Effects of Nitrate on the Stability of Uranium in a Bioreduced Region of the Subsurface

Wu, W; Carley, J; Green, SJ; Luo, J; Kelly, SD; Van Nostrand, Joy; Lowe, K; Mehlhorn, T; Carroll, Sue; Boonchayanant, B; Loefller, FE; Watson, D; Kemner, KM; Zhou, J; Kitanidis, PK; Kostka, JE; Jardine, PM; Criddle, CS

HERO ID

2009219

Reference Type

Journal Article

Year

2010

Language

English

PMID

20527772

HERO ID 2009219
In Press No
Year 2010
Title Effects of Nitrate on the Stability of Uranium in a Bioreduced Region of the Subsurface
Authors Wu, W; Carley, J; Green, SJ; Luo, J; Kelly, SD; Van Nostrand, Joy; Lowe, K; Mehlhorn, T; Carroll, Sue; Boonchayanant, B; Loefller, FE; Watson, D; Kemner, KM; Zhou, J; Kitanidis, PK; Kostka, JE; Jardine, PM; Criddle, CS
Journal Environmental Science & Technology
Volume 44
Issue 13
Page Numbers 5104-5111
Abstract The effects of nitrate on the stability of reduced, immobilized uranium were evaluated in field experiments at a U.S. Department of Energy site in Oak Ridge, TN. Nitrate (2.0 mM) was injected into a reduced region of the subsurface containing high levels of previously immobilized U(IV). The nitrate was reduced to nitrite, ammonium, and nitrogen gas; sulfide levels decreased; and Fe(II) levels increased then deceased. Uranium remobilization occurred concomitant with nitrite formation, suggesting nitrate-dependent, iron-accelerated oxidation of U(IV). Bromide tracer results indicated changes in subsurface flowpaths likely due to gas formation and/or precipitate. Desorption-adsorption of uranium by the iron-rich sediment impacted uranium mobilization and sequestration. After rereduction of the subsurface through ethanol additions, background groundwater containing high levels of nitrate was allowed to enter the reduced test zone. Aqueous uranium concentrations increased then decreased. Clone library analyses of sediment samples revealed the presence of denitrifying bacteria that can oxidize elemental sulfur, H(2)S, Fe(II), and U(IV) (e.g., Thiobacillus spp.), and a decrease in relative abundance of bacteria that can reduce Fe(III) and sulfate. XANES analyses of sediment samples confirmed changes in uranium oxidation state. Addition of ethanol restored reduced conditions and triggered a short-term increase in Fe(II) and aqueous uranium, likely due to reductive dissolution of Fe(III) oxides and release of sorbed U(VI). After two months of intermittent ethanol addition, sulfide levels increased, and aqueous uranium concentrations gradually decreased to <0.1 microM.
Doi 10.1021/es1000837
Pmid 20527772
Wosid WOS:000279304700047
Is Certified Translation No
Dupe Override No
Is Public Yes
Language Text English