Unravelling the origin of long-term stability for Cs⁺ and Sr²⁺ solidification inside sodalite

Cesium (Cs⁺) and strontium (Sr²⁺) ions are the main fission byproducts in the reprocessing of spent nuclear fuels for nuclear power plants. Their long half-live period (30.17 years for ¹³⁷Cs and 28.80 years for ⁹⁰Sr) makes them very dangerous radionuclides. Hence the solidification of Cs⁺ and Sr²⁺ is of paramount importance for preventing them from entering the human food chain through water. Despite tremendous efforts for solidification, the long-term stability remains a great challenge due to the experimental limitation and lack of good evaluation indicators for such long half-life radionuclides. Using density functional theory (DFT), we investigate the origin of long-term stability for the solidification of Cs⁺ and Sr²⁺ inside sodalite and establish that the exchange energy and the diffusion barrier play an important role in gaining the long-term stability both thermodynamically and kinetically. The acidity/basicity, solvation, temperature, and diffusion effect are comprehensively studied. It is found that solidification of Cs⁺ and Sr²⁺ is mainly attributed to the solvation effect, zeolitic adsorption ability, and diffusion barriers. The present study provides theoretical evidence to use geopolymers to adsorb Cs⁺ and Sr²⁺ and convert the adsorbed geopolymers to zeolites to achieve solidification of Cs⁺ and Sr²⁺ with long-term stability.