SREL Reprint #2763




Uranium Complexes Formed at Hematite Surfaces Colonized by Sulfate-Reducing Bacteria

Andrew L. Neal1,2, James E. Amonette3, Brent M. Peyton4, and Gill G. Geesey1,2

1Department of Microbiology, Montana State University, Bozeman Montana 59717-3520
2Center for Biofilm Engineering, Montana State University, Bozeman, Montana 59717-3980
3Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory,
Richland, Washington 99352
4Center for Multiphase Environmental Research, Washington State University, Pullman, Washington 99164

Abstract: Modeling uranium (U) transport in subsurface environments requires a thorough knowledge of mechanisms likely to restrict its mobility, such as surface complexation, precipitation, and colloid formation. ln closed systems, sulfate-reducing bacteria (SRB) such as Desulfovibrio spp, demonstrably affect U immobilization by enzymatic reduction of U(VI) species (primarily the uranyl ion, UO22+, and its complexes) to U(IV). However, our understanding of such interactions under chronic U(VI) exposure in dynamic systems is limited. As a first step to understanding such interactions, we performed bioreactor experiments under continuous flow to study the effect of a biofilm of the sulfate-reducing bacterium Desulfovlorio desulfuricans attached to specular hematite (α-Fe203) surfaces on surface-associated U(VI) complexation, transformation, and mobility. Employing real-time microscopic observation and X-ray photoelectron spectroscopy (XPS), we show that the characteristics of the U(VI) complex(es) formed at the hematite surface are influenced by the composition of the bulk aqueous phase flowing across the surface and by the presence of surface-associated SRB. The XPS data further suggest higher levels of U associated with hematite surfaces colonized by SRB than with bacteria-free surfaces. Microscopic observations indicate that at least a portion of the U(VI) that accumulates in the presence of the SRB is exterior to the cells possibly associated with the extracellular biofilm matrix. The U4f7/2 core-region spectrum and U5f2 valence-band spectrum provide preliminary evidence that the SRB-colonized hematite surface accumulates both U(VI) and U(IV) phases, whereas only the U(VI) phase(s) accumulates on uncolonized hematite surfaces. The results suggest that mineral surfaces exposed to a continuously replenished supply of U(VI)-containing aqueous phase will accumulate U phases that may be more representative of those that exist in U-contaminated aquifers than those which accumulate in closed experimental systems. These phases should be considered in models attempting to predict U transport through subsurface environments.

SREL Reprint #2763

Neal, A. L., J. E. Amonette, B. M. Peyton, and G. G. Geesey. 2004. Uranium complexes formed at hematite surfaces colonized by sulfate-reducing bacteria. Environmental Science & Technology 38:3019-3027.

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