Chris M. Yeager

Factors controlling mobility of 127I and 129I species in an acidic groundwater plume at the Savannah River Site

In order to quantify changes in iodine speciation and to assess factors controlling the distribution and mobility of iodine at an iodine-129 ((129)I) contaminated site located at the U.S. Department of Energys Savannah River Site (SRS), spatial distributions and transformation of (129)I and stable iodine ((127)I) species in groundwater were investigated along a gradient in redox potential (654 to 360 mV), organic carbon concentration (5 to 60 μmol L(-1)), and pH (pH 3.2 to 6.8). Total (129)I concentration in groundwater was 8.6±2.8 Bq L(-1) immediately downstream of a former waste seepage basin (well FSB-95DR), and decreased with distance from the seepage basin. (127)I concentration decreased similarly to that of (129)I. Elevated concentrations of (127)I or (129)I were not detected in groundwater collected from wells located outside of the mixed waste plume of this area. At FSB-95DR, the majority (55-86%) of iodine existed as iodide for both (127)I and (129)I. Then, as the iodide move down gradient, some of it transformed into iodate and organo-iodine. Considering that iodate has a higher K(d) value than iodide, we hypothesize that the production of iodate in groundwater resulted in the removal of iodine from the groundwater and consequently decreased concentrations of (127)I and (129)I in downstream areas. Significant amounts of organo-iodine species (30-82% of the total iodine) were also observed at upstream wells, including those outside the mixed waste plume. Concentrations of groundwater iodide decreased at a faster rate than organo-iodine along the transect from the seepage basin. We concluded that removal of iodine from the groundwater through the formation of high molecular weight organo-iodine species is complicated by the release of other more mobile organo-iodine species in the groundwater.

Iodide Accumulation by Aerobic Bacteria Isolated from Subsurface Sediments of a 129I-Contaminated Aquifer at the Savannah River Site, South Carolina

ABSTRACT 129I is of major concern because of its mobility in the environment, excessive inventory, toxicity (it accumulates in the thyroid), and long half-life (∼16 million years). The aim of this study was to determine if bacteria from a 129I-contaminated oxic aquifer at the F area of the U.S. Department of Energys Savannah River Site, SC, could accumulate iodide at environmentally relevant concentrations (0.1 μM I−). Iodide accumulation capability was found in 3 out of 136 aerobic bacterial strains isolated from the F area that were closely related to Streptomyces/Kitasatospora spp., Bacillus mycoides, and Ralstonia/Cupriavidus spp. Two previously described iodide-accumulating marine strains, a Flexibacter aggregans strain and an Arenibacter troitsensis strain, accumulated 2 to 50% total iodide (0.1 μM), whereas the F-area strains accumulated just 0.2 to 2.0%. Iodide accumulation by FA-30 was stimulated by the addition of H2O2, was not inhibited by chloride ions (27 mM), did not exhibit substrate saturation kinetics with regard to I− concentration (up to 10 μM I−), and increased at pH values of <6. Overall, the data indicate that I− accumulation likely results from electrophilic substitution of cellular organic molecules. This study demonstrates that readily culturable, aerobic bacteria of the F-area aquifer do not accumulate significant amounts of iodide; however, this mechanism may contribute to the long-term fate and transport of 129I and to the biogeochemical cycling of iodine over geologic time.

A versatile method for preparation of hydrated microbial–latex biocatalytic coatings for gas absorption and gas evolution

We describe a latex wet coalescence method for gas-phase immobilization of microorganisms on paper which does not require drying for adhesion. This method reduces drying stresses to the microbes. It is applicable for microorganisms that do not tolerate desiccation stress during latex drying even in the presence of carbohydrates. Small surface area, 10–65xa0μm thick coatings were generated on chromatography paper strips and placed in the head-space of vertical sealed tubes containing liquid to hydrate the paper. These gas-phase microbial coatings hydrated by liquid in the paper pore space demonstrated absorption or evolution of H2, CO, CO2 or O2. The microbial products produced, ethanol and acetate, diffuse into the hydrated paper pores and accumulate in the liquid at the bottom of the tube. The paper provides hydration to the back side of the coating and also separates the biocatalyst from the products. Coating reactivity was demonstrated for Chlamydomonas reinhardtii CC124, which consumed CO2 and produced 10.2xa0±xa00.2xa0mmolxa0O2xa0m−2xa0h−1, Rhodopseudomonas palustris CGA009, which consumed acetate and produced 0.47xa0±xa00.04xa0mmolxa0H2xa0m−2xa0h−1, Clostridium ljungdahlii OTA1, which consumed 6xa0mmol COxa0m−2xa0h−1, and Synechococcus sp. PCC7002, which consumed CO2 and produced 5.00xa0±xa00.25xa0mmol O2xa0m−2xa0h−1. Coating thickness and microstructure were related to microbe size as determined by digital micrometry, profilometry, and confocal microscopy. The immobilization of different microorganisms in thin adhesive films in the gas phase demonstrates the utility of this method for evaluating genetically optimized microorganisms for gas absorption and gas evolution.

Groundwater Radioiodine: Prevalence, Biogeochemistry, and Potential Remedial Approaches

Iodine-129 ({sup 129}I) has not received as much attention in basic and applied research as other contaminants associated with DOE plumes. These other contaminants, such as uranium, plutonium, strontium, and technetium are more widespread and exist at more DOE facilities. Yet, at the Hanford Site and the Savannah River Site {sup 129}I occurs in groundwater at concentrations significantly above the primary drinking water standard and there is no accepted method for treating it, other than pump-and-treat systems. With the potential arrival of a Nuclear Renaissance, new nuclear power facilities will be creating additional {sup 129}I waste at a rate of 1 Ci/gigawatts energy produced. If all 22 proposed nuclear power facilities in the U.S. get approved, they will produce more {sup 129}I waste in seven years than presently exists at the two facilities containing the largest {sup 129}I inventories, ({approx}146 Ci {sup 129}I at the Hanford Site and the Savannah River Site). Hence, there is an important need to fully understand {sup 129}I behavior in the environment to clean up existing plumes and to support the expected future expansion of nuclear power production. {sup 129}I is among the key risk drivers at all DOE nuclear disposal facilities where {sup 129}Imorexa0» is buried, because of its long half-life (16 million years), high toxicity (90% of the bodys iodine accumulates in the thyroid), high inventory, and perceived high mobility in the subsurface environment. Another important reason that {sup 129}I is a key risk driver is that there is the uncertainty regarding its biogeochemical fate and transport in the environment. We typically can define {sup 129}I mass balance and flux at sites, but can not accurately predict its response to changes in the environment. This uncertainty is in part responsible for the low drinking water standard, 1 pCi/L {sup 129}I, and the low permissible inventory limits (Ci) at the Savannah River Site, Hanford Site, and the former Yucca Mountain disposal facilities. The objectives of this report are to: (1) compile the background information necessary to understand behavior of {sup 129}I in the environment, (2) discuss sustainable remediation approaches to {sup 129}I contaminated groundwater, and (3) identify areas of research that will facilitate remediation of {sup 129}I contaminated areas on DOE sites. Lines of scientific inquiry that would significantly advance the goals of basic and applied research programs for accelerating {sup 129}I environmental remediation and reducing uncertainty associated with disposal of {sup 129}I waste are: (1) Evaluation of amendments or other treatment systems that can sequester subsurface groundwater {sup 129}I. (2) Develop analytical techniques for measurement of total {sup 129}I that eliminate the necessity of collecting and shipping large samples of groundwater. (3) Develop and evaluate ways to manipulate areas with organic-rich soil, such as wetlands, to maximize {sup 129}I sorption, minimizing releases during anoxic conditions. (4) Develop analytical techniques that can identify the various {sup 129}I species in the subsurface aqueous and solid phases at ambient concentrations and under ambient conditions. (5) Identify the mechanisms and factors controlling iodine-natural organic matter interactions at appropriate environmental concentrations. (6) Understand the biological processes that transform iodine species throughout different compartments of subsurface waste sites and the role that these processes have on {sup 129}I flux.«xa0less

Direct analysis of sulfate reducing bacterial communities in gas hydrate-impacted marine sediments by PCR–DGGE

Molecular investigations of the sulfate reducing bacteria that target the dissimilatory sulfite‐reductase subunit A gene (dsr A) are plagued by the nonspecific performance of conventional PCR primers. Here we describe the incorporation of the FailSafe™ PCR System to optimize environmental analysis of dsr A by PCR amplification and denaturing gradient gel electrophoresis. PCR–DGGE analysis of dsr A composition revealed that SRB diversity was greater and more variable throughout the vertical profile of a marine sediment core obtained from a gas hydrate site (GC234) in the Gulf of Mexico than in a sediment core collected from a nearby site devoid of gas hydrates (NBP). Depth profiled dsr B abundance corresponded with sulfate reduction rates at both sites, though measurements were higher at GC234. This study exemplifies the numerical and functional importance of sulfate reducing bacteria in deep‐sea sedimentary environments, and incremental methodological advancements, as described herein, will continue to streamline the analysis of sulfate reducer communities in situ. (© 2009 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)

Preservation of H2 production activity in nanoporous latex coatings of Rhodopseudomonas palustris CGA009 during dry storage at ambient temperatures

To assess the applicability of latex cell coatings as an ‘off‐the‐shelf’ biocatalyst, the effect of osmoprotectants, temperature, humidity and O2 on preservation of H2 production in Rhodopseudomonas palustris coatings was evaluated. Immediately following latex coating coalescence (24u2009h) and for up to 2 weeks of dry storage, rehydrated coatings containing different osmoprotectants displayed similar rates of H2 production. Beyond 2 weeks of storage, sorbitol‐treated coatings lost all H2 production activity, whereas considerable H2 production was still detected in sucrose‐ and trehalose‐stabilized coatings. The relative humidity level at which the coatings were stored had a significant impact on the recovery and subsequent rates of H2 production. After 4 weeks storage under air at 60% humidity, coatings produced only trace amounts of H2 (0–0.1% headspace accumulation), whereas those stored at <u20095% humidity retained 27–53% of their H2 production activity after 8 weeks of storage. When stored in argon at <u20095% humidity and room temperature, R.u2009palustris coatings retained full H2 production activity for 3 months, implicating oxidative damage as a key factor limiting coating storage. Overall, the results demonstrate that biocatalytic latex coatings are an attractive cell immobilization platform for preservation of bioactivity in the dry state.