Interaction of U(VI) with Äspö diorite: A batch and in situ ATR FT-IR sorption study

Schmeide, Katja; Gürtler, Salete; Müller, K.; Steudtner, Robin; Joseph, Claudia; Bok, Frank; Brendler, Vinzenz

doi:10.1016/j.apgeochem.2014.05.003

Cited by 28 publications

(9 citation statements)

References 39 publications

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“…Finally, Eu 3+ speciation on the crystalline rock was characterized on the molecular level by µTRLFS under conditions where Eu 3+ sorption is at its maximum, but dissolution of the substrate and precipitation of Eu 3+ solids are not yet prevalent ([Eu 3+ ] = 5.0 × 10 −5 mol L −1 , pH = 8.0, 0.1 M NaCl as background electrolyte, in air). These conditions are reasonably close to observed pH values and ionic strengths of ground water in several granitic formations 30–33 .…”

Section: Introductionsupporting

confidence: 87%

Sorption of Eu(III) on Eibenstock granite studied by µTRLFS: A novel spatially-resolved luminescence-spectroscopic technique

Molodtsov

Schymura

Rothe

et al. 2019

Sci Rep

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In this study a novel technique, micro-focus time-resolved laser-induced luminescence spectroscopy (µTRLFS) is presented to investigate heterogeneous systems like granite (mainly consisting of quartz, feldspar, and mica), regarding their sorption behavior. µTRLFS is a spatially-resolved upgrade of conventional TRLFS, which allows point-by-point analysis of single minerals by reducing the beam size of the analytic laser beam to below the size of mineral grains. This provides visualization of sorption capacity as well as speciation of a luminescent probe, here Eu 3+ . A thin-section of granitic rock from Eibenstock, Saxony, Germany was analyzed regarding its mineralogy with microprobe X-ray fluorescence (µXRF) and electron probe microanalysis (EPMA). Afterwards, it was reacted with 5.0 × 10 −5 mol/L Eu 3+ at pH 8.0 and uptake was quantified by autoradiography. Finally, the µTRLFS studies were conducted. The results clearly show that the materials interact differently with Eu 3+ , and often even on one mineral grain different speciations can be found. Alkali-feldspar shows very high uptake, with an inhomogeneous distribution, and intermediate sorption strength. On quartz uptake is almost 10-fold lower, while the complexation strength is higher than on feldspar. This may be indicative of adsorption only at surface defect sites, in accordance with low hydration of the observed species.

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Section: Introductionsupporting

confidence: 87%

Sorption of Eu(III) on Eibenstock granite studied by µTRLFS: A novel spatially-resolved luminescence-spectroscopic technique

Molodtsov

Schymura

Rothe

et al. 2019

Sci Rep

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“…The details of the Eu 3+ environment in crystalline structures can be obtained from the combined excitation ( 5 D 0 ← 7 F 0 ) and fluorescence emission ( 5 D 0 → 7 F J , J = 1, 2) spectra. Eu 3+ TRLFS is a versatile tool that can respond to small structural differences for a luminescent center in solids, solutions and at the interface. − Eu 3+ is considered the most extensively used spectroscopic probe, attributable to its high sensitivity and relatively simple luminescence spectrum. The use of optical spectra of Eu 3+ in solving complex problems in inorganic chemistry has been studied extensively among many important natural minerals such as apatite (Ca 5 (PO 4 ) 3 X, X = Cl – , OH – , or F – ), , calcite (CaCO 3 ), and alumina (Al 2 O 3 ). , …”

Section: Materials and Methodsmentioning

confidence: 99%

Incorporation of Europium(III) into Scheelite-Related Host Matrixes ABO₄ (A = Ca²⁺, Sr²⁺, Ba²⁺; B = W⁶⁺, Mo⁶⁺): Role of A and B Sites on the Dopant Site Distribution and Photoluminescence

Xiao

Schmidt

2017

Inorg. Chem.

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Scheelite- and powellite-related materials doped with trivalent lanthanides or actinides have been the subject of extensive research due to their important role in mineralogical, technological, and environmental implications. Detailed structural knowledge of these solid solutions is essential for understanding their physicochemical properties and predicting material properties. In this work, we conduct a comprehensive spectroscopic analysis by means of polarization-dependent site-selective time-resolved laser-induced fluorescence spectroscopy, to delineate the influence of the host phase cations for a series of scheelite-type matrixes based on a general formula of ABO (A = Ca, Sr, Ba; B = W, Mo) on the local environment of the Eu dopant. Eu has been used as a luminescent probe to access the local structural environment of crystalline substitutional sites suitable for trivalent lanthanide or actinide occupation. Our results show that the lattice distortion is overall minor, but increases with increasing mismatch of host and guest cation size. We observe a linear dependence of Eu's excitation energy on the host cation size and the A-O bond distance, which can be used to determine the hitherto unknown Eu-O bond distance in NaEu(WO). A value of 2.510 Å was determined, somewhat larger than a previously reported number for NaEu(MoO). The results also show clear evidence that the local coordination environment of Eu in WO materials is more symmetrical than in their isostructural MoO counterparts. The detailed spectroscopic interpretation conducted in this study resolves the relation between local distortion around a dopant and the host phase cations in structural disordered materials and may give novel insights with respect to rational design and tailoring of functional materials.

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“…Bonales et al reported spent nuclear fuel oxidizes into U 3 O 8 upon exposure to air or into uranyl carbonates and silicates if exposed to groundwater from Sierra Albarrana (Spain) [71,233]. Schmeide et al explored the redox behavior of uranyl on silicate rock (diorite) surfaces under anoxic conditions and found that uranyl carbonate species reduced the affinity of U(VI) to mineral surfaces and stabilized soluble high valence species in solution [234]. In a final example, Traboulsi et al used Raman spectroscopy to explore alpha radiolysis of water and oxidation of solid UO 2 to form uranyl peroxide species [66,235].…”

Section: Surface Speciation Studied By Ir and Raman Spectroscopiesmentioning

confidence: 99%

Detection and identification of solids, surfaces, and solutions of uranium using vibrational spectroscopy

Haes

Forbes

2018

Coordination Chemistry Reviews

133

128

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The purpose of this review is to provide an overview of uranium speciation using vibrational spectroscopy methods including Raman and IR. Uranium is a naturally occurring, radioactive element that is utilized in the nuclear energy and national security sectors. Fundamental uranium chemistry is also an active area of investigation due to ongoing questions regarding the participation of 5f orbitals in bonding, variation in oxidation states and coordination environments, and unique chemical and physical properties. Importantly, uranium speciation affects fate and transportation in the environment, influences bioavailability and toxicity to human health, controls separation processes for nuclear waste, and impacts isotopic partitioning and geochronological dating. This review article provides a thorough discussion of the vibrational modes for U(IV), U(V), and U(VI) and applications of infrared absorption and Raman scattering spectroscopies in the identification and detection of both naturally occurring and synthetic uranium species in solid and solution states. The vibrational frequencies of the uranyl moiety, including both symmetric and asymmetric stretches are sensitive to the coordinating ligands and used to identify individual species in water, organic solvents, and ionic liquids or on the surface of materials. Additionally, vibrational spectroscopy allows for the in situ detection and real-time monitoring of chemical reactions involving uranium. Finally, techniques to enhance uranium species signals with vibrational modes are discussed to expand the application of vibrational spectroscopy to biological, environmental, inorganic, and materials scientists and engineers.

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Interaction of U(VI) with Äspö diorite: A batch and in situ ATR FT-IR sorption study

Cited by 28 publications

References 39 publications

Sorption of Eu(III) on Eibenstock granite studied by µTRLFS: A novel spatially-resolved luminescence-spectroscopic technique

Sorption of Eu(III) on Eibenstock granite studied by µTRLFS: A novel spatially-resolved luminescence-spectroscopic technique

Incorporation of Europium(III) into Scheelite-Related Host Matrixes ABO₄ (A = Ca²⁺, Sr²⁺, Ba²⁺; B = W⁶⁺, Mo⁶⁺): Role of A and B Sites on the Dopant Site Distribution and Photoluminescence

Detection and identification of solids, surfaces, and solutions of uranium using vibrational spectroscopy

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Interaction of U(VI) with Äspö diorite: A batch and in situ ATR FT-IR sorption study

Cited by 28 publications

References 39 publications

Sorption of Eu(III) on Eibenstock granite studied by µTRLFS: A novel spatially-resolved luminescence-spectroscopic technique

Sorption of Eu(III) on Eibenstock granite studied by µTRLFS: A novel spatially-resolved luminescence-spectroscopic technique

Incorporation of Europium(III) into Scheelite-Related Host Matrixes ABO4 (A = Ca2+, Sr2+, Ba2+; B = W6+, Mo6+): Role of A and B Sites on the Dopant Site Distribution and Photoluminescence

Detection and identification of solids, surfaces, and solutions of uranium using vibrational spectroscopy

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Incorporation of Europium(III) into Scheelite-Related Host Matrixes ABO₄ (A = Ca²⁺, Sr²⁺, Ba²⁺; B = W⁶⁺, Mo⁶⁺): Role of A and B Sites on the Dopant Site Distribution and Photoluminescence