A cryogenic fluorescence spectroscopic study of uranyl carbonate, phosphate, and oxyhydroxide minerals

Journal Article · Mon Nov 03 04:00:00 EST 2008 · Radiochimica Acta, 96(9-11):591-598

DOI:https://doi.org/10.1524/ract.2008.1541· OSTI ID:946378

Wang, Zheming; Zachara, John M; Liu, Chongxuan; Gassman, Paul L; Felmy, Andrew R; Clark, Sue B

In this work we have applied liquid-helium temperature (LHeT) time-resolved laser-induced fluorescence spectroscopy (TRLIF) to characterize a series of natural and synthetic minerals of uranium carbonate, phosphate and oxyhydroxides including rutherfordine, zellerite, liebigite, phosphuranylite, meta-autunite, meta-torbernite, uranyl phosphate, sodium-uranyl-phosphate, bequerelite, clarkeite, curite, schoepite and compregnacite, and compared their spectral characteristics among these minerals as well as our previously published data on uranyl silicates. For the carbonate minerals, the fluorescence spectra depend on the stoichiometry of the mineral. For the phosphate minerals the fluorescence spectra closely resemble each other despite the differences in their composition and structure. For all uranium oxyhydroxides, the fluorescence spectra are largely red-shifted as compared with those of the uranium carbonates and phosphates and their vibronic bands are broadened and less resolved. The much enhanced spectra resolution at LHeT allows more accurate calculation of the O=U=O symmetrical stretch frequency, ν1, corresponding to the average spacing of the vibronic peaks of the fluorescence spectra and the spectral origin as reflected by the position of the first vibronic band. It was found that both the average ν1 and λ1 values correlate well with the average basicity of the inorganic anion.

• Research Organization: Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
• Sponsoring Organization: USDOE
• DOE Contract Number: AC05-76RL01830
• OSTI ID: 946378
• Report Number(s): PNNL-SA-57377; 4691a; KP1504010
• Journal Information: Radiochimica Acta, 96(9-11):591-598, Journal Name: Radiochimica Acta, 96(9-11):591-598 Journal Issue: 9-11 Vol. 96; ISSN RAACAP; ISSN 0033-8230
• Country of Publication: United States
• Language: English

Related Subjects

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS
CARBONATE MINERALS
CLARKEITE
CRYOGENICS
Environmental Molecular Sciences Laboratory
FLUORESCENCE
FLUORESCENCE SPECTROSCOPY
ORIGIN
OXIDE MINERALS
PHOSPHATE MINERALS
PHOSPHATES
RESOLUTION
SCHOEPITE
SPECTRA
STOICHIOMETRY
URANIUM
URANIUM CARBONATES
URANIUM MINERALS
URANYL CARBONATES
URANYL PHOSPHATES
URANYL SILICATES