Kinetics of Na- and K- uranyl arsenate dissolution

Isabel Meza; Noah Jemison; Jorge Gonzalez-Estrella; Peter C. Burns; Virginia Rodriguez; Ginger E. Sigmon; Jennifer E.S. Szymanowski; Abdul Mehdi S. Ali; Kaelin Gagnon; José M. Cerrato; Peter Lichtner

doi:10.1016/j.chemgeo.2023.121642

Kinetics of Na- and K- uranyl arsenate dissolution

Isabel Meza
, Noah Jemison
, Jorge Gonzalez-Estrella
, Peter C. Burns
, Virginia Rodriguez
, Ginger E. Sigmon
, Jennifer E.S. Szymanowski
, Abdul Mehdi S. Ali
, Kaelin Gagnon
, José M. Cerrato
, Peter Lichtner

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

2 Scopus citations

Abstract

We integrated aqueous chemistry analyses with geochemical modeling to determine the kinetics of the dissolution of Na and K uranyl arsenate solids (UAs_(s)) at acidic pH. Improving our understanding of how UAs_(s) dissolve is essential to predict transport of U and As, such as in acid mine drainage. At pH 2, Na_0.48H_0.52(UO₂)(AsO₄)(H₂O)_2.5(s) (NaUAs_(s)) and K_0.9H_0.1(UO₂)(AsO₄)(H₂O)_2.5(s) (KUAs_(s)) both dissolve with a rate constant of 3.2 × 10⁻⁷ mol m⁻² s⁻¹, which is faster than analogous uranyl phosphate solids. At pH 3, NaUAs_(s) (6.3 × 10⁻⁸ mol m⁻² s⁻¹) and KUAs_(s) (2.0 × 10⁻⁸ mol m⁻² s⁻¹) have smaller rate constants. Steady-state aqueous concentrations of U and As are similarly reached within the first several hours of reaction progress. This study provides dissolution rate constants for UAs_(s), which may be integrated into reactive transport models for risk assessment and remediation of U and As contaminated waters.

Original language	English
Article number	121642
Journal	Chemical Geology
Volume	636
DOIs	https://doi.org/10.1016/j.chemgeo.2023.121642
State	Published - Oct 5 2023
Externally published	Yes

Funding

Funding for this research was provided by the National Science Foundation (CAREER Award 1652619 , CREST Award 1914490 ), the National Institute of Environmental Health Sciences (Superfund Research Program Award 1 P42 ES025589), and the Army Research Office (ARO), Chemical Sciences Branch , Environmental Chemistry Research Area under contract W911NF-21-1-0249 . We would like to thank the Multicultural and Underserved Nanoscience Initiative and the Nanoscale Characterization and Fabrication Laboratory (NSF NanoEarth Award #2025151) at Virginia Tech for the BET analyses. PCB'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, the Army Research Office, or the Department of Energy. We appreciate the editorial handling of Dr. Karen Johannesson and the helpful comments of Dr. Benjamin Tutolo and three anonymous reviewers.

Keywords

Geochemical modeling
Rate constants
Reaction kinetics
Solubility
Uranyl arsenate

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10.1016/j.chemgeo.2023.121642

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title = "Kinetics of Na- and K- uranyl arsenate dissolution",

abstract = "We integrated aqueous chemistry analyses with geochemical modeling to determine the kinetics of the dissolution of Na and K uranyl arsenate solids (UAs(s)) at acidic pH. Improving our understanding of how UAs(s) dissolve is essential to predict transport of U and As, such as in acid mine drainage. At pH 2, Na0.48H0.52(UO2)(AsO4)(H2O)2.5(s) (NaUAs(s)) and K0.9H0.1(UO2)(AsO4)(H2O)2.5(s) (KUAs(s)) both dissolve with a rate constant of 3.2 × 10−7 mol m−2 s−1, which is faster than analogous uranyl phosphate solids. At pH 3, NaUAs(s) (6.3 × 10−8 mol m−2 s−1) and KUAs(s) (2.0 × 10−8 mol m−2 s−1) have smaller rate constants. Steady-state aqueous concentrations of U and As are similarly reached within the first several hours of reaction progress. This study provides dissolution rate constants for UAs(s), which may be integrated into reactive transport models for risk assessment and remediation of U and As contaminated waters.",

keywords = "Geochemical modeling, Rate constants, Reaction kinetics, Solubility, Uranyl arsenate",

author = "Isabel Meza and Noah Jemison and Jorge Gonzalez-Estrella and Burns, \{Peter C.\} and Virginia Rodriguez and Sigmon, \{Ginger E.\} and Szymanowski, \{Jennifer E.S.\} and Ali, \{Abdul Mehdi S.\} and Kaelin Gagnon and Cerrato, \{Jos{\'e} M.\} and Peter Lichtner",

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year = "2023",

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doi = "10.1016/j.chemgeo.2023.121642",

language = "English",

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T1 - Kinetics of Na- and K- uranyl arsenate dissolution

AU - Meza, Isabel

AU - Jemison, Noah

AU - Gonzalez-Estrella, Jorge

AU - Burns, Peter C.

AU - Rodriguez, Virginia

AU - Sigmon, Ginger E.

AU - Szymanowski, Jennifer E.S.

AU - Ali, Abdul Mehdi S.

AU - Gagnon, Kaelin

AU - Cerrato, José M.

AU - Lichtner, Peter

PY - 2023/10/5

Y1 - 2023/10/5

N2 - We integrated aqueous chemistry analyses with geochemical modeling to determine the kinetics of the dissolution of Na and K uranyl arsenate solids (UAs(s)) at acidic pH. Improving our understanding of how UAs(s) dissolve is essential to predict transport of U and As, such as in acid mine drainage. At pH 2, Na0.48H0.52(UO2)(AsO4)(H2O)2.5(s) (NaUAs(s)) and K0.9H0.1(UO2)(AsO4)(H2O)2.5(s) (KUAs(s)) both dissolve with a rate constant of 3.2 × 10−7 mol m−2 s−1, which is faster than analogous uranyl phosphate solids. At pH 3, NaUAs(s) (6.3 × 10−8 mol m−2 s−1) and KUAs(s) (2.0 × 10−8 mol m−2 s−1) have smaller rate constants. Steady-state aqueous concentrations of U and As are similarly reached within the first several hours of reaction progress. This study provides dissolution rate constants for UAs(s), which may be integrated into reactive transport models for risk assessment and remediation of U and As contaminated waters.

AB - We integrated aqueous chemistry analyses with geochemical modeling to determine the kinetics of the dissolution of Na and K uranyl arsenate solids (UAs(s)) at acidic pH. Improving our understanding of how UAs(s) dissolve is essential to predict transport of U and As, such as in acid mine drainage. At pH 2, Na0.48H0.52(UO2)(AsO4)(H2O)2.5(s) (NaUAs(s)) and K0.9H0.1(UO2)(AsO4)(H2O)2.5(s) (KUAs(s)) both dissolve with a rate constant of 3.2 × 10−7 mol m−2 s−1, which is faster than analogous uranyl phosphate solids. At pH 3, NaUAs(s) (6.3 × 10−8 mol m−2 s−1) and KUAs(s) (2.0 × 10−8 mol m−2 s−1) have smaller rate constants. Steady-state aqueous concentrations of U and As are similarly reached within the first several hours of reaction progress. This study provides dissolution rate constants for UAs(s), which may be integrated into reactive transport models for risk assessment and remediation of U and As contaminated waters.

KW - Geochemical modeling

KW - Rate constants

KW - Reaction kinetics

KW - Solubility

KW - Uranyl arsenate

UR - https://www.scopus.com/pages/publications/85169544932

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DO - 10.1016/j.chemgeo.2023.121642

M3 - Article

AN - SCOPUS:85169544932

SN - 0009-2541

VL - 636

JO - Chemical Geology

JF - Chemical Geology

M1 - 121642

ER -

Kinetics of Na- and K- uranyl arsenate dissolution

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Keywords

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