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Effects of surface roughness and mineralogy on the sorption of Cm(III) on crystalline rock

Demnitz, M.; Molodtsov, K.; Schymura, S.; Schierz, A.; Müller, K.; Jankovsky, F.; Havlova, V.; Stumpf, T.; Schmidt, M.

Crystalline rock is one of the considered host rocks for a future deep geological repository for highly active radiotoxic nuclear waste. The safety assessment requires reliable information on the retention behavior of minor actinides. In this work, we applied various spatially resolved techniques to investigate the sorption of Curium onto crystalline rock (granite, gneiss) thin sections from Eibenstock, Germany and Bukov, Czech Republic. We combined Raman-microscopy, calibrated autoradiography and µTRLFS (micro-focus time-resolved fluorescence spectroscopy) with vertical scanning interferometry to study in situ the impact of mineralogy and surface roughness on Cm(III) uptake and molecular speciation on the surface. Heterogeneous sorption of Cm(III) on the surface depends primarily on the mineralogy. However, for the same mineral class sorption uptake and strength of Cm(III) increases with growing surface roughness around surface holes or grain boundaries. When competitive sorption between multiple mineral phases occurs, surface roughness becomes the major retention parameter on low sorption uptake minerals. In high surface roughness areas primarily Cm(III) inner-sphere sorption complexation and surface incorporation are prominent and in select sites formation of stable Cm(III) ternary complexes is observed. Our molecular findings confirm that predictive radionuclide modelling should implement surface roughness as a key parameter in their simulations.

Keywords: curium; luminescence; crystalline rock; granite; sorption; correlative spectroscopy

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  • Secondary publication expected from 21.08.2022

Publ.-Id: 32811