Papers by Lucie N'Guessan
An in-situ acetate amendment at a DOE Uranium Mill Tailings Remedial Action (UMTRA) site near Rif... more An in-situ acetate amendment at a DOE Uranium Mill Tailings Remedial Action (UMTRA) site near Rifle, CO demonstrated successful reduction of aqueous U(VI), to less soluble U(IV) through stimulated microbial activity. U(VI) reduction rates were highest during iron reduction and decreased with the onset of sulfate reduction. However, sustained U(IV) attenuation was observed following subsequent termination of the acetate amendment. These findings illustrate the importance of the transition between iron and sulfate reducing conditions in stimulating bioreduction of uranium. The sulfur isotope compositions of sulfate and sulfide were measured through this transition in order to explore the utility of these data in tracking the extent of microbial sulfate reduction and to assess the stability of sulfide precipitates. Samples for isotopic analyses and aqueous measurements of sulfate, ferrous iron, U(VI) and acetate were collected in one background well and three monitoring wells down-gradient of the acetate injection. Results show an increase of up to 7‰ in the δ34S of sulfate at the onset of sulfate reduction, followed by a return to background δ34S values of -8‰ following cessation of the acetate amendment. The δ34S values of sulfide increased from roughly -20‰ at the onset of sulfate reduction to a maximum of -0.8‰ during peak sulfate removal, followed by a gradual return to values of roughly -28‰ upon cessation of the acetate amendment. These data present a unique perspective on the processes governing the bioreduction experiment in that the sulfate isotopes are a function of both transport and mixing processes, whereas the sulfide isotopes represent biogenic sulfide that is rapidly removed from the aqueous phase. Thus a comparable enrichment in sulfate isotopic data noted in the closest and furthest wells from the injection gallery suggest bioreduction in both of these locations, while a larger increase in sulfide isotopic values in the closest well indicates greater rates of sulfate reduction closer to the injection gallery. In addition, a steady decline in δ34S of sulfide concurrent with increased sulfide concentrations following cessation of acetate amendment suggests that this increase is not a result of reoxidation of precipitated FeS species. FeS precipitates formed during the height of sulfate reduction therefore appear to be stable on a timeframe of months following acetate amendment and may support the stability and long-term sequestration of precipitated U(IV).
Bookmarks Related papers MentionsView impact
Flow-through sediment column experiments were conducted to determine the stability of biogenic U(... more Flow-through sediment column experiments were conducted to determine the stability of biogenic U(IV) after biostimulation has been discontinued, and to isolate the key biogeochemical processes that affect the post-biostimulation U(IV) stability. Columns, packed with sediments from an UMTRA site (Rifle Colorado) were biostimulated for two months by injecting groundwater containing 3 mM acetate and 20 uM U(VI) at flow rates typically encountered at the Rifle site. After the biostimulation period, acetate injection was discontinued, and groundwater containing dissolved oxygen was allowed to enter the columns. Columns were then sacrificed at two week intervals to examine the sediment geochemistry and associated microbial community. Results showed that iron sulfide precipitates, that formed during the bioreduction phase, acted as a buffer to partially prevent biogenic U(IV) oxidation during the month post stimulation period. Groundwater and sediment microbial community compositions were analyzed over a period of one month post-biostimulation. The results indicate that two distinct biological processes, characterized by oxygen utilization, played important roles during this period. Within two weeks post stimulation, organisms such as Hydrogenophaga sp. and Thiobacillus sp. were observed in the columns. These bacteria, are able to use Fe(II), sulfide, or thiosulfate as their electron donor in the presence of O2. Furthermore, organisms closely related to Lysobacter sp. and Sterolibacterium sp. were also detected in the groundwater and sediment. It was suggested that these organisms may be feeding on decaying biomass and consuming O2 in the process. The presence of these oxidizing and spoilage bacteria is thought to have resulted in the consumption of oxygen, therefore protecting the biogenic U(IV) from being reoxidized in the sediment columns. To simulate the in situ U(IV) stability under post biostimulation conditions, columns bioreduced in the laboratory, as described above, were placed in wells located upstream and downstream of a experimental plot at the Rifle site, shortly after a field biostimulation experiment was terminated. Columns have been withdrawn and analyzed over the first six month period and additional columns will be withdrawn for a full year of observations. Groundwater is being pumped through the columns at the same velocity as the local groundwater flow-velocity. Results to date have shown that some U(IV) was mobilized within the first few days of placing the columns in the wells, but that U(IV) has remained relatively constant thereafter.
Bookmarks Related papers MentionsView impact
Understanding how microorganisms alter their physical and chemical environment during bioremediat... more Understanding how microorganisms alter their physical and chemical environment during bioremediation is hindered by our inability to resolve subsurface microbial activity with high spatial resolution. Here we demonstrate the use of a minimally invasive geophysical technique to monitor microbe-mediated iron and sulfate reduction during acetate amendment of a uranium-contaminated aquifer near Rifle, CO. During induced polarization (IP) measurements, spatiotemporal variations in the phase response between applied and measured voltages correlated with changes in groundwater geochemistry indicative of microbial iron and sulfate reduction and sulfide mineral precipitation. The enhanced sensitivity of the high and low frequency phase responses to accumulated aqueous iron and sulfide, respectively, provide the ability to discriminate the dominant subsurface biogeochemical process. The spectral effect was verified and calibrated using a biostimulated column experiment containing Rifle sediments and groundwater. Sediments and fluids recovered from regions of the field site exhibiting an anomalous phase response were enriched in sorbed Fe(II) and cell-associated 2-4 nm diameter FeS nanoparticles. These mineral precipitates and accumulated electroactive ions altered the ability of pore fluids to conduct electrical charge, accounting for the IP response. The results reveal the usefulness of multi-frequency IP measurements for discriminating mineralogical and geochemical changes during stimulated subsurface bioremediation.
Bookmarks Related papers MentionsView impact
Isme Journal, 2009
Bookmarks Related papers MentionsView impact
Isme Journal, 2007
Bookmarks Related papers MentionsView impact
Uploads
Papers by Lucie N'Guessan