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DOE OSTI2020

At-source Recovery of Rare Earth Elements from Coal Mine Drainage

Conventional acid mine drainage (AMD) treatment consists of pH adjustment, oxidation, and separation of solid precipitates from discharge quality water. Alkaline addition increases the pH to the range 7 to 9 to precipitate the regulated metals Al and Mn ions as hydroxides. Mechanical or chemical oxidation then converts the reduced iron species Fe 2+ to Fe 3+ which precipitates at a low pH value as ferric hydroxide (Fe(OH) 3 ). Co-precipitation of Rare Earth Elements (REEs) with hydroxides creates a gangue-rich matrix from which REEs must be separated. Fe(OH)3 is generally the most abundant gangue-forming metal. Current research by the project team has shown raw, untreated AMD has an average total rare earth element content (TREE) of about 287 μg/L (0.287 ppm). Operators of AMD-producing facilities are obliged to treat it to neutralize acidity and remove regulated metals (e.g., iron (Fe), aluminum (Al), and manganese (Mn)) prior to discharge. Ongoing research indicates conventional AMD treatment concentrates TREE in resulting precipitates (AMD sludge) by an average factor of 2,635x to an average dry weight, elemental concentration of 708 g/t (ppm). While the economics of recovering REEs from AMD sludge are appealing, much of the cost of REE recovery would be incurred during separation of REEs from the gangue metals: Fe, Al, and Mn. Significant gains can be made by precipitating REEs when most of these gangue metals are still in solution. Significant improvements in REE extraction efficiency can be obtained through separation of REEs from the aqueous phase AMD, upstream of conventional AMD treatment by: 1) creating an enriched REE feedstock, 2) producing a more consistent feedstock, 3) reducing transportation costs to an REE refinery, 4) reducing acid consumption in the acid leaching step, and 5) reducing the volume of waste produced at the ALSX plant. This project is exploring two novel approaches for extracting REEs upstream of the conventional AMD treatment plants to create a purified REE feedstock while leaving the bulk of the Fe, Al, and Mn in solution for subsequent treatment. While the average TREE concentration of raw AMD is low and individual sites range between 10 and 2,200 μg/L, successful at-source REE separation will generate a superior feedstock to a conventional ALSX process and significantly improve the economics and environmental performance of REE extraction from AMD. AMD can be classified into two types: type A is net acid and iron is partly oxidized while type B is net alkaline, and iron occurs in the reduced, ferrous state. In Case A, the pH is raised slightly, which will precipitate Fe 3+ and Al 3+ but not REEs. The other important type of AMD is net alkaline water found in flooded, anoxic deep mines. These generally have a pH > 6.0 and are net alkaline. REE concentrations are also much lower than those found in acidic AMD while the volumes and flux are much higher. Most of these are pumped discharges with almost no Al. Case B AMD is strongly reduced and, like Case A water, Fe and Mn ions are similarly reduced and therefore soluble at pH <9.0. REEs and an array of transition ions will be the only trivalent cations in this type of AMD. In Case B, both upward pH adjustment under reducing conditions and application of an electrochemically stimulated supported liquid membrane strategy to separate REEs from ferrous ion will be explored.

01 COAL, LIGNITE, AND PEAT↗

DOE OSTI2020

Evaluation of Dose- and Risk-Based Groundwater Cleanup Levels for Low Energy Beta Radioisotopes

Low-energy beta-emitting radionuclides that were released historically during reactor operations and plutonium separations activities at some U.S. Department of Energy sites have migrated into the groundwater, forming contaminant plumes that are subject to federally regulated remediation actions. At the Hanford Site, the low-energy beta-emitting radionuclides include iodine-129, technetium-99, chlorine-36, carbon-14, and tritium (H-3). All are highly mobile in the subsurface, and except for tritium, and have very long half-lives—thousands to millions of years. The geochemistry and transport behavior of these contaminants in the subsurface present significant challenges for remediation of groundwater to federal drinking water standards (DWS)—the appropriate or relevant and applicable requirements (ARARs) for cleanup. For some of the low-energy beta-emitter contaminants, particularly iodine-129, cleanup and restoration of groundwater to DWS may not be attainable within a reasonable timeframe using currently available treatment technologies.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2021

ORNL Input to GDSA Repository Systems Analysis FY21

This document satisfies the M3 milestone M3SF-21OR010304082 titled “ORNL Input to GDSA Repository Systems.” This document describes the current status of Oak Ridge National Laboratory’s (ORNL’s) efforts related to analyses of dual-purpose canister (DPC) disposal in unsaturated alluvium with a focus on thermal hydrological constraints on criticality timing and power output. This analysis updates previous analyses of thermal hydrological constraints on timing and power output of a potential criticality event in Dual-Purpose Canisters (DPCs) in a hypothetical repository in unsaturated alluvium using a more realistic representation of heat transport inside dry DPCs. PFLOTRAN was used for the simulations of multiphase thermal hydrology near a single DPC. The scenario considers a DPC failure at 9000 years, allowing water to enter and eventually fill the DPC. Once the DPC is filled to a level that could support a criticality event, different values for criticality power output were added to the decay heat. The main objective is to bound the power output that could be produced by a criticality event without driving water out of the package. For the conditions analyzed here, following a package breach, the alluvial formation could supply enough water to allow enough accumulation in the DPC to support a criticality event. However, the power output that would be generated is limited to modest values by loss of water moderator due to evaporation and vapor diffusion. In the reference case scenario, the DPC would not start to fill with water until about 16,000 years post closure and would not fill to a level that allows a criticality event until approximately 25,000 years post closure. The long-term average power output that could be sustained without driving off the water and terminating the criticality event is limited to approximately 100 W. Sensitivity to assumed conditions and parameters in the reference case, especially the deep percolation rate, need to be addressed but could not be undertaken because of numerical failures of the PFLOTRAN code running in general mode in the dry conditions of an unsaturated alluvium repository

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2020

Epidemiological Investigation of a Mortality Event in a Translocated Gopher Tortoise (Gopherus polyphemus) Population in Northwest Florida

Nokuse Plantation, a 22,055 ha private conservation preserve in northwest Florida, is a recipient site for gopher tortoises translocated from development sites in Florida. Since 2006, Nokuse has received over 5,000 tortoises from multiple development sites. During 2013–2015, 52 tortoises were found sick (n = 14) or dead (n = 38) in multiple soft-release enclosures in which tortoises consistently exhibited clinical signs, with additional sick (n = 5) and dead (n = 5) tortoises presenting similarly during 2016–2017. When found alive, tortoises behaved abnormally (e.g., frequently out of burrows during cold weather, pacing along enclosure fencing), appeared emaciated, were lethargic, and had developed redness under plastron scutes. Similar numbers of male (n = 28) and female (n = 32) tortoises were recovered along with two of unidentified sex, including mainly adults (n = 59) and three subadults. Physical examination, blood analysis, and other diagnostics were indicative of starvation and dehydration. Most sick tortoises provided with supportive care recovered. Necropsy findings generally confirmed starvation, with no evidence of infectious pathogens or contaminants. There were no apparent differences in quality of habitat, plant community, or soil or water among affected and unaffected enclosures. Botanical surveys indicated adequate forage quality and quantity, with no poisonous exotic or native plants detected. No land management practices changed prior to this event. Analysis of epidemiological data and demographic factors from before and during this mortality event identified initial density of tortoises in the enclosures as exerting the strongest influence on detection of tortoise morbidity and mortality. We believe that the stress associated with mixing tortoises from different populations and at higher densities during translocation impacted an individual tortoise’s ability to obtain or absorb adequate nutrients from foraging, ultimately leading to a wasting condition consistent with starvation. Based on our findings, we recommend a maximum of 3 gopher tortoises per ha in soft-release enclosures for translocation, but further research is warranted to investigate the complexity of stress and social pressures associated with translocation.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2020

Acceleration of Glass Alteration Rates Induced by Zeolite Seeds at Controlled pH

As the glass-water reaction proceeds, certain glass compositions undergo a delayed acceleration in the alteration rate – a phenomenon that is commonly referred to as Stage III behavior – which generally coincides with zeolite formation. However, studying Stage III in the laboratory is difficult because the time scale required to observe Stage III behavior can vary from months to several years, and the solution conditions that initiate this acceleration remain poorly understood. Consequently, the development of a corrosion test method capable of quantifying Stage III rates in a timely manner would be of great benefit to both the scientific community and policy makers concerned with nuclear waste disposal. In this work, we induced and measured the acceleration in the corrosion rate of the AFCI glass by seeding static corrosion tests with zeolite Na-P2 at fixed pH90°C values ranging from 9.5 to 11.5. The induced Stage III rates increased linearly with increasing pH and were measured to be between the forward and residual rates of AFCI. Tests designed to compare induced Stage III rates obtained for different seeding times showed that the induced Stage III rates were faster in the absence of an alteration layer. In summary, the use of the seeded test method allows for a conservative quantification of Stage III rates in a relatively short, one-month time period.

Neeway, James J.↗

DOE OSTI2024

Sustainable Aviation Fuels from 30,000 feet – Scoping Report

A literature review, first principles analysis, and mapping of the airline-fuel infrastructure were performed to reassess the potential for various means of realizing a sustainable aviation sector. The literature review found a plethora of technical methods to make the airline industry net-zero CO 2 but limited work on the emergent barriers to sustainable aviation implementation such as land use, repurposing of fuel refining assets, and airline cost structures. First principles analyses of the energy, land, and costs of three broad net-zero strategies were performed to determine if sustainable aviation is feasible even in the most optimistic scenarios. Those methods were biomass-derived sustainable aviation fuel (SAF), fuel produced from CO 2 captured from the air and H 2 produced from water electrolysis (air-to-fuel: ATF), and offsetting fossil-derived Jet Fuel with carbon dioxide removal from the atmosphere (direct air capture and storage: DACS). Offsetting CO 2 emissions from using fossil Jet Fuel with DACS was found to consume the least energy, require the smallest quantity of land, and be the cheapest option. Replacing Jet Fuel with SAF was found to be only slightly more expensive than DACS but require substantially more land. ATF was found to be the most expensive and energy intensive option, though it did spare land relative to SAF. We found that calls to utilize waste biomass are well-founded, but wastes alone cannot cover the needs of the global airline industry. This means additional land will need to be allocated for biomass cultivation if SAF becomes the primary pathway to sustainable aviation. While differences were found in the performance of different types of biomass, those differences were small relative to differences with ATF and DACS. An analysis of the pricing structure of the airline industry suggests that some of the cost advantage of DACS may be erased by consumer sentiment which could explain why, to-date, the airline industry is focused primarily on SAF and to a lesser extent ATF. Further work is required to estimate the transportation, capital cost, and financing cost implications of greenfield and brownfield sites for SAF, DACS, and ATF. In the final report, we will analyze the potential to retrofit corn ethanol facilities to operate the ethanol-to-jet fuel process in response to decreasing gasoline demand as the electrification of road transport progresses. We will also construct a prioritization of land use to determine whether each net-zero CO 2 aviation pathway can make claim to the land required by their technology.

09 BIOMASS FUELS↗

DOE OSTI2024

Characterization of Nitrate, Nitrite, Ammonia, and Tritium in D0220 Cores

This report describes characterization of nitrogen species (nitrate, nitrite, ammonia) in aqueous and solid phases in cores taken in borehole D0220 (well 299-E25-245) under crib 216-A-37-1 at the Hanford Site in 2022 to evaluate (a) the types of nitrogen species currently in the vadose zone and (b) the migration of nitrogen species in the vadose zone. Ammonia and tritium from PUREX decladding condensate were sporadically discharged to the crib from 1977 to 1989. During discharge operations, the estimated travel time through the vadose zone to groundwater was 2.5 to 9 months. By 2003, a characterization borehole (C4106) showed residual pore water with elevated tritium and nitrate in the first 100 ft of the vadose zone, which is likely from the crib. However, there was significantly more nitrate present at the shallowest depth (15 to 22 ft), which may indicate a different source for nitrate, such as adsorbed ammonia slowly being oxidized or nitrogen species precipitates slowly dissolving. In this study, more extensive nitrogen species characterization was done on D0220 cores (drilled in 2022) at 40- and 262-ft depths, which included (a) aqueous nitrate, nitrite, and tritium; (b) adsorbed ammonia; (c) nitrogen in carbonates (or other minerals dissolved in acidic acid); (d) nitrogen in iron oxides (or other minerals dissolved in oxalic acid); and (e) nitrogen in hard-to-extract minerals (minerals dissolved in nitric acid). High pore water nitrate (226 to 331 mg/L) at 40-ft depth measured in D0220 (2022) compared to 60 mg/L at 40-ft depth in C4106 (2003) may indicate nitrate is migrating deeper. Tritium concentrations (pore water 132,000 to 148,000 pCi/L) measured in D0220 at 40-ft depth in 2022 were considerably higher than in C4106 at 40-ft depth (160 pCi/L). Additional nitrogen species mass was present in adsorbed and precipitated phases in D0220 cores. Low adsorbed ammonia was measured at 40.1- and 261.7-ft depths. Low concentrations of carbonate associated nitrogen and iron oxide-associated nitrogen were present at 40.1 and 40.6 ft depths. Nitrogen species in solid phase extractions indicate nitrogen precipitates or aqueous nitrate or ammonia trapped in sediment microfractures that are coated by precipitates. Overall, the nitrogen species and tritium characterization at two depths in D0220 showed that additional nitrogen species were present in the vadose zone. In addition, elevated pore water nitrate in D0220 at 40 ft depth from 2022 may indicate vertical migration compared to C4106 nitrate profile from 2003. Analysis of additional depths in D0220 and spatial variability of the nitrate plume along the length of the crib (from surface electrical resistivity) would be extremely useful for this comparison.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2023

Biomethanation to Upgrade Biogas to Pipeline Grade Methane

NREL is working closely with DOE, Electrochaea GmbH, and Southern California Gas Company (SoCalGas) to reduce costs of a biomethanation process capable of megawatt-scale deployment that upgrades organic biogas waste streams to produce pipeline quality renewable natural gas (RNG). Biomethanation is a two-step process using a single-celled methanogenic archaea that converts low-carbon low-cost hydrogen (H2) and waste carbon dioxide (CO2) to produce renewable methane (CH4). The process upgrades the biogenic CO2 - while allowing the CH4 to pass through - from biogas sources like dairies, wastewater treatment plants, and landfills. The CH4 produced is a drop-in direct replacement fuel and producers can participate in the growing number of carbon markets; like California's Low Carbon Fuel Standard and the Federal Renewable Fuel Standard. NREL and Argonne National Laboratory have completed a life cycle analysis using the GREET model to show that the biomethanation process produces RNG that is carbon negative even when H2 production via low-temperature water electrolysis is driven by the existing carbon intensity of California's electricity grid. And of course, even further carbon negative (-233 kg CO2e/kWh) when the electricity is produced from low-carbon sources like wind and solar. Leveraging lessons learned from operating SoCalGas' 700L 18-bar bioreactor system, NREL is designing and building a flexible RD&D platform that will enable field trials at biogas and other CO2 sources. A custom 16' long trailer will house a 20L 18-bar bioreactor, 3 - 25 kW proton exchange membrane electrolyzer, and dosing, thermal, and controls systems to support operations with only power, biogas, and water feedstocks required by the field locations. The end-of-project goal is to demonstrate pipeline quality RNG production (> 95% CH4, < 4% H2, <1% CO2, < 0.2% O2 and < 4 parts per million H2 sulfide) using real biogas feedstocks - thereby recycling both greenhouse gases for injection into the natural gas network or to be used onsite.

biogas upgrading↗

DOE OSTI2023

Aqueous buffer solution-induced crystallization competes with enzymatic depolymerization of pre-treated post-consumer poly (ethylene terephthalate) waste

In this paper, the complex relationship between kinetics and substrate morphology during enzymatic depolymerization of melt processed poly(ethylene terephthalate) (PET) is explored and the effects of competing transformations are analyzed. Extruded PET substrates from post-consumer recycled PET (RPET) bottles flakes subjected to enzymatic depolymerization are examined to reveal increases in crystallinity from ~10% post-extrusion to >30% after 3 days of depolymerization as well as increases in glass transition temperature (T g ) from ~66°C to > 80°C. Further investigation into this behavior shows that post-extrusion RPET substrates do not exhibit changes in crystallinity when subjected to dry annealing at 65°C in an oven over 7 days, but they do experience annealing in depolymerization buffer solution with no enzymes at 65°C within 3 days. This difference may be attributed to plasticization of PET in the presence of water, also known as solvent induced crystallization. The impact of this plasticized annealing behavior is demonstrated by subjecting RPET substrates to increasing enzyme-to-substrate loads. As enzyme load increases, overall conversion of substrates increases despite crystallinity also increasing to similar levels regardless of the initial enzyme loading. The competition between depolymerization and crystallization suggests that the rate at which PET substrates are depolymerized at the operational temperature is integral to achieving high conversion to monomeric product. This, in turn, also suggests that savings from lowered enzyme loadings may be more detrimental than helpful in pursuing the most cost-effective recycling systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Effects of sodium and calcium chloride ionic stresses on model yeast membranes revealed by molecular dynamics simulation

As efforts to move a renewable economy grow, it will be necessary to make use of microbial conversion strategies for the production of novel materials or the upgrading of waste to high-value products. One critical technical challenge currently limiting waste upgrading remains the difficulty in obtaining single-pot conversion techniques where physical, chemical, and biological conversion are performed in a single step. To overcome this challenge, a detailed understanding of how different stresses impact microbial membrane stability will be necessary. In this work, using all-atom molecular dynamics simulations, we examine the impacts of moderate concentrations of NaCl and CaCl 2 on a model yeast plasma membrane. Weak, though statistically significant, changes in membrane morphology and dynamics functions are observed that are consistent with swelling and stiffening. Additionally, an examination of the ion-lipid contacts and the behavior of water at the water-membrane interface suggests that the impacts of these common salts may, in part, be mediated through changes to water-membrane hydrogen-bonding and hydration water dynamics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

State-of-the-Art Organic- and Inorganic-Based Hollow Fiber Membranes in Liquid and Gas Applications: Looking Back and Beyond

The aggravation of environmental problems such as water scarcity and air pollution has called upon the need for a sustainable solution globally. Membrane technology, owing to its simplicity, sustainability, and cost-effectiveness, has emerged as one of the favorable technologies for water and air purification. Among all of the membrane configurations, hollow fiber membranes hold promise due to their outstanding packing density and ease of module assembly. Herein, this review systematically outlines the fundamentals of hollow fiber membranes, which comprise the structural analyses and phase inversion mechanism. Furthermore, illustrations of the latest advances in the fabrication of organic, inorganic, and composite hollow fiber membranes are presented. Key findings on the utilization of hollow fiber membranes in microfiltration (MF), nanofiltration (NF), reverse osmosis (RO), forward osmosis (FO), pervaporation, gas and vapor separation, membrane distillation, and membrane contactor are also reported. Moreover, the applications in nuclear waste treatment and biomedical fields such as hemodialysis and drug delivery are emphasized. Subsequently, the emerging R&D areas, precisely on green fabrication and modification techniques as well as sustainable materials for hollow fiber membranes, are highlighted. Last but not least, this review offers invigorating perspectives on the future directions for the design of next-generation hollow fiber membranes for various applications. As such, the comprehensive and critical insights gained in this review are anticipated to provide a new research doorway to stimulate the future development and optimization of hollow fiber membranes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Direct Extraction of Uranium Oxides with N,N -Di(2-ethylhexyl)isobutyramide

The direct extraction of uranium from voloxidized nuclear fuel into an organic solvent offers several potential advantages over conventional hydrometallurgical reprocessing, including reducing the reprocessing plant footprint, providing an initial degree of decontamination from fission products, and minimizing the amount of secondary waste from nitric acid. In this work, the direct extraction of uranium oxides into 1.5 M N,N-di(2-ethylhexyl)isobutyramide (DEHiBA) in n-dodecane is examined. UV–vis spectra and distribution ratios of HNO 2 in 1.5 M DEHiBA as well as the equilibrium organic phase H 2 O concentrations in HNO 3 -loaded 1.5 M DEHiBA are also reported. Hypothesized reaction stoichiometries for the direct extraction of uranium from UO 2 , α-U 3 O 8 , and ε-UO 3 are verified through analysis of organic-phase U, HNO 2 , and HNO 3 concentrations after dissolution. Water generated by the dissolution results in the formation of a separate aqueous phase, which will need to be accounted for in future flowsheet design.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI1994

Nuclear Safety [Vol. 35, No. 2, July-December 1994]

Nuclear Safety is a journal that covers significant issues in the field of nuclear safety. Its primary scope is safety in the design, construction, operation, and decommissioning of nuclear power reactors worldwide and the research and analysis activities that promote this goal, but it also encompasses the safety aspects of the entire nuclear fuel cycle, including fuel fabrication, spent-fuel processing and handling, and nuclear waste disposal, the handling of fissionable materials and radioisotopes, and the environmental effects of all these activities. Table of Contents for this issue follows. GENERAL SAFETY CONSIDERATIONS: 179 Consideration of Postaccident Consequences in the Determination of Safety Objectives for Future Nuclear Power Plants in France, D. Queniart, A. Sugier, and J. Lochard; ACCIDENT ANALYSIS: 187 Nuclear Safety Research: The Phebus FP Severe Accident Experimental Program, P. von der Hardt, A. V. Jones, C. Lecomte, and A. Tattegrain; 205 Containment Performance Analysis of the Advanced Neutron Source Reactor at the Oak Ridge National Laboratory, S. H. Kim, R. P. Taleyarkhan, and V. Georgevich; 213 Assessment of Fission Product Deposits in the Reactor Coolant System: The DEVAP Program, G. Le Marois and M. Megnin; 222 Erratum to “A Review of the Available Information on the Triggering Stage of a Steam Explosion," Vol. 35, No. 1, CONTROL AND INSTRUMENTATION: 223 Effects of Normal Aging on Calibration and Response Time of Nuclear Plant Resistance Temperature Detectors and Pressure Sensors, H. M. Hashemian; DESIGN FEATURES: 235 Defense in Depth Against the Hydrogen Risk—A European Research Program, F. Fineschi; ENVIRONMENTAL EFFECTS: 246 Technical Note: A Preliminary Analysis of the Risks to Hong Kong Resulting from Potential Accidents of Daya Bay Nuclear Power Plant, Z. Shi and X. Wei; OPERATING EXPERIENCES: 253 Reactor Shutdown Experience, Compiled by J. W. Cletcher; SPECIAL SECTION ON TMI-2 VESSEL INVESTIGATION PROJECT: 256 Three Mile Island—New Findings 15 Years After the Accident A. M. Rubin and E. Beckjord; 269 Relocation of Molten Material to the TMI-2 Lower Head, J. R. Wolf, D. W. Akers, and L. A. Neimark; 280 Insight Into the TMI-2 Core Material Relocation Through Examination of Instrument Tube Nozzles, L. A. Neimark; 288 Physical and Radiochemical Examinations of Debris from the TMI-2 Lower Head, D. W. Akers and B. K. Schuetz; 301 Results of Metallographic Examinations and Mechanical Tests of Pressure Vessel Samples from the TMI-2 Lower Head, D. R. Diercks and G. E. Korth; 313 Margin-to-Failure Calculations for the TMI-2 Vessel, J. Rempe, L. Stickler, S. Chavez, G. Thinnes, R. Witt, and M. Corradini; U.S. NUCLEAR REGULATORY COMMISSION INFORMATION AND ANALYSES: 328 1993 Accident Sequence Precursor (ASP) Program Results, L. N. Vanden Heuvel, J. W. Cletcher, D. A. Copinger, J. W. Minarick, B. W. Dolan, and P. D. O’Reilley; RECENT DEVELOPMENTS: 339 Reports, Standards, and Safety Guides, D. S. Queener; 345 Proposed Rule Changes as of June 30, 1994; ANNOUNCEMENTS: 234 Thirty-First Annual Meeting of the National Council on Radiation Protection and Measurements; 356 1995 International Incineration Conference; 358 Fifth International Controls and Instrumentation Conference; 359 ANS International Topical Meeting on Safety of Operating Reactors; 359 Fifth International Conference on Nuclear Criticality Safety; 360 International Conference on Probabilistic Safety Assessment Methodology and Applications; 351 The Authors; 357 Reviewers of Nuclear Safety, Vol. 35.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2023

Ammonia Electrosynthesis from Nitrate Using a Ruthenium–Copper Cocatalyst System: A Full Concentration Range Study

Electrochemical synthesis of ammonia via the nitrate reduction reaction (NO3RR) has been intensively researched as an alternative to the traditional Haber–Bosch process. Most research focuses on the low concentration range representative of the nitrate level in wastewater, leaving the high concentration range, which exists in nuclear and fertilizer wastes, unexplored. The use of a concentrated electrolyte (≥1 M) for higher rate production is hampered by poor hydrogen transfer kinetics. Herein, we demonstrate that a cocatalytic system of Ru/Cu 2 O catalyst enables NO3RR at 10.0 A in 1 M nitrate electrolyte in a 16 cm 2 flow electrolyzer, with 100% faradaic efficiency toward ammonia. Detailed mechanistic studies by deuterium labeling and operando Fourier transform infrared (FTIR) spectroscopy allow us to probe the hydrogen transfer rate and intermediate species on Ru/Cu 2 O. Ab initio molecular dynamics (AIMD) simulations reveal that adsorbed hydroxide on Ru nanoparticles increases the density of the hydrogen-bonded water network near the Cu 2 O surface, which promotes the hydrogen transfer rate. Finally, our work highlights the importance of engineering synergistic interactions in cocatalysts for addressing the kinetic bottleneck in electrosynthesis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

MODELING A SPENT NUCLEAR FUEL CASK SEISMIC TEST

The US Department of Energy Spent Fuel and Waste Science and Technology (SFWST) program is planning to conduct a series of full-scale shake table tests to simulate hypothetical earthquake conditions and record the response of surrogate spent nuclear fuel (SNF) assemblies in a canister dry storage system mockup. The shake table motions will represent a range of hypothetical earthquake conditions at hypothetical locations in the continental US to generally define the range of mechanical loads that SNF can be expected to experience during extended dry storage periods. The earthquake conditions will represent seismic hazards in the 2,000-to-20,000-year return period range. The test will use instrumented pressurized water reactor fuel assemblies with surrogate mass inside the fuel rods instead of radioactive fuel pellets. Dummy assemblies with similar mass and dimensions to actual fuel assemblies will occupy the rest of the fuel assembly locations in a SNF canister that holds 32 fuel assemblies. The canister will be located inside a mockup vertical concrete cask. Instrumentation will record the motion of the major components of the complex dynamic system, and strain gauges will be used to record the cladding strain at select locations. Preparations for the test require modeling predictions to identify the range of response of the system and to help select specific earthquake cases to be simulated on the shake table from a large set of potential cases. This paper describes the pretest nonlinear finite element modeling efforts that have been completed to date, including cask system level modeling and fuel assembly modeling in LS-DYNA. The cask system level models are critical for anticipating sliding or tipping of an unanchored cask during the test. The fuel assembly model is needed to estimate the range of cladding strain response and fuel assembly structural response to be expected during the test and cladding strain measurements will be key metrics for model validation and the development of modeling best practices after the test is concluded.

Klymyshyn, Nicholas A.↗

DOE OSTI2021

Aquifer Injection Modeling (AIM) Toolbox User Guide

The Aquifer Injection Modeling Toolbox (“AIM Toolbox”) software was developed by the Pacific Northwest National Laboratory (PNNL) for the U.S. Environmental Protection Agency’s (EPA) to provide a collection of analytical solutions suitable for evaluating the potential extent of the area impacted by subsurface injection operations. Subsurface injection operations are regulated under the EPA’s Underground Injection Control (UIC) program and are typically related to oil/gas development, waste disposal, or subsurface mining or storage. The analytical algorithms provided in the AIM Toolbox each have different approaches/assumptions/focus with respect to the nature and processes in subsurface and the nature of the injection operations. Collectively the set of analysis algorithms provides a broader evaluation of the area that can potentially be impacted by an injection operation. By providing estimates for the injectate plume extent, the software supports technical aspects of planning, evaluation, and overseeing injection activities. That is, the results help assess when further regulatory controls (e.g., monitoring, reporting) may be required and, in the case of disposal into an underground source of drinking water, the extent of the impacted area would require exemption from protection under the Safe Drinking Water Act. The AIM Toolbox software is available as a single-page web application, providing an interface to provide the necessary inputs, and both chart and map panes for visualizing the results. This User Guide describes the AIM Toolbox software, information required, user interactions, and the underlying basis of the calculations.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Aquifer Injection Modeling (AIM) Toolbox User Guide

58 GEOSCIENCES↗

DOE OSTI2023

Tailoring biogenic straw insulation from additive manufacturing

In the pursuit of carbon-storing materials that could help accomplish high levels of building sustainability, wheat straw has emerged as a promising alternative to fossil fuel-based building materials. Straw is 100% biodegradable and abundant agricultural waste used in the construction 400 years ago, and it has been reported to have the lowest embodied carbon when measured against other typical insulating materials. Here, in this study, we report additive manufacturing of carbon-sequestration insulation panel materials by upcycling cellulose fibrils from wheat straw. Cellulose obtained from alkaline and 2,2,6,6-tetramethylpiperidine-1-oxyl radical-mediated oxidation shows thermal conductivity of 0.036 W m -1 K -1 , alongside elastic and flexural modulus of 900 MPa and 502 MPa, respectively. In addition, an in-situ hydrophobic treatment in the cellulose-based insulation panels is achieved with an average water contact angle of 133.7° Furthermore, the extrusion-based additive manufacturing of a 3D-printable ink obtained by mixing the cellulose and silica aerogel precursor is accomplished, with the printed material exhibiting structural integrity, thus showing great potential towards the development of state-of-the-art, sustainable materials for carbon-sequestration building applications.

36 MATERIALS SCIENCE↗