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At least 1,081 records · Page 60

Detection and Mitigation of Radionuclides in the Environment: Toward a Clean Ecosystem

This research describes a straightforward approach to producing surface-engineered nanomaterials for the detection and mitigation of radionuclides generated in nuclear facilities. Here, a micelle forming surfactant ligand, namely cetyltrimethylammonium bromide (CTAB), was engineered on the surface of iron oxide nanoparticles and explored for the removal of radioactive materials, such as pertechnetate (TcO 4 – ), from aqueous environments. A series of analytical tools were employed to characterize the nanocomposite materials, such as SEM, EDS, UV-Vis spectroscopy, DLS, and PALS, and evaluated for their ability to capture a model analyte, perrhenate (ReO 4 – ) ions. The iron oxide magnetic nanoparticles retain their magnetic properties after surface functionalization and can be easily manipulated and collected with a magnet. Therefore, these nanocomposite materials can be used to remotely remediate environments by scavenging and collecting radionuclide species at the desired location.

63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗

Chapter Four—MSW characterization and preprocessing for biofuels and bioproducts

The organic fraction of MSW (OFMSW) has a high carbohydrate and lipid content, indicating its good potential as a feedstock for bioethanol and biodiesel production. However, variability in feedstock composition for MSW is a critical challenge for downstream conversion processes such as pyrolysis, gasification, incineration, and biotechnological conversion. MSW characterization is critical to inform and optimize the design of physical handling processes to minimize costs and environmental impacts, and improve the downstream conversion performance of MSW materials. Here, this book chapter focuses on current MSW characterization and preprocessing technologies and discusses the costs, benefits, and environmental impacts associated with MSW preprocessing. Also, the book chapter outlines the potential strategies to increase total revenue and mitigate negative environmental impacts for MSW recycling systems.

09 BIOMASS FUELS↗

Partitioning of tritium between surface and bulk of 316 stainless steel at room temperature

The distribution of tritium between the near surface and the bulk of 316 stainless steel has been measured using two independent techniques: pulsed-plasma exposures and a zinc-chloride wash. Between 17% and 20% of the total inventory absorbed into a stainless-steel sample during a 24-h exposure to DT gas at room temperature resides in the water layers present on the metal surface. Redistribution of tritium between the surface and the bulk of stainless steel, if it occurs, is very slow. Finally, tritium does not appear to enter into the bulk at a rate defined solely by lattice diffusivity.

316 stainless steel↗

Experimental validation of simplified radionuclide transport bubble scrubbing code in sodium coolant pool

Solid radionuclides released following fuel pin failure may become entrained in gaseous fission products and be rapidly transported through the coolant pool to the cover gas region. Sensitivity studies on radionuclide transport have identified this potential pathway as one of both high concern and high uncertainty. The simplified radionuclide transport scrubbing code utilizes classical aerosol scrubbing mechanisms to model this phenomenon and predict aerosol masses reaching the cover gas region. This paper serves to validate this code in a sodium environment while conducting a parametric study to analyze the effects of aerosol size, bubble size, pool temperature, pool depth, aerosol density, and aerosol concentration. Through a series of experimental tests, it was determined that aerosol sizes ranging from 0.001 to 1.0 µm are of primary concern as aerosols in this range have a ratio of aerosol mass entering the sodium pool from the fuel pin to aerosol mass exiting the sodium pool to the cover gas region of less than 10. Further, the experimental results were found to match the trends found in the scrubbing model closely, but significantly more scrubbing was seen experimentally. Decreasing bubble size and increasing pool depth and aerosol density were all found to increase scrubbing both experimentally and theoretically. Pool temperature was found to have a negligible effect on scrubbing amounts; however, this was largely due to a subsequent increase in bubble size corresponding to increasing temperatures which offset the increase in scrubbing due to increased temperature. Varying aerosol concentration was found to have no effect on scrubbing ratios. A final series of tests was conducted for a more prototypic fuel pin failure with a heterogenous bubble swarm. From these tests, it was found that the experimental scrubbing quantities were larger than for the single bubble case. Overall, it was found that the simplified bubble transport scrubbing code accurately models the trends of the bubble scrubbing but provides a conservative estimate of scrubbing quantities. Model limitations fail to model the complex phenomena present for fission product scrubbing via bubble transport, but match trends seen experimentally.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Adsorption and Destruction of the G-Series Nerve Agent Simulant Dimethyl Methylphosphonate on Zinc Oxide

Organophosphorus chemical warfare agents (CWAs) are extremely toxic compounds that are nominally mitigated with gas mask filtration employing metal oxide impregnated activated carbon filtration material. To develop more effective sorbents, it is important to understand the surface chemistry between these organophosphorus compounds and the individual components that make up these filtration materials. In this study, density functional theory (DFT) and Fourier transform infrared spectroscopy (FTIR) were employed to investigate the adsorption and decomposition mechanisms between a sarin simulant molecule, dimethyl methylphosphonate (DMMP), and zinc oxide, which is a component found in current filtration materials. Theoretical calculations show that DMMP readily adsorbs to a pristine and hydroxylated ZnO ($101\bar 0$) surface with average adsorption energies of 132 and 65 kJ mol –1 , respectively. Experimental diffuse reflectance fourier transform infrared spectroscopy (DRIFTS) reveals that ZnO adsorbs water and readily hydroxylates under ambient conditions, which can facilitate adsorption through hydrogen bonding of the P$=$O to ZnO surface hydroxyls. FTIR gas phase analysis also reveals that DMMP decomposes in the presence of ZnO nanoparticles (NPs) to produce methanol at room temperature. Assuming a fully hydroxylated surface of ZnO, DFT calculations reveal several plausible mechanisms for DMMP decomposition to form methanol with an activation energy barrier of 99.6 kJ mol –1 . Finally, on the basis of this energy barrier to decompose DMMP, a turnover frequency (TOF) of only 3.5 × 10 –7 s –1 is calculated assuming full coverage of DMMP on the ZnO nanoparticles tested. This value is qualitatively consistent with experimental results.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Removal of long-lived {sup 222}Rn daughters by electropolishing thin layers of stainless steel

Long-lived alpha and beta emitters in the {sup 222}Rn decay chain on detector surfaces may be the limiting background in many experiments attempting to detect dark matter or neutrinoless double beta decay. Removal of tens of microns of material via electropolishing has been shown to be effective at removing radon daughters implanted into material surfaces. Some applications, however, require the removal of uniform and significantly smaller thicknesses. Here, we demonstrate that electropolishing < 1 μm from stainless-steel plates reduces the contamination efficiently, by a factor > 100. Examination of electropolished wires with a scanning electron microscope confirms that the thickness removed is reproducible and reasonably uniform. Together, these tests demonstrate the effectiveness of removal of radon daughters for a proposed low-radiation, multi-wire proportional chamber (the BetaCage), without compromising the screener’s energy resolution. More generally, electropolishing thin layers of stainless steel may effectively remove radon daughters without compromising precision-machined parts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Computational design of soft materials for the capture of Cs-137 in contaminated environments: From 2D covalent cucurbituril networks to 3D supramolecular materials

Using computational quantum chemistry methods we design novel 2D and 3D soft materials made of cucurbituril macrocycles covalently connected with each other via rigid linkers. Such covalent cucurbituril networks might be useful for the capture of radioactive Cs-137 (present as Cs{sup +}) in the contaminated environment.

54 ENVIRONMENTAL SCIENCES↗

Tc removal from the waste treatment and immobilization plant low-activity waste vitrification off-gas recycle

Vitrification of Low Activity Waste in the Hanford Waste Treatment and Immobilization Plant generates a condensate stream from the off-gas processes. Components in this stream are partially volatile and accumulate to high concentrations through recycling, which impacts the waste glass loading and facility throughput. The primary radionuclide that vaporizes and accumulates in the stream is 99 Tc. This program is investigating Tc removal via reductive precipitation with stannous chloride to examine the potential for diverting this stream to an alternate disposition path. As a result, research has shown stannous chloride to be effective, and this paper describes results of recent experiments performed to further mature the technology.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Glacier ice archives nearly 15,000-year-old microbes and phages

Background Glacier ice archives information, including microbiology, that helps reveal paleoclimate histories and predict future climate change. Though glacier-ice microbes are studied using culture or amplicon approaches, more challenging metagenomic approaches, which provide access to functional, genome-resolved information and viruses, are under-utilized, partly due to low biomass and potential contamination. Results We expand existing clean sampling procedures using controlled artificial ice-core experiments and adapted previously established low-biomass metagenomic approaches to study glacier-ice viruses. Controlled sampling experiments drastically reduced mock contaminants including bacteria, viruses, and free DNA to background levels. Amplicon sequencing from eight depths of two Tibetan Plateau ice cores revealed common glacier-ice lineages including Janthinobacterium, Polaromonas, Herminiimonas, Flavobacterium, Sphingomonas, and Methylobacterium as the dominant genera, while microbial communities were significantly different between two ice cores, associating with different climate conditions during deposition. Separately, ~355- and ~14,400-year-old ice were subject to viral enrichment and low-input quantitative sequencing, yielding genomic sequences for 33 vOTUs. These were virtually all unique to this study, representing 28 novel genera and not a single species shared with 225 environmentally diverse viromes. Further, 42.4% of the vOTUs were identifiable temperate, which is significantly higher than that in gut, soil, and marine viromes, and indicates that temperate phages are possibly favored in glacier-ice environments before being frozen. In silico host predictions linked 18 vOTUs to co-occurring abundant bacteria (Methylobacterium, Sphingomonas, and Janthinobacterium), indicating that these phages infected ice-abundant bacterial groups before being archived. Functional genome annotation revealed four virus-encoded auxiliary metabolic genes, particularly two motility genes suggest viruses potentially facilitate nutrient acquisition for their hosts. Finally, given their possible importance to methane cycling in ice, we focused on Methylobacterium viruses by contextualizing our ice-observed viruses against 123 viromes and prophages extracted from 131 Methylobacterium genomes, revealing that the archived viruses might originate from soil or plants. Conclusions Together, these efforts further microbial and viral sampling procedures for glacier ice and provide a first window into viral communities and functions in ancient glacier environments. Such methods and datasets can potentially enable researchers to contextualize new discoveries and begin to incorporate glacier-ice microbes and their viruses relative to past and present climate change in geographically diverse regions globally.

59 BASIC BIOLOGICAL SCIENCES↗

Preliminary Study of Iodine Gas Removal in Sodium Pools

Potential iodine gas release from failed fuel pins is a critical factor in the source term analysis of oxide fuel-loaded sodium fast reactors (SFRs). The accumulated iodine-containing gas mixtures inside pin plenums are expected to be ejected during pin failures and rise through sodium pool, with potential release of gaseous iodine to the cover gas region. Due to its potential radiological impacts, a proper assessment of iodine behavior is necessary for an accurate source term assessment. Throughout the bubble rise trajectory in the sodium pool, iodine gas is continuously removed or transformed at the bubble interface by diffusion, as the combining reaction between the iodine and sodium to form sodium iodide (NaI) is a chemically preferred process. As the final amount of iodine released from the facility is strongly influenced by the removal phenomenon inside the sodium pool, experiments were previously performed by PNC (Power Reactor and Nuclear Fuel Development Corporation) to provide insight into this phenomenon. To assess the accuracy of present methods for predicting iodine gas removal within sodium pools, several candidate approaches, available in source term analysis codes, have been summarized and evaluated in this study. Spherical cap bubbles and spherical bubbles are considered in accordance with the methods adopted in each approach, and different forms of correlations for major parameters have been implemented in accordance with the original adoptions. Based on the summarized results, important aspects to be considered have been derived.

Decontamination↗

Pilot Scale Advanced Fogging Demonstration

Radiological contamination control is crucial during decommissioning and demolition (D&D) activities, as well as during modifications to existing radiological systems. It is well known that contamination, in some cases substantial contamination, is present throughout the exhaust ductwork in several older processing facilities within the Department of Energy (DOE) complex, due to years of processing radioactive materials in areas served by closed ventilation systems. Accumulations of radioactive dust and lint – commonly found in laundry facilities, exhaust ventilation ducting, and exhaust stacks – present a specific contamination control issue. Particle suspension is more likely to occur during cleaning, modification, or demolition of these systems and during disposal site exhumation. In a recent demolition of large ventilation ducting (~10’ × 10’ cross section, ~100’ long) at Brookhaven National Laboratory, a spray coating was manually applied to the inside of the duct – requiring painters, dressed in anti-contamination clothing and an airline respirator system, to enter the duct.1 The advanced fogging technique offers an alternative method to mitigate these airborne contamination hazards with minimal personnel entry. Experiments in 2006 developed a useful fog solution using three different chemical constituents. Optimization of the fog recipe and use of commercially available equipment were identified as needs that had not been addressed. During 2012 development work it was noted that low concentrations of the components hampered coverage and drying in the United Kingdom’s National Nuclear Laboratory’s testing much more so than was evident in the 2006 tests. In fiscal year 2014 the Idaho National Laboratory undertook a systematic optimization of the fogging formulation and conducted a non-radioactive, pilot scale demonstration using commercially available fogging equipment. While not as sophisticated as the equipment used in earlier testing, the new approach is much less expensive and readily available for smaller scale operations. Pilot scale testing was important to validate new equipment of an appropriate scale, optimize the chemistry of the fogging solution, and to realize the conceptual approach.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Irreversible Wash Aid Additive for Cesium Mitigation. Small-Scale Demonstration and Lessons Learned

The Irreversible Wash Aid Additive process has been under development by the U.S. Environmental Protection Agency (EPA) and Argonne National Laboratory (Argonne). This process for radioactive cesium mitigation consists of a solution to wash down contaminated structures, roadways, and vehicles and a sequestering agent to bind the radionuclides from the wash water and render them environmentally immobile. The purpose of this process is to restore functionality to basic services and immediately reduce the consequences of a radiologically-contaminated urban environment. Research and development have resulted in a down-selection of technologies for integration and demonstration at the pilot-scale level as part of the Wide Area Recovery and Resiliency Program (WARRP) under the Department of Homeland Security and the Denver Urban Area Security Initiative. As part of developing the methods for performing a pilot-scale demonstration at the WARRP conference in Denver in 2012, Argonne conducted small-scale field experiments at Separmatic Systems. The main purpose of these experiments was to refine the wash water collection and separations systems and demonstrate key unit operations to help in planning for the large scale demonstration in Denver. Since the purpose of these tests was to demonstrate the operations of the system, we used no radioactive materials. After a brief set of experiments with the LAKOS unit to familiarize ourselves with its operation, two experiments were completed on two separate dates with the Separmatic systems.

61 RADIATION PROTECTION AND DOSIMETRY↗

Irreversible Wash Aid Additive for Cesium Mitigation: WARRP Demonstration

This activity demonstrated, on a practical scale, the primary unit operations for building a containment structure for radioactive wash waters, washing down a hypothetically radioactively contaminated vehicle, collecting the hypothetically radioactive slurry waste water, filtering the hypothetically radioactive wash waters, disassembling the containment, and transporting the materials for final disposition.

61 RADIATION PROTECTION AND DOSIMETRY↗

Irreversible Wash Aid Additive for Cesium Mitigation: Phase II. Selection and/or Modification of COTS Field Portable Waste Water Systems

After an accidental or malicious release of radioactivity, large urban areas may be contaminated, compromising response efforts by first responders and law enforcement officials. In addition, some public services (e.g., drinking water and wastewater treatment, electrical power distribution, etc.) may be disrupted. In such an event, it may be important to deploy mitigation efforts in certain areas to restore response activities and public services (Fig. S-1). This report explores the state-of-the-art approach for a system to rapidly return critical infrastructure components to service following a cesium-137 (Cs-137) radiological dispersal device (RDD) release while avoiding the spread of Cs-137 beyond its original deposition area and minimizing the amount of Cs-137-contaminated wastewater. Specifically, we describe a wash system consisting of chemical additives added to fire hydrant water and irreversible solid sequestering agents added as the water is collected and treated for recycle in situ. The wash system is intended to be a rapidly deployable, cost-effective means of mitigating an urban setting for the purpose of restoring critical infrastructure and operational activities after a radiological release.

61 RADIATION PROTECTION AND DOSIMETRY↗

2015 Site Environmental Report Fernald Preserve

The Fernald Preserve 2015 Site Environmental Report provides stakeholders with the results from the Fernald, Ohio, Site’s environmental monitoring programs for 2015; a summary of the U.S. Department of Energy’s (DOE’s) activities conducted onsite; and a summary of the Fernald Preserve’s compliance with the various environmental regulations, compliance agreements, and DOE policies that govern site activities. This report has been prepared in accordance with the “Integrated Environmental Monitoring Plan,” which is Attachment D of the Comprehensive Legacy Management and Institutional Controls Plan (LMICP) (DOE 2016). Remediation of the Fernald Preserve has been successfully completed with the exception of the groundwater. During 2015, activities at the Fernald Preserve included: environmental monitoring activities related to direct radiation, groundwater, and surface water; ecological restoration monitoring and maintenance as well as inspections, care, and monitoring of the site and the OSDF to ensure that provisions of the LMICP are fully implemented; OSDF leak detection monitoring and collection, monitoring, and treatment of leachate from the OSDF; extraction, monitoring, and treatment of contaminated groundwater from the Great Miami Aquifer (Operable Unit 5); ongoing operation of the Fernald Preserve Visitors Center, associated outreach, and educational activities; and monitoring as specified in the site’s National Pollutant Discharge Elimination System (NPDES) permit. Environmental monitoring programs were developed to ensure that the remedy remains protective of the environment. The requirements of these programs are described in detail in the LMICP and reported in this Site Environmental Report.

54 ENVIRONMENTAL SCIENCES↗

Characterization of Solids Deposited on the Modular Caustic-Side Solvent Extraction Unit (MCU) Strip Effluent (SE) Coalescer Media Removed in April 2015

On June 2015, Savannah River National Laboratory (SRNL) received a Strip Effluent (SE) coalescer (FLT-304) from MCU. That coalescer was first installed at MCU in late October 2014 and removed in April 2015. While processing approximately 48,700 gallons of strip solution, the pressure drop steadily increased linearly from 1 psi to near 16 psi (the administrative limit is 17 psi) with the total filtrate volume (2.1E-4 psi/gal of filtrate). The linear behavior is due to the combined effect of a constant deposition of material that starts from the closed-end to the mid-section of the coalescer reducing the available surface area of the coalescer for fluid passage (linearly with filtrate volume) and the formation of a secondary emulsion (water in NG-CSSX) on the fibers of the coalescer media. Both effects reduced the coalescer porosity by at least 13% (after processing 48,700 gallons). Before the coalescer was removed, it was flushed with a 10 mM boric acid solution to reduce the dose level. To determine the nature of the deposited material, a physical and chemical analysis of the coalescer was conducted. Characterization of this coalescer revealed the adsorption of organic containing amines (secondary amides and primary amines), TiDG, degraded modifier (with no hydroxyl group), MaxCalix, and oxidized hydrocarbon (possibly from Isopar™L or from lubricant used at MCU) onto the coalescer media. The amide and amines are possibly from the decomposition of the suppressor (TiDG). The modifier and MaxCalix were the largest components of the deposited organic material, as determined from leaching the coalescer with dichloromethane. Both the Fourier-Transformed Infrared (FTIR) and Fourier-Transformed Hydrogen Nuclear Magnetic Resonance (FT-HNMR) results indicated that some of the modifier was degraded (missing their OH groups). The modifier was observed everywhere in the examined coalescer pieces (FTIR), while the TiDG and its decomposition products were observed at the entrance discs of the coalescer. A solvent trim (a cocktail of solvent components with a high concentration of modifier) was added to the solvent on 2/22/2015. It is believed that the trim did not mix completely with the solvent and that it was subsequently spread around the MCU components including the coalescers, where it may have deposited. Chronologically, the modifier, the TiDG’s decomposition products and silicates deposited on the entrance discs first and after the pressure drop increased significantly, parts of the coalescer media detached itself from the central porous steel mandrel and a significant amount of steel debris, mercury, titanium, and additional aluminum and silicates deposited on the coalescer.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Preparation and evaporation of Hanford Waste treatment plant direct feed low activity waste effluent management facility simulant

The Hanford Waste Treatment and Immobilization Plant (WTP) Low Activity Waste (LAW) vitrification facility will generate an aqueous condensate recycle stream (LAW Melter Off-Gas Condensate, LMOGC) from the off-gas system. The baseline plan for disposition of this stream during full WTP operations is to send it to the WTP Pretreatment Facility, where it will be blended with LAW, concentrated by evaporation, and recycled to the LAW vitrification facility. However, during the Direct Feed LAW (DFLAW) scenario, planned disposition of this stream involves concentrating the condensate in a new evaporator at the Effluent Management Facility (EMF) and returning it to the LAW melter. The LMOGC stream will contain components, e.g. halides and sulfates, that are volatile at melter temperatures, have limited solubility in glass waste forms, and present a material corrosion concern. Because this stream will recycle within WTP, these components are expected to accumulate in the LMOGC stream, exacerbating their impact on the number of LAW glass containers that must be produced. Diverting the stream reduces the halides and sulfates in the glass and is a key objective of this program. In order to determine the disposition path, it is key to experimentally determine the fate of contaminants. To do this, testing is needed to account for the buffering chemistry of the components, determine the achievable evaporation end point, identify insoluble solids that form, determine the formation and distribution of key regulatoryimpacting constituents, and generate an aqueous stream that can be used in testing of the subsequent immobilization step. This overall program examines the potential treatment and immobilization of the LMOGC stream to enable alternative disposal. The objective of this task was to (1) prepare a simulant of the LAW Melter Off-gas Condensate expected during DFLAW operations, (2) demonstrate evaporation in order to predict the final composition of the effluents from the EMF evaporator to aid in planning for their disposition, and (3) generate concentrated evaporator bottoms for use in immobilization testing.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗