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At least 1,135 records · Page 63
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Future Intensity‐Duration‐Frequency Curves of Extreme Precipitation in the Midwest United States From Convection‐Permitting Modeling

Abstract During the last four decades, global warming has statistically significant intensified extreme precipitation events in the Midwestern United States (defined here as the region covering Illinois, Indiana, Ohio, and Kentucky), leading to increased risks to human life, property, and infrastructure. To enable climate change adaptation and resilience across various economic and social sectors in this region, updated information about future climate changes, specifically at finer spatial scales, is essential. Leveraging a new 150‐year dynamical downscaling data set at convection‐permitting resolution, this study introduces a framework to construct the projected future intensity‐duration‐frequency (IDF) curves of heavy precipitation, which are prominent tools for infrastructure design and water resources management. This framework generates IDF curves at both sub‐daily and multi‐day duration utilizing hourly in situ observations as well as quantile‐based statistical techniques in bias‐correction and return levels selection. The assumption of non‐stationarity in the distribution parameter fitting process is also implemented in this workflow. Compared to historical IDF curves for 1980–2022, future projected IDF curves for 2058–2100 under Representative Concentration Pathway (RCP) 4.5 and RCP 8.5 scenarios indicate an average intensity increase of approximately 15% and 25%, respectively, across 74 stations, considering both annual and seasonal timescales. Future projections suggest that extreme precipitation events may become more severe across six investigated return periods, with longer return periods showing a greater increase. The frequency of future extreme precipitation events in the Midwest region is also projected to double. Furthermore, current results reveal spatial heterogeneity of future trends across stations owing to the high‐resolution input data set. Plain Language Summary This study investigates the evolving nature of extreme precipitation events in the Midwestern United States under a changing climate. By leveraging a high‐resolution dynamical downscaling data set, we construct projected intensity‐duration‐frequency (IDF) curves for future extreme rainfall events. These curves serve as vital tools for infrastructure planning and water resource management. Our analysis reveals a significant increase in both the intensity and frequency of extreme precipitation events in the region. Future projected IDF curves for the late century indicate an average intensity increase of approximately 15%–25% compared to historical values. Moreover, the frequency of such events is expected to double. Spatial heterogeneity in future trends is observed across different stations within the Midwest, highlighting the importance of high‐resolution modeling in capturing localized climate variability. These findings underscore the urgent need for climate adaptation strategies to mitigate the increasing risks associated with extreme precipitation events in the region. Key Points This study introduces a workflow to construct future intensity‐duration‐frequency (IDF) curves over the Midwest United States using a new convection‐permitting modeling data set The current IDF construction workflow reproduces well the historical observed IDF 30 curves in summer months with median relative errors of 2.4% among 74 stations and 6 investigated durations The projected IDF curves show diverse future trends of extreme precipitation across stations, with intensity increases of approximately 15% and 25% under RCP4.5 and RCP8.5 climate scenarios, respectively, and a doubling of frequency on average

Nguyen, Trung↗
DOE OSTI2025

Development of an Energy-Efficient and High-Productivity Ammonia Recovery and Removal Process Using Resin-Wafer Electrodeionization

As efforts to develop various energy resources, ammonia energy is emerging as a promising carbon-free fuel alternative. Recovering high-concentration ammonia and ammonium from wastewater potentially offers significant environmental and economic benefits. However, research on recovery technologies for industries such as semiconductors remains limited. This study develops an efficient, energy-saving ammonia recovery technology using Resin Wafer Electrodeionization (RW-EDI), specifically for the semiconductor industry. RW-EDI shows promise for recovering ammonia from high-concentration wastewater. By optimizing parameters, such as voltage and initial concentration, a balance between productivity and energy consumption is achieved. Results indicate that ammonium and fluoride ion transport kinetics are similar, with minimal competition and selectivity values between 0.95 and 1.08. As the initial ammonia/ammonium concentration increases from 500 to 8000 ppm, reaction rate constants and the overall mass transfer coefficient decrease. Increasing the voltage can enhance mass transfer and eliminate barriers. Ion transport primarily occurs in the RW solid phase, accounting for 93.89% of the total current. Additionally, RW-EDI shows superior specific energy consumption within a concentration range of 500 ppm to 8000 ppm, outperforming technologies like electrodialysis by reducing specific energy consumption from 8−15 kWh/kg-NH 4 + to 1.2−2.5 kWh/kg-NH 4 + . This study highlights RW-EDI’s potential for ammonia recovery, providing valuable insights for future applications in wastewater treatment.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Thermal-Mechanical Elastic-Plastic and Ductile Failure Model Calibrations for 304L Stainless Steel Alloy

Numerical simulations of metallic structures undergoing rapid loading into the plastic range require material models that accurately represent the response. In general, the material response can be seen as having four interrelated parts: the baseline response under slow loading, the effect of strain rate, the conversion of plastic work into heat and the effect of temperature. In essence, the material behaves in a thermal-mechanical manner if the loading is fast enough so when heat is generated by plastic deformation it raises the temperature and therefore influences the mechanical response. In these cases, appropriate models that can capture the aspects listed above are necessary. The material of interest here is 304L stainless steel, and the objective of this work is to calibrate thermal-mechanical models: one for the constitutive behavior and another for failure. The work was accomplished by first designing and conducting a material test program to provide data for the calibration of the models. The test program included uniaxial tension tests conducted at room temperature, 150 and 300 C and at strain rates between 10 –4 and 10 3 1/s. It also included notched tension and shear-dominated compression hat tests specifically designed to calibrate the failure model. All test specimens were extracted from a single piece of plate to maintain consistency. The constitutive model adopted was a modular $J_2$ plasticity model with isotropic hardening that included rate and temperature dependence. A criterion for failure initiation based on a critical value of equivalent plastic strain fitted the failure data appropriately and was adopted. Possible ranges of the values of the parameters of the models were determined partially on historical data from calibrations of the same alloy from other lots and are given here. The calibration of the parameters of the models were based on finite element simulations of the various material tests using relatively ne meshes and hexahedral elements. When using the model in structural finite element calculations, however, element formulations and sizes different from those in the calibration are likely to be used. A brief investigation demonstrated that the failure initiation predictions can be particularly sensitive to the element selection and provided an initial guide to compensate for the effect of element size in a specific example.

36 MATERIALS SCIENCE↗
DOE OSTI2020

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

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

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2024

An experimental, theoretical, and kinetic modeling study of post-flame oxidation of ammonia

The post -flame oxidation rate of ammonia was investigated in a novel atmospheric pressure flow reactor at temperatures of 1280 ± 16 K and as a function of residence time and mixture composition (1-10% O 2 , dry and moist). The experimental results, as well as selected data from literature, were analyzed using an updated detailed chemical kinetic model. The medium temperature, very lean conditions enhance the importance of reactions of the nitroxyl (HNO) intermediate. High-level theory was used to calculate the rate constant for HNO + NH 2 , indicating that this step is significantly faster than values used in literature. Furthermore, a trajectory based approach was used to determine collision efficiencies for selected bath gases for HNO + M. The experimental results show that the NH 3 oxidation rate increases with temperature and O 2 concentration, while the presence of water vapor slightly inhibits reaction. Formation of NO and N 2 O was strongly promoted at higher levels of O 2 . Modeling results agreed well with the measurements, except at the lowest level of O 2 . The predicted oxidation rate of NH 3 was shown to result from a delicate balance between chain branching and terminating steps involving NH 2 , H 2 NO, and HNO. Recent theoretical work on reactions of these species by Klippenstein and coworkers and Stagni et al. was instrumental in improving modeling predictions. After initiation, NO reached a pseudo -steady-state level, where the pathways to NO were largely balanced by the NH 2 + NO reaction. Nitric oxide was partly oxidized to NO 2 , with the NH 2 + NO 2 reaction responsible for most of the N 2 O formation. Novelty and significance statement: This study provides the first detailed kinetic analysis of the lean postflame oxidation of ammonia, based on time -resolved flow reactor data in a novel reactor. In addition to the post -flame oxidation rate of ammonia, data for formation of NO and N 2 O were compared with modeling predictions. The medium temperature, very lean conditions enhance the importance of reactions of the HNO and H 2 NO intermediates. Inclusion in the model of results from recent high-level theoretical work, including present calculations for HNO + NH 2 and HNO + M, was crucial for capturing the observed behavior. It is argued that the post -initiation steady-state NH 3 oxidation rates constitute important data for model validation, along with ignition delays and laminar flame speeds.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Controlling Structural, Electronic, and Energy Flow Dynamics of Catalytic Processes through Tailored Nanostructures

MoS 2 (molybdenum disulfide) is a highly-versatile catalyst material for support of numerous reactions from hydrodesulfurization and denitrogenation to the focus of this renewal proposal: hydrogenation of CO/CO 2 towards (higher) alcohols. At the same time, MoS 2 is a non-toxic, environmentally-benign and rather inert material- which under ambient conditions for some time has served as a lubricant and, more recently, as next-generation electronic material. The apparent contrast between inertness and stability in ambient, and catalytic activity under reactive conditions is puzzling and calls for a synergistic theoretical and experimental investigation with the long-term objective of enabling the rational design of MoS 2 -based catalysts for alcohol-formation reactions by providing a microscopic understanding of the environmental factors that determines site activity and selectivity. Our research project seeks answers to the questions (a) what conformation does MoS 2 adopt under reaction conditions (as opposed to that under ultrahigh vacuum and low temperatures)?; (b) what reaction pathways exist on such a material?; (c) how can the local environment of the active sites be manipulated so as to make MoS 2 an efficient catalyst for production of higher alcohol from syngas? In particular, research strategies will explore how the basal plane composed of sulfur atoms can be activated so as to exhibit a reactivity of its own, by addressing three research targets and building on extensive preliminary and enabling work: (1) vacancies and vacancy aggregates on the basal plane; (2) non-local catalyst transformation through alkali doping, hydrogenation and phase transition; (3) fabrication of a metal-nanoparticle-activated MoS 2 system, in which particle anchoring, reactive sites and pathways as well as selectivity are controlled by design, as an example of predictive development of a catalyst material,. All strategies are directed to improve the efficacy of the key reactive sites and selectivity of chemical pathways by design, to replace the inefficient methodology of trial and error in catalyst development. This research project represents a synergistic combination of computational guidance, foundational surface-science-based experiments and validation under reactive conditions that aims at transformative new insights into the working of MoS 2 -based hydrogenation-catalysts, a topic squarely at the center of the interest of DOE BES. Guided and led by Talat Rahman, a computational physicist, this project will apply density functional theory to understand structure, reaction pathways and chemical potentials associated with MoS 2 -based CO/CO 2 hydrogenation, augmented by kinetic Monte Carlo methods for reaction rates and prefactors as well as ab-initio molecular dynamics for evaluation of thermal stability. Complementary experimental input and validation will originate from co-PI Ludwig Bartels, a physical chemist and materials scientist, whose group focuses on local imaging and preparation of MoS 2 materials, from co-PI Peter Dowben, an experimental physicist, whose group is expert in the spectroscopy of occupied and unoccupied electronic states, and from senior collaborator Michael White of Brookhaven National Laboratory, whose group generates high-resolution electronic and activity information on size-selected well-defined metal chalcogenide clusters. This collaborative effort will enable a comprehensive understanding of the correlation of structural integrity and catalytic activity of MoS 2 in forms ranging from extended films to individual particles with known geometries and binding sites. Alcohol formation from syngas is a rapidly emerging application that has great potential through facile, economic, and decentralized biomass gasification. CO 2 activation is one of the most pressing concerns of our time: increasing CO 2 levels in the atmosphere change the climate and expose the globe to environmental transformations with the potential for enormous economic and societal impact. We will investigate CO/CO 2 hydrogenation via an interdisciplinary research collaboration with established synergy – one that, in accordance with the mission of the DOE, involves accredited Hispanic-Serving Institutions and that, through student exchange with international collaborators and National Labs, will directly benefit a broad spectrum of communities and generate human resources in sciences essential to their future.

2D materials↗
DOE OSTI2025

Selective Electrochemical Reduction of CO 2 to Metal Oxalates in Nonaqueous Solutions Using Trace Metal Pb on Carbon Supports Enhanced by a Tailored Microenvironment

In this work, the electroreduction of carbon dioxide (CO 2 ) to oxalate is enabled by incorporating trace metallic lead (Pb) on carbon‐based supports (CBS) with polymer overlayers. These composite materials serve as an efficient electrocatalytic system for the facile conversion and storage of CO 2 , a pernicious atmospheric pollutant. Results from controlled potential electrolysis experiments indicate that 1) trace metallic Pb on the ppb scale is active toward the reductive coupling of CO 2 to oxalate at comparable Faradaic efficiencies to bulk metallic Pb and 2) polymer encapsulation of this trace metallic Pb leads to promotion of CO 2 reduction (CO 2 R) selectively to metal oxalates over other products such as CO. Importantly, metal oxalates are important alternative cementitious materials and precursors for other materials’ synthesis applications. The solid products undergo rigorous spectroscopic characterization, including 13 CO 2 labeling experiments, to ensure the metal oxalates are in fact produced from CO 2 R. These findings serve as a model for leveraging microenvironment effects to enhance activity and selectivity for CO 2 R using trace‐metal catalysts for carbon utilization and storage technologies.

alternative cementitious materials↗
DOE OSTI2023

Revolutionizing Porous Liquids: Stabilization and Structural Engineering Achieved by a Surface Deposition Strategy

Facile approaches capable of constructing stable and structurally diverse porous liquids (PLs) that can deliver high-performance applications are a long-standing, captivating, and challenging research area that requires significant attention. Here, in this work, a facile surface deposition strategy is demonstrated to afford diverse type III-PLs possessing ultra-stable dispersion, external structure modification, and enhanced performance in gas storage and transformation by leveraging the expeditious and uniform precipitation of selected metal salts. The Ag(I) species-modified zeolite nanosheets are deployed as the porous host to construct type III-PLs with ionic liquids (ILs) containing bromide anion , leading to stable dispersion driven by the formation of AgBr nanoparticles. The as-afforded type-III PLs display promising performance in CO 2 capture/conversion and ethylene/ethane separation. Property and performance of the as-produced PLs can be tuned by the cation structure of the ILs, which can be harnessed to achieve polarity reversal of the porous host via ionic exchange. The surface deposition procedure can be further extended to produce PLs from Ba(II)-functionalized zeolite and ILs containing [SO 4 ] 2– anion driven by the formation of BaSO 4 salts. The as-produced PLs are featured by well-maintained crystallinity of the porous host, good fluidity and stability, enhanced gas uptake capacity, and attractive performance in small gas molecule utilization.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Molten Salt Reactor Experiment Benchmark Evaluation

As one of the six advanced reactor concepts selected by the 2002 Generation IV roadmap as a technology meriting future research, Molten Salt Reactors (MSRs) attracted broad attention and multiple private and public entities are working towards its commercialization. Facing stringent regulatory requirements, validations of computational codes used to calculate and prove the safety characteristics of MSRs play a key role. This project developed the world-first, MSR-related reactor physics benchmark based on a series of zero-power experiments conducted at the Molten Salt Reactor Experiment (MSRE). The benchmark was successfully reviewed by the International Reactor Physics Experiment Evaluation Project (IRPhEP) committee and is available in the IRPhEP handbook starting form the 2019 edition. To benchmark experimental data from the MSRE, a three-dimensional high-fidelity model was developed using the Monte Carlo neutron transport code Serpent 2 and ad-hoc methods have been implemented to account for the unique feature of fuel salt motion. The calculated effective multiplication factor, k eff , for the first criticality experiment, when 235 U was progressively added to the fuel salt in order to achieve criticality with stationary salt and isothermal conditions, was 1.02132 (±3 pcm). The total uncertainty for experimental k eff was estimated to be 420 pcm. The calculated k eff is 2.154% larger than the experimental and benchmark model value, which is approximately five times the benchmark model uncertainty. It is to be noted that, for systems containing large volume of graphite (or other carbonaceous materials), Monte Carlo codes tend to overestimate the keff of the benchmark model by 1% to 2%. The bias is possibly due to uncertainties in the impurity content of the graphite blocks, uncertainty in the neutron capture cross section of carbon or uncertainty in the properties of nuclear-grade graphite. The calculated reactivity coefficient of 235 U concentration (0.2228 ± 0.0014, represented as the change of reactivity over the relative change of 235 U mass in loop) matches well with the experimental value (0.223 ± 0.006), strengthening the confidence on the accurate representation of the fuel salt composition in the MSRE benchmark. Additional reactivity effect calculations, including the control rod bank worth, reactivity effects of fuel circulation and isothermal and fuel temperature coefficients show good agreement with the experimental values (within 1σ) as well.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
DOE OSTI2024

Soil Desiccation Treatability Testing at BC Waste Disposal Cribs

During Hanford’s production period, low-level waste products generated from chemical processing of uranium fuel rods were discharged directly to the ground through a system of cribs and trenches located in the 200-BC-1 Operable Unit (OU). The site consists of 6 cribs and 20 trenches that received more than 117,000 m3 of radioactive liquid waste discharged to the soil. These unlined infiltration galleries held volumes of liquid waste while it seeped into the ground, with the understanding that the 100 m (330 ft) thick vadose zone in the area would effectively capture the effluent and prevent groundwater impacts. A conceptual model showing the operation of cribs and trenches is shown in Figure 1. Data show effluent from the 26 cribs and trenches containing about 410 curies of Technetium-99 (Tc-99) is primarily located between 30 m and 70 m (98 ft and 230 ft) depth (Corbin et al., 2005; Ward et al., 2004). Despite no evidence indicating that the contamination has reached the groundwater at BC cribs and trenches, the mobility of Tc-99 had been demonstrated in laboratory tests and was recognized as a threat to groundwater at the site. Using data from numerical models, laboratory analyses, field investigations, and information on historical discharges, the EPA and Ecology identified Tc-99 and U contamination of the vadose zone as a remediation priority. The U.S. DOE was notified by EPA and Ecology regarding risks associated with Tc-99 contamination in a letter requesting development of a strategy for improved methods to understand the nature and extent of vadose zone contamination, specifically Tc-99, and to develop remedial options for addressing such contamination. To develop the appropriate technology for characterizing, remediating, and monitoring the deep vadose zone Tc-99 contamination, the U.S. DOE worked with the EPA and Ecology to create a Treatability Test Plan under a Remedial Investigation/Feasibility Study (RI/FS) for the Hanford 200 Areas. Under this RI/FS, it was determined that a treatability test for soil desiccation should be carried out as it was identified as a promising in-situ treatment technology for mitigating risks posed by Tc-99 contamination to the groundwater table. The BC Cribs and Trenches site was identified as a representative site for Tc-99 and U contamination and selected for the soil desiccation treatability test. In this chapter, we summarize the overlying regulatory framework of RI/FS and treatability tests and illustrate how development and experimentation supported the evaluation of selected remedies. We briefly discuss the RI/FS for the 200 Areas of the Hanford Site and focus on the soil desiccation treatability testing performed at the BC cribs and trenches site under the Deep Vadose Zone Treatability Test Plan for the Hanford Central Plateau (DVZ-TT). The DVZ-TT is one component of the remedial investigation/feasibility study for the Hanford 200 Areas and represents the underlying regulatory framework that drives site operations towards records of decision and site closure.

Mangel, Adam R.↗
DOE OSTI2025

Advanced Computational Modeling of High-Level Waste Vitrification at the Hanford Site

The U.S. Department of Energy (DOE) has selected vitrification for stabilizing legacy tank waste at the Hanford site, where radioactive waste from plutonium production was historically stored in underground tanks. This waste will be separated into low-activity waste (LAW) and high-level waste (HLW) fractions and processed at the Waste Treatment and Immobilization Plant (WTP). At WTP, glass melters are used for the vitrification of radioactive tank waste, transforming it into a stable borosilicate glass form for safe long-term storage. The melter vessel is constructed from highly durable and heat-resistant materials, where the vitrification process occurs. The main regions that are modeled are the melt pool, plenum, cold cap, riser/discharge chamber, and surrounding structure with insulation layers. Forced convection induced by air bubblers at the base of the melter ensure uniform temperature distribution and provide heat to the cold cap layer. The cold cap is a region of reacting batch feed that floats on top of the molten glass and is where the batch-to-glass reactions occur. Joule heating provided by electrodes mounted along the vertical walls of the melter and immersed directly in the glass, generates the necessary heat for the net endothermic conversion processes that occur in the cold cap. The high temperatures, radioactivity, and opaque nature of the glass prevent direct observation inside the melters. Therefore, computational models are essential for providing insight into factors that affect melter throughput. Thermocouples in the plenum provide operators with plenum temperature measurements. Operational adjustments include bubbling rate, voltage supplied to the electrodes, feed adjustments, and glass removal rate. Different computational fluid dynamics (CFD) models have been developed, each serving a specific purpose. There are CFD models of different scale melters, as well as models that capture the two-phase flow interfaces of rising bubbles in the molten glass or models with a simplified molten glass region so that the surrounding structure and plenum can be feasibly incorporated. Pilot-scale melter models have been developed to serve as validation of the methods employed in the simulation of the full-scale WTP melters. Models incorporating resolved bubbling are used to develop momentum source terms to implement into a single phase, multi-region, steady-state flow model that is being validated by measured process parameters such as glass production rate, voltage, input power, plenum temperatures, etc. The resolved bubbling model uses the multiphase volume of fluid approach to model the system with a high-resolution interface capturing scheme to maintain sharp interfaces between the molten glass and the air phase. The suite of CFD models is continually being improved to incorporate more realistic physics and achieve faster turnaround time. For example, an incremental controller is implemented to automatically adjust electrode voltage within the simulation to a molten glass set point temperature of 1150°C. Newer models feature improved meshes to ensure conformal meshes between regions and eliminate unnecessary mesh refinement in areas that are not of interest (such as boundary layers in offgas ports). Instead of explicitly modeling the structural, refractory, and insulation layers of the melter, a thermal resistance approach is used with published correlations used for boundary conditions. The development of robust and efficient CFD models will be instrumental in enabling the WTP to successfully fulfill its mission of safely stabilizing legacy nuclear waste.

12 - MGMT OF RADIOACTIVE AND NON-RADIOACTIVE WASTE↗
DOE OSTI2020

Implicit fast sweeping method for hyperbolic systems of conservation laws

Implicit time-accurate methods are often used to integrate stiff problems where explicit schemes impose severe time step restrictions. This paper presents an efficient numerical framework based on the Fast Sweeping Method (FSM) for solving linear and nonlinear hyperbolic systems of conservation laws. The solution at each discrete location is computed by sweeping the numerical domain in several predetermined directions that follow the causality of the characteristic families. The use of a fractional step strategy eliminates the need for a solution selection criterion while one-sided stencils limit the number of sweeps to at most 2 d for d space dimensions. This work focuses on the first-order implicit upwind method since it constitutes the building block for high-order conservative schemes. For problems where the degree of stiffness evolves over time, implicit-explicit hybridization can be accomplished with the same algorithm by simply switching the stencil at each time level. As opposed to traditional implicit solvers, the sweeping method does not require a local time linearization of the fluxes thereby preserving the nonlinear stability properties of the original implicit scheme. It also avoids the large computational and memory requirements associated with solving large block-diagonal systems of equations. Here, a series of one- and two-dimensional test cases are presented for the inviscid Burgers' equation and the reactive Euler equations. The results indicate that the implicit FSM can allow a major reduction in the number of time steps even in the presence of discontinuous solution profiles.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2026

Local Structural Coherence and Interfacial Charge Transfer in Cu 2 ⁢S/Mo⁢S 2 Heterostructure

Precise control over electronic coupling at nanoscale interfaces is critical for designing materials with tunable charge-transfer behavior and catalytic function. Heterostructures with locally coherent interfaces provide a platform for interrogating interfacial charge redistribution in coupled material systems. Here, we report Cu 2 ⁢S/Mo⁢S 2 heterostructures exhibiting nanoscale crystallographic alignment, which are synthesized through a rapid thermal transformation pathway. We employed electrochemical reduction reactions to probe interfacial charge transfer, revealing shifts in product distribution attributable to modified interfacial energetics, even in the absence of optimized catalytic performance. The observed formate Faradaic efficiency suggests that interfacial electronic modulation in the heterostructure shifts product selectivity towards formate, highlighting how interface-driven electronic modulation can direct reaction pathways and influence product selectivity. Optimizing catalyst loading, architecture, and reactor configuration will be critical for future improvement. Structural and compositional integrity were confirmed through powder x-ray diffraction, x-ray photoelectron spectroscopy, and high-resolution transmission electron microscopy. Electron transfer between Cu 2 ⁢S and Mo⁢S 2 domains was further evaluated by electrochemical impedance spectroscopy, while selected-area electron diffraction revealed local crystallographic alignment consistent with a local epitaxial relationship at the Cu 2 S/Mo⁢S 2 heterointerface. To illustrate the broader applicability of this approach, a Zn⁢S/Mo⁢S 2 heterostructure was also synthesized using the same microwave strategy, confirming the generalizability of interfacial engineering principles across metal sulfide-Mo⁢S 2 systems. Collectively, these findings demonstrate that controlled local epitaxial alignment serves as an effective design principle for tuning interfacial energetics and catalytic reactivity in complex heterostructure materials.

carbon capture & utilization↗
DOE OSTI2022

Hydrogen Storage for Load-Following and Clean Power: Duct-firing of Hydrogen to Improve the Capacity Factor of NGCC Plants (Final Report, Phase I Conceptual Study)

The 12-month Feasibility study in Phase I study was completed and confirmed the system is feasible and the proposed system is an improvement over alternate low carbon dispatchable power options. Our demonstration will include 54 MWh of hydrogen storage. CO 2 capture inherent to the CHG process can capture 90% of the CO 2 (with upgrades to >98%) in a commercial system (~300 MWth) for sequestration or other uses. The hydrogen will be utilized in a duct burner in a Heat Recovery Steam Generator (HRSG) integrated with the existing Southern Company fossil asset. Here, the firing rate of the duct burner is varied to let the plant respond to fluctuations of electrical load. However, H 2 production is relatively constant by storing H 2 , and revenues are improved by arbitrage between use of low-cost off-peak variable electricity generation or use of stored H 2 under peak demand. The study enabled the fidelity of the concept to be improved and allowed identification of the requirements for the system. Defining the individual system and component requirements was performed via system requirements review with the whole team. These requirements were then incorporated into/iterated with our Heat & Mass Balance models and process flow diagrams were generated to reflect the overall system. This information was then used to complete the TEA and show economic feasibility. Our system generates power at 17.4% lower cost than other low carbon approaches for the H 2 generation, H 2 compression and storage, carbon sequestration, and HRSG added electricity production for a large-scale duct-fired system. Our team recommends completing the Phase II Pre-FEED study for the proposed system as the next step for the project and its tasks will achieve the overall objective and be ready to launch the FEED. The Pre-FEED tasks include updating the requirements, Concept of Operations, plant scope/process description, component modeling, system modeling, performance estimates, emission estimates, block flow diagrams, fluid/process conditions (PFD), utility usage, and facility sizing/definition. The approach will be to complete these updates in a greater level of detail for the selected site. The approach for developing the EIV is to use the updated results, including model outputs, for carbon dioxide and waste streams.

03 NATURAL GAS↗
DOE OSTI2024

Local ionic transport enables selective PGM-free bipolar membrane electrode assembly

Bipolar membranes in electrochemical CO 2 conversion cells enable different reaction environments in the CO 2 -reduction and O 2 -evolution compartments. Under ideal conditions, water-splitting in the bipolar membrane allows for platinum-group-metal-free anode materials and high CO 2 utilizations. In practice, however, even minor unwanted ion crossover limits stability to short time periods. Here we report the vital role of managing ionic species to improve CO 2 conversion efficiency while preventing acidification of the anodic compartment. Through transport modelling, we identify that an anion-exchange ionomer in the catalyst layer improves local bicarbonate availability and increasing the proton transference number in the bipolar membranes increases CO 2 regeneration and limits K + concentration in the cathode region. Through experiments, we show that a uniform local distribution of bicarbonate ions increases the accessibility of reverted CO 2 to the catalyst surface, improving Faradaic efficiency and limiting current densities by twofold. Using these insights, we demonstrate a fully platinum-group-metal-free bipolar membrane electrode assembly CO 2 conversion system exhibiting <1% CO 2 /cation crossover rates and 80-90% CO 2 -to-CO utilization efficiency over 150 h operation at 100 mA cm -2 without anolyte replenishment.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Polymer-Derived Amorphous Aluminosilicate Nanomembranes for H 2 Purification

Aluminosilicate zeolite membranes with robust microporous crystalline structures are attractive for the molecular separation of H 2 from light gases, but their large-scale fabrication is complicated and costly, hindering their practical applications. Herein, we present polymer-derived amorphous aluminosilicate nanomembranes that combine the exceptional processability of polymers with the superior gas separation properties of aluminosilicates. Specifically, thin-film composite membranes comprising 150 nm polydimethylsiloxane were first treated with oxygen plasma to generate 10 nm polyorganosilica (POSi) on the surface, which were then subjected to few-cycle atomic layer deposition (ALD) using trimethylaluminum as a metal precursor and water vapor as a coreactant. This scalable two-step process yields few-nanometer amorphous aluminosilicates with strong size-sieving ability. For example, three-cycle ALD treatment of POSi increases H 2 /CO 2 selectivity from 39 to 200 and H 2 /CH 4 selectivity from 190 to 500, while decreasing H 2 permeance from 990 to 210 GPU at 150 °C, superior to the state-of-the-art membranes. In conclusion, rapid and scalable manufacturing of amorphous aluminosilicate nanolayers can also be of interest for catalysis and adsorption applications.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Direct observations and characterization of crack closure during microstructurally small fatigue crack growth via in-situ high-energy X-ray characterization

This study provides direct observation of the crack closure mechanism of a naturally occurring, tortuous, 3D microstructurally small fatigue crack (SFC) in additively manufactured Inconel 718. In-situ non-destructive characterization is performed using high-energy X-ray diffraction techniques to capture the evolution of the 3D microstructure and micromechanical response in the vicinity of the crack front. Based on the stress state of twelve grains analyzed at the crack tip, the crack closure events of the SFC front was found to be spatially heterogeneous with respect to loading progression governed by the local stress state of the grains (specifically the stress reversal from compression to tension). From this analysis, three grains that displayed different degrees of crack closure were further investigated, based on the orientation of the crack relative to the grains and the associated modality of crack growth. The stress normal to the crack plane and the associated degree of Mode I crack behavior were correlated with events of the crack opening earlier during the loading cycle. This was further corroborated by diffraction spot spreading analysis that quantified the crystallographic lattice distortion caused by the opening crack. Additionally, the detailed characterization of the opening behavior of the grains located at the crack tip and their associated states of stress elucidates the mechanism governing crack closure and will inform future modeling efforts of this phenomenon.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Next Generation Co-Molded One-Piece Automotive Parts

The purpose of this project was to determine the feasibility of co-molding Class A Sheet Molding Compound (SMC), structural SMC, and continuous fiber prepreg materials to produce a single piece co-molded automotive part, such as a hood. The combination of the three molding materials and the incorporation of selective design features (ribs, flanges, corrugations) was expected to eliminate the need for inner reinforcement panels, significantly reducing tooling costs and simplifying the manufacturing process. A multi-material solution would also result in significant weight savings. The scope of this project included the material characterization of the three materials, development of cure and flow simulation models, and validation of the models against parts molded with different combinations of the materials on an 11”x11” plaque tool with rib features. The intent of this project was to apply the learnings obtained from co-molding a part with simplified geometry to a Phase 2 project that would produce a single piece hood, co-molded with the same materials. Resins from INEOS Composites were provided to IDI to produce SMC and continuous fiber prepregs. Purdue University and INEOS Composites characterized the rheological and curing behavior of the different materials as well as the mechanical properties of the co-molded parts. This data was used by Purdue University to create simulation models. Models were created to predict both flow patterns and predict mechanical properties of different laminate constructions in and around the ribs. Michigan State University - Corktown validated Purdue’s models by co-molding the three materials in different combinations on a tool containing rib features provided by Century Tool. The co-molded parts were evaluated against the simulation models by Purdue, Corktown and INEOS. The project team demonstrated the following: • The ability to obtain a cohesive co-molded structure made up of Class A SMC, Structural SMC, and continuous fiber prepreg. • The ability to obtain a co-molded part with a Class A surface • Modeling of flow and fiber orientation • Modeling to predict mechanical properties of multi-material co-molded structures The predicted flow behavior and fiber orientation from simulations were then compared with the molded samples. Exact local orientation state was difficult to compare between microscopy and flow simulation, but captured general trends. Multi-material flow behavior was generally modeled well with SMC materials, but the introduction of woven material sheets requires further model development. Purdue compared the predicted versus actual mechanical properties, and INEOS Composites evaluated the surface appearance of unpainted and painted co-molded parts. The models developed by Purdue demonstrated that the mechanical properties can be predicted for parts with varying material configurations. The resulting models can be applied to future co-molded part design, tooling design, and molding conditions.

36 MATERIALS SCIENCE↗