Chemical reduction of U(VI) by Fe(II) at the solid-water interface using natural and synthetic Fe(III) oxides

Byong Hun Jeon, Brian A. Dempsey, William D. Burgos, Mark O. Barnett, Eric E. Roden

Research output: Contribution to journalArticle

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Abstract

Abiotic reduction of 0.1 mM U(VI) by Fe(II) in the presence of synthetic iron oxides (biogenic magnetite, goethite, and hematite) and natural Fe(III) oxide-containing solids was investigated in pH 6.8 artificial groundwater containing 10 mM NaHCO 3. In most experiments, more than 95% of added U(VI) was sorbed to solids. U(VI) was rapidly and extensively (≥80%) reduced in the presence of synthetic Fe-(III) oxides and highly Fe(III) oxide-enriched (18-35 wt % Fe) Atlantic coastal plain sediments. In contrast, long-term (20-60 d) U(VI) reduction was less than 30% in suspensions of six other natural solids with relatively low Fe(III) oxide content (1-5 wt % Fe). Fe(II) sorption site density was severalfold lower on these natural solids (0.2-1.1 Fe(II) nm -2) compared to the synthetic Fe(III) oxides (1.6-3.2 Fe(II) nm -2), which may explain the poor U(VI) reduction in the natural solid-containing systems. Addition of the reduced form of the electron shuttling compound anthrahydroquinone-2,6-disulfonate (AH 2DS; final concentration 2.5 mM) to the natural solid suspensions enhanced the rate and extent of U(VI) reduction, suggesting that AH 2-DS reduced U(VI) at surface sites where reaction of U(VI) with sorbed Fe(II) was limited. This study demonstrates that abiotic, Fe(II)-driven U(VI) reduction is likely to be less efficient in natural soils and sediments than would be inferred from studies with synthetic Fe(III) oxides.

Original languageEnglish (US)
Pages (from-to)5642-5649
Number of pages8
JournalEnvironmental Science and Technology
Volume39
Issue number15
DOIs
StatePublished - Aug 1 2005

Fingerprint

Oxides
oxide
Water
water
Suspensions
Sediments
Ferrosoferric Oxide
Hematite
Magnetite
goethite
Iron oxides
coastal plain
iron oxide
hematite
sediment
Intermetallics
Sorption
magnetite
Groundwater
sorption

All Science Journal Classification (ASJC) codes

  • Chemistry(all)
  • Environmental Chemistry

Cite this

Jeon, Byong Hun ; Dempsey, Brian A. ; Burgos, William D. ; Barnett, Mark O. ; Roden, Eric E. / Chemical reduction of U(VI) by Fe(II) at the solid-water interface using natural and synthetic Fe(III) oxides. In: Environmental Science and Technology. 2005 ; Vol. 39, No. 15. pp. 5642-5649.
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abstract = "Abiotic reduction of 0.1 mM U(VI) by Fe(II) in the presence of synthetic iron oxides (biogenic magnetite, goethite, and hematite) and natural Fe(III) oxide-containing solids was investigated in pH 6.8 artificial groundwater containing 10 mM NaHCO 3. In most experiments, more than 95{\%} of added U(VI) was sorbed to solids. U(VI) was rapidly and extensively (≥80{\%}) reduced in the presence of synthetic Fe-(III) oxides and highly Fe(III) oxide-enriched (18-35 wt {\%} Fe) Atlantic coastal plain sediments. In contrast, long-term (20-60 d) U(VI) reduction was less than 30{\%} in suspensions of six other natural solids with relatively low Fe(III) oxide content (1-5 wt {\%} Fe). Fe(II) sorption site density was severalfold lower on these natural solids (0.2-1.1 Fe(II) nm -2) compared to the synthetic Fe(III) oxides (1.6-3.2 Fe(II) nm -2), which may explain the poor U(VI) reduction in the natural solid-containing systems. Addition of the reduced form of the electron shuttling compound anthrahydroquinone-2,6-disulfonate (AH 2DS; final concentration 2.5 mM) to the natural solid suspensions enhanced the rate and extent of U(VI) reduction, suggesting that AH 2-DS reduced U(VI) at surface sites where reaction of U(VI) with sorbed Fe(II) was limited. This study demonstrates that abiotic, Fe(II)-driven U(VI) reduction is likely to be less efficient in natural soils and sediments than would be inferred from studies with synthetic Fe(III) oxides.",
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Chemical reduction of U(VI) by Fe(II) at the solid-water interface using natural and synthetic Fe(III) oxides. / Jeon, Byong Hun; Dempsey, Brian A.; Burgos, William D.; Barnett, Mark O.; Roden, Eric E.

In: Environmental Science and Technology, Vol. 39, No. 15, 01.08.2005, p. 5642-5649.

Research output: Contribution to journalArticle

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T1 - Chemical reduction of U(VI) by Fe(II) at the solid-water interface using natural and synthetic Fe(III) oxides

AU - Jeon, Byong Hun

AU - Dempsey, Brian A.

AU - Burgos, William D.

AU - Barnett, Mark O.

AU - Roden, Eric E.

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Y1 - 2005/8/1

N2 - Abiotic reduction of 0.1 mM U(VI) by Fe(II) in the presence of synthetic iron oxides (biogenic magnetite, goethite, and hematite) and natural Fe(III) oxide-containing solids was investigated in pH 6.8 artificial groundwater containing 10 mM NaHCO 3. In most experiments, more than 95% of added U(VI) was sorbed to solids. U(VI) was rapidly and extensively (≥80%) reduced in the presence of synthetic Fe-(III) oxides and highly Fe(III) oxide-enriched (18-35 wt % Fe) Atlantic coastal plain sediments. In contrast, long-term (20-60 d) U(VI) reduction was less than 30% in suspensions of six other natural solids with relatively low Fe(III) oxide content (1-5 wt % Fe). Fe(II) sorption site density was severalfold lower on these natural solids (0.2-1.1 Fe(II) nm -2) compared to the synthetic Fe(III) oxides (1.6-3.2 Fe(II) nm -2), which may explain the poor U(VI) reduction in the natural solid-containing systems. Addition of the reduced form of the electron shuttling compound anthrahydroquinone-2,6-disulfonate (AH 2DS; final concentration 2.5 mM) to the natural solid suspensions enhanced the rate and extent of U(VI) reduction, suggesting that AH 2-DS reduced U(VI) at surface sites where reaction of U(VI) with sorbed Fe(II) was limited. This study demonstrates that abiotic, Fe(II)-driven U(VI) reduction is likely to be less efficient in natural soils and sediments than would be inferred from studies with synthetic Fe(III) oxides.

AB - Abiotic reduction of 0.1 mM U(VI) by Fe(II) in the presence of synthetic iron oxides (biogenic magnetite, goethite, and hematite) and natural Fe(III) oxide-containing solids was investigated in pH 6.8 artificial groundwater containing 10 mM NaHCO 3. In most experiments, more than 95% of added U(VI) was sorbed to solids. U(VI) was rapidly and extensively (≥80%) reduced in the presence of synthetic Fe-(III) oxides and highly Fe(III) oxide-enriched (18-35 wt % Fe) Atlantic coastal plain sediments. In contrast, long-term (20-60 d) U(VI) reduction was less than 30% in suspensions of six other natural solids with relatively low Fe(III) oxide content (1-5 wt % Fe). Fe(II) sorption site density was severalfold lower on these natural solids (0.2-1.1 Fe(II) nm -2) compared to the synthetic Fe(III) oxides (1.6-3.2 Fe(II) nm -2), which may explain the poor U(VI) reduction in the natural solid-containing systems. Addition of the reduced form of the electron shuttling compound anthrahydroquinone-2,6-disulfonate (AH 2DS; final concentration 2.5 mM) to the natural solid suspensions enhanced the rate and extent of U(VI) reduction, suggesting that AH 2-DS reduced U(VI) at surface sites where reaction of U(VI) with sorbed Fe(II) was limited. This study demonstrates that abiotic, Fe(II)-driven U(VI) reduction is likely to be less efficient in natural soils and sediments than would be inferred from studies with synthetic Fe(III) oxides.

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