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At least 199 records · Page 11

Surface regulation enables high stability of single-crystal lithium-ion cathodes at high voltage

Abstract Single-crystal cathode materials for lithium-ion batteries have attracted increasing interest in providing greater capacity retention than their polycrystalline counterparts. However, after being cycled at high voltages, these single-crystal materials exhibit severe structural instability and capacity fade. Understanding how the surface structural changes determine the performance degradation over cycling is crucial, but remains elusive. Here, we investigate the correlation of the surface structure, internal strain, and capacity deterioration by using operando X-ray spectroscopy imaging and nano-tomography. We directly observe a close correlation between surface chemistry and phase distribution from homogeneity to heterogeneity, which induces heterogeneous internal strain within the particle and the resulting structural/performance degradation during cycling. We also discover that surface chemistry can significantly enhance the cyclic performance. Our modified process effectively regulates the performance fade issue of single-crystal cathode and provides new insights for improved design of high-capacity battery materials.

25 ENERGY STORAGE↗

Automated Framework for Groundwater Monitoring Using DWT with LSTM and Transformers

Environmental monitoring is critical for safeguarding public health and ecological well-being. Traditional data structuring and workflow monitoring methods consume significant time and effort, hindering timely insights and effective decision-making. Our study addresses this challenge by presenting an AI framework that automates data cleaning, structuring, and modeling processes, specifically targeting applications in groundwater monitoring. By leveraging automation for data processing and model training, our framework establishes a novel and efficient paradigm for environmental monitoring, with its potential application to the vast network of over a hundred Department of Energy Environmental Management (DoE-EM) cleanup sites across the country. It analyzes data streams from a network of groundwater Internet-of-Things (IoT) sensors deployed at the Savannah River Site (SRS) for prediction modeling. This allows human experts to focus on analysis and decision-making, ultimately leading to better environmental outcomes.The framework employs multivariate time-series forecasting methods to study and model the behavior of varying chemical analytes. The continuous learning process is enabled by utilizing deep learning techniques. It allows the framework to become more nuanced in its analysis over time, adapting to the specific characteristics of the environmental site and the evolving nature of contaminant behavior. Deep learning models known for sequence modeling, LSTM, and Transformers are employed for time series forecasting. Data processing and structuring are essential components significantly impacting the final model's performance. This hypothesis was proven by presenting a comparative analysis of model performance with processed and unprocessed data. The feature engineering approach utilized was the Discrete Wavelet Transform, which works well with time series data.

Discrete Wavelet Transform (DWT)↗

System Configuration Evaluation for Process Settling of Hanford Waste Solid Particles

Direct Feed High-Level Waste (DFHLW) is a potential flowsheet operations approach to initiating high-level waste (HLW) vitrification prior to completion of the Hanford Waste Treatment and Immobilization Plant (WTP) Pretreatment Facility. A settle/decant process has been proposed to concentrate solids prior to delivery to the WTP HLW Facility during DFHLW operations, wherein the solids in a settled layer would be remixed with the supernatant liquid remaining after decanting operations to provide the feed at required solids concentrations. Settling would be used in lieu of purpose-built filtration or other solids separation equipment. Pacific Northwest National Laboratory (PNNL) is providing baseline technical support to the Washington River Protection Solutions (WRPS) Flowsheet Integration group. To support planning for DFHLW, WRPS previously requested that PNNL evaluate the current data set available to predict the time needed for HLW solids to settle and the solids concentration and strength of that settled layer, to identify gaps in the understanding and predictive capability of HLW solids waste settling times, and to provide scoping estimates of the potential settling times. Eight technical gaps were identified for predicting settling times and characteristics of the formed sediment layers. In addition to the data gaps, an overarching observation was made that there is significant variation in behavior of settling rate and settled layer data. The settling time required to concentrate solids via a settle/decant process was determined from the limited data to have a difference of potentially more than a factor of 5,000 in the estimated settling times, varying from 0.2 to 1,060 days for example depending on process vessel depth and final sediment solids concentration. In contrast, successful processes of liquid-forward output streams resulting from in-tank settling and decanting forward liquid have been reported for operations conducted at the Hanford Site. The purpose of this current report is to further support DFHLW planning by evaluating double-shell tank (DST) and alternate vessel equipment and operational configurations to enable optimization of the settle/decant process to concentrate solids. Hanford waste processing behavior specific to liquid feed availability following a slurry transfer in a DST is summarized, including process stream characteristics and process equipment configurations. The performance of DST process equipment configurations is evaluated for possible improvements using computational fluid dynamics (CFD) and simple analytical models. Potential new vessel design(s) specific to enabling effective settle/decant processes, and cursory summary of other separate and inline solids separations processes, are also provided. The CFD results indicated that improvement in outflow solids concentration was promoted by a reduction in the slurry flow rate, angling the distributor nozzles downward, and lifting the transfer pump. The solid-liquid analysis evaluating particle trajectory confirmed that the potential for particle ingestion (in the transfer pump) was decreased with increased radial separation between the inlet and outlet (transfer pump inlet), decreased inlet flow, and decreased liquid density and viscosity for a neutrally buoyant inlet flow. An assessment was also made of the potential for inflow configuration changes to result in the discrete mounding or piling of solids within the tank. Based on the characterization of the settled waste to date, HLW sediments will be unlikely to sustain a substantial angle of repose to facilitate significant variations in the elevation of the settled solids.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

A Novel Approach to Investigate Thermal Protection Systems Materials

The Koo Research Group (KRG) at The University of Texas at Austin (UT) and KAI has specialized in “Ablation Research” for more than fifteen years. Recently, the group has developed several incredibly unique capabilities that can advance “Thermal Protection Systems (TPS) Materials Research & Development” using an integrated experimental and numerical approach. The paper aims to introduce the methodology KRG has developed to solve this challenging problem. It will discuss how the KRG develops “Process-Properties-Performance” relationships of novel TPS materials in a systematical approach using (a) processing and fabrication, (b) thermal characterization of properties, (c) aerothermal testing, (d) microstructures characterization and analysis, and (e) numerical modeling. Progress and challenges of this research will also be discussed.

Engineering↗

Recent developments in 3D-printed membranes for water desalination

The recognition of membrane separations as a vital technology platform for enhancing the efficiency of separation processes has been steadily increasing. Concurrently, 3D printing has emerged as an innovative approach to fabricating reverse osmosis membranes for water desalination and treatment purposes. This method provides a high degree of control over membrane chemistry and structural properties. In particular, when compared to traditional manufacturing techniques, 3D printing holds the potential to expedite customization, a feat that is typically achieved through conventional manufacturing methods but often involves numerous processes and significant costs. This review aims to present the current advancements in membrane manufacturing technology specifically tailored for water desalination purposes, with a particular focus on the development of 3D-printed membranes. A comprehensive analysis of recent progress in 3D-printed membranes is provided. However, conducting experimental work to investigate various influential factors while ensuring consistent results poses a significant challenge. To address this, we explore how membrane manufacturing processes and performance can be effectively pre-designed and guided through the use of molecular dynamics simulations. Finally, this review outlines the challenges faced and presents future perspectives to shed light on research directions for optimizing membrane manufacturing processes and achieving optimal membrane performance.

3D printing membranes↗

Coating adhesion of a chromate-containing epoxy primer on Al2024-T3 surface processed by laser-interference

In this work, the coating adhesion test results are presented for a primer that was coated on laser-interference structured surfaces of as-received Al2024-T3 specimens, i.e., without employing any polishing, cleaning, or any other surface alteration techniques. All of the laser-interference processing was performed by splitting the primary beam of a Q-switched Nd:YAG pulsed nanosecond laser into two beams and focused them to the same spot. The specimens were spray painted with a chromate-containing epoxy primer, CA7233, compliant to MIL-PRF-23377 Type I Class C2 specification. The adhesion of primer on Al surface with different treatments was assessed using the ASTM D3359 X-cut and cross-hatch tests. It was found that the laser processed specimens meet the performance requirements in the coating adhesion specifications by having a higher or identical ranking for coating adhesion specimens than those prepared with current state-of-the-art chemical conversion or sulfuric acid anodizing. The rastering with either 4 mm/s or 6 mm/s with a laser fluence of 1.78 J/cm2 is recommended to attain acceptable coating adhesion, even higher than that with the anodizing surface treatment.These results indicate that laser-interference shows significant potential as a non-chemical surface preparation technique for these coatings.

36 MATERIALS SCIENCE↗

Direct Recycling of Lithium-Ion Battery Cathodes: A Multi-Stage Annealing Process to Recover the Pristine Structure and Performance

Direct recycling is an alternative low-cost process that retains the structure of the lithium-ion battery cathode rather than going through materials dissolution and repurification. While the process shows promise, various steps need to be better understood and studied to identify possible roadblocks, cost intensive steps, and needed variations in protocol that may be necessary based on the feedstock of recycled cathodes available. In this study, we have evaluated the process of thermal relithiation as it applies to end-of-life cathode materials. For recovered end-of-life cathodes, approximately 20% of the useable lithium has been lost due to solid electrolyte interface formation, parasitic reactions, and particle isolation; this lost lithium contributes to higher cell impedance and a gradual shift in electrode potentials. As a first step in the direct recycling process, this lithium needs to be restored not only to recover capacity but also to eliminate surface vacancies and hinder surface reconstruction that may increase impedance and impact performance. Here, we have optimized a coating method followed by a two-stage annealing process that restores a model delithiated NMC333 material to pristine performance. Comparisons to single-stage processes are made, and new characterization tools have been used to better understand the processes.

25 ENERGY STORAGE↗

Safety Functions and Features, Events and Processes for the E-Area Performance Assessment

The DOE Technical Standard, “Disposal Authorization Statement and Tank Closure Documentation,” (DOE 2017) recommends the use of safety functions and features, events and processes (FEPs) to support development of conceptual models and identification of scenarios to be considered in a performance assessment (PA). The FEP process provides a means to describe how a PA considers and addresses the factors that could influence the performance of key barriers. Understanding the roles of barriers in terms of limiting migration helps to focus on how changes in the system could lead to a situation where those roles cannot be fulfilled and there is the potential for compromised performance. The FEPs screening and review process was used to identify FEPs that are relevant for the EArea Low-Level Waste Facility (LLWF) and specifically those FEPs that could have a detrimental impact on the effectiveness of a given safety function. For this PA, a default list of FEPs developed at the International Atomic Energy Agency (IAEA 2004) and an approach implemented for PAs at the Hanford and Idaho sites (Mehta et al. 2016, DOE-ID 2019) are used to identify processes and events that could influence the effectiveness of a given safety function for the E-Area LLWF (e.g., subsidence can impact the safety function of the cover system and lead to increased infiltration). The Hanford and Idaho PAs represent two of the most recent applications of this approach. The PA evaluates the potential impacts of changes in performance of different features of the system and demonstrates that the safety functions represent multiple and redundant barriers. Barrier analyses, assuming a safety function is not present, also test the robustness of the system in the event of the loss of one or more safety functions. Such evaluations also support a qualitative illustration of the concept of defense in depth. The safety concept for closure of the E-Area LLWF (generically referred to as “E-Area”) encompasses a variety of different features (i.e., administrative controls, natural site features, and engineered barriers) that reduce the potential impacts on human health and the environment from the residual waste that will remain after closure. These features can be represented as a collection of safety functions acting independently and as a system to provide for overall safety. In some applications, there have been attempts to assign numerical expectations to specific safety functions, but that is not the intent in this case. The concept of safety functions is used more qualitatively in two ways for this PA: 1. To illustrate the robustness of the E-Area design, operational practices and closure approach by documenting features that are and are not credited in different modeling cases. 2. To identify the roles of the different features and potential processes and events that could compromise the performance of safety features and need to be considered when developing the modeling approach. This report addresses both safety functions and FEPs for the E-Area PA.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Benchmarking performance changes in the simulation of extratropical modes of variability across CMIP generations

In this work, we evaluate extratropical modes of variability in the three most recent phases of the Coupled Model Intercomparison Project (CMIP3, 5, and 6) to gauge improvement of climate models over time. A suite of high-level metrics is employed to objectively evaluate how well climate models simulate the qobserved Northern Annular Mode (NAM), North Atlantic Oscillation (NAO), Pacific North America pattern (PNA), Southern Annular Mode (SAM), Pacific Decadal Oscillation (PDO), North Pacific Oscillation (NPO), and North Pacific Gyre Oscillation (NPGO). We apply a Common Basis Function (CBF) approach that projects model anomalies onto observed empirical orthogonal functions (EOFs), together with the traditional EOF approach, to CMIP Historical and AMIP models. We find simulated spatial patterns of those modes have been significantly improved in the newer models, although the skill improvement is sensitive to the mode and season considered. We identify some potential contributions to the pattern improvement of certain modes (e.g., the Southern Hemisphere jet and High-top vertical coordinate), however the performance changes are likely attributed to gradual improvement of the base climate and multiple relevant processes. Less performance improvement is evident in the mode amplitude of these modes and systematic overestimation of the mode amplitude in spring remains in the newer climate models. We find that the post-dominant season amplitude errors in atmospheric modes are not limited to coupled runs but are often already evident in AMIP simulations. This suggests that rectifying the egregious post-dominant season amplitude errors found in many models can be addressed in an atmospheric-only framework making it more tractable to address in the model development process.

54 ENVIRONMENTAL SCIENCES↗

Study of e + e − → π + π − π 0 at s from 2.00 to 3.08 GeV at BESIII

With the data samples taken at center-of-mass energies from 2.00 to 3.08 GeV with the BESIII detector at the BEPCII collider, a partial wave analysis on the e + e − → π + π − π 0 process is performed. The Born cross sections for e + e − → π + π − π 0 and its intermediate processes e + e − → ρ π and ρ ( 1450 ) π are measured as functions of s . The results for e + e − → π + π − π 0 are consistent with previous results measured with the initial state radiation method within one standard deviation, and improve the uncertainty by a factor of ten. By fitting the line shapes of the Born cross sections for the e + e − → ρ π and e + e − → ρ ( 1450 ) π , a structure with mass M = 2119 ± 11 ± 15 MeV / c 2 and width Γ = 69 ± 30 ± 5 MeV is observed with a significance of 5.9 σ , where the first uncertainties are statistical and the second ones are systematic. This structure can be interpreted as an excited ω state. Published by the American Physical Society 2024

Astronomy & Astrophysics↗

Production of mechanically-generated 316L stainless steel feedstock and its performance in directed energy deposition processing as compared to gas-atomized powder

The objective of this work is to study the feasibility of mechanically-generated feedstock for use in directed energy deposition (DED) processing. Mechanically-generated powder was created by machining 316L stainless steel bar stock followed by comminution of the resulting chips through oscillation ball milling. This methodology's production yield and processing time for the specifications of a commercially available DED system are presented along with resulting powder morphology. Performance of the mechanically-generated feedstock was compared to gas-atomized powder and evaluated based on the following figures of merit: flowability, printed part height, printed part density, and chemical compositional stability throughout processing. Mechanically-generated feedstock was created to meet deposition system requirements. Compared with gas-atomized powder, mechanically-generated powder did not flow as well through the powder-delivery system. Parts printed from mechanically-generated feedstock were generally taller than their counterparts from gas-atomized feedstock, but their densities were less predictable. As a result, chemical composition of prints using both feedstocks was within standard nominal compositions for 316L stainless steel.

36 MATERIALS SCIENCE↗

Design, performance, and cost savings of using GF-PC additively manufactured tooling for stamping of HSS 590 sheet metal

Conventional sheet metal forming tooling in the automotive industry is made up of hardened steel and used for mass-production. Prototype tooling made of metal is durable, but it is only used for a small number of parts despite its high cost, contributing heavily to the vehicle development cost. Additive Manufacturing (AM) offers a low-cost alternative for fabricating tooling suitable for low-volume production. Here, this study investigates the feasibility of using AM polymer composite tooling for the stamping of 1.5mm thickness HSS 590 steel sheets through a two-pronged approach – experimental and numerical analysis. Sheet metal stamping experiments were conducted with glass fiber reinforced polycarbonate (GF-PC) AM polymer tooling and their performance was evaluated based on various metrics such as tool deformation and part accuracy. Finite element simulations of the stamping process were performed, which accurately captured the tool deformations seen in experiments with the use of anisotropic material models. The effective use of simulations in optimizing process parameters to achieve the desired final part geometry is also demonstrated. The GF-PC AM polymer composite tooling was found to be well suited for low volume production applications with potential cost savings.

36 MATERIALS SCIENCE↗

Antioxidant-induced transformations of a metal-acid hydrocracking catalyst in the deconstruction of polyethylene waste

Plastics are ideal for numerous applications, as driven by the development of complex formulations containing various additives to improve performance and processability. Unfortunately, chemical valorization strategies (e.g., catalytic deconstruction) often can be challenged by the presence of small-molecule additives, and quantification of the impact of these molecular constituents on upcycling processes remains elusive. Here, this dearth of information restricts catalyst design efforts to combine the robustness and performance necessary to improve plastics circularity. In this communication, we describe a systematic study of common plastics additives—phenolic antioxidants, and we quantify the relationship between additive content and deconstruction yields of high-density polyethylene (HDPE) over a platinum on tungstated zirconium (Pt/WO 3 /ZrO 2 ) hydrocracking catalyst. In the simplest case of a base (antioxidant- and slip agent-containing) HDPE resin versus a pure (additive-stripped) HDPE polymer, a two-fold decrease in the yield of gas and liquid products is noted for base HDPE resin. Furthermore, both antioxidant chemistry and concentration strongly impact conversion and individual product selectivities. Using infrared spectroscopy, we determine that antioxidants change the effective ratio of metal to acid sites (i.e., metal-acid balance) through reactions of phenols and/or other functional groups (e.g., acids, esters) with catalyst active sites. Overall, this work demonstrates the impact of one common set of additives on plastics deconstruction, and the analysis herein provides a blueprint for quantitatively assessing the effects of additives on plastics deconstruction processes and for evaluating the development of more robust catalytic strategies or more tolerable additive formulations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

In-depth analysis on parallel processing patterns for high-performance Dataframes

The Data Science domain has expanded monumentally in both research and industry communities during the past decade, predominantly owing to the Big Data revolution. Artificial Intelligence (AI) and Machine Learning (ML) are bringing more complexities to data engineering applications, which are now integrated into data processing pipelines to process terabytes of data. Typically, a significant amount of time is spent on data preprocessing in these pipelines, and hence improving its efficiency directly impacts the overall pipeline performance. The community has recently embraced the concept of Dataframes as the de-facto data structure for data representation and manipulation. However, the most widely used serial Dataframes today (R, pandas) experience performance limitations while working on even moderately large data sets. We believe that there is plenty of room for improvement by taking a look at this problem from a high-performance computing point of view. In a prior publication, we presented a set of parallel processing patterns for distributed dataframe operators and the reference runtime implementation, Cylon. In this paper, we are expanding on the initial concept by introducing a cost model for evaluating the said patterns. Furthermore, we evaluate the performance of Cylon on the ORNL Summit supercomputer.

97 MATHEMATICS AND COMPUTING↗

Direct internal recycling fractions approaching unity

Direct internal recycling (DIR) refers to the process of recovering pure hydrogen isotopes (D/T) from helium and other impurities in the fusion plasma exhaust and directing them back to the fuel injection system. Increasing the exhaust fraction purified through DIR significantly reduces the size and cost of the tritium plant and provides additional benefits including reduced requirements for both the tritium startup inventory and tritium breeding ratio. Metal foil pumps (MFPs) are the dominant technology for this separation, relying on the concept of superpermeation. We recently demonstrated that PdCu foils operated at low temperature provide both exceptional flux and resilience to helium absorption as the DIR fraction is increased. Herein we design and demonstrate continuous and semi-batch DIR processes using PdCu MFPs. Under continuous processing, stable performance was observed for DIR fractions up to 92 %. In addition, we demonstrate a semi-batch process capable of extending the DIR fraction to unity (> 99.8 %). Under the experimental conditions described within a PdCu MFP area of ~22 m 2 would be sufficient to process the fusion exhaust with 92 % DIR fraction at expected flowrates of 100 Pa·m 3 ·s -1 for a future fusion power plant.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

GDSA PFLOTRAN Development (FY2021)

The Spent Fuel & Waste Science and Technology (SFWST) Campaign of the U.S. Department of Energy (DOE) Office of Nuclear Energy (NE), Office of Spent Fuel & Waste Disposition (SFWD) is conducting research and development (R&D) on geologic disposal of spent nuclear fuel (SNF) and high-level nuclear waste (HLW). A high priority for SFWST disposal R&D is to develop a disposal system modeling and analysis capability for evaluating disposal system performance for nuclear waste in geologic media. This report describes fiscal year (FY) 2021 advances of the PFLOTRAN Development group of the SFWST Campaign. The mission of this group is to develop a geologic disposal system modeling capability for nuclear waste that can be used to probabilistically assess the performance of generic disposal concepts. In FY 2021, development proceeded along three main thrusts: software infrastructure, code performance, and process model advancement. Software infrastructure improvements included implementing an Agile software development framework and making improvements to the QA Test Suite. Code performance improvements included development of advanced linear and nonlinear solvers as well as design of flexible smoothing algorithms for capillary pressure functions. Process modeling advancements included the addition of flexible thermal conductivity function definitions and refinement of multi-continuum reactive transport to support Sandia’s participation in DECOVALEX

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

PFLOTRAN Development FY2021

The Spent Fuel & Waste Science and Technology (SFWST) Campaign of the U.S. Department of Energy (DOE) Office of Nuclear Energy (NE), Office of Spent Fuel & Waste Disposition (SFWD) is conducting research and development (R&D) on geologic disposal of spent nuclear fuel (SNF) and high-level nuclear waste (HLW). A high priority for SFWST disposal R&D is to develop a disposal system modeling and analysis capability for valuating disposal system performance for nuclear waste in geologic media. This report describes fiscal year (FY) 2021 advances of the PFLOTRAN Development group of the SFWST Campaign. The mission of this group is to develop a geologic disposal system modeling capability for nuclear waste that can be used to probabilistically assess the performance of generic disposal concepts. In FY 2021, development proceeded along three main thrusts: software infrastructure, code performance, and process model advancement. Software infrastructure improvements included implementing an Agile software development framework and making improvements to the QA Test Suite. Code performance improvements included development of advanced linear and nonlinear solvers as well as design of flexible smoothing algorithms for capillary pressure functions. Process modeling advancements included the addition of flexible thermal conductivity function definitions and refinement of multi-continuum reactive transport to support Sandia’s participation in DECOVALEX. This report fulfills the GDSA PFLOTRAN Development Work Package Level 3 Milestone – PFLOTRAN Development, FY2021, M3SF-21SN010304072.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

A Large Eddy Simulation Study of Flow Turbulence, Alumina Transport, and Bath Temperature Evolution in Conventional Aluminum-Smelting Cell Using OpenFOAM

In this study, a Large Eddy Simulation (LES) of the aluminum-smelting process is performed using OpenFOAM. To understand the coupled behavior of heat transfer, mass transfer, and flow of the smelting process, a multi-physics computational fluid dynamics (CFD) model based on the Eulerian–Eulerian multi-fluid approach is adopted. The model accounts for CO 2 bubble and magnetohydrodynamics (MHD)-driven flow, along with alumina dissolution, transport, and bath temperature evolution. The simulation predictions show small-scale turbulent vortical structures in the anode–cathode space caused by combined effect of MHD and CO 2 bubble-bath interactions and relatively large-scale asymmetric vortices in the inter-anode space caused by the CO 2 bubble-bath interactions. The vortex formation at the edges of the anodes evidently aids in transporting alumina from the central channel to the bottom of the anodes and prevents accumulation of gas bubbles in the periphery of the anode bottom. Symmetric bath cold spots are observed in the vicinity of the feeder. Cold spots are also observed in the anode–cathode distance space below the anode bottom due to the transport of undissolved solid to this region by the flow. The findings from the work are useful in developing and designing alumina-feeding strategy leading to reduced anode effects and smooth operation of the cell. The work also highlights the important flow structures in conventional aluminum-smelting cell.

36 MATERIALS SCIENCE↗