Journal of Physical Chemistry C
Journal of Physical Chemistry C
5 years ago

Influence of Tetrahedral Layer Charge on the Fixation of Cesium in Synthetic Smectite

Influence of Tetrahedral Layer Charge on the Fixation of Cesium in Synthetic Smectite
Laurent J. Michot, Fabien Hubert, Eric Ferrage, Emmanuel Tertre, Jean-Louis Robert, Alfred Delville, Heloïse Verron, Liva Dzene
After radionuclide pollution of soils by nuclear power plant accidents, Cs+ strongly interacts with swelling clay minerals, which in turn controls the fixation or the migration of this pollutant in the natural media. Little is known, however, about the role played by the amount of layer charge and the two-dimensional confinement on Cs+ fixation. In this study a series of tetrahedrally charged smectites with structural formula inter[M+x]oct[Mg6]tet[Si8–xAlx]O20(OH)4 and with a layer charge (x) varying from 0.8 to 2.0 and with Na+ or Cs+ as interlayer cation M+ were used. While Na+ remains fully exchangeable over the entire range of layer charges investigated, the fraction of exchangeable Cs+ decreased gradually for samples with x ≥ 1.4/O20(OH)4. Structure analysis of Cs+-samples in water-saturated or at 80% relative humidity conditions showed a gradual decrease of the layer-to-layer distance. The results were found to qualitatively agree with analysis of the thermodynamics of the clay/water interfaces derived from molecular simulations. Quantitative structure analysis by modeling of 00l reflections on experimental X-ray diffraction patterns suggested that exchangeable Cs+ can be correlated with the amount of hydrated interlayers, whereas fixed Cs+ in these conditions corresponds to the amount of collapsed layers. To describe the coexistence of both exchangeable and fixed Cs+, a toy model accounting for the presence of heterogeneous charge distribution was used, in agreement with experimental data obtained on these samples. This model successfully interprets the overall reactivity of Cs+ toward smectite over a large range of layer charge values and may contribute to an improved description of Cs+ mobility in contaminated soil environments.

Publisher URL: http://dx.doi.org/10.1021/acs.jpcc.7b06308

DOI: 10.1021/acs.jpcc.7b06308

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