Variability of radionuclide sorption efficiency on muscovite cleavage planes
Variability of radionuclide sorption efficiency on muscovite cleavage planes
Schabernack, J.; Faria Oliveira, A.; Heine, T.; Fischer, C.
In deep geological repositories for nuclear waste, the surrounding rock formation serves as an important barrier against radionuclide migration. Multiple potential host rocks contain phyllosilicates, which have shown high efficiency in radionuclide sorption. Recent experimental studies reported a heterogeneous distribution of adsorbed radionuclides on nanotopographic mineral surfaces. In this study, we investigated the energetic differences of surface sorption sites available at nanotopographic structures such as steps, pits, and terraces. Eleven important surface sites were selected and the energies of ad- and desorption reactions were obtained from density functional theory calculations. The adsorption energies were then used for the parameterization of a kinetic Monte Carlo model simulating the distribution of adsorbed europium on a typical nanotopographic muscovite surface. On muscovite, silicon step sites are favorable for europium sorption and lead to an increased adsorption in regions with high step concentrations. Under identical chemical conditions, sorption on typical nanotopographic surfaces is increased by a factor of three compared to atomically flat surfaces. Desorption occurs preferentially at terrace sites, leading to an overall 2.5 times increased retention at nanotopographic structures. This study provides a mechanistic explanation for heterogeneous sorption on nanotopographic mineral surfaces due to the availability of energetically favorable sorption sites.
Keywords: Radionuclide Sorption; Kinetic Monte Carlo; Density Functional Theory; Muscovite; Europium
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Data publication: Variability of radionuclide sorption efficiency on muscovite …
ROBIS: 35469 HZDR-primary research data are used by this (Id 35468) publication
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Advanced Theory and Simulations 6(2023)2, 2300406
DOI: 10.1002/adts.202300406
Permalink: https://www.hzdr.de/publications/Publ-35468
Publ.-Id: 35468