Thermodynamic properties of autunite, uranyl hydrogen phosphate, and uranyl orthophosphate from solubility and calorimetric measurements

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

doi:10.1021/es9012933

Thermodynamic properties of autunite, uranyl hydrogen phosphate, and uranyl orthophosphate from solubility and calorimetric measurements

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

Research output: Contribution to journal › Article › peer-review

70 Scopus citations

Abstract

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.

Original language	English (US)
Pages (from-to)	7416-7422
Number of pages	7
Journal	Environmental Science and Technology
Volume	43
Issue number	19
DOIs	https://doi.org/10.1021/es9012933
State	Published - Oct 1 2009
Externally published	Yes

ASJC Scopus subject areas

Chemistry(all)
Environmental Chemistry

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Gorman-Lewis, D., Shvareva, T., Kubatko, K. A., Burns, P. C., Wellman, D. M., Mcnamara, B., Szymanowski, J. E. S., Navrotsky, A., & Fein, J. B. (2009). Thermodynamic properties of autunite, uranyl hydrogen phosphate, and uranyl orthophosphate from solubility and calorimetric measurements. Environmental Science and Technology, 43(19), 7416-7422. https://doi.org/10.1021/es9012933

Gorman-Lewis, D, Shvareva, T, Kubatko, KA, Burns, PC, Wellman, DM, Mcnamara, B, Szymanowski, JES, Navrotsky, A & Fein, JB 2009, 'Thermodynamic properties of autunite, uranyl hydrogen phosphate, and uranyl orthophosphate from solubility and calorimetric measurements', Environmental Science and Technology, vol. 43, no. 19, pp. 7416-7422. https://doi.org/10.1021/es9012933

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abstract = "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.",

author = "Drew Gorman-Lewis and Tatiana Shvareva and Kubatko, {Karrie Ann} and Burns, {Peter C.} and Wellman, {Dawn M.} and Bruce Mcnamara and Szymanowski, {Jennifer E.S.} and Alexandra Navrotsky and Fein, {Jeremy B.}",

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AU - Gorman-Lewis, Drew

AU - Shvareva, Tatiana

AU - Kubatko, Karrie Ann

AU - Burns, Peter C.

AU - Wellman, Dawn M.

AU - Mcnamara, Bruce

AU - Szymanowski, Jennifer E.S.

AU - Navrotsky, Alexandra

AU - Fein, Jeremy B.

PY - 2009/10/1

Y1 - 2009/10/1

N2 - 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.

AB - 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.

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Thermodynamic properties of autunite, uranyl hydrogen phosphate, and uranyl orthophosphate from solubility and calorimetric measurements

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