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Diffusion and sorption of neptunium(V) in compacted montmorillonite; Effects of carbonate and salinity

Tachi, Yukio; Nakazawa, Toshiyuki*; Ochs, M.*; Yotsuji, Kenji; Suyama, Tadahiro; Seida, Yoshimi; Yamada, Norikazu*; Yui, Mikazu

Diffusion and sorption of radionuclides in compacted bentonite are the key processes in the safe geological disposal. The effects of carbonate and salinity on Np(V) diffusion and sorption in compacted montmorillonite were investigated by experimental and modeling approaches. Effective diffusion coefficients ($$D$$$$_{rm e}$$) and distribution coefficients ($$K$$$$_{rm d}$$) of Np in montmorillonite compacted to dry density of 800 kg/m$$^{3}$$ were measured under four conditions with different salinities (0.05/0.5 M NaCl) and carbonate concentrations (0/0.01 M NaHCO$$_{3}$$). The $$D$$$$_{rm e}$$ for carbonate-free conditions decreased as salinity increased, and those for carbonate conditions showed the opposite dependency. The $$K$$$$_{rm d}$$ decreased by one order of magnitude under high carbonate condition. Diffusion and sorption behaviors were interpreted by coupling the thermodynamic aqueous speciation, the thermodynamic sorption model based on ion exchange and surface complexation, and the diffusion model based on electrical double layer theory in narrow pores. The mechanistic model could be useful in predicting the sorption and diffusion behavior of complex species in compacted systems.

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Category:Chemistry, Inorganic & Nuclear

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