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At least 73 records · Page 4
All sourcesNASA NTRSDOE OSTI
DOE OSTI2019

Development of Processing Technology for Radioactively Contaminated Water at Chernobyl Nuclear Power Plant - 19656

During the operation of the Chernobyl Nuclear Power Plant, distillation by evaporation was the main method for processing radioactively contaminated water. When the plant was decommissioned, the evaporation facility was mothballed and floor drain treatment was suspended in 2016. At present, the existing tanks with the capacity of 26,000 m{sup 3} are more than 60% full with radioactively contaminated floor drains, which requires alternative processing methods. The current process flow for radioactive waste management at State Specialized Enterprise 'Chernobyl NPP' includes processing of accumulated liquid radioactive wastes at a liquid radioactive wastes processing plant. Under the processing technology, liquid radioactive waste is immobilized at the plant by cementation and the resulting solid radioactive waste is then buried in a near-surface storage. Key factors for the selection of alternative radioactively contaminated water processing methods are the possibility to clear the processed water (no control monitoring), which requires the same degree of processing as for drinking water, and minimization of radioactive waste generation due to the lack of free space for solid waste disposal in the near-surface storage. Floor drains that require processing contain radionuclides such as {sup 137}Cs, {sup 90}Sr, {sup 60}Co and {sup 40}K. The current level of the total beta and gamma activity is about 4*105 Bq/kg. The following criteria are set for the Chernobyl NPP site for water to be disposed to the sewerage system: - Max. 37 Bq/kg for the total beta and gamma containing radionuclide activity; - Max. 0.7 Bq/kg for the total alpha containing radionuclide activity. METOIL produces inorganic sorbents for removing radionuclides from liquids and develops sorbent-based technology for a variety of applications related to liquid radioactive waste processing. In 2017-2018, experts from the Chernobyl NPP and METOIL ran several joint laboratory tests to evaluate the efficiency of inorganic sorbents made by METOIL for processing floor drains at the Chernobyl NPP. The test procedure included treatment of radioactively contaminated water in a two-stage sorption process: static sorption (sorbents are mixed in a liquid) and dynamic sorption (the liquid is filtered through a sorbent column). NIKET and MODIKS sorbents were provided for the tests. The results of the test measurements showed that the total alpha containing radionuclide activity is less than 0.026 Bq/kg and the total beta and gamma containing radionuclide activity is 9.2 Bq/kg. The physical and chemical parameters after processing also met the water disposal criteria. High sorption capacity of the sorbents used for the tests allows processing hundreds of water volumes with just one sorbent volume. At present, preparations are underway for full-scale tests at a pilot plant with a capacity of minimum 10 m{sup 3}/day. At a later stage, spent sorbents may be immobilized by inclusion into the cement matrix, which will substantially reduce the amount of radioactive waste to be buried. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2020

Novel Foaming Solutions for High Level Waste (HLW) Processing - 20195

Foaming occurs during treatment of high level waste (HLW) at Savannah River Site's Defense Waste Processing Facility (DWPF) in the Chemical Process Cell (CPC) due to high gas generation from process steam and chemical offgas products [1]. The presence of amphiphilic particles in the waste slurry stabilizes the foam [2], [3]. Efficient processing of HLW requires foam control, as foam-overs lead to lower productivity and potential radioactive contamination of condensate streams. DWPF currently employs Siovation Antifoam 747, a surfactant produced by Momentive Performance Materials, as an antifoaming agent during waste treatment. Despite its ability to control foam generation, processing issues have arisen from its use [4]. During DWPF chemical processing, a chemical antifoam agent must be effective at temperatures up to 103 deg. C between pH 3-13. Antifoam 747 is effective at pH 7 but degrades as pH deviates [5]. Antifoam 747 is 90% by weight Momentive{sup TM} L77 and 10% by weight Momentive{sup TM} Y-17580. These ingredients are trisiloxane products, which are especially vulnerable to attack in acidic and caustic environments. Since Antifoam 747 readily degrades, periodic addition is required. Several processing concerns related to Antifoam 747 have affected DWPF operation. Its overuse warranted concern of potential flammable melter offgas under upset conditions due to the generation of carbon dioxide and hydrogen. As a result, a Potential Inadequacy in the Safety Analysis (PISA) was declared [6]. Antifoam contribution has been included in the melter offgas flammability strategy and the quantity of antifoam is monitored to ensure limits are not exceeded. Testing at Savannah River National Laboratory (SRNL) determined that propanal, tri-methylsilanol, and hexamethyldisiloxane are generated as Antifoam 747 degrades, leading to a second PISA [7]. The formation of these byproducts poses additional flammability risks. Furthermore, the methyl and ethyl groups of these compounds may be responsible for the formation of the methyl and ethyl mercury discovered in DWPF [8], [9]. The formation of organomercury has specifically been called out by DOE as a need for increased research. The effectiveness of non-chemical methods for foam control and the efficiency of alternative antifoam agents were evaluated as part of an effort to improve HLW treatment operations at DWPF and to reduce, or eliminate, the flammability hazards associated with Antifoam 747 currently in use. Foaming of high-level waste (HLW) slurries is an issue at the Defense Waste Processing Facility (DWPF) Chemical Process Cell (CPC) which is currently mitigated with a chemical antifoam agent. The effectiveness of non-chemical methods for foam control and the efficiency of alternative antifoams were examined to improve HLW treatment at DWPF and to eliminate the flammability hazards associated with Siovation Antifoam 747 currently in use. Non-chemical foam control methods were deemed unviable for chemical processing at DWPF, as the spray/mist technique requires too much water and space limitations make installation and implementation of headspace agitators unfeasible. The use of ultrasonic energy thickened and further stabilized the foam. Two suitable alternative defoaming agents, Momentive{sup TM} Y- 17112 and Evonik Surfynol{sup R} MD-20, were identified. Both defoamers control foam over a pH range of 4- 13 at boiling, with no flammable degradation products, and only minimal quantities (100-200 mg/kg) are required under glycolic acid conditions. In order to validate the effectiveness of these defoaming agents, SRNL recommends irradiation testing and laboratory scale SRAT/SME experiments with actual radioactive waste. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2017

Redox Controls over the Stability of U(IV) in Floodplains of the Upper Colorado River Basin

Here, aquifers in the Upper Colorado River Basin (UCRB) exhibit persistent uranium (U) groundwater contamination plumes originating from former ore processing operations. Previous observations at Rifle, Colorado, have shown that fine grained, sulfidic, organic-enriched sediments accumulate U in its reduced form, U(IV), which is less mobile than oxidized U(VI). These reduced sediment bodies can subsequently act as secondary sources, releasing U back to the aquifer. There is a need to understand if U(IV) accumulation in reduced sediments is a common process at contaminated sites basin-wide, to constrain accumulated U(IV) speciation, and to define the biogeochemical factors controlling its reactivity. We have investigated U(IV) accumulation in organic-enriched reduced sediments at three UCRB floodplains. Noncrystalline U(IV) is the dominant form of accumulated U, but crystalline U(IV) comprises up to ca. 30% of total U at some locations. Differing susceptibilities of these species to oxidative remobilization can explain this variability. Particle size, organic carbon content, and pore saturation, control the exposure of U(IV) to oxidants, moderating its oxidative release. Further, our data suggest that U(IV) can be mobilized under deeply reducing conditions, which may contribute to maintenance and seasonal variability of U in groundwater plumes in the UCRB.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2014

Evapotranspiration And Geochemical Controls On Groundwater Plumes At Arid Sites: Toward Innovative Alternate End-States For Uranium Processing And Tailings Facilities

Management of legacy tailings/waste and groundwater contamination are ongoing at the former uranium milling site in Tuba City AZ. The tailings have been consolidated and effectively isolated using an engineered cover system. For the existing groundwater plume, a system of recovery wells extracts contaminated groundwater for treatment using an advanced distillation process. The ten years of pump and treat (P&T) operations have had minimal impact on the contaminant plume – primarily due to geochemical and hydrological limits. A flow net analysis demonstrates that groundwater contamination beneath the former processing site flows in the uppermost portion of the aquifer and exits the groundwater as the plume transits into and beneath a lower terrace in the landscape. The evaluation indicates that contaminated water will not reach Moenkopi Wash, a locally important stream. Instead, shallow groundwater in arid settings such as Tuba City is transferred into the vadose zone and atmosphere via evaporation, transpiration and diffuse seepage. The dissolved constituents are projected to precipitate and accumulate as minerals such as calcite and gypsum in the deep vadose zone (near the capillary fringe), around the roots of phreatophyte plants, and near seeps. The natural hydrologic and geochemical controls common in arid environments such as Tuba City work together to limit the size of the groundwater plume, to naturally attenuate and detoxify groundwater contaminants, and to reduce risks to humans, livestock and the environment. The technical evaluation supports an alternative beneficial reuse (“brownfield”) scenario for Tuba City. This alternative approach would have low risks, similar to the current P&T scenario, but would eliminate the energy and expense associated with the active treatment and convert the former uranium processing site into a resource for future employment of local citizens and ongoing benefit to the Native American Nations.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2022

Alternative Conceptual Models of the Subsurface at the Hanford Site

This report describes the use of a multipoint geostatistics (MPS) framework with multiple data types for developing alternative conceptual-mathematical models of the subsurface at the Hanford Site. Developing multiple conceptual-mathematical models of the site is important for assessing potential uncertainties related to the features, events, and processes that control the subsurface flow of groundwater and the transport of contaminants of concern (COCs). Evaluating the effects of these uncertainties can result in better site characterization, monitoring, and remedial decisions.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2012

Advanced process control and novel test methods for PVD silicon and elastomeric silicone coatings utilized on ion implant disks, heatsinks and selected platens

Coatings play multiple key roles in the proper functioning of mature and current ion implanters. Batch and serial implanters require strategic control of elemental and particulate contamination which often includes scrutiny of the silicon surface coatings encountering direct beam contact. Elastomeric Silicone Coatings must accommodate wafer loading and unloading as well as direct backside contact during implant plus must maintain rigid elemental and particulate specifications. The semiconductor industry has had a significant and continuous effort to obtain ultra-pure silicon coatings with sustained process performance and long life. Low particles and reduced elemental levels for silicon coatings are a major requirement for process engineers, OEM manufacturers, and second source suppliers. Relevant data will be presented. Some emphasis and detail will be placed on the structure and characteristics of a relatively new PVD Silicon Coating process that is very dense and homogeneous. Wear rate under typical ion beam test conditions will be discussed. The PVD Silicon Coating that will be presented here is used on disk shields, wafer handling fingers/fences, exclusion zones of heat sinks, beam dumps and other beamline components. Older, legacy implanters can now provide extended process capability using this new generation PVD silicon - even on implanter systems that were shipped long before the advent of silicon coating for contamination control. Low particles and reduced elemental levels are critical performance criteria for the silicone elastomers used on disk heatsinks and serial implanter platens. Novel evaluation techniques and custom engineered tools are used to investigate the surface interaction characteristics of multiple Elastomeric Silicone Coatings currently in use by the industry - specifically, friction and perpendicular stiction. These parameters are presented as methods to investigate the critical wafer load and unload function. Unique tools and test methods have been developed that deliver accurate and repeatable data, which will be described.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Conditioning and Requalification of Legacy Waste Packages - 18648

In most German interim storage facilities, hundreds of waste packages are waiting for re-conditioning and qualification to comply with the waste acceptance criteria (WAC) for the Konrad repository. Especially the waste classification as well as some characteristics and the description of the material composition in its current state do not comply with the Konrad requirements since the conditioning of these waste packages took place up to 40 years ago. The German name for these waste packages is 'Altgebinde', hereafter referred to as 'legacy waste packages'. The present article will provide an overview of the measures for the qualification of these legacy waste packages to fulfill the Konrad requirements. The following measures, when necessary, are carried out for the qualification of legacy waste packages: - Collection and evaluation of all documents related to the primary conditioning process, e. g. the used equipment, documented waste and packaging properties, conditioning and radiology, if available (hereafter 'old documents'). - Preparation of a conceptual report and a process control quality plan based on existing data, with appropriate measures to qualify the waste packages. Assessment and approval of the process control quality plan by the competent authority. - Characterization of the waste and packaging properties by visual inspection or tomography, recording or updating of dose rate, contamination and mass, verification of product stability, for example by gas analysis of the interior atmosphere of the container. - Characterization of the nuclide inventory by gammas scans, sample taking to analyze nuclides which can not be measured by means of in-situ gamma spectrometry, and for material declaration. - Qualification or post-conditioning of the legacy waste packages if necessary, e. g. by drying the waste packages and packaging them in containers approved for disposal. - Compilation of all results of the above mentioned tests and steps to create a waste package documentation, including the calculations for the nuclide inventory and the description of the material composition of the waste packages. - Receiving approval by the competent authority after evaluation of the final documentation. The aim behind this structured approach is to prevent additional, unnecessary measures and treatment of the waste. Consequently, the additional characterization is preferably carried out on the basis of the available documents. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2018

Biochemical Mechanisms and Associated Biomolecular Signatures Underlying Energy Strategies of Geobacter Sulfurreducens

To provide the scientific understanding required to allow DOE sites to incorporate relevant biological, chemical, and physical processes into decisions concerning environmental remediation, a fundamental understanding of the controls on micro-organism growth in the subsurface is necessary. Specifically, mobility of metals in the environment, including chromium, technetium and uranium, is greatly affected by the process of dissimilatory metal reduction (DMR). DMR has been shown to be an important biological activity controlling contaminant mobility in the subsurface at many DOE sites. Long-term maintenance of DMR at constant rates must rely upon steady fluxes of electron donors to provide the maintenance energy needed by organisms such as Geobacter sulfurreducens to maintain steady state populations in the subsurface. At present, much effort has been put forth to develop biomolecular signatures which inform on the relevant biological processes at DOE field sites. These signatures are also being developed in defined laboratory conditions to which the field data can be compared to. These signatures include metagenomic, metatranscriptomic and proteomic characterization. While the relevant processes involve reduction of metal contaminants, we suggest that the predominant biochemistry that impacts the biomolecular signature is nutrient availability/limitation. As such, the present proposal aims at characterizing the survival strategy of Geobacter and obtaining biomolecular signatures that would reflect on its energy flux status. In addition, we lack the fundamental knowledge needed to answer fundamental questions such as these: What influxes of electron donors are required to maintain a growing versus a non-growing population of Geobacter? How do changes in nutrient availability or other environmental conditions such as pH and ionic strength affect such required electron-donor influxes? How are these electron-donor influxes controlled by availability and nature of electron acceptors? Under survival conditions, where availability of electron acceptors and nutrients are extremely low, what physiological and genetic modifications occur in Geobacter to enable long-term survival? How do these changes affect the required electron-donor influxes? Is it possible to relate the metabolic activities of Geobacter living under survival mode to the required fluxes of electron donors? What conceptual models can be used to predict maintenance energies of Geobacter under different phases of growth when measured under different environmental conditions? How can these models help the DOE predict the long-term evolution of contaminated sites? We outline a strategy to tackle these questions and lay the framework for DOE to make long-term predictions concerning DMR in the subsurface. We will test the following hypothesis: Geobacter requires different fluxes of substrate for metabolism when existing under growth, stationary, or survival modes, and these substrate fluxes can be related to specific metabolic activities utilized under different geochemical conditions. Our project has two specific objectives: i) Determine the survival characteristics of Geobacter under long-term stationary phase by characterize the physiological response of Geobacter in growth, stationary, and survival phases using genomic sequencing, DNA microarray chips and iTRAQ (proteomics) and relate these responses to the measured substrate fluxes; ii) Determination of growth yield and maintenance energy. While site-specific studies are necessary for site-specific remediation, our work will provide the fundamental knowledge necessary for long-term stewardship of all DOE sites where contaminant mobility is affected by dissimilatory metal reduction.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2017

Post-Closure Monitoring Report for Corrective Action Unit 98, Frenchman Flat, Underground Test Area, Nevada National Security Site, Nevada for Calendar Year 2016 (January 2016–December 2016), Revision 0

Corrective Action Unit (CAU) 98: Frenchman Flat on the Nevada National Security Site was the location of 10 underground nuclear tests. CAU 98 underwent a series of investigations and actions in accordance with the Federal Facility Agreement and Consent Order to assess contamination of groundwater by radionuclides from the tests. A Closure Report completed that process in 2016 and called for long-term monitoring, use restrictions (URs), and institutional controls to protect the public and environment from potential exposure to contaminated groundwater. Three types of monitoring are performed for CAU 98: water quality, water level, and institutional control. These are evaluated to determine whether the UR boundaries remain protective of human health and the environment, and to ensure that the regulatory boundary objectives are being met. Additionally, monitoring data are used to evaluate consistency with the groundwater flow and contaminant transport models because the contaminant boundaries (CBs) calculated with the models are the primary basis of the UR boundaries. In summary, the monitoring results from 2016 indicate the regulatory controls on the closure of CAU 98 remain effective in protection of human health and the environment. Recommendations resulting from this first year of monitoring activities include formally incorporating wells UE-5 PW-1, UE-5 PW-2, and UE-5 PW-3 into the groundwater-level monitoring network given their strategic location in the basin; and early development of a basis for trigger levels for the groundwater-level monitoring given the observed trends. Additionally, it is recommended to improve the Real Estate/Operations Permit process for capturing information important for evaluating the impact of activities on groundwater resources, and to shift the reporting requirement for this annual report from the second quarter of the federal fiscal year (end of March) to the second quarter of the calendar year (end of June).

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2012

Kinetic Modeling of Microbiological Processes

Kinetic description of microbiological processes is vital for the design and control of microbe-based biotechnologies such as waste water treatment, petroleum oil recovery, and contaminant attenuation and remediation. Various models have been proposed to describe microbiological processes. This editorial article discusses the advantages and limiation of these modeling approaches in cluding tranditional, Monod-type models and derivatives, and recently developed constraint-based approaches. The article also offers the future direction of modeling researches that best suit for petroleum and environmental biotechnologies.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2022

Design Considerations for Controlling Silicon Nanoparticle Nucleation and Growth in a Nonthermal Plasma

Controlling the nucleation and growth of nanoparticles in low temperature plasma systems is imperative for controlling nanoparticle size distributions; and for some applications such as deposition and etching in microelectronic processing, preventing particle contamination. In this work, silicon nanoparticle (NP) production from silane is used as a model system to investigate the nucleation process. Although the mechanisms responsible for silicon NP nucleation and growth have been studied, it is unclear how controllable system parameters (e.g., pressure, system geometry, and gas composition) can be used to inhibit or promote NP formation. For example, the transport of reactive silane species is expected to significantly affect the feed fraction of silane required to nucleate silicon NP (the nucleation onset fraction) due to losses at the reactor walls. In this work, NP mass density was determined as a function of system pressure, gas composition, and reactor diameter for a tubular flow-through radiofrequency (RF) plasma using Ar/H2/He/SiH4 gas mixtures. A quartz crystal microbalance (QCM) impactor was developed to measure the total aerosol mass density downstream of the plasma and thereby identify the nucleation onset and its dependence on process parameters. Finally, a reaction mechanism was developed and incorporated into a global plasma chemistry model to better understand the nucleation onset and NP growth.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Current Status of Decommissioning Plans and Chemical Decontamination of Metal Scraps in Chinshan NPP - 19304

The decommissioning of nuclear facilities has become a significantly attractive and worldwide topic due to the end of lifetime of many nuclear power plants within next coming years. In Taiwan, Chinshan nuclear power plant owned by the Taiwan Power Company will be the first candidate to be decommissioned according to the Nuclear Reactor Facilities Regulation Act. The Chinshan nuclear power plant located in New Taipei City has two units of 636 MWe boiling water reactors (BWRs) for the generation of 9 billion kWh of electricity per year. The date of cessation of operation of Unit No. 1 and Unit No. 2 will be December in 2018 and July in 2019, respectively. Based on the Regulations for the Review and Approval of Applications for a Decommissioning Permit of Nuclear Reactor Facilities, Taiwan Power Company have submitted a decommissioning plan of Chinshan nuclear power plant to the authority, Atomic Energy Council (AEC). After the review process, the decommissioning plan of Chinshan nuclear power plant has been permitted by AEC in 2017. Decontamination is generally utilized during the period of decommissioning of nuclear facility in order to minimize the radiation exposure of personnel and the cost of management of radioactive wastes. The successful decontamination also probably provides the benefits of lowering the level of radioactive wastes, facilitating potential releases, permitting the reuse of metals and facilitating the radiation principle of As Low As Reasonably Achievable (ALARA) management. Decontamination aims at the removal of radioactive materials from the contaminated surfaces by several technologies such as washing, heating, chemical reaction and mechanical process. The selection of proper decontamination technologies are depended on the requirement of the target materials and the purpose of the decontamination. Chemical decontamination has been proven to be an effective in reducing the radioactivity for metallic materials by using chemical reagents in contact with the contaminated surfaces. During the operation of Chinshan nuclear power plant, chemical decontamination was performed for Unit No.1 and No.2 in 2000 to decontaminate the Reactor Recirculation System (RRS) and Reactor Water Clean-up Systems (RWCU) by using LOMI-NP-LOMI process. Based on the previous experience of chemical decontamination, the dismantled metallic piping is provided as sample by Chinshan nuclear power plant for the evaluation of the feasibility of chemical decontamination. The provided metallic sample is composed of carbon steel with dose rate around 0.2 mSv/hr. In this report, a multistep decontamination process using strongly oxidizing solution and organic acid solution is performed to remove the contaminated oxide layer from the metal surface, and the resulting contact dose rate and decontamination factor (DF) are also shown to discuss the performance in relation to the process control factors. In this paper, the recent progress in decommissioning programs and preliminary results of the decontamination experiment are described to provide usable information regarding the future decommissioning for Chinshan nuclear power plant. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2012

Laboratory and Lysimeter Experimentation and Transport Modeling of Neptunium and Strontium in Savannah River Site Sediments

The Savannah River Site (SRS) conducts performance assessment (PA) calculations to determine the appropriate amount of low-level radiological waste that can be safely disposed on site. Parameters are included in these calculations that account for the interaction between the immobile solid phase and the mobile aqueous phase. These parameters are either the distribution coefficient (K$_{d}$ value) or the apparent solubility value (K$_{sp}$). These parameters are readily found in the literature and are used throughout the DOE complex. One shortcoming of K$_{d}$ values is that they are only applicable to a given set of solid and aqueous phase conditions. Therefore, a given radionuclide may have several K$_{d}$ values as it moves between formations and comes into contact with different solids and different aqueous phases. It is expected that the K$_{d}$ construct will be appropriate to use for a majority of the PA and for a majority of the radionuclides. However, semi-mechanistic models would be more representative in isolated cases where the chemistry is especially transitory or the radionuclide chemistry is especially complex, bringing to bear multiple species of varying sorption tendencies to the sediment. Semi-mechanistic models explicitly accommodate the dependency of K$_{d}$ values, or other sorption parameters, on contaminant concentration, competing ion concentrations, pH-dependent surface charge on the adsorbent, and solute species distribution. Incorporating semi-mechanistic concepts into geochemical models is desirable to make the models more robust and technically defensible. Furthermore, these alternative models could be used to augment or validate a K$_{d}$-based DOE Order 435.1 Performance Assessment. The objectives of this study were to: 1) develop a quantitative thermodynamically-based model for neptunium sorption to SRS sediments, and 2) determine a sorption constant from an SRS 11-year lysimeter study. The modeling studies were conducted with existing data sets. The first data set used laboratory generated Np sorption data as a function of concentration (three orders of magnitude) and as a function of pH (four orders of magnitude of proton concentration). In this modeling exercise, a very simple solution was identified by assuming that all sorption occurred only to the iron oxides in the sediment and that all the added NpO$_{4}$$^{-}$ remained in the oxidized state and was not reduced to the Np(IV) state (as occurs rapidly with Pu(V)). With rather limited input data, very good agreement between experimental and modeling results was observed. This modeling approach would be easy to add to the PA with little additional data requirements. This model would be useful in a system where pH is expected to change greatly, such as directly beneath a grout or concrete structure. The second model discussed in the report was to derive strontium K$_{d}$ values from data collected in an 11-year-old field transport study. In this controlled lysimeter study, a sensitivity analysis was conducted of hydrological and chemical processes that influence contaminant transport, including diffusion coefficients, seepage velocity, and K$_{d}$ value. The best overall K$_{d}$ derived from the model fit to the data was 32 L kg$^{-1}$, which was the same value that was previously measured in traditional laboratory batch sorption studies. This was an unexpected result given the differences in experimental conditions between the batch test and the lysimeter flow through test, in particular the differences between strontium adsorption and desorption processes occurring in the latter test and not in the former. There were some trends in the lysimeter strontium data that were not predicted by the K$_{d}$ model, which suggest that other geochemical processes are likely also controlling strontium transport. Strontium release and cation exchange are being evaluated. These results suggest that future modeling efforts (e.g., PAs) could be improved by employing a more robust semi-empirical modeling approach to transient or complex conditions.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2016

Mineral solubility and free energy controls on microbial reaction kinetics: Application to contaminant transport in the subsurface

Recent developments in the theoretical treatment of geomicrobial reaction processes have resulted in the formulation of kinetic models that directly link the rates of microbial respiration and growth to the corresponding thermodynamic driving forces. The overall objective of this project was to verify and calibrate these kinetic models for the microbial reduction of uranium(VI) in geochemical conditions that mimic as much as possible field conditions. The approach combined modeling of bacterial processes using new bioenergetic rate laws, laboratory experiments to determine the bioavailability of uranium during uranium bioreduction, evaluation of microbial growth yield under energy-limited conditions using bioreactor experiments, competition experiments between metabolic processes in environmentally relevant conditions, and model applications at the field scale. The new kinetic descriptions of microbial U(VI) and Fe(III) reduction should replace those currently used in reactive transport models that couple catabolic energy generation and growth of microbial populations to the rates of biogeochemical redox processes. The above work was carried out in collaboration between the groups of Taillefert (batch reactor experiments and reaction modeling) at Georgia Tech and Van Cappellen (retentostat experiments and reactive transport modeling) at University of Waterloo (Canada).

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2014

MURMoT. Design and Application of Microbial Uranium Reduction Monitoring Tools

Uranium (U) contamination in the subsurface is a major remediation challenge at many DOE sites. Traditional site remedies present enormous costs to DOE; hence, enhanced bioremediation technologies (i.e., biostimulation and bioaugmentation) combined with monitoring efforts are being considered as cost-effective corrective actions to address subsurface contamination. This research effort improved understanding of the microbial U reduction process and developed new tools for monitoring microbial activities. Application of these tools will promote science-based site management decisions that achieve contaminant detoxification, plume control, and long-term stewardship in the most efficient manner. The overarching hypothesis was that the design, validation and application of a suite of new molecular and biogeochemical tools advance process understanding, and improve environmental monitoring regimes to assess and predict in situ U immobilization. Accomplishments: This project (i) advanced nucleic acid-based approaches to elucidate the presence, abundance, dynamics, spatial distribution, and activity of metal- and radionuclide-detoxifying bacteria; (ii) developed proteomics workflows for detection of metal reduction biomarker proteins in laboratory cultures and contaminated site groundwater; (iii) developed and demonstrated the utility of U isotopic fractionation using high precision mass spectrometry to quantify U(VI) reduction for a range of reduction mechanisms and environmental conditions; and (iv) validated the new tools using field samples from U-contaminated IFRC sites, and demonstrated their prognostic and diagnostic capabilities in guiding decision making for environmental remediation and long-term site stewardship.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Fitness factors impacting survival of a subsurface bacterium in contaminated groundwater

Many factors contribute to the ability of a microbial species to persist when encountering complexly contaminated environments, including time of exposure, the nature and concentration of contaminants, availability of nutritional resources, and possession of a combination of appropriate molecular mechanisms needed for survival. Herein we sought to identify genes that are most important for survival of Gram-negative Enterobacteriaceae in contaminated groundwater environments containing high concentrations of nitrate and metals using the metal-tolerant Oak Ridge Reservation isolate, Pantoea sp. MT58 (MT58). Survival fitness experiments in which a randomly barcoded transposon insertion (RB-TnSeq) library of MT58 was exposed directly to contaminated Oak Ridge Reservation groundwater samples from across a nitrate and mixed metal contamination plume were used to identify genes important for survival with increasing exposure times and concentrations of contaminants, and availability of a carbon source. Genes involved in controlling and using carbon, encoding transcriptional regulators, and related to Gram-negative outer membrane processes were among those found to be important for survival in contaminated Oak Ridge Reservation groundwater. A comparative genomics analysis of 75 Pantoea genus strains allowed us to further separate the survival determinants into core and non-core genes in the Pantoea pangenome, revealing insights into the survival of subsurface microorganisms during contaminant plume intrusion.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2018

Annual Closure Monitoring Report for Corrective Action Unit 98, Frenchman Flat, Underground Test Area, Nevada National Security Site, Nevada: (CY2017 January 2017–December 2017, Rev. 0)

Corrective Action Unit (CAU) 98: Frenchman Flat on the Nevada National Security Site was the location of 10 underground nuclear tests. CAU 98 underwent a series of investigations and actions in accordance with the Federal Facility Agreement and Consent Order to assess contamination of groundwater by radionuclides from the tests. A Closure Report completed that process in 2016 and called for long-term monitoring, use restrictions (URs), and institutional controls to protect the public and environment from potential exposure to contaminated groundwater. Three types of monitoring are performed for CAU 98: water quality, water level, and institutional control. These are monitored to determine whether the URs remain protective of human health and the environment, and to ensure that the regulatory boundary objectives are being met. Monitoring data will be used in the future, once multiple years of data are available, to evaluate consistency with the groundwater flow and contaminant transport models because the contaminant boundaries calculated with the models are the primary basis of the UR boundaries. Six wells were sampled for water-quality monitoring in 2017. Contaminants of concern were detected only in the two source/plume wells already known to contain contamination as a result of a radionuclide migration experiment. The 86,000-picocuries-per-liter (pCi/L) tritium concentration in one of the wells is about 12 percent higher than measured in 2016 but is over an order of magnitude less than the peak value measured in the well in 1980. The concentration in the other source/plume well is lower than measured in 2016. The water-level monitoring network includes 16 wells. Depth to water measured in 2017 is generally consistent with recent measurements for most wells. Water-level declines differing from long-term trends were observed in four wells. Three of these (WW-4, WW-4A, and WW-5B) are water-supply wells that experienced increases in pumping during the year. No definitive cause for the sharp decline in the fourth well (ER-5-3-2) in 2016 is known as yet. Institutional control monitoring confirmed the URs are recorded in U.S. Department of Energy and U.S. Air Force land management systems, and that no activities within Frenchman Flat basin are occurring that could potentially affect the contaminant boundaries. Survey of groundwater resources in basins surrounding Frenchman Flat similarly identify no current or pending development that would indicate the need to increase monitoring activities or would otherwise cause concern for the closure decision. The URs continue to prevent exposure of the public, workers, and the environment to contaminants of concern by preventing use of potentially contaminated groundwater.

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