Syntheses and spectroscopic characterization of uranium(VI) silicate minerals

Lehmann, S.; Geipel, Gerhard; Foerstendorf, Harald; Bernhard, Gert

doi:10.1007/s10967-007-7060-z

Cited by 14 publications

(11 citation statements)

References 23 publications

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“…1,2 The main spectroscopic features are usually reported in the literature and spectral attributions have been proposed for many aqueous inorganic complexes [3][4][5][6][7][8][9] and minerals. [10][11][12][13][14][15][16][17][18] The case of the carbonate species is particularly interesting. 8,13,15,[19][20][21] Both anionic complexes UO2(CO3)2 2and UO2(CO3)3 4-are characterized by an absorption spectrum shifted to longer wavelengths as compared with UO2 2+ aqua ion and its hydrolyzed species.…”

Section: Introductionmentioning

confidence: 99%

“…This information is looked for by chemists in order to give the best description of uranium speciation both in solutions and in solids. Time-resolved laser-induced fluorescence spectroscopy (TRLFS) has been widely used for the identification and characterization of U(VI) compounds since it is a non-intrusive, sensitive, and selective technique to detect the luminescence of U(VI) species, even with traces of uranium. , The main spectroscopic features are usually reported in the literature, and spectral attributions have been proposed for many aqueous inorganic complexes − and minerals. − …”

Section: Introductionmentioning

confidence: 99%

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Influence of Alkaline Earth Metal Ions on Structures and Luminescent Properties of Na_mM_nUO₂(CO₃)₃^{(4–m–2n)–} (M = Mg, Ca; m, n = 0–2): Time-Resolved Fluorescence Spectroscopy and Ab Initio Studies

et al. 2020

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HAL is a multidisciplinary open access archive for the deposit and dissemination of scientific research documents, whether they are published or not. The documents may come from teaching and research institutions in France or abroad, or from public or private research centers. L'archive ouverte pluridisciplinaire HAL, est destinée au dépôt et à la diffusion de documents scientifiques de niveau recherche, publiés ou non, émanant des établissements d'enseignement et de recherche français ou étrangers, des laboratoires Influence of alkaline earth metal ions on structures and luminescent properties of Na m M n UO 2 (CO 3) 3 (4-m-2n)-(M = Mg, Ca; m, n = 0-2): time-resolved fluorescence spectroscopy and ab initio studies

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Influence of Alkaline Earth Metal Ions on Structures and Luminescent Properties of Na_mM_nUO₂(CO₃)₃^{(4–m–2n)–} (M = Mg, Ca; m, n = 0–2): Time-Resolved Fluorescence Spectroscopy and Ab Initio Studies

et al. 2020

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“…In addition, the fluorescence emission spectra and decay lifetimes (the two most common TRLFS parameters used for data analysis) of the different species can be used to confirm actinide speciation in aqueous phase environmental media by a “finger‐printing” process. A similar approach has been adopted to develop fluorescence spectra and decay lifetime databases for uranium minerals (Geipel et al, 2000; Lehmann et al, 2008; Wang et al, 2008a; Wang et al, 2008b), which have subsequently been used to identify the solid‐phase speciation of hexavalent uranium [U(VI)] in soils and sediments (Duff et al, 2000; Morris et al, 1996; Um et al, 2009; Um et al, 2010; Wang et al, 2005a,b). Many of these studies have been applied to the determination of U(VI) speciation in soils and sediments of U.S. Department of Energy sites (e.g., Hanford, Fernald, Savannah River), where a range of uranium species have been identified with TRLFS.…”

Section: Applications Of Time‐resolved Laser Fluorescence Spectroscopmentioning

confidence: 99%

Applications of Time-Resolved Laser Fluorescence Spectroscopy to the Environmental Biogeochemistry of Actinides

et al. 2011

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Time-resolved laser fluorescence spectroscopy (TRLFS) is a useful means of identifying certain actinide species resulting from various biogeochemical processes. In general, TRLFS differentiates chemical species of a fluorescent metal ion through analysis of different excitation and emission spectra and decay lifetimes. Although this spectroscopic technique has largely been applied to the analysis of actinide and lanthanide ions having fluorescence decay lifetimes on the order of microseconds, such as UO , Cm, and Eu, continuing development of ultra-fast and cryogenic TRLFS systems offers the possibility to obtain speciation information on metal ions having room-temperature fluorescence decay lifetimes on the order of nanoseconds to picoseconds. The main advantage of TRLFS over other advanced spectroscopic techniques is the ability to determine in situ metal speciation at environmentally relevant micromolar to picomolar concentrations. In the context of environmental biogeochemistry, TRLFS has principally been applied to studies of (i) metal speciation in aqueous and solid phases and (ii) the coordination environment of metal ions sorbed to mineral and bacterial surfaces. In this review, the principles of TRLFS are described, and the literature reporting the application of this methodology to the speciation of actinides in systems of biogeochemical interest is assessed. Significant developments in TRLFS methodology and advanced data analysis are highlighted, and we outline how these developments have the potential to further our mechanistic understanding of actinide biogeochemistry.

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“…The shift in peak location and shape, relative to the aqueous species, has been used to infer the mode (i.e. inner versus outer sphere) of U(VI) sorbed to hematite [31][32][33] and U(VI) and Np(V) sorbed to other minerals [32,[34][35][36][37][38][39][40][41][42] (Table 1). However sorbed Pu(VI) species (and the reduced Pu(IV) species following interaction with a solid phase) have yet to be reported in literature.…”

Section: Introductionmentioning

confidence: 99%

Observations of surface-mediated reduction of Pu(VI) to Pu(IV) on hematite nanoparticles by ATR FT-IR

Emerson

Powell

2015

Radiochimica Acta

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Previous studies have shown that mineral surfaces may facilitate the reduction of plutonium though the mechanisms of the reduction are still unknown. The objective of this study is to use batch sorption and attenuated total reflectance Fourier transform infrared spectroscopy experiments to observe the surface-mediated reduction of plutonium on hematite nanoparticles. These techniques allow for in situ measurement of reduction of plutonium with time and may lead to a better understanding of the mechanisms of surface mediated reduction of plutonium. For the first time, ATR FT-IR peaks for Pu(VI) sorbed to hematite are measured at ∼ 916 cm −1 , respectively. The decrease in peak intensity with time provides a real-time, direct measurement of Pu(VI) reduction on the hematite surface. In this work pseudo first order rate constants estimated at the high loadings (22 mg Pu /g hematite , 1.34 × 10 −6 M Pu /m 2 ) for ATR FT-IR are approximately 10× slower than at trace concentrations based on previous work. It is proposed that the reduced rate constant at higher Pu loadings occurs after the reduction capacity due to trace Fe(II) has been exhausted and is dependent on the oxidation of water and possibly electron shuttling based on the semiconducting nature of hematite. Therefore, the reduction rate at higher loadings is possibly due to the thermodynamic favorability of Pu(IV)-hydroxide complexes.

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Syntheses and spectroscopic characterization of uranium(VI) silicate minerals

Cited by 14 publications

References 23 publications

Influence of Alkaline Earth Metal Ions on Structures and Luminescent Properties of Na_mM_nUO₂(CO₃)₃^{(4–m–2n)–} (M = Mg, Ca; m, n = 0–2): Time-Resolved Fluorescence Spectroscopy and Ab Initio Studies

Influence of Alkaline Earth Metal Ions on Structures and Luminescent Properties of Na_mM_nUO₂(CO₃)₃^{(4–m–2n)–} (M = Mg, Ca; m, n = 0–2): Time-Resolved Fluorescence Spectroscopy and Ab Initio Studies

Applications of Time-Resolved Laser Fluorescence Spectroscopy to the Environmental Biogeochemistry of Actinides

Observations of surface-mediated reduction of Pu(VI) to Pu(IV) on hematite nanoparticles by ATR FT-IR

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Syntheses and spectroscopic characterization of uranium(VI) silicate minerals

Cited by 14 publications

References 23 publications

Influence of Alkaline Earth Metal Ions on Structures and Luminescent Properties of NamMnUO2(CO3)3(4–m–2n)– (M = Mg, Ca; m, n = 0–2): Time-Resolved Fluorescence Spectroscopy and Ab Initio Studies

Influence of Alkaline Earth Metal Ions on Structures and Luminescent Properties of NamMnUO2(CO3)3(4–m–2n)– (M = Mg, Ca; m, n = 0–2): Time-Resolved Fluorescence Spectroscopy and Ab Initio Studies

Applications of Time-Resolved Laser Fluorescence Spectroscopy to the Environmental Biogeochemistry of Actinides

Observations of surface-mediated reduction of Pu(VI) to Pu(IV) on hematite nanoparticles by ATR FT-IR

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Influence of Alkaline Earth Metal Ions on Structures and Luminescent Properties of Na_mM_nUO₂(CO₃)₃^{(4–m–2n)–} (M = Mg, Ca; m, n = 0–2): Time-Resolved Fluorescence Spectroscopy and Ab Initio Studies

Influence of Alkaline Earth Metal Ions on Structures and Luminescent Properties of Na_mM_nUO₂(CO₃)₃^{(4–m–2n)–} (M = Mg, Ca; m, n = 0–2): Time-Resolved Fluorescence Spectroscopy and Ab Initio Studies