Sorption of Arsenate, Selenate, and Molybdate on the Barite (001) Surface

Peng Yang; Sang Soo Lee; Paul Fenter; Jacquelyn N. Bracco; Andrew G. Stack

doi:10.1021/acsearthspacechem.3c00096

Sorption of Arsenate, Selenate, and Molybdate on the Barite (001) Surface

Peng Yang, Sang Soo Lee, Paul Fenter, Jacquelyn N. Bracco, Andrew G. Stack

Geochemistry & Interfacial Science

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

2 Scopus citations

Abstract

Interactions of ions with ionically bonded minerals such as barite (BaSO₄) influence the fate and transport of the ions, while the factors that control the sorption of toxic oxyanions on barite remain elusive. In this study, the sorption of arsenate, selenate, and molybdate on the barite (001) surface was examined at pH ∼5 using in situ crystal truncation rod analysis, resonant anomalous X-ray reflectivity, and atomic force microscopy. The results show that arsenate and selenate mainly incorporate into the top monolayer of barite, while molybdate primarily adsorbs above the surface. The sorption coverage of arsenate is greater (by ∼100%) than that of selenate but similar to that of molybdate. The different incorporation coverages between arsenate and selenate can be explained by their different protonation states at pH 5. The incorporated arsenate may be stabilized by hydrogen bonds between arsenate and oxygen atoms of neighboring sulfate compared to selenate, which exists predominantly in the deprotonated state. The adsorption of molybdate above the surface probably stems from a surface-induced oligomerization, as the anion and the oligomer may be too large for incorporation. Our observation of these different sorption mechanisms demonstrates how the physicochemical properties of the anions control the selective uptake of the toxic metals on the dominant surface of the ionically bonded mineral barite.

Original language	English
Pages (from-to)	1545-1556
Number of pages	12
Journal	ACS Earth and Space Chemistry
Volume	7
Issue number	8
DOIs	https://doi.org/10.1021/acsearthspacechem.3c00096
State	Published - Aug 17 2023

Funding

This work was supported by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division. This work utilized resources of the Advanced Photon Source (APS), a U.S. DOE Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. The X-ray data were collected at the beamline 33-ID-D, APS. The submitted manuscript has been created by UChicago Argonne, LLC, Operator of Argonne National Laboratory (“Argonne”). Argonne, a U.S. Department of Energy Office of Science laboratory, is operated under contract no. DE-AC02-06CH11357. The U.S. Government retains for itself and others acting on its behalf a paid-up nonexclusive, irrevocable worldwide license in said article to reproduce, prepare derivative works, distribute copies to the public, and perform publicly and display publicly by or on behalf of the Government.

Funders	Funder number
U.S. Department of Energy
Office of Science
Basic Energy Sciences
Argonne National Laboratory	DE-AC02-06CH11357
Chemical Sciences, Geosciences, and Biosciences Division

Keywords

barite
incorporation
ionically bonded minerals
mineral−water interfacial reactions
sorption
tetrahedral oxyanions

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10.1021/acsearthspacechem.3c00096

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title = "Sorption of Arsenate, Selenate, and Molybdate on the Barite (001) Surface",

abstract = "Interactions of ions with ionically bonded minerals such as barite (BaSO4) influence the fate and transport of the ions, while the factors that control the sorption of toxic oxyanions on barite remain elusive. In this study, the sorption of arsenate, selenate, and molybdate on the barite (001) surface was examined at pH ∼5 using in situ crystal truncation rod analysis, resonant anomalous X-ray reflectivity, and atomic force microscopy. The results show that arsenate and selenate mainly incorporate into the top monolayer of barite, while molybdate primarily adsorbs above the surface. The sorption coverage of arsenate is greater (by ∼100%) than that of selenate but similar to that of molybdate. The different incorporation coverages between arsenate and selenate can be explained by their different protonation states at pH 5. The incorporated arsenate may be stabilized by hydrogen bonds between arsenate and oxygen atoms of neighboring sulfate compared to selenate, which exists predominantly in the deprotonated state. The adsorption of molybdate above the surface probably stems from a surface-induced oligomerization, as the anion and the oligomer may be too large for incorporation. Our observation of these different sorption mechanisms demonstrates how the physicochemical properties of the anions control the selective uptake of the toxic metals on the dominant surface of the ionically bonded mineral barite.",

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AU - Yang, Peng

AU - Lee, Sang Soo

AU - Fenter, Paul

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AU - Stack, Andrew G.

PY - 2023/8/17

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N2 - Interactions of ions with ionically bonded minerals such as barite (BaSO4) influence the fate and transport of the ions, while the factors that control the sorption of toxic oxyanions on barite remain elusive. In this study, the sorption of arsenate, selenate, and molybdate on the barite (001) surface was examined at pH ∼5 using in situ crystal truncation rod analysis, resonant anomalous X-ray reflectivity, and atomic force microscopy. The results show that arsenate and selenate mainly incorporate into the top monolayer of barite, while molybdate primarily adsorbs above the surface. The sorption coverage of arsenate is greater (by ∼100%) than that of selenate but similar to that of molybdate. The different incorporation coverages between arsenate and selenate can be explained by their different protonation states at pH 5. The incorporated arsenate may be stabilized by hydrogen bonds between arsenate and oxygen atoms of neighboring sulfate compared to selenate, which exists predominantly in the deprotonated state. The adsorption of molybdate above the surface probably stems from a surface-induced oligomerization, as the anion and the oligomer may be too large for incorporation. Our observation of these different sorption mechanisms demonstrates how the physicochemical properties of the anions control the selective uptake of the toxic metals on the dominant surface of the ionically bonded mineral barite.

AB - Interactions of ions with ionically bonded minerals such as barite (BaSO4) influence the fate and transport of the ions, while the factors that control the sorption of toxic oxyanions on barite remain elusive. In this study, the sorption of arsenate, selenate, and molybdate on the barite (001) surface was examined at pH ∼5 using in situ crystal truncation rod analysis, resonant anomalous X-ray reflectivity, and atomic force microscopy. The results show that arsenate and selenate mainly incorporate into the top monolayer of barite, while molybdate primarily adsorbs above the surface. The sorption coverage of arsenate is greater (by ∼100%) than that of selenate but similar to that of molybdate. The different incorporation coverages between arsenate and selenate can be explained by their different protonation states at pH 5. The incorporated arsenate may be stabilized by hydrogen bonds between arsenate and oxygen atoms of neighboring sulfate compared to selenate, which exists predominantly in the deprotonated state. The adsorption of molybdate above the surface probably stems from a surface-induced oligomerization, as the anion and the oligomer may be too large for incorporation. Our observation of these different sorption mechanisms demonstrates how the physicochemical properties of the anions control the selective uptake of the toxic metals on the dominant surface of the ionically bonded mineral barite.

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Sorption of Arsenate, Selenate, and Molybdate on the Barite (001) Surface

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