Interlaced Characterization and Calibration: In-situ Bayesian optimal experimental design for constitutive model calibration
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Ricciardi, Denielle↗
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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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Developing Techniques for Focused Ion Beam Milling and In-Situ Micro-Compression to Characterize Orientation-Dependent Mechanical Properties of Molecular Crystals
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Stirrup, Kerry-Ann Megan [Sandia National Laborato↗
Rotating Disk Electrode Standardization and Best Practices in Acidic Oxygen Evolution for Low-Temperature Electrolysis
Efforts in oxygen evolution catalyst development have significantly increased and often use rotating disk electrode half-cells to evaluate intrinsic kinetics and screen materials for short-term durability. Standardizing rotating disk electrode test protocols is critical to experimental accuracy, to realistically assess their potential impact at a device level and to assess how different catalyst approaches and concepts are prioritized. The goal of this study is to provide standardized test protocols and suggest best practices to help reduce variability in ex situ materials characterization in the broader community. Specifically, these protocols focus on test cleanliness and materials choices, including how electrodes are prepared and tested, and the impact on activity observations.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Understanding Selectivity in CO2 Hydrogenation to Methanol for MoP Nanoparticle Catalysts Using In Situ Techniques
Molybdenum phosphide (MoP) catalyzes the hydrogenation of CO, CO2, and their mixtures to methanol, and it is investigated as a high-activity catalyst that overcomes deactivation issues (e.g., formate poisoning) faced by conventional transition metal catalysts. MoP as a new catalyst for hydrogenating CO2 to methanol is particularly appealing for the use of CO2 as chemical feedstock. Herein, we use a colloidal synthesis technique that connects the presence of MoP to the formation of methanol from CO2, regardless of the support being used. By conducting a systematic support study, we see that zirconia (ZrO2) has the striking ability to shift the selectivity towards methanol by increasing the rate of methanol conversion by two orders of magnitude compared to other supports, at a CO2 conversion of 1.4% and methanol selectivity of 55.4%. In situ X-ray Absorption Spectroscopy (XAS) and in situ X-ray Diffraction (XRD) indicate that under reaction conditions the catalyst is pure MoP in a partially crystalline phase. Results from Diffuse Reflectance Infrared Fourier Transform Spectroscopy coupled with Temperature Programmed Surface Reaction (DRIFTS-TPSR) point towards a highly reactive monodentate formate intermediate stabilized by the strong interaction of MoP and ZrO2. This study definitively shows that the presence of a MoP phase leads to methanol formation from CO2, regardless of support and that the formate intermediate on MoP governs methanol formation rate.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
In-Situ Calibrated Modeling of Residual Stresses Induced in Machining under Various Cooling and Lubricating Environments
Although many functional characteristics, such as fatigue life and damage resistance depend on residual stresses, there are currently no industrially viable ‘Digital Process Twin’ models (DPTs) capable of efficiently and quickly predicting machining-induced stresses. By leveraging advances in ultra-high-speed in-situ experimental characterization of machining and finishing processes under plane strain (orthogonal/2D) conditions, we have developed a set of physics-based semi-analytical models to predict residual stress evolution in light of the extreme gradients of stress, strain and temperature, which are unique to these thermo-mechanical processes. Initial validation trials of this novel paradigm were carried out in Ti-6Al4V and AISI 4340 alloy steel. A variety dry, cryogenically cooled and oil lubricated conditions were evaluated to determine the model’s ability to capture the tribological changes induced due to lubrication and cooling. The preliminarily calibrated and validated model exhibited an average correlation of better than 20% between the predicted stresses and experimental data, with calculation times of less than a second. Based on such fast-acting DPTs, the authors envision future capabilities in pro-active surface engineering of advanced structural components (e.g., turbine blades).
36 MATERIALS SCIENCE↗
In Situ XAFS, XRD, and DFT Characterization of the Sulfur Adsorption Sites on Cu and Ce Exchanged Y Zeolites
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99 GENERAL AND MISCELLANEOUS↗
Instrument for in situ hard x-ray nanobeam characterization during epitaxial crystallization and materials transformations
Solid-phase epitaxy (SPE) and other three-dimensional epitaxial crystallization processes pose challenging structural and chemical characterization problems. The concentration of defects, the spatial distribution of elastic strain, and the chemical state of ions each vary with nanoscale characteristic length scales and depend sensitively on the gas environment and elastic boundary conditions during growth. The lateral or three-dimensional propagation of crystalline interfaces in SPE has nanoscale or submicrometer characteristic distances during typical crystallization times. Here, an in situ synchrotron hard x-ray instrument allows these features to be studied during deposition and crystallization using diffraction, resonant scattering, nanobeam and coherent diffraction imaging, and reflectivity. The instrument incorporates a compact deposition system allowing the use of short-working-distance x-ray focusing optics. Layers are deposited using radio-frequency magnetron sputtering and evaporation sources. The deposition system provides control of the gas atmosphere and sample temperature. The sample is positioned using a stable mechanical design to minimize vibration and drift and employs precise translation stages to enable nanobeam experiments. Results of in situ x-ray characterization of the amorphous thin film deposition process for a SrTiO 3 /BaTiO 3 multilayer illustrate implementation of this instrument.
47 OTHER INSTRUMENTATION↗
Tensile behavior and microstructural evolution of a Fe-25Ni-20Cr austenitic stainless steel (alloy 709) from room to elevated temperatures through in-situ synchrotron X-ray diffraction characterization and transmission electron microscopy
Uniaxial tensile tests were done on Fe-25Ni-20Cr Austenitic Stainless Steel (Alloy 709) along with in-situ synchrotron measurement at different temperatures (25 degrees C, 500 degrees C, 700 degrees C and 900 degrees C). The X-Ray diffraction data was collected in-situ in order to follow the phases present as well as to derive the dislocation density as a function of strain through peak broadening analysis based on the modified Williamson-Hall method and see how trends are affected as a function of temperature. The XRD data were complemented by TEM and STEM-EDX characterization done on the post-experiment samples to observe the deformed microstructures. Finally, the paper presents a depiction of the tensile behavior of this advanced steel by interpreting the stress-strain curves and the effect of temperature through the information gained by in-situ XRD and TEM observations as well as fractography done ex-situ on the samples tested to rupture.
36 MATERIALS SCIENCE↗
Quantifying and modeling of stress-driven short-circuits in lithium-ion batteries in electrified vehicles
Despite the huge expansion of electric vehicle sales in the market, customers are discouraged by the possible catastrophic consequences brought by the safety issues of lithium-ion batteries, such as internal short circuits, especially in crash scenarios. Herein, we reveal the quantitative relationship between the deformations of the battery and the internal short circuit. By in situ and ex situ observations and post mortem characterization of the component materials, we quantify the stress-driven internal short circuit and failure behavior of the component material. With the aid of a validated numerical computational model as well as the in situ characterization of the global-field temperature, we successfully identify the minor and major short circuits of the cells upon various mechanical abusive loadings. Finally, we establish the internal short circuit criteria for typical formats of batteries. Furthermore, this discovery also provides a fundamental understanding of both internal and external stress-driven short circuits in a much broader context.
25 ENERGY STORAGE↗
Cationic Copper Species Stabilized by Zinc during the Electrocatalytic Reduction of CO 2 Revealed by In Situ X‐Ray Spectroscopy
Abstract Advanced in situ X‐ray absorption spectroscopy characterization of electrochemically co‐electrodeposited bi‐element copper alloy electrodes shows that zinc yields the formation of a stable cationic Cu species during the electroreduction of CO 2 at high cathodic polarization. In contrast, the formation/stabilization of cationic Cu species in copper oxides, or doping Cu with another element, like Ni, is not possible. It is found that the pure and mixed Cu:Zn electrodes behave similarly in term of electrocatalytic selectivity to multi‐carbon products. At higher Zn concentrations the electrode behaves like the pure Zn catalyst, which indicates that the Cu cationic species do not have a significant influence on the selectivity to multi‐carbon products. It is found that in the non‐monotonically distribution of products is dominated in term of surface energy in which copper prefers the surface. Otherwise, this work highlights the importance of in situ characterization to uncover the mechanisms mediating the catalytic reactions in contrast to ex situ or post mortem analysis, which can be a source of misinterpretation.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Fundamental Understanding of Dynamic Interfacial Phenomena in Solid State Batteries
Solid-state batteries (SSBs) are considered as one of the most promising battery technologies for resolving the intrinsic limitations of current lithium-ion batteries, such as safety and insufficient energy density. However, the degradation associated with interfaces in SSBs is still a critical issue leading to short cycle life. To get fundamental understanding of the failure mechanism of the interfaces, we first developed a comprehensive set of in situ diagnostic techniques combined with atomic/continuum modeling schemes to investigate and understand the coupled mechanical/chemical degradation associated with dynamic interfacial phenomena in SSBs. Specifically, we focused on in situ observations and characterizations of lithium plating-stripping processes, lithium dendrite formation, interphase formation, and the induced interfacial stresses, as well as the mechanical and electrochemical properties of interfaces and interphases. The final project report first gives an overview of the project background, objectives, technical approaches, and final deliverables for all the budget periods; then follows with a summary on main accomplishments based on main tasks. We particularly would like to highlight some capabilities developed from this project which can also be implemented to our advanced battery development.
25 ENERGY STORAGE↗
Creep properties of advanced austenitic steel 709 determined through short experiments under in-situ neutron diffraction followed by TEM characterization
Here in this study, the creep mechanisms at play in Alloy 709 (Fe-20Cr-25Ni) are investigated by performing short-term creep-type tests under in-situ neutron diffraction experiments. Short tests are performed in the temperature range of 500 to 900 °C under constant load with a load ranging from 50 to 150 MPa. The creep exponent and activation energy are determined using the Bird-Mukherjee-Dorn relation and compared to that obtained from conventional longer creep tests from the literature. Scanning transmission electron microscopy (S/TEM) of the post-creep microstructure indicates that interaction of dislocations with precipitates are a dominant mechanism at play. Furthermore, local elemental mapping indicated chemical segregation at grain boundaries and formation of complex precipitates.
36 MATERIALS SCIENCE↗
Coordination-Dependent Chemical Reactivity of TFSI Anions at a Mg Metal Interface
Charge transfer across the electrode–electrolyte interface is a highly complex and convoluted process involving diverse solvated species with varying structures and compositions. Despite recent advances in in situ and operando interfacial analysis, molecular specific reactivity of solvated species is inaccessible due to a lack of precise control over the interfacial constituents and/or an unclear understanding of their spectroscopic fingerprints. However, such molecular-specific understanding is critical to the rational design of energy-efficient solid–electrolyte interphase layers. We have employed ion soft landing, a versatile and highly controlled method, to prepare well-defined interfaces assembled with selected ions, either as solvated species or as bare ions, with distinguishing molecular precision. Equipped with precise control over interfacial composition, we employed in situ multimodal spectroscopic characterization to unravel the molecular specific reactivity of Mg solvated species comprising (i.e., bis(trifluoromethanesulfonyl)imide, TFSI – ) anions and solvent molecules (i.e., dimethoxyethane, DME/G1) on a Mg metal surface relevant to multivalent Mg batteries. In situ multimodal spectroscopic characterization revealed higher reactivity of the undercoordinated solvated species [Mg-TFSI-G1] + compared to the fully coordinated [Mg-TFSI-(G1) 2 ] + species or even the bare TFSI – . These results were corroborated by the computed reaction pathways and energy barriers for decomposition of the TFSI – within Mg solvated species relative to bare TFSI – . Finally, we evaluated the TFSI reactivity under electrochemical conditions using Mg(TFSI) 2 –DME-based phase-separated electrolytes representing different solvated constituents. Based on our multimodal study, we report a detailed understanding of TFSI – decomposition processes as part of coordinated solvated species at a Mg-metal anode that will aid the rational design of improved sustainable electrochemical energy technologies.
25 ENERGY STORAGE↗
Development and validation of time‐domain 1 H‐NMR relaxometry correlation for high‐throughput phenotyping method for lipid contents of lignocellulosic feedstocks
Abstract The bioenergy crops such as energycane, miscanthus, and sorghum are being genetically modified using state of the art synthetic biotechnology techniques to accumulate energy‐rich molecules such as triacylglycerides (TAGs) in their vegetative cells to enhance their utility for biofuel production. During the initial genetic developmental phase, many hundreds of transgenic phenotypes are produced. The efficiency of the production pipeline requires early and minimally destructive determination of oil content in individuals. Current screening methods require time‐intensive sample preparation and extraction with chemical solvents for each plant tissue. A rapid screen will also be needed for developing industrial extraction as these crops become available. In the present study, we have devised a proton relaxation nuclear magnetic resonance ( 1 H‐NMR) method for single‐step, non‐invasive, and chemical‐free characterization of in‐situ lipids in untreated and pretreated lignocellulosic biomass. The systematic evaluation of NMR relaxation time distribution provided insight into the proton environment associated with the lipids in the biomass. It resolved two distinct lipid‐associated subpopulations of proton nuclei that characterize total in‐situ lipids into bound and free oil based on their “molecular tumbling” rate. The T1T2 correlation spectra also facilitated the resolution of the influence of various pretreatment procedures on the chemical composition of molecular and local 1 H population in each sample. Furthermore, we show that hydrothermally pretreated biomass is suitable for direct NMR analysis unlike dilute acid and alkaline pretreated biomass which needs an additional step for neutralization.
pretreatment↗
Utah FORGE 2-2446: Closing the Loop Between In-situ Stress Complexity and EGS Fracture Complexity - Workshop Presentation
This is a presentation on the Closing the Loop Between In-situ Stress Complexity and EGS Fracture Complexity project by Lawrence Livermore National Laboratory, presented by Dr. Matteo Cusini. The project's objective was to employ a combination of high-fidelity simulations and true-triaxial block fracturing tests at high temperature to explore the intricate relationship between in-situ stress and hydraulic fracture patterns and better characterize the in-situ stress at Utah FORGE. This presentation was featured in the Utah FORGE R&D Annual Workshop on September 7, 2023. The workshop provided a valuable opportunity to explore the progress made in each of the 17 Research and Development projects funded under Solicitation 2020-1 which aim to enhance our understanding of the crucial factors influencing the development of Enhanced Geothermal Systems (EGS) reservoirs and resources.
15 GEOTHERMAL ENERGY↗
Closing the loop between in-situ stress complexity and EGS fracture complexity
The goal of the project is to employ a combination of high-fidelity simulations and true-triaxial block fracturing tests at high temperature to explore the intricate relationship between in-situ stress and hydraulic fracture patterns and better characterize the in-situ stress at Utah FORGE. Laboratory experiments are used to validate numerical models and better understand the impact of various parameters (e.g., temperature, well orientation, stress, etc) on the hydraulic fracture nucleation process in EGS. The project will have a significant impact as it will (1) improve the characterization of the in-situ stress field at FORGE; (2) demonstrate how high-fidelity modeling tools can be employed to analyze data for EGS; (3) provide a unique set of high-temperature hydraulic fracturing experimental results for EGS to help identifying the most important components for in-situ stress estimation and to validate the current in-situ stress estimation theory and establish a strong foundation for proposing a new one; (4) provide a validated set of numerical tools in an open source simulation framework (GEOS) that can be used to model EGS.
15 GEOTHERMAL ENERGY↗
Expanding the Zinc Precursor Toolbox: A Comparative Study of Precursors for Thermal ALD of ZnO Thin Films
Atomic layer deposition (ALD) of zinc oxide (ZnO) has been widely researched using diethyl zinc (DEZ)-based methods. The significant importance of thin films of ZnO as transparent conductive oxides (TCO) in optoelectronic devices and photovoltaics warrants examining alternative Zn precursors for ZnO ALD as potential replacements for the pyrophoric DEZ. In this study, we investigated three alternative Zn precursors: Zn(EEKI)2, Zn(DMP)2, ZnEt(HMDS), in the process development for high-quality ZnO thin films and compared them to DEZ. The ALD processes were studied using in situ spectroscopic ellipsometry. The properties of the ALD ZnO films were characterized using ex situ X-ray photoelectron spectroscopy (XPS), Rutherford backscattering spectrometry and nuclear reaction analysis (RBS/NRA), X-ray diffraction (XRD), atomic force microscopy (AFM), transmission electron microscopy (TEM), and ultraviolet-visible (UV/Vis) spectrophotometry. These measurements confirmed the formation of pure, stoichiometric, and polycrystalline ZnO films using all four Zn precursors. Although the selected precursors are chemically diverse Zn compounds, they all yielded saturating ALD processes and high-quality ZnO thin films at 200 °C. This study highlights the potential benefits of alternative zinc precursors in designing ALD processes for ZnO thin films.
Obenlüneschloß, Jorit↗
Energy storage emerging: A perspective from the Joint Center for Energy Storage Research
Energy storage is an integral part of modern society. A contemporary example is the lithium (Li)-ion battery, which enabled the launch of the personal electronics revolution in 1991 and the first commercial electric vehicles in 2010. Most recently, Li-ion batteries have expanded into the electricity grid to firm variable renewable generation, increasing the efficiency and effectiveness of transmission and distribution. Important applications continue to emerge including decarbonization of heavy-duty vehicles, rail, maritime shipping, and aviation and the growth of renewable electricity and storage on the grid. This perspective compares energy storage needs and priorities in 2010 with those now and those emerging over the next few decades. The diversity of demands for energy storage requires a diversity of purpose-built batteries designed to meet disparate applications. Advances in the frontier of battery research to achieve transformative performance spanning energy and power density, capacity, charge/discharge times, cost, lifetime, and safety are highlighted, along with strategic research refinements made by the Joint Center for Energy Storage Research (JCESR) and the broader community to accommodate the changing storage needs and priorities. Innovative experimental tools with higher spatial and temporal resolution, in situ and operando characterization, first-principles simulation, high throughput computation, machine learning, and artificial intelligence work collectively to reveal the origins of the electrochemical phenomena that enable new means of energy storage. This knowledge allows a constructionist approach to materials, chemistries, and architectures, where each atom or molecule plays a prescribed role in realizing batteries with unique performance profiles suitable for emergent demands.
Trahey, Lynn↗