Radiation and thermal effects on porous and layer structured materials as getters of radionuclides

Abstract

The long term radiation and thermal effects on porous and layer structured materials that may function as getters for radionuclides have been evaluated using accelerated laboratory experiments including energetic electron, ion or neutron irradiation, as well as high-temperature thermal annealing. The materials studied include: zeolites, layered silicates (mica and smectite clays), open framework structured apatite and crystalline silicotitanate (CST) which is an important synthetic ion-exchange material for the chemical separation of high-level liquid radioactive wastes. In situ transmission electron microscopy during irradiation by energetic electrons and ions has shown that all the studied materials are susceptible to irradiation-induced amorphization. Amorphization can be induced by ionization and/or direct displacement processes. Amorphization may be preceded or accompanied with dehydration, layer spacing reduction and gas bubble formation. In the case of zeolites, CST and some layer silicates, radiation effects are significantly enhanced at higher temperatures. In fact, thermal annealing at high temperatures alone can cause complete amorphization of zeolites. Our experiments have shown that amorphization or even partial amorphization will cause a dramatic reduction (up to 95%) in ion-exchange and sorption/desorption capacities of zeolite for radionuclides, such as Cs and Sr. Because the near-field or chemical processing materials (e.g., zeolites or CST) will receive a substantial radiation dose after they have incorporated radionuclides, our results suggest that radiation effects may, in some cases, retard the release rate of sorbed or ion-exchanged radionuclides.