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DOE OSTI2021

Toward Optimizing Electrospun Nanofiber Fuel Cell Catalyst Layers: Polymer–Particle Interactions and Spinnability

We investigate the effect of the poly(acrylic acid) (PAA) carrier polymer concentration on the microstructure and rheological properties of catalyst inks for electrospun polymer–electrolyte membrane fuel-cell catalyst layers. Characterization of an ink microstructure using oscillatory shear rheology showed that the catalyst particles (platinum on carbon) are significantly agglomerated in the absence of PAA or an ionomer. Both the ionomer and PAA promoted the stability of the particles against agglomeration via electrosteric stabilization by adsorbing onto the particle surface. Increasing the PAA concentration increased the stability of the particles (or reduced the agglomerated structure) due to increasing PAA coverage onto the free surface area of the particles. However, beyond a certain increase in concentration, PAA was found to predominantly remain as an excess free polymer in the ink due to an insufficient free/available surface area on the particles for further PAA coverage. Extensional rheology measurements demonstrated that PAA enhances the extensional viscosities of the inks. Consequently, increasing the PAA concentration in the ink promoted the evolution of uniform nanofibers. However, beyond a certain concentration, a significant increase in the shear viscosities of the inks led to defective fiber morphologies because of the onset of flow instabilities. Electrochemical performance comparisons between catalyst layers with different PAA concentrations showed maximum performance at the PAA concentration that led to the least agglomerated structure of the catalyst, most uniform fiber morphologies, and low concentrations of free (non-adsorbing) PAA in the electrode. These results provide a rationale for optimization of electrospun catalyst nanofibers for both spinnability and electrochemical performance.

25 ENERGY STORAGE↗

DOE OSTI2021

Evaluating Effects of Shear Processing on 2D Crystalline Materials in 3D Metal Matrices: Atomistic Understanding of High Shear Deformation of Copper Graphene Composites

Composites made of copper and graphene demonstrate high strength, lubricity and enhanced electrical and thermal conductivity compared pure copper. However, manufacturing these composites at bulk volumes for industrial applications has been a big challenge. Shear deformation assisted processing is an effective method for manufacturing materials such as copper-graphene composites demonstrating ultra-fine grain structures and compositional homogeneity. Nevertheless, microstructural evolution of the composites and their property development under such conditions is not clearly understood currently. To rectify this gap in literature, high strain shear deformation of copper coated graphene foils was performed using a tribometer pin in this study. Changes in microstructure of the composite as well as the constituent components under shear deformation was correlated to process conditions. A sharp increase in the coefficient of friction attributed to rupture and smearing of graphene layer into copper substrate was observed during the shear processing. The coefficient of friction of the sheared copper/graphene composite was lower than that of pure copper, suggesting that partially worn graphene is effectively lubricious at the macroscale. A multimodal characterization of the processed region further revealed a shear deformation-induced ultrafine two-phase grain-structure consisting of copper and graphitic domains. Shear deformation reduced the copper grain size from around 50 – 100 µm to ~200 nm on an average and ~2 – 5 nm in some locations. The semicrystalline graphene films were observed to fracture into 10 – 50 µm size flakes. Oxygen enrichment was observed in the processed region. Finally, graphitic domain were identified for the first time in the copper matrix and not just at the grain boundaries providing evidence for a metastable composite microstructure as a result of solid phase processing at room temperature.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Rapid manufacturing of tailored preforms

A method for rapid manufacturing of three dimensional discontinuous fiber preforms is provided. The method includes the deposition of a polymeric material containing fibers on a surface to form a tailored charge for compression molding. The reinforced polymeric material may be a thermoplastic or a reactive polymer with viscosity low enough to allow flow through an orifice during deposition, yet high enough zero shear viscosity to retain the approximate shape of the deposited charge. The material can be deposited in a predetermined pattern to induce the desired mechanical properties through alignment of the fibers. This deposition can be performed in a single layer or in multiple layers. The alignment is achieved passively by shear alignment of the fibers or actively through fiber orientation control or mixing. The fibers can be of the desired material, length, and morphology, including short and long filaments.

Kunc, Vlastimil↗

DOE OSTI2025

On Master-Length Scale Formulations for Stable Conditions in Turbulence Closure Models

Three formulations of the turbulence-length scales used in numerical modelling of atmospheric flows are compared. The comparison is made using the Mellor–Yamada–Nakanishi–Niino turbulence closure model within the stable boundary layer local similarity framework. With an appropriate choice of model constants, the model predictions are barely discernible and compare well with the empirical data obtained from the SHEBA campaign.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Evaluation of Monin‐Obukhov Similarity Theory Wind Profiles in Convective Storm Environments and Cold Pools at the ARM Southern Great Plains Atmospheric Observatory

Monin-Obukhov similarity theory (MOST) is widely used in numerical weather prediction to model surface fluxes of momentum, heat, and water vapor. However, MOST is based on assumptions of steady state and horizontally homogeneous turbulence that can lead to prediction errors in and around convective storms. To understand the nature of these errors, we used wind and eddy covariance flux measurements from the Atmospheric Radiation Measurement Southern Great Plains Atmospheric Observatory to evaluate MOST wind profiles in fair-weather and convective storm environments, specifically those of mesoscale convective systems and ordinary thunderstorms. MOST wind profiles agreed well with observations in fair-weather cases, while in convective storm cases the theory systematically overestimated shear in cold pools after gust front passage. Surface layer stability was found to be important in assessing MOST within convective storm environments. The overestimation of wind shear in cold pools suggests the role of non-local fluxes in transferring momentum downward. We discuss reasons for differences and agreement with past studies, and conclude with recommendations to improve prediction of surface winds and fluxes in convective storm simulations.

58 GEOSCIENCES↗

DOE OSTI2024

Flashback characterization of additively manufactured swirl-stabilized fuel injector with varying surface roughness

This work investigates the effects of as-built surface roughness on the flashback propensity in additively manufactured (AM) swirl-stabilized lean premixed (LPM) fuel injectors. Adoption of AM for rapid prototyping and fabrication of complex fuel-flexible injector designs requires investigating surface roughness effects on the flow and flame stability characteristics of the combustor. Wall roughness increases the near-wall shear, which could alter the boundary layer structure and change the propensity for flame flashback. Accounting for the realistic as-built surface roughness is crucial in carrying out computational modeling and experimental analysis to establish a feedback loop for the precision designing of fuel-flexible injectors. The presented numerical analysis of as-built AM injector is an essential consideration to optimize injector design for aerodynamics and additive manufacturability.

Mohanty, Pratikshya↗

DOE OSTI2020

The Effects of Wind Veer During the Morning and Evening Transitions

Direction and speed wind shear modify turbine performance by changing inflow conditions on turbine blades. Using observations from the 2013 CWEX campaign, we found the daily atmospheric boundary layer transitions (morning and evening) match periods of high electricity demand for a wind farm in central Iowa. Power production during these periods was undermined for large direction shear and low speed shear scenarios. The morning transition displayed larger direction shear over the rotor layer for most wind speeds compared to the evening period. This resulted in lower turbine performance for the morning compared to the evening and whole day. This study shows that the combined effect of direction and speed shear is affecting turbine operation during high electricity demand times of day, predominantly during the morning at this wind farm.

17 WIND ENERGY↗

DOE OSTI2020

Fabrication of films and coatings used to activate shear thickening, impact resistant electrolytes

A method of making a passively impact resistant composite electrolyte and separator layer includes providing a suspension composition including electrically non-conducting particles that enable shear thickening. The particles can have a polydispersity index of no greater than 0.1, an average particle size in a range of from 50 nm to 1 um, and an absolute zeta potential of greater than ±40 mV. A particle suspension solvent is provided for suspending the particles. The suspension composition is applied to a porous separator material. A portion of the particles and suspension solvent penetrate the pores and the remainder of the particles in the suspension composition are distributed across the surface of the separator material. The suspension solvent is evaporated from the separator material to provide a shear thickening particle loaded separator. A separator assembly and a passivated battery are also disclosed.

25 ENERGY STORAGE↗

DOE OSTI2022

Fabrication of films and coatings used to activate shear thickening, impact resistant electrolytes

Armstrong, Beth L.↗

DOE OSTI2022

Mixing Driven by Critical Reflection of Near-Inertial Waves over the Texas–Louisiana Shelf

Studies of internal wave-driven mixing in the coastal ocean have been focused on internal tides, while wind-driven near-inertial waves (NIWs) have received less attention in this regard. Here, this study demonstrates a scenario of NIW-driven mixing over the Texas–Louisiana shelf. Supported by a high-resolution simulation over the shelf, the NIWs driven by land–sea breeze radiate downward at a sharp front and enhance the mixing in the bottom boundary layer where the NIWs are focused because of slantwise critical reflection. The criterion for slantwise critical reflection of NIWs is ω=$\sqrt{f{^2}+s^{2}_{bot}N{^2}(1-s_{ρ}/s_{bot})}$ (where ω is the wave frequency, s bot is the bottom slope, and s ρ is the isopycnal slope), under the assumption that the mean flow is in a thermal wind balance and only varies in the slope-normal direction. The mechanism driving the enhanced mixing is explored in an idealized simulation. During slantwise critical reflection, NIWs are amplified with enhanced shear and periodically destratify a bottom boundary layer via differential buoyancy advection, leading to periodically enhanced mixing. Turbulent transport of tracers is also enhanced during slantwise critical reflection of NIWs, which has implications for bottom hypoxia over the Texas–Louisiana shelf.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Traction-separation response of bilayer graphene interfaces: The role of an intercalated single atomic layer of water molecules and hydroxyl groups

Molecular dynamics simulations of the normal and shear traction-separation response of dry and wet bilayer graphene interfaces were performed. The influence of a single, atomic layer of water molecules sandwiched between graphene layers and hydroxyl functionalization on one or both layers were investigated. Hydroxyl groups provided a shielding effect during normal separation while favoring stick-slip friction under sliding conditions. The single, atomic layer of water molecules confined between hydrophilic and asymmetric hydrophobic/hydrophilic surfaces was found to ease sliding friction. The mechanisms arose from the balance between the attractive and repulsive graphene/water interactions through bridges of single water molecules between the two surfaces and the structure of the water monolayer under confinement for which an out-of-plane water/water hydrogen bond network could not be developed. The single, atomic layer of water molecules reduced the sliding friction the most when both surfaces were hydrophilic and lowered the sliding friction of the asymmetric hydrophobic/hydrophilic interfaces to that when both surfaces were hydrophobic. An optimal hydroxyl surface coverage of less than 10% may exist for efficient water lubrication, with diminishing effect with increasing number of hydroxyl groups. Finally, the findings offer a design strategy for assembling bilayer graphene interfaces with tailored friction and sliding contact properties.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Turbulent Kinetic Energy Budgets over Gentle Topography Covered by Forests

Large-eddy simulations of flow over a “horizontally” uniform model forest are used to investigate the effects of gentle topography on the turbulent kinetic energy (TKE) budget within the canopy roughness sublayer. Despite significant differences between simulations using idealized sinusoidal topography and real topography of the Amazon forest, results indicate that the effects of topography are located predominantly in the upper canopy and above, and are mostly caused by mean advection of TKE. The “horizontally” averaged TKE budget from idealized and real gentle topographies are almost identical to that for flat terrain, including a clear inertial layer above the roughness sublayer in which shear production is balanced by local dissipation. At topography crests, where observational towers are usually located, mean vertical advection of TKE can be as important as horizontal advection. Here, we propose the use on an approximate TKE balance equation to estimate mean advection from single tower measurements, and introduce a new advection index that can be used as a proxy to quantify the importance of the topography on the TKE budget.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Exfoliation of surfactant swollen layered MWW zeolites into two-dimensional zeolite nanosheets using telechelic liquid polybutadiene

We report two-dimensional (2D) zeolites have the potential to enhance mass transport by reducing diffusion lengths and thus find applications in catalysis and separation. High aspect ratio 2D zeolite nanosheets are required for fabrication of thin, high-flux zeolite membranes. Preparation of 2D zeolite nanosheets can be achieved by exfoliation of layered zeolite precursors, which usually requires multiple steps including swelling with cationic surfactants, exfoliation by applying a mechanical force such as shearing or sonication, purification and removal of the surfactants. The exfoliation of surfactant swollen layered zeolite precursors has been studied using molten polystyrene and telechelic liquid polybutadiene, but still requires extensive shearing force. Recently, a novel one-step exfoliation method has been developed for nonswollen MWW zeolite precursors using tetrabutylammonium hydroxide (TBAOH) solution. In this work, we study the exfoliation of surfactant swollen MWW layered precursors (with and without aluminum) in commercially available liquid hydroxyl-terminated polybutadiene (HTPB) with the aim to provide fundamental understanding of the interaction between the liquid polybutadiene and the surfactant swollen layered zeolite precursors. It was found that surfactant swollen ITQ-1, (ITQ-1(S)), a pure silica layered precursor with MWW framework after being swollen with a cationic surfactant, can be exfoliated in liquid HTPB at room temperature without applying any additional shearing force. The aluminum containing surfactant swollen MWW precursors can be also exfoliated in HTPB at room temperature, but require additional shearing forces. The exfoliation process was monitored using rheology experiments and studied by tuning the composition of the zeolite precursors. The interaction between the layered zeolite precursor and the hydroxyl group of the liquid polybutadiene allows the polymer to intercalate the precursor and exfoliate it into nanosheets. The presence of framework aluminum and the nature of the organic structure directing agents (OSDAs) are key parameters affecting the exfoliation process. Framework Al is unfavorable for the exfoliation possibly due to the surface charges introduced by the aluminum. Bulky OSDA, trimethyladamantammonium (TMAda + ), in the interlayer spacing may facilitate the exfoliation.

2D nanosheets↗

DOE OSTI2023

Analysis of real-fluid thermodynamic effects on turbulent statistics in transcritical channel flows

Wall-bounded turbulence at high-pressure transcritical conditions with intense density fluctuations are encountered in many technical applications. In this study, we analyze the turbulent energy transport in transcritical channel flows specifically focusing on dissipation rate, turbulent kinetic energy budgets, heat fluxes, and momentum-fluctuation statistics; results from this analysis are used to guide the development of turbulent scaling laws. Furthermore, we find that the dissipation rate of turbulent kinetic energy is dominated by the enstrophy in the logarithmic layer, and the fluctuating viscosity results in the reduced tilting of the vortical structures and the attenuation of streamwise vorticity in the near-wall layer; the fluctuating viscosity attenuates the dissipation rate by reducing the shear strain and the enstrophy production. Local equilibrium of the turbulent kinetic energy exists in the logarithmic layer. We show that the real-fluid thermodynamic effects significantly change the turbulent heat flux correlated with the sweep and the ejection events; the density changes alter the turbulent transport and result in noticeable magnitudes of density-fluctuation-related momentum-fluctuation statistics. From these results, scaling laws for the turbulent length scales and turbulent kinetic energy budgets are proposed, thereby contributing to improvement of the wall models in large-eddy simulations and Reynolds-averaged Navier-Stokes (RANS) simulations.

42 ENGINEERING↗

DOE OSTI2022

Dynamical criticality of spin-shear coupling in van der Waals antiferromagnets

Abstract The interplay between a multitude of electronic, spin, and lattice degrees of freedom underlies the complex phase diagrams of quantum materials. Layer stacking in van der Waals (vdW) heterostructures is responsible for exotic electronic and magnetic properties, which inspires stacking control of two-dimensional magnetism. Beyond the interplay between stacking order and interlayer magnetism, we discover a spin-shear coupling mechanism in which a subtle shear of the atomic layers can have a profound effect on the intralayer magnetic order in a family of vdW antiferromagnets. Using time-resolved X-ray diffraction and optical linear dichroism measurements, interlayer shear is identified as the primary structural degree of freedom that couples with magnetic order. The recovery times of both shear and magnetic order upon optical excitation diverge at the magnetic ordering temperature with the same critical exponent. The time-dependent Ginzburg-Landau theory shows that this concurrent critical slowing down arises from a linear coupling of the interlayer shear to the magnetic order, which is dictated by the broken mirror symmetry intrinsic to the monoclinic stacking. Our results highlight the importance of interlayer shear in ultrafast control of magnetic order via spin-mechanical coupling.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Additively manufactured polymer composites for heat exchanger applications: evaluation of critical thermophysical properties

Polymeric heat exchangers (PHXs) have been used in applications involving weight restrictions, chemical compatibility, and fouling issues. Additive manufacturing (AM) or 3D printing provide new solutions to previously inaccessible combinations of properties and geometries. There are some advancements in the PHXs by AM; however, the process and the properties of materials still need further investigation to improve the overall performance. In this study, additively manufactured polyethylene terephthalate glycol (PETG) composites reinforced with graphite and pitch-based carbon fibers were evaluated for their potential application as PHXs. The thermal conductivity, volumetric heat capacity, coefficient of thermal expansion, creep behavior, and long-term performance were studied in detail. Our results reveal that the composites have an anisotropic thermal conductivity. The thermal conductivity along the printing direction is higher than the layer building direction due to the shear-induced alignment of the fillers. The printed composites achieve good thermal stability with 80% lower CTE at room temperature than neat PETG. Creep tests suggest the creep and creep recovery were highly temperature-dependent, and the deformation can be recovered when the temperature is below glass transition. These results suggest additive manufactured composites be potentially used for heat exchanger applications at low temperatures.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Two phase transitions driven by surface electron doping in WTe 2

WTe 2 is a multifunctional quantum material exhibiting numerous emergent phases in which tuning of the carrier density plays an important role. In this work, we demonstrate two nonmonotonic changes in the electronic structure of WTe 2 upon in situ electron doping. The first phase transition is interpreted in terms of a shear displacement of the top WTe 2 layer, which realizes a local crystal structure not normally found in bulk WTe 2 . The second phase transition is associated with stronger interactions between the dopant atoms and the host, both through hybridization and electric field. These results demonstrate that electron doping can drive structural and electronics changes in bulk WTe 2 with implications for realizing nontrivial band-structure changes in heterointerfaces and devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2025

Elasticity of davemaoite as a primary contributor to lower-mantle heterogeneities

Geophysical detection of subducted mid–ocean ridge basalt (MORB) in the lower mantle is hindered by uncertainties in the elasticity of Fe,Al,Mg,Ti–bearing davemaoite, a key MORB component. Using Brillouin spectroscopy and x-ray diffraction, we determined the elasticity of a Ca 0.906(1) Fe 2+ 0.027(1) Fe 3+ 0.042(1) Mg 0.033(1) Al 0.072(1) Ti 0.020(1) Si 0.912(1) O 3 davemaoite up to 113 gigapascals and 2294 K. Here, we found that it exhibited a shear wave velocity 10 to 20% slower than end-member davemaoite, making it the slowest phase among major lower-mantle minerals. Our models show that MORB, containing 20 to 25 volume percent davemaoite, potentially contributes to large low-shear-velocity provinces (LLSVPs), whereas a cumulate layer enriched in davemaoite crystallized from basal magma ocean may comprise ultralow-velocity zones (ULVZs). Davemaoite’s ability to host incompatible and heat-producing elements possibly links LLSVPs and ULVZs to mantle plume initiation and geochemical signatures of ocean island basalts.

Zhou, Wen-Yi [Texas A & M Univ., College Station, ↗