Solubility and Thermodynamic Investigation of Meta-Autunite Group Uranyl Arsenate Solids with Monovalent Cations Na and K

Isabel Meza; Jorge Gonzalez-Estrella; Peter C. Burns; Virginia Rodriguez; Carmen A. Velasco; Ginger E. Sigmon; Jennifer E.S. Szymanowski; Tori Z. Forbes; Lindsey M. Applegate; Abdul Mehdi S. Ali; Peter Lichtner; José M. Cerrato

doi:10.1021/acs.est.2c06648

Solubility and Thermodynamic Investigation of Meta-Autunite Group Uranyl Arsenate Solids with Monovalent Cations Na and K

Isabel Meza
, Jorge Gonzalez-Estrella
, Peter C. Burns
, Virginia Rodriguez
, Carmen A. Velasco
, Ginger E. Sigmon
, Jennifer E.S. Szymanowski
, Tori Z. Forbes
, Lindsey M. Applegate
, Abdul Mehdi S. Ali
, Peter Lichtner
, José M. Cerrato

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

5 Scopus citations

Abstract

We investigated the aqueous solubility and thermodynamic properties of two meta-autunite group uranyl arsenate solids (UAs). The measured solubility products (log K_sp) obtained in dissolution and precipitation experiments at equilibrium pH 2 and 3 for NaUAs and KUAs ranged from −23.50 to −22.96 and −23.87 to −23.38, respectively. The secondary phases (UO₂)(H₂AsO₄)₂(H₂O)_(s) and trögerite, (UO₂)₃(AsO₄)₂·12H₂O_(s), were identified by powder X-ray diffraction in the reacted solids of KUA precipitation experiments (pH 2) and NaUAs dissolution and precipitation experiments (pH 3), respectively. The identification of these secondary phases in reacted solids suggest that H₃O⁺ co-occurring with Na or K in the interlayer region can influence the solubilities of uranyl arsenate solids. The standard-state enthalpy of formation from the elements (ΔH_f-el) of NaUAs is −3025 ± 22 kJ mol^-1 and for KUAs is −3000 ± 28 kJ mol^-1 derived from measurements by drop solution calorimetry, consistent with values reported in other studies for uranyl phosphate solids. This work provides novel thermodynamic information for reactive transport models to interpret and predict the influence of uranyl arsenate solids on soluble concentrations of U and As in contaminated waters affected by mining legacy and other anthropogenic activities.

Original language	English
Pages (from-to)	255-265
Number of pages	11
Journal	Environmental Science and Technology
Volume	57
Issue number	1
DOIs	https://doi.org/10.1021/acs.est.2c06648
State	Published - Jan 10 2023
Externally published	Yes

Funding

Funding for this research was provided by the National Science Foundation (CAREER Award 1652619, CREST Award 1914490) and the National Institute of Environmental Health Sciences (Superfund Research Program Awards 1 P42 ES025589 and R01ES027145). P.C.B.’s contribution to this work was funded by the Chemical Sciences, Geosciences and Biosciences Division, Office of Basic Energy Sciences, Office of Science, U.S. Department of Energy, Grant No. DE-FG02-07ER15880. Partial funding for the PerkinElmer NexION ICP/MS coupled with the ESI SeaFast SP3 was provided by the UNM Office of the Vice President for Research (OVPR) and the College of Art and Sciences. We also would like to acknowledge PerkinElmer and ESI for their valuable technical and applications support for the use of their analytical instruments used to support this research project and providing quality data. Any opinions, findings, and conclusions or recommendations expressed in this publication are those of the author(s) and do not necessarily reflect the views of the National Science Foundation, the National Institutes of Health, or the U.S. Department of Energy. The TOC art was created with www.BioRender.com.

Keywords

arsenate
interlayer cation
solubility
thermodynamic
uranyl

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10.1021/acs.est.2c06648

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Meza, I., Gonzalez-Estrella, J., Burns, P. C., Rodriguez, V., Velasco, C. A., Sigmon, G. E., Szymanowski, J. E. S., Forbes, T. Z., Applegate, L. M., Ali, A. M. S., Lichtner, P., & Cerrato, J. M. (2023). Solubility and Thermodynamic Investigation of Meta-Autunite Group Uranyl Arsenate Solids with Monovalent Cations Na and K. Environmental Science and Technology, 57(1), 255-265. https://doi.org/10.1021/acs.est.2c06648

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title = "Solubility and Thermodynamic Investigation of Meta-Autunite Group Uranyl Arsenate Solids with Monovalent Cations Na and K",

abstract = "We investigated the aqueous solubility and thermodynamic properties of two meta-autunite group uranyl arsenate solids (UAs). The measured solubility products (log Ksp) obtained in dissolution and precipitation experiments at equilibrium pH 2 and 3 for NaUAs and KUAs ranged from −23.50 to −22.96 and −23.87 to −23.38, respectively. The secondary phases (UO2)(H2AsO4)2(H2O)(s) and tr{\"o}gerite, (UO2)3(AsO4)2·12H2O(s), were identified by powder X-ray diffraction in the reacted solids of KUA precipitation experiments (pH 2) and NaUAs dissolution and precipitation experiments (pH 3), respectively. The identification of these secondary phases in reacted solids suggest that H3O+ co-occurring with Na or K in the interlayer region can influence the solubilities of uranyl arsenate solids. The standard-state enthalpy of formation from the elements (ΔHf-el) of NaUAs is −3025 ± 22 kJ mol-1 and for KUAs is −3000 ± 28 kJ mol-1 derived from measurements by drop solution calorimetry, consistent with values reported in other studies for uranyl phosphate solids. This work provides novel thermodynamic information for reactive transport models to interpret and predict the influence of uranyl arsenate solids on soluble concentrations of U and As in contaminated waters affected by mining legacy and other anthropogenic activities.",

keywords = "arsenate, interlayer cation, solubility, thermodynamic, uranyl",

author = "Isabel Meza and Jorge Gonzalez-Estrella and Burns, \{Peter C.\} and Virginia Rodriguez and Velasco, \{Carmen A.\} and Sigmon, \{Ginger E.\} and Szymanowski, \{Jennifer E.S.\} and Forbes, \{Tori Z.\} and Applegate, \{Lindsey M.\} and Ali, \{Abdul Mehdi S.\} and Peter Lichtner and Cerrato, \{Jos{\'e} M.\}",

note = "Publisher Copyright: {\textcopyright} 2022 American Chemical Society.",

year = "2023",

month = jan,

day = "10",

doi = "10.1021/acs.est.2c06648",

language = "English",

volume = "57",

pages = "255--265",

journal = "Environmental Science and Technology",

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Meza, I, Gonzalez-Estrella, J, Burns, PC, Rodriguez, V, Velasco, CA, Sigmon, GE, Szymanowski, JES, Forbes, TZ, Applegate, LM, Ali, AMS, Lichtner, P & Cerrato, JM 2023, 'Solubility and Thermodynamic Investigation of Meta-Autunite Group Uranyl Arsenate Solids with Monovalent Cations Na and K', Environmental Science and Technology, vol. 57, no. 1, pp. 255-265. https://doi.org/10.1021/acs.est.2c06648

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T1 - Solubility and Thermodynamic Investigation of Meta-Autunite Group Uranyl Arsenate Solids with Monovalent Cations Na and K

AU - Meza, Isabel

AU - Gonzalez-Estrella, Jorge

AU - Burns, Peter C.

AU - Rodriguez, Virginia

AU - Velasco, Carmen A.

AU - Sigmon, Ginger E.

AU - Szymanowski, Jennifer E.S.

AU - Forbes, Tori Z.

AU - Applegate, Lindsey M.

AU - Ali, Abdul Mehdi S.

AU - Lichtner, Peter

AU - Cerrato, José M.

PY - 2023/1/10

Y1 - 2023/1/10

N2 - We investigated the aqueous solubility and thermodynamic properties of two meta-autunite group uranyl arsenate solids (UAs). The measured solubility products (log Ksp) obtained in dissolution and precipitation experiments at equilibrium pH 2 and 3 for NaUAs and KUAs ranged from −23.50 to −22.96 and −23.87 to −23.38, respectively. The secondary phases (UO2)(H2AsO4)2(H2O)(s) and trögerite, (UO2)3(AsO4)2·12H2O(s), were identified by powder X-ray diffraction in the reacted solids of KUA precipitation experiments (pH 2) and NaUAs dissolution and precipitation experiments (pH 3), respectively. The identification of these secondary phases in reacted solids suggest that H3O+ co-occurring with Na or K in the interlayer region can influence the solubilities of uranyl arsenate solids. The standard-state enthalpy of formation from the elements (ΔHf-el) of NaUAs is −3025 ± 22 kJ mol-1 and for KUAs is −3000 ± 28 kJ mol-1 derived from measurements by drop solution calorimetry, consistent with values reported in other studies for uranyl phosphate solids. This work provides novel thermodynamic information for reactive transport models to interpret and predict the influence of uranyl arsenate solids on soluble concentrations of U and As in contaminated waters affected by mining legacy and other anthropogenic activities.

AB - We investigated the aqueous solubility and thermodynamic properties of two meta-autunite group uranyl arsenate solids (UAs). The measured solubility products (log Ksp) obtained in dissolution and precipitation experiments at equilibrium pH 2 and 3 for NaUAs and KUAs ranged from −23.50 to −22.96 and −23.87 to −23.38, respectively. The secondary phases (UO2)(H2AsO4)2(H2O)(s) and trögerite, (UO2)3(AsO4)2·12H2O(s), were identified by powder X-ray diffraction in the reacted solids of KUA precipitation experiments (pH 2) and NaUAs dissolution and precipitation experiments (pH 3), respectively. The identification of these secondary phases in reacted solids suggest that H3O+ co-occurring with Na or K in the interlayer region can influence the solubilities of uranyl arsenate solids. The standard-state enthalpy of formation from the elements (ΔHf-el) of NaUAs is −3025 ± 22 kJ mol-1 and for KUAs is −3000 ± 28 kJ mol-1 derived from measurements by drop solution calorimetry, consistent with values reported in other studies for uranyl phosphate solids. This work provides novel thermodynamic information for reactive transport models to interpret and predict the influence of uranyl arsenate solids on soluble concentrations of U and As in contaminated waters affected by mining legacy and other anthropogenic activities.

KW - arsenate

KW - interlayer cation

KW - solubility

KW - thermodynamic

KW - uranyl

UR - https://www.scopus.com/pages/publications/85144350275

U2 - 10.1021/acs.est.2c06648

DO - 10.1021/acs.est.2c06648

M3 - Article

C2 - 36525634

AN - SCOPUS:85144350275

SN - 0013-936X

VL - 57

SP - 255

EP - 265

JO - Environmental Science and Technology

JF - Environmental Science and Technology

IS - 1

ER -

Solubility and Thermodynamic Investigation of Meta-Autunite Group Uranyl Arsenate Solids with Monovalent Cations Na and K

Abstract

Funding

Keywords

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