Behavior of clay materials under ionizing radiation

The aim of this PhD thesis is to study and understand, by proposing reaction mechanisms, the behavior under irradiation of various clay materials. The systems of interest were first synthetic talc, which is the prototype of a non-swelling material. Under irradiation by accelerated electrons, the production of dihydrogen in this system, due solely to surface hydroxyl groups, is of the same order of magnitude as the one obtained in liquid water. This yield is divided by 30 in the case of natural talc from Luzenac, thus highlighting the importance of the impurities as scavengers of the precursors of dihydrogen. Synthetic smectites, which are swelling materials, were then studied. The results evidence the radiolysis of water confined in the interlayer space, leading to H₂ yields which may be two to three times higher than those measured in water. Moreover, they are similar for montmorillonite and saponite, evidencing that the charge location plays only a minor role. Finally, the study of double layered hydroxides or anionic clays shows that, in this case, the nature of the anion in the inter lamellar space controls the reactivity. Parallel to these measurements, electron paramagnetic spectroscopy experiments have enabled proposing reaction mechanisms. Finally, all these results are of interest in the context of the disposal of radioactive waste. (author)