Thermodynamic Properties of Autunite, Uranyl Hydrogen Phosphate, and Uranyl Orthophosphate from Solubility and Calorimetric Measurements

Gorman-Lewis, Drew; Shvareva, Tatiana; Kubatko, Karrie-Ann; Burns, Peter C.; Wellman, Dawn M.; McNamara, Bruce; Szymanowski, Jennifer S.; Navrotsky, Alexandra; Fein, Jeremy B.

doi:10.1021/es9012933

Thermodynamic Properties of Autunite, Uranyl Hydrogen Phosphate, and Uranyl Orthophosphate from Solubility and Calorimetric Measurements

Journal Article · Thu Sep 03 04:00:00 EDT 2009 · Environmental Science and Technology

DOI:https://doi.org/10.1021/es9012933· OSTI ID:1064429

Gorman-Lewis, Drew ^[1]; Shvareva, Tatiana ^[2]; Kubatko, Karrie-Ann ^[2]; Burns, Peter C. ^[2]; Wellman, Dawn M. ^[2]; McNamara, Bruce ^[2]; Szymanowski, Jennifer S. ^[2]; Navrotsky, Alexandra ^[2]; Fein, Jeremy B. ^[2]

Department of Civil Engineering and Geological Sciences, University of Notre Dame, 156 Fitzpatrick Hall, Notre Dame, Indiana 46556, Peter A. Rock Thermochemistry Laboratory, University of California Davis, One Shields Avenue, Davis, California 95616, and Pacific Northwest National Laboratory, P.O. Box 999, Richland, Washington 99352; University of Notre Dame
Department of Civil Engineering and Geological Sciences, University of Notre Dame, 156 Fitzpatrick Hall, Notre Dame, Indiana 46556, Peter A. Rock Thermochemistry Laboratory, University of California Davis, One Shields Avenue, Davis, California 95616, and Pacific Northwest National Laboratory, P.O. Box 999, Richland, Washington 99352

In this study, we use solubility and drop-solution calorimetry measurements to determine the thermodynamic properties of the uranyl phosphate phases autunite, uranyl hydrogen phosphate, and uranyl orthophosphate. Conducting the solubility measurements from both supersaturated and undersaturated conditions and under different pH conditions rigorously demonstrates attainment of equilibrium and yields well-constrained solubility product values. We use the solubility data and the calorimetry data, respectively,to calculate standard-state Gibbs free energies of formation and standard-state enthalpies of formation for these uranyl phosphate phases Combining these results allows us also to calculate the standard-state entropy of formation for each mineral phase. The results from this study are part of a combined effort to develop reliable and internally consistent thermodynamic data for environmentally relevant uranyl minerals, Data such as these are required to optimize and quantitatively assess the effect of phosphate amendment remediation technologies for uranium contaminated systems.

Research Organization:: University of Notre Dame, IN (United States)

Sponsoring Organization:: USDOE SC Office of Biological and Environmental Research (SC-23)

DOE Contract Number:: FG02-07ER64395

OSTI ID:: 1064429

Report Number(s):: DOE/ER/64395-1

Journal Information:: Environmental Science and Technology, Journal Name: Environmental Science and Technology Journal Issue: 19 Vol. 43; ISSN 0013-936X

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

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