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DOE OSTI2023

Understanding the Effect of Electrochemical Properties and Microstructure on the Microgalvanic Corrosion of Mg Alloys via Phase-Field Simulations

In this work, we apply a phase-field model to gain insights into the corrosion behavior of Mg alloys. Specifically, we study the effect of electrochemical properties of the materials and their environment and the spatial distribution of second phases in a magnesium alloy. To this end, we perform sensitivity analyses in which we separately vary the exchange current density and corrosion potential of the second phase, as well as the electrolyte conductivity. We describe the effects of these parameters on the corrosion current and the resulting corrosion-front morphology. We also confirm that the ratio between the Wagner length, calculated for the anodic phase, and the initial width of the anodic domain is a good predictor of the morphological characteristic of the corroding surface. In addition, we examine the effect of the microstructure on the corrosion behavior in both 2D and 3D systems by varying the shape, size, and distribution of the second-phase regions. Our findings provide insights into the influence of the two-phase microstructure on the corrosion behavior in a magnesium alloy.

Electrochemistry↗

DOE OSTI2025

Mantaray: A Rust Package for Ray Tracing Ocean Surface Gravity Waves

Ocean surface gravity waves are an important component of air-sea interaction, influencing energy, momentum, and gas exchanges across the ocean-atmosphere interface. In specific applications such as refraction by ocean currents or bathymetry, ray tracing provides a computationally efficient way to gain insight into wave propagation. In this paper, we introduce Mantaray, an open-source software package implemented in Rust, with a Python interface, that solves the ray equations for ocean surface gravity waves. Mantaray is designed for performance, robustness, and ease of use. The package is modular to facilitate further development and can currently be applied to both idealized and realistic wave propagation problems (Fig. 1).

16 TIDAL AND WAVE POWER↗

DOE OSTI2020

Sample Preparation for 3D Characterization of Irradiated Fuel

Thorough characterization of nuclear fuel is essential when striving to understand its microstructural evolution in response to varying irradiation conditions. A detailed understanding of the microstructural evolution of irradiated fuel can be useful when predicting the fuel’s response to off-normal conditions and related phenomena such as high burnup fuel fragmentation (HBFF) and fission gas release. This sort of characterization and the study of complex phenomena like HBFF that are related to fuel performance are an important part of the US Department of Energy Office of Nuclear Energy’s Advanced Fuels Campaign (AFC). Multiple characterization techniques are commonly used to perform post-irradiation examination (PIE) analysis on an irradiated fuel sample, but many of these techniques are limited to the 2D surface analysis of the fuel pellet. Although there is a lot of useful information to be gained by analyzing the fuel pellet surface, a 2D analysis provides only an approximation of the nature of the material’s features, such as porosity and grain structure. Therefore, it is critical to analyze the 3D structure of the material, as materials exist and respond to conditions in all three dimensions.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2023

Department of Energy’s Atmospheric System Research (ASR) Program’s Workshop on the Future of Atmospheric Large Eddy Simulation (LES): Workshop Report

Large-eddy simulation (LES) is used as a tool to understand physical processes such as turbulence, aerosols, clouds, precipitation, radiation, the interactions among all these, and their interactions with the underlying surface. Over the next 10 years, LES will drive fundamental progress in open scientific questions in these areas as LES is increasingly used to gain understanding of complex interacting physical processes involving atmospheric turbulence. This growth will be driven both by scientific demand and the expansion of computational resources needed to conduct LES, and the form that the growth takes will largely be determined by how computational resources are leveraged for scientific gain. In particular, we suggest that computational resources are likely to be leveraged in two separate but not necessarily distinct ways. On one hand, growth in computational resources will allow LES to be made more routine, that is, performed more frequently, while on the other hand, the computational expense (measured in total floating point operations) afforded to individual LES will expand dramatically, allowing simulations to increase in both domain size and resolution as well as physical detail. Current U.S. Department of Energy (DOE) projects such as LES ARM Symbiotic Simulation and Observation Activity (LASSO) are leading the way in conducting routine LES, building large, public databases that are accessible for data science, sensitivity studies, and training for machine learning. LES will also become more routine as it becomes more accessible for individual researchers to address their scientific questions of interest. Scientific questions addressed by LES over the next 10 years are likely to include cloud organization and aggregation; aerosol cloud interactions and atmospheric chemistry (including geo-engineering); urban-scale LES; atmospheric extreme events, ranging from small-scale severe weather to wildfires; and ocean-wave-atmosphere interactions. Further LES-related research will likely grow significantly in areas related to societal impact studies of air quality and extreme weather events, applications to renewable energy forecasting and resource assessment, and aid in decision-making processes. The growth in the use of LES in atmospheric science research will drive the need for better physical process representations (e.g., cloud aerosol microphysics, radiation, and atmospheric chemistry) at the scales resolved by LES. To date, many of the process representations used by LES have been taken directly from coarser-resolution models. Promising methods for LES process representations include superdroplet and quadrature methods for microphysics, 3D approaches for radiation, and better representation of chemistry and aerosol processes. At LES resolution, land-atmosphere interactions for complex terrains, land cover/types, biogeochemistry, and plant canopy models are needed as an improvement beyond traditional and widely used Monin-Obuhkov similarity theory.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Department of Energy’s Atmospheric System Research (ASR) Program’s Workshop on the Future of Atmospheric Large Eddy Simulation (LES) (Workshop Report)

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Department of Energy’s Atmospheric System Research (ASR) Program’s Workshop on the Future of Atmospheric Large Eddy Simulation (LES) (Workshop Report)

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Excessive Aurantiochytrium acetophilum docosahexaenoic acid supplementation decreases growth performance and breast muscle mass of broiler chickens

We report Docosahexaenoic acid (DHA) is an n-3 polyunsaturated fatty acid with health-promoting potential. This study was to investigate effects of supplemental DHA from Aurantiochytrium acetophilum on growth performance, health status, meat quality, and protein synthesis signaling of broiler chickens. Day-old male chicks were housed in an environmental control room (6 cages/treatment, 8 chicks/cage), and fed a corn-soybean meal basal diet supplemented with the DHA-rich A. acetophilum biomass (Heliae, Gilbert, AZ) at 0, 1, 2, and 4% (0, 1.7, 3.4 and 6.8 g DHA/kg diet) for 6 weeks. Growth performance was measured weekly. Blood samples were collected at weeks 3 and 6 (2 chicks/cage). Four tissues were sampled (2 chicks/cage) for biochemical and meat quality analyses. Data were analyzed by one-way ANOVA and regression. Compared with the control, the 4% A. acetophilum diet decreased (p < 0.05) body weight gain (19%) and gain to feed ratio (19%) during weeks 4–6. The A. acetophilum supplementation dose-dependently decreased (p < 0.05, R 2 = 0.21–0.54) plasma alanine amino transferase activity and glucose concentrations, but had little effect on plasma activity of alkaline phosphatase or concentrations of inorganic phosphorus and uric acid at weeks 3 and 6. Compared with the control, the 4% A. acetophilum diet decreased (p < 0.05) breast muscle weight by 21%, and down-regulated (p < 0.05) mRNA levels of mammalian target of rapamycin and ribosomal s6 protein (S6), and protein levels of phosphorylated S6 to S6 and phosphorylated S6 kinase beta 1 to S6 kinase beta 1. The A. acetophilum supplementation linearly increased (p < 0.01) lipid peroxidation (R 2 = 0.62–0.90) and hardness and chewiness (R 2 = 0.34–0.44) of breast and thigh muscles. In conclusion, supplemental 4% (6.8 g DHA/kg), but not 1 or 2%, of A. acetophilum impaired growth performance, breast muscle mass accumulation, and(or) protein synthesis signaling of broilers.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2021

Supplemental dietary full-fatted and defatted Desmodesmus sp. exerted similar effects on growth performance, gut health, and excreta hydrothermal liquefaction of broiler chicks

This study determined effects of full-fatted (C046, 41% crude protein) and lipid extracted (LEA, 39% crude protein) microalgae Desmodesmus sp. on growth performance, gut health, and excreta hydrothermal liquefaction of broiler chickens. Two experiments were conducted by feeding day-old Cornish male chicks: 1) a corn-soybean meal basal diet (control) 2) control +5% C046, or 3) control +5% LEA for 2 weeks. Growth performance was measured weekly in both experiments. Blood, liver, and duodenum samples of chickens were collected for biochemical analyses, and excreta samples were collected for hydrothermal liquefaction (300 °C, 60 min) at the end of Experiment 2. Compared with the control, supplemental dietary C046 and LEA enhanced average daily gain (13% to 40%, p < 0.05) in both experiments, and improved feed efficiency (15% and 11%, p < 0.01) in Experiment 2. The C046 and LEA diets enhanced the duodenum (19% to –2 fold, p < 0.05), but decreased the liver (17 to 78%, p < 0.05) mRNA abundances of interleukins-1, 6 and 8 and (or) tumor necrosis factor-α, respectively, compared with the controls. Meanwhile, the two types of biomass enhanced the protein amounts of claudin-1 in the duodenum (5–34%, p < 0.05) than the controls. Hydrothermal liquefaction of the excreta derived from the three diets showed no major differences in total bio-crude oil (average of 23%), hydrochar yield (average of 12%), or elemental compositions. However, the heating values of the resultant two bio-crude oils from the microalgae-fed chicken excreta (average of 34 MJ/kg) were 16% greater than those from the control chickens (29 MJ/kg). In conclusion, supplementing the full- and de-fatted Desmodesmus sp. microalgal biomass in the starter diets for broiler chickens produced largely similar improvements of growth performance, gut health, and excreta-derived oil quality.

09 BIOMASS FUELS↗

DOE OSTI2024

Progress in development of characterization capabilities to evaluate candidate materials for direct air capture applications

As part of U.S. national efforts to combat the detrimental effect of global climate change, the National Institute of Standards and Technology (NIST) was recently tasked to support efforts in direct air capture (DAC) of carbon dioxide research and deployment. In order to develop test procedures, materials, and documentary standards, key characterization methods relevant to DAC materials have been investigated and used to identify desirable properties for a potential Standard Reference Material (SRM). Select amine-supported materials that previously showed potential for DAC applications have been characterized using commonly available laboratory methods. Further insights into the adsorption characteristics have been gained from developing and applying more specialized characterization tools ideal for probing low concentrations of carbon dioxide. A broad suite of capabilities that examine relevant properties under appropriate conditions gives the most profound insights into a material's specific performance. We advocate for even more specialized capabilities to be developed and standardized to quantitatively monitor the interactions of CO 2 with molecular species in complex and often disordered systems to advance DAC and support carbon dioxide reduction (CDR) in general.

carbon dioxide↗

DOE OSTI2020

Ionic conductive polymers as artificial solid electrolyte interphase films in Li metal batteries – A review

Lithium (Li) metal has been considered as the ultimate anode material for next-generation rechargeable batteries due to its ultra-high theoretical specific capacity (3860 mAh g -1 ) and the lowest reduction voltage (-3.04 V vs the standard hydrogen electrode). However, the dendritic Li formation, uncontrolled interfacial reactions, and huge volume variations lead to unstable solid electrolyte interphase (SEI) layer, low Coulombic efficiency and hence short cycling lifetime. Designing artificial solid electrolyte interphase (artificial SEI) films on the Li metal electrode exhibits great potential to solve the aforementioned problems and enable Li–metal batteries with prolonged lifetime. Polymer materials with good ionic conductivity, superior processability and high flexibility are considered as ideal artificial SEI film materials. In this review, according to the ionic conductive groups, recent advances in polymeric artificial SEI films are summarized to afford a deep understanding of Li ion plating/stripping behavior and present design principles of high-performance artificial SEI films in achieving stable Li metal electrodes. Perspectives regarding to the future research directions of polymeric artificial SEI films for Li–metal electrode are also discussed. The insights and design principles of polymeric artificial SEI films gained in the current review will be definitely useful in achieving the Li–metal batteries with improved energy density, high safety and long cycling lifetime toward next-generation energy storage devices.

25 ENERGY STORAGE↗

DOE OSTI2020

Exploring the Effects of Node Topology, Connectivity, and Metal Identity on the Binding of Nerve Agents and Their Hydrolysis Products in Metal–Organic Frameworks

Recent studies have shown that metal–organic frameworks (MOFs) built from hexanuclear M(IV) oxide cluster nodes are effective catalysts for nerve agent hydrolysis, where the properties of the active sites on the nodes can strongly influence the reaction energetics. The connectivity and metal identity of these M6 nodes can be easily tuned, offering extensive opportunities for computational screening to predict promising new materials. Thus, we used density functional theory (DFT) to examine the effects of node topology, connectivity, and metal identity on the binding energies of multiple nerve agents and their corresponding hydrolysis products. By computing an optimization metric based on the relative binding strengths of key hydrolysis reaction species (water, agent, and bidentate-bound products), we predicted optimal M6 nodes for hydrolyzing specific nerve agent and simulant molecules, where our results are in qualitative agreement with observed experimental trends. This analysis highlighted the notion that no single metal or node topology is optimal for all possible organophosphates, suggesting that MOFs should be selected based on the agent of interest. Using the large amount of data generated from our DFT calculations, we then derived quantitative structure–activity relationship (QSAR) models to help explain the complex trends observed in the binding energies. Through linear regression, we identified the most important descriptors for describing the binding of nerve agents and their hydrolysis products to M6 nodes. These results suggested that both molecular and node properties, including both structural and chemical features, collectively contribute to the binding energetics. By performing a thorough statistical analysis, we showed that our QSAR models are capable of making quantitatively accurate binding energy predictions for nerve agents and their hydrolysis products in a wide variety of M(IV)-MOFs. In conclusion, the insights gained herein can be used to guide future experiments for the synthesis of MOFs with enhanced catalytic activity for organophosphate hydrolysis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Emerging investigator series: kinetics of diopside reactivity for carbon mineralization in mafic–ultramafic rocks

The ongoing use of fossil fuels to supply modern energy demands has necessitated research on combating carbon dioxide (CO 2 ) emissions and climate change. Carbon storage via mineral trapping in basalt and related rocks is a promising strategy. However, mineralization rates depend on the variable minerology that makes up these rock formations. Diopside (CaMgSi 2 O 6 ) is a common pyroxene mineral in ultramafic and mafic rocks including basalt, but relatively little work has been done to understand its carbon mineralization kinetics using hydrated supercritical CO 2 , which induces the formation of reactive nanoscale interfacial water films. Here, in situ XRD experiments at 50–110 °C and 90 bar indicate that diopside transforms into a myriad of Mg/Ca carbonates, including huntite [Mg 3 Ca(CO 3 ) 4 ] and very high magnesium calcite (VHMC, i.e., protodolomite). Through ex situ characterization, we were able to constrain reaction pathways for the dissolution–precipitation transformation process including metastable intermediate precipitates. Experiments performed at variable temperatures enabled Avrami-derived rate constants and an apparent activation energy of 97 ± 16 kJ mol –1 , implying the dissolution of diopside is the rate-limiting step. Density functional theory (DFT) calculations, used to gain molecular insight into the surface stability of the diopside during dissolution, suggest that exposed calcium cations are susceptible to dissolution when put in contact with water given their coordination environment. The collective results point to the high CO 2 mineralization potential of diopside in basalts, which could help guide parameterization of reactive transport models needed to design and permit commercial-scale subsurface carbon storage operations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Suppressing the enhancement of stimulated Raman scattering in inhomogeneous plasmas by tuning the modulation frequency of a broadband laser

The stimulated Raman scattering (SRS) instability can inhibit the performance of laser driven inertial confinement fusion (ICF) implosions by scattering light into unwanted directions or by generating hot electrons that preheat the target fuel. In principle, ICF target designs can avoid parameter regimes conducive to large, linear SRS gains. In practice, kinetic inflation—the nonlinear enhancement of SRS due to electron trapping in the excited plasma wave—makes this difficult. Here we show that laser bandwidth in the form of frequency modulation can either decrease or increase the inflationary SRS (iSRS) threshold in inhomogeneous plasmas depending on the maximum chirp of the laser pulse. The threshold, mapped out by a series of particle-in-cell simulations, exhibits a minimum when the frequency change within the pulse cancels the spatial detuning due to density inhomogeneities along the trajectory of the scattered light. In conclusion, by tuning the pump laser parameters away from this minimum, the iSRS threshold can be larger than at zero bandwidth, providing a path to mitigating kinetic inflation in ignition relevant plasmas.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2023

High-Fidelity Energy Deposition Ignition Model Coupled with Flame Propagation Models at Engine-like Flow Conditions

With the heightened pressure on car manufacturers to increase the efficiency and reduce the carbon emissions of their fleets, more challenging engine operation has become a viable option. Highly dilute, boosted, and stratified charge, among others, promise engine efficiency gains and emissions reductions. At such demanding engine conditions, the spark-ignition process is a key factor for the flame initiation propagation and the combustion event. From a computational standpoint, there exist multiple spark-ignition models that perform well under conventional conditions but are not truly predictive under strenuous engine operation modes, where the underlying physics needs to be expanded. In this paper, a hybrid Lagrangian-Eulerian spark-ignition (LESI) model is coupled with different turbulence models, grid sizes, and combustion models. The ignition model, previously developed, relies on coupling Eulerian energy deposition with a Lagrangian particle evolution of the spark channel, at every time-step. The spark channel is attached to the electrodes and allowed to elongate at a speed derived from the flow velocity. The LESI model is used to simulate spark ignition in a nonquiescent crossflow environment at engine-like conditions, using converge commercial computational fluid dynamics (CFD) solver. The results highlight the consistency, robustness, and versatility of the model in a range of engine-like setups, from typical with Reynolds-averaged Navier-Stokes (RANS) and a larger grid size to high fidelity with large-eddy simulation (LES) and a finer grid size. The flame kernel growth is then evaluated against Schlieren images from an optical constant volume ignition chamber with a focus on the performance of flame propagation models, such as G-equation and thickened flame model, versus the baseline well-stirred reactor model. Finally, future development details are discussed.

Advanced ignition modeling↗

DOE OSTI2021

Advanced Cost-Effective Coal-Fired Rotating Detonation Combustor for High Efficiency Power Generation

Coal-based detonation as a means of heat addition in power generation devices is a revolutionary “out of the box” technology concept, wherein it is theoretically possible to achieve an increase in total pressure across the combustor as opposed to a loss of available energy as is the case in conventional combustion systems. Detonation is a revolutionary technology concept of pressure gain combustion that exploits pressure rise from the combustion process to augment high flow momentum and pressures. Recognizing that pressure gain combustion has become a topic of elevated national interest, high energetic modes (exergy) pressure gain combustion (PGC) systems are required. Pressure gain combustion is a key enabling technology for maintaining technological superiority in the development of advanced power generation systems. Pressure gain combustion is an innovative scheme of turbulent combustion that considerably increases thermodynamic cycle efficiencies (~10-20%). This project extends the State-of-the-Art by providing the first direct experimental and computational data of operability dynamics and performance characterization data and create the first validated Coal-Fired RDC investigations. Coal-based RDC is an innovative revolutionary technology that would result in high efficiency power generation and reduced of harmful emissions. Also, the fundamental and open source nature of the project will benefit a broader scientific and industry audience who will be able to utilize the outcomes of this project for advancing the coal-fired RDC power generation development.

01 COAL, LIGNITE, AND PEAT↗

DOE OSTI2020

FPGAs-as-a-Service Toolkit (FaaST)

Computing needs for high energy physics are already intensive and are expected to increase drastically in the coming years. In this context, heterogeneous computing, specifically as-a-service computing, has the potential for significant gains over traditional computing models. Although previous studies and packages in the field of heterogeneous computing have focused on GPUs as accelerators, FPGAs are an extremely promising option as well. A series of workflows are developed to establish the performance capabilities of FPGAs as a service. Multiple different devices and a range of algorithms for use in high energy physics are studied. For a small, dense network, the throughput can be improved by an order of magnitude with respect to GPUs as a service. For large convolutional networks, the throughput is found to be comparable to GPUs as a service. This work represents the first open-source FPGAs-as-a-service toolkit.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2022

Durable, High-Performance Unitized Reversible Fuel Cells Based on Proton Conductors

The main objective of this project was to develop robust, highly efficient, and economically viable H + -conducting membrane-based, unitized reversible fuel cell (H-URFC) technology for large-scale co-located energy storage and power generation. Another objective of this project is to gain a profound understanding of the degradation mechanisms of key stack materials and interfaces using various in situ, ex situ, and operando measurements guided by theoretical analysis. Nanostructured components will be integrated into cell design and the interfaces between electrodes and electrolyte will be modified with active bi-functional catalysts and protective coatings in order to achieve >70% roundtrip efficiency at 1 A/cm2 in both the fuel cell and the electrolysis modes. The end goal of the project is to advance the technology to the point that a university-industry collaboration can be established to scale up the technology for early adoption, and eventually enabling a pathway to large-scale energy storage that utilizes chemical storage and conversion for electrical grid balancing.

08 HYDROGEN↗

DOE OSTI2020

Life-Cycle Baseline Customization for the Formerly Utilized Sites Remedial Action Program - 20304

One of the responsibilities of the federal government is to estimate sound and defensible life-cycle baseline costs for use in federal budget estimates and to meet federal financial reporting requirements. To accomplish this, the US Department of Energy (DOE) Office of Legacy Management (LM) and the US Army Corps of Engineers (USACE) have partnered together to ensure that the liabilities documented in each Formerly Utilized Sites Remedial Action Program (FUSRAP) site's life-cycle baseline are specifically tailored. FUSRAP was created in the mid-1970's to clean up radiological contamination resulting from the early development of nuclear weapons. DOE was responsible for FUSRAP until October 1997, when Congress transferred the administration and execution of FUSRAP site cleanups to USACE. By 1997, DOE had completed the cleanup of 25 of the 46 sites that were active within the program and had begun cleanup at 13 additional sites. USACE was assigned responsibility for the cleanup of the 21 remaining FUSRAP sites, and at 8 additional sites that had since been referred for cleanup. The LM mission for the FUSRAP sites is to perform long-term surveillance and maintenance (LTS and M). Currently, LM provides long-term stewardship for 34 completed FUSRAP sites. Another 20 sites are under active remediation by USACE. Within the last 5 years, USACE has completed the cleanup at five FUSRAP sites and the LTS and M responsibility has been transferred to LM. By 2029, USACE will compete remediation at eight additional sites and LTS and M for those sites will transfer to LM. Because responsibilities for the FUSRAP sites transfer between USACE and LM upon completion of remedial actions, both agencies maintain life-cycle baselines for different stages of the project and both must have a strong understanding of the needs and requirements for each site. This understanding ensures that the life-cycle baselines form a complete and accurate picture of what is required for the site and for the FUSRAP program. LM focuses on several things when customizing the life-cycle baseline estimates for the FUSRAP sites, including (1) Understanding the unique requirements for each site. By reviewing site-specific documents prepared by USACE, such as Feasibility Studies and Records of Decision, and partnering with USACE to gain additional insight about site conditions and requirements for stewardship, as well as potential risks, LM can better develop the life-cycle baselines. (2) Developing site-specific labor breakdowns. This ensures the required labor mix is baselined for specific activities by comparing the labor mix required to perform activities at (a) other LM-managed FUSRAP sites and (b) non-FUSRAP LM sites and (c) by USACE at active FUSRAP sites. (3) Taking a tiered approach to life-cycle baseline planning. Estimates for sites transferring to LM in the near term (5 years) are more definitive than for sites transferring in the out-year period. Remedial actions at the near-term sites are at or near completion, providing LM a strong understanding of the LTS and M requirements and remaining liabilities. This in turn allows for site-specific customization of the baseline. (4) Using a robust risk management approach to ensure that liabilities specific to each site are identified, evaluated by probability and severity, and documented in relation to the impact to cost or schedule. To ensure the most accuracy within all the baselines, the FUSRAP life-cycle baselines are updated as needed to support program, project, and contract management needs. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗