Metaschoepite Dissolution in Sediment Column Systems - Implications for Uranium Speciation and Transport

William R. Bower, Katherine Morris, Francis R. Livens, J. Frederick W. Mosselmans, Connaugh M. Fallon, Adam J. Fuller, Louise Natrajan, Christopher Boothman, Jonathan R. Lloyd, Satoshi Utsunomiya, Daniel Grolimund, Dario Ferreira Sanchez, Tom Jilbert, Julia Parker, Thomas S. Neill, Gareth T.W. Law

Research output: Contribution to journalArticle

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 languageEnglish
Pages (from-to)9915-9925
Number of pages11
JournalEnvironmental Science and Technology
Volume53
Issue number16
DOIs
Publication statusPublished - Aug 20 2019

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Uranium
Colloids
Effluents
uranium
Sediments
Dissolution
Bearings (structural)
Biogeochemistry
dissolution
Electrons
Fluorescence spectroscopy
X ray spectroscopy
Waste disposal
sediment
Sulfates
Groundwater
colloid
Dynamical systems
Transmission electron microscopy
effluent

All Science Journal Classification (ASJC) codes

  • Chemistry(all)
  • Environmental Chemistry

Cite this

Bower, W. R., Morris, K., Livens, F. R., Mosselmans, J. F. W., Fallon, C. M., Fuller, A. J., ... Law, G. T. W. (2019). Metaschoepite Dissolution in Sediment Column Systems - Implications for Uranium Speciation and Transport. Environmental Science and Technology, 53(16), 9915-9925. https://doi.org/10.1021/acs.est.9b02292

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 journalArticle

Bower, WR, Morris, K, Livens, FR, Mosselmans, JFW, Fallon, CM, Fuller, AJ, Natrajan, L, Boothman, C, Lloyd, JR, Utsunomiya, S, Grolimund, D, Ferreira Sanchez, D, Jilbert, T, Parker, J, Neill, TS & Law, GTW 2019, 'Metaschoepite Dissolution in Sediment Column Systems - Implications for Uranium Speciation and Transport', Environmental Science and Technology, vol. 53, no. 16, pp. 9915-9925. https://doi.org/10.1021/acs.est.9b02292
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. / Metaschoepite Dissolution in Sediment Column Systems - Implications for Uranium Speciation and Transport. In: Environmental Science and Technology. 2019 ; Vol. 53, No. 16. pp. 9915-9925.
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