Comparison of the kinetic rate law parameters for the dissolution of natural and synthetic autunite in the presence of aqueous bicarbonate ions

Gudavalli, Ravi K.P.; Katsenovich, Yelena P.; Wellman, Dawn M.; Idarraga, Melina; Lagos, Leonel E.; Tansel, Berrin

doi:10.1016/j.chemgeo.2013.05.038

Title: Comparison of the kinetic rate law parameters for the dissolution of natural and synthetic autunite in the presence of aqueous bicarbonate ions

Journal Article · Thu Aug 01 00:00:00 EDT 2013 · Chemical Geology

DOI:https://doi.org/10.1016/j.chemgeo.2013.05.038· OSTI ID:1086708

Gudavalli, Ravi K.P.; Katsenovich, Yelena P.; Wellman, Dawn M.; Idarraga, Melina; Lagos, Leonel E.; Tansel, Berrin

This research evaluated the effect of aqueous hydrogen carbonate solutions on the uranium rate of release from natural Ca-autunite and quantified the process kinetic rate law for a better prediction of the stability of autunite-group minerals. Testing was accomplished via a single-pass flow-through (SPFT) apparatus using buffered aqueous bicarbonate solutions (0.0005 to 0.003 M) at temperatures of 23–90 °C and pH values of 7–11. The release rate of uranium from Ca-autunite was directly correlated to increasing concentrations of hydrogen carbonate solutions and showed strong pH dependency. Ca-autunite kinetic rate law parameters were compared to the values obtained for synthetic Na-autunite. The power law coefficient and intrinsic rate constant were higher at pH 9–11 for Ca-autunite than for Na-autunite. The lower stability of Ca-autunite was attributed to the high Ca-autunite surface cracking, fractures and basal plane cleavages as compared to Na-autunite and the combined effect of the formation of aqueous uranyl–carbonate and calcium uranyl carbonate species as a driving force for uranium(VI) detachment and the formation of secondary Ca–P hydroxyapatite and uranyl phosphate mineral phases as a driving force for phosphate and calcium detachment controlling the net release of elements.

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Research Organization:: Florida International Univ. (FIU), Miami, FL (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Environmental Management (EM)

DOE Contract Number:: EM0000598; AC05-76RL01830

OSTI ID:: 1086708

Report Number(s):: DOE/EM0000598/FIU-ARC-2012-800000438-12c-216

Journal Information:: Chemical Geology, Vol. 351; ISSN 0009-2541

Publisher:: Elsevier

Country of Publication:: United States

Language:: English

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42 ENGINEERING
54 ENVIRONMENTAL SCIENCES
Autunite
Dissolution
Uranium
Activation energy
Enthalpy
Bicarbonate

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