Arsenic mobilization from iron oxides in the presence of oxalic acid under hydrodynamic conditions

Jing Sun, Benjamin C. Bostick, Brian J. Mailloux, James Jamieson, Beizhan Yan, Masha Pitiranggon, Steven N. Chillrud

Research output: Contribution to journalArticle

Abstract

Oxalic acid potentially enhances pump-and-treat for groundwater As remediation by accelerating mobilization. This study examines how oxalic acid mobilizes As from Fe(III)-oxide coated sand under hydrodynamic conditions. Four columns were packed with metal-substituted ferrihydrite or goethite to 1% Fe, presorbed to 50% As surface coverage, and reacted with pH = 2.2 artificial groundwater amended with 10 mM oxalic acid at 1 m day(-1). Arsenic elution was affected by both As and Fe speciation. Although the As(V) columns experienced faster substrate dissolution, As(V) elution was delayed by re-adsorption, whereas As(III) elution was rapid due to pH decrease that prevented re-adsorption. Cr-ferrihydrite and Ni-goethite dissolved both effectively initially but then diverged. The Cr-ferrihydrite columns experienced continuous stoichiometric Fe and Cr release, and As release could be sustained. The Ni-goethite columns initially experienced nonstoichiometric Fe and Ni release, and As release was extensive. Such release, however, was not sustained. We hypothesized that Ni-goethite contained sites with distinct reactivity, and oxalic acid targeted readily-dissolved, sorption-dense sites. Our data indicate that oxalic acid-enhanced pump-and-treat methods would be easier to apply to aquifers dominated by As(III), requiring less amendment to be injected; such oxalic acid-enhanced methods remove reactive sediment Fe and As, potentially preventing future groundwater contamination.
Original languageEnglish
Pages (from-to)219-227
JournalChemosphere
Volume212
DOIs
Publication statusPublished - 1 Dec 2018

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oxalic acid
iron oxide
mobilization
arsenic
hydrodynamics
goethite
ferrihydrite
pump and treat
groundwater
adsorption
remediation
sorption
dissolution
oxide
aquifer
substrate
sand
metal
sediment

Cite this

Sun, J., Bostick, B. C., Mailloux, B. J., Jamieson, J., Yan, B., Pitiranggon, M., & Chillrud, S. N. (2018). Arsenic mobilization from iron oxides in the presence of oxalic acid under hydrodynamic conditions. Chemosphere, 212, 219-227. https://doi.org/10.1016/j.chemosphere.2018.08.058
Sun, Jing ; Bostick, Benjamin C. ; Mailloux, Brian J. ; Jamieson, James ; Yan, Beizhan ; Pitiranggon, Masha ; Chillrud, Steven N. / Arsenic mobilization from iron oxides in the presence of oxalic acid under hydrodynamic conditions. In: Chemosphere. 2018 ; Vol. 212. pp. 219-227.
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abstract = "Oxalic acid potentially enhances pump-and-treat for groundwater As remediation by accelerating mobilization. This study examines how oxalic acid mobilizes As from Fe(III)-oxide coated sand under hydrodynamic conditions. Four columns were packed with metal-substituted ferrihydrite or goethite to 1{\%} Fe, presorbed to 50{\%} As surface coverage, and reacted with pH = 2.2 artificial groundwater amended with 10 mM oxalic acid at 1 m day(-1). Arsenic elution was affected by both As and Fe speciation. Although the As(V) columns experienced faster substrate dissolution, As(V) elution was delayed by re-adsorption, whereas As(III) elution was rapid due to pH decrease that prevented re-adsorption. Cr-ferrihydrite and Ni-goethite dissolved both effectively initially but then diverged. The Cr-ferrihydrite columns experienced continuous stoichiometric Fe and Cr release, and As release could be sustained. The Ni-goethite columns initially experienced nonstoichiometric Fe and Ni release, and As release was extensive. Such release, however, was not sustained. We hypothesized that Ni-goethite contained sites with distinct reactivity, and oxalic acid targeted readily-dissolved, sorption-dense sites. Our data indicate that oxalic acid-enhanced pump-and-treat methods would be easier to apply to aquifers dominated by As(III), requiring less amendment to be injected; such oxalic acid-enhanced methods remove reactive sediment Fe and As, potentially preventing future groundwater contamination.",
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Sun, J, Bostick, BC, Mailloux, BJ, Jamieson, J, Yan, B, Pitiranggon, M & Chillrud, SN 2018, 'Arsenic mobilization from iron oxides in the presence of oxalic acid under hydrodynamic conditions' Chemosphere, vol. 212, pp. 219-227. https://doi.org/10.1016/j.chemosphere.2018.08.058

Arsenic mobilization from iron oxides in the presence of oxalic acid under hydrodynamic conditions. / Sun, Jing; Bostick, Benjamin C.; Mailloux, Brian J.; Jamieson, James; Yan, Beizhan; Pitiranggon, Masha; Chillrud, Steven N.

In: Chemosphere, Vol. 212, 01.12.2018, p. 219-227.

Research output: Contribution to journalArticle

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T1 - Arsenic mobilization from iron oxides in the presence of oxalic acid under hydrodynamic conditions

AU - Sun, Jing

AU - Bostick, Benjamin C.

AU - Mailloux, Brian J.

AU - Jamieson, James

AU - Yan, Beizhan

AU - Pitiranggon, Masha

AU - Chillrud, Steven N.

PY - 2018/12/1

Y1 - 2018/12/1

N2 - Oxalic acid potentially enhances pump-and-treat for groundwater As remediation by accelerating mobilization. This study examines how oxalic acid mobilizes As from Fe(III)-oxide coated sand under hydrodynamic conditions. Four columns were packed with metal-substituted ferrihydrite or goethite to 1% Fe, presorbed to 50% As surface coverage, and reacted with pH = 2.2 artificial groundwater amended with 10 mM oxalic acid at 1 m day(-1). Arsenic elution was affected by both As and Fe speciation. Although the As(V) columns experienced faster substrate dissolution, As(V) elution was delayed by re-adsorption, whereas As(III) elution was rapid due to pH decrease that prevented re-adsorption. Cr-ferrihydrite and Ni-goethite dissolved both effectively initially but then diverged. The Cr-ferrihydrite columns experienced continuous stoichiometric Fe and Cr release, and As release could be sustained. The Ni-goethite columns initially experienced nonstoichiometric Fe and Ni release, and As release was extensive. Such release, however, was not sustained. We hypothesized that Ni-goethite contained sites with distinct reactivity, and oxalic acid targeted readily-dissolved, sorption-dense sites. Our data indicate that oxalic acid-enhanced pump-and-treat methods would be easier to apply to aquifers dominated by As(III), requiring less amendment to be injected; such oxalic acid-enhanced methods remove reactive sediment Fe and As, potentially preventing future groundwater contamination.

AB - Oxalic acid potentially enhances pump-and-treat for groundwater As remediation by accelerating mobilization. This study examines how oxalic acid mobilizes As from Fe(III)-oxide coated sand under hydrodynamic conditions. Four columns were packed with metal-substituted ferrihydrite or goethite to 1% Fe, presorbed to 50% As surface coverage, and reacted with pH = 2.2 artificial groundwater amended with 10 mM oxalic acid at 1 m day(-1). Arsenic elution was affected by both As and Fe speciation. Although the As(V) columns experienced faster substrate dissolution, As(V) elution was delayed by re-adsorption, whereas As(III) elution was rapid due to pH decrease that prevented re-adsorption. Cr-ferrihydrite and Ni-goethite dissolved both effectively initially but then diverged. The Cr-ferrihydrite columns experienced continuous stoichiometric Fe and Cr release, and As release could be sustained. The Ni-goethite columns initially experienced nonstoichiometric Fe and Ni release, and As release was extensive. Such release, however, was not sustained. We hypothesized that Ni-goethite contained sites with distinct reactivity, and oxalic acid targeted readily-dissolved, sorption-dense sites. Our data indicate that oxalic acid-enhanced pump-and-treat methods would be easier to apply to aquifers dominated by As(III), requiring less amendment to be injected; such oxalic acid-enhanced methods remove reactive sediment Fe and As, potentially preventing future groundwater contamination.

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JO - Chemosphere

JF - Chemosphere

SN - 0045-6535

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