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DOE OSTI2024

Investigation of acoustic waves under subsurface conditions to improve the predictions of rock mechanical properties and natural fracture characteristics

Mechanical properties and natural fracture characteristics are critical to investigate for subsurface engineering applications, including carbon storage, well drilling, and stimulation, as they govern rock stability, fluid flow, and mechanical behavior under stress. This dissertation integrates experimental and machine learning approaches to enhance the prediction and understanding of these properties by analyzing acoustic wave behavior under varied subsurface conditions. First, the influence of temperature, pore pressure, and supercritical CO2 (scCO2) saturation on poroelastic properties is examined using Gray Berea sandstone samples. The results show that temperature and pore pressure significantly affect the bulk modulus and Biot’s coefficient, while scCO2 saturation impacts rock compressibility, informing strategies for effective geological carbon storage. The study extends this understanding by experimentally evaluating the impact of reservoir depletion on the dynamic mechanical properties of the emerging Caney shale in South Oklahoma with the employment of unsupervised machine learning to predict static mechanical properties across the Caney shale. Integrating petrophysical data and chemostratigraphy, the workflow—featuring K-means clustering, principal component analysis (PCA), and inverse distance weighting (IDW)—improves stratigraphic characterization and the estimation of static-to-dynamic modulus ratios, which is vital for optimizing drilling and stimulation strategies. Finally, the work explores how natural fracture characteristics in shale influence acoustic waveforms and shear wave splitting (SWS) analysis. Experimental data on fractured samples under different stress and temperature conditions, combined with machine learning models such as K-nearest neighbors (KNN) and extreme gradient boosting (XGBoost), reveal key fracture properties impacting SWS and wave propagation. Together, these studies provide a comprehensive framework for linking acoustic wave behavior with rock properties, advancing the methods for monitoring and predicting geomechanical changes. The insights offered valuable implications for safer, more efficient CO2 injection, hydrocarbon extraction, and subsurface management.

Elkholy, Sherif↗

DOE OSTI2025

Challenges in Continuous In-Field Critical Current Testing of High-Temperature Superconducting Tapes: Thermal and Mechanical Perspectives

High-temperature superconductors (HTS) are essential for ultra-high-field applications requiring exceptional current-carrying capacity under extreme conditions. However, systematic characterization of critical current in long-length conductors remains challenging due to complex thermal, electromag netic, and mechanical interactions during continuous testing. This study reports the development of a continuous in-field magnetization testing system for position-dependent critical current measurement in HTS tapes at 20 K under 7.5 T fields applied normal to the tape plane, enabling identification of performance-limiting regions that could compromise magnet stability. Here, the system addresses two fundamental challenges inherent to cryogenic reel to-reel testing. First, thermal management requires continuous cooling of a moving conductor to 20 K, achieved through liquid nitrogen precooling combined with a 100 W@20 K Gifford McMahon cryocooler. Second, screening currents in high fields generate Lorentz forces that induce twisting, bowing, and potential delamination. To mitigate these risks, we propose mechanical reinforcement and active current density suppression strategies. Numerical simulations using the stream function formulation reveal four primary failure modes: frictional heating at guide interfaces, unstable equilibria causing deformation, transverse current-induced stresses at guide transitions, and unsupported forces in vertical spans. Our mitigation strategies include PTFE coated guides to minimize friction, spring-loaded stabilization mechanisms to maintain tape alignment, controlled pre-heating using the liquid nitrogen thermal jacket to suppress critical current at stress points, and optimized guide positioning to minimize force accumulation. The experimental system is nearing completion, with testing planned to commence within two months. Preliminary validation at 65 K under 0.5 T demonstrates strong correlation between simulation-predicted mechanical instabilities and observed critical current variations during conductor tran sitions through the measurement region. These findings establish a robust foundation for quality assurance protocols essential to next-generation superconducting magnet applications.

Chen, Siwei [Princeton Plasma Physics Laboratory (↗

DOE OSTI2021

Fire effects on the persistence of soil organic matter and long-term carbon storage

One paradigm in biogeochemistry is that frequent disturbance tends to deplete carbon (C) in soil organic matter (SOM) by reducing biomass inputs and promoting losses. However, disturbance by fire has challenged this paradigm because soil C responses to frequent and/or intense fires are highly variable, despite observed declines in biomass inputs. Here, we review recent advances to illustrate that fire-driven changes in decomposition, mediated by altered SOM stability, are an important compensatory process offsetting declines in aboveground biomass pools. Fire alters the stability of SOM by affecting both the physicochemical properties of the SOM and the environmental drivers of decomposition, potentially offsetting C lost via combustion, but the mechanisms affecting the SOM stability differ across ecosystems. Thus, shifting our focus from a top-down view of fire impacting C cycling via changes in plant biomass to a bottom-up view of changes in decomposition may help to elucidate counterintuitive trends in the response of SOM to burning. Finally, given that 70% of global topsoil C is in fire-prone regions, using fire to promote SOM stability may be an important nature-based climate solution to increase C storage.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Revealing the Internal Architecture of Alkaline Fuel Cell Membranes with Cryo-4D-STEM and Cryo-STEM-EELS

Characterization of the internal architecture of polymer materials plays an important role in the development of energy devices such as fuel cells. The beam sensitivity of polymer materials coupled with their inherent low contrast makes imaging using conventional TEM and STEM techniques a challenge. Here, we demonstrate robust mapping of the internal architecture of fuel cell polymer membranes using cryo-4D-STEM and cryo-STEM-EELS. Here, we will focus on characterization of alkaline anion exchange membranes (AAEMs) used in AAEM fuel cells, a cheaper alternative to current fuel cell technologies as they allow for platinum group metal-free catalysts. In fuel cell polymer membranes, the internal architecture is critical in performance metrics such as conductivity, mechanical durability, and chemical stability.

30 DIRECT ENERGY CONVERSION↗

DOE OSTI2021

Carbon sequestration of steel slag and carbonation for activating RO phase

Carbonation of Ca/Mg minerals in industrial alkaline residues is a technology to sequester CO{sub 2} and reduce its emissions to the atmosphere. In this work, BSE-EDS were used to determine the mineral phase in steel slag; compositions of RO phase were identified and simulated. The carbon sequestration of steel slag was studied, and RO phase was activated by carbonation. Result shows that the amount of CO{sub 2} sequestered in steel slag and RO phase increases as carbonation time increases. Under autoclaving condition, the hydration ratio of MgO in RO phase was 20.10%. Through carbonation, up to 58.83% of MgO in RO phase can be converted into MgCO{sub 3}, and the activation of RO phase by carbonation was manifested. The mechanical properties and volume stability of carbonated steel slag were improved, proving that the positive effect of carbonation on steel slag when applied in cement and cementitious materials.

36 MATERIALS SCIENCE↗

DOE OSTI2020

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↗

DOE OSTI2024

Wehnelt photoemission in an ultrafast electron microscope: Stability and usability

We tested and compared the stability and usability of three different cathode materials and configurations in a thermionic-based ultrafast electron microscope: (1) on-axis thermionic and photoemission from a custom 100 μm diameter LaB 6 source with a graphite guard ring, (2) off-axis photoemission from the Ni aperture surface of the Wehnelt electrode, and (3) on-axis thermionic and photoemission from a custom 200 μm diameter polycrystalline Ta source. For each cathode type and configuration, including the Ni Wehnelt aperture, we illustrate how the photoelectron beam-current stability is deleteriously impacted by simultaneous cooling of the source following thermionic heating. Furthermore, we demonstrate usability via collection of parallel- and convergent-beam electron diffraction patterns and by formation of the optimum probe size. We find that usability of the off-axis Ni Wehnelt-aperture photoemission is at least comparable to on-axis LaB 6 thermionic emission, as well as to on-axis photoemission [the heretofore conventional approach to ultrafast electron microscopy (UEM) in thermionic-based instruments]. However, the stability and achievable beam currents for off-axis photoemission from the Wehnelt aperture were superior to that of the other cathode types and configurations, regardless of the electron-emission mechanism. Beam-current stability for this configuration was found to be ±1% (one standard deviation from the mean) for 70 min (longest duration tested), and steady-state beam current was reached within the sampling-time resolution used here (~1 s) for 15 pA beam currents (i.e., 460 electrons per packet for a 200 kHz repetition rate). Repeatability and robustness of the steady-state condition were also found to be within ±1% of the mean. We discuss the implications of these findings for UEM imaging and diffraction experiments, for pulsed-beam damage measurements, and for practical switching between optimum conventional TEM and UEM operation within the same instrument.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2021

Improving Photostability of Cesium-Doped Formamidinium Lead Triiodide Perovskite

Using time-resolved in situ X-ray photoelectron spectroscopy, we identify and suppress rapid degradation mechanisms for cesium-stabilized formamidinium lead iodide perovskite materials used in state-of-the-art photovoltaics. Accelerated degradation under high light intensity and heating reveals a photocatalytic reaction pathway responsible for rapid decomposition in iodide-rich compositions and a slower pathway for more stoichiometric samples. Using Avrami–Erofe’ev kinetic analysis, we find that the fast process is consistent with a 2D crystallization and growth mechanism fueled by excess halide salt at grain boundaries and surfaces. Moreover, the rate of decomposition varies dramatically with the wavelength of light used to illuminate the thin films. Furthermore, our results reveal the photodegradation mechanisms of PbI 2 and excess iodide and provide a path to increasing perovskite stability under photoexcitation.

14 SOLAR ENERGY↗

DOE OSTI2024

The association of structural chirality and liquid crystal anchoring in polymer stabilized cholesteric liquid crystals

Polymer stabilized cholesteric liquid crystals (PSCLCs) are electrically reconfigurable reflective elements. Prior studies have hypothesized and indirectly confirmed that the electro-optic response of these composites is associated with the electrically mediated distortion of the stabilizing polymer network. The proposed mechanism is based on the retention of structural chirality in the polymer stabilizing network, which upon deformation is spatially distorted, which accordingly affects the pitch of the surrounding low molar-mass liquid crystal host. Here, we utilize fluorescent confocal polarized microscopy to directly assess the electro-optic response of PSCLCs. By utilizing dual fluorescent probes, sequential imaging experiments confirm that the periodicity of the polymer stabilizing network matches that of the low molar-mass liquid crystal host. Further, we isolate distinct ion-polymer interactions that manifest in certain photopolymerization conditions.

Radka, Brian P.↗

DOE OSTI2020

Mechanisms of mechanochemical synthesis of cesium lead halides: pathways toward stabilization of α-CsPbI 3

Cesium lead iodide with cubic perovskite structure (α-CsPbI 3 ) is gaining significant interest in photovoltaic applications due to its excellent absorbance of the visible solar light and other attractive optoelectronic properties. However, the synthesis of stable α-CsPbI 3 poses a significant challenge. Mechanochemical synthesis is emerging as a suitable method for the preparation of cesium lead halides. This work investigates the ball milling-induced synthesis of cesium lead halides perovskite phase using halide mixing or doping approaches. The synthesis in the CsI + PbI 2 , CsBr + PbBr 2 , CsBr + PbI 2 , and CsI + PbI 2 + NdI 3 mixtures and halide exchange reactions in the CsPbBr 3 + 3KI and CsBr + PbBr 2 + 3KI systems are investigated to elucidate the mechanism of this process. Then, CsPb(I 1–x Br x ) 3 and CsPb( 1–y )Nd y I 3 materials with different x and y ratios are prepared, and their stability is probed in the air using light absorption spectroscopy. These results suggest that Nd doping is more efficient in the stabilization of the perovskite structure than partial replacement of iodine with bromine. Microstructure observations reveal the existence of two different product formation mechanisms depending on the mechanical properties of reactants. The results reveal that the milling temperature has a significant impact on the reaction kinetics. Here, the produced particles nucleate and grow at the reactant interface and retard the synthesis reaction by creating a diffusion barrier. Extended milling reduces the product particle size and creates fresh contact between reactants, thus facilitating reaction completion.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Phase stability in the Hf-N and Zr-N systems

Hf and Zr nitrides are promising compounds for many technologically important areas, including high-temperature structural applications, quantum computing, and solar and optical applications. Here, this article reports on a comprehensive first-principles statistical mechanics study of phase stability in the Hf-N and Zr-N binary systems. A high solubility of nitrogen in the hcp forms of Hf and Zr is predicted. The rocksalt forms of HfN and ZrN can also tolerate a high degree of off-stoichiometry through the introduction of nitrogen and metal vacancies. The Hf-N binary favors a family of stacking faulted parent crystal structures at intermediate nitrogen concentrations that host a unique form of short-range order among nitrogen interstitials and vacancies. These phases can accommodate some degree of configurational entropy and remain ordered to temperatures as high as 1200 K.

Monte Carlo methods↗

DOE OSTI2026

Design Trade-Offs in Composite Fuel Cell Membranes: Effects of Reinforcement and Chemical Additives

Perfluorosulfonic acid (PFSA) membranes are critical components in proton exchange membrane fuel cells, where performance depends on balancing ionic conductivity, mechanical durability, and chemical stability. This study characterizes a composite membrane (NC700) featuring PFSA-impregnated expanded polytetrafluoroethylene (ePTFE) reinforcement and cerium-based radical scavengers, benchmarked against unreinforced NR211. Complementary techniques, including electron microscopy, X-ray scattering, infrared spectroscopy, thermogravimetric analysis, and dynamic mechanical analysis, identify the structural and compositional strategies employed in NC700. Water sorption isotherms reveal lower water uptake for NC700 across all conditions, attributed to reinforcement and cerium incorporation. Reinforcement reduces in-plane swelling from 11% to 2.1% at 90% RH, confirming strong swelling anisotropy, while maintaining mechanical properties at elevated temperatures. While the ionic conductivity of NC700 is approximately 10% lower than that of NR211, the reduced thickness yields a 40% decrease in calculated area-specific resistance, suggesting the composite architecture can favorably shift the conductivity-stability trade-off. The composite structure also reduces gas permeability, indicating potential for improved separator function alongside favorable transport properties. Systematic deconvolution of reinforcement and additive contributions shows that conductivity losses from cerium incorporation are largely offset by gains from the lower equivalent-weight polymer, providing quantitative relationships that may guide composite membrane design for fuel cells and other electrochemical applications.

25 ENERGY STORAGE↗

DOE OSTI2024

From phase decomposition to evaporation: A multi-modal evaluation of thermally degraded model lightweight high-entropy alloy

Lightweight high-entropy alloys (LHEAs) have the potential to replace conventional lightweight materials due to their superior mechanical properties and thermal stability. However, the thermal degradation pattern of LHEAs from phase decomposition to evaporation is not clear. We develop a new Al-based dual phase (FCC + HCP) LHEA—AlTi 0.45 CuZn, and further investigate its thermal degradation behavior for potential high-temperature structural applications. Using multimodal advanced characterization techniques such as differential scanning calorimetry/thermogravimetric analysis, scanning/transmission electron microscopy, and synchrotron X-ray diffraction/pair distribution function (XRD/PDF), a sequence of thermal degradation events beyond the thermal phase stability limit—between 250 and 360 °C—is observed. These include phase decomposition at ~360 °C, Zn evaporation at ~750 °C, and LHEA melting at 880 °C which results in ~25% cumulative weight loss. The formation of Al-Ti phase off the AlTi 0.45 CuZn matrix is due to the largest negative mixing enthalpy for Al-Ti than other binary pairs. Similarly, Zn evaporation from AlTi 0.45 CuZn LHEA is due to its faster evaporation rate than other constituent elements. The high-resolution synchrotron XRD and PDF results support the aforementioned observations; in addition, they reveal local atomic arrangements, local strain, and sluggish grain growth in the LHEA. Among other LHEAs of close density range (5.55 ≤ ρ ≤ 5.85 g/cc), the investigated LHEA exhibits outstanding nano-indentation hardness values due to the coupled grain size effect and HCP phase strengthening of the FCC matrix. As the search for LHEAs for lightweight applications grows, this study shows the potential use of AlTi 0.45 CuZn LHEA for structural applications even at elevated temperatures.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2023

Synergistic effect of polyaniline on stabilizing Pt nanoparticles in PEMFCs†

The stability of Pt nanoparticles on a carbon support is crucial for the lifespan of polymer electrolyte membrane fuel cells as well as other electrocatalysis systems such as electrolyzers. Here we took the approach of utilizing the covalently grafted polyaniline on carbon to stabilize Pt nanoparticles by simultaneously alleviating the particle migration and mitigating the Ostwald ripening, which are two major mechanisms for loss of the catalyst stability. A comprehensive investigation of the stability and performance of Pt catalyst nanoparticles on these supports reveals that the polyaniline can shift the Pt L edge binding energy and the Pt 4f peak energy, leading to the increased redox potential of the Pt nanoparticles and making them more resistant to oxidation. Interestingly, the highest polyaniline density (50 wt%) does not show the best catalyst stability, rather, the second (33 wt%) demonstrates the best catalyst stability among these catalysts. Combining the XPS, XAS and fuel cell stability studies, we concluded that the locations of the Pt nanoparticles over the polyaniline layer on the carbon surface depend on the surface density of the polyaniline over the carbon surface. The Pt nanoparticles in the 50 wt% polyaniline catalyst are wrapped by the polyaniline polymer but do not sit directly on the carbon surface, while Pt nanoparticles in the 33 wt% polyaniline catalyst sit on the carbon surface and are densely surrounded by the polyaniline polymer. The results show that the mass activity loss is 12.5% while the ECSA (electrochemically active surface area) loss is 37.1% after 30k cycles of accelerating stress test for the 33 wt% polyaniline catalyst, far exceeding the DOE 2020 target for MEA (i.e., mass activity loss < 50%, and ECSA loss < 40%). Overall, the polyaniline has a synergistic effect on mitigating the surface migration and slowing down the Ostwald ripening to stabilize the Pt nanoparticles in fuel cells. The novel strategy to stabilize Pt nanoparticles using polyaniline opens a new pathway in the development of highly stable catalysts: relying on the functionalization group on the carbon support, instead of just focusing on the catalyst itself.

Li, Chenzhao↗

DOE OSTI2021

Polyethylene Glycol Crowder’s Effect on Enzyme Aggregation, Thermal Stability, and Residual Catalytic Activity

Protein stability and performance in various natural and artificial systems incorporating many other macromolecules for therapeutic, diagnostic, sensor, and biotechnological applications attract increasing interest with the expansion of these technologies. Here we address the catalytic activity of lysozyme protein (LYZ) in the presence of a polyethylene glycol (PEG) crowder in a broad range of concentrations and temperatures in aqueous solutions of two different molecular mass PEG samples (Mw = 3350 and 10000 g/mol). The phase behavior of PEG–protein solutions is examined by using dynamic light scattering (DLS) and small-angle X-ray scattering (SAXS), while the enzyme denaturing is monitored by using an activity assay (AS) and circular dichroism (CD) spectroscopy. Molecular dynamic (MD) simulations are used to illustrate the effect of PEG concentration on protein stability at high temperatures. The results demonstrate that LYZ residual activity after 1 h incubation at 80 °C is improved from 15% up to 55% with the addition of PEG. The improvement is attributed to two underlying mechanisms. (i) Primarily, the stabilizing effect is due to the suppression of the enzyme aggregation because of the stronger PEG–protein interactions caused by the increased hydrophobicity of PEG and lysozyme at elevated temperatures. (ii) The MD simulations showed that the addition of PEG to some degree stabilizes the secondary structures of the enzyme by delaying unfolding at elevated temperatures. The more pronounced effect is observed with an increase in PEG concentration. This trend is consistent with CD and AS experimental results, where the thermal stability is strengthened with increasing of PEG concentration and molecular mass. Overall, the results show that the highest stabilizing effect is approached at the critical overlap concentration of PEG.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2025

Anomalous elastic softening in ferroelectric hafnia under pressure

his study employs first-principles density-functional theory (DFT) calculations to explore the elastic and mechanical properties of ferroelectric hafnia (HfO 2 ) in its polar orthorhombic 𝑃⁢𝑐⁢𝑎⁢2 1 phase under varying hydrostatic pressure conditions up to 30 GPa. Utilizing a plane-wave basis set and Perdew-Burke-Ernzerhof generalized-gradient approximation for solids in our DFT calculations, we investigate both pure and yttrium-substituted HfO 2 . Our findings reveal an anomalous reduction in the 𝐶 33 component of the elastic tensor with increasing pressure, which becomes significant above 15 GPa and signals a potential pressure-driven structural phase transition at higher pressure. The analysis of atomic displacements under pressure sheds light on the unusual mechanical behavior and phase stability of this material. Additionally, we observe a transition from an indirect band gap to a direct band gap with increasing pressure, which could have significant implications for optical applications. Here, the effects of yttrium substitution on the mechanical and electronic properties are further examined, revealing that yttrium substitution softens the elastic response of this material and reduces the electronic band gap. These results enhance our understanding of elastic and mechanical responses of ferroelectric hafnia and its potential for applications in microelectronics, piezoelectric devices, and nonvolatile ferroelectric random-access memories. Further experimental validation is recommended to confirm our predictions and explore the practical implications of the observed phase transitions and electronic behavior of the ferroelectric hafnia under high-pressure conditions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2022

Highly Loaded Sulfur Cathode, Coated Separator and Gel Electrolyte for High Rate Li-Sulfur Batteries

As one of DOE Battery 500 Seedling projects, Cornell University and EIC Labs investigated and developed i) highly loaded sulfur cathodes (> 3 mg/cm 2 ), ii) hybrid separators, and iii) gel ceramic electrolytes (GCE) to mitigate the low rate capability, shuttling effect and limited cycle life in high performance Li-Sulfur batteries. Scalable nanomanufacturing processes such as air-controlled electrospray (ACES) and gas-assisted electrospinning (GAES) have been utilized to develop directly deposited electrodes and polymer/ceramic hybrid separators. First, in the development of highly loaded cathodes, alternating layers of sulfur impregnated mesoporous carbon and graphene were fabricated via ACES and the resulting layered cathodes and coated separators exhibit higher capacity and capacity retention (about 1,000 mAh/g capacity with less than 0.02% fade/cycles) than single layer cathode or cathode prepared by conventional slurry cast. Alternating layer approach via ACES has been applied to high loading systems (3 - 5 mg S/cm 2 ), demonstrating the potential to increase sulfur utilization and capacity retention. We have also incorporated iron oxides (Fe 3 O 4 ) into S/mesoporous carbon/graphene cathodes to enhance sulfur utilization and mitigation of polysulfide shuttling. and the effect of Fe 3 O 4 in mesoporous carbon and Gr is highly pronounced at high C rates of 1C and 2C cycling performance. To further improve the cathodes at high rates, graphene nanoribbons (GNR) which can promote ion transport were incorporated in the cathode, resulting in 550 mAh/g at 5C/5C rates. Hybrid Li-ion/Li-S cathodes has also been explored to better engage unreacted polysulfides during charge/discharge. S/LFP hybrid cathodes offer higher sulfur utilization and enhanced rate capability, as well as higher areal loading. This study suggests inclusion of iron phosphide (Fe2P) which can chemically interact with polysulfides can further enhance sulfur utilization and mitigation of soluble polysulfides at high rates. Secondly, in the development of hybrid separators, we first employed graphene coating on the commercial polyolefin separators, which exhibits higher capability, better capacity retention and enhanced rate capability. To improve the rate capability with enhanced safety features such as thermal stability and nonflammability, we developed polymer/ceramic hybrids based on thermally stable polyimide (PI) and room temperature curable ceramic precursors such as organopolysilazane (OPSZ) or polysilsesquioxanes (PSSQ), which exhibit no shrinkages up to 300 ºC and non-flammability. To improve mechanical properties and electrochemical stability, polybenzimidazole (PBI) and alumina have been incorporated in polymer/ceramic hybrid separator, replacing PI and OPSZ/PSSQ, respectively. Finally, the gel ceramic electrolyte (GCE) based on ceramic cross linkers have been applied to make Li-S cells even safer and also to mitigate the polysulfide shuttling further. The resulting gel ceramic electrolyte offers improved capacity retention and rate capability, and also effectively mitigates polysulfide shuttling which was also confirmed by modeling. Inclusion of high ion conducting additives into GCE together with polymer/ceramic hybrid separators exhibit the higher ionic conductivity than liquid electrolyte with commercial polyolefin separator. We demonstrated that the developed highly loaded sulfur cathodes, polymer/ceramic hybrid separators and gel ceramic electrolyte can effectively mitigate the low rate capability, shuttling effect and limited cycle life in high performance Li-Sulfur batteries with improved safety.

25 ENERGY STORAGE↗

DOE OSTI2022

Vorticity-induced flow-focusing leads to bubble entrainment in an inkjet printhead: Synchrotron x-ray and volume-of-fluid visualizations

The oscillatory flows present in an inkjet printhead can lead to strong deformations of the air-liquid interface at the nozzle exit. Such deformations may lead to an inward directed air jet with bubble pinch-off and the subsequent entrainment of an air bubble, which is highly detrimental to the stability of inkjet printing. Understanding the mechanisms of bubble entrainment is therefore crucial to improving print stability. Here, in the present work, we use ultrafast x-ray phase-contrast imaging and direct numerical simulations based on the volume-of-fluid method to study the mechanisms underlying the bubble entrainment in a piezoacoustic printhead. We first demonstrate good agreement between experiments and numerics. We then show the different classes of bubble pinch-off obtained in experiments, and that those were also captured numerically. The numerical results are then used to show that the baroclinic torque, which is generated at the gas-liquid interface due to the misalignment of density and pressure gradients, results in a flow-focusing effect that drives the formation of the air jet from which a bubble can pinch off.

42 ENGINEERING↗