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

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

doi:10.1021/acsearthspacechem.3c00096

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

Journal Article · Fri Jul 28 00:00:00 EDT 2023 · ACS Earth and Space Chemistry

DOI:https://doi.org/10.1021/acsearthspacechem.3c00096· OSTI ID:1995651

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Argonne National Laboratory (ANL), Argonne, IL (United States)
City Univ. of New York (CUNY), NY (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

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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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC05-00OR22725; AC02-06CH11357

OSTI ID:: 1995651

Journal Information:: ACS Earth and Space Chemistry, Vol. 7, Issue 8; ISSN 2472-3452

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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