Combining batch experiments and spectroscopy for realistic surface complexation modelling of the sorption of americium, curium, and europium onto muscovite

Bezzina, James P.; Neumann, Julia; Brendler, Vinzenz; Schmidt, Moritz

doi:10.1016/j.watres.2022.119032

Cited by 4 publications

(4 citation statements)

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“…The mobility of REEs in the environment is largely controlled by their interactions with mineral surfaces. , Many studies have been carried out to assess the retention potential of major rock-forming minerals, such as quartz − and micas − for trivalent heavy metals M(III), including REEs and trivalent actinides. The impact of pH, metal concentration, and ligands on the adsorption was investigated, and models have been developed to predict the fate of REEs. ,, Mechanistically, studies of ion adsorption on muscovite mica showed that multivalent ions tend to adsorb farther from the mineral surface than monovalent ions, − which is related to multivalent ions’ ability to retain water molecules. Some ions, for example, Al(III) and some actinides such as Pu(III/IV) and Th(IV), polymerize at the interface to form secondary-phase thin films or nanoparticles.…”

Section: Introductionmentioning

confidence: 99%

Y(III) Sorption at the Orthoclase (001) Surface Measured by X-ray Reflectivity

Neumann

Lessing

Lee

et al. 2022

Environ. Sci. Technol.

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Interactions of heavy metals with charged mineral surfaces control their mobility in the environment. Here, we investigate the adsorption of Y(III) onto the orthoclase (001) basal plane, the former as a representative of rare earth elements and an analogue of trivalent actinides and the latter as a representative of naturally abundant K-feldspar minerals. We apply in situ highresolution X-ray reflectivity to determine the sorption capacity and molecular distribution of adsorbed Y species as a function of the Y 3+ concentration, [Y 3+ ], at pH 7 and 5. With [Y 3+ ] ≥ 1 mM at pH 7, we observe an inner-sphere (IS) sorption complex at a distance of ∼1.5 Å from the surface and an outer-sphere (OS) complex at 3−4 Å. Based on the adsorption height of the IS complex, a bidentate, binuclear binding mode, in which Y 3+ binds to two terminal oxygens, is proposed. In contrast, mostly OS sorption is observed at pH 5. The observed maximum Y coverage is ∼1.3 Y 3+ /A UC (A UC : area of the unit cell = 111.4 Å 2 ) for all the investigated pH values and Y concentrations, which is in the expected range based on the estimated surface charge of orthoclase (001).

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Section: Introductionmentioning

confidence: 99%

Y(III) Sorption at the Orthoclase (001) Surface Measured by X-ray Reflectivity

Neumann

Lessing

Lee

et al. 2022

Environ. Sci. Technol.

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“…Crystal powder samples are often used to determine experimentally the sorption potential of minerals in batch experiments. [ 5,12 ] Our data suggest that powder sorption results lead to an overestimation of retention by at least a factor of three, with potential implications for prognostic use. For desorption, a factor is estimated based on the relation between the adsorption factors and the corresponding predominant energy barrier (Table 2).…”

Section: Resultsmentioning

confidence: 90%

“…Eu 3+ has shown a highly similar behavior for sorption reactions and in solution to trivalent actinides. [5,[9][10][11][12] The sorption properties of radionuclides are an important aspect of quantitative migration prediction. Several experimental studies have investigated europium sorption on muscovite and structurally similar clay minerals, which show potential mechanistic influences on the sorption reactions.…”

Section: Introductionmentioning

confidence: 99%

Variability of Radionuclide Sorption Efficiency on Muscovite Cleavage Planes

Schabernack,

Oliveira,

Heine

et al. 2023

Advcd Theory and Sims

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In deep geological repositories for nuclear waste, the surrounding rock formation serves as an important barrier against radionuclide migration. Multiple potential host rocks contain phyllosilicates, which have shown high efficiency in radionuclide sorption. Recent experimental studies report a heterogeneous distribution of adsorbed radionuclides on nanotopographic mineral surfaces. In this study, the energetic differences of surface sorption sites available at nanotopographic structures such as steps, pits, and terraces are investigated. Eleven important surface sites are selected and the energies of ad‐ and desorption reactions are obtained from density functional theory calculations. The adsorption energies are then used for the parameterization of a kinetic Monte Carlo model simulating the distribution of adsorbed europium on a typical nanotopographic muscovite surface. On muscovite, silicon step sites are favorable for europium sorption and lead to an increased adsorption in regions with high step concentrations. Under identical chemical conditions, sorption on typical nanotopographic surfaces is increased by a factor of three compared to atomically flat surfaces. Desorption occurs preferentially at terrace sites, leading to an overall 2.5 times increased retention at nanotopographic structures. This study provides a mechanistic explanation for heterogeneous sorption on nanotopographic mineral surfaces due to the availability of energetically favorable sorption sites.

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“…Insulants such as muscovite are representative. It is a “2:1” (tetrahedron–octahedron–tetrahedron, TOT) stacked, layered silicate crystal with an ideal chemical formula of KAl 2 (AlSi 3 O 10 )(OH) 2 , 2 in which two SiO 4 tetrahedron sheets are linked together by an AlO 6 octahedron layer forming sandwich structure. In tetrahedron sheet, one‐fourth tetrahedral Si elements are substituted by Al displaying negative charges, which are balanced by interlayer cations like K + and Na + 3 .…”

Section: Introductionmentioning

confidence: 99%

An exploration of lattice transformation mechanism of muscovite single crystal under EB irradiation at 0–1000 kGy

Wang,

Sun,

Xia

et al. 2023

J Am Ceram Soc.

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Electronic components made by inorganics (e.g., mica) play key roles in function exertion of instruments working in outer‐layer space, enduring long‐term β ray irradiation. Its damage is vital while explored rarely. Herein, pure muscovite crystals were chosen and irradiated by an electron beam (EB) in air with dose up to 1000 kGy. Then, micro‐geometry morphology variation in Z‐axis and microstructural transformation mechanism were explored by XRD, FT‐ATR IR, TGA, XPS and CA analysis. Main results reveal that muscovite lattice is unstable to EB irradiation. With dose increases to 1000 kGy interlayer space d of (002) lattice varied 2% near 0.2 Å. At low dose irradiation lattice expansion is readily to occur while at higher dose it is lattice shrinkage, showing a transformation from expansion to shrinkage. Concurrently, chemical structure varied, H2O amount increased, metal element valance and surface wettability were reduced. Where, dehydroxylation occurred exceeding H2O radiaolysis and evaporation, and framework cleavage be severe. Binding energies of metals of 1000 kGy‐irradiated species decreased by 0.2 eV, CA of 100 kGy‐irradiated species increased by 10°. Intrinsic mechanisms involve framework destruction, H‐atom migration, hydrogen bond formation/destruction and H2O radiolysis. At low dose irradiation, H‐atom migration and hydrogen bond formation/destruction are predominant, inducing lattice expansion; at higher dose, framework cleavage is intensive and crucial, inducing shrinkage. During which, partial H2O occurred radiolysis, reducing valence. Generally, H‐atom migration and interface cleavage played key roles in microgeometry morphology variation of muscovite crystal under EB irradiation at 0–1000 kGy. To enhance muscovite geometry morphology‐stability under a long‐term β‐ray irradiation condition OH and hydrogen bond contents should be reduced and interface region should be strengthened (e.g., lessening vacancies or compacting stacking). This conclusion promotes design of radiation‐resistant silicate material, guiding manufacture of electronic component used in aerospace industry, significant.This article is protected by copyright. All rights reserved

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Combining batch experiments and spectroscopy for realistic surface complexation modelling of the sorption of americium, curium, and europium onto muscovite

Cited by 4 publications

References 56 publications

Y(III) Sorption at the Orthoclase (001) Surface Measured by X-ray Reflectivity

Y(III) Sorption at the Orthoclase (001) Surface Measured by X-ray Reflectivity

Variability of Radionuclide Sorption Efficiency on Muscovite Cleavage Planes

An exploration of lattice transformation mechanism of muscovite single crystal under EB irradiation at 0–1000 kGy

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