Scaling effect on cesium diffusion in compacted MX-80 bentonite for buffer materials in HLW repository

Abstract

Abstract In this study, radionuclide behavior in high-level radioactive waste (HLW) disposal repositories is complicated because of the spatial heterogeneity of porous media, coupled flow-transport mechanisms, and multiple chemical reaction processes. Discrepancies in the diffusion behavior of a non-sorbing tracer (HTO) and a reactive tracer (137Cs) in porous media have long been recognized but are not yet fully understood, which hinders effective assessment of the capabilities of buffer materials. This paper was dedicated to exploring and explaining the discrepancies in the transport behavior of non-sorbing and reactive tracers through laboratory experiments and an investigation of contributing mechanisms. Our results showed that for a bentonite sample of the same thickness, 137Cs has smaller apparent and less effective diffusion coefficients than those for HTO. These discrepancies can be attributed to the negative surface electric effects, atomic properties, and chemical reactions. In the case of bentonite samples with different thicknesses (0.5, 0.75, 2.0, 2.5 cm), the apparent and effective diffusion coefficients show an increasing trend with bentonite thickness. According to the experimental data and fitting results, the apparent and effective diffusion coefficients are highly related to bentonite thickness. Thus, scaling effects on transport parameters were proposed to explain the results, which were attributed to the nonuniform distribution of the pore space in the bentonite sample. The scale effect behavior of radionuclide was quantified through a regression analysis. The results can be used to improve buffer designs for radionuclides diffusion.