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DOE OSTI2024

Catalytically Active Site Mapping Realized through Energy Transfer Modeling

Abstract The demands of a sustainable chemical industry are a driving force for the development of heterogeneous catalytic platforms exhibiting facile catalyst recovery, recycling, and resilience to diverse reaction conditions. Homogeneous‐to‐heterogeneous catalyst transitions can be realized through the integration of efficient homogeneous catalysts within porous matrices. Herein, we offer a versatile approach to understanding how guest distribution and evolution impact the catalytic performance of heterogeneous host–guest catalytic platforms by implementing the resonance energy transfer (RET) concept using fluorescent model systems mimicking the steric constraints of targeted catalysts. Using the RET‐based methodology, we mapped condition‐dependent guest (re)distribution within a porous support on the example of modular matrices such as metal–organic frameworks (MOFs). Furthermore, we correlate RET results performed on the model systems with the catalytic performance of two MOF‐encapsulated catalysts used to promote CO 2 hydrogenation and ring‐closing metathesis. Guests are incorporated using aperture‐opening encapsulation, and catalyst redistribution is not observed under practical reaction conditions, showcasing a pathway to advance catalyst recyclability in the case of host–guest platforms. These studies represent the first generalizable approach for mapping the guest distribution in heterogeneous host–guest catalytic systems, providing a foundation for predicting and tailoring the performance of catalysts integrated into various porous supports.

Thompson, William J.↗

DOE OSTI2024

Catalytically Active Site Mapping Realized through Energy Transfer Modeling

Thompson, William J.↗

NASA NTRS2015

Predicting Clear-Sky Reflectance Over Snow/Ice in Polar Regions

Satellite remote sensing of clouds requires an accurate estimate of the clear-sky radiances for a given scene to detect clouds and aerosols and to retrieve their microphysical properties. Knowing the spatial and angular variability of clear-sky albedo is essential for predicting clear-sky radiance at solar wavelengths. The Clouds and the Earth's Radiant Energy System (CERES) Project uses the nearinfrared (NIR; 1.24, 1.6 or 2.13 micrometers), visible (VIS; 0.63 micrometers) and vegetation (VEG; 0.86 micrometers) channels available on the Terra and Aqua Moderate Resolution Imaging Spectroradiometer (MODIS) to help identify clouds and retrieve their properties in both snow-free and snow-covered conditions. Thus, it is critical to have reliable distributions of clear-sky albedo for all of these channels. In CERES Edition 4 (Ed4), the 1.24-micrometer channel is used to retrieve cloud optical depth over snow/ice-covered surfaces. Thus, it is especially critical to accurately predict the 1.24-micrometer clear-sky albedo alpha and reflectance rho for a given location and time. Snow albedo and reflectance patterns are very complex due to surface texture, particle shapes and sizes, melt water, and vegetation protrusions from the snow surface. To minimize those effects, this study focuses on the permanent snow cover of Antarctica where vegetation is absent and melt water is minimal. Clear-sky albedos are determined as a function of solar zenith angle (SZA) from observations over all scenes determined to be cloud-free to produce a normalized directional albedo model (DRM). The DRM is used to develop alpha(SZA=0 degrees) on 10 foot grid for each season. These values provide the basis for predicting r at any location and set of viewing & illumination conditions. This paper examines the accuracy of this approach for two theoretical snow surface reflectance models.

Chen, Yan↗

NASA NTRS1995

High speed nozzles task

Supersonic cruise exhaust nozzles for advanced applications are optimized for a high nozzle pressure ratio (NPR) at design supersonic cruise Mach number and altitude. The performance of these nozzles with large expansion ratios are severely degraded for operations at subsonic speeds near sea level for NPR significantly less than the design values. The prediction of over-expanded 2DCD nozzles performance is critical to evaluating the internal losses and to the optimization of the integrated vehicle and propulsion system performance. The reported research work was aimed at validating and assessing existing computational methods and turbulence models for predicting the flow characteristics and nozzle performance at over-expanded conditions. Flow simulations in 2DCD nozzles were performed using five different turbulence models. The results are compared with the experimental data for the wall pressure distribution and thrust and flow coefficients at over-expanded static conditions.

Hamed, Awatef↗

DOE OSTI2017

Fragmentation of a Filamentary Cloud Permeated by a Perpendicular Magnetic Field

We examine the linear stability of an isothermal filamentary cloud permeated by a perpendicular magnetic field. Our model cloud is assumed to be supported by gas pressure against self-gravity in the unperturbed state. For simplicity, the density distribution is assumed to be symmetric around the axis. Also for simplicity, the initial magnetic field is assumed to be uniform, and turbulence is not taken into account. The perturbation equation is formulated to be an eigenvalue problem. The growth rate is obtained as a function of the wavenumber for fragmentation along the axis and the magnetic field strength. The growth rate depends critically on the outer boundary. If the displacement vanishes in regions very far from the cloud axis (fixed boundary), cloud fragmentation is suppressed by a moderate magnetic field, which means the plasma beta is below 1.67 on the cloud axis. If the displacement is constant along the magnetic field in regions very far from the cloud, the cloud is unstable even when the magnetic field is infinitely strong. The cloud is deformed by circulation in the plane perpendicular to the magnetic field. The unstable mode is not likely to induce dynamical collapse, since it is excited even when the whole cloud is magnetically subcritical. For both boundary conditions, the magnetic field increases the wavelength of the most unstable mode. We find that the magnetic force suppresses compression perpendicular to the magnetic field especially in regions of low density.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2020

Impact of boundary layer simulation on predicting radioactive pollutant dispersion: a case study for HANARO Research Reactor using the WRF-MMIF-CALPUFF modeling system

Wind plays an important role in cases of unexpected radioactive pollutant dispersion, deciding distribution and concentration of the leaked substance. The accurate prediction of wind has been challenging in numerical weather prediction models, especially near the surface because of the complex interaction between turbulent flow and topographic effect. As such, in this study, we investigated the characteristics of atmospheric dispersion of radioactive material (i.e. 137 Cs) according to the simulated boundary layer around the HANARO research nuclear reactor in Korea using the Weather Research and Forecasting (WRF)-Mesoscale Model Interface (MMIF)-California Puff (CALPUFF) model system. We examined the impacts of orographic drag on wind field, stability calculation methods, and planetary boundary layer parameterizations on the dispersion of radioactive material under a radioactive leaking scenario. We found that inclusion of the orographic drag effect in the WRF model improved the wind prediction most significantly over the complex terrain area, leading the model system to estimate the radioactive concentration near the reactor more conservatively. We also emphasized the importance of the stability calculation method and employing the skillful boundary layer parameterization to ensure more accurate low atmospheric conditions, in order to simulate more feasible spatial distribution of the radioactive dispersion in leaking scenarios.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1999

A Critical Examination of Wind-Wave Spectral Functional Form

Traditionally, data from random ocean waves are presented in spectral functions. The spectra are the result of Fourier analysis. Fourier spectral analysis has dominated data analysis for, at least, the last hundred years. It has been the standard method for is examining the global amplitude-frequency distributions. Although Fourier transform valid under extremely general conditions, there are some crucial restrictions for the Fourier spectral analysis. The system must be linear, and the data must be stationary- otherwise, the resulting spectrum will make little physical sense. The stationarity requirement is also a common required criterion for most of other available data analysis methods. Nevertheless, few, if any, natural phenomena are linear and stationary. To compound these complications is the imperfection of our probes or numerical schemes the interactions of the imperfect probes even with a perfect linear system can make the final data nonlinear. Furthermore, all the available data are usually of finite duration. Under these conditions, Fourier analysis is of limited use, For lack of alternatives, however, Fourier analysis is still used to process such data. The loose application of Fourier analysis and the insouciant adoption of the stationary and linear assumptions may lead to misleading conclusions. Ocean waves are know to be nonlinear, and the wind system generating the wave field are seldom stationary- As a result, the traditional examination of the spectral form hardly made physical sense. A new method for analyzing nonlinear and nonstationary data has been developed. The key part is the Empirical Mode Decomposition (EMD) method with which any complicated data set can be decomposed into a finite and often small number of Intrinsic Mode Functions (IMF) that serve as the basis of the representation of the data, This decomposition method is adaptive, and, therefore, highly efficient. The IMFs admit well-behaved Hilbert transforms, and yield instantaneous energy and frequency as functions of time that give sharp identifications of imbedded structures. The final presentation of the results is an energy-frequency-time distribution, designated as the Hilbert Spectrum. Among the main conceptual innovations is the introduction of the instantaneous frequencies for complicated data sets, which eliminate the need of spurious harmonics to represent nonlinear and nonstationary signals. The spectral forms of the ocean waves are very different. This new method offers the first physical meaningful view of the wave spectrum. Data from laboratory and field will be presented to illustrate the differences.

Huang, Norden E.↗

DOE OSTI2024

GrainGNN: A dynamic graph neural network for predicting 3D grain microstructure

We propose GrainGNN, a surrogate model for the evolution of polycrystalline grain structure under rapid solidification conditions in metal additive manufacturing. High fidelity simulations of solidification microstructures are typically performed using multicomponent partial differential equations (PDEs) with moving interfaces. The inherent randomness of the PDE initial conditions (grain seeds) necessitates ensemble simulations to predict microstructure statistics, e.g., grain size, aspect ratio, and crystallographic orientation. Here, currently such ensemble simulations are prohibitively expensive and surrogates are necessary.In GrainGNN, we use a dynamic graph to represent interface motion and topological changes due to grain coarsening. We use a reduced representation of the microstructure using hand-crafted features; we combine pattern finding and altering graph algorithms with two neural networks, a classifier (for topological changes) and a regressor (for interface motion). Both networks have an encoder-decoder architecture; the encoder has a multi-layer transformer long-short-term-memory architecture; the decoder is a single layer perceptron.We evaluate GrainGNN by comparing it to high-fidelity phase field simulations for in-distribution and out-of-distribution grain configurations for solidification under laser power bed fusion conditions. GrainGNN results in 80%–90% pointwise accuracy; and nearly identical distributions of scalar quantities of interest (QoI) between phase field and GrainGNN simulations compared using Kolmogorov-Smirnov test. GrainGNN's inference speedup (PyTorch on single x86 CPU) over a high-fidelity phase field simulation (CUDA on a single NVIDIA A100 GPU) is 150×–2000× for 100-initial grain problem. Further, using GrainGNN, we model the formation of 11,600 grains in 220 seconds on a single CPU core.

36 MATERIALS SCIENCE↗

NASA NTRS1985

Moments of catchment storm area

The portion of a catchment covered by a stationary rainstorm is modeled by the common area of two overlapping circles. Given that rain occurs within the catchment and conditioned by fixed storm and catchment sizes, the first two moments of the distribution of the common area are derived from purely geometrical considerations. The variance of the wetted fraction is shown to peak when the catchment size is equal to the size of the predominant storm. The conditioning on storm size is removed by assuming a probability distribution based upon the observed fractal behavior of cloud and rainstorm areas.

Eagleson, P. S.↗

DOE OSTI2014

Resolved H I imaging of a population of massive H I-rich galaxies with suppressed star formation

Despite the existence of well-defined relationships between cold gas and star formation, there is evidence that some galaxies contain large amounts of H I that do not form stars efficiently. By systematically assessing the link between H I and star formation within a sample of galaxies with extremely high H I masses (log M{sub H{sub I}}/M{sub ☉} > 10), we uncover a population of galaxies with an unexpected combination of high H I masses and low specific star formation rates that exists primarily at stellar masses greater than log M{sub *}/M{sub ☉} ∼ 10.5. We obtained H I maps of 20 galaxies in this population to understand the distribution of the H I and the physical conditions in the galaxies that could be suppressing star formation in the presence of large quantities of H I. We find that all of the galaxies we observed have low H I surface densities in the range in which inefficient star formation is common. The low H I surface densities are likely the main cause of the low specific star formation rates, but there is also some evidence that active galactic nuclei or bulges contribute to the suppression of star formation. The sample's agreement with the global star formation law highlights its usefulness as a tool for understanding galaxies that do not always follow expected relationships.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2017

An adaptive fast multipole accelerated Poisson solver for complex geometries

Here, we present a fast, direct and adaptive Poisson solver for complex two-dimensional geometries based on potential theory and fast multipole acceleration. More precisely, the solver relies on the standard decomposition of the solution as the sum of a volume integral to account for the source distribution and a layer potential to enforce the desired boundary condition. The volume integral is computed by applying the FMM on a square box that encloses the domain of interest. For the sake of efficiency and convergence acceleration, we first extend the source distribution (the right-hand side in the Poisson equation) to the enclosing box as a $C$ 0 function using a fast, boundary integral-based method. We demonstrate on multiply connected domains with irregular boundaries that this continuous extension leads to high accuracy without excessive adaptive refinement near the boundary and, as a result, to an extremely efficient “black box” fast solver.

97 MATHEMATICS AND COMPUTING↗

DOE OSTI2017

Continuation Power Flow Analysis for PV Integration Studies at Distribution Feeders

This paper presents a method for conducting continuation power flow simulation on high-solar penetration distribution feeders. A load disaggregation method is developed to disaggregate the daily feeder load profiles collected in substations down to each load node, where the electricity consumption of residential houses and commercial buildings are modeled using actual data collected from single family houses and commercial buildings. This allows the modeling of power flow and voltage profile along a distribution feeder on a continuing fashion for a 24- hour period at minute-by-minute resolution. By separating the feeder into load zones based on the distance between the load node and the feeder head, we studied the impact of PV penetration on distribution grid operation in different seasons and under different weather conditions for different PV placements.

AC Chronological Power Flow↗

DOE OSTI2025

Development and Validation of MALAMUTE model for Electric Field Assisted Sintering of Structural Materials

Fusion power plant designs feature extreme material performance requirements for structural material candidates. In addition to conventional alloys, more advanced composites and oxide dispersion strengthened (ODS) alloys are being explored, however, achieving the desired microstructures to maximize performance using traditional manufacturing methods can be challenging. The advanced manufacturing (AM) electric field-assisted sintering (EFAS) technique offers improved control over the final microstructure through higher heating and cooling rates and moderate pressures. Modeling and simulation tools show promise in elucidating the process-structure-property-performance (PSPP) correlation for AM-produced parts, including the EFAS process. An inherently multiscale process, the EFAS technique aligns well with the multiscale modeling capability of the open-source Multiphysics Object-Oriented Simulation Environment (MOOSE)[cite]. We present here an electro-thermo-mechanical approach to modeling the EFAS process using the MOOSE Application Library for Advanced Manufacturing UTilitiEs (MALAMUTE) code. Prediction of the field and gradient distributions across the EFAS tooling is required to accurately describe the conditions for the lower-scale microstructural evolution models. In this work we present the MALAMUTE model developed to predict the electrical potential, temperature, and mechanical stress distribution across the EFAS graphite tooling and part at the larger engineering-scale. Validation of the MALAMUTE engineering-scale model is completed using data from experimental densification and pre-densified runs of iron powder via EFAS at 1000oC. These runs were conducted using a Thermal Technology DCS-5 EFAS system. Data collected during the experiment runs include the direct current (DC) supplied to the graphite tooling, the temperature of the graphite tooling as measured with a pyrometer, and the force applied to the top of the graphite tooling stack, and the data were recorded every 10 seconds. Our validation approach used the current and force data from the EFAS run as boundary condition inputs to the MAMALUTE simulation; the temperature data were used to evaluate the MALAMUTE EFAS model prediction. Results of the MALAMUTE simulations are employed to connect the external pyrometer temperature measurement to the temperature profile across the part undergoing consolidation. We investigate the impact of material property variation and mesh deformation on the temperature profile as predicted by MALAMUTE. We conclude by highlighting projects where the MALAMUTE EFAS modeling and simulation capabilities will be used to assist experimental design.

36 - MATERIALS SCIENCE↗

NASA NTRS1988

Galerkin approximation for inverse problems for nonautonomous nonlinear distributed systems

An abstract framework and convergence theory is developed for Galerkin approximation for inverse problems involving the identification of nonautonomous nonlinear distributed parameter systems. A set of relatively easily verified conditions is provided which are sufficient to guarantee the existence of optimal solutions and their approximation by a sequence of solutions to a sequence of approximating finite dimensional identification problems. The approach is based on the theory of monotone operators in Banach spaces and is applicable to a reasonably broad class of nonlinear distributed systems. Operator theoretic and variational techniques are used to establish a fundamental convergence result. An example involving evolution systems with dynamics described by nonstationary quasilinear elliptic operators along with some applications are presented and discussed.

Banks, H. T.↗

NASA NTRS1994

High-lift flow-physics flight experiments on a subsonic civil transport aircraft (B737-100)

As part of the subsonic transport high-lift program, flight experiments are being conducted using NASA Langley's B737-100 to measure the flow characteristics of the multi-element high-lift system at full-scale high-Reynolds-number conditions. The instrumentation consists of hot-film anemometers to measure boundary-layer states, an infra-red camera to detect transition from laminar to turbulent flow, Preston tubes to measure wall shear stress, boundary-layer rakes to measure off-surface velocity profiles, and pressure orifices to measure surface pressure distributions. The initial phase of this research project was recently concluded with two flights on July 14. This phase consisted of a total of twenty flights over a period of about ten weeks. In the coming months the data obtained in this initial set of flight experiments will be analyzed and the results will be used to finalize the instrumentation layout for the next set of flight experiments scheduled for Winter and Spring of 1995. The main goal of these upcoming flights will be: (1) to measure more detailed surface pressure distributions across the wing for a range of flight conditions and flap settings; (2) to visualize the surface flows across the multi-element wing at high-lift conditions using fluorescent mini tufts; and (3) to measure in more detail the changes in boundary-layer state on the various flap elements as a result of changes in flight condition and flap deflection. These flight measured results are being correlated with experimental data measured in ground-based facilities as well as with computational data calculated with methods based on the Navier-Stokes equations or a reduced set of these equations. Also these results provide insight into the extent of laminar flow that exists on actual multi-element lifting surfaces at full-scale high-life conditions. Preliminary results indicate that depending on the deflection angle, the slat and flap elements have significant regions of laminar flow over a wide range of angles of attack. Boundary-layer transition mechanisms that were observed include attachment-line contamination on the slat and inflectional instability on the slat and fore flap. Also, the results agree fairly well with the predictions reported in a paper presented at last year's AIAA Fluid Dynamics Conference. The fact that extended regions of laminar flow are shown to exist on the various elements of the high-lift system raises the question what the effect is of loss of laminar flow as a result of insect contamiantion, rain or ice accumulation on high-life performance.

Vandam, Cornelis P.↗

NASA NTRS2019

Consistency Between NASS Surveyed Soil Moisture Conditions and SMAP Soil Moisture Observations

The USDA National Agricultural Statistics Survey (NASS) collects and publishes crop growth status and soil moisture conditions in major US agricultural regions. The operationally-produced weekly reports are based on survey information. The surveys are based on visual assessments and ? in the case of soil moisture ? report soil moisture levels in one of four categories (Very Short, Short, Adequate and Surplus). In this study, we show that these reports have remarkable correspondence with the NASA Soil Moisture Active Passive (SMAP) Level-4 Soil Moisture (L4SM) product. This consistency allows the combining the two distinct types of data to produce a value-added combination, which is mapped fields rather than State-by-State tables and it is refreshed daily rather than weekly. In this study classification thresholds are derived for L4SM by mapping cumulative distribution functions of L4SM surface and root-zone SM to the categorical NASS SM conditions. The results show that, year-over-year, the SMAP cumulative SM distributions are consistent with the NASS SM conditions and, furthermore, that the temporal evolution of the SMAP-derived thresholds is consistent with the seasonal crop growth cycles from year to year. The results signify that the SMAP SM retrievals are relatable to SM estimation conducted in agriculture by land managers and farmers, which underlines the general applicability of the SMAP data.

Andreas Colliander↗

DOE OSTI2015

Random Sampling of Correlated Parameters – a Consistent Solution for Unfavourable Conditions

Two methods for random sampling according to a multivariate lognormal distribution – the correlated sampling method and the method of transformation of correlation coefficients – are briefly presented. The methods are mathematically exact and enable consistent sampling of correlated inherently positive parameters with given information on the first two distribution moments. Furthermore, a weighted sampling method to accelerate the convergence of parameters with extremely large relative uncertainties is described. However, the method is efficient only for a limited number of correlated parameters.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2014

Radionuclide Inventory and Distribution: Fourmile Branch, Pen Branch, and Steel Creek IOUs

As a condition to the Department of Energy (DOE) Low Level Waste Disposal Federal Facility Review Group (LFRG) review team approving the Savannah River Site (SRS) Composite Analysis (CA), SRS agreed to follow up on a secondary issue, which consisted of the consolidation of several observations that the team concluded, when evaluated collectively, could potentially impact the integration of the CA results. This report addresses secondary issue observations 4 and 21, which identify the need to improve the CA sensitivity and uncertainty analysis specifically by improving the CA inventory and the estimate of its uncertainty. The purpose of the work described herein was to be responsive to these secondary issue observations by re-examining the radionuclide inventories of the Integrator Operable Units (IOUs), as documented in ERD 2001 and Hiergesell, et. al. 2008. The LFRG concern has been partially addressed already for the Lower Three Runs (LTR) IOU (Hiergesell and Phifer, 2012). The work described in this investigation is a continuation of the effort to address the LFRG concerns by re-examining the radionuclide inventories associated with Fourmile Branch (FMB) IOU, Pen Branch (PB) IOU and Steel Creek (SC) IOU. The overall approach to computing radionuclide inventories for each of the IOUs involved the following components: Defining contaminated reaches of sediments along the IOU waterways, Identifying separate segments within each IOU waterway to evaluate individually, Computing the volume and mass of contaminated soil associated with each segment, or “compartment”, Obtaining the available and appropriate Sediment and Sediment/Soil analytical results associated with each IOU, Standardizing all radionuclide activity by decay-correcting all sample analytical results from sample date to the current point in time, Computing representative concentrations for all radionuclides associated with each compartment in each of the IOUs, Computing the radionuclide inventory of each DOE-added radionuclide for the compartments of each IOU by applying the representative, central value concentration to the mass of contaminated soil, Totaling the inventory for all compartments associated with each of the IOUs Using this approach the 2013 radionuclide inventories for each sub-compartment associated with each of the three IOUs were computed, by radionuclide. The inventories from all IOU compartments were then rolled-up into a total inventory for each IOU. To put the computed estimate of radionuclide activities within FMB, PB, and SC IOUs into context, attention was drawn to Cs-137, which was the radionuclide with the largest contributor to the calculated dose to a member of the public at the perimeter of SRS within the 2010 SRS CA (SRNL 2010). The total Cs-137 activity in each of the IOUs was calculated to be 9.13, 1.5, and 17.4 Ci for FMB, PB, and SC IOUs, respectively. Another objective of this investigation was to address the degree of uncertainty associated with the estimated residual radionuclide activity that is calculated for the FMB, PB, and SC IOUs. Two primary contributing factors to overall uncertainty of inventory estimates were identified and evaluated. The first related to the computation of the mass of contaminated material in a particular IOU compartment and the second to the uncertainty associated with analytical counting errors. The error ranges for the mass of contaminated material in each IOU compartment were all calculated to be approximately +/- 9.6%, or a nominal +/-10%. This nominal value was added to the uncertainty associated with the analytical counting errors that were associated with each radionuclide, individually. This total uncertainty was then used to calculate a maximum and minimum estimated radionuclide inventories for each IOU.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗