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rHealth One Demonstration Aboard ISS: A Microfluidic Bioanalyzer Based on Sheath/Hydrodynamic Focusing Flow Cytometry

The Exploration Medical Capability (ExMC) element aims to provide astronauts with the means for their own health monitoring, diagnosis, and treatment during exploration missions. As space flight ventures further from earth, the need for autonomous medical care increases under greater constraints on size, mass, and resources. One pillar for diagnosis that crew would be separated from is laboratory analysis. Even now on ISS, blood samples must be collected and returned to earth for testing. In response, ExMC is assessing how assays for hematology, bone health, radiation exposure etc. could be addressed through commercial-off-the-shelf (COTS) and Small Business Innovation Research (SBIR) funded bioanalyzers that are miniaturizing lab technology. Since missions will reach distances where there are no timely replacements, validation on the International Space Station (ISS) is a necessary part of that assessment. In partnership with NASA Johnson Space Center (JSC) Immunology Lab and the Research Operations and Integration (ROI) element, ExMC conducted a technology demonstration on ISS of the rHEALTH ONE, a flow cytometry based bioanalyzer, to assess future devices based on this design. In flow cytometry, there are predominantly three ways to focus the cells (or particles) into a single file stream: hydrodynamic focusing, microcapillary, and acoustic focusing. The rHEALTH ONE utilizes the commercial standard, sheath-based hydrodynamic focusing. rHEALTH itself represents both a company and a suite of medical tools NASA has funded through SBIR grants towards the development of a promising diagnosis instrument for exploration missions. rHEALTH ONE is the interim version of the technology, functional as a benchtop analyzer and test bed for the next generation of rHEALTH in development. Several modifications were made to the rHEALTH ONE analyzer for operation in microgravity. For function, fluid management was key. A sheath-based analyzer uses sheath fluid to flow the sample, cleaning fluid to prevent biological contamination, and a reservoir to collect the liquid waste. The rHEALTH ONE analyzer uses bottles dependent on gravity to separate the air and liquid pathways and keep the liquids contained. It uses only 1 psig of air pressure to directly push the liquid through the device, requiring little-to-no resistance at inlet and outlet. A microtubing assembly with self-sealing luer connectors was designed – featuring 0.014 mm thick durable medical balloons to hold water inside the supply bottles – to create safe containment and easy access for the crew while maintaining the analyzer’s function. For safety, copper tape was added to the interior of the plastic housing to reduce electromagnetic interference, fluid and electrical connections were secured against vibration and leaks, and gaps were further sealed to ensure containment of the optical block and lasers. Water as the sheath and cleaning fluid and TOX 0 samples were used to reduce the biohazard risk to the crew. In May 2022, European Space Agency astronaut Samantha Cristoforetti demonstrated the rHEALTH ONE aboard ISS for its sample loading, flow cytometry, and data collection capability in microgravity. The JSC Immunology Lab provided flow cytometry expertise, designed the sample test protocol, and manufactured and benchmarked the flight samples on a ‘gold-standard’ flow cytometer. The analyzer was primed with water, purged of air, and four calibration solutions of polystyrene microparticles were tested to characterize its performance. Tightly controlled procedures and excellent execution prevented air bubble interference during air/water separation, fluid transfer, sample mixing and loading. Data showed a slight increase in signal noise on 3 of 5 channels and an anomaly of fluorophores migrating in one sample (confirmed by JSC post-flight). Flight results correctly detected the change in sample, matched the analyzer’s ground performance, and were consistent with the gold-standard’s ground results. Although areas were noted for improvement, these outcomes signified complete mission success.

R. S. Miller↗

DOE OSTI2026

Effects of Composition and Oxidation States on the Structures of Chromium-Containing Sodium Silicate Glasses: Molecular Dynamics Simulations using Machine Learning Interatomic Potentials

Chromium represents a significant challenge for the vitrification of high-level nuclear waste into silicate and borosilicate glasses due to its low solubility and variable oxidation states, which can limit the waste loading due to promotion of crystallization or phase separation during processing. In this study, we modeled chromium containing silicate glasses using molecular dynamics simulations with three machine learning interatomic potentials (MLIPs), MACE, CHGNet, and PFP were employed, to gain insights on glass composition and oxidation states on the structures of these glasses. One of the goals is to evaluate their ability of these MLIPs to accurately represent the general structure of silicate glasses and chromium local environments as a function of chromium oxidation states. Density Functional Theory (DFT) based calculations and experimental data such as neutron structure factors were used to validate the structural models. It was found that the foundation models of all three MLIPs are able to reproduce general structural features of the sodium silicate glass structure consistent with experimental and DFT data, but only CHGNet and PFP can accurately capture the oxidation states and local environment of chromium: tetrahedral for Cr6+ and octahedral for Cr3+. Furthermore, we studied the effect of varying Cr3+/ Cr6+ (Cr3+/Crtotal) ratio and total chromium content using PFP. Our results show that Cr6+ enhances network polymerization by reducing non-bridging oxygens through Na? charge compensation required due to the formation of chromate (CrO42-) species, while Cr³? acts as a network modifier that disrupts connectivity. System size effects on the structural characteristics and chromium environments were also tested using the PFP potential. This work highlights the importance of careful validation on the precision, transferability, and potential of MLIPs for modeling glasses containing transition metal elements that can exist in multiple oxidation states. It is also encouraging to see the foundational models are all three MLFFs are able to reproduce the basic sodium silicate glass structures, while suggesting additional training or refining is needed to improve the description of more complex systems containing transition metals.

Puga, Christina L.↗

DOE OSTI2017

Integrated Solutions for Interim Used Fuel Management: From Pool Unloading to Safe Delivery to Recycling or Repository Facilities - 17235

Safe management of used nuclear fuel (UNF) is key to the survival of the nuclear industry. That is why it is more important than ever to have a consent-based, practical, credible, and sustainable roadmap for managing the back-end of the nuclear cycle. Worldwide UNF Light Water Reactors (LWR) inventories are currently around 200,000 tons and are estimated to grow to more than 350,000 tons by 2030, and operating nuclear reactors in the U.S. continue to discharge UNF every 18 to 24 months. International experience has demonstrated that the development of a permanent geological repository can be a multi-decade process, especially in the face of public acceptance challenges. Meanwhile, the solution for permanent disposal of UNF in the U.S. is moving at a glacial pace. As a result, industrial stakeholders have been forced to find practical interim UNF storage solutions in order to continue safely operating their reactors. Among those interim solutions are the cask- or canister-based dry storage systems that have dramatically increased in the last 10 years as they provide flexibility for expansion with a low up-front investment. With interim dry storage in place for more than 30 years, our industry is entering a new phase as we are forced to prepare for a few more decades before geological repositories begin operating. Consequently, interim dry storage has to be extended for 80 years or more. Thus, new considerations have to be taken into account to ensure the safety of this stored used fuel: - Interim storage systems are aging; - High burn-up fuel behavior overtime is uncertain; - Used fuel is losing its self-protection; - The number of shutdown sites without a fuel transfer facility, such as a pool, is increasing; - Some owners of Independent Spent Fuel Storage installation (ISFSI) at shutdown sites are not nuclear operators anymore. With increasing uncertainties, AREVA TN -- based on its long expertise with used fuel transportation and interim storage systems -- is adapting its portfolio to develop integrated and flexible solutions that will remove the burden of interim used fuel management from nuclear operators. AREVA TN is developing comprehensive solutions to reduce risks including the continued supply of proven safe high-performance dry storage systems; on-site services to safely transfer used fuel from pool to pad; the optimization of fuel heat load in the storage pool and pad; innovative aging management services including inspection, monitoring and repair; a realistic solution for consolidated interim storage with a priority to remove Used Nuclear Fuel stored in dry storage systems from shutdown sites; world-class transport and logistics services to safely move the used fuel from nuclear reactor sites to consolidated storage and repository or recycling as applicable, and turnkey management of shutdown ISFSIs. Due to the lack of an available path for transporting used fuel away from reactors, nuclear operators are faced with many challenges and growing uncertainties. Our presentation will describe the practical solutions developed and being developed in order to manage used fuel on behalf of nuclear operators and allows them to continue focusing on the important job of producing carbon-free clean energy. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2023

Benchmarking the AirSquared All-Metal Scroll Pump Against the Normetex 15 - Preliminary report

Tritium operations require specialized equipment for material compatibility, safety, and waste considerations. Non-metallic pump materials (polymer, oil, or grease) on a tritium-wetted surface can absorb tritium and/or undergo isotope exchange between tritium and more common protium, creating tritiated compounds that can result in material property modification via beta-radiolysis, inventory loss, reduced performance and special waste considerations, all of which increase the operating cost for a facility. Vacuum pumps move gas via a pressure differential between volumes of an operation. Several types of all-metal vacuum pumps exist for this application including metal bellows, diaphragm and scroll pumps. A metal bellows pump incorporates only metal components at the wetted surfaces. The common metal bellows pump employed in tritium facilities, the MB601 (Senior Metal Bellows, Sharon, PA, USA) creates a gas-motive force with a vacuum pressure between 30-40 torr. These pumps can efficiently move gas from one process step to another, as long as sub-30 torr pressures are not required. However, for higher vacuum demand, an all-metal scroll pump can be used with the bellows pump serving as a “backing” pump. This configuration typically provides an achievable vacuum of less than 20 mTorr. All-metal scroll pumps are a technology uniquely applicable to tritium gas handling. The industry standard all-metal scroll pump for glovebox-scale tritium operations is the Normetex 15 m 3 /hr, typically referred to as the Normetex 15 (Normetex Pompes, Pont Audemer, France). However, the final Normetex pumps were manufactured in 2012, rendering them no longer available. Eumeca SaRL (formerly Normetex) has developed and is marketing a scroll pump based on the design of the Normetex 15. A US company, AirSquared (Broomfield, Colorado), has developed and is marketing a potential alternative to the Normetex 15. The Gas Transfer Systems group (Q-7) of the Los Alamos National Laboratory (LANL) procured serial number 0001 of the AirSquared All Metal Vacuum Scroll pump model number V16H034A-C01 in 2019. The LANL Hydrogen Processing Laboratory (HPL) has been evaluating the performance of the pump compared to a Normetex pump as a potential replacement in tritium and fusion facilities requiring this type of pump.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

NASA NTRS1999

Tissue Engineered Skeletal Myofibers can Directly "Sense" Gravitational Force Changes

Long-term manned space flight requires a better understanding of skeletal muscle atrophy resulting from microgravity. Atrophy most likely results from changes at both the systemic level (e.g. decreased circulating growth hormone, increased circulating glucocorticoids) and locally (e.g. decreased myofiber resting tension). Differentiated skeletal myofibers in tissue culture have provided a model system over the last decade for gaining a better understanding of the interactions of exogenous growth factors, endogenous growth factors, and muscle fiber tension in regulating protein turnover rates and muscle cell growth. Tissue engineering these cells into three dimensional bioartificial muscle (BAM) constructs has allowed us to extend their use to Space flight studies for the potential future development of countermeasures. Embryonic avian muscle cells were isolated and BAMs tissue engineered as described previously. The myoblasts proliferate and fuse into aligned postmitotic myofibers after ten to fourteen days in vitro. A cylindrical muscle-like structure containing several thousand myofibers is formed which is approximately 30 mm in length, 2-3 mm in diameter, and attached at each end. For the Space Shuttle experiments, the BAMs were transferred to 55 mL bioreactor cartridges (6 BAMs/cartridge). At Kennedy Space Center, the cartridges were mounted in two Space Tissue Loss (STL) Modules (three to four cartridges per Module) and either maintained as ground controls or loaded in a Mid-Deck locker of the Space Shuttle. The BAM cartridges were continuously perfused during the experiment at 1.5 mL/ min with tissue culture medium. Eighteen BAMs were flown for nine days on Mission STS66 while eighteen BAMs served as ground controls. The complete experiment was repeated on Mission STS77 with twenty four BAMs in each group. BAMs could be maintained in a healthy state for at least 30 days in the perfusion bioreactor cartridges. The BAM muscle fibers directly detected both the loss of gravity and the reloading effects of 1 x g. While total cellular metabolism and total protein degradation rates were not altered during 9 to 10 days in Space, protein synthesis rates were significantly reduced and resulted in significant myofiber atrophy compared to ground controls. One g reloading of the flight muscle cells post-flight significantly increased protein synthesis rates and the synthesis rates of myosin heavy chain, fibronectin, and collagen. Tissue cultured muscle cells can directly "sense" changes in gravity and provide a valid model to begin the study of countermeasures. Based on our ground based experiments, and the experiments of others, growth hormone and/or insulin-like growth factors are attractive protein therapeutics which may assisting attenuating skeletal muscle wasting in space. Our laboratory is developing a new cell-based delivery system for this and other potential therapeutic factors for attenuating muscle and bone wasting.

Vandenburgh, Herman H.↗

DOE OSTI2023

Developing a Carbon Negative Biorefinery for Organic Waste Valorization

Production of bio-based chemicals have become increasingly attractive as efforts to meet carbon neutrality goals expand. Diverse organic waste feedstocks can be valorized via arrested anaerobic digestion and chain elongation to produce important key intermediates, such as medium chain carboxylic acids. Our work aims to develop a carbon negative biorefinery that funnels multiple organic waste feedstocks into a chemically consistent stream of carboxylic acids that are then upgraded to exemplary carbon negative products. The pairing of a hydrolysis reactor with a chain elongation reactor will allow each biological step to be optimized to improve the ability to valorize a variety of organic waste streams. Specifically, this work has so far been aimed at screening for potential chain elongating organisms to produce VFAs and MCCAs of interest. Four chain elongating organisms were tested for their chain elongation potential with diverse single and mixed substrates. So far, Megasphaera elsdenii and Actinobacillus succinogenes have been tested to determine potential differences in titer as well as product speciation due to variations in pH. To do this, each organism was tested under 3 different substrate combinations with pH maintained at either 5.5, 6, or 7. With better understanding of their metabolic needs and optimal operating conditions, these chain elongating organisms could provide a valuable option to facilitate the chain elongation necessary to produce precursor molecules. In addition to optimizing the bioconversion steps, downstream processing of carboxylic acids is also a key component for the overall feasibility of the process. Our group previously developed a downstream in-situ product recovery (ISPR) process for continuously recovering bio-based carboxylic acids from fermentation broth. The ISPR includes: (i) a solid-liquid separation as a cell retention device, (ii) a liquid-liquid extraction (LLE) to selectively extract the desired bio-based acids, and (iii) a distillation to obtain the neat product. The integrated process was demonstrated at bench-scale and is now scaled up for pilot-scale operations. A more cost-efficient membrane-based emulsion separation is introduced for LLE in downstream separation process with greatly promoted mass transfer, leading to -2800 times smaller needed membrane area than membrane contactors to achieve the same butyric acid extraction rate.

BIOMASS FUELS↗

DOE OSTI2019

Selective Recovery of Rare Earth Elements from Coal Fly Ash Leachates Using Liquid Membrane Processes

Coal combustion residues and other geological waste materials have been proposed as a resource for rare earth elements (REEs, herein defined as the 14 stable lanthanides, yttrium, and scandium). The extraction of REEs from residues often generate acidified leachates that require highly selective separation methods to recover the REEs from other major soluble ions in the leachates. We studied two liquid membrane processes (liquid emulsion membranes, LEM, and supported liquid membranes, SLM) and compared them to standard solvent extraction techniques for selective recovery and concentration of REEs from a leachate of coal fly ash. All separation methods involved an organic solution of di(2-ethylhexyl)phosphoric acid dissolved in kerosene or mineral oil and an acid strippant solution of 5 M nitric acid for the liquid-based separations. The LEM configuration, which separated REEs by immersing an acid-in-oil emulsion in the ash leachate, resulted in similar recovery percentages of individual REEs as the conventional solvent extraction approach. The recovery of REEs in the SLM configuration, which involved the impregnation of the solvent in a hydrophobic membrane, was slower than the LEM process. However, the SLM process was notably more selective for the heavy (and higher value) REEs, while the conventional extraction and LEM processes were more selective for the light REEs. A flux-based model of the extraction processes suggested that recovery rates were limited by REE affinity for the solvent chelator in the SLM, while the rates of REEs separation via LEM were limited by diffusive mass transfer across the liquid membrane. Altogether, these results help to identify specific steps in the recovery process that future work should target in the development of scalable liquid membrane separations for REE recovery.

42 ENGINEERING↗

DOE OSTI2025

Findings on subtask 3.3 – applicability of automated brine chemistry determinations for treatment and recovery processes through facility automation/modularization: engineering design study

Under the Energy & Environmental Research Center’s (EERC’s) ~$\$$22 million Phase II Brine Extraction and Storage Test (BEST) Program, a multimillion-dollar brine treatment technology test bed facility was established in western North Dakota to provide a platform for evaluating developing technologies and approaches for brine treatment and volume reduction. The initial facility, and associated research effort, was funded by the U.S. Department of Energy (DOE), with in-kind contributions provided by several industry participants and the state of North Dakota. Since its opening, the Brine Technology Test Facility (BTTF) has supported performance evaluations of desalination technologies capable of treating high-salinity produced water (PW) and enabled data collection for multiple approaches of PW management and critical material recovery. As part of the decommissioning process for the original project, facility ownership and liability were transferred to Select Water, which is providing the EERC with a continuing site access option for state or federal research and/or commercial technology development. This report documents the findings from a design study conducted by the EERC and the engineering firm that was originally contracted to design and construct the facility (Advanced Engineering and Environmental Services, LLC [AE2S]) that evaluated the current status of BTTF and its systems and developed a retrofit design to increase the facility’s capabilities through automation and modularization of its PW treatment infrastructure. The proposed retrofit will provide DOE and industry with an expanded range of conditioned PW that can be produced at the facility for evaluating fit-for-purpose water treatment technologies, online instrumentation for brine chemistry determination, and systems that recover critical materials like lithium and magnesium. The current facility consists of an 9600-square-foot facility that includes a 40-foot by 65-foot Class 1, Division 2-rated demonstration area and associated control rooms and lab-ready space capable of sourcing oil and gas PW and wastewater from industrial sources or tailoring brine compositions up to 300,000 mg/L total dissolved solids (TDS) and supplying them at rates up to 25 gpm for extended-duration technology demonstrations. The colocation of the facility with Select Water’s water management facilities allows for access and unloading of more than 10,000 bbl/day of trucked water delivered to site and associated access to on-site Class I and Class II brine disposal wells and nearby hazardous waste landfills operated and/or contracted by Select Water to dispose of concentrate and/or effluents associated with the testing.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS2004

A 100 kW-Class Technology Demonstrator for Space Solar Power

A first step in the development of solar power from space is the flight demonstration of critical technologies. These fundamental technologies include efficient solar power collection and generation, power management and distribution, and thermal management. In addition, the integration and utilization of these technologies into a viable satellite bus could provide an energy-rich platform for a portfolio of payload experiments such as wireless power transmission (WPT). This paper presents the preliminary design of a concept for a 100 kW-class free-flying platform suitable for flight demonstration of technology experiments. Recent space solar power (SSP) studies by NASA have taken a stepping stones approach that lead to the gigawatt systems necessary to cost-effectively deliver power from space. These steps start with a 100 kW-class satellite, leading to a 500 kW and then a 1 MW-class platform. Later steps develop a 100 MW bus that could eventually lead to a 1-2 GW pilot plant for SSP. Our studies have shown that a modular approach is cost effective. Modular designs include individual laser-power-beaming satellites that fly in constellations or that are autonomously assembled into larger structures at geosynchronous orbit (GEO). Microwave power-beamed approaches are also modularized into large numbers of identical units of solar arrays, power converters, or supporting structures for arrays and microwave transmitting antennas. A cost-effective approach to launching these modular units is to use existing Earth-to-orbit (ETO) launch systems, in which the modules are dropped into low Earth orbit (LEO) and then the modules perform their own orbit transfer to GEO using expendable solar arrays to power solar electric thrusters. At GEO, the modules either rendezvous and are assembled robotically into larger platforms, or are deployed into constellations of identical laser power-beaming satellites. Since solar electric propulsion by the modules is cost-effective for both self-transport of the modules from LEO to GEO, and for on-orbit stationkeeping and repositioning capability during the satellite’s lifetime, this technology is also critical in technology development for SSP. The 100 kW-class technology demonstrator will utilize advanced solar power collection and generation technologies, power management and distribution, advanced thermal management, and solar electric propulsion. State-of-the-art solar concentrators, highly efficient multi-junction solar cells, integrated thermal management on the arrays, and innovative deployable structure design and packaging make the 100 kW satellite feasible for launch on one existing launch vehicle. Early SSP studies showed that a major percentage of the on-orbit mass for power-beaming satellites was from massive power converters at the solar arrays, at the bus, at the power transmitter, or at combinations of these locations. Higher voltage mays and power management and distribution (PMAD) systems reduce or eliminate the need for many of these massive power converters, and could enable direct-drive of high-voltage solar electric thrusters. Lightweight, highly efficient thermal management systems are a critical technology that must be developed and flown for SSP feasibility. Large amounts of power on satellites imply that large amounts of waste heat will need to be managed. In addition, several of the more innovative lightweight configurations proposed for SSP satellites take advantage of solar concentrators that are intractable without advanced thermal management technologies for the solar arrays. These thermal management systems include efficient interfaces with the WPT systems or other high-power technology experiments, lightweight deployable radiators that can be easily integrated into satellite buses, and efficient reliable thermal distribution systems that can pipe heat from the technology experiments to the radiators. In addition to demonstrating the integration and use of these mission-critical technologies, the 100 kw-class satellite will provide a large experiment deck for a portfolio of technology experiments. Current plans for this technology demonstrator allow 2000 kg of payload capability and up to 100 kW of power. The technology experiments could include one or more wireless power transmission demonstrations, either to the Earth’s surface or to a suitable space-based receiver. Technology experiments to quantify the on-orbit performance of critical technologies for SSP or space exploration are welcomed. In addition, the technology experiments provide an opportunity for international cooperation, to advance technology readiness levels of SSP technologies that require flight demonstration. This paper will present the preliminary design for a 100 kW solar-powered satellite and a variety of technology experiments that may be suitable for flight demonstration. In addition, a space-to-Earth-surface WPT experiment will be discussed.

Connie Carrington↗

DOE OSTI2020

Closure Report for the Project Shoal Area: Subsurface Corrective Action Unit 447 Shoal,Nevada, Site

The U.S. Department of Energy (DOE) Office of Legacy Management (LM) has prepared this Closure Report for subsurface Corrective Action Unit (CAU) 447 at the Shoal, Nevada, Site, which was formerly called the Project Shoal Area. The Shoal site was the location of an underground nuclear test in 1963 that resulted in residual radionuclide contamination at the detonation depth of 1211 feet (ft) (DOE 2015a). The environmental restoration process and Corrective Action strategy are conducted in accordance with the Federal Facility Agreement and Consent Order (FFACO) (FFACO 1996, as amended) and all applicable Nevada Division of Environmental Protection (NDEP) statues and regulations. Responsibility for the environmental site restoration was transferred from the DOE, National Nuclear Security Administration, Nevada Field Office, to LM on October 1, 2006. The Shoal site is south of U.S. Highway 50, approximately 30 miles southeast of Fallon, in Churchill County, Nevada (Figure 1). The site was selected for underground nuclear testing in 1961, as part of the Vela Uniform Program. Vela was a research and development program directed toward locating, detecting, and identifying underground and high-altitude nuclear detonations. The Vela Uniform program was specific to underground detonations (AEC 1964). The objective of Project Shoal was to detonate a nuclear device underground in an active seismic area to improve the United States’ ability to detect, identify, and locate underground nuclear detonations. The underground nuclear test at Shoal was a joint effort between the U.S. Department of Defense (DOD) and the U.S. Atomic Energy Commission (AEC), which was the predecessor agency to DOE. Figure 1 is a map showing the site location.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2018

Encapsulation of Defective Fuel Rods for Transport and Dry Storage - 18190

Removing of the whole inventory of fissile and non-fissile material out of the spent fuel pool is performed when the power plant is about to start its last operation phases or may occur during the extended operating life cycle due to plant storage space limitation. Removal of defective spent fuel is then definitely required for emptying the pool and may in addition also be performed in the course of plant operation for reducing pool contamination. Depending on the general used fuel management solution chosen for post-storage pool operations, specific management of a defective fuel assembly (DFA) and/or a defective fuel rod (DFR) should be implemented accordingly to the regulation requirements to be followed. For meeting these DFA and/or DFR management needs, Framatome together with New AREVA offer wide portfolio of solutions with flexibility and adaptability advantages: - from simple to advanced technologies; - for several types of fuel assemblies and/or defective rods; - for suitable and compatible cask designs; - for compatible solution with both used fuel final management strategies (closed and open fuel cycles). For instance, a technology is jointly proposed and developed by New AREVA and Framatome for implementing dry storage of DFR. It consists in: - encapsulating each DFR by loading the fuel rod in a respective capsule, drying the fuel rod using a process which allows to physically verify with high accuracy the dryness inside the DFR, and seal welding the capsule - assembling the capsules in a capsule canister (a skeleton with external dimensions similar to a respective fuel assembly) and - transferring the capsule canister along with intact spent fuel assemblies in an associated dry transport and storage (dual purpose) cask. Such a project is currently being implemented in Belgium. After successfully obtaining the cask transport and storage license extensions for including the encapsulated DFR content, the first encapsulation campaign has been started in 2017. The purpose of the paper is to present the industrial solutions proposed by Framatome and New AREVA together, for management of DFR, notably the one related to dry storage of encapsulated DFR implemented in Belgium and the perspectives opened by this successful project. The paper presents: - the available solutions for management of DFA and/or DFR depending on applicable requirements - the drying method, welding of a capsule and associated cask as the state of art technology for dry storage of DFR and/or DFA; - lessons learned from project management and encapsulation campaign performed in Belgium; - perspectives for management of DFR and/or DFA. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2020

Analysis of Hydrology and Interim Measure Performance in the Chromium Plume at Los Alamos National Laboratory - 20498

Hexavalent chromium, Cr(VI), is present in the regional aquifer beneath Los Alamos National Laboratory (LANL) at concentrations greater than the New Mexico groundwater standard (50 ppb). The source of the Cr is blowdown from a power plant where potassium dichromate was used as a corrosion inhibitor from 1956 to 1972. Blowdown comingled with effluent from another source and migrated approximately 3 miles down a canyon, primarily as surface flow, until reaching an alluvial infiltration zone. The infiltrating water moved vertically through a thick (approximately 900 ft), complex stratigraphic sequence of unsaturated tuffs, basalt, and unconsolidated alluvial deposits. Horizontal transport also took place within spatially limited perched groundwater horizons in the vadose zone (VZ). Breakthrough at the regional aquifer water table is thought to have occurred in multiple hydraulic windows or 'drip points' located approximately 3 miles from the initial release site at the power plant. The regional aquifer is highly heterogeneous and anisotropic, and displays unconfined behavior in an upper zone and confined behavior at depth. The Cr(VI) contamination has so far remained confined to the upper approximately 25 m of the aquifer. The ambient hydraulic gradient in the regional aquifer is toward the east/southeast, but the water table is extremely flat in the Cr plume area compared to surrounding areas. There is some local variability in flow direction, potentially related to effects of seasonal pumping from nearby Los Alamos county water-supply wells, which draw from the regional aquifer several hundred feet below the water table. An interim measure (IM) is currently operating at the site to achieve hydraulic control of plume migration using a series of extraction wells, ion-exchange treatment, and injection along the downgradient portion of the plume. The migration of Cr contamination in the aquifer has been previously evaluated using a calibrated probabilistic numerical model, which has also been used to design the spatial configuration of extraction and injection wells for the IM, and to identify locations for monitoring wells. The model is built using the Finite Element Heat and Mass (FEHM) transfer code, and the Model Analysis and Decision Support (MADS) software is used for analyses. To date, the portion of the IM system that has operated in a continuous manner has been very effective at hydraulic control. Modifications to the flow field associated with the influence of IM pumping and injection are evaluated here, with modeling constraints to be provided by recent observations of tracers injected into both monitoring wells and IM injection wells, as well as opportunistic observations of geochemical signatures of treated ion-exchange effluent injected into IM injection wells. The tracer and geochemical data provide insights into modified flow directions within the Cr plume area that cannot be otherwise obtained. Results of the modeling work are being used to inform adaptive management of IM operations and will be a valuable tool for development and refinement of long-term remediation strategies. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2011

Bioreduction of Fe-bearing clay minerals and their reactivity toward pertechnetate (Tc-99)

99 Technetium ( 99 Tc) is a fission product of uranium-235 and plutonium-239 and poses a high environmental hazard due to its long half-life (t1/2 = 2.13 x 10 5 y), abundance in nuclear wastes, and environmental mobility under oxidizing conditions [i.e., Tc(VII)]. Under reducing conditions, Tc(VII) can be reduced to insoluble Tc(IV). Ferrous iron [Fe(II)], either in aqueous form or in mineral form, has been used to reduce Tc(VII) to Tc(IV). However, the reactivity of Fe(II) from clay minerals, other than nontronite, toward immobilization of Tc(VII) and its role in retention of reduced Tc(IV) have not been investigated. In this study the reactivity of a suite of clay minerals toward Tc(VII) reduction and immobilization was evaluated. The clay minerals chosen for this study included five members in the smectite-illite (S-I) series, (montmorillonite, nontronite, rectorite, mixed layered I-S, and illite), chlorite, and palygorskite. Fe-oxides were removed from these minerals with a modified dithionite-citrate-bicarbonate (DCB) procedure. The total Fe content of these clay minerals, after Fe-oxide removal, ranged from 0.7 to 30.4% by weight, and the Fe(III)/Fe(total) ratio ranged from 44.9 to 98.5%. X-ray diffraction (XRD) and Mossbauer spectroscopy results showed that after Fe oxide removal the clay minerals were free of Fe-oxides. Scanning electron microscopy (SEM) revealed that little dissolution occurred during the DCB treatment. Bioreduction experiments were performed in bicarbonate buffer (pH-7) with Fe(III) in the clay minerals as the sole electron acceptor, lactate as the sole electron donor, and Shewanella Putrifaciens CN32 cells as mediators. In select tubes, anthraquinone-2,6-disulfate (AQDS) was added as electron shuttle to facilitate electron transfer. The extent of Fe(III) bioreduction was the highest for chlorite (~43 wt%) and the lowest for palygorskite (~4.17 wt%). In the S-I series, NAu-2 was the most reducible (~31 %) and illite the least (~0.4 %). The extent and initial rate of bioreduction were positively correlated with the percent smectite in the S-I series (i.e., layer expandability). Fe(II) in the bioreduced clay minerals subsequently was used to reduce Tc(VII) to Tc(IV) in PIPES buffer. Similar to the trend of bioreduction, in the S-I series, reduced smectite showed the highest reactivity toward Tc(VII), and reduced illite exhibited the least. The initial rate of Tc(VII) reduction, after normalization to clay and Fe(II) concentrations, was positively correlated with the percent smectite in the S-I series. Fe(II) in chlorite and palygorskite was also reactive toward Tc(VII) reduction. These data demonstrate that crystal chemical parameters (layer expandability, Fe and Fe(II) contents, and surface area etc.) play important roles in controlling the extent and rate of bioreduction and the reactivity toward Tc(VII) reduction. Reduced Tc(IV) resides within clay mineral matrix, and this association could minimize any potential of reoxidation over long term.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2019

Development of Alternative Vacuum Pumps for Tritium Service

In tritium process systems, vacuum pumps are typically used to evacuate volumes and piping, as well as transfer gas to other parts of the process. This was done using the combination of an all-metal scroll pump with a metal bellows backing pump. The all-metal scroll pump, manufactured by Normetex, has been unavailable since 2012, and efforts continue to find a suitable replacement. The main obstacle is finding a pump that has no oils or polymer components, which degrade when exposed to tritium and introduce corrosive and/or hazardous impurities into the process. Since turbomolecular pumps are used in tritium processing, it is thought that pumps similar to the turbomolecular pumps would be of interest. The pumps would need to operate at lower rotational speeds to handle higher pressures and flow rates, which is best suited for Molecular Drag Pumps (MDP). To determine this, the vacuum pump characteristics must be determined for the MDP. This report details pump characteristics using an MDP backed by a Metal Bellows (Met-Bel) pump under static and flow conditions for various gases.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

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 OSTI2024

Effect of Anoxic Iron Corrosion on WIPP Brine Geochemistry FY23 Final Report (U)

A 280-day study was completed to evaluate the effect of zero-valent iron (Fe 0 ) on the Waste Isolation Pilot Plant (WIPP) brine geochemistry under anticipated reducing conditions. Hydrogen (H 2 ) gas is expected to be present in the repository after closure due to the anoxic corrosion of a vast quantity of iron contained in the waste forms disposed at WIPP; therefore, a background argon atmosphere containing H 2 was chosen for this study. WIPP groundwater brine pH and E h will impact the mobility and fate of plutonium within the repository. Modeling and laboratory results for Castile WIPP brine indicate that equilibrium fa values relative to the standard hydrogen electrode (SHE) are 40 mV more reducing (i.e., more negative) than those for Salado WIPP brine (-480 mV vs. -440 mV, respectively) because of the higher pH of the Castile brine (pH 9 .3 for Castile vs. pH 8.8 for Salado). The E h and pH data were corrected for the effects of high ionic strength. The experimental results for both brines are consistent with thermodynamic predictions using OLI Systems' Mixed Solvent Electrolyte chemical equilibrium model. The measured and corrected pH and E h data from this study are provided in Table ES-I and Table ES-2, respectively. The experimental study, with four test conditions in triplicate, was performed in a dual glovebox with a nominally 3 vol.% H 2 in argon atmosphere (target H 2 range: 3 ± I vol.%). Simulants containing MgO only ( experimental control) and MgO+Fe 0 (WIPP base case) were prepared for both the Salado and Castile brines. MgO was included in all simulants to account for the use of bulk magnesium oxide in the WIPP repository. Fe 0 was included in some simulants to incorporate the effects of the anoxic corrosion of iron and in-situ hydrogen generation in the study. The brine compositions were developed by Sandia National Laboratory (SNL; Xiong, 2008) and have been used in previous WIPP evaluations. The test method (agitation, etc.) is partially based on ASTM D3987-12. Twelve rounds of periodic measurements of pH and E h were performed over the course of the study. Chemical analysis results for liquids and solids (ICP-MS, ICP-ES, IC Anion, TIC, SEM-EDX) are consistent with the pH, E h , and thermodynamic modeling results. This study included the following conditions that deviate from anticipated post-closure conditions following brine intrusion, but were selected to facilitate bench-scale testing to validate modeling of pH and E h for the post-closure WIP P repository: an anoxic glove box atmosphere containing ≤ 4 vol. % H 2 vs. substantially higher H 2 gas concentrations assumed in the WIPP Performance Assessment (PA); a significantly higher liquid-to-solid test ratio compared to the much lower phase ratio anticipated in the WIP P repository; agitation of the simulant bottles to maximize mass transfer; and finally the use of Fe 0 reagents having a much greater surface area than expected in the WIP P repository. Non-representative conditions were chosen for various reasons such as: to provide bounding conservative results, to provide a margin of safety for testing, or to facilitate simulant sub-sampling and analysis. In a parallel effort, aqueous electrolyte thermodynamic models were developed for the synthetic Salado and Castile brines to inform the experimental design, facilitate laboratory data interpretation, and allow extension of evaluations beyond the parameters tested. Thermodynamic modeling simulations including the MgO and Fe 0 additives that are directly relevant to the experimental measurements (e.g., pH calibration curve, ORP corrections) are included in this report. The measured fa of the simulants was close to the OLI model predictions for both brines and was largely controlled by the background H 2 partial pressure in the vapor phase as well as H 2 generated in situ in the aqueous phase by the Fe 0 corrosion. The H 2 gas-phase concentration tested and thermodynamically evaluated was much lower than is assumed in the WIPP PA; however, H 2 (g) concentrations significantly below this level are still predicted to result in very reducing conditions. In conclusion: • The experimental results are consistent with thermodynamic model predictions for fa, pH, and the effects of high ionic strength. • Evidence to date suggests that the H2 concentration in the glovebox atmosphere ultimately determined the final E h values of the simulants and resulted in highly reducing conditions. As a result, little difference was observed between the control simulants containing only MgO and the WIPP base-case simulants that contained MgO and Fe 0 . • This test methodology is recommended for future studies evaluating WIPP repository conditions. The methodology includes: (1) background H 2 in argon with agitation ( or could alternatively include in-situ-generated H 2 in sealed bottles); (2) carefully measured and corrected ORP data ( with much effort focused on allowing the probes to fully stabilize); and (3) ionic-strength-corrected pH data. Other best practices, such as simulant sparging/handling, ORP probe replacement, etc., should also be considered. • The coupling of experimental studies and thermodynamic modeling is also highly recommended because these methods inform and direct one another leading to greater confidence in and understanding of the results.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2015

Analysis of Tank 13H (HTF-13-14-156, 157) Surface and Subsurface Supernatant Samples in Support of Enrichment Control, Corrosion Control and Sodium Aluminosilicate Formation Potential Programs

The 2H Evaporator system includes mainly Tank 43H (feed tank) and Tank 38H (drop tank) with Tank 22H acting as the DWPF recycle receipt tank. The Tank 13H is being characterized to ensure that it can be transferred to the 2H evaporator. This report provides the results of analyses on Tanks 13H surface and subsurface supernatant liquid samples to ensure compliance with the Enrichment Control Program (ECP), the Corrosion Control Program and Sodium Aluminosilicate Formation Potential in the Evaporator. The U-235 mass divided by the total uranium averaged 0.00799 (0.799 % uranium enrichment) for both the surface and subsurface Tank 13H samples. This enrichment is slightly above the enrichment for Tanks 38H and 43H, where the enrichment normally ranges from 0.59 to 0.7 wt%. The U-235 concentration in Tank 13H samples ranged from 2.01E-02 to 2.63E-02 mg/L, while the U-238 concentration in Tank 13H ranged from 2.47E+00 to 3.21E+00 mg/L. Thus, the U-235/total uranium ratio is in line with the prior 2H-evaporator ECP samples. Measured sodium and silicon concentrations averaged, respectively, 2.46 M and 1.42E-04 M (3.98 mg/L) in the Tank 13H subsurface sample. The measured aluminum concentration in Tanks 13H subsurface samples averaged 2.01E-01 M.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2015

Quantity, Quality, and Availability of Waste Heat from United States Thermal Power Generation

Secondary application of unconverted heat produced during electric power generation has the potential to improve the life-cycle fuel efficiency of the electric power industry and the sectors it serves. Here this work quantifies the residual heat (also known as waste heat) generated by U.S. thermal power plants and assesses the intermittency and transport issues that must be considered when planning to utilize this heat. Combining Energy Information Administration plant-level data with literature-reported process efficiency data, we develop estimates of the unconverted heat flux from individual U.S. thermal power plants in 2012. Together these power plants discharged an estimated 18.9 billion GJ th of residual heat in 2012, 4% of which was discharged at temperatures greater than 90 °C. We also characterize the temperature, spatial distribution, and temporal availability of this residual heat at the plant level and model the implications for the technical and economic feasibility of its end use. Increased implementation of flue gas desulfurization technologies at coal-fired facilities and the higher quality heat generated in the exhaust of natural gas fuel cycles are expected to increase the availability of residual heat generated by 10.6% in 2040.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗