Abstract
Metaschoepite is commonly found in U-contaminated environments and metaschoepite-bearing wastes may be managed via shallow or deep disposal. Understanding metaschoepite dissolution and tracking the fate of any liberated U is thus important. Here, discrete horizons of metaschoepite (UO3·nH2O) particles were emplaced in flowing sediment/groundwater columns representative of the UK Sellafield Ltd. site. The column systems either remained oxic or became anoxic due to electron donor additions, and the columns were sacrificed after 6- and 12-months for analysis. Solution chemistry, extractions, and bulk and micro/nano-focus X-ray spectroscopies were used to track changes in U distribution and behavior. In the oxic columns, U migration was extensive, with UO2 2+ identified in effluents after 6-months of reaction using fluorescence spectroscopy. Unusually, in the electron-donor amended columns, during microbially mediated sulfate reduction, significant amounts of UO2-like colloids (>60% of the added U) were found in the effluents using TEM. XAS analysis of the U remaining associated with the reduced sediments confirmed the presence of trace U(VI), noncrystalline U(IV), and biogenic UO2, with UO2 becoming more dominant with time. This study highlights the potential for U(IV) colloid production from U(VI) solids under reducing conditions and the complexity of U biogeochemistry in dynamic systems.
| Original language | English |
|---|---|
| Pages (from-to) | 9915-9925 |
| Number of pages | 11 |
| Journal | Environmental Science and Technology |
| Volume | 53 |
| Issue number | 16 |
| DOIs | |
| Publication status | Published - Aug 20 2019 |
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All Science Journal Classification (ASJC) codes
- Chemistry(all)
- Environmental Chemistry
Cite this
Metaschoepite Dissolution in Sediment Column Systems - Implications for Uranium Speciation and Transport. / Bower, William R.; Morris, Katherine; Livens, Francis R.; Mosselmans, J. Frederick W.; Fallon, Connaugh M.; Fuller, Adam J.; Natrajan, Louise; Boothman, Christopher; Lloyd, Jonathan R.; Utsunomiya, Satoshi; Grolimund, Daniel; Ferreira Sanchez, Dario; Jilbert, Tom; Parker, Julia; Neill, Thomas S.; Law, Gareth T.W.
In: Environmental Science and Technology, Vol. 53, No. 16, 20.08.2019, p. 9915-9925.Research output: Contribution to journal › Article
}
TY - JOUR
T1 - Metaschoepite Dissolution in Sediment Column Systems - Implications for Uranium Speciation and Transport
AU - Bower, William R.
AU - Morris, Katherine
AU - Livens, Francis R.
AU - Mosselmans, J. Frederick W.
AU - Fallon, Connaugh M.
AU - Fuller, Adam J.
AU - Natrajan, Louise
AU - Boothman, Christopher
AU - Lloyd, Jonathan R.
AU - Utsunomiya, Satoshi
AU - Grolimund, Daniel
AU - Ferreira Sanchez, Dario
AU - Jilbert, Tom
AU - Parker, Julia
AU - Neill, Thomas S.
AU - Law, Gareth T.W.
PY - 2019/8/20
Y1 - 2019/8/20
N2 - Metaschoepite is commonly found in U-contaminated environments and metaschoepite-bearing wastes may be managed via shallow or deep disposal. Understanding metaschoepite dissolution and tracking the fate of any liberated U is thus important. Here, discrete horizons of metaschoepite (UO3·nH2O) particles were emplaced in flowing sediment/groundwater columns representative of the UK Sellafield Ltd. site. The column systems either remained oxic or became anoxic due to electron donor additions, and the columns were sacrificed after 6- and 12-months for analysis. Solution chemistry, extractions, and bulk and micro/nano-focus X-ray spectroscopies were used to track changes in U distribution and behavior. In the oxic columns, U migration was extensive, with UO2 2+ identified in effluents after 6-months of reaction using fluorescence spectroscopy. Unusually, in the electron-donor amended columns, during microbially mediated sulfate reduction, significant amounts of UO2-like colloids (>60% of the added U) were found in the effluents using TEM. XAS analysis of the U remaining associated with the reduced sediments confirmed the presence of trace U(VI), noncrystalline U(IV), and biogenic UO2, with UO2 becoming more dominant with time. This study highlights the potential for U(IV) colloid production from U(VI) solids under reducing conditions and the complexity of U biogeochemistry in dynamic systems.
AB - Metaschoepite is commonly found in U-contaminated environments and metaschoepite-bearing wastes may be managed via shallow or deep disposal. Understanding metaschoepite dissolution and tracking the fate of any liberated U is thus important. Here, discrete horizons of metaschoepite (UO3·nH2O) particles were emplaced in flowing sediment/groundwater columns representative of the UK Sellafield Ltd. site. The column systems either remained oxic or became anoxic due to electron donor additions, and the columns were sacrificed after 6- and 12-months for analysis. Solution chemistry, extractions, and bulk and micro/nano-focus X-ray spectroscopies were used to track changes in U distribution and behavior. In the oxic columns, U migration was extensive, with UO2 2+ identified in effluents after 6-months of reaction using fluorescence spectroscopy. Unusually, in the electron-donor amended columns, during microbially mediated sulfate reduction, significant amounts of UO2-like colloids (>60% of the added U) were found in the effluents using TEM. XAS analysis of the U remaining associated with the reduced sediments confirmed the presence of trace U(VI), noncrystalline U(IV), and biogenic UO2, with UO2 becoming more dominant with time. This study highlights the potential for U(IV) colloid production from U(VI) solids under reducing conditions and the complexity of U biogeochemistry in dynamic systems.
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U2 - 10.1021/acs.est.9b02292
DO - 10.1021/acs.est.9b02292
M3 - Article
VL - 53
SP - 9915
EP - 9925
JO - Environmental Science & Technology
JF - Environmental Science & Technology
SN - 0013-936X
IS - 16
ER -