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DOE OSTI2025

Interface chemistry informs about cathode and anode degradation during fast charging

Here, the aim of this study is to examine the development and makeup of the Solid Electrolyte Interphase (SEI) and Cathode Electrolyte Interphase (CEI) in lithium-ion batteries during rapid charging. Using X-ray photoelectron spectroscopy (XPS) and depth profiling, we investigate the chemical modifications occurring on the electrode surfaces during the initial formation and subsequent fast charge-discharge cycles. Our research shows that the anode's SEI initially comprises a thin layer rich in ketones, which then transforms into a thicker layer dominated by carbonaceous compounds during rapid charging cycles. Following assembly, lithium fluoride (LiF) quickly becomes a key element of the SEI, and its presence continues to grow substantially during the formation cycle, remaining the primary component throughout subsequent cycles. Initially, the cathode forms a thin oxide layer rich in ketones, with no noticeable carbonaceous CEI. The CEI primarily comprises LiF, which experiences an increase during the formation cycle and retains a thin layer of carbon coating after the initial rapid discharge. These findings show how the interphase layers impact the performance and stability of lithium-ion batteries, especially during fast charging for electric vertical take-off and landing (eVTOL) vehicles.

Fast charging↗

DOE OSTI2020

Improved Capacity Retention of Lithium Ion Batteries under Fast Charge via Metal-Coated Graphite Electrodes

A primary barrier preventing repetitive fast charging of Li-ion batteries is lithium metal plating at the graphite anode. One approach toward mitigating Li metal deposition is the deliberate modification of the graphite anode surface with materials demonstrating high overpotentials unfavorable for Li metal nucleation, such as Ni or Cu nanoscale films. This research explores Ni and Cu surface coatings at different areal loadings (3 or 11 μg cm -2 ) on the electrochemistry of graphite/LiNi 0.6 Mn 0.2 Co 0.2 O 2 (NMC622) type Li-ion batteries. Extended galvanostatic cycling of control and metal-coated electrodes in graphite/NMC622 pouch cells are conducted under high rate conditions. Based on the overpotential of Li deposition on metal foil, both Ni and Cu treatments were anticipated to result in reduced lithium deposition. The higher metal film loadings of 11 μg cm -2 Ni- or Cu-coated electrodes exhibit the highest capacity retention after 500 cycles, with mean improvements of 8% and 9%, respectively, over uncoated graphite electrodes. Li plating quantified by X-ray diffraction indicates that the metal films effectively reduce the quantity of plated Li compared to untreated electrodes, with 11 μg cm -2 Cu providing the greatest benefit.

25 ENERGY STORAGE↗

DOE OSTI2020

Kelvin Waves during GOAmazon and Their Relationship to Deep Convection

The 2014–15 Observations and Modeling of the Green Ocean Amazon (GOAmazon) field campaign over the central Amazon near Manaus, Brazil, occurred in coordination with the larger Cloud Processes of the Main Precipitation Systems in Brazil: A Contribution to Cloud-Resolving Modeling and to the Global Precipitation Measurement (CHUVA) project across Brazil. These programs provide observations of convection over the central Amazon on diurnal to annual time scales. Here, we address the question of how Kelvin waves, observed in satellite observations of deep cloud cover over the GOAmazon region during the 2014–15 time period, modulate the growth, type, and organization of convection over the central Amazon. The answer to this question has implications for improved predictability of organized systems over the region and representation of convection and its growth on local to synoptic scales in global models. Our results demonstrate that Kelvin waves are strong modulators of synoptic-scale low- to midlevel free-tropospheric moisture, integrated moisture convergence, and surface heat fluxes. These regional modifications of the environment impact the local diurnal cycle of convection, favoring the development of mesoscale convective systems. As a result, localized rainfall is also strongly modulated, with the majority of rainfall in the GOAmazon region occurring during the passage of these systems.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Microstructure development in a cold worked SRF Nb sheet undergoing 700°C-900°C/3h heat treatments.

Bulk Nb for TESLA shaped SRF cavities is a mature technology, with high gradient (>35 MV/m) and high Q cavities (>1010, ~2K) routinely fabricated. Significant advances are in order to push Q?s to 1011 (~2K), and involve modifications to the sub-surface Nb layers by impurity doping (N, O). In order to achieve the lowest surface resistance any trapped flux needs to be expelled for cavities to reach high Q?s. There is clear evidence that cavities fabricated from polycrystalline sheets meeting current specifications require higher temperatures beyond 800oC leads to better flux expulsion, and hence improves Q. Recently, cavities fabricated with a non-traditional Nb sheet with initial cold work due to cold rolling expelled flux better after 800°C/3h heat treatment than cavities fabricated using fine-grain polycrystalline Nb sheets. Here, we analyze the microstructure development in Nb from the vendor supplied cold work non-annealed sheet that was fabricated into an SRF cavity as a function of heat treatment building upon the methodology development to analyze microstructure being developed by the FSU-MSU-UT-Austin- JLAB collaboration. The results indicate correlation between full recrystallization and better flux expulsion.

Balachandran, S.↗

DOE OSTI2021

Dynamic Rupture Modeling of the M7.1, 2019 Ridgecrest, California, Earthquake

An important part of the simulation technique implemented in the strong motion prediction recipe developed in Japan, originally proposed by Irikura and Miyake (2011) is the earthquake rupture characterization that is based on established empirical scaling relationships between source parameters and seismic moment. These scaling relationships and rupture characterization are derived from recorded data and are tested by simulations. Recent analysis of results obtained with the Recipe for the 2016 M7.1 Kumamoto earthquake performed by several researchers, indicate that in order to reproduce near-fault long-period ground motions with permanent displacements, typical for earthquakes with surface rupturing, the recipe needs modifications. In particular, improvements are required in characterizing the rupture kinematics at shallow depths, above the seismogenic zone (Irikura et al., 2019). Modeling of rupture dynamics for recorded earthquakes, and numerical simulations for different rupture scenarios, provides physical constrains on slip evolution in time and space, which can be used in adjustments of empirical source scaling relationships for large crustal earthquakes. In this study we mainly focused on rupture dynamics modeling of the 2019 M7 Ridgecrest, California earthquake. The characterization of the kinematic rupture model derived from the dynamic rupture models of this earthquake can inform further refinements of rupture modeling proposed by the Recipe. Through different rupture scenarios we investigated potential relationships between characteristics of Long Period Ground Motion Generation Area (LMGA), used in the Recipe, and asperity depth and rupture initiation.

58 GEOSCIENCES↗

NASA NTRS1976

Stellar evolution at high mass with semiconvective mixing according to the Schwarzschild criterion

Evolutionary sequences for stellar models with 10, 15, 30, and 60 solar masses, as well as four different initial chemical compositions, are calculated to the end of core helium burning using the Schwarzschild criterion for convection. The results are analyzed in terms of the modifications of interior structure and surface parameters induced by semiconvective mixing as a result of adopting the Schwarzschild criterion. It is found that the main differences from results based on the Ledoux criterion are the great extent of the convectively unstable layers in the intermediate zone and the eventual development of a fully convective zone at the base of the semiconvective one. It is shown that semiconvection develops outside the convective core just after the ZAMS stage for masses greater than 12 solar masses and just before the stage of central hydrogen exhaustion for masses greater than 6 solar masses. The present models are found to be insufficiently hot in comparison with the bulk of observed stable blue supergiants and to predict far too many red supergiants fro the range above 20 solar masses. It is concluded that something is fundamentally wrong with the models, the most likely suspects being the stellar opacities adopted and the neglect of mass loss.

Stothers, R.↗

NASA NTRS1980

Performance, emissions, and physical characteristics of a rotating combustion aircraft engine, supplement A

Testing was conducted using the basic RC2-75 engine, to which several modifications were incorporated which were designed to reduce the hydrocarbon emissions and reduce the specific fuel consumption. The modifications included close-in surface gap spark plugs, increased compression ratio rotors, and provisions for utilizing either side or peripheral intake ports, or a combination of the two if required. The proposed EPA emissions requirements were met using the normal peripheral porting. The specific fuel economy demonstrated for the modified RC2-75 was 283 g/kW-hr at 75% power and 101 brake mean effective pressure (BMEP) and 272.5 g/kW-hr at 75% power and 111 BMEP. The latter would result from rating the engine for takeoff at 285 hp and 5500 rpm, instead of 6000 rpm.

Lamping, R. K.↗

NASA NTRS1989

Applying Elastomeric Insulation Inside A Round Case

Elastomer wound onto inside surface in continuous strip. Technique being developed to apply elastomeric insulation to inner surfaces of axisymmetric cases. Requires modification of machine wrapping strip of elastomer on outside of rotating mandrel. Intended for coating insides of rocket-motor cases, technique also used to install elastomeric linings in pressure vessels, containers for chemical, and environmental chambers.

Russell, Peter G.↗

NASA NTRS1990

Platform evolution studies

The polar orbiting platform (POP), being developed by the Work Package 3 (WP3) Project at the Goddard Space Flight Center, will play a key role in the NASA Leadership Initiative, Mission to Planet Earth (MPE). It becomes, with the addition of payloads, an Earth observation satellite observatory. Mission to Planet Earth also has geostationary platforms (GEOP) as part of its global observational system. A study was begun in March 1988 to assess the applicability of the POP orbital replacement units (ORUs) for a geostationary Earth observing mission. Two test cases, representative of MPE payloads, were studied. Case A was used to emphasize the GEOP configuration and design; it used a Titan/Centaur to achieve orbit. Case B, considered to be much further in the future, included some assembly at the Space Station Freedom manned base and use of an orbital transfer vehicle to achieve orbit; requirements on the manned base to support such a mission were emphasized. The study found the POP systems more than adequate to meet GEOP requirements. Two types of changes were required for the POP ORUs: (1) modification to use only one surface for heat rejection; for the battery ORU, this meant 'opening up' the ORU to retain the radiator area with a corresponding decrease in depth; and (2) deletion of equipment not needed. The Case A configuration was shown to be within the planned capability of the Titan IV/Centaur. Assembly requirements were included for the Case B configuration, which is driven by the large microwave antennas of two of the payloads. The final review was April 19, 1989.

Walton, Barbara A.↗

NASA NTRS1994

High-temperature behavior of advanced spacecraft TPS

The objective of this work has been to develop more efficient, lighter weight, and higher temperature thermal protection systems (TPS) for future reentry space vehicles. The research carried out during this funding period involved the design, analysis, testing, fabrication, and characterization of thermal protection materials to be used on future hypersonic vehicles. This work is important for the prediction of material performance at high temperature and aids in the design of thermal protection systems for a number of programs including programs such as the National Aerospace Plane (NASP), Pegasus and Pegasus/SWERVE, the Comet Rendezvous and Flyby Vehicle (CRAF), and the Mars mission entry vehicles. Research has been performed in two main areas including development and testing of thermal protection systems (TPS) and computational research. A variety of TPS materials and coatings have been developed during this funding period. Ceramic coatings were developed for flexible insulations as well as for low density ceramic insulators. Chemical vapor deposition processes were established for the fabrication of ceramic matrix composites. Experimental testing and characterization of these materials has been carried out in the NASA Ames Research Center Thermophysics Facilities and in the Ames time-of-flight mass spectrometer facility. By means of computation, we have been better able to understand the flow structure and properties of the TPS components and to estimate the aerothermal heating, stress, ablation rate, thermal response, and shape change on the surfaces of TPS. In addition, work for the computational surface thermochemistry project has included modification of existing computer codes and creating new codes to model material response and shape change on atmospheric entry vehicles in a variety of environments (e.g., earth and Mars atmospheres).

Pallix, Joan↗

NASA NTRS2020

Experimental Impacts into Strength-Layered Targets: Crater Morphology and Morphometry

Impact cratering is a fundamental physical process that has dominated the evolution and modification of nearly every planetary surface in the Solar System. Impact craters serve as a means to probe the subsurface structure of a planetary body and provide hints about target surface properties. By examining small craters on the lunar maria and comparing these to experimental impacts in the laboratory, Oberbeck and Quaide first suggested that crater morphology can be used to estimate the thickness of a regolith layer on top of a more competent unit. Lunar craters show a morphological progression from a simple bowl shape to flat-floored and concentric craters as crater diameter increases for a given regolith thickness. This quantitative relationship is commonly used to estimate regolith thicknesses on the lunar surface and has also been explored via numerical and experimental studies. Here we report on a series of experimental impact craters formed in targets com-posed of a thin layer of loose sand on top of a stronger substrate at the Experimental Impact Laboratory at NASA Johnson Space Center.

Anderson, J. L. B.↗

NASA NTRS1992

Hypersonic code efficiency and validation studies

Renewed interest in hypersonic and supersonic flows spurred the development of the Compressible Navier-Stokes (CNS) code. Originally developed for external flows, CNS was modified to enable it to also be applied to internal high speed flows. In the initial phase of this study CNS was applied to both internal flow applications and fellow researchers were taught to run CNS. The second phase of this research was the development of surface grids over various aircraft configurations for the High Speed Research Program (HSRP). The complex nature of these configurations required the development of improved surface grid generation techniques. A significant portion of the grid generation effort was devoted to testing and recommending modifications to early versions of the S3D surface grid generation code.

Bennett, Bradford C.↗

NASA NTRS1995

Regional scale hydrology with a new land surface processes model

Through the CaPE Hydrometeorology Project, we have developed an understanding of some of the unique data quality issues involved in assimilating data of disparate types for regional-scale hydrologic modeling within a GIS framework. Among others, the issues addressed here include the development of adequate validation of the surface water budget, implementation of the STATSGO soil data set, and implementation of a remote sensing-derived landcover data set to account for surface heterogeneity. A model of land surface processes has been developed and used in studies of the sensitivity of surface fluxes and runoff to soil and landcover characterization. Results of these experiments have raised many questions about how to treat the scale-dependence of land surface-atmosphere interactions on spatial and temporal variability. In light of these questions, additional modifications are being considered for the Marshall Land Surface Processes Model. It is anticipated that these techniques can be tested and applied in conjunction with GCIP activities over regional scales.

Laymon, Charles↗

DOE OSTI2024

Material and Interface Engineering Strategies to Mitigate Decoherence in Superconducting Qubits

While significant strides have been made to increase the coherence time of superconducting qubits, further advancements are essential for realizing scalable quantum computing. Decoherence is often a result of loss and noise stemming from two-level systems and excess quasiparticles, arising due to material defects, fabrication processes, and ambient exposure, particularly at surfaces and interfaces. Our recent efforts to mitigate these decoherence mechanisms have employed a variety of strategies, including low-loss surface encapsulation materials, advanced substrate preparation techniques, modifications to metal film growth, and the development of novel fabrication processes. The structural and chemical properties of materials, surfaces, and interfaces are studied using scanning probe microscopy, electron microscopy, photoelectron spectroscopy, mass spectrometry, and X-ray diffraction, which is correlated to device performance metrics, including superconducting resonator internal quality factor and qubit T1 time. This information is used to identify and understand material sources of loss and their origins in the device fabrication process. Through multi-institution efforts within SQMS we have identified the loss mechanism of interstitial hydrogen in niobium-based devices and shown how standard fabrication processes introduce these hydrides, developing strategies to mitigate their formation.1 Furthermore, we have characterized the metal-substrate interface, including the loss of niobium-silicides formed at that interface, and developed silicon surface treatments that reduce atomic scale roughness and oxygen content at the metal-substrate and Josephson junction interfaces.2-4 By developing the connection between materials properties and the overall performance of superconducting quantum circuitry, we can develop fabrication strategies to mitigate material losses, thus supporting the ongoing efforts to enhance coherence time in superconducting quantum devices. 1. Torres-Castanedo, C. G.*, Goronzy, D. P.*, et al., Adv. Funct. Mater., 2401365 (2024) 2. Lu, X., et al., Phys. Rev. Materials 6, 064402 (2022) 3. Berti, G., Appl. Phys. Lett. 122, 192605 (2023) 4. Kopas, C. J., Goronzy, D. P., et al., arXiv:2408.02863 (2024)

Goronzy, Dominic P.↗

DOE OSTI2021

Controlling Heterogeneous Catalysis with Organic Monolayers on Metal Oxides

A key theme of heterogeneous catalysis research is achieving control of the environment surrounding the active site to precisely steer the reactivity toward desired reaction products. One method toward this goal has been the use of organic ligands or self-assembled monolayers (SAMs) on metal nanoparticles. Metal-bound SAMs are typically employed to improve catalyst selectivity but often decrease the reaction rate as a result of site blocking from the ligands. Recently, the use of metal oxide-bound organic modifiers such as organophosphonic acid (PA) SAMs has shown promise as an additional method for tuning reactions on metal oxide surfaces as well as modifying oxide-supported metal catalysts. In this Account, we summarize recent approaches to enhance catalyst performance with oxide-bound monolayers. These approaches include (1) modification of metal oxide catalysts to tune surface reactions, (2) formation of SAMs on the oxide component of supported metal catalysts to modify sites at the metal–support interface, and (3) enhancement of catalyst performance (e.g., stability) through modification of sites remote from the active sites. Further, both the headgroups and organic tail groups of PA SAMs or other ligands can influence reactions on metal oxide surfaces. Binding of the headgroup can selectively poison certain active sites, altering the selectivity in a manner analogous to metal-bound ligands (at the expense of active site quantity). Moreover, tail groups can be functionalized to interact favorably with reactants and intermediates, for instance through dipole–dipole interactions. On supported metal catalysts like Pt/Al 2 O 3 , PA SAMs can selectively form on the oxide support. This selective deposition allows for modification of the metal–support interface with minimal blockage of metal sites. PA headgroups were shown to provide tunable acid sites at the interface, dramatically improving hydrodeoxygenation rates of various alcohols. Additionally, organic tail functionality was used to activate or stabilize specific reactants at the interface, such as with the use of amine-functionalized PAs to stabilize chemisorption of CO 2 during the reverse water gas shift reaction. PAs have also been found to affect the electronic properties of bulk metal sites through long-range electron withdrawal via the oxide, providing an additional avenue to tune catalytic behavior. Finally, organic modifiers were shown to enhance catalytic performance without directly modifying the active site. For instance, in biphasic liquid environments the modification of catalyst particles with hydrophobic or hydrophilic SAMs shifts the selectivity of multipath reactions on the basis of the hydrophobicities of different intermediates and products. As another “long-range” effect, the deposition of ligands on oxide supports improved catalyst stability through both improved resistance to sintering and suppression of active site poisoning. The recent contributions discussed in this Account demonstrate the versatility and significant potential for the approach of modifying catalysts with oxide-bound organic monolayers.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Factors influencing quantum evaporation of helium from polar semiconductors from first principles

While there is much indirect evidence for the existence of dark matter (DM), to date it has evaded detection. Current efforts focus on DM masses over ~GeV—to push the sensitivity of DM searches to lower masses, new DM targets and detection schemes are needed. In this work, we focus on the latter—a novel detection scheme recently proposed to detect 10–100 meV phonons in polar target materials. Previous work showed that well-motivated models of DM can interact with polar semiconductors to produce an athermal population of phonons. This new sensing scheme proposes that these phonons then facilitate quantum evaporation of 3 He from a van der Waals film deposited on the target material. However, a fundamental understanding of the underlying process is still unclear, with several uncertainties related to the precise rate of evaporation and how it can be controlled. In this work, we use ab initio density functional theory calculations to compare the adsorption energies of helium atoms on a polar target material, sodium iodide, to understand the underlying evaporation physics. We explore the role of surface termination, monolayer coverage, and elemental species on the rate of He evaporation from the target material. Using this, we discuss the optimal target features for He-evaporation experiments and their range of tunability through chemical and physical modifications such as applied field and surface termination.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Polymer-Grafted Cellulose Nanofibrils with Enhanced Interfacial Compatibility for Stronger Poly(lactic acid) Composites

Cellulose nanofibrils (CNFs) are a promising reinforcement for biodegradable composite matrices such as poly(lactic acid) (PLA), but they require commercially scalable drying methods that preserve their fibrillar morphology along with improved interfacial interactions with polymer matrices. In this work, a water-based grafting-through polymerization scheme to modify CNFs improved spray drying behavior and reinforcement capacity in PLA composites. All polymer modifications yielded CNFs with a more fibrillar morphology after spray drying, increasing specific surface area by up to 490% compared to unmodified CNFs, values similar to conventional freeze drying. Polymer-grafted CNFs in PLA composites improved the tensile strength by 16% at 20 wt % loading and stiffness by 22% at a 10 wt % loading with two different graft-polymer chemistries compared to unmodified CNF composites. Surface energy heterogeneity measurements of the reinforcements and PLA matrix were employed to understand the improvements in composite properties. Polymer modifications lowered the total surface energy of the CNFs, and calculated ratios of work of adhesion to work of cohesion suggested improved interfacial compatibility for four of the modified CNFs with PLA. Rheological oscillatory shear studies of the composites correlated solid-like melt behavior, as demonstrated by storage moduli dominance, with higher tensile strength. Thermal analysis of the composites revealed that excessive plasticization by the poly(oligoethylene glycol methyl ether methacrylate)-grafted sample potentially offset mechanical property improvements imparted by the more fibrillar morphology. This work provides an opportunity for large-scale manufacturing of CNF/PLA composites via an entirely aqueous modification scheme and industrially relevant spray drying process.

36 MATERIALS SCIENCE↗

NASA NTRS1992

Floor-fractured crater models for igneous crater modification on Venus

Although crater modification on the Earth, Moon, and Mars results from surface erosion and crater infilling, a significant number of craters on the Moon also exhibit distinctive patterns of crater-centered fracturing and volcanism that can be modeled as the result of igneous crater modification. Here, we consider the possible effects of Venus surface conditions on this model, describe two examples of such crater modification, and then briefly discuss the constraints these craters place on conditions at depth.

Wichman, R. W.↗