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DOE OSTI2024

Evaluating Liquid Waste Transfers and their Impacts to the SRS Tank Farm to Support Operations and Closure

The Liquid Waste (LW) contractor at the Savannah River Site, Savannah River Mission Completion (SRMC), supports the storage, processing, and safe disposition of legacy, radioactive liquid waste. The LW Tank Farms contain approximately 127 million liters (33.5 million gallons) of liquid waste within 43 active, underground waste tanks. To meet mission critical milestones for the closure of waste tanks and processing of 34 million liters (9 million gallons) of salt waste per year by the LW Salt Waste Processing Facility (SWPF), an increase in Tank Farm operations, including waste tank transfers, is required. Waste is compiled in salt and sludge batches in the Tank Farms and transferred to SWPF and the Defense Waste Processing Facility (DWPF) for treatment. All waste tank transfers, such as waste removal and batch compilation transfers, must be pre-evaluated to ensure Documented Safety Analysis (DSA) requirements are met via Evaluated Transfer Approval Forms (ETAFs). Facility conditions and configurations may change as a result of a waste transfer. These changes must be reflected in the Tank Farms Emergency Response Datasheet (ERD), which contains data utilized for operation and emergency situations.

Peterson, Shelby R.↗

DOE OSTI2021

Proton Nuclear Magnetic Resonance (H NMR) of Glycolate in Real Waste: Developing and Testing Analytical Methods for the Savannah River Site Liquid Waste System

In preparation for implementing the NG acid flowsheet for the SRS LWS, analytical methods for determining glycolate at low concentration are desired to support system management and safety. Previous work documented that the IC method performed well for samples with low to moderate ionic strength. That work also included a scoping effort to determine if an alternate analytical strategy using H NMR would complement and extend the capabilities of the IC method. The H NMR scoping results indicated that the method had the potential to expand glycolate analysis in LWS samples to higher ionic strength tanks/solutions. The scope of this work is to develop innovative proton NMR techniques, including demonstrating ion exchange decontamination protocols needed for application of the technique to real waste samples. Part of radioactive waste processing at SRS uses formic acid to reduce oxidized (Hg 2+ ) to more volatile elemental Hg for steam striping, collecting, and disposal. Under acidic conditions found in the Chemical Processing Cell (CPC) at the Defense Waste Processing Facility (DWPF), formic acid has a much higher hydrogen generation rate than an alternative reductant, glycolic acid. Thus, an NG acid flowsheet has been developed utilizing glycolic acid with the benefit of easing the need for headspace monitoring requirements for hydrogen and ammonia at DWPF. Low concentrations of glycolate are conservatively assumed to be in the recycle stream, which will collect in the Recycle Collection Tank (RCT). The DWPF recycle stream collected in the RCT has a distinct pathway to the LWS waste tanks that feed the 2H and 3H Evaporator. This route involves transfer of the DWPF recycle to Tank 22 in the Concentration, Storage, and Transfer Facilities (CSTF) followed by transfer to the LWS tank farm/evaporators.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2019

Advanced Fuels Campaign 2019 Accomplishments

The mission of the Advanced Fuels Campaign (AFC) is to perform or support research, development, and demonstration (RD&D) activities to identify and mature innovative fuels and cladding materials and associated technologies with the potential to improve the performance and safety of current and future reactors; increase the efficient utilization of nuclear energy resources; contribute to enhancing proliferation resistance of the nuclear fuel cycle; and address challenges related to waste management and ultimate disposal. AFC pursues its mission objectives using a goal-oriented, science-based approach that seeks to establish a fundamental understanding of fuel and cladding behaviors under conditions that arise during fabrication, normal steady-state irradiation, off-normal transient scenarios, and storage/disposal. This approach includes advancing the theoretical understanding of fuel behavior, conducting fundamental and integral experiments, and supporting the mechanistic, multi-scale modeling of nuclear fuels to inform and guide fuel development projects, advance the technological readiness of promising fuel candidates, and ultimately support fuel qualification and licensing initiatives. In the area of advanced tools for the modeling and simulation of nuclear fuels, the AFC works in close partnership with the Nuclear Energy Advanced Modeling and Simulation (NEAMS) program, participating with NEAMS in developing mechanistic fuel behavior models and providing experimental data to inform and validate its most advanced tools. Specifically, AFC objectives in thecoming five year horizon include: 1. support the industry-led development of Accident Tolerant Fuel (ATF) technologies with improved reliability and performance under normal operations and enhanced tolerance during hypothetical accident scenarios, with implementation of lead test rods/assemblies of one or more ATF concepts in commercial reactor(s) by or before 2022 and batch reloads of near-term concept(s) in the 2023-2026 timeframe; 2. lead research and development on innovative fuel and cladding technologies for applications to future advanced reactors, especially fast-spectrum reactors, including reactors that utilize both once-through and recycle scenarios; 3. continue the development and demonstration of a multi-scale,science-based approach to fuel development and testing, andcontribute to the establishment of a state-of-the-art R&D infrastructure necessary to accelerate the development of new fuel concepts; and collaborate with NEAMS on the development and validation of multi-scale, multi-physics, and increasingly predictive fuel performance models and codes. 4. collaborate with NEAMS on the development and validation of multi-scale, multi-physics, and increasingly predictive fuel performance models and codes.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2023

A decision support tool for e-waste recycling operations using the hen-and-chicks bio-inspired optimization metaheuristic

E-waste from end-of-life electrical and electronic devices is one of the fastest growing waste streams from households and businesses. E-waste recycling yields environmental sustainability and economic benefits. Due to continuous changes in e-waste types and compositions, recycling businesses face challenges to optimize their operational configuration to achieve better economic and environmental performance. To help e-waste recyclers mitigate this problem, we have developed a modular decision support tool called the Comprehensive Manufacturing Assessment Tool (CMAT) that can simulate both e-waste recycling operations and economics. This tool can give valuable insights regarding the profitability of the entire operation and different e-waste types. In addition, a new bio-inspired metaheuristic optimization algorithm, hen-and-chicks optimization (HACO), was developed to assign manpower to different workstations to maximize operational efficiencies. According to the results of our case study, laptops, desktops, and computer peripherals are the three electronic waste products that produce the most profit. Our examination of the sensitivity of material prices shows that the price of steel has the most significant influence on total profit, because it is the most widely used material in the majority of electronic devices. We have released the decision support tool as open-source software under a general public license. It could be customized for other recycling industries beyond e-waste to achieve business sustainability by making their operations more efficient.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

DOE OSTI2021

Additively Manufactured Solid-State Luminaire

This project addresses several key barriers to wide-spread adoption of additive manufacturing (AM) technology as applied to solid state lighting luminaires. The solution will utilize cutting edge AM approaches for integrating structure with thermal management solutions, electronic functionality, and optics. The research team (Eaton, Lighting Research Center (LRC) at Rensselaer Polytechnic Institute, Xerox Research Centre of Canada (XRCC)) utilize their AM and lighting expertise to investigate breakthrough manufacturing approaches that will significantly reduce cost, eliminate manufacturing process waste, and improve luminaire efficacy. The team has identified critical areas of research and proposed novel technical approaches to achieve these goals. Key areas of focus in Budget Period 1 (BP1) of the project quantified the impact of applying AM methodologies to the main, discrete subsystem components (Heat Sink, Housing, Optics, Electronics). Budget Period 2 (BP2) research explored similar impact on a fully integrated, AM modular luminaire concept. Final Achievement of the Target Metrics for the project are as follows: Material Reduction: achieved > 57.45% (target is 50%) Manufacturing Process: achieved > 51% reduction (target is 50%) Application Efficacy: achieved 126 lm/W (target is 130 lm/W) First Cost vs Baseline: demonstrated 49% improvement in project timing, 59% improvement in man hour savings and 89% worse BOM costs (due to deficiencies in current “state of the art” equipment). The BOM costs improve to 53% savings if state of the art processes and equipment could have been used.

3D Printing↗

DOE OSTI2022

Hanford Site Composite Analysis Special Analysis: P2R Model Predictive Contaminant Transport Simulations - Sensitivity Case

This environmental calculation file (ECF) documents the methodologies, assumptions, and results of predictive fate and transport simulations using the Plateau-to-River (P2R) model. This ECF supports the reevaluation of the representativeness of solid-waste radionuclide inventory and release rate from three solid waste sites included in the recently completed Hanford Site Composite Analysis (CA) (DOE-RL-2019-52, Composite Analysis for Low-Level Waste Disposal in the Hanford Site Central Plateau (FY 2020)). Specifically, this ECF supports the reevaluation of the representativeness of the base case inventory and radionuclide waste release rates from three solid waste sites (i.e., 218-E-12B, 218-W-3A and 218-W-3AE) and two radionuclides (carbon-14 [C-14] and technetium [Tc-99]). These three waste sites and two radionuclides were identified as being the most significant contributors to groundwater contamination and dose in the CA at time periods after the compliance period. The release rates and footprints of the releases from the vadose zone are implemented in the fate and transport modeling utilizing the HSS package.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2020

Reduced Neutralization Feasibility Study for H-Canyon Accelerated Basin De- Inventory (ABD) Program

An alternative approach to Spent Nuclear Fuel (SNF) and Nuclear Material Processing was developed for future H-Canyon (HCAN) and L-Area operations that involves a paradigm shift from current HCAN, Concentrate, Storage, and Transfer Facility (CSTF), and Defense Waste Processing Facility (DWPF) operations. The alternative, referred to as Accelerated Basin De-inventory (ABD), requires that all Domestic and Foreign Research Reactor SNF currently at the Savannah River Site (SRS) will be dissolved, stored, and then transferred to CSTF without recovery of Highly Enriched Uranium (HEU). Concentrated nitric acid is utilized to dissolve aluminum spent nuclear fuel (ASNF) in HCAN. The vessels and piping in HCAN are fabricated from 304L stainless steel and are ideally suited to handle the acidic waste stream. However, as the waste is transferred to the CSTF and DWPF, it will contact the carbon steel waste tanks in CSTF. In order to prevent corrosion of the carbon steel, the acidic waste is neutralized (i.e., pH adjusted over 11) by the addition of sodium hydroxide (NaOH). The NaOH is added until the final solution contains 1.2 M excess -OH. Additionally, if the waste is not neutralized to a pH greater than 11, then aluminum hydroxide (Al(OH) 3 ) would form, and solids may form in the piping as it is transferred to CSTF. This document presents an analysis of the influence of reducing the excess caustic that is added to the neutralization tanks on the corrosion protection scheme primarily for the CSTF waste tanks. The implications to HCAN and DWPF were also assessed.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2023

Advanced biorefinery feedstock from non-recyclable municipal solid waste by mechanical preprocessing

Because of accelerated urbanization and the development of a global economy, a large quantity of municipal solid waste (MSW) has been collected and disposed of by the municipalities. Due to this drastic increase in the disposal of MSW, the need for its management is a must to preserve the environment. Currently, approximately 50% of the total MSW generated in the United States has been utilized through various recycling, combustion, and composting technologies, which means the remaining 50% is sent to landfill; this is often known as non-recyclable MSW (nMSW). As this nMSW is physically and chemically heterogenous and contains very high amounts of inorganic material, processing is required prior to using it as a biorefinery feedstock. Thus, this study focused on how mechanical preprocessing advanced the physical and chemical properties of nMSW. The physical and chemical properties were investigated in terms of particle size distribution, bulk density, ultimate and proximate analysis, and the higher heating value (HHV). The combustion properties were examined in terms of ignition temperature, peak heat release rate, and combustion efficiency. Results showed that the variability of physical and chemical properties of nMSW can be reduced by mechanical preprocessing. For example, the variability of the bulk density of the as-received nMSW was approximately 17.3% while it reduced to 5.8% when the sample size was reduced to 2 mm. Similarly, the variability of ash and HHV reduced from 49.2% to 11.0% and 13.4%–4.2%, respectively. Combustion thermograms showed that the size reduction positively improved the combustion properties. For example, 2 mm of spec sample started to ignite approximately 4 times earlier and took 6.5 folds less time to reach the peak heating rate compared to as-received nMSW. Overall, the mechanical preprocessing reduced the variability of physical and chemical properties in addition to the improvement of combustion behavior of the nMSW which is one step forward toward the biorefinery feedstock.

09 BIOMASS FUELS↗

DOE OSTI2021

Synthetic Methanol/Fischer–Tropsch Fuel Production Capacity, Cost, and Carbon Intensity Utilizing CO 2 from Industrial and Power Plants in the United States

Captured CO 2 is a potential feedstock to produce fuel/chemicals using renewable electricity as the energy source. In this study, we explored resource availability and synergies by region in the United States and conducted cost and environmental analysis to identify unique opportunities in each region to inform possible regional and national actions for carbon capture and utilization development. This study estimated production cost of synthetic methanol and Fischer–Tropsch (FT) fuels by using CO 2 captured from the waste streams emitted from six industrial [ethanol, ammonia, natural gas (NG) processing, hydrogen, cement, and iron/steel production plants] and two power generation (coal and NG) processes across the United States. The results showed that a total of 1594 million metric ton per year of waste CO 2 can be captured and converted into 85 and 319 billion gallons of FT fuels and methanol, respectively. FT fuels can potentially substitute for 36% of the total petroleum fuels used in the transportation sector in 2018. Technoeconomic analysis shows that the minimum selling prices for synthetic FT fuels and methanol are 1.8–2.8 times the price of petroleum fuel/chemicals, but the total CO 2 reduction potential is 935–1777 MMT/year.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Development of PFLOTRAN Transport Capability for Use in the Waste Isolation Pilot Plant Performance Assessment - 20545

Waste Isolation Pilot Plant (WIPP) performance assessment (PA) calculations estimate the probability of radionuclide release from the repository to the land surface and across the land withdrawal boundary for a regulatory period of 10,000 years after facility closure. Simulations of flow and transport in the repository and the surrounding Salado Formation are foundational to the PA. Because proposed additional waste emplacement panels would result in an asymmetric repository layout, the US Department of Energy (DOE) is preparing to transition to use of a three-dimensional (3-D) model domain for simulation of flow and transport instead of the two-dimensional (2-D) flared grid domain currently used. DOE has charged Sandia National Laboratories with developing the capability necessary to simulate processes affecting flow and transport in the WIPP in PFLOTRAN, an open-source massively parallel multi-phase flow and reactive transport code. The new flow and transport capabilities developed in PFLOTRAN incorporate WIPP-specific process models and will replace the 2-D simulators (BRAGFLO and NUTS) that are currently utilized for Salado flow and transport calculations in WIPP PA. The focus of this paper is on the development of a new Nuclear Waste Transport (NWT) mode in PFLOTRAN that has all of the capabilities necessary for Salado transport simulations, including the ability to handle complete dry-out (100% gas saturation) of arbitrary cells in the model domain, radionuclide mass conservation at step changes in porosity associated with borehole intrusion, and the ability to calculate fluxes on a flared grid. The new PFLOTRAN transport capability and a suite of verification tests were designed around a list of functional requirements for WIPP PA calculations. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2020

Low Energy Ultrasonic Separation

Separations exist in all manufacturing sectors, accounting for 22% of in-plant energy use. Whereas energy-intense technologies such as centrifuges are well established, low energy separations account for only 1% of industrial energy consumption. Researchers at Los Alamos National Lab are developing a low energy ultrasonic particle concentrator for industry. This technology may reduce energy use, improve separations, reduce wastes, and cut manufacturing costs.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

DOE OSTI2022

Produced Water and Waste Heat-aided Blowdown Water Treatment: Using Chemical and Energy Synergisms for Value Creation

The project objective was to develop a cooling blowdown water (BDW) treatment process utilizing produced water (PW) and low-grade heat to maximize water reuse and saleable by-product generation while reducing chemical and energy footprints of the treatment. The proposed treatment process consists of mixing, softening, organics and suspended solids removal, reverse osmosis (RO), thermal desalination, and brine electrolysis. BDW samples collected from a local coal-fired power plant and PW samples from two shale gas production wells were used in this study. Each treatment unit was first designed and tested to quantify its treatment efficiency, and its chemical and energy requirements. In addition, a process model was developed and model simulations were conducted based on the experimental results and literature data to optimize the treatment process. A techno-economic analysis was conducted to quantify chemical and energy savings as well as production of 10-lb brine as a saleable product. With the field-collected BDW and PW samples, mixing experiments determined a volumetric mixing ratio 10:1 (BDW:PW) resulted in the best performance of multivalent ions removal and largest chemical savings for softening. Softening of the BDW/PW mixtures using alkaline chemicals (Na 2 CO 3 and NaOH) achieved 95%-100% removal of scaling-forming cations (Ca, Mg, Fe, Ba, Sr) and 60% of silicon, and 10% of total organic carbon (TOC). The mixing and softening treatments yielded an effluent with total dissolved solids (TDS) concentration of 23 g/L. Activated carbon (AC) filtration removed TOC to a low level (< 3 mg/L) and further removed remaining scale-forming divalent metals and silica from the softened water. The AC filtration resulted in a slight reduction of TDS from 23 g/L to 20 g/L, leaving behind only mostly monovalent ions (i.e., sodium and chloride) in the filtered water. These pretreatments yielded a feed water that met the criteria of the downstream reverse osmosis (RO) to prevent membrane fouling. A cross-flow RO system was used to further concentrate the TDS of the AC effluent. Various factors including TDS, pH, and applied pressure were examined and optimal conditions were determined for the co-treatment process. An integrated process consisting of mixing, softening, AC filtration and RO was used to treat a continuous flow (0.25 – 1.2 L/min, or 0.07 – 0.32 gpm) and successfully generated RO permeate as product water (TDS < 0.5 g/L) for reuse in cooling operation, and a concentrate (TDS ~ 45 g/L) to be further treated in a thermal desalination unit. These flow rates meet the FOA’s criterion of 0.01 – 1 gpm. Overall, the co-treatment of BDW/PW allowed shorter ramp-up time compared to treatment of BDW alone. It resulted in 40% and 55% savings of Na 2 CO 3(s) and NaOH, respectively, compared to treating the BDW and PW individually for the same level of softening. The co-treatment also resulted in a 29% energy saving compared to treatment of BDW only for the level of TDS concentration. A thermal desalination system was designed using CFD simulations and manufactured in the WVU Innovation Hub for further treatment of the RO concentrate to generate 10-lb brine. The system has a design flow rate of 2 gpm and has been successfully tested. A bench-scale brine electrolysis system was developed for on-site generation of chlorine/hypochlorite (Cl 2 /OCl - ) and caustic soda (NaOH) as useful chemicals for the co-treatment process. Using salt solutions (0.5 M and 1 M), the system achieved faradaic efficiencies of 93%-97% and 70%-77% for caustic soda and chlorine/hypochlorite generation, respectively. An economic analysis showed that the electricity costs for on-site generation of these chemicals were significantly lower than the chemical prices offered by suppliers. An industrial-scale process model consisting of mixing, softening, AC filtration, RO, thermal desalination, and brine electrolysis was developed using the Aspen Plus V9 in conjunction with Aspen Custom Modeler V9. The model serves as a solvable Aspen Plus model and as basis to form the costing infrastructure. In addition, techno-economic analysis considering capital, operating, and transportation costs was conducted. An optimization solution showed that produced water for mixing is still advantageous in low quantities. The optimum solution approaches a leveled cost of water (LCW) of 2 $/m 3 which becomes cost competitive with nominal water treatment prices.

20 FOSSIL-FUELED POWER PLANTS↗

DOE OSTI1993

Nuclear Safety [Vol. 34, No. 1, January-March 1993]

Nuclear Safety is a review journal that covers significant developments in the field of nuclear safety. Its scope includes the analysis and control of hazards associated with nuclear energy, operations involving fissionable materials, and the products of nuclear fission and their effects on the environment. Primary emphasis is on safety in reactor design, construction, and operation; however, the safety aspects of the entire fuel cycle, including fuel fabrication, spent-fuel processing, nuclear waste disposal, handling of radioisotopes, and environmental effects of these operations, are also treated. Table of Contents for this issue follows. GENERAL SAFETY CONSIDERATIONS: 1 An Integrated Regional Approach To Risk Management of Industrial Systems, S. Chakraborty and R. Stratton; 9 Annual Technical Meeting of the NRC Cooperative Severe Accident Research Program, E. G. Silver; ACCIDENT ANALYSIS: 13 Deterministic Severe Accident Criteria as Severe Accident Design Criteria and Policy for the New Production Reactor-Heavy Water Reactor, P. T. Rhoads; 20 Proposed Deterministic Severe Accident Criteria for the Heavy Water Reactor-New Production Reactor Containment, K. D. Bergeron, S. E. Slezak, and C. E. Leach; 33 Quasi-Static Core Liquid Level Depression and Long-Term Core Uncovery During a PWR LOCA, Y. Kukita, R. R. Schultz, H. Nakamura, and J. Katayama; 49 LIRA: An Advanced Containment System to Minimize the Accidental Radioactivity Releases, A. Turricchia; 63 Errata to “A Review of Hydrogen Production During Melt/Water Interaction in LWRs,” Vol. 33, No. 4; CONTROL AND INSTRUMENTATION: 64 The Nuplex 80+™ Advanced Control Complex from ABB Combustion Engineering, F. Ridolfo, D. Harmon, and K. Scarola; DESIGN FEATURES: 76 A Scheme for Passive Isolation of the Containment of a Reactor, A. K. Ghosh, V. V. Raj, and K. Kakodkar; 84 Utility Requirements for Safety in the Passive Advanced Light-Water Reactor, T. U. Marston, W. H. Layman, and G. Bockhold, Jr.; WASTE AND SPENT FUEL MANAGEMENT: 91 Activities Related to Waste and Spent Fuel Management, Compiled by M. D. Muhlheim and E. G. Silver; OPERATING EXPERIENCES: 103 Testing Deficiencies in Auxiliary Systems Feedwater Systems, J. D. Kueck; 110 Reactor Shutdown Experience, Compiled by J. W. Cletcher; 113 Selected Safety-Related Events, Compiled by G. A. Murphy; 115 Operating U.S. Power Reactors, Compiled by M. D. Muhlheim and E. G. Silver; RECENT DEVELOPMENTS: 133 General Administrative Activities, Compiled by M. D. Muhlheim and E. G. Silver; 145 Reports, Standards, and Safety Guides, D. S. Queener; 150 Proposed Rule Changes as of Sept. 30, 1992; ANNOUNCEMENTS: 75 Harvard Short Course on Risk: Science, Assessment, and Management; 102 International Conference on Reactor Physics and Reactor Computations; 102 The Fourth International Conference on Nuclear Waste Reprocessing and Waste Management [RECOD ’94]; 132 International Symposium on the Radiological Exposure of the Population of the European Community from Radioactivity in the Mediterranean Sea [MARINA-MED]; 162 International High-Level Radioactive Waste Conference ‘Technology Integration—Above and Below”; 154 The Authors; 158 Indexes to Nuclear Safety, Volume 33.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI1993

Nuclear Safety [Vol. 34, No. 1, January-March 1993]

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2024

Minimizing grid energy consumption in wastewater treatment plants: Towards green energy solutions, water sustainability, and cleaner environment

Wastewater treatment plants (WWTPs) consume significant amount of energy to sustain their operation. From this point, the current study aims to enhance the capacity of these facilities to meet their energy needs by integrating renewable energy sources. The study focused on the investigation of two primary solar energy systems in As Samra WWTP in Jordan. The first system combines parabolic trough collectors (PTCs) with thermal energy storage (TES). This system primarily serves to fulfill the thermal energy demands of the plant by reducing the demands from boiler units, which allows more biogas for electricity generation. The second system is a photovoltaic (PV) system with Lithium-Ion batteries, which directly produces electricity that will be used to cover part of the electrical energy demands of plant. To assess the optimal configuration, two distinct scenarios have been formulated and compared to the current case scenario (SC#1). The first scenario focuses on maximizing the net present value (NPV) and minimizing the levelized cost of electricity (LCOE). The second scenario is centred on minimizing the levelized cost of heat (LCOH). The findings indicate that both scenarios succeeded in reducing the reliance on the grid to a value that reach 1 %. Moreover, they both reduced biogas percentage in energy production from 88 % to approximately 65 % through the integration of the PV system. In terms of thermal demand, SC#2 reduced the reliance on biogas boiler units from 100 % to 25 %, while SC#3 achieved an even more impressive reduction to just 8 %. The best LCOE value was attained in SC#2, at 0.0895 USD/kWh, with an NPV of 10.54 million USD. Conversely, SC# 3 yielded an LCOH value of 0.0432 USD/kWh th compared to 0.0534 USD/kWh th USD for SC#2. In conclusion, despite their relatively high capital and operating costs, SC#2 and SC#3 managed to substantially decrease the annual electricity expenditure from approximately 2 million USD to 86,000 USD and 0 USD, respectively.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

DOE OSTI2023

Synthesis of Carbohydrates from Methanol Using Electrochemical Partial Oxidation over Palladium with the Integrated Formose Reaction

Electrochemically derived multicarbon products are a golden target for valorization of captured carbon dioxide due to the potential of turning a waste product into useful commodity chemicals with renewable energy sources. As a tantalizing approach toward their synthesis, the formose reaction utilizes catalytic condensation of formaldehyde to generate carbohydrates. Furthermore, while a sustainable approach to artificial carbohydrate production through electrochemical generation of formaldehyde is desirable, to date, it has not been fully realized. Here, we study the electrocatalytic conversion of methanol to formaldehyde on palladium with faradaic efficiency of over 90% at 0.9 V vs Ag/AgCl and with the partial current density of nearly 3 mA cm -2 at 1.6 V vs Ag/AgCl. We observe the concurrent generation of palladium oxides as a consequence of the high overpotentials employed, which may partially explain the higher selectivity toward the partial oxidation product. Moreover, we demonstrate that formaldehyde produced electrochemically from methanol is feasible for formose reactions without the need for further purification, achieving 21-28% carbon conversion to carbohydrates. This process, therefore, represents a potential avenue for the electrochemical generation of formaldehyde and its utilization in generating multicarbon products inaccessible by other electrocatalytic means.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

THERMAL STRESS ANALYSIS OF A SPENT NUCLEAR FUEL CANISTER

The potential for chloride induced stress corrosion cracking (CISCC) in spent nuclear fuel dry storage canisters is a current topic of research by the US Department of Energy Spent Fuel and Waste Science and Technology program. One of the important prerequisites for CISCC is a tensile residual stress state. This study utilizes computational models to provide an initial analysis of thermal stresses in a generic spent nuclear fuel canister. A STAR-CCM+ thermal fluid model provides a temperature profile analysis of the canister based on four different ambient temperature conditions. An ANSYS APDL finite element model incorporates the temperature profiles to analyze the thermal stresses in the canister. The calculated thermal stress magnitudes are in the range of 10 MPa to 80 MPa, which could be significant for crack propagation through the canister wall. The maximum thermal stress is not a concern for the structural failure of the canister, but it is high enough that it is a significant contribution to the total stress state of the canister wall, which also includes residual stress from fabrication, internal pressure from helium cover gas, and potential transient mechanical loads, such as earthquakes. This paper describes the initial finite element thermal stress analysis that was completed in 2020, reports the initial findings, and identifies areas where model refinement is still needed to complete this work in the future.

Jensen, Ben J.↗

DOE OSTI2021

Gas-phase stability of large lanthanide:diglycolamide clusters evaluated using collision-induced dissociation

Efficient utilization of long-term deep geologic storage repositories is critical for the large-scale deployment of nuclear energy. As the minor actinides (americium and curium) are the largest contributor to the decay heat of used nuclear fuel after a few hundred years, their removal from used fuel prior to disposal can significantly increase the amount of waste that can be stored in a given volume. The development of ligands that can effectively separate the minor actinides from other components of used nuclear fuel are crucial to efficient utilization of geological storage repositories. N,N,N’,N’-tetraoctyl diglycolamide (TODGA) is a promising extractant for the separation of lanthanides and the minor actinides from other components of used nuclear fuel. While the use of TODGA in f-element separations has been investigated in process-based formulations, gas-phase metal ion cluster experiments enable the study of covalent interactions in reprocessing systems absent from solvent effects. Exploring fundamental differences in lanthanide-ligand covalent interactions can impact the development and implementation of actinide-lanthanide separation systems in nuclear fuels reprocessing. In this study, lanthanide-TODGA clusters were synthesized in the gas-phase and identified using mass spectrometry fragmentation experiments. Large europium and samarium clusters were identified that contained up to 8 and 10 bound TODGA ligands, respectively; this was surprising due to the size and multidentate binding that is normal for TODGA. In addition, while smaller clusters showed evidence of sequential ligand fragmentation, larger clusters displayed the loss of neutral TODGA with applied collision voltage. Interestingly, the voltage required for this removal decreased as more TODGA ligands were bound to the metal, suggesting that the metal coordination sphere was becoming more saturated and TODGA ligands were more weakly bound as the clusters got larger.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗