Trivalent lanthanide sorption onto illite in the presence of carbonate; A Study combining thermodynamic sorption modeling, time-resolved laser fluorescence spectroscopy, and parallel factor analysis

Sugiura, Yuki  ; Ishidera, Takamitsu ; Aoyagi, Noboru   ; Mei, H.  ; Saito, Takumi*; Tachi, Yukio  

This study performed batch sorption experiments using Eu and Sm as chemical analogs of trivalent actinides to evaluate their sorption behavior onto illite in the presence of dissolved inorganic carbon (DIC). The results were analyzed using a thermodynamic sorption model (TSM), which predicted that Eu/Sm forms ternary-surface complexes with carbonate ions. Time-resolved laser fluorescence spectroscopy (TRLFS) measurements were performed to gather information on the chemical forms of sorbed Eu on illite. Parallel factor analysis (PARAFAC) of the TRLFS data indicated the presence of two Eu chemical species. The pH dependence of the chemical species was consistent with that of the surface species predicted by TSM. The dominant chemical species in the presence of carbonate was inferred to be coordinating carbonate ions based on the fluorescence lifetime, supporting the validity of the TSM.