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At least 181 records · Page 10

Replication Data for: Growth and auto-oxidation of Pd on single-layer AgOx/Ag(111)

The data underlying this published work have been made publicly available in this repository as part of the IMASC Data Management Plan. This work was supported as part of the Integrated Mesoscale Architectures for Sustainable Catalysis (IMASC), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under Award # DE-SC0012573.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Replication Data for: Quantifying oxygen induced surface enrichment of a dilute PdAu alloy catalyst

The data underlying this published work have been made publicly available in this repository as part of the IMASC Data Management Plan. This work was supported as part of the Integrated Mesoscale Architectures for Sustainable Catalysis (IMASC), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under Award # DE-SC0012573.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Replication Data for: Formation of a Ti-Cu(111) single atom alloy: Structure and CO binding

The data underlying this published work have been made publicly available in this repository as part of the IMASC Data Management Plan. This work was supported as part of the Integrated Mesoscale Architectures for Sustainable Catalysis (IMASC), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under Award # DE-SC0012573.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Replication Data for: Evolution of Metastable Structures at Bimetallic Surfaces from Microscopy and Machine-Learning Molecular Dynamics

The data underlying this published work have been made publicly available in this repository as part of the IMASC Data Management Plan. This work was supported as part of the Integrated Mesoscale Architectures for Sustainable Catalysis (IMASC), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under Award # DE-SC0012573.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Replication Data for: Oxophilicity Drives Oxygen Transfer at a Palladium−Silver Interface for Increased CO Oxidation Activity

The data underlying this published work have been made publicly available in this repository as part of the IMASC Data Management Plan. This work was supported as part of the Integrated Mesoscale Architectures for Sustainable Catalysis (IMASC), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under Award # DE-SC0012573.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Replication Data for: The dynamic behavior of dilute metallic alloy PdxAu1-x/SiO2 raspberry colloid templated catalysts under CO oxidation

The data underlying this published work have been made publicly available in this repository as part of the IMASC Data Management Plan. This work was supported as part of the Integrated Mesoscale Architectures for Sustainable Catalysis (IMASC), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under Award # DE-SC0012573.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Replication Data for: Predicting X-ray Photoelectron Peak Shapes: the Effect of Electronic Structure

The data underlying this published work have been made publicly available in this repository as part of the IMASC Data Management Plan. This work was supported as part of the Integrated Mesoscale Architectures for Sustainable Catalysis (IMASC), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under Award # DE-SC0012573.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Replication Data for: The effect of frustrated rotations on the pre-exponential factor for unimolecular reactions on surfaces: a case study of alkoxy dehydrogenation

The data underlying this published work have been made publicly available in this repository as part of the IMASC Data Management Plan. This work was supported as part of the Integrated Mesoscale Architectures for Sustainable Catalysis (IMASC), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under Award # DE-SC0012573.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Control of Two Solid Electrolyte Interphases at the Negative Electrode of an Anode‐Free All Solid‐State Battery based on Argyrodite Electrolyte

Abstract Anode‐free all solid‐state batteries (AF‐ASSBs) employ “empty” current collector with three active interfaces that determine electrochemical stability; lithium metal – Solid electrolyte (SE) interphase (SEI‐1), lithium – current collector interface, and collector – SE interphase (SEI‐2). Argyrodite Li 6 PS 5 Cl (LPSCl) solid electrolyte (SE) displays SEI‐2 containing copper sulfides, formed even at open circuit. Bilayer of 140 nm magnesium/30 nm tungsten (Mg/W‐Cu) controls the three interfaces and allows for state‐of‐the‐art electrochemical performance in half‐cells and fullcells. AF‐ASSB with NMC811 cathode achieves 150 cycles with Coulombic efficiency (CE) above 99.8%. With high mass‐loading cathode (8.6 mAh cm −2 ), AF‐ASSB retains 86.5% capacity after 45 cycles at 0.2C. During electrodeposition of Li, gradient Li‐Mg solid solution is formed, which reverses upon electrodissolution. This promotes conformal wetting/dewetting by Li and stabilizes SEI‐1 by lowering thermodynamic driving force for SE reduction. Inert refractory W underlayer is required to prevent ongoing formation of SEI‐2 that also drives electrochemical degradation. Inert Mo and Nb layers likewise protect Cu from corroding, while Li‐alloying layers (Mg, Sn) are less effective due to ongoing volume changes and associated pulverization. Mechanistic explanation for observed Li segregation within alloying Li x Mg layer is provided through mesoscale modelling, considering opposing roles of diffusivity differences and interfacial stresses.

Wang, Yixian [Materials Science and Engineering Pr↗

A Machine Learning Assisted Development of a Model for the Populations of Convective and Stratiform Clouds

Abstract Traditional parameterizations of the interaction between convection and the environment have relied on an assumption that the slowly varying large‐scale environment is in statistical equilibrium with a large number of small and short‐lived convective clouds. They fail to capture nonequilibrium transitions such as the diurnal cycle and the formation of mesoscale convective systems as well as observed precipitation statistics and extremes. Informed by analysis of radar observations, cloud‐permitting model simulation, theory, and machine learning, this work presents a new stochastic cloud population dynamics model for characterizing the interactions between convective and stratiform clouds, with the goal of informing the representation of these interactions in global climate models. Fifteen wet seasons of precipitating cloud observations by a C‐band radar at Darwin, Australia are fed into a machine learning algorithm to obtain transition functions that close a set of coupled equations relating large‐scale forcing, mass flux, the convective cell size distribution, and the stratiform area. Under realistic large‐scale forcing, the derived transition functions show that, on the one hand, interactions with stratiform clouds act to dampen the variability in the size and number of convective cells and therefore in the convective mass flux. On the other, for a given convective area fraction, a larger number of smaller cells is more favorable for the growth of stratiform area than a smaller number of larger cells. The combination of these two factors gives rise to solutions with a few convective cells embedded in a large stratiform area, reminiscent of mesoscale convective systems.

54 ENVIRONMENTAL SCIENCES↗

Effects of Horizontal Resolution, Domain Size, Boundary Conditions, and Surface Heterogeneity on Coarse LES of a Convective Boundary Layer

Atmospheric properties in a convective boundary layer vary over a wide range of spatial scales and are commonly studied using large-eddy simulations (LES) in various configurations. We examine how the boundary layer depth and distribution of variability across scales are affected by LES grid spacing, domain size, inhomogeneity of surface properties, and external forcing. Two different setups of the Weather Research and Forecasting (WRF) model are analyzed. A semi-idealized configuration uses a periodic domain, flat surface, prescribed homogeneous surface heat fluxes, and horizontally uniform profiles of large-scale advective tendencies. A nested LES setup employs a larger domain and realistic initial and boundary conditions, including an interactive land surface model with representative topography and vegetation and soil types. Subdomains of identical size are analyzed for all simulations. Characteristic structure sizes are quantified using the variability scales L 50 and L 95 , defined such that features smaller than that contain 50% and 95% of the total variance, respectively. Progressive increase in L 50 from vertical velocity to temperature and moisture structures is systematically reproduced in all simulation configurations. This dependence of L 50 on the considered variable complicates the development of scale-aware parameterizations for models with grid spacing in the “terra incognita”. In simulations using a larger domain with heterogeneous surface properties, the development of internal mesoscale patterns significantly affects variance distributions inside analyzed subdomains. Sizes of boundary layer structures also strongly depend on the LES grid spacing and, in case of heterogeneous surface and topography, on location of the subdomain inside a larger computational domain.

54 ENVIRONMENTAL SCIENCES↗

Evidence of a liquid–liquid transition in a glass-forming ionic liquid

A liquid–liquid transition (LLT) is a transformation from one liquid to another through a first-order transition. The LLT is fundamental to the understanding of the liquid state and has been reported in a few materials such as silicon, phosphorus, triphenyl phosphite, and water. Furthermore, it has been suggested that the unique properties of materials such as water, which is critical for life on the planet, are linked to the existence of the LLT. However, the experimental evidence for the existence of an LLT in many molecular liquids remains controversial, due to the prevalence and high propensity of the materials to crystallize. In this work, we show evidence of an LLT in a glass-forming trihexyltetradecylphosphonium borohydride ionic liquid that shows no tendency to crystallize under normal laboratory conditions. We observe a step-like increase in the static dielectric permittivity at the transition. Furthermore, the sizes of nonpolar local domains and ion-coordination numbers deduced from wide-angle X-ray scattering also change abruptly at the LLT. We independently corroborate these changes in local organization using Raman spectroscopy. The experimental access to the evolution of local order and structural dynamics across a liquid–liquid transition opens up unprecedented possibilities to understand the nature of the liquid state.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Near-Cloud Atmospheric Ingredients for Deep Convection Initiation

A lack of routine environmental observations located near deepening cumulus congestus clouds limits verification of important theorized and simulated updraft–environment interaction processes occurring during deep convection initiation (CI). We analyze radiosonde profiles collected during several hundred CI events near a mountain range in central Argentina during the CACTI field campaign. Statistical analyses illustrate environmental conditions supporting radar-observed CI outcomes that span a spectrum of convective cell depths, widths, and durations, as well as events lacking precipitating convection. Tested environmental factors include a large variety of sounding-derived measurements of CAPE, CIN, moisture, terrain-relative winds, vertical shear, and lifted parcel properties, with supplemental model reanalysis of background larger-scale vertical motion. CAPE and CIN metrics do not consistently differentiate CI success from failure. Only a few environmental factors contain consistent monotonic relationships among the spectrum of cloud depths achieved during CI: (i) the depth and strength of background ascent, and (ii) the component of low-level flow oriented parallel to the ridgeline. These metrics suggest that the ability of the surrounding flow to lift parcels to their LFC and terrain-modified flow are consistently relevant processes for CI. Low- to midlevel relative humidity strongly discriminated between CI and non-CI events, likely reflecting entrainment-driven dilution processes. However, we could not confidently conclude that relative humidity similarly discriminated robust from marginal CI events. Circumstantial evidence was found linking cell width, an important cloud property governing the probability of CI, to LCL height, boundary layer depth, depth and magnitude of the CIN layer, and ambient wind shear.

Storm environments↗

Calibration of a mesoscale tritium transport model for ceramic breeder materials in TMAP8 using experimental data

Due to the scarcity of the long-term external tritium supply, lithium-containing breeder materials are used in the blanket of fusion reactors to produce tritium faster than the deuterium-tritium fusion reaction consumes it. A cellular breeder is a promising material with higher lithium density and thermal conductivity than conventional ceramic pebbles and enhanced tritium extraction with interconnected pores. Although several experimental and modeling efforts have improved our understanding of tritium transport, the exact mechanisms governing tritium release from breeder materials are still unknown. As a result, current models cannot reliably assess the tritium breeding capabilities of cellular breeder materials. This work presents a tritium transport multiphysics model and calibrates it using experimental data of deuterium absorption and desorption from cellular breeder materials at different temperatures and pressures. This model accounts for ceramic and pore diffusion, trapping and detrapping, and several surface reactions at the pore surface. After calibrating the model and performing sensitivity analysis, we discuss pre-dominant mechanisms governing tritium release from cellular breeder materials. The model is part of the Tritium Migration Analysis Program [TMAP8], a multiscale, multiphysics framework for tritium transport based on the finite element multiphysics framework MOOSE. This study demonstrates some of TMAP8’s capabilities and provides insight into the mechanisms governing tritium transport in cellular ceramic breeder materials.

08 HYDROGEN↗

Characterizing Land-Atmosphere Interactions During the Afternoon-to-Evening Transition Using ARM SGP Observations

The land-atmosphere (LA) system consists of the soil, vegetation, and lowest layer of the atmosphere. The energy and water transport processes in this system contribute to the structure and the daily cycle of the atmospheric boundary layer (ABL), which is the layer between the land surface and the free troposphere that controls the exchange of momentum, energy, and water. The state of the ABL is the result of complex two-way interactions between local processes such as surface fluxes and entrainment at the ABL top as well as large-scale and mesoscale processes such as advection and subsidence.

54 ENVIRONMENTAL SCIENCES↗

Forest Breeze–Cold Pool Interactions Drive Convective Organization over Heterogeneous Vegetation

Heterogeneous landscapes can influence the development of convection through the generation of thermally driven mesoscale circulations. To assess the impacts of these circulations and their interaction with sea breezes, we simulated convection in an idealized coastal environment using the Regional Atmospheric Modeling System (RAMS). We compared simulations with striped patterns of surface vegetation to those of uniform vegetation to identify the importance of vegetation heterogeneity in impacting convective development. Under dry soil conditions representative of those during the Tracking Aerosol Convection Interactions Experiment (TRACER) and Experiment of Sea Breeze Convection, Aerosols, Precipitation, and Environment (ESCAPE) campaigns in June 2022, we found that these vegetation-induced circulations, referred to in the literature as “forest breezes,” are more important than the sea breeze in determining the location of convection initiation. Convection and precipitation are also found to be favored over forests and suppressed over pasture and suburban landscapes as a result of greater surface sensible heat flux over the forest. Our findings also indicate that forest breezes are important for initiating convection along the boundaries of the forest, but that cold pools may play a key role in propagating the forest breezes toward the center of the forest stripe. In our simulations, the collisions of these breezes in the center of the forest stripe lead to uplift and strong convection there; however, a different width of the forest stripe would alter when the forest breezes collide or whether they collide at all. The presence of these cold pools may therefore impact the “ideal stripe width,” the width of each vegetation stripe which maximizes domain-wide precipitation.

54 ENVIRONMENTAL SCIENCES↗

Improved Representation of Horizontal Variability and Turbulence in Mesoscale Simulations of an Extended Cold-Air Pool Event

Abstract Cold-air pools (CAPs), or stable atmospheric boundary layers that form within topographic basins, are associated with poor air quality, hazardous weather, and low wind energy output. Accurate prediction of CAP dynamics presents a challenge for mesoscale forecast models in part because CAPs occur in regions of complex terrain, where traditional turbulence parameterizations may not be appropriate. This study examines the effects of the planetary boundary layer (PBL) scheme and horizontal diffusion treatment on CAP prediction in the Weather Research and Forecasting (WRF) Model. Model runs with a one-dimensional (1D) PBL scheme and Smagorinsky-like horizontal diffusion are compared with runs that use a new three-dimensional (3D) PBL scheme to calculate turbulent fluxes. Simulations are completed in a nested configuration with 3-km/750-m horizontal grid spacing over a 10-day case study in the Columbia River basin, and results are compared with observations from the Second Wind Forecast Improvement Project. Using event-averaged error metrics, potential temperature and wind speed errors are shown to decrease both with increased horizontal grid resolution and with improved treatment of horizontal diffusion over steep terrain. The 3D PBL scheme further reduces errors relative to a standard 1D PBL approach. Error reduction is accentuated during CAP erosion, when turbulent mixing plays a more dominant role in the dynamics. Last, the 3D PBL scheme is shown to reduce near-surface overestimates of turbulence kinetic energy during the CAP event. The sensitivity of turbulence predictions to the master length-scale formulation in the 3D PBL parameterization is also explored. Significance Statement In this article, we demonstrate how a new framework for modeling atmospheric turbulence improves cold pool predictions, using a case study from January 2017 in the Columbia River basin (U.S. Pacific Northwest). Cold pools are regions of cold, stagnant air that form within valleys or basins, and improved forecasts could help to mitigate the risks they pose to air quality, transportation, and wind energy production. For the chosen case study, our tests show a reduction in temperature and wind speed errors by up to a factor of 2–3 relative to standard model options. These results strongly motivate continued development of the framework as well as its application to other complex weather events.

17 WIND ENERGY↗