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Brooks, Scott C

Publications and source records attributed to Brooks, Scott C.

WHONDRS 48 Hour Diel Cycling Study at the East Fork Poplar Creek in Tennessee, USA

This dataset is from a sampling campaign completed over the course of 48 hours to investigate the effects of wastewater treatment plant effluent induced water level variation on aqueous chemistry, dissolved organic matter chemistry, and metabolic potential of microbial communities at the East Fork Poplar Creek, TN, USA. Filtered surface water (SW) and pore water (PP) samples were collected every three hours in August 2018. This dataset is one of seven companion datasets that were part of the WHONDRS 48 Hour Diel Cycling Study of freshwater rivers. All seven datasets are available on ESS-DIVE; they can be found by searching for WHONDRS 48 Hour.This package contains a variety of chemical and hydrologic variables. All data types are provided in a standard format. Basic geochemistry analyses (e.g., non-purgeable organic carbon concentration, cations, anions, SpC, pH) were conducted, standardized photos were taken, surface water hydrographs were collated from existing instrumentation, and extensive metadata were captured. Aqueous chemistry variables include USGS codes in the first portion of the variable name (e.g., 00940_Cl_mg_per_L). These codes allow for interoperability with USGS water quality data. In addition, samples were delivered to the Environmental Molecular Sciences Laboratory (EMSL; https://www.pnnl.gov/environmental-molecular-sciences-laboratory) for high resolution characterization of dissolved organic matter via 12 Tesla Fourier transform ion cyclotron resonance mass spectrometry (FTICR-MS). The data package contains instructions to process the FTICR data based on the user’s specific needs, and sample-level summary indices derived from the FTICR data will be added to the data package. Beyond the data in this data package, metagenomic data are being generated on associated microbial communities. When these data are available, the data package will be updated with information on accessing them. Please contact WHONDRS@pnnl.gov for more information. Please use the data package’s DOI to cite the data package. We ask that you email us at WHONDRS@pnnl.gov to let us know that you're using the data and acknowledge WHONDRS and the U.S. Department of Energy's Subsurface Biogeochemical Research program—which generously provides funding to WHONDRS—in your publications, proposals, presentations, etc. All data are free to be used for any purpose, such as for manuscripts, presentations, and grant proposals. Note that the included hydrograph has a separate DOI that should also be cited. There is no obligation to include WHONDRS members as co-authors.

54 ENVIRONMENTAL SCIENCES↗

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↗

Impact of collection container material and holding times on sample integrity for mercury and methylmercury in water

Mercury (Hg) and methylmercury (MeHg) concentrations in streamwater can vary on short timescales (hourly or less) during storm flow and on a diel cycle; the frequency and timing of sampling required to accurately characterize these dynamics may be difficult to accomplish manually. Automated sampling can assist in sample collection; however use has been limited for Hg and MeHg analysis due to stability concerns of trace concentrations during extended storage times. We examined the viability of using automated samplers with disposable low-density polyethylene (LDPE) sample bags to collect industrially contaminated streamwater for unfiltered and filtered Hg and MeHg analysis. Specifically we investigated the effect of holding times ranging from hours to days on streamwater collected during baseflow and storm flow. Unfiltered and filtered Hg and MeHg concentrations decreased with increases in time prior to sample processing; holding times of 24 hours or less resulted in concentration changes (mean 11 7% different) similar to variability in duplicates collected manually during analogous field conditions (mean 7 10% different). Comparisons of samples collected with manual and automated techniques throughout a year for a wide range of stream conditions were also found to be similar to differences observed between duplicate grab samples. These results demonstrate automated sampling into LDPE bags with holding times of 24 hours or less can be effectively used to collect streamwater for Hg and MeHg analysis, and encourage the testing of these materials and methods for implementation in other aqueous systems where high-frequency sampling is warranted.

holding time↗

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↗

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↗

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↗

Characterization of the Deltaproteobacteria in contaminated and uncontaminated stream sediments and identification of potential mercury methylators

Microbial communities were examined in surface stream sediments at 5 contaminated sites and 1 control site near Oak Ridge, TN, USA, to identify bacteria that could be contributing to mercury (Hg) methylation. The phylogenetic composition of the sediment bacterial community was examined over 3 quarterly sampling periods (36 samples) using 16S rRNA gene pyrosequencing. Only 3064 sequences (0.85% of the total community) were identified as Deltaproteobacteria, the only group known to methylate Hg, using the Ribosomal Database Project classifier at the 99% confidence threshold. Constrained ordination techniques indicated statistically significant positive linear correlations between Desulfobulbus spp., Desulfonema spp. and Desulfobacca spp. and methyl-Hg concentrations at the Hg-contaminated sites. In contrast, the distribution of organisms related to Byssovorax spp. was significantly correlated to inorganic carbon, nitrate and uranium concentrations but not to Hg or methyl-Hg. Overall, the abundance and richness of Deltaproteobacteria sequences were higher in uncontaminated sediments, while the majority of the members present at the contaminated sites were either known potential metal-reducers/methylators or metal tolerant species. Given the abundance relative to other known Hg methylators and the association with methyl-Hg, Desulfobulbus spp. is considered a prime candidate for involvement in Hg methylation in these streams.

59 BASIC BIOLOGICAL SCIENCES↗