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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

The Critical Role of Process Analysis in Chemical Recycling and Upcycling of Waste Plastics

There is an urgent need for new technologies to enable circularity for synthetic polymers, spurred by the accumulation of waste plastics in landfills and the environment and the contributions of plastics manufacturing to climate change. Chemical recycling is a promising means to convert waste plastics into molecular intermediates that can be remanufactured into new products. Given the growing interest in the development of new chemical recycling approaches, it is critical to evaluate the economics, energy use, greenhouse gas emissions, and other life cycle inventory metrics for emerging processes, relative to the incumbent, linear manufacturing practices employed today. Here we offer specific definitions for classes of chemical recycling and upcycling and describe general process concepts for the chemical recycling of mixed plastics waste. We present a framework for techno-economic analysis and life cycle assessment for both closed- and open-loop chemical recycling. Rigorous application of these process analysis tools will be required to enable impactful solutions for the plastics waste problem.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Evaluation of Hydrogen Generation in High Burnup Demonstration Dry Storage Cask

This report provides a best-estimate evaluation of residual water content (post-dry out) in the High Burnup (HBU) LWR Spent Fuel Demonstration project TN-32 cask, and evaluates the radiolysis of the residual free water, and the physisorbed and chemisorbed waters on the surfaces of the fuel and cask internal contents. The evaluation of radiolytic breakdown of those waters with gamma radiation causing the generation of hydrogen gas (H 2 ) is made using available literature data and models. This evaluation is part of the overall materials performance evaluation of the SNF-in-canister system, and is part of the technical bases for their continued safe dry storage. The TN-32 cask contents included 32 HBU LWR spent fuel assemblies each with 264 fuel rods clad in zirconium alloys, aluminum neutron absorber components, and aluminum and stainless steel structural components. The residual free and surface (physisorbed/chemisorbed) waters are ascribed to water vapor in the free volume and to components’ surfaces, respectively. The total potential radiolytic hydrogen inventory from the water vapor and from waters ascribed to surfaces has been calculated assuming all the water produced molecular H 2 . The residual water that is chemically incorporated into the bulk of a hydrated oxide, i.e., chemisorbed water, and its total potential hydrogen inventory has been calculated. These calculations are at the physical limit of material available and are used for a bounding assessment purpose only.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2023

The circular nutrient economy of terrestrial ecosystems and the consequences for rock weathering

Earth’s biosphere is thought to exert a substantial influence on regolith evolution and chemical weathering rates. However, ecosystems are also highly efficient at retaining and recycling nutrients. Thus, when the ecological demand for rock-derived nutrients (e.g., P, Ca, K) exceeds the rates of regolith supply, ecological retention and recycling strategies can minimize nutrient limitations. To evaluate the balance between nutrient recycling and new nutrient input, we combined a plant model that drives growth according to foliar P levels with a weathering model that includes regolith rejuvenation via erosion and export via chemical weathering according to water flow, regolith thickness, mineral dissolution rates, secondary minerals, and nutrient storage in organic and mineral phases. We find that plant growth is strongly dependent on the total regolith nutrient inventory, resulting in a strong correlation between plant productivity and erosion. Increased water export or decreased regolith thickness diminish the total inventory of nutrient corresponding to lower rates of recycling and lower plant growth. In contrast, purported biogenic drivers of weathering, such as enhanced mineral dissolution, only support higher growth rates at high erosion rates. At erosion rates typical of the global land surface, more rapid mineral dissolution combined with enhanced formation of secondary minerals, depletes the inventory of mineral P, resulting in no benefit for plant growth. We also find that the increased chemical weathering export does not scale directly with plant growth. For example, accelerated mineral weathering does increase chemical weathering export but not potential plant growth. Conversely, thicker regolith is associated with a small increase in weathering export, but a large increase in potential plant growth. Collectively, when plant growth is coupled to regolith weathering our calculations suggest that plant productivity is not directly correlated with silicate weathering fluxes, and that biotic drivers of silicate weathering may only be effective at high erosion rates not typical at the Earth’s surface.

58 GEOSCIENCES↗
DOE OSTI2026

Source-Resolved Inversion of Elemental Carbon Emissions in California Using Log-Space Bayesian Inference

Elemental carbon (EC), operationally quantified by thermal-optical analysis, is widely used as a proxy for black carbon (BC) relevant to short-term climate forcing and public health. Current EC emission inventories remain highly uncertain, with persistent discrepancies between bottom-up and top-down estimates. In this study, we develop a source-resolved, log-space Bayesian inversion framework applied to estimate California’s statewide EC emissions in 2019. By integrating surface EC measurements from the EPA’s Air Quality System network with high-resolution source contributions simulated by a chemical transport model, we identify a one-third underestimation in the existing statewide EC inventory, requiring an increase of the total from a prior of 8.58 [5.49–13.75] Gg year–1 to a posterior estimate of 12.78 [10.71–15.37] Gg year–1. This discrepancy is primarily driven by substantial underestimations in the power and industrial and off-road mobile sectors. Furthermore, population-weighted exposure analysis reveals a marked sectoral divergence between emission mass and health burden: off-road mobile sources dominate both emissions and exposure, accounting for 31% of statewide exposure, while residential wood combustion contributes 26% of total exposure despite comprising only 19% of total emissions, due to its source proximity to population. These findings underscore the need to update sector-specific EC speciation profiles and demonstrate that mitigation strategies targeting off-road mobile sources and residential wood combustion are critical for reducing EC-related health impacts in California.

Zhang, Jie↗
DOE OSTI2025

Calculating the Effects of Solids Input and Removal as a Temperature Control in the Advanced Scale Up Reactor Experiment (ASURE) Facility at NETL Using Aspen

The Advanced Scale Up Reactor Experiment (ASURE) facility at NETL is being designed to be a fuel-flexible multi-purpose reactor that can be used for pyrolysis/gasification or evaluation of other high pressure “circulating fluidized bed” (CFB) chemical processes. The initial system design calculations for pyrolysis/gasification are presented in this work showing the expected performance of the ASURE facility when used as a biomass conversion reactor. Several other areas of application include gasification of any carbonaceous fuel including biomass, coal, plastics, and other waste materials. The reactor can therefore be used to produce SYNGAS of various compositions and hydrogen as well as other high value chemicals resulting from a typical tuned gasification process. This paper discusses an ASPEN model of the facility, focusing on the riser of the CFB reactor and the solids recirculation loop. The ASPEN model divides the riser into two sections. A bottom section which receives ash, char and sand which have been recirculated from a return loop. In this section an inert fluidization gas, (N2 or CO2), is introduced which acts as the primary mover of the solids through the system. The bottom section is equipped with a restricted air feed so that the recirculated char can be partially oxidized. This oxidation process along with the inventory of recirculating sand are used to effectively control the temperature in the following two chemical conversion sections of the reactor which are the pyrolysis zone followed by a tar cracking zone. Fresh fuel is added to the pyrolysis zone and undergoes drying and devolatilization. The products ash, char, volatile matter, and water vapor exit the pyrolysis zone and enter the reaction block for tar cracking. Steam and CO2 gasification reactions will be incorporated into the tar cracking zone, however at the design operating temperature, conversion from these reactions is expected to be essentially zero. The unit when completed in 2026 will test mixtures of biomass, plastics, and waste coal. This presentation discusses the basic ASPEN engineering design model for this project and provides preliminary sensitivity studies to determine how the various parts of the reactor will perform.

ASSURE↗
DOE OSTI2025

Calculating the Effects of Solids Input and Removal as a Temperature Control in the Advanced Scale Up Reactor Experiment (ASURE) Facility at NETL Using Aspen

The Advanced Scale Up Reactor Experiment (ASURE) facility at NETL is being designed to be a fuel-flexible multi-purpose reactor that can be used for pyrolysis/gasification or evaluation of other high pressure “circulating fluidized bed” (CFB) chemical processes. The initial system design calculations for pyrolysis/gasification are presented in this work showing the expected performance of the ASURE facility when used as a biomass conversion reactor. Several other areas of application include gasification of any carbonaceous fuel including biomass, coal, plastics, and other waste materials. The reactor can therefore be used to produce SYNGAS of various compositions and hydrogen as well as other high value chemicals resulting from a typical tuned gasification process. This paper discusses an ASPEN model of the facility, focusing on the riser of the CFB reactor and the solids recirculation loop. The ASPEN model divides the riser into two sections. A bottom section which receives ash, char and sand which have been recirculated from a return loop. In this section an inert fluidization gas, (N2 or CO2), is introduced which acts as the primary mover of the solids through the system. The bottom section is equipped with a restricted air feed so that the recirculated char can be partially oxidized. This oxidation process along with the inventory of recirculating sand are used to effectively control the temperature in the following two chemical conversion sections of the reactor which are the pyrolysis zone followed by a tar cracking zone. Fresh fuel is added to the pyrolysis zone and undergoes drying and devolatilization. The products ash, char, volatile matter, and water vapor exit the pyrolysis zone and enter the reaction block for tar cracking. Steam and CO2 gasification reactions will be incorporated into the tar cracking zone, however at the design operating temperature, conversion from these reactions is expected to be essentially zero. The unit when completed in 2026 will test mixtures of biomass, plastics, and waste coal. This paper presents the basic ASPEN engineering design model for this project and provides preliminary sensitivity studies to determine how the various parts of the reactor will perform.

ASSURE↗
DOE OSTI2026

Life Cycle Inventories and Data Gap Analysis for Rare Earth Elements: Neodymium and Dysprosium from Mining to Magnets

The United States demand for Neodymium-Iron-Boron (NdFeB) magnets, produced from rare earth elements (REEs) such as (Nd) and Dysprosium (Dy), far exceeds its nascent domestic production capacity, rendering it reliant on vulnerable global supply chains dominated by China. To guide research and development investments in securing U.S. REE supply, defensible benchmark metrics across environmental, economic, and social dimensions are needed. In this study, we built globally-representative, process-based cradle-to-cradle life cycle inventories for Nd and Dy in NdFeB magnets lifecycles, encompassing primary material acquisition, beneficiation, smelting and refining, metal processing, specialty alloy and chemical transformation, subcomponent manufacturing, consumer application (use phase) and end-of-life management. We carried out detailed literature review, and applied process engineering principles to build industry-representative upscaled life cycle inventories for both metals. We used these models to conduct bottom-up literature review and gap analysis on existing literature, compilation of data sources for each life cycle stage (and transformations where necessary), and a preliminary technoeconomic analysis (TEA)/life cycle costing analysis (LCCA). Findings from this work emphasize the need for metal specific, representative REE LCIs to establish robust benchmarks for advancing sustainable REE technologies and guiding R&D in REE supply chains.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗
DOE OSTI2021

Vitrification of Hanford Tank Wastes for Condensate Recycle and Feed Composition Changeover Testing

During the vitrification of Hanford Site nuclear waste at the Waste Treatment and Immobilization Plant (WTP), which is a part of the safe and efficient retrieval, treatment, and disposal mission of the U.S. Department of Energy Office of River Protection, the offgas condensate generated from the waste-to-glass conversion is currently planned to be concentrated by evaporation in the Effluent Management Facility (EMF). This concentrated condensate can then be recycled back to the incoming waste and vitrified. To test the recycle process, an apparatus was designed and built to mimic the EMF evaporator and was then used to concentrate a volume of condensate produced during the vitrification of a sample of Hanford tank 241-AP-107 (referred to herein as AP-107) waste in a continuous laboratory-scale melter (CLSM). The concentrated condensate was added to an additional sample of AP-107 waste, to mimic one round of the recycle process, and the combined solution was vitrified, producing a second round of recycle condensate. In the current study, the EMF test apparatus was used to concentrate the second-round recycle condensate under evaporation conditions (at 45 °C and 1.4 psia) designed to emulate EMF operation. The condensate was successfully concentrated by a factor of ~10 while retaining over 95 % of the technetium-99 ( 99 Tc), Cs, and I inventories in the concentrate. Another portion of AP-107 waste was retrieved by Washington River Protection Solutions, LLC (WRPS) and transferred to Pacific Northwest National Laboratory (PNNL), where it was pretreated and then combined with the second-round recycle AP-107 condensate concentrate and glass-forming chemicals (GFCs) to form the two-time recycle AP-107 melter feed, approximating a second round to the recycling action to be performed at the WTP. A portion of AP-105 waste was also retrieved by WRPS and provided to PNNL for pretreatment and combining with GFCs to form AP-105 melter feed. The two-time recycle AP-107 and AP-105 melter feeds were processed consecutively in the CLSM. The CLSM run proceeded for 13.63 hours, producing 9.70 kg of glass for an average glass production rate of 1464 kg m 2 d -1 during the two-time recycle AP-107 feed charging and 1568 kg m 2 d -1 during the AP-105 feed charging. The rate during AP-107 charging was essentially equivalent to the rate when processing no-recycle AP-107 feed and lower than that achieved when processing one-time recycle AP-107 feed. However, all rates were within the potential range of variability when processing melter feeds with similar composition in the CLSM. Likewise, the rate during AP-105 charging was higher than the previous rate processing AP-105, but within the potential CLSM range. The cold-cap characteristics changed from the typically thin AP-107 cold cap to a foamy-edged cold cap as previously seen with AP-105 shortly after transitioning to the AP-105 melter feed. The glass produced during the CLSM run was within 10 % of its target composition for the primary glass components. The CaO and Li 2 O targets varied by more than 1 wt% between the two-time recycle AP-107 and AP-105 glass targets and it took about 2 turnovers of the CLSM glass inventory to reach a relative chemical steady state in the glass for CaO and Li 2 O after the melter feed inputs were switched. The 99 Tc and total cesium content in the melter feeds were maintained at concentrations expected to be experienced at the WTP. During the CLSM run, while processing the two-time recycle AP-107 melter feed at a relative chemical steady state, the 99 Tc/Cs ratio was 10, and 34% of 99 Tc and 74% of Cs were retained in the glass. These values were higher than those measured in the CLSM run with one-time recycle AP-107 melter feed. After the transition to processing the AP-105 melter feed, when the production reached a relative chemical steady state, the 99 Tc/Cs ratio was 77 while 44% of 99 Tc was retained in the glass. The C's retention during this time frame reached 200% due to the excess C's in the glass after the target content decreased to 15% of its initial level in the two-time recycle AP-107 melter feed to the lower target in the Ap-105 melter feed. While iodine was below inductively coupled plasma mass spectrometry analytical reporting limits in the melter feed and glass samples, it was detected in quantities above the analytical reporting limits in the liquid and filter samples collected from the CLSM offgas treatment system. The behavior of iodine in the CLSM offgas treatment system followed a similar pattern to those of 99 Tc and Cs.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2022

Vitrification of Hanford Tank Wastes for Condensate Recycle and Feed Composition Changeover Testing (Rev. 1)

During the vitrification of Hanford Site nuclear waste at the Waste Treatment and Immobilization Plant (WTP), which is a part of the safe and efficient retrieval, treatment, and disposal mission of the U.S. Department of Energy Office of River Protection, the offgas condensate generated from the waste-to-glass conversion is currently planned to be concentrated by evaporation in the Effluent Management Facility (EMF). This concentrated condensate can then be recycled back to the incoming waste and vitrified. To test the recycle process, an apparatus was designed and built to mimic the EMF evaporator and was then used to concentrate a volume of condensate produced during the vitrification of a sample of Hanford tank 241-AP-107 (referred to herein as AP-107) waste in a continuous laboratory-scale melter (CLSM). The concentrated condensate was added to an additional sample of AP-107 waste, to mimic one round of the recycle process, and the combined solution was vitrified, producing a second round of recycle condensate. In the current study, the EMF test apparatus was used to concentrate the second-round recycle condensate under evaporation conditions (at 45 °C and 1.4 psia) designed to emulate EMF operation. The condensate was successfully concentrated by a factor of ~10 while retaining over 95 % of the technetium-99 (99Tc), Cs, and I inventories in the concentrate. Another portion of AP-107 waste was retrieved by Washington River Protection Solutions, LLC (WRPS) and transferred to Pacific Northwest National Laboratory (PNNL), where it was pretreated and then combined with the second-round recycle AP-107 condensate concentrate and glass-forming chemicals (GFCs) to form the two-time recycle AP-107 melter feed, approximating a second round to the recycling action to be performed at the WTP. A portion of AP-105 waste was also retrieved by WRPS and provided to PNNL for pretreatment and combining with GFCs to form AP-105 melter feed. The two-time recycle AP-107 and AP-105 melter feeds were processed consecutively in the CLSM. The CLSM run proceeded for 13.63 hours, producing 9.70 kg of glass for an average glass production rate of 1464 kg m 2 d -1 during the two-time recycle AP-107 feed charging and 1568 kg m 2 d -1 during the AP-105 feed charging. The rate during AP-107 charging was essentially equivalent to the rate when processing no-recycle AP-107 feed and lower than that achieved when processing one-time recycle AP-107 feed. However, all rates were within the potential range of variability when processing melter feeds with similar composition in the CLSM. Likewise, the rate during AP-105 charging was higher than the previous rate processing AP-105, but within the potential CLSM range. The cold-cap characteristics changed from the typically thin AP-107 cold cap to a foamy-edged cold cap as previously seen with AP-105 shortly after transitioning to the AP-105 melter feed. The glass produced during the CLSM run was within 10 % of its target composition for the primary glass components. The CaO and Li 2 O targets varied by more than 1 wt% between the two-time recycle AP-107 and AP-105 glass targets and it took about 2 turnovers of the CLSM glass inventory to reach a relative chemical steady state in the glass for CaO and Li 2 O after the melter feed inputs were switched.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2021

Editors’ Choice—Necessity to Avoid Titanium Oxide as Electrocatalyst Support in PEM Fuel Cells: A Membrane Durability Study

Pt/TiO 2 as electrocatalyst was found to significantly increase the rate of the membrane chemical degradation in a polymer electrolyte membrane (PEM) fuel cell. The increased degradation was proved to be due to TiO x (TiO 2 or Ti 4 O 7 ), which is widely recognized as a promising corrosion-resistant electrocatalyst support. The membrane degradation (thinning) appears to be preferentially in the side facing anode electrode. Migrated Ti species as a result of TiO x dissolution during fuel cell operation in an acidic environment was quantified by electron probe microanalysis (EPMA). Total fluorine inventory loss of the membrane strongly depends on the quantity of migrated Ti species (likely Ti 3+ and/or Ti 4+ ). The membrane chemical degradation induced by TiO x is proposed to be due to dissolved ionic Ti species reacting with H 2 O 2 through a Fenton reaction. TiO x is determined to be inviable as electrocatalyst support for PEM fuel cells, and future research is suggested to be directed toward alternative oxides with similar corrosion-resistance.

08 HYDROGEN↗
DOE OSTI2022

Milestone 1.2.10: Steady-state H 2 “roll over” point data for aluminum alloys 1100 and 6061

Extended (> 50 years) dry storage is being evaluated by the U.S. Department of Energy (DOE) for the disposition of ~ 18 metric tons of aluminum-clad spent nuclear fuel (ASNF). Transition of the current ASNF inventory into dry storage—using the standard DOE canister—necessitates a rigorous, predictive understanding of the long-term physical and chemical factors that may influence the integrity of the proposed storage canister, including radiolytic molecular hydrogen (H 2 ) generation. Current model predictions employ initial radiolytic yields of H 2 , the values of which change as the cladding’s H 2 -precursor inventory is depleted and H 2 itself becomes progressively more involved in radiolytic and surface dissociation processes. Consequently, the absorbed radiation dose that this steady-state H 2 yield corresponds to is essential for the evaluation and improvement of model predictions. Here, we report our findings on the long-term generation of H 2 from the gamma irradiation (≤ 36 MGy) of corroded AA1100 and AA6061 coupons in helium environments at ambient temperature and ~ 50% RH. Our findings show that AA1100 systems reached steady-state by ~ 36 MGy, while higher doses were necessary for AA6061 systems. This discrepancy was attributed to the AA6061 coupons developing a thicker corrosion layer that led to the trapping of H 2 and its precursors, and potentially additional chemistries, ultimately delaying the depletion of H 2 precursors and the system’s “roll over” point. Further, current model predictions—based on previous AA1100 data—do not show steady-state attainment until above 120 MGy, which is not the case for the AA1100 data collected here. Consequently, the new alloy dependent data presented here are important for the continued improvement of predictive computer models for evaluating the feasibility of extended storage of ASNF in helium backfilled canisters.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2025

Effect of Annealing on Direct Recycled NMC Cathodes

A substantial number of electric vehicle batteries are poised to reach end-of-life conditions in the next decade. Direct recycling has advantages over typical recycling processes because it preserves the chemical structure of the material. One key step of direct recycling materials like nickel manganese cobalt oxide (NMC) cathodes is relithiation, which includes replacing the depleted lithium inventory in the cathode and annealing the material to fix crystallographic degradation. This work uses multiple characterization techniques (synchrotron X-ray diffraction, Ni X-ray absorption near edge structure, scanning transmission electron microscopy) to understand the lithiation mechanism of degraded and chemically relithiated NMC 622. Despite the necessary reconstruction after relithiation being limited to the surface of the degraded NMC 622, a high annealing temperature of 720 °C is still necessary to restore the NMC 622 structure back to pristine condition after relithiation. This work also finds that treating degraded NMC 622 with an annealing step is sufficient to restore key electrochemical and structural properties, other essential features of pristine NMC 622 material such as particle porosity and morphology are largely unaffected. Understanding the effect of this annealing step has important implications on defining the degree of success of any given direct recycling strategy.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Assessing the Relative Climate Impact of Carbon Utilization for Concrete, Chemical, and Mineral Production

Estimates show that 6.2 gigatons of carbon dioxide (CO2) can be captured and utilized across three pathways, concrete, chemical, and minerals, by 2050. However, it is difficult to compare the climate benefit across these three carbon capture and utilization (CCU) pathways to determine the most effective use of captured CO2. The life cycle assessment methods to evaluate the climate benefit of CCU chemicals should additionally account for the change in material properties of concrete due to CO2 utilization. Furthermore, with most CO2 utilization technologies being in the early stages of research and development, the uncertainty and variability in process and inventory data present a significant challenge in evaluating the climate benefit. We present a stochastically determined climate return on investment (ROI) metric to rank and prioritize CO2 utilization across 20 concrete, chemical and mineral pathways based on the realized climate benefit. We show that two concrete pathways, which use CO2 during concrete mixing, and two chemical pathways, which produce formic acid through hydrogenation of CO2 and carbon monoxide through dry reforming of methane, generate the greatest climate ROI and are the only CCU pathways with a higher likelihood of generating a climate benefit than a climate burden.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗
DOE OSTI2026

Using Best Basis Inventory Data to Direct Strategies for Real Time Monitoring of Hanford High Level Waste – 26226

The potential to accelerate the processing of low- and high-level tank waste by applying real-time monitoring (RTM) of chemical and physical properties has prompted research into the suitability of multiple analytical methods for that purpose. The broad variety of waste stream properties and the large number of analytes of interest (as evidenced by Waste Acceptance Criteria (WAC) and Process Control Limit (PCL) lists) lead to an overwhelming set of possible analytical scenarios. This report describes the use of Best Basis Inventory (BBI) data to find the most relevant analytical targets for the specific case of monitoring the blending of High Level Waste from multiple tanks prior to introduction into a vitrification facility. Campaigns for blending this waste to minimize the risk of exceeding WACs and PCLs have been proposed. However, the predicted compositions of the blended materials do not incorporate any uncertainties that may be associated with the representativeness of the waste layer samples or the laboratory analyses that generated the BBI data. Also, they do not include any uncertainty associated with the precision of collecting highly specific fractions of the layers during a blending campaign or any inhomogeneities that may exist in those layers. Monte Carlo methods are used to apply uncertainties to the compositions of the individual layers specified in the campaign recipes. The resulting variations in the compositions of the blended materials allow estimation of the risks of exceeding WACs and PCLs for each campaign. A critical subset of WACs/PCLs – NOx, NaK, AlFeZr, and S – are especially at risk of being exceeded in multiple campaigns. These analytes should be the focus of instrument development. We also have extracted the expected solid/supernate distribution for these analytes, which establishes important performance criteria for individual analytical methods. The BBI data also permits an understanding of the different chemical forms in which the analytes appear. Thus, the need to establish instrumental sensitivity to these forms can be gainfully addressed. Although concentrating on one specific application – the blending of tank waste - this approach should be generalizable for the analysis of other possible RTM applications for waste processing.

Lascola, Robert [Savannah River National Laborator↗
DOE OSTI2022

Coupled chemical–CFD modeling of unsealed dry storage of advanced test reactor spent fuel

We report given the current lack of long-term disposal for spent nuclear fuel storage in the United States, the current inventory of advanced test reactor (ATR) fuel at Idaho National Laboratory (INL) is expected to be stored in a dry storage facility for an extended storage period. As part of an effort to understand the conditions during a 50-year period, a three-dimensional computational fluid dynamics (CFD) of the unsealed canisters packed with spent fuel in the storage facility was constructed, this CFD model is coupled with radiolytic chemical reactions associated with water vapor and other species. The coupled model is simulated over a range of sensitivity parameters for the fuel decay heat, relative humidity, and oxyhydroxide film thickness for undried and fully-dried fuel. The most important parameter was the initial fuel decay heat. Over the range of cases, the hydrogen and nitric acid concentrations are low enough no significant impact is expected.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2020

An atom probe tomography and inventory calculation examination of second phase precipitates in neutron irradiated single crystal tungsten

Tungsten is the prime candidate material for the plasma facing divertor system and first wall armor of future nuclear fusion reactors. However, the understanding of the microstructural and chemical evolution of pure tungsten under neutron irradiation is relatively unknown, in part due to a lack of experimental data on this topic. Here, single crystal tungsten has been irradiated in the High Flux Isotope Reactor (HFIR) at Oak Ridge National Laboratory at a nominal temperature of 700–800 °C to damage levels of 0.1 and 1.8 displacements per atom (dpa). Inventory calculations of the neutron irradiation experiments have been used to track isotope generation and decay to inform atom probe tomography (APT) results in the determination of the transmutation-induced precipitate compositions. Furthermore, APT crystallography has been used to show the relationship between precipitates and matrix. The composition of the precipitates is shown to progress towards that of the σ-phase at the highest dose studied, with those precipitates lying along crystallographic planes similar to those of displacement-induced dislocations. This work also sets the framework for APT studies of materials that contain isotopic ratios far from those observed in the natural state.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2022

Contribution of Ryugu-like material to Earth’s volatile inventory by Cu and Zn isotopic analysis

We report initial analyses showed that asteroid Ryugu’s composition is close to CI (Ivuna-like) carbonaceous chondrites (CCs) – the chemically most primitive meteorites, characterized by near-solar abundances for most elements. However, some isotopic signatures (for example, Ti, Cr) overlap with other CC groups, so the details of the link between Ryugu and the CI chondrites are not yet fully clear. Here we show that Ryugu and CI chondrites have the same zinc and copper isotopic composition. As the various chondrite groups have very distinct Zn and Cu isotopic signatures, our results point at a common genetic heritage between Ryugu and CI chondrites, ruling out any affinity with other CC groups. Since Ryugu’s pristine samples match the solar elemental composition for many elements, their Zn and Cu isotopic compositions likely represent the best estimates of the solar composition. Earth’s mass-independent Zn isotopic composition is intermediate between Ryugu/CC and non-carbonaceous chondrites (NCs), suggesting a contribution of Ryugu-like material to Earth’s budgets of Zn and other moderately volatile elements.

58 GEOSCIENCES↗
DOE OSTI2024

A Molten Salt Aerosol Spectroscopy Approach to Online Process Monitoring in Molten Salt Reactors

Recent research and development in molten salt reactors (MSRs) has led to many advanced reactor designs, many of which have demonstrations planned in the next decade. However, a significant challenge that must be overcome before liquid fueled MSRs become viable globally is nuclear material accountancy (NMA) and safeguards. Liquid-fueled MSRs are problematic to safeguards because the nuclear material is in the bulk phase, inventories are constantly changing, and there are potentially many outlet pathways that must be monitored, especially in designs with online chemical processing. At the Idaho National Laboratory, we have developed a process monitoring tool to circulate molten salt through a nebulizer and optical cell, where laser-induced breakdown spectroscopy (LIBS) and ultraviolet-visible (UV-VIS) are applied to track the elemental and oxidation states of the constituents in the salt aerosol. This approach has the potential to provide information on the actinides, fission products, and corrosion in the reactor or process. Preliminary testing in aqueous praseodymium chloride (PrCl3) and neodymium chloride (NdCl3) showed good sensitivity detection limits n developed calibration curves. Additional tests and analysis or ongoing in aqueous solutions while equipment is being scaled up for high temperature molten salt testing. Results for continued testing as well as a status of the molten salt design and anticipated commissioning will be presented.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗