ions of different natures occurs in various ways during different times of mechanochemical treatment. The appropriateness of the Langmuir and Freundlich models for the sorption parameters of uranium, strontium, and cesium ions on montmorillonite after its mechanochemical activation was established. The effect of natural organic substances—humic acids—on the efficiency of water purification from uranium on mechanoactivated montmorillonite was studied. The obtained sorbents can be effectively used for the removal of trace amounts of radionuclides of different chemical natures (uranium, cesium, and strontium) from polluted surface and ground waters.

The modification of the layered silicate with a structural type 2:1 montmorillonite by the cationic surfactant hexadecyltrimethylammonium bromide was carried out. The obtained organomontmorillonite was milled for 2–25 min in a high-energy planetary ball mill. The structural and physicochemical characteristics of the modified montmorillonite and the mechanochemically activated montmorillonite were investigated using various methods such as X-ray diffraction, thermal analysis, scanning electron microscopy, energy-dispersive X-ray spectroscopy, transmission electron microscopy, and determination of the specific surface area as well as the parameters of the porous structure by the low-temperature adsorption–desorption of nitrogen. The modification of montmorillonite with the quaternary ammonium salt led to a slowdown of deformation and subsequent amorphization of the montmorillonite structure during the high-energy milling. Mechanochemical activation of the modified montmorillonite increased its sorption capacity nine times, with the maximum uranium sorption achieved after mechanochemical treatment for 10 min.