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Sensitive Resources Assessment and Forest Analysis for the Proposed Versatile Test Reactor, Oak Ridge, Tennessee

The US Department of Energy’s (DOE’s) Oak Ridge National Laboratory (ORNL) is a leading institution in advanced materials, supercomputing, neutrons, and nuclear science. As a research laboratory managed by UT-Battelle, LLC for DOE, ORNL has national priorities in energy, security, and scientific discovery that necessitate facility improvements and expansions. DOE is also committed to environmental stewardship. The laboratory is located on the ~32,000-acre (~13,000-ha) Oak Ridge Reservation (ORR), much of which is categorized as a National Environmental Research Park (NERP) and a state Wildlife Management Area. DOE works with the Tennessee Wildlife Resources Agency (TWRA), Tennessee Department of Environment and Conservation (TDEC), US Fish and Wildlife Service (USFWS), US Department of Agriculture, and other agencies to serve as an effective steward of the ORR. Accordingly, project managers must conform to environmental regulations, agreements, and policies at the federal, state, and institutional levels. Per 40 CFR (Code of Federal Regulations) 1508.14, potential effects on research and science education also represent potential effects of federal actions on the NERP, and impacts on, e.g., deer harvest, must be considered on the Oak Ridge Wildlife Management Area when other aspects of the human environment are affected. The United States currently has no fast neutron testing capability to support advanced nuclear research and development. The proposed Versatile Test Reactor (VTR) will take advantage of current investments by the US government and private industry in nuclear reactors to expedite the design and construction process, using proven technology to create a world-class scientific infrastructure. The VTR will take advantage of fast neutrons provided by this proven technology, along with a capability to rapidly insert, conduct, and remove state-of-the-art experiments. An advantage of the VTR is that it can support future innovations in experimental capabilities without modifying the facility. The VTR will support progress in a variety of science and technology areas, including testing and qualification of advanced reactor fuels; testing and qualification of innovative structural materials; testing of innovative components and instruments; validation of advanced modeling and simulation tools; and versatility for future technical missions. Through proven technology, the VTR can take advantage of existing reactor designs and operating experience to reduce the risk, cost, and time for design and construction. The top available resources of DOE laboratories, industry, and universities will be used to expedite reactor design and construction toward developing the scientific infrastructure that affords a strong testing capability that can be sustained over many years. This report summarizes current knowledge of natural and cultural resources primarily within the VTR construction area. At the time of this report, the proposed VTR site design includes a construction area of ~150.4 acres (~69.9 ha), which contains an ~51.3-acre (~20.8-ha) operations area, located within forested natural areas of the ORR. The primary goal of the work presented here was to evaluate potential effects on sensitive resources that might result from development and construction activities associated with VTR. In addition to on-the-ground surveys during spring and summer 2020 by the ORNL Natural Resources Management Program and Aquatic Ecology Group staff, this report makes use of historical (pre-1995) and contemporary (1995 to present) data from additional confirmed sources (e.g., TDEC). Likewise, forest conditions were compiled from a 2011 forest inventory and supplemented with limited ground observations in 2020. The individuals who obtained and compiled the data presented here are familiar with and routinely assess sensitive resources on the ORR. Anyone who references this report must consider that the timing of surveys did not permit a complete delineation of the resources that will be affected. If the VTR project proceeds, additional surveys will be required to account for the seasonal patterns of various threatened and endangered species. Data deficiencies and potential resources that likely went undetected are indicated where possible. Accordingly, this report should facilitate more environmentally sound decisions during planning and 2 development of the VTR site, provide a foundation for further assessment of sensitive and cultural resources, and help project managers better address regulatory guidance and DOE policies on sustainable development in compliance with, for example, the US Endangered Species Act (ESA), Migratory Bird Treaty Act (MBTA), Tennessee Rare Plant Protection and Conservation Act of 1985, Tennessee Nongame and Endangered or Threatened Wildlife Species Conservation Act of 1974, several federal and state regulations regarding aquatic resource protection, and site-specific policies as outlined in various ORR management plans developed by ORNL and TWRA for DOE.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Evaluation of Hanford Tank Supernatant Availability for Technetium Management Project Studies in FY16

This report examines the need for actual Hanford tank waste solutions to support tasks in the Technetium Management Program in fiscal year (FY) 2016. One key need is to identify both samples where a majority of the soluble technetium is present as pertechnetate and samples where it is not. The total amount of tank supernatant needed from any given tank waste supernatant was determined by polling the tasks leaders for their technology testing needs in FY16 and then arbitrarily ascribing a 10% process loss associated with consolidation and the Cs-137 removal needed to reduce the dose to a level suitable for testing in radiological fumehoods. These polling results identified a need for approximately 2.1 to 3.6 kg of any particular targeted Hanford tank waste supernatant.

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Creative absorber design and optimization for CO 2 capture with aqueous piperazine

The Texas Carbon Management Program is preparing a Front-End Engineering Design (FEED) of the PZASTM (Piperazine with the Advanced Stripper TM ) for CO 2 capture at a natural gas combined cycle power plant in West Texas. This paper develops the absorber design for the capture system and studies the operational strategies of the absorber in response to ambient temperature swing. The design uses 2 absorber trains, and each train integrates absorption and a water-wash section in one column. Each column has a cross-section area of 174 m 2 and consists of 3 sections of MellapakPlus® 252Y structured packing. Packing heights for each section are 3, 4.9, and 2.7 m from top to bottom. A pump-around intercooler applied at the bottom bed circulates solvent and eliminates the direct contact cooler. The baseline CO 2 removal rate is 90% and will vary between 78% and 90% with ambient temperature. The system uses air cooling to eliminate cooling water usage. The water balance in the system will be managed by operating the water wash at a high circulation rate (1300 kg/h) to condense water during the night and make up for water loss during the day. Finally, the proposed design reduces the capital cost of the absorber column by minimizing the packing height and eliminating the direct contact cooler (DCC), and improves the energy cost by lowering the pump-around intercooling temperature and increasing the pump-around rate.

03 NATURAL GAS↗

Nuclear Energy Infrastructure Database Fitness and Suitability Review

In 2014, the Deputy Assistant Secretary for Science and Technology Innovation (NE-4) initiated the Nuclear Energy-Infrastructure Management Project by tasking the Nuclear Science User Facilities (NSUF) to create a searchable and interactive database of all pertinent NE supported or related infrastructure. This database will be used for analyses to establish needs, redundancies, efficiencies, distributions, etc. in order to best understand the utility of NE’s infrastructure and inform the content of the infrastructure calls. The NSUF developed the database by utilizing data and policy direction from a wide variety of reports from the Department of Energy, the National Research Council, the International Atomic Energy Agency and various other federal and civilian resources. The NEID contains data on 802 R&D instruments housed in 377 facilities at 84 institutions in the US and abroad. A Database Review Panel (DRP) was formed to review and provide advice on the development, implementation and utilization of the NEID. The panel is comprised of five members with expertise in nuclear energy-associated research. It was intended that they represent the major constituencies associated with nuclear energy research: academia, industry, research reactor, national laboratory, and Department of Energy program management. The Nuclear Energy Infrastructure Database Review Panel concludes that the NSUF has succeeded in creating a capability and infrastructure database that identifies and documents the major nuclear energy research and development capabilities across the DOE complex. The effort to maintain and expand the database will be ongoing. Detailed information on many facilities must be gathered from associated institutions added to complete the database. The data must be validated and kept current to capture facility and instrumentation status as well as to cover new acquisitions and retirements.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Adaptation of the NWM Cloud Environment for an ISF Project

The DOE-NE NWM Cloud was designed to be a generic set of tools and applications for any nuclear waste management program. As policymakers continue to consider approaches that emphasize consolidated interim storage and transportation of spent nuclear fuel, a gap analysis of the tools and applications provided for spent nuclear fuel and high-level radioactive waste disposal in comparison those needed for siting, licensing, and developing a consolidated interim storage facility and/or for a transportation campaign will help prepare DOE for implementing such potential policy direction. This report evaluates the points of alignment and potential gaps between the applications on the NWM Cloud that supported SNF disposal project, and the applications needed to address QA requirements and for other project support needs of an SNF storage project.

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Status of HLW disposal in the USA and rational, progressive, paths forward based upon lessons learned in the USA and abroad since 1973 - 15103

The development of the USA's only candidate (since 1987) HLW-repository at the Yucca Mountain (YM) site, Nevada, was halted by the Obama administration in 2009. Four years later, the Obama administration proposed a new strategy for the back end of the nuclear fuel cycle that would open a consent-based HLW repository 'by 2048'. At the end of 2014, both the YM HLW repository and the new HLW-disposition (storage and disposal) strategy remain on hold due to lack of enabling legislation. With this as background, and based upon our active involvement in, monitoring of, and reporting on HLW management programs in the USA and abroad since 1973, we submit that: 1. Politics, political will, and legal actions and outcomes will continue to govern progress. 2. Public acceptance and sustained support (PASS) may influence politics and political will. 3. PASS is time-dependent and governed by: a. Ideologies; b. Perceived benefits and risks; c. Level and equity of radiation protection provided by applicable regulations; d. Perceived robustness/safety of the proposed disposition concept; and e. Perceived credibility and competency vested in the involved organizations and their respective leaders (= TRUST). We therefore recommend that the USA concurrently pursues at least two, 'centralized' HLW-storage and -disposal solutions based upon best-available relevant knowledge and majority-PASS at facility-host locations. Furthermore, safe(r) and more secure disposal of defense/government-generated HLW could probably commence at least 15 years earlier than 'by 2048' in/at: 1. The YM repository/site. 2. The WIPP repository/site. 3. 'Local' deep boreholes. (authors)

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Minimizing treatment planning errors in proton therapy using failure mode and effects analysis

Purpose: Failure mode and effects analysis (FMEA) is a widely used tool to evaluate safety or reliability in conventional photon radiation therapy. However, reports about FMEA application in proton therapy are scarce. The purpose of this study is to apply FMEA in safety improvement of proton treatment planning at their center. Methods: The authors performed an FMEA analysis of their proton therapy treatment planning process using uniform scanning proton beams. The authors identified possible failure modes in various planning processes, including image fusion, contouring, beam arrangement, dose calculation, plan export, documents, billing, and so on. For each error, the authors estimated the frequency of occurrence, the likelihood of being undetected, and the severity of the error if it went undetected and calculated the risk priority number (RPN). The FMEA results were used to design their quality management program. In addition, the authors created a database to track the identified dosimetric errors. Periodically, the authors reevaluated the risk of errors by reviewing the internal error database and improved their quality assurance program as needed. Results: In total, the authors identified over 36 possible treatment planning related failure modes and estimated the associated occurrence, detectability, and severity to calculate the overall risk priority number. Based on the FMEA, the authors implemented various safety improvement procedures into their practice, such as education, peer review, and automatic check tools. The ongoing error tracking database provided realistic data on the frequency of occurrence with which to reevaluate the RPNs for various failure modes. Conclusions: The FMEA technique provides a systematic method for identifying and evaluating potential errors in proton treatment planning before they result in an error in patient dose delivery. The application of FMEA framework and the implementation of an ongoing error tracking system at their clinic have proven to be useful in error reduction in proton treatment planning, thus improving the effectiveness and safety of proton therapy.

60 APPLIED LIFE SCIENCES↗

Large Plate Experiment of Chloride-induced Stress Corrosion Cracking in Spent Nuclear Fuel Storage Canisters

This report provides a description of the testing (in progress at the Savannah River National Laboratory) to evaluate the corrosion behavior of a large section of welded plate material harvested from the Sandia National Laboratories’ full-size mockup of a spent nuclear fuel (SNF) dry storage canister. The details of the establishment of this plate test, the interim corrosion results (from visual examination), and the general plan for examination of the plate in CY21 to evaluate crack growth behavior (if any) are provided. This work is intended to inform aging management programs for SNF canisters under conditions of extended dry storage. A “large plate” (approximately 51 x 46 cm with thickness 16 mm and weight about 30 kg) and containing a circumferential weldment from the mockup is the test specimen. The knowledge of the salt, temperature, humidity conditions for chloride-induced stress corrosion cracking (CISCC) including the threshold stress intensity factor, K iscc , were used to setup the large plate test in which a set of part-through-wall and through-wall electrical discharge machined (EDM) defects were positioned in the weld residual stress field of the welded plate material from the mockup canister. A marine salt solution was applied to this plate specimen with an air-brush spray, then dried, and then exposed to a sustained 71-73% RH condition at an ambient room temperature of 22 °C. The salt loading and environmental condition is expected to be aggressive to cause CISCC

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Systems and Tools to Facilitate Aging Management Inspections of Used Nuclear Fuel Dry Storage Systems - 18382

The Used Nuclear Fuel (UNF) dry storage systems (DSSs) are currently used at almost all the nuclear plants in the USA for the storage of their UNF as the spent fuel pools are running out of capacity to store any additional discharged fuel. Even though these DSSs are supposed to be at the reactor site for a short amount of time, they are expected to be at the reactor sites for an extended duration due to the unavailability of Interim Storage Facilities (ISF) or a permanent disposal sites like Yucca Mountain. Maintaining the integrity of the DSS canisters and storage overpacks so they can safely protect the fuel and maintain the integrity of UNF is of utmost importance during storage at reactor site ISFSI or at the ISF. Comprehensive and robust Aging Management Program (AMP) is an important aspect for DSSs to satisfy these requirements. In order to address this industry need, TN Americas have developed an enhanced NUHOMS{sup R} DSS licensed by NRC under 10 CFR Part 72 regulations and a comprehensive AMP development which includes prevention, inspection, monitoring and mitigation of any corrosion or degradation of DSS components. For DSC and HSM inspection, two remotely operating delivery systems have been developed using non-destructive examination (NDE) methods including robotic crawler and inspection ring system. This paper describes details of these developments and status of their deployment for implementation at various utility ISFSI sites. TN Americas completed the detailed design of the DSC inspection system and conducted functional tests of the inspection system on a DSC mockup and the system is ready for deployment at any NUHOMS{sup R} ISFSI site. TN Americas is committed to offer the most robust and comprehensive AMP systems, tools and services to the industry to assure the safety of the deployed DSS at the utility sites. (authors)

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Investigation into Reductive Separation of Tc-99 from Low Activity Waste Off-Gas Condensate by Zero Valent Iron Materials - 20311

This study is investigating the potential for reductive separation of technetium-99 (Tc) from off-gas condensate generated from vitrification of legacy tank waste at the Hanford Tank Waste Treatment and Immobilization Plant. Management of Tc is a high-priority activity for the U.S. Department of Energy (DOE) Office of Environmental Management (EM) complex, which must be addressed based on knowledge gaps and technology development needs outlined in the DOE-EM Technetium Management Program Plan [1]. Technetium is one of the main risk drivers in the permanent disposal of low activity waste (LAW) by vitrification at the Hanford Site due to its high volatility and only fractional incorporation into borosilicate glass. Volatilized Tc will be captured by an off-gas treatment system, and the current plan is to continuously recycle generated condensate back to the LAW glass melter feed. Off-gas recycling is effective at increasing Tc loading in the LAW glass, but it also disproportionately increases concentrations of sulfate, halides, and other volatile compounds impeding overall LAW processing leading to significantly greater waste glass volume requirements. Removal of Tc from secondary liquid waste offers an alternative disposal route to continuous off-gas recycling which may result in significant reduction of the volumes of LAW waste glass and substantial cost savings. The objective of this research funded by the DOE-EM Minority Serving Institutions Partnership Program (MSIPP) is to determine the suitability of zero valent iron (ZVI) as a separation technology to remove Tc from the off-gas condensate stream to minimize its recycle. While ZVI has been proposed for various remediation applications with Tc, it has not been studied for its suitability for removing Tc from the LAW off-gas condensate. The goal is to identify the optimal conditions for which Tc{sup (VII)} will be reduced to Tc{sup (IV)} species and incorporated into an iron matrix. This paper presents a programmatic overview of our evaluation of commercial ZVI materials for their efficiency towards Tc{sup (VII)} reductive removal from simplified off-gas simulant solutions under aerobic conditions. Tc concentrations in solutions were monitored for up to 30 days to determine efficiency and kinetics of reductive removal of Tc. The best performing candidate materials were selected for further experiments evaluating the effects of (1) variable ionic strength, (2) the presence of chromium and corrosive anions, and (3) ZVI aging on Tc{sup (VII)} reductive removal in batch experiments. (authors)

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Demolition of the K-27 Building at the East Tennessee Technology Park (ETTP) - 17423

On February 8, 2016, URS - CH2M Oak Ridge LLC (UCOR) initiated the demolition of the East Tennessee Technology Park's (ETTP's) final gaseous diffusion building in DOE's Oak Ridge Environmental Management program. Building K-27 was a 35,582 m{sup 2} (383,000 ft{sup 2}) gaseous diffusion building that contained approximately 92,903 m{sup 2} (1 million ft{sup 2}) of floor space. It was one of five gaseous diffusion buildings at the site, formerly known as the Oak Ridge Gaseous Diffusion Plant. The actual demolition of this facility took approximately seven months to complete; however, planning and preparation took more than three years. The deactivation process was a critical element in preparing the building for demolition. UCOR's K-27 deactivation activities began in April 2012 with the installation of safe walking paths and fall protection systems to allow safe work access. Next, all mechanical and electrical systems associated with the facility were shut down and isolated, a process known as 'cold and dark.' More than 19.3 km (12 mi) of process piping and components were marked and measured. Additionally, workers performed nondestructive assay (NDA) and vent-purge-and-drain activities and applied foam to piping and components as needed [1]. Based on characterization results, approximately 4.8 km (3 mi) of process piping, and 372 converters and compressors were removed and shipped offsite prior to demolition. Lower-hazard materials and equipment were demolished with the building structure and transported to onsite disposal facilities. Upfront waste characterization and ongoing monitoring were key to the successful disposal of demolition debris at onsite facilities. Due to process improvements in waste loading recommended by work crews, the project achieved a 50 percent improvement in the daily hauling rate during the 9,000-truckload shipping campaign. Crews worked in high-risk, high-hazard conditions and were exposed to radiological and chemical contaminants, extreme temperatures, and deteriorating infrastructure. However, the hazard controls that were put in place, based on the Integrated Safety Management System (ISMS) walk-downs and hazard determination, made the effort manageable. The overall safety performance during demolition of the facility was excellent, with no significant injuries, and exceeded industry standards and DOE target levels. Outstanding safety performance was a testament to the dedication of the workforce, given the significant hazards presented by the demolition of the Hazard Category 2 nuclear facility. Another key element to the success of the K-27 demolition was the support and approval of all stakeholders involved in this effort, including DOE, the surrounding communities, the State of Tennessee, the UCOR management team, and, most importantly, the workforce that performed this highly hazardous work. This $52 million demolition project was completed ahead of schedule with no significant injuries and in compliance with all DOE orders, site procedures, and environmental controls. (authors)

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NUHOMS{sup R} EOS (Extended Optimized Storage): Robust, Advanced, and Dual Purpose Dry Storage System - 16472

AREVA TN has completed the design, analysis, and US NRC license submittal for the NUHOMS{sup R} Extended Optimized Storage (EOS) system. NUHOMS{sup R} EOS offers a large capacity and high heat load dry storage and transportation solution for UNF. EOS is not a new system, but an evolution of the already-proven safe and low-risk horizontal NUHOMS{sup R} storage system, which is one of the most widely used UNF dry storage systems in the United States. The EOS system features a 37PTH dry shielded canister (DSC) for 37 PWR UNF assemblies and an 89BTH DSC for the 89 BWR UNF assemblies. The EOS DSCs will be stored inside a horizontal storage module (HSM) that is a robust, fortress-like concrete storage overpack. Designed with the lessons learned from the Fukushima event in Japan in mind, EOS has robust margins for beyond design basis (BDB) events and offers the lowest risk and highest safety margin of any dry storage system design for recovery from BDB events. EOS also offers innovative aging management features with an aging management program (AMP) to assure safe and low dose long-term storage at the utility sites. EOS incorporates ports for AMP inspections and offers the option of using duplex stainless steel (DSS) for the DSC shell in order to negate corrosion issues. EOS is stored horizontally and above ground, making it easy and quick to access for visual inspection, monitoring, and mitigating actions during AMP. NUHOMS{sup R} EOS is optimized for high capacity, high burnup, high enrichments, and very low cooling times for UNF assemblies. It enables the highest heat load per canister (50 kW) and low dose rates. Even with high heat loads, EOS has significant margins to design basis limits. As the future of used fuel disposition will require the need to move fuel off-site to interim or consolidated storage, EOS is the ideal solution as it enables on-site loading and unloading operations that mitigate risk when transferring fuel on-site or transporting fuel off-site. The EOS design can be safely located in a traditional outdoor setting with fortress-like concrete reinforced modules that offer superior resistance to attack or can be safely operated inside of a building enclosure for those utilities desiring a more discreet siting for its used fuel storage systems. EOS has an innovative basket design that is made of high strength low alloy (HSLA) material and is easy to fabricate due to its non-welded design. Its innovative inlet and outlet air vent design, which incorporates dose reduction hardware, allows for optimal ambient airflow for highly efficient heat transfer with minimal radiation dose. The NUHOMS{sup R} EOS storage modules are interlocked in a side-by-side configuration offering superior and robust seismic performance. The license application for NUHOMS{sup R} EOS is currently under US NRC review and this system will be available for deployment in 2017. (authors)

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An Overview of R and D on Retrievability and Retrieval Technology in Germany - 20462

Retrievability is a term that is included in most radioactive waste management programs around the world. Although national definitions vary, the overall understanding of retrievability concerns the ability to recover waste packages from the repository mine after their emplacement. Different countries may implement retrievability in very different ways, ranging from a built-in reversibility into the emplacement process to the stipulation that retrievability may in no way impede passive safety in the post-closure phase. Germany takes a middle course such that retrievability in a HLW repository (repository for high level radioactive waste) may have no significant detrimental effect on passive safety. In Germany, the current siting process considers rock salt, clay rock, and crystalline rock as potential host rocks. Therefore, Research and Development (R and D) has been investigating repository concepts and retrievability in all host rocks. After introduction of retrievability in 2010, existing repository concepts were modified to facilitate retrieval. The changes made comprised, for example, equipping boreholes with steel liners, developing new technologies, and modifying existing emplacement devices. Apart from retrieval of HLW, retrieval of other wastes from underground repositories that were designed and operated without retrievability in mind, poses major technical and scientific challenges. Currently, studies are under way to investigate the feasibility and costs of partial retrieval of waste from an underground repository for hazardous and highly toxic waste in France, Stocamine. With regard to retrieval, the rock-mechanical conditions are deteriorating rapidly, so time is of the essence. In the Asse II mine in Germany, about 126,500 waste casks with low and intermediate level waste await retrieval. The repository mine suffers from difficult rock-mechanical conditions and inflow of brine, locally into emplacement areas. The Federal Company for Radioactive Waste Disposal (BGE) is legally required to retrieve all wastes from the Asse. Due to the specific challenges, R and D is needed to develop technical solutions for the safe retrieval from each of the emplacement chambers. R and D on retrievability and retrieval technology does not only address challenges in radioactive or toxic waste retrieval but may also help to germinate innovation to better master complex underground situations in general, e.g. in deep mining, tunneling, or repository construction. (authors)

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Mercury Remediation in Oak Ridge, Tennessee; Successes and Remaining Challenges - 19390

Mercury remediation is a high priority for the US Department of Energy's (DoE's) Environmental Management program in Oak Ridge, Tennessee because of large historical losses of mercury to the environment, and the potential health risks to humans and wildlife primarily through fish consumption. Remedial solutions for mercury contaminated aquatic systems are limited - many aquatic systems have diffuse sources of mercury (Hg) and depending on the environmental conditions, these low concentrations of inorganic Hg can result in fish consumption advisories due to the production of the more toxic methylmercury (MeHg) and its bioaccumulation and biomagnification. From the 1980's to the present, long-term monitoring of mercury concentrations in water and fish downstream of DOE facilities in Oak Ridge have provided an opportunity to assess the performance and effectiveness of various remedial and abatement actions to address mercury. Early actions in the mid-1980's focused on pollution control that positively affected mercury discharges to one local stream, including consolidation and elimination of untreated discharges, sanitary sewer relining, the construction of a pollution control facility, and the replacement of a contaminated settling basin. The 1990's were an intensive period of facility remedial actions designed to improve stream water quality and reduce mercury discharges. Actions included dechlorinating cooling water discharges, an additional phase of storm sewer relining, the addition of flow from a nearby reservoir, the addition of two small-scale mercury treatment systems, the bypass of stream flow around the settling basin, and the removal of high mercury-contaminated floodplain soils. Because of these multiple remedial actions total mercury concentrations in receiving streams decreased significantly; however, mercury concentrations in fish did not respond commensurately and remain a challenge to the present day. Although the mercury remedial strategy in Oak Ridge will continue to focus in the near-term on upstream facility source reduction, recent research suggests that understanding mercury transport, methylation, and bioaccumulation processes in the downstream environment is essential to reducing mercury fish concentrations. Since 2014, mercury remediation research and technology development activities have been underway to develop potential remedial solutions for the downstream environment, including use of sorbents to control soil leaching and the potential use of chemical or biological manipulations. The Oak Ridge mercury remediation story is a valuable case study for flowing systems that can inform our national-level understanding of potential mercury cleanup actions and their likely environmental response. (authors)

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Analysis of Krypton-85 Legacy Waste Forms: Part II

During a removal of legacy materials from one hot cell at the Idaho National Laboratory in 2010, five metal capsules and some loose zeolite material were identified as krypton (Kr) immobilization test specimens produced in the late 1970s under the Airborne Waste Management Program (AWMP). This AWMP research and development effort examined the encapsulation of 85Kr within a collapsed zeolite structure for use as a potential waste form for long-term storage. The recovered capsules appeared to have been placed to the side and remained untouched after the AWMP was halted in the mid-1980s. These reclaimed capsules and loose material presented a unique opportunity to study a potential 85 Kr waste form after three half-lives had elapsed. The first phase of this study included two parts: The first was to assess the physical condition of the capsule walls, and the second was to examine the Kr-containing material within the capsules. The first part of this study was previously reported and noted that substantial corrosion was observed throughout each capsule wall of the two previously breached capsules that were examined. One of these capsules had been hot isostatic pressed (HIPed) and one was not HIPed. The second part of the study examined the materials contained in the two previously breached capsules. There appears to be a relatively uniform distribution of Kr and rubidium throughout the pellets examined. The chemical composition of the pellets appears to be consistent with 5A molecular sieves. The material contained within the HIPed capsules showed ~1 at. % lead (Pb). The origin of the Pb is currently indeterminate. X-ray diffraction analysis shows a significant shift from the 5A structure, most likely due to the Kr encapsulation/sintering process that occurred when the samples were made. Calculations based on the energy dispersive spectrometry elemental analysis show a residual Kr level within the pellets that is within a factor of 2 of the reported Kr capacities for this type of processed material. This provides a clear indication that a significant fraction of the Kr initially encapsulated in the material remained within the waste form even following a significant breach of the capsule wall. As a result, it would appear that this Kr immobilization method, even in non-HIPed form, is very promising as a waste form for long-term storage. The successful analysis of these two breached capsules forms a solid basis for the future analysis of the remaining unbreached capsules, which offers the opportunity to provide an even more complete understanding of the long-term Kr retention performance of this promising waste form.

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Synthesis and Characterisation of Caesium Phosphomolybdate and Zirconium Molybdate found in the Highly Active Storage Tanks at Sellafield - 18154

Caesium phosphomolybdate (Cs{sub 3}PMo{sub 12}O{sub 40}.xH{sub 2}O, CPM) and zirconium molybdate (ZrMo{sub 2}O{sub 7}(OH){sub 2}.xH{sub 2}O, ZM) are two known fission products that precipitate out within the Highly Active Storage Tanks (HASTs) at Sellafield, potentially causing 'hot-spots' and blocking pipes. Currently, there is not enough behavioural understanding of these compounds present in the Highly Active Liquor (HAL) for effective Post Operational Clean Out (POCO) strategic planning. As the HASTs do not have an in situ monitoring system the behaviour of the HAL cannot be directly observed. Therefore, as with this research, non-radioactive simulants can be utilised to aid behavioural understanding to assist with the planning of future waste management programs. CPM, along with two different morphologies of ZM were characterised and compared to the common oxide particle material titanium dioxide (TiO{sub 2}). The study provides a detailed physical characterisation of the simulants including: particle shape, particle size, water content and crystal structure, along with zeta particle potential, suspension settling and compressive yield stress. CPM was found to be spheroidal in nature with a particle size of 275 nm and an x value of 13 H{sub 2}O which crystallises as a cubic lattice with space group Pn-3m. ZM was found to have a range of morphologies from cuboidal to wheat-sheaf, varying in size from 10 μm to 20 μm, with an x value of between 3 and 4 H{sub 2}O, which crystallise as a body-centred tetragonal lattice with space group I4{sub 1cd}. TiO{sub 2} used as a comparison simulant was found to be spheroidal in shape with particle size of 725 nm. The isoelectric points (IEPs) of the two ZM samples (ZM-A and ZM-B) with different morphologies were found to be pH 2.5, while for TiO{sub 2} it was pH 3.2. For CPM it could not be confidently identified due to its instability within the acidic environment. The settling rates and compressive yield stress of all simulants were tested in both water and 2 M nitric acid, conditions that replicate the HASTs. TiO{sub 2}, ZM-A and ZM-B all found settled faster in acid than in water. For CPM, slightly faster settling in acid was measured. For all samples it was found that as the particle concentration increased the settling rate decreased, which is a result of hindered settling. For compressive yield stress, similar trends were observed for CPM with little variation in its behaviour in acid and water, suggesting that the particles are highly aggregated in both fluids. For ZM samples little change in equilibrium volume fraction was measured with an increase in pressure (both acid and water). However, overall the sediment bed was denser in water, a result of the rapid settling in acid not allowing the non-spherical particles to pack in an ordered manner. It has been highlighted that both CPM and ZM within the acidic conditions of the HASTs, result in unstable and aggregated compounds, which settle quickly to form large open networks. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Approximating Dose and Risk for Contaminants in Groundwater from the Underground Nuclear Test Areas of the Nevada National Security Site (NNSS)

As part of the Environmental Management Program at the Nevada National Security Site (NNSS), the Underground Test Area (UGTA) Activity investigates the potential impacts of radionuclides that were introduced into groundwater from the underground nuclear tests conducted near or below the NNSS water table between 1951 and 1992. Groundwater models are being used to simulate contaminant transport and forecast contaminant boundaries that encompass areas where the groundwater has a five percent or greater probability of containing contaminants above the Safe Drinking Water Act Maximum Contaminant Levels (SDWA MCLs) at any time during the next 1,000 years. Transport modeling conducted for the Frenchman Flat Corrective Action Unit (CAU) at the NNSS identified the beta/photon-emitting radionuclides tritium (3H), carbon-14 ( 14 C), chlorine-36 ( 36 Cl), technetium-99 ( 99 Tc), and iodine-129 ( 129 I) as having the greatest influence in defining the farthest extent of the modeled CAU contaminant boundary. These same radionuclides are assumed here as the contaminants of concern (COCs) for all underground nuclear tests at the NNSS because models are not yet complete for the other CAUs. Potential public exposure to the COCs will only occur and be of concern if the COCs migrate into the groundwater beneath public or private lands at levels that exceed either individual SDWA MCLs or dose and risk limits. Groundwater flow directions strongly suggest that any contaminant boundary predicted by contaminant fate and transport modeling to overlap public or private lands is more likely to occur to the west and/or southwest of the NNSS and the adjacent Nevada Test and Training Range (NTTR). Well-established, rural communities exist in these directions. Estimates of representative activity concentrations at the applicable SDWA MCL were developed for the five COCs. It is assumed that these COC concentrations may collectively occur at some public or private location in the future, but that situation does not exist today. These representative activity concentrations are evaluated with respect to conforming collectively to a modern annual committed effective dose (CED) and lifetime excess cancer morbidity risk for a hypothetical reasonably maximally exposed individual (RMEI). This approach goes beyond the SDWA MCL focus of the contaminant boundary because individual COC concentrations may comply with the SDWA MCL but not collectively meet the modern health-protection metrics and the SDWA language, especially if future modeling studies or monitoring activities show multiple radionuclides from different SDWA MCL categories to be COCs. For the drinking water exposure pathway alone, the annual committed effective dose (CED) for the RMEI from all five COCs that are collectively at estimated activity concentrations equal to their SDWA MCL is well below the U.S. Department of Energy health-protective CED limit of 100 millirem (mrem)/yr. This is consistent using both the NNSS unclassified, 1992 decay-corrected radionuclide atom inventory and the atom inventory based on radionuclides measured in groundwater obtained from the ALMENDRO cavity in 2009 to calculate the SDWA MCL activity concentrations in groundwater. The RMEI’s total lifetime excess cancer risk from the drinking water exposure pathway for both atom inventories is within the range of 1 × 10 -4 to ≤ 1 × 10 -6 , which is considered health protective according to modern SDWA MCL regulatory language. The biosphere exposure pathways are drinking water, garden produce, animal products, inadvertent soil ingestion, and indoor and outdoor air inhalation. The exposure parameters for communities west and southwest of the NNSS were developed when the Yucca Mountain high-level, nuclear-waste disposal facility was under consideration. For all biosphere exposure pathways, calculations of the annual CED and lifetime excess cancer morbidity risk for the RMEI revealed that: 1) The annual CED is well within health-protective guidance (<< 100 mrem CED /yr) for the COC activity concentrations at the SDWA MCL, regardless of the atom inventory used. 2) The calculated 70-year lifetime excess cancer morbidity risk (6 x 10 -5 ) is within the health-protective range when the five COC activity concentrations are derived using the NNSS 1992 atom inventory, but it is at the upper limit of the acceptable range (1 x 10 -4 ) using the ALMENDRO 2009 atom inventory. 3) Tritium (3H) is the principal COC for producing annual dose and lifetime excess cancer risk, regardless of the atom inventory used. 4) Overall, the drinking water ingestion pathway is the dominant exposure pathway contributing to the total annual CED and lifetime excess cancer risk, followed by eating locally grown produce and animal products. 5) When tritium completely decays (after about 100 years), the RMEI’s lifetime risk will fall well within the health-protective range (i.e., 1 × 10-4 to ≤ 1 × 10 -6 ) and 36Cl will then become the most important contributor to the RMEI’s total annual CED and lifetime excess cancer morbidity risk from eating local produce and animal products. In the event that radionuclide concentrations begin to approach SDWA MCLs, a reasonable risk-management strategy for keeping lifetime risk more in compliance with regulatory guidance would be to use local sources of groundwater that are below SDWA MCLs or to limit the consumption of local produce and animal products that have ingested COC-contaminated groundwater. The viability of the latter strategy increases where the annual CED due to 36Cl approaches that of 3H.The dose and risk values calculated here for an RMEI are specific to the assumption that the five COCs occur in groundwater beneath public or private lands at concentrations that are collectively at the SDWA MCL. Currently, these COCs are essentially absent from groundwater beneath public or private lands beyond the boundaries of the NNSS and NTTR other than at very low, naturally occurring concentrations. The analyses presented here can be readily applied to determine dose and risk for COC concentrations actually measured in future monitoring samples.

54 ENVIRONMENTAL SCIENCES↗