Fate of arsenic during the interactions between Mn-substituted goethite and dissolved Fe(II)

Liu, Huan; Lu, Xiancai; Flynn, Elaine D.; Catalano, Jeffrey G.

doi:10.1016/j.gca.2023.06.028

Fate of arsenic during the interactions between Mn-substituted goethite and dissolved Fe(II)

Journal Article · Thu Jun 29 00:00:00 EDT 2023 · Geochimica et Cosmochimica Acta

DOI:https://doi.org/10.1016/j.gca.2023.06.028· OSTI ID:2423434

Liu, Huan ^[1]; Lu, Xiancai ^[2]; ^[3]; ^[3]

Nanjing Univ. (China); Washington Univ., St. Louis, MO (United States)
Nanjing Univ. (China)
Washington Univ., St. Louis, MO (United States)

Geogenic arsenic has become a globally-distributed groundwater contaminant, liberated from the weathering of arsenic-bearing sulfide minerals and often transported to aquifer sediments adsorbed to iron oxides. Among the iron oxides, goethite (α-FeOOH) is uniquely important for the fate of arsenic because of its widespread abundance, stability, and high affinity for binding arsenic. Goethite is ubiquitous in soils and sediments and often contains substituted elements, including manganese. Structural manganese may affect the surface reactivity and redox capacity of goethite and alter the mechanisms of recrystallization catalyzed by dissolved Fe(II), potentially affecting arsenic adsorption. Here, this study examined the fate of As(V) during the interactions between dissolved Fe(II) and Mn-substituted goethites at pH 4 and 7 as well as associated changes in arsenic speciation. At pH 7, the addition of dissolved Fe(II) initially increases the adsorption of As(V) onto Mn-bearing and Mn-free goethites. For the Mn-substituted goethites, the adsorbed As(V) slowly releases to solution at longer aging times. Fe(II) addition at pH 4 slightly increases As(V) uptake by Mn-substituted goethites, with differences in total sorption correlating with the Mn content in goethite. The addition of Fe(II) releases substantial dissolved manganese but the amount solubilized is higher at pH 4 compared to 7, suggesting that the presence of adsorbed As(V) may substantially promote the Mn release at pH 4. X-ray absorption fine structure spectroscopy shows that arsenic is stabilized as As(V) in all the samples and adsorbed on goethite via a bidentate binuclear mechanism. Fitting results show that the binding distance and coordination numbers are stable in Mn-free goethite and Mn-substituted goethite samples; the effect of substituted Mn on the surface complex structure is minor. High resolution transmission electron microscopy and X-ray diffraction confirm that no secondary ferrous arsenate minerals precipitate under both pH conditions. This study improves our understanding of the Fe(II)-As(V) interactions on iron oxides, and demonstrates that the substituted cations such as manganese may quantitatively alter the geochemical fate of arsenic during the reaction of dissolved Fe(II) with Fe(III) oxides.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 2423434

Journal Information:: Geochimica et Cosmochimica Acta, Vol. 356; ISSN 0016-7037

Publisher:: Elsevier; The Geochemical Society; The Meteoritical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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58 GEOSCIENCES
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Goethite
Mn-substitution
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Fate of arsenic during the interactions between Mn-substituted goethite and dissolved Fe(II)

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