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Watson, David B

Publications and source records attributed to Watson, David B.

An integrated systems-based approach to mercury research and technology development

A 3-year strategic planning process was undertaken in Oak Ridge, Tennessee, to develop a research and technology development approach that can help guide mercury remediation in East Fork Poplar Creek (EFPC). Mercury remediation is a high priority for the US Department of Energy s (DOE s) Oak Ridge Office of Environmental Management because of large historical losses of mercury to the environment at the Y-12 National Security Complex (Y-12). Because of the extent of mercury losses and the complexities of mercury transport and fate in the stream environment, the success of conventional options for mercury remediation in the downstream sections of EFPC is uncertain. The overall Oak Ridge mercury remediation strategy focuses on mercury treatment actions at Y-12 in the short-term and research and technology development to evaluate longer-term solutions in the downstream environment. The technology development strategy is consistent with a phased, adaptive management paradigm and DOE s Technology Readiness Level guidelines. That is, early evaluation includes literature review, site characterization, and small-scale studies of a broad number of potential technologies. As more information is gathered, technologies that may have the most promise and potential remediation benefit will be chosen for more extensive and larger-scale pilot testing before being considered for remedial implementation. Field and laboratory research in EFPC is providing an improved level of understanding of mercury transport and fate processes in EFPC that will inform the development of site-specific remedial technologies. Technology development has centered on developing strategies that can mitigate the primary factors affecting mercury risks in the stream: (1) the amount of inorganic mercury available to the stream system, (2) the conversion of inorganic mercury to methylmercury, and (3) the bioaccumulation of methylmercury through the food web. Given the downstream complexities and interdependencies between sources and processes in EFPC, no one task or approach is likely to solve the mercury problem in the creek, thus highlighting the importance of using an integrated, systems-based approach to develop remedial solutions.

Peterson, Mark J↗

Watershed scale fungal community characterization along a pH gradient in a subsurface environment co-contaminated with uranium and nitrate

The objective of this study was to characterize fungal communities in a subsurface environment co-contaminated with uranium and nitrate at the watershed scale, and to determine the potential contribution of fungi to contaminant transformation (nitrate attenuation). The abundance, distribution and diversity of fungi in subsurface groundwater samples were determined using quantitative and semi-quantitative molecular techniques, including quantitative PCR of eukaryotic SSU rRNA genes and pyrosequencing of fungal internal transcribed spacer (ITS) regions. Potential bacterial and fungal denitrification was assessed in sediment-groundwater slurries amended with antimicrobial compounds and in fungal pure cultures isolated from subsurface. Our results demonstrate that subsurface fungal communities are dominated by members of the phylum Ascomycota, and a pronounced shift in fungal community composition occurs across the groundwater pH gradient at the field site, with lower diversity observed under acidic (pH < 4.5) conditions. Fungal isolates recovered from subsurface sediments were shown to reduce nitrate to nitrous oxide, including cultures of the genus Coniochaeta that were detected in abundance in pyrosequence libraries of site groundwater samples. Denitrifying fungal isolates recovered from the site were classified, and found to be distributed broadly within the phylum Ascomycota, and within a single genus within the Basidiomycota. Potential denitrification rate assays with sediment-groundwater slurries showed the potential for subsurface fungi to reduce nitrate to nitrous oxide under in situ acidic pH conditions.

Jasrotia, Puja↗

Mercury Source Zone Identification using Soil Vapor Sampling and Analysis

Development and demonstration of reliable measurement techniqes that can detect and help quantify the nature and extent of elemental mercury (Hg(0)) in the subsurface are needed to reduce certainties in the decision making process and increase the effectiveness of remedial actions. We conducted field tests at the Y-12 National Security Complex (NSC) in Oak Ridge, TN, to determine if sampling and analysis of Hg(0) vapors in the shallow subsurface (<0.3 m depth) can be used to as an indicator of the location and extent of Hg(0) releases in the subsurface. We constructed a rigid PVC pushprobe assembly, which was driven into the ground. Soil gas samples were collected through a sealed inner tube of the assembly and analyzed immediately in the field with a Lumex and/or Jerome Hg(0) analyzer. Time-series sampling showed that Hg vapor concentrations were fairly stable over time suggesting that the vapor phase Hg(0) was not being depleted and that sampling results were not dependent on the soil gas purge volume. Hg(0) vapor data collected at over 200 pushprobe locations at 3 different release sites correlated well to areas of known Hg(0) contamination. Vertical profiling of Hg(0) vapor concentrations conducted at 2 locations provided information on the vertical distribution of Hg(0) contamination in the subsurface. We concluded from our studies that soil gas sampling and analysis can be conducted rapidly and inexpensively at a large scale to help identify areas contaminated with Hg(0).

Watson, David B↗

Surge Block Method for Controlling Well Clogging and Sampling Sediment during Bioremediation

A surge block treatment method (i.e. inserting a solid rod plunger with a flat seal that closely fits the casing interior into a well and stocking it up and down) was performed for the rehabilitation of wells clogged with biomass and for the collection of time series sediment samples during in situ bioremediation tests for U(VI) immobilization at a the U.S. Department of Energy site in Oak Ridge, TN. The clogging caused by biomass growth had been controlled by using routine surge block treatment for18 times over a nearly four year test period. The treatment frequency was dependent of the dosage of electron donor injection and microbial community developed in the subsurface. Hydraulic tests showed that the apparent aquifer transmissivity at a clogged well with an inner diameter (ID) of 10.16 cm was increased by 8 13 times after the rehabilitation, indicating the effectiveness of the rehabilitation. Simultaneously with the rehabilitation, the surge block method was successfully used for collecting time series sediment samples composed of fine particles (clay and silt) from wells with ID 1.9 10.16 cm for the analysis of mineralogical and geochemical composition and microbial community during the same period. Our results demonstrated that the surge block method provided a cost-effective approach for both well rehabilitation and frequent solid sampling at the same location.

Wu, Wei-min↗

U(VI) bioreduction with emulsified vegetable oil as the electron donor-- Microcosm tests and model development

Microcosm tests were conducted to study U(VI) bioreduction in contaminated sediments with emulsified vegetable oil (EVO) as the electron donor. In the microcosms, EVO was degraded by indigenous microorganisms and stimulated Fe, U, and sulfate bioreduction, and methanogenesis. Removal of aqueous U occurred concurrently with sulfate reduction, with more reduction of total U in the case of higher initial sulfate concentrations. X-ray absorption near-edge spectroscopy (XANES) analysis confirmed U(VI) reduction to U(IV). As the acetate concentration peaked in 10~20 days in oleate microcosms, the maximum was reached in 100~120 days in the EVO microcosms, indicating that EVO hydrolysis was rate-limiting. The acetate accumulation was sustained over 50 days longer in the oleate and EVO than in the ethanol microcosms, suggesting that acetate-utilizing methanogenesis was slower in the cases of oleate and EVO. Both slow hydrolysis and methanogenesis could contribute to potential sustained bioreduction in field application. Biogeochemical models were developed to couple degradation of EVO, production and oxidation of long-chain fatty acids, glycerol, acetate, and hydrogen, reduction of Fe(III), U(VI) and sulfate, and methanogenesis with growth and decay of microbial functional groups. The models were used to simulate the coupled processes in a field test in a companion article.

Tang, Guoping↗

U(VI) bioreduction with emulsified vegetable oil as the electron donor-Model application to a field test

A one-time 2-hour emulsified vegetable oil (EVO) injection in a fast flowing aquifer decreased U discharge to a stream for over a year. Using a comprehensive biogeochemical model developed in the companion article based on microcosm tests, we approximately matched the observed acetate, nitrate, Fe, U, and sulfate concentrations, and described the major evolution trends of multiple microbial functional groups in the field test. While the lab-determined parameters were generally applicable in the field-scale simulation, the EVO hydrolysis rate constant was estimated to be an order of magnitude greater in the field than in the microcosms. The model predicted substantial biomass (sulfate reducers) and U(IV) accumulation near the injection wells and along the side boundaries of the treatment zone where electron donors (long-chain fatty acids) from the injection wells met electron acceptors (sulfate) from the surrounding environment. While EVO retention and hydrolysis characteristics were expected to control treatment longevity, modeling results indicated that electron acceptors such as sulfate may not only compete for electrons but also play a conducive role in degrading complex substrates and enhancing U(VI) reduction and immobilization. As a result, the spacing of the injection wells could be optimized for effective sustainable bioremediation.

Tang, Guoping↗

Modeling Precipitation and Sorption of Al, U and Co-contaminants during Titration of Acidic Sediments in Recirculation Flow-Through Experiments

We conducted batch and recirculating column titration tests with contaminated acidic sediments with controlled CO2 in the headspace, and extended the geochemical model by Gu et al. (2003, GCA) to better understand and quantify the reactions governing trace metal fate in the subsurface. The sediment titration curve showed slow pH increase due to strong buffering by Al precipitation and CO2 uptake. Assuming precipitation of basaluminite at low saturation index (SI=-4), and decreasing cation exchange selectivity coefficient (kNa\Al=0.3), the predictions are close to the observed pH and Al; and the model explains 1) the observed Ca, Mg, and Mn concentration decrease by cation exchange with sorbed Al, and 2) the decrease of U by surface complexation with Fe hydroxides at low pH, and precipitation as liebigite (Ca2UO2(CO3)3:10H2O) at pH>5.5. Without further adjustment geochemical parameters, the model describes reasonably well previous sediment and column titration tests without CO2 in the headspace, as well as the new large column test. The apparent inhibition of U and Ni decrease in the large column can be explained by formation of aqueous carbonate complexes and/or competition with carbonate for surface sites. These results indicated that ignoring labile solid phase Al would underestimate base requirement in titration of acidic aquifers.

Tang, Guoping↗

Hydrogeophysical investigations of the former S-3 ponds contaminant plumes

At the Oak Ridge Integrated Field Research Challenge site, near Oak Ridge, Tennessee, contaminants from the former S-3 ponds have infiltrated the shallow saprolite for over 60 years. Two- and three-dimensional DC-resistivity tomography is used to characterize the number and location of the main contaminant plumes, which include high concentration of nitrate. These contaminant plumes have typically an electrical resistivity in the range 2 20 ohm-m while the background saprolite resistivity is in the range 60 120 ohm-m, so the difference of resistivity can be easily mapped using DC-resistivity tomography to locate the contaminant pathways. We develop a relationship to derive the in situ nitrate concentrations from the 3D resistivity tomograms accounting for the effect of surface conductivity. The footprint of the contamination upon the resistivity is found to be much stronger than the local variations associated with changes in the porosity and the clay content. With this method, we identified a total of five main plumes (termed CP1 to CP5). Plume CP2 corresponds to the main plume in terms of nitrate concentration ( 50,000 ). We also used an active time constrained approach to perform time-lapse resistivity tomography over a section crossing the plumes CP1 and CP2. The sequence of tomograms is used to determine the changes in the nitrate concentrations associated with infiltration of fresh (meteoritic) water from a perched aquifer. This study highlights the importance of accounting for surface conductivity when characterizing plume distributions in clay-rich subsurface systems.

Revil, Andre↗

Description of Rhodanobacter denitrificans sp. nov., isolated from nitrate-rich zones of a contaminated aquifer

Bacterial strains 2APBS1T and 116-2 were isolated from the subsurface of a nuclear legacy waste site where sediments are co-contaminated with large amounts of acidity, nitrate, metal radionuclides and other heavy metals. A combination of physiological and genetic assays indicated that these strains represent the first members of the Rhodanobacter genus shown to be capable of complete denitrification. Cells of strain 2APBS1T and 116-2 were Gram negative, non-spore-forming, rods, 3-5 micro;m long and 0.25-0.5 m in diameter. The isolates were facultative anaerobes, and had temperature and pH optima for growth at 30 C and pH 6.5, respectively, and could tolerate up to 2.0 % NaCl, though growth improved in its absence. Strains 2APBS1T and 116-2 contained fatty acid profiles and 100 % Q-8 ubiquinone, that are characteristic features of the genus Rhodanobacter. Although strains 2APBS1T and 116-2 share high SSU rRNA gene sequence similarity to R. thiooxydans (>99%), DNA-DNA hybridization values were substantially below the 70% threshold used to designate novel species. Thus, based on genotypic, phylogenetic, chemotaxonomic and physiological differences, strains 2APBS1T and 116-2 are considered to represent a novel species of the genus Rhodanobacter, for which the name Rhodanobacter denitrificans sp. nov is proposed. The type strain is 2APBS1T (=DSM 23569T =JCM 17641T). Strain 116-2 (=DSM 24678 = JCM 17642) is a reference strain.

Prakash, Om↗

A Microsoft Excel Program for Two-Well Tracer Test Data Analysis

Two-well tracer tests are often conducted to investigate subsurface solute transport in the field. Analyzing breakthrough curves in the extraction and monitoring wells using numerical methods is nontrivial due to highly nonuniform flow conditions. We extended, and implemented analytical solutions for the convection-dispersion equation for an injection-extraction well-duplet in a homogeneous confined aquifer under steady state conditions. Functions were provided to calculate the concentrations in the extraction and monitoring wells at any location due to a step or pulse injection. Type curves for a step injection were compared with those calculated by numerically integrating the solution for a pulse injection. The results from the two approaches are similar when the dispersivity is small. As the dispersivity increases, the latter was found to be more accurate but requires more computing time. The code was verified by comparing the results with published type curves and applied to analyze data from the literature. It can be used as a first approximation for two-well tracer test data analysis, and to check accuracy of numerical solutions. The code and example files are publically-available.

54 ENVIRONMENTAL SCIENCES↗

Genome sequences for six Rhodanobacter strains isolated from soils and the terrestrial subsurface with variable denitrification capabilities

We report the first genome sequences for six strains of Rhodanobacter species isolated from a variety of soil and subsurface environments. Three of these strains are capable of complete denitrification and three others are not. However, all six strains contain most of the genes required for the respiration of nitrate to gaseous nitrogen. The nondenitrifying members of the genus lack only the gene for nitrate reduction, the first step in the full denitrification pathway. The data suggest that the environmental role of bacteria from the genus Rhodanobacter should be reevaluated.

54 ENVIRONMENTAL SCIENCES↗