Uranyl Surface Speciation on Silica Particles Studied by Time-Resolved Laser-Induced Fluorescence Spectroscopy

Gabriel, Uta; Charlet, Laurent; Schläpfer, C. W.; Vial, Jean-Claude; Brachmann, A.; Geipel, Gerhard

doi:10.1006/jcis.2001.7602

Cited by 89 publications

(129 citation statements)

References 27 publications

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“…Differences in U(VI) adsorption extent to quartz and ferrihydrite as compared to the results of Fox et al (2006) were noted that result from solid-liquid ratio effects. Direct comparisons are not easily made with other previous studies of U(VI) adsorption to smectites Morris et al, 1994;McKinley et al, 1995;Turner et al, 1996;Sylwester et al, 2000;Chisholm-Brause et al, 2001;Hennig et al, 2002;Chisholm-Brause et al, 2004;Kowal-Fouchard et al, 2004;Catalano and Brown, 2005) and quartz or amorphous silica (Glinka et al, 1997;Arnold et al, 1998;Gabriel et al, 2001;Froideval et al, 2003) because of differences in solution pH, U(VI) concentration, solid-to-liquid ratio, and carbonate concentration as well as the procedure of mineral preparation. U(VI) affinity varied by more than two orders of magnitude for the phyllosilicates with the highest K d values observed for chlorites, particularly the ones rich in Mg but poor in Fe (Table 3).…”

Section: U(vi) Adsorption Affinity On Reference Mineralsmentioning

confidence: 90%

“…U(VI) adsorption increased as a function of pH and reached nearly 100% at pH 7 even in the presence of 5 Â 10 À4 mol L À1 fluoride. Similarly, Gabriel et al (2001) …”

Section: Mineralogical Association Of U(vi) In Spp1 Gwfmentioning

confidence: 98%

“…Inner-sphere U(VI) complexes with deprotonated silanols under near-neutral conditions have been identified on quartz by multiple methods (Waite et al, 1994;Reich et al, 1996;Sylwester et al, 2000;Gabriel et al, 2001). In the presence of atmospheric CO 2 , Gabriel et al (2001) identified three surface complexes on amorphous silica: SiO 2 UO 0 2 with a fluorescence lifetime of 170 ± 25 ls that appeared between pH 4 and 7, SiO 2 UO 2 OH À with a fluorescence lifetime of 360 ± 50 ls dominated between pH 6.5 and 8.5, and a non-fluorescent ternary uranyl-silica-carbonate surface complex, SiO 2 UO 2 OHCO 3À 3 , that was present between pH 8-9.…”

Section: U(vi) Surface Speciesmentioning

confidence: 99%

“…Iron oxides, calcium carbonate, quartz/amorphous silica and phyllosilicates can all be important U(VI) adsorbents in subsurface materials Reeder et al, 2000;Gabriel et al, 2001;Reeder et al, 2001;Duff et al, 2002;Chisholm-Brause et al, 2004;Kohler et al, 2004;Chang et al, 2006;Fox et al, 2006). Subsurface sediments are heterogeneous mixture of mineral phases.…”

Section: Introductionmentioning

confidence: 99%

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Determining individual mineral contributions to U(VI) adsorption in a contaminated aquifer sediment: A fluorescence spectroscopy study

Wang

Zachara

Boily

et al. 2011

Geochimica et Cosmochimica Acta

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The adsorption and speciation of U(VI) was investigated on contaminated, fine grained sediment materials from the Hanford 300 area (SPP1 GWF) in simulated groundwater using cryogenic laser-induced U(VI) fluorescence spectroscopy combined with chemometric analysis. A series of reference minerals (montmorillonite, illite, Michigan chlorite, North Carolina chlorite, California clinochlore, quartz and synthetic 6-line ferrihydrite) was used for comparison that represents the mineralogical constituents of SPP1 GWF. Surface area-normalized K d values were measured at U(VI) concentrations of 5 Â 10 À7 and 5 Â 10 À6 mol L À1 that displayed the following affinity series: 6-line-ferrihydrite > North Carolina chlorite % California clinochlore > quartz % Michigan chlorite > illite > montmorillonite. Both time-resolved spectra and asynchronous twodimensional (2D) correlation analysis of SPP1 GWF at different delay times indicated that two major adsorbed U(VI) species were present in the sediment that resembled U(VI) adsorbed on quartz and phyllosilicates. Simulations of the normalized fluorescence spectra confirmed that the speciation of SPP1 GWF was best represented by a linear combination of U(VI) adsorbed on quartz (90%) and phyllosilicates (10%). However, the fluorescence quantum yield for U(VI) adsorbed on phyllosilicates was lower than quartz and, consequently, its fractional contribution to speciation may be underestimated. Spectral comparison with literature data suggested that U(VI) exist primarily as inner-sphere complexes with surface silanol groups on quartz and as surface U(VI) tricarbonate complexes on phyllosilicates. Published by Elsevier Ltd.

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Section: U(vi) Adsorption Affinity On Reference Mineralsmentioning

confidence: 90%

“…U(VI) adsorption increased as a function of pH and reached nearly 100% at pH 7 even in the presence of 5 Â 10 À4 mol L À1 fluoride. Similarly, Gabriel et al (2001) …”

Section: Mineralogical Association Of U(vi) In Spp1 Gwfmentioning

confidence: 98%

Section: U(vi) Surface Speciesmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

Determining individual mineral contributions to U(VI) adsorption in a contaminated aquifer sediment: A fluorescence spectroscopy study

Wang

Zachara

Boily

et al. 2011

Geochimica et Cosmochimica Acta

View full text Add to dashboard Cite

show abstract

“…Therefore, a more likely explanation of the pH effect on the absorption and emission of uranyl in solution is the driving of chemical reactions. Experimentally, it is found that in acidic solutions the uranyl radical tends to be free, and in basic solutions the uranyl radical tends to be bound to carbonates or other ligands (Gabriel, 2001).…”

Section: Solvation Structurementioning

confidence: 99%