TY - JOUR

T1 - Mechanism of Cs Immobilization within a Sodalite Framework: The Role of Alkaline Cations and the Si/Al Ratio

AU - Kasprzhitskii, Anton

AU - Ermolov, Yakov

AU - Mischinenko, Vasilii

AU - Vasilchenko, Andrey

AU - Yatsenko, Elena A

AU - Smoliy, Victoria A

N1 - This research on the local structure of zeolite with cesium was funded by a grant from the Ministry of Science and Higher Education of the Russian Federation (Agreement No. 075-15-2022-1111; “Carbon-neutral technologies for recycling large-tonnage fuel energy waste with the production of functional geopolymer materials”). The study of the electronic structure of the Na- and K-type zeolite with different Si/Al ratios was funded by a grant from the Russian Science Foundation No. 19-79-10266, https://rscf.ru/en/project/19-79-10266/ (accessed on 30 November 2023).

PY - 2023/11/30

Y1 - 2023/11/30

N2 - Conditioning of radioactive waste generated from the operation of medical institutions, nuclear cycle facilities, and nuclear facilities is important for the safety of the environment. One of the most hazardous radionuclides is radioactive cesium. There is a need for more effective solutions to contain radionuclides, especially cesium (Cs+). Geopolymers are promising inorganic materials that can provide a large active surface area with adjustable porosity and binding capacity. The existence of nanosized zeolite-like structures in aluminosilicate gels was shown earlier. These structures are candidates for immobilizing radioactive cesium (Cs+). However, the mechanisms of their interactions with the aluminosilicate framework related to radionuclide immobilization have not been well studied. In this work, the influence of alkaline cations (Na+ or K+) and the aluminosilicate framework structure on the binding capacity and mechanism of interaction of geopolymers with Cs+ is explored in the example of a sodalite framework. The local structure of the water molecules and alkaline ions in the equilibrium state and its behavior when the Si/Al ratio was changed were studied by DFT.

AB - Conditioning of radioactive waste generated from the operation of medical institutions, nuclear cycle facilities, and nuclear facilities is important for the safety of the environment. One of the most hazardous radionuclides is radioactive cesium. There is a need for more effective solutions to contain radionuclides, especially cesium (Cs+). Geopolymers are promising inorganic materials that can provide a large active surface area with adjustable porosity and binding capacity. The existence of nanosized zeolite-like structures in aluminosilicate gels was shown earlier. These structures are candidates for immobilizing radioactive cesium (Cs+). However, the mechanisms of their interactions with the aluminosilicate framework related to radionuclide immobilization have not been well studied. In this work, the influence of alkaline cations (Na+ or K+) and the aluminosilicate framework structure on the binding capacity and mechanism of interaction of geopolymers with Cs+ is explored in the example of a sodalite framework. The local structure of the water molecules and alkaline ions in the equilibrium state and its behavior when the Si/Al ratio was changed were studied by DFT.

UR - https://www.scopus.com/record/display.uri?eid=2-s2.0-85179323083&origin=inward&txGid=0a64772c1041665d228c74bf292bed77

U2 - 10.3390/ijms242317023

DO - 10.3390/ijms242317023

M3 - Article

C2 - 38069346

VL - 24

JO - International Journal of Molecular Sciences

JF - International Journal of Molecular Sciences

SN - 1661-6596

IS - 23

M1 - 17023

ER -