Infrared and Raman spectra of uranyl(VI) oxo-hydroxo complexes in acid aqueous solutions: a chemometric study

Quilès, Fabienne; Burneau, A.

doi:10.1016/s0924-2031(00)00067-9

Cited by 72 publications

(85 citation statements)

References 21 publications

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“…It shifts from ca. 960 cm -1 to 950 cm -1 at temperatures from 25 ºC to 275 ºC; the lower-wavenumber shift should be ascribed to the ion association between UO2 2+ and SO4 2- [18,33]. The va(UO2 2+ ) band is weak in the Urich phase and cannot be detected at temperatures above 350 ºC.…”

Section: Ion Association Between Uo2 2+ and So4 2-mentioning

confidence: 91%

In situ observations of liquid–liquid phase separation in aqueous ZnSO4 solutions at temperatures up to 400 °C: Implications for Zn2+–SO42− association and evolution of submarine hydrothermal fluids

Wang

Wan

et al. 2016

Geochimica et Cosmochimica Acta

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spectroscopic observations of the liquid-liquid immiscibility in aqueous uranyl sulfate solutions at temperatures up to 420 circ C, The Journal of Supercritical Fluids http://dx.doi.org/10. 1016/j.supflu.2016.03.005 This is a PDF file of an unedited manuscript that has been accepted for publication. As a service to our customers we are providing this early version of the manuscript. The manuscript will undergo copyediting, typesetting, and review of the resulting proof before it is published in its final form. Please note that during the production process errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal pertain. 2. The immiscible liquids are either UO2SO4-rich (Urich) or UO2SO4-poor (Upoor).3. Analyses of UO2 2+ and SO4 2-spectra imply increasing ion association upon heating.4. Decrease of ion hydration in Urich phase due to increasing concentration upon heating.5. Reversible strong UO2 2+ -SO4 2-association results in the liquid-liquid immiscibility. AbstractThe phase behaviors of aqueous UO2SO4 solutions were investigated in situ with a microscope and a Raman spectrometer at temperatures from 25 to 420 ºC. Resultsshow that aqueous UO2SO4 solution separated into UO2SO4-rich (Urich) and UO2SO4-poor (Upoor) liquid phases coexisted with a vapor phase at ≥285.8±0.5 o C.Both visual and Raman spectroscopic investigations suggest that a reversible strong UO2 2+ -SO4 2-association was responsible for the liquid-liquid immiscibility in aqueous UO2SO4 solutions. Main evidences were summarized as: (1)

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Section: Ion Association Between Uo2 2+ and So4 2-mentioning

confidence: 91%

In situ observations of liquid–liquid phase separation in aqueous ZnSO4 solutions at temperatures up to 400 °C: Implications for Zn2+–SO42− association and evolution of submarine hydrothermal fluids

Wang

Wan

et al. 2016

Geochimica et Cosmochimica Acta

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“…Computed harmonic frequencies are unscaled. [1,2,4,61], suggesting that the ligands are more weakly bound in the gas phase, since the ⌬ asym-sym tends to vary inversely with metal-carboxylate binding strength [13].…”

Section: Infrared Multiple Photon Dissociation (Irmpd)mentioning

confidence: 99%

“…A comparison of the frequencies of the analogous stretches measured in the condensed phases for what are thought to be monodentate acetate [1,2,4,61] show that the gas-phase asym value is blue shifted by about 80 cm Ϫ1 , while the sym is red shifted by slightly more than 100 cm Ϫ1 . Thus, while these frequencies do not closely resemble those assigned to monodentate acetate in the condensed phase, they begin to approach values measured for gas-phase acetic acid [62], in which the proton is not considered to be evenly shared by the oxygen atoms [63].…”

Section: Infrared Multiple Photon Dissociation (Irmpd)mentioning

confidence: 99%

Variable denticity in carboxylate binding to the uranyl coordination complexes

Groenewold

Jong

Stipdonk

2010

J. Am. Soc. Mass Spectrom.

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Tris-carboxylate complexes of uranyl [UO 2 ] 2ϩ with acetate and benzoate were generated using electrospray ionization mass spectrometry, and then isolated in a Fourier transform ion cyclotron resonance mass spectrometer. Wavelength-selective infrared multiple photon dissociation (IRMPD) of the tris-acetato uranyl anion resulted in a redox elimination of an acetate radical, which was used to generate an IR spectrum that consisted of six prominent absorption bands. These were interpreted with the aid of density functional theory calculations in terms of symmetric and antisymmetric ϪCO 2 stretches of the monodentate and bidentate acetate, CH 3 bending and umbrella vibrations, and a uranyl O-U-O asymmetric stretch. The comparison of the calculated and measured IR spectra indicated that the predominant conformer of the tris-acetate complex contained two acetate ligands bound in a bidentate fashion, while the third acetate was monodentate. In similar fashion, the tris-benzoate uranyl anion was formed and photodissociated by loss of a benzoate radical, enabling measurement of the infrared spectrum that was in close agreement with that calculated for a structure containing one monodentate and two bidentate benzoate ligands.

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“…The ATR-FTIR spectra of these sorption samples exhibit the m 3 ðUO 2 2þ Þ stretching vibration at 903 cm À1 . The assignment of this band to dissolved UO 2 2þ carbonato or hydroxo complexes can be ruled out because these compounds are known to excite bands at substantially higher wavenumbers (>920 cm À1 , Khilla et al, 1986;Liger et al, 1999;Quilès and Burneau, 2000). In addition, none of the measured ATR-FTIR spectra show any vibrational indication of secondary minerals of uranyl hydrous oxides from the schoepite family ([(UO 2 ) 8 O 2 (OH) 12 ] (H 2 O) x , x 6 12) in the samples.…”

Section: Refinement Of the U(vi)-ferrihydrite Complexmentioning

confidence: 99%

Molecular characterization of uranium(VI) sorption complexes on iron(III)-rich acid mine water colloids

Ulrich

Roßberg

Foerstendorf

et al. 2006

Geochimica et Cosmochimica Acta

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Infrared and Raman spectra of uranyl(VI) oxo-hydroxo complexes in acid aqueous solutions: a chemometric study

Cited by 72 publications

References 21 publications

In situ observations of liquid–liquid phase separation in aqueous ZnSO4 solutions at temperatures up to 400 °C: Implications for Zn2+–SO42− association and evolution of submarine hydrothermal fluids

In situ observations of liquid–liquid phase separation in aqueous ZnSO4 solutions at temperatures up to 400 °C: Implications for Zn2+–SO42− association and evolution of submarine hydrothermal fluids

Variable denticity in carboxylate binding to the uranyl coordination complexes

Molecular characterization of uranium(VI) sorption complexes on iron(III)-rich acid mine water colloids

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