Mixed Close-Packed Cobalt Molybdenum Nitrides as Non-noble Metal Electrocatalysts for the Hydrogen Evolution Reaction
Abstract not provided
Cao, Bingfei↗
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Results for “MIXING”
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On the alternatives for bath correlators and spectral densities from mixed quantum-classical simulations
We investigate on the procedure of extracting a 'spectral density' from mixed QM/MM calculations and employing it in open quantum systems models. In particular, we study the connection between the energy gap correlation function extracted from ground state QM/MM and the bath spectral density used as input in open quantum system approaches. We introduce a simple model which can give intuition on when the ground state QM/MM propagation will give the correct energy gap. We also discuss the role of higher order correlators of the energy-gap fluctuations which can provide useful information on the bath. Further, various semiclassical corrections to the spectral density, are applied and investigated. Finally, we apply our considerations to the photosynthetic Fenna-Matthews-Olson complex. For this system, our results suggest the use of the Harmonic prefactor for the spectral density rather than the Standard one, which was employed in the simulations of the system carried out to date.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Numerical Simulation and Experimental Comparison of System Analysis Module 1D Mixing Model for Cold Shock Transients in the Gallium Thermal-Hydraulic Mixing Facility
Abstract Liquid metals are being investigated as coolants in many advanced reactor designs because of their high thermal conductivity and effectiveness at high temperatures. However, they often pose challenges to reactor operation and safety because of the complex thermal mixing and stratification in the plenum of pool-type reactor designs. The advanced system analysis code System Analysis Module (SAM) currently under development at Argonne National Laboratory aims to develop and implement thermal mixing models to accurately capture these complex thermal fluid behaviors. In this study, the SAM thermal mixing model was compared against experimental data from the Gallium Thermal-Hydraulic Experiment facility, a scaled liquid metal test facility that uses gallium as a surrogate fluid to investigate the stratification and thermal mixing of low-Prandtl-number fluids in the upper plenum of a liquid metal-cooled reactor. Two cold shock transient cases were used: one with stable stratified flow (Ri = 32) and one with stronger thermal mixing (Ri = 0.5). The resultant temperatures were then compared with the experimental temperatures over the entire plenum to assess the ability of the mixing models to capture the thermal behavior and to better correspond mixing parameters to various flow scenarios. Generally, the zero-dimensional mixing model was more capable of capturing the bulk temperature of the component modeled assuming that an accurate mass flow rate was provided, but it was inherently unable to capture thermal gradients in space. The one-dimensional mixing model was capable of capturing that the thermal gradients provided accurate selection of the mixing coefficients. Further, the temperature at the outlet junction was compared over time for each of the mixing models with the recorded experimental temperature. The implemented mixing models demonstrated the ability to effectively capture the overall thermal behavior for stronger mixing scenarios but struggled with more stably stratified flows. It was found that a system analysis code's covering of the entire range of different operating conditions still remains a challenging task, and it is suggested that further model and closure improvements are necessary to accurately capture complex thermal mixing and stratification phenomena.
stratification↗
Evaluating Entrainment–Mixing Characteristics through Direct Comparisons of Drop Size Distributions Using In Situ Observations from ACE-ENA
Abstract Constraining the impacts of entrainment and associated mixing (i.e., entrainment–mixing) on cloud properties continues to be difficult, partly due to observational uncertainties as well as a lacking consensus of which methodologies for diagnosing entrainment–mixing are most appropriate. This study introduces a novel method to evaluate the presence and degree of inhomogeneous and homogeneous mixing using ∼100 h of in situ observations from a research aircraft over the northeastern Atlantic. Specifically, drop size distributions are compared between regions containing negligible and significant entrainment for select flight legs, making a direct characterization of the degree of homogeneous and inhomogeneous mixing possible. A measure of drop concentration variance is used as a proxy variable to diagnose entrainment–mixing. Results correspond well with entrainment–mixing metrics, showing lower Damköhler numbers where drop size distributions shift toward smaller drop sizes (i.e., inhomogeneous mixing) and greater transition length scales where drop size distributions do not (i.e., homogeneous mixing). Inhomogeneous mixing occurs in most samples from Aerosol and Cloud Experiment in the Eastern North Atlantic (ACE-ENA) (regardless of homogeneous mixing frequencies increasing with increasing spatial resolution from ∼100 to ∼10 m) and is associated with decreased drop size relative dispersion and both greater aerosol and drop concentrations compared with homogeneous mixing. Precipitating clouds have a greater frequency of homogeneous mixing compared with nonprecipitating clouds. The proposed methodology is similarly applied to in situ observations of southeast Pacific stratocumulus, shallow convective clouds over central Oklahoma and low-level clouds over the Southern Ocean. All four locations are primarily dominated by inhomogeneous mixing with minimal variability among each region.
Clouds↗
Analytical and Experimental Demonstration of an Alternate Mixing Performance Metric for High-Speed Fuel Mixing Studies
To experimentally assess the fuel/air mixing performance of high-speed fuel injectors, one-dimensional metrics that quantify the degree of mixing completeness downstream of the fuel injection location are required. The most accurate assessment of mixing performance is achieved with the mixing efficiency parameter. In order to experimentally determine the mixing efficiency parameter, the spatial distributions of both mass flux and fuel mass fraction must be measured. In-stream gas sampling techniques are commonly used to measure the fuel mass fraction distribution; however, the mass flux distribution is not easily determined because it requires the measurement of three independent aerothermodynamic variables in addition to the gas composition. Therefore, to experimentally determine the mixing efficiency parameter, the spatial distributions of four independent properties must be measured, with each property generally requiring its own unique probe. Because of this difficulty, it is commonly assumed that alternate metrics, which rely solely on the fuel distribution, are good indicators of mixing performance. However, since these alternate metrics do not provide a mass flux-weighted measure of mixing completeness, they can lead to incorrect conclusions being drawn about the mixing performance of the studied fuel injector configuration. Recognizing this shortcoming, this work proposes two new alternate mixing performance metrics that are easier to obtain than the mixing efficiency parameter. The analytical development of the new metrics, as well as their application to relevant CFD and experimental data of high-speed fuel injector configurations, is presented in this work. For two different experiments, the new metrics are shown to provide an excellent representation of the true mass flux-weighted mixing performance, unlike the traditionally-used alternatives. The results presented herein suggest that the new metrics can serve as accurate surrogates for mixing efficiency in future high-speed fuel/air mixing studies.
Cody R Ground↗
Contrasting Scale Dependence of Entrainment-Mixing Mechanisms in Stratocumulus Clouds
The apparent turbulent entrainment-mixing mechanism between clouds and surrounding air is scale-dependent; however, such scale dependence has been rarely studied, hindering development of scale-aware entrainment-mixing parameterizations. Here we extend our previous study on cumulus clouds to investigate scale dependence of entrainment-mixing processes in stratocumulus clouds during ACE-ENA and RACORO. In contrast to previous studies, two opposite scale dependencies are found: entrainment-mixing can become more homogeneous or more inhomogeneous with increasing averaging scales, which is quantified by the difference between homogeneous mixing degree at the 100 m and 10 m resolutions. A new heuristic model and two new quantities are introduced. The observations and model show that microphysical properties near and far away from droplet-free air and relative humidity of entrained air determine both the sign and strength of scale dependence, while droplet-free air fraction only affects the strength. The results shed new light on developing scale-aware parameterizations of entrainment-mixing mechanisms.
Gao, Sinan↗
Mixing of the Connecticut River Plume During Ambient Flood Tides: Spatial Heterogeneity and Contributions of Bottom–Generated and Interfacial Mixing
The Connecticut River plume is influenced by energetic ambient tides in the Long Island Sound receiving waters. The objectives of this modeling study are (a) characterizing the spatial heterogeneity of turbulent buoyancy fluxes, (b) partitioning turbulent buoyancy fluxes into bottom-generated and interfacial shear contributions, and (c) quantifying contributions to plume-integrated mixing within the tidal plume. The plume formed during ambient flood tides under low river discharge, spring tides, and no winds is analyzed. Turbulent buoyancy fluxes (B) and depth-integrated B through the plume (Bd) are characterized by pronounced spatial heterogeneity. Strong mixing (Bd ~ 10 –5 -10 –4 m 3 /s 3 ) occurs near the mouth, in the nearfield plume turning region, over shoals, and nearshore shallow areas. Low to moderate mixing (Bd ~ 10 –8 -10 –6 m 3 /s 3 ) occupies half the plume. Buoyancy fluxes are first partitioned based on the depth of the shear stress minimum between plume-generated and bottom-generated shear maxima. Four other tested partitioning methods are based on open channel flow and stratified shear flow parameterizations. Interfacial and bottom-generated shear contribute to different areas of intense and moderate mixing. All methods indicate a significant plume mixing role for bottom-generated mixing, but interfacial mixing is a bigger contributor. Plume-integrated total and interfacial mixing peak at max ambient flood and the timing of peak bottom-generated mixing varies among partitioning methods. Two-thirds of the mixing occurs in concentrated intense mixing areas. A parameter space with the ambient tidal Froude number and plume thickness to depth ratio as axes indicates many tidally modulated plumes are moderately to dominantly influenced by bottom-generated tidal mixing.
54 ENVIRONMENTAL SCIENCES↗
Analysis of turbulent transport and mixing in transitional Rayleigh–Taylor unstable flow using direct numerical simulation data
Data from a 1152X760X1280 direct numerical simulation (DNS) of a transitional Rayleigh-Taylor mixing layer modeled after a small Atwood number water channel experiment is used to comprehensively investigate the structure of mean and turbulent transport and mixing. The simulation had physical parameters and initial conditions approximating those in the experiment. The budgets of the mean vertical momentum, heavy-fluid mass fraction, turbulent kinetic energy, turbulent kinetic energy dissipation rate, heavy-fluid mass fraction variance, and heavy-fluid mass fraction variance dissipation rate equations are constructed using Reynolds averaging applied to the DNS data. The relative importance of mean and turbulent production, turbulent dissipation and destruction, and turbulent transport are investigated as a function of Reynolds number and across the mixing layer to provide insight into the flow dynamics not presently available from experiments. The analysis of the budgets supports the assumption for small Atwood number, Rayleigh/Taylor driven flows that the principal transport mechanisms are buoyancy production, turbulent production, turbulent dissipation, and turbulent diffusion (shear and mean field production are negligible). As the Reynolds number increases, the turbulent production in the turbulent kinetic energy dissipation rate equation becomes the dominant production term, while the buoyancy production plateaus. Distinctions between momentum and scalar transport are also noted, where the turbulent kinetic energy and its dissipation rate both grow in time and are peaked near the center plane of the mixing layer, while the heavy-fluid mass fraction variance and its dissipation rate initially grow and then begin to decrease as mixing progresses and reduces density fluctuations. All terms in the transport equations generally grow or decay, with no qualitative change in their profile, except for the pressure flux contribution to the total turbulent kinetic energy flux, which changes sign early in time (a countergradient effect). The production-to-dissipation ratios corresponding to the turbulent kinetic energy and heavy-fluid mass fraction variance are large and vary strongly at small evolution times, decrease with time, and nearly asymptote as the flow enters a self-similar regime. The late-time turbulent kinetic energy production-to-dissipation ratio is larger than observed in shear-driven turbulent flows. The order of magnitude estimates of the terms in the transport equations are shown to be consistent with the DNS at late-time, and also confirms both the dominant terms and their evolutionary behavior. Thus, these results are useful for identifying the dynamically important terms requiring closure, and assessing the accuracy of the predictions of Reynolds-averaged Navier-Stokes and large-eddy simulation models of turbulent transport and mixing in transitional Rayleigh-Taylor instability-generated flow.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
Vertical variation of turbulent entrainment mixing processes in marine stratocumulus clouds using high-resolution digital holography
Marine stratocumulus clouds contribute signi?cantly to the Earth’s radiation budget due to their extensive coverage and high albedo. Yet, subgrid variability in cloud properties such as aerosol concentration, droplet number and precipitation rates lead to considerable errors in global climate models. While these clouds usually have small vertical ex-tent, turbulent entrainment-mixing and precipitation can generate signi?cant variations in droplet number, size and relative dispersion with altitude. In this paper, we analyze turbulent entrainment-mixing processes and the variability in cloud microphysical properties as a function of height within a warm marine stratocumulus cloud layer over the Eastern North Atlantic. We use high resolution airborne holographic measurements and compare them with local turbulence measurements. We ?nd that entrainment-mixing is primarily inhomogeneous near cloud top leading to larger droplet sizes and homogeneous near cloud base leading to smaller droplet sizes. Further analysis of Damk¨ohler number measurements are able to explain the mixing mechanisms at di?erent cloud heights, reinforcing the importance of turbulent mixing and microphysical time scales in deter-mining cloud microphysics.
Desai, Neel↗
Development of the CD Symcap platform to study gas-shell mix in implosions at the National Ignition Facility
Surrogate implosions play an important role at the National Ignition Facility (NIF) for isolating aspects of the complex physical processes associated with fully integrated ignition experiments. The newly developed CD Symcap platform has been designed to study gas-shell mix in indirectly driven, pure T{sub 2}-gas filled CH-shell implosions equipped with 4 μm thick CD layers. This configuration provides a direct nuclear signature of mix as the DT yield (above a characterized D contamination background) is produced by D from the CD layer in the shell, mixing into the T-gas core. The CD layer can be placed at different locations within the CH shell to probe the depth and extent of mix. CD layers placed flush with the gas-shell interface and recessed up to 8 μm have shown that most of the mix occurs at the inner-shell surface. In addition, time-gated x-ray images of the hotspot show large brightly radiating objects traversing through the hotspot around bang-time, which are likely chunks of CH/CD plastic. This platform is a powerful new capability at the NIF for understanding mix, one of the key performance issues for ignition experiments.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
Separated reactant mix width across diffusion-dominated and hydrodynamically dominated interface mix in inertial confinement fusion implosions
Diffusion-dominated mix in inertial confinement fusion (ICF) is characterized where the majority of the mix occurs in the immediate fuel-shell interface while hydrodynamic-dominated mix pulls shell material from farther away into the central fuel. A thin (150 nm) separated reactants ICF mix platform is highly sensitive to the amount of mix from the first micron of shell-fuel interface. This fine-spatial resolution platform has revealed that material mix in moderate convergence ( CR ∼ 12 ) ICF implosions is dominated by a diffusion mechanism. This technique has now been expanded across a set of OMEGA ICF implosions, observing an increase in mix width and mix amount for cooler, slower, and more compressive implosions. Hydrodynamic simulations require a buoyancy-drag mix model to capture the increasing mix width, suggesting a transition between these two mix mechanisms. Published by the American Physical Society 2024
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
Theoretical analysis of mixing in liquid clouds – Part 3: Inhomogeneous mixing
An idealized diffusion–evaporation model of time-dependent mixing between a cloud volume and a droplet-free volume is analyzed. The initial droplet size distribution (DSD) in the cloud volume is assumed to be monodisperse. It is shown that evolution of the microphysical variables and the final equilibrium state are unambiguously determined by two non-dimensional parameters. The first one is the potential evaporation parameter R, proportional to the ratio of the saturation deficit to the liquid water content in the cloud volume, that determines whether the equilibrium state is reached at 100 % relative humidity, or is characterized by a complete evaporation of cloud droplets. The second parameter Da is the Damkölher number equal to the ratio of the characteristic mixing time to the phase relaxation time. Parameters R and Da determine the type of mixing. The results are analyzed within a wide range of values of R and Da. It is shown that there is no pure homogeneous mixing, since the first mixing stage is always inhomogeneous. The mixing type can change during the mixing process. Any mixing type leads to formation of a tail of small droplets in DSD and, therefore, to DSD broadening that depends on Da. At large Da, the final DSD dispersion can be as large as 0.2. The total duration of mixing varies from several to 100 phase relaxation time periods, depending on R and Da. The definitions of homogeneous and inhomogeneous types of mixing are reconsidered and clarified, enabling a more precise delimitation between them. The paper also compares the results obtained with those based on the classic mixing concepts.
54 ENVIRONMENTAL SCIENCES↗
Hydrodynamic instabilities and mix studies on NIF: predictions, observations, and a path forward
The goals of the Mix Campaign are to determine how mix affects performance, locate the "mix cliff", locate the source of the mix, and develop mitigation methods that allow performance to be increased. We have used several different drive pulse shapes and capsule designs in the Mix Campaign, to understand sensitivity to drive peak power, level of coast, rise time to peak power, adiabat, and dopant level in the capsule. Ablator material mixing into the hot spot has been shown conclusively with x-ray spectroscopy. The observed neutron yield drops steeply when the hot spot mix mass becomes too large. The mix appears to be driven by ablation- front Rayleigh-Taylor instabilities. A high foot, higher adiabat drive has a more stable ablation front and has allowed the mix mass in the hot spot to be reduced significantly. We found two recent high foot shots achieved neutron yields > 10 15 and measured neutron yield over clean 1D simulation (YOC) > 50%, which was one of the central goals of the Mix Campaign.
73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
Mixing model with multi-particle interactions for Lagrangian simulations of turbulent mixing
We report on the numerical study of the mixing volume model (MVM) for molecular diffusion in Lagrangian simulations of turbulent mixing problems. The MVM is based on the multi-particle interaction in a finite volume (mixing volume). A priori test of the MVM, based on the direct numerical simulations of planar jets, is conducted in the turbulent region and the interfacial layer between the turbulent and non-turbulent fluids. The results show that the MVM predicts well the mean effects of the molecular diffusion under various numerical and flow parameters. The number of the mixing particles should be large for predicting a value of the molecular diffusion term positively correlated to the exact value. The size of the mixing volume relative to the Kolmogorov scale η is important in the performance of the MVM. The scalar transfer across the turbulent/non-turbulent interface is well captured by the MVM especially with the small mixing volume. Furthermore, the MVM with multiple mixing particles is tested in the hybrid implicit large-eddy-simulation/Lagrangian-particle-simulation (LES–LPS) of the planar jet with the characteristic length of the mixing volume of O(100η). Despite the large mixing volume, the MVM works well and decays the scalar variance in a rate close to the reference LES. The statistics in the LPS are very robust to the number of the particles used in the simulations and the computational grid size of the LES. Both in the turbulent core region and the intermittent region, the LPS predicts a scalar field well correlated to the LES.
42 ENGINEERING↗
Theoretical analysis of mixing in liquid clouds – Part IV: DSD evolution and mixing diagrams
Evolution of droplet size distribution (DSD) due to mixing between cloudy and dry volumes is investigated for different values of the cloud fraction and for different initial DSD shapes. The analysis is performed using a diffusion–evaporation model which describes time-dependent processes of turbulent diffusion and droplet evaporation within a mixing volume. Time evolution of the DSD characteristics such as droplet concentration, LWC and mean volume radii is analyzed. The mixing diagrams are plotted for the final mixing stages. It is shown that the difference between the mixing diagrams for homogeneous and inhomogeneous mixing is insignificant and decreases with an increase in the DSD width. The dependencies of the normalized cube of the mean volume radius on the cloud fraction were compared with those on normalized droplet concentration and found to be quite different. If the normalized droplet concentration is used, mixing diagrams do not show any significant dependence on relative humidity in the dry volume. The main conclusion of the study is that traditional mixing diagrams cannot serve as a reliable tool for analysis of mixing type.
54 ENVIRONMENTAL SCIENCES↗
Probing the role of solids loading and mix procedure on the properties of acoustically mixed materials for additive manufacturing
We report resonant acoustic mixing has been of particular interest for use in additive manufacturing since viscous, solids-loaded materials can be difficult to mix and inhomogeneity has adverse effects on print quality. In this study, we detail a method to iterate through different formulations and mix procedures and assess mixture quality. The approach utilizes a constant pressure-driven flow test to collect statistics on flow rate through a standard geometry. This test is first applied to well mixed formulations containing particulate solids and find that the results are sensitive to viscosity produced by solids content. We then consider the formulations at various stages of mixing and find that the spread in the volume measurements is indicative of the mixing quality; poorly mixed material yields measurements with wide distributions. We believe this testing approach can be useful when screening new formulations, developing mixing processes, or for quality control.
36 MATERIALS SCIENCE↗
Conversion of Syngas-Derived C2+ Mixed Oxygenates to C3-C5 Olefins over ZnxZryOz Mixed Oxides Catalysts
In this study we report on a ZnxZryOz mixed oxide type catalyst capable of converting a syngas-derived C2+ mixed oxygenate feedstock to isobutene-rich olefins. Aqueous model feed comprising of ethanol, acetaldehyde, acetic acid, ethyl acetate, methanol, and propanol was used as representative liquid product derived from a Rh-based mixed oxygenate synthesis catalyst. Greater than 50% carbon yield to C3-C5 mixed olefins was demonstrated when operating at 400-450oC and 1 atm. In order to rationalize formation of the products observed feed components were individually evaluated. Major constituents of the feed mixture (ethanol, acetaldehyde, acetic acid, and ethyl acetate) were found to produce isobutene-rich olefins. C-C coupling was also demonstrated for propanol feedstock - a minor constituent of the mixed oxygenate feed - producing branched C6 olefins, revealing scalability to alcohols higher than ethanol following an analogous reaction pathway. Using ethanol and propanol feed mixtures, cross-coupling reactions produced mixtures of C4, C5, and C6 branched olefins. The presence of H2 in the feed was found to facilitate hydrogenation of the ketone intermediates, thus producing straight chain olefins as byproducts. While activity loss from coking is observed complete catalyst regeneration is achieved by employing mild oxidation. For conversion of the mixed oxygenate feed a Zr/Zn ratio of 2.5 and a reaction temperature of 450oC provides the best balance of stability, activity, and selectivity. X-ray diffraction and scanning transmission electron microscopy analysis reveals the presence of primarily cubic phase ZrO2 and a minor amount of the monoclinic phase, with ZnO being highly dispersed in the lattice. The presence of ZnO appears to stabilize the cubic phase resulting in less monoclinic phase as the ZnO concentration increases. Infrared spectroscopy shows the mixed oxide acid sites are characterized as primarily Lewis type acidity. The direct relationship between isobutene production and the ratio of basic/acidic sites was demonstrated. An optimized balance of active sites for isobutene production from acetone was obtained with a basic/acidic site ratio of ~2. This technology for the conversion of aqueous mixtures of C2+ mixed oxygenates provides significant advantages over other presently studied catalysts in that its unique properties permit the utilization of a variety of feeds in a consistently selective manner.
biomass, catalyst, mixed oxides, ethanol, acetic a↗