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

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At least 181 records · Page 10
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

A self-referenced in-situ arrival time monitor for X-ray free-electron lasers

We present a novel, highly versatile, and self-referenced arrival time monitor for measuring the femtosecond time delay between a hard X-ray pulse from a free-electron laser and an optical laser pulse, measured directly on the same sample used for pump-probe experiments. Two chirped and picosecond long optical supercontinuum pulses traverse the sample with a mutually fixed time delay of 970 fs, while a femtosecond X-ray pulse arrives at an instant in between both pulses. Behind the sample the supercontinuum pulses are temporally overlapped to yield near-perfect destructive interference in the absence of the X-ray pulse. Stimulation of the sample with an X-ray pulse delivers non-zero contributions at certain optical wavelengths, which serve as a measure of the relative arrival time of the X-ray pulse with an accuracy of better than 25 fs. We find an excellent agreement of our monitor with the existing timing diagnostics at the SACLA XFEL with a Pearson correlation value of 0.98. We demonstrate a high sensitivity to measure X-ray pulses with pulse energies as low as 30 μJ. Using a free-flowing liquid jet as interaction sample ensures the full replacement of the sample volume for each X-ray/optical event, thus enabling its utility even at MHz repetition rate XFEL sources.

47 OTHER INSTRUMENTATION↗
DOE OSTI2021

Antifouling strategies for protecting bioelectronic devices

Bioelectronic devices are playing an increasingly important role in many areas of our lives. They power a significant portion of medical diagnostics and are becoming more and more important for delivery of therapeutics and monitoring of chronic symptoms. However, surface fouling phenomena, and especially biofouling in complex biological fluids, restricts the performance of these devices and severely reduces their useful lifespan. In this Research Update, we discuss the main principles and strategies that researchers use to prevent fouling and minimize or remove the foulants from bioelectronic device surfaces. We also survey a variety of antifouling approaches that can enhance device performance.

36 MATERIALS SCIENCE↗
DOE OSTI2025

High Spatial Resolution Mapping of Retained Fission Gas

Fission gas isotopic analysis provides quantitative high precision determination of irradiated nuclear fuel burnup, offers diagnostic value, and informs fuel performance models. A measurement capability has been developed at Idaho National Laboratory (INL) for the release of retained fission gas using a focused laser and static noble gas mass spectrometry (MS) analysis. This high resolution (10s microns spot size) capability was demonstrated using Xe implanted metal foils.

07 - ISOTOPES AND RADIATION SOURCES↗
DOE OSTI2023

Battery data integrity and usability: Navigating datasets and equipment limitations for efficient and accurate research into battery aging

A tremendous commitment of resources is needed to acquire, understand and apply battery data in terms of performance and aging behavior. There are many state of performance (SOP) and state of health (SOH) metrics that are useful to guide alignment of batteries to end-use, yet how these metrics are measured or extracted can make the difference between usable, valuable datasets versus data that lacks the necessary integrity to meet baseline confidence levels for SOP/SOH quantification. This work will speak to 1) types of data that support SOP and SOH evaluations on mechanistic terms, 2) measurement conditions needed to assure high data integrity, 3) equipment limitations that can compromise data high fidelity, and 4) the impact of cell polarization on data quality. A common goal in battery research and field use is to work from a data platform that supports economical paths of data capture while minimizing down-time for battery diagnostics. An ideal situation would be to utilize data obtained during normal daily use (“pulses or cycles of convenience”) without stopping the daily duty cycles to perform dedicated SOP/SOH diagnostic routines. However, difficulties arise in trying to make use of daily duty cycle data (denoted as cycle-by-cycle, CBC) that underscores the need for standardization of conditions: temperature and duty cycles can vary over the course of a day and throughout a week, month and year; polarization can develop within an immediate cycle and throughout successive cycles as a hysteresis. If CBC data is envisioned as a data source to determine performance and aging trends, it should be recognized that polarization is a frequent consequence of CBC and thus makes it difficult to separate reversible and irreversible components to metrics such as capacity loss and resistance increase over aging. Since CBC conditions can have a major impact on data usability, we will devote part of this paper to CBC data conditioning and management. Differential analyses will also be discussed as a means to detect changing trends in data quality. Our target cell chemistries will be lithium-ion types NMC/graphite and LMO/LTO.

25 ENERGY STORAGE↗
DOE OSTI2025

Mitigating Electrochemical Impedance Spectroscopy Artifacts in PEMWE Reference Electrode Measurements

This study investigates strategies to improve the quality of electrochemical impedance spectroscopy (EIS) measurements using reference electrodes (RE) in proton exchange membrane water electrolyzers (PEMWE). We demonstrate that adding a low impedance wire in parallel to the RE significantly enhances signal accuracy, especially at high frequencies. Additionally, we identify electrical pad heaters as a source of measurement noise. EIS measurements fulfilling Kramers–Kronig validity criteria were only achieved in their absence. These insights advance the diagnostic capabilities of REs in water electrolyzers and support more reliable, spatially resolved analysis of electrochemical losses within the cell.

08 HYDROGEN↗
DOE OSTI2022

A new TEVA-DGA chromatography procedure to separate Pu, Am, and Np from bulk U materials

Trace actinides present within uranium (U) material are diagnostic signatures of U processing history. For example, the emplacement of U material within the high neutron-flux environment of a nuclear reactor can cause neutron capture of U to form 241-plutonium ( 241 Pu). Plutonium-241 then decays to progeny isotopes 241-americium ( 241 Am) and 237-neptunium ( 237 Np); therefore, the presence and relative abundances of these trace actinides is indicative of the material’s production history and intended employment (Mayer et al., 2013). During a pre-detonation nuclear forensics investigation, measurement of trace actinide 241 Pu, 241 Am, and 237 Np concentrations by an analytical laboratory may be requested. However, chemically purifying these elements from bulk U is a challenging and involved procedure requiring several sequential chromatography columns across 4+ days. To expedite Pu-Am-Np separation from bulk U material, and to improve the yield recovery of these elements, this DHS Postdoc Fellowship has worked to create a new chromatography separation chemistry.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2026

KBKit: A Python Toolkit for Kirkwood–Buff Theory from Molecular Dynamics

Thermodynamic properties of liquid mixtures govern processes that range from drug delivery to energy storage, yet extracting these properties from molecular simulations remains challenging. Kirkwood–Buff (KB) theory offers a rigorous route by linking microscopic pair distribution functions to macroscopic free energies, but practical use of the theory has been hindered by two obstacles: (i) the long simulations needed to obtain well-converged Kirkwood-Buff integrals (KBIs) and (ii) the specialized corrections required to translate finite-size data to the thermodynamic limit. $\texttt{KBKit}$ is an open-source Python package that removes these barriers. It automatically computes KBIs and derived thermodynamic quantities from GROMACS input files, applies state-of-the-art finite-size corrections, and provides built-in diagnostic tools to quantify statistical uncertainty. Written with modern software-engineering practices—continuous integration, extensive unit testing, and thorough documentation—$\texttt{KBKit}$ is both reliable and easy to extend. By condensing complex KBI analysis into a few intuitive commands, $\texttt{KBKit}$ enables researchers to incorporate KB theory into routine simulation workflows and accelerate the discovery of solution-phase thermodynamics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Dataset of theoretical multinary perovskite oxides

Perovskite oxides (ternary chemical formula ABO 3 ) are a diverse class of materials with applications including heterogeneous catalysis, solid-oxide fuel cells, thermochemical conversion, and oxygen transport membranes. However, their multicomponent (chemical formula $A_xA^{'}_{1-x}B_yB^{'}_{1-y}O_3$) chemical space is underexplored due to the immense number of possible compositions. To expand the number of computed $A_xA^{'}_{1-x}B_yB^{'}_{1-y}O_3$ compounds we report a dataset of 66,516 theoretical multinary oxides, 59,708 of which are perovskites. First, 69,407 $A_{0.5}A^{'}_{0.5}B_{0.5}B^{'}_{0.5}O_3$ compositions were generated in the a - b + a - Glazer tilting mode using the computationally-inexpensive Structure Prediction and Diagnostic Software (SPuDS) program. Next, we optimized these structures with density functional theory (DFT) using parameters compatible with the Materials Project (MP) database. Our dataset contains these optimized structures and their formation (ΔH f ) and decomposition enthalpies (ΔH d ) computed relative to MP tabulated elemental references and competing phases, respectively. This dataset can be mined, used to train machine learning models, and rapidly and systematically expanded by optimizing more SPuDS-generated $A_{0.5}A^{'}_{0.5}B_{0.5}B^{'}_{0.5}O_3$ perovskite structures using MP-compatible DFT calculations.

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

Deciphering the influence of high-flux helium plasma exposure on tungsten nanostructure growth using real-time, in situ spectroscopic ellipsometry

In situ analysis of surfaces during high-flux plasma exposure represents a long-standing challenge in the study of plasma–material interactions. While post-mortem microscopy can provide a detailed picture of structural and compositional changes, in situ techniques can capture the dynamic evolution of the surface. In this study, we demonstrate how spectroscopic ellipsometry can be applied to the real-time characterization of W nanostructure (also known as “fuzz”) growth during exposure to low temperature, high-flux He plasmas. Strikingly, over a wide range of sample temperatures and helium fluences, the measured ellipsometric parameters (Ψ,Δ) collapse onto a single curve that can be directly correlated with surface morphologies characterized by ex situ helium ion microscopy. The initial variation in the (Ψ,Δ) parameters appears to be governed by small changes in surface roughness (<50 nm) produced by helium bubble nucleation and growth, followed by the emergence of 50 nm diameter W tendrils. This basic behavior appears to be reproducible over a wide parameter space, indicating that the spectroscopic ellipsometry may be of general practical use as a diagnostic to study surface morphologies produced by high-flux He implantation in refractory metals. An advantage of the methods outlined here is that they are applicable at low incident ion energies, even below the sputtering threshold. As an example of this application, we apply in situ ellipsometry to examine how W fuzz growth is affected both by varying ion energy and the temperature of the surface.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2020

Using Raman scattering to study reacting gas flow over a catalyst

l present a series of computational methods for analyzing and correcting Raman scattering from a reacting gas flow. My work focused on the laser diagnostic measurements of formaldehyde production over a silver catalyst, specifically the Raman spectroscopy component. This technique offers a non-intrusive, in situ way to measure the coupling between the gas phase and surface activity of a catalytic reaction at relevant industrial conditions. This report outlines the steps followed for correcting the non-idealities in the data due to both the detection optics and scattering mechanics. By implementing such refinement steps, l can generate an accurate 2D spatial map of the temperature profile, number densities for major species, and relative consumption of reactants throughout the reactor cell.

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

The influence of particle size on the fluid dynamics of a laser-induced plasma

The interaction of a laser-induced shock wave with nanoparticles and microparticles of aluminum oxide is investigated through experiments and modeling. The chemistry and physics of the interaction between the particles and plasma generated from laser ablation shows similarities and discrete differences for the two particle sizes. For both particle sizes, early stage (< 10 μs) ionization was dominant and evidenced by higher concentrations of Al II. While both sizes exhibit ionization over the same duration, the intensity of emission was greater for nanoparticles indicating greater concentrations of ionized species. Moreover, the dispersion of species was notably more elongated for microparticles while radial dispersion was more pronounced for nanoparticles with elevated drag forces. At later stages (i.e., > 10 μs), oxidation reactions were dominant for both particle sizes, but the same distinctions in flow field were observed and attributed to particle drag. In all stages of interaction, microparticles expand axially with less drag that suppresses their radial expansion. As a result, the dispersion of reactive species was mapped over an up to 80% larger area for nanoparticles relative to microparticles. Results shown here can be applied toward advancing experimental diagnostics and particle-shock wave modeling and simulation efforts for energetic materials.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Editors’ Choice—Ionomer Side Chain Length and Equivalent Weight Impact on High Current Density Transport Resistances in PEMFC Cathodes

Cell voltage at high current densities (HCD) of an operating proton-exchange membrane fuel cell (PEMFC) suffers from losses due to the local-O 2 and bulk-H + transport resistances in the cathode catalyst layer (CCL). Particularly, the interaction of perfluorosulfonic acid (PFSA) ionomer with the carbon supported platinum catalyst plays a critical role in controlling reactant transport to the active site. In this study, we perform a systematic analysis of the side chain length and equivalent weight (EW) of PFSA ionomers on the CCL transport resistances. Ex situ measurements were carried out to quantify the ionomer characteristics such as the molecular weight, proton conductivity and water uptake. Nanomorphology of ionomers cast as 60–120 nm thin-films is characterized using grazing-incidence X-ray scattering. In situ fuel cell electrochemical diagnostic measurements were carried out to quantify the reactant (H + /O 2 ) transport properties of the CCL. Ionomer EW was found to play a major role with decreasing EW yielding higher proton conductivity and water uptake that led to lower bulk-H + and local-O 2 transport resistances in the CCL. Finally, a 1D-semi-empirical performance model has been developed to quantify the impact of ionomer EW on cell voltage loss factors.

08 HYDROGEN↗
DOE OSTI2021

Development of New Experimental Methods for Correlated Operando Surface/Gas Characterization

The predictive understanding of catalytic surface reactions requires accurate microkinetic models, and while decades of work has been devoted to the elucidation of the reaction steps in these models, many open questions remain. One key issue is a lack of approaches enabling the local spatially resolved assessment of catalytic activity over a surface. In this report, we detail efforts to develop a new diagnostic approach to solve this problem. The approach is based upon laser resonance enhanced multiphoton ionization of reaction products emitted into the gas phase followed by spatially resolved imaging of the resultant ions or electrons. Ion imaging is pursued with a velocity-selected spatially resolved ion imaging microscope, while electron imaging was attempted in a low energy electron microscope. Successful demonstration of the ion imaging microscope coupled with the development of transport simulations shows promise for a revolutionary new tool to assess local catalytic activity

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

A Miniaturized Ignition Screening Rapid Compression Machine for probing low-to-intermediate temperature chemistry

With an objective to achieve net-zero emissions by no later than 2050, biofuels hold enormous potential as sustainable, renewable fuels that can be produced on a large scale. However, fuels of a similar type, derived from limited feedstock batch can dramatically vary in terms of their chemical structures and compositions, causing significant differences in physicochemical properties mainly influencing ignition-relevant properties. Rigorous prescreening and testing efforts are involved to evaluate fuels to comply with engines equipped with advanced combustion modes. The testing of some of these fuels implies low quantity fuel samples, access to relevant temperature and pressure conditions, high reproducibility, and a high throughput rate. In light of these considerations, a Miniaturized Ignition Screening Rapid Compression Machine (MISR) has been developed and built at the University of Illinois Chicago (UIC). Some design features include a smaller bellows-actuated driver section compared to other RCM designs, an adjustable brake section, and full optical access. The setup is designed to achieve reaction conditions (T > 600K and P < 100 bar with repetition rates of about 8 seconds per experiment). These conditions are relevant to low-to-intermediate temperature auto-ignition and can generate data for developing relevant chemical kinetics models or ignition maps. A brief insight into MISR design and its operating mechanism is shown. Also, to demonstrate the performance characteristics of the MISR, Ignition Delay (I.D) experiments for ethanol fuel at different equivalence ratios (Φ) are discussed in the context of plans with additional optical diagnostics, high-speed imaging, and gas sampling experiments.

Tomar, Mukul↗
DOE OSTI2023

High-throughput ab initio reaction mechanism exploration in the cloud with automated multi-reference validation

Quantum chemical calculations on atomistic systems have evolved into a standard approach to studying molecular matter. These calculations often involve a significant amount of manual input and expertise, although most of this effort could be automated, which would alleviate the need for expertise in software and hardware accessibility. Here, we present the AutoRXN workflow, an automated workflow for exploratory high-throughput electronic structure calculations of molecular systems, in which (i) density functional theory methods are exploited to deliver minimum and transition-state structures and corresponding energies and properties, (ii) coupled cluster calculations are then launched for optimized structures to provide more accurate energy and property estimates, and (iii) multi-reference diagnostics are evaluated to back check the coupled cluster results and subject them to automated multi-configurational calculations for potential multi-configurational cases. All calculations are carried out in a cloud environment and support massive computational campaigns. Key features of all components of the AutoRXN workflow are autonomy, stability, and minimum operator interference. We highlight the AutoRXN workflow with the example of an autonomous reaction mechanism exploration of the mode of action of a homogeneous catalyst for the asymmetric reduction of ketones.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Refining Methods to Determine the Isotopic Composition of Uranium Particles by Laser Ablation MC-ICP-MS

We report on efforts to mitigate the generation of isotopic anomalies during the ablation of micrometer-sized uranium oxide particles and analysis by MC-ICP-MS. The results of testing on particles of U200 indicate that laser fluence and frequency can affect isotopic data produced by laser ablation, but no settings were tested that could eradicate the signal spiking effect and generation of anomalous isotopic data for 234U/238U and 236U/238U. These anomalies are more frequent in samples with higher 235U enrichments, which is expected given their higher abundances of 234U and 236U. Of the standards tested here, only U005-A was anomaly-free. Efforts to compare the laser traces for particles with normal and anomalous isotopic compositions showed subtle differences in the behavior of the 234U/238U and 236U/238U ratios. However, it would be challenging to identify anomalous data points from a population of unknowns using this distinction, i.e., this is unlikely to be diagnostic. Thus, using current analytical hardware, we cannot eradicate the signal spiking phenomenon and cannot unambiguously identify isotopic anomalies from laser ablation traces. Ultimately, laser ablation ICP-MS would either require dramatic improvement to the ablation process and generation of more homogenous aerosols and/or improvements to detector electronics to identify and correct for the spiking phenomenon. Even if the reliability of the technique could be improved, a broader question to address is whether current data quality is of a high enough standard for laser ablation MC-ICP-MS to be used as a complementary technique to LG-SIMS for Safeguards.

organic↗
DOE OSTI2025

Monitoring the long-term performance of organic redox flow battery by a distribution of relaxation time analysis

Organic redox flow batteries hold great promise as an energy storage technology, but their intricate chemistry makes them vulnerable to various degradation mechanisms. Monitoring this degradation is essential for identifying the limiting processes within the cells. Electrochemical impedance spectroscopy (EIS) offers a straightforward, in-situ method for measuring the total resistance of an operating cell. However, to pinpoint the limiting processes during long-term cycling, EIS data must be complemented by other techniques. Distribution of relaxation time (DRT) analysis is particularly effective for differentiating resistance components. Here, in this study, we perform a comprehensive analysis of resistance evolution and the separation of anode and cathode contributions during long-term cycling of a full cell employing 7,8-dihydroxyphenazine-2-sulfonic acid (DHPS) as the anolyte. Separate analyses of the DHPS anolyte and ferri-/ferrocyanide catholyte were conducted using a symmetric cell setup. The relaxation times derived from symmetric cells facilitate the identification of peaks in the DRT profiles from the full cell. Importantly, the DRT profiles indicate a correlation between the evolution of charge transfer resistance and the chemical degradation of DHPS. The methodologies and results outlined in this study offer significant insights for developing diagnostic tools applicable to other types of redox flow batteries.

Distribution of relaxation time↗
DOE OSTI2022

Changes in active-site geometry on X-ray photoreduction of a lytic polysaccharide monooxygenase active-site copper and saccharide binding

The recently discovered lytic polysaccharide monooxygenases (LPMOs) are Cu-containing enzymes capable of degrading polysaccharide substrates oxidatively. The generally accepted first step in the LPMO reaction is the reduction of the active-site metal ion from Cu 2+ to Cu + . Here we have used a systematic diffraction data collection method to monitor structural changes in two AA9 LPMOs, one from Lentinus similis (LsAA9_A) and one from Thermoascus auranti­acus (TaAA9_A), as the active-site Cu is photoreduced in the X-ray beam. For LsAA9_A, the protein produced in two different recombinant systems was crystallized to probe the effect of post-translational modifications and different crystallization conditions on the active site and metal photoreduction. We can recommend that crystallographic studies of AA9 LPMOs wishing to address the Cu 2+ form use a total X-ray dose below 3 × 10 4 Gy, while the Cu + form can be attained using 1 × 10 6 Gy. In all cases, we observe the transition from a hexa­coordinated Cu site with two solvent-facing ligands to a T-shaped geometry with no exogenous ligands, and a clear increase of the θ 2 parameter and a decrease of the θ 3 parameter by averages of 9.2° and 8.4°, respectively, but also a slight increase in θ T . Thus, the θ 2 and θ 3 parameters are helpful diagnostics for the oxidation state of the metal in a His-brace protein. On binding of cello-oligosaccharides to LsAA9_A, regardless of the production source, the θ T parameter increases, making the Cu site less planar, while the active-site Tyr—Cu distance decreases reproducibly for the Cu 2+ form. Thus, the θ T increase found on copper reduction may bring LsAA9_A closer to an oligosaccharide-bound state and contribute to the observed higher affinity of reduced LsAA9_A for cellulosic substrates.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗