Sorption properties of152Eu and241 Am in geological materials: Eu as an analogue for monitoring the Am behaviour in heterogeneous geological environments
“…The results from Payne et al [10] are of particular interest for PA in that they show the presence of TiO 2 in kaolinite, even at trace levels, appears to play an important role in retaining U at low uranyl concentrations. No study has yet been conducted with trivalent actinides but few reports of trivalent lanthanides sorption onto TiO 2 [20][21][22][23][24][25] exist, which are considered as homologs for the trivalent actinides [26].…”
“…The results from Payne et al [10] are of particular interest for PA in that they show the presence of TiO 2 in kaolinite, even at trace levels, appears to play an important role in retaining U at low uranyl concentrations. No study has yet been conducted with trivalent actinides but few reports of trivalent lanthanides sorption onto TiO 2 [20][21][22][23][24][25] exist, which are considered as homologs for the trivalent actinides [26].…”
“…Rare-earth (RE) doped glasses are well known candidates for many applications as optical fibre amplification, upconversion laser and many other applications [1][2][3][4]. Eu 3+ ions are more particularly used as luminescent probe in nuclear waste glasses [5][6][7][8] since Eu 3+ ion acts as an analogue of minor actinides [9] and are found also as fission products in nuclear waste glasses. In the recent years the use of the molecular dynamics (MD) technique has become very common in glasses studies, especially in the determination of local structure around rare-earth [10].…”
“…α spectrometry was applied to determine the total coverage (θ tot ) of M(III) adsorbed on the mica surface ex situ , using the α-emitting radioisotope 243 Am. To ensure comparability to the SXRD experiments (see Section ) and to keep the activity of the samples moderate, a solution of 0.1 mM Eu(III) as an inactive trivalent analogue for trivalent actinides − was spiked with ∼0.38% 243 Am ([Am 3+ ] = 3.8 × 10 –7 M; t 1/2 = 7370 a). The sulfate concentration was adjusted to 0.1–4 mM (Na 2 SO 4 ), and the pH was set to 5.5 ± 0.1 by adding small amounts of diluted HCl/NaOH.…”
Section: Experimental
Sectionmentioning
confidence: 99%
“…One group of relevant contaminants is the rare earth elements (REEs), which are released into the environment due to their increasing usage, e.g., in high-technology electronic devices . Main anthropogenic sources of REEs to natural waters are mining, , medical applications, , and electronic wastes and their recycling. , The total REE concentrations at contaminated mining sites are reported to reach up to 80 μM. − Ecotoxicological effects of REEs, such as stress reactions in plants as well as health effects on animals and humans, have been demonstrated previously. ,, In addition, REEs have a typical oxidation state of +III and serve as analogues for trivalent actinides (Pu, Am, Cm) in various studies. − Here as well, the actinides’ interaction with mineral surfaces is of particular interest, , which needs to be understood for making critical decisions in selecting deep geological repository sites for radioactive waste …”
The environmental fate of metal ions is influenced by their interactions with natural organic and inorganic ligands, which modify the ions' structure and charge and thus influence their interactions with mineral phases. We investigate the impact of ubiquitous sulfate on the retention of trivalent f-element cations (M(III) = Am, Eu, Y) by muscovite. We combine ex situ α spectrometry and in situ surface X-ray diffraction (i.e., crystal truncation rod and resonant anomalous X-ray reflectivity) to determine M(III) coverages and interfacial structures at the molecular level. M(III) cations adsorb as two distinct outer-sphere (OS) complexes (i.e., adsorbed and extended OS complexes) whose coverages vary with increasing sulfate concentration, [SO 42− ]. When [SO 4 2− ] ≤ 0.4 mM, M(III) coverages increase with increasing [SO 4 2− ] and exceed the amounts needed for surface charge compensation of muscovite by a factor of ∼3. This overcompensation is likely controlled by ion−ion correlations at the mineral/water interface rather than adsorption of MSO 4 + , which has a lower thermodynamic stability in the solutions and weaker electrostatic attraction to the mica surface than M 3+ . For higher [SO 42− ], MSO 4 + and M(SO 4 ) 2 − dominate solution speciation, leading to a strong decrease of the M(III) coverage due to their lower sorption affinity and weaker ion−ion correlations compared to M 3+ . These results indicate that interactions between electrolyte anions and metal ions at charged interfaces need to be explored for a more realistic prediction of contaminant transport in the environment.
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