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654 records · Page 37

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DOE OSTI2023

Arctic tropospheric ozone: assessment of current knowledge and model performance

As the third most important greenhouse gas (GHG) after carbon dioxide (CO 2 ) and methane (CH 4 ), tropospheric ozone (O 3 ) is also an air pollutant causing damage to human health and ecosystems. This study brings together recent research on observations and modeling of tropospheric O 3 in the Arctic, a rapidly warming and sensitive environment. At different locations in the Arctic, the observed surface O 3 seasonal cycles are quite different. Coastal Arctic locations, for example, have a minimum in the springtime due to O 3 depletion events resulting from surface bromine chemistry. In contrast, other Arctic locations have a maximum in the spring. The 12 state-of-the-art models used in this study lack the surface halogen chemistry needed to simulate coastal Arctic surface O 3 depletion in the springtime; however, the multi-model median (MMM) has accurate seasonal cycles at non-coastal Arctic locations. There is a large amount of variability among models, which has been previously reported, and we show that there continues to be no convergence among models or improved accuracy in simulating tropospheric O 3 and its precursor species. The MMM underestimates Arctic surface O 3 by 5% to 15% depending on the location. The vertical distribution of tropospheric O 3 is studied from recent ozonesonde measurements and the models. The models are highly variable, simulating free-tropospheric O 3 within a range of ±50% depending on the model and the altitude. The MMM performs best, within ±8% for most locations and seasons. However, nearly all models overestimate O 3 near the tropopause (~300 hPa or ~8 km), likely due to ongoing issues with underestimating the altitude of the tropopause and excessive downward transport of stratospheric O 3 at high latitudes. For example, the MMM is biased high by about 20% at Eureka. Observed and simulated O 3 precursors (CO, NO x , and reservoir PAN) are evaluated throughout the troposphere. Models underestimate wintertime CO everywhere, likely due to a combination of underestimating CO emissions and possibly overestimating OH. Throughout the vertical profile (compared to aircraft measurements), the MMM underestimates both CO and NO x but overestimates PAN. Perhaps as a result of competing deficiencies, the MMM O 3 matches the observed O 3 reasonably well. Our findings suggest that despite model updates over the last decade, model results are as highly variable as ever and have not increased in accuracy for representing Arctic tropospheric O 3 .

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Shock-induced chemical decomposition and overdriven detonation in hexahydro-1,3,5-trinitro-1,3,5-triazine (RDX) single crystals

Understanding the differences in the shock compression and detonation response of insensitive high explosives (IHEs) and conventional HEs (CHEs) is a long-standing need in HE science and technology. Having previously examined 1,1-diamino-2,2-dinitroethene (FOX-7) IHE single crystals, the shock and detonation response of hexahydro-1,3,5-trinitro-1,3,5-triazine (RDX)—a widely used CHE—was determined using wave profile measurements in ~250 μm thick single crystals shock compressed to 63 GPa. In marked contrast to FOX-7, RDX single crystals shocked along the [100] and [111] orientations showed wave profile features consistent with chemical decomposition onset at 15 GPa. These features were more pronounced for [100] RDX, suggesting a higher decomposition rate compared to [111] RDX. At 51 GPa and above, flat-topped single waves were observed for both orientations, showing the classic Chapman–Jouget (C–J) detonation response in which the decomposition is completed within the detonation front. The Hugoniot states and sound speeds determined for the detonation products were similar for both [100] and [111] orientations, showing that the overdriven detonation response for RDX does not depend on crystal orientation. The C–J pressure for RDX single crystals (35 GPa)—determined experimentally—is comparable to that of FOX-7. However, compared to FOX-7, chemical decomposition onset for RDX occurs at much lower pressures and the overdriven C–J detonation response occurs at higher pressures. Lastly, the present findings constitute the first experimental comparison of the shock and detonation response of conventional and insensitive HE single crystals over a broad pressure range below and above the C–J pressure.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Thermal and radiation response of 4H–SiC Schottky diodes with direct-write electrical contacts

In this work, a high-sensitivity 4H–SiC temperature sensor and an alpha detector have been fabricated using additively printed metal contacts. The surface morphology and electrical conductivity of the printed electrodes were established prior to Schottky diode development. 4H–SiC Schottky diodes with direct-write printed silver contacts on the 5 μ m-thick epilayer on 4H–SiC were characterized electrically in terms of the forward and reverse current–voltage and high-frequency capacitance–voltage characteristics. Furthermore, the turn-on voltage of the Schottky diodes, as established from the forward current–voltage characteristics measured up to a temperature of 400 °C, showed a linear temperature dependence. Schottky diodes with direct-write printed Ag electrodes were able to measure alpha particles emitted from Americium-241. The high temperature and radiation response of the Schottky diodes show their suitability for multi-modal sensor fusion on the 4H–SiC platform for harsh environment applications.

42 ENGINEERING↗

DOE OSTI2021

Stepwise Dynamic Calibration of a Hydromechanical Simulation Using Time-Lapse Vertical Seismic Profile

This study aims to develop a methodology for calibrating subsurface stress changes through time-lapse Vertical Seismic Profiling (VSP) integration. The selected study site is the 13-10A injector well within the ongoing CO2-EOR operation of the Farnsworth Field Unit. The Time-lapse VSP dataset carries the combined effects of fluid substitution and mean effective stress changes, thereby providing a dataset amenable for the calibration of production and injection-induced stress changes. The concept is similar to calibrating a reservoir simulation model in that the process honor real field data to set up an inverse problem. The solution optimizes the independent and impactful geomechanical parameters that replicate the observed time-lapse seismic velocity changes. This stress calibration is enabled by 4D geomechanical modeling and the VSP Integration workflow. This calibration benefits from extensive geological, geophysical and geomechanical characterization through 3D seismic data, geophysical well logs, and core assessed as part of the 1D MEM conducted on the 13-10A subject well. These data are used to develop a site-specific rock physics model. The Biot Gassmann workflow combines rock physics and reservoir simulation outputs to determine the fluid substitution contribution to seismic velocity change. Additionally, modeled seismic velocity attributed to mean effective stress are determined from the geomechanical simulation outputs, and the stress-velocity relationship developed from the ultrasonic seismic velocity measurements on the extracted Morrow B core. A penalty function is then formed between the modeled seismic velocities and the observed time-lapse VSP dataset. Four independent and impactful geomechanical parameters have been determined. These are the bulk modulus and shear modulus for zero porosity and the shear and compressional seismic velocity to mean effective stress derivatives. The dataset of numerous coupled hydromechanical- geomechanical simulation realizations is built by combining variations of the four stated geomechanical parameters. A machine learning-assisted workflow comprised of an artificial neural network and a particle swarm optimizer are used to converge on the optimal geomechanical parameters. The successful execution of this workflow has affirmed the suitability of acoustic time-lapse measurements for 4D-VSP geomechanical stress calibration pending measurable stress sensitivities within the anticipated effective stress changes and the availability of suitable and reliable datasets for petroelastic modeling.

02 PETROLEUM↗

DOE OSTI2022

Medium-Scale Methanol Pool Fire Model Validation

In this work, medium scale (30 cm diameter) methanol pool fires were simulated using the latest fire modeling suite implemented in Sierra/Fuego, a low Mach number multiphysics reacting flow code. The sensitivity of model outputs to various model parameters was studied with the objective of providing model validation. This work also assesses model performance relative to other recently published large eddy simulations (LES) of the same validation case. Two pool surface boundary conditions were simulated. The first was a prescribed fuel mass flux and the second used an algorithm to predict mass flux based on a mass and energy balance at the fuel surface. Gray gas radiation model parameters (absorption coefficients and gas radiation sources) were varied to assess radiant heat losses to the surroundings and pool surface. The radiation model was calibrated by comparing the simulated radiant fraction of the plume to experimental data. The effects of mesh resolution were also quantified starting with a grid resolution representative of engineering type fire calculations and then uniformly refining that mesh in the plume region. Simulation data were compared to experimental data collected at the University of Waterloo and the National Institute of Standards and Technology (NIST). Validation data included plume temperature, radial and axial velocities, velocity temperature turbulent correlations, velocity velocity turbulent correlations, radiant and convective heat fluxes to the pool surface, and plume radiant fraction. Additional analyses were performed in the pool boundary layer to assess simulated flame anchoring and the effect on convective heat fluxes. This work assesses the capability of the latest Fuego physics and chemistry model suite and provides additional insight into pool fire modeling for nonluminous, non-sooting flames.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Analysis of furnace contamination on superconducting radio frequency niobium using secondary-ion mass spectrometry

Detection of surface contamination on niobium materials used in superconducting radio frequency (SRF) applications is difficult due to quantitative sensitivity and near-atomic depth resolution needed. Inspection of samples known to have experienced surface contamination was found to have inconsistent nitride coverage after high-temperature nitrogen gas exposure (“doping”). Here we compare contaminating species found on samples treated in several different vacuum furnaces, both “exposed” directly in the chamber and “protected” by containment shielding from evaporative sources with “furnace caps.” Typically, furnace caps are used to impede contamination from reaching the interior surface of cavities during the high-temperature vacuum bake that immediately precedes exposure to nitrogen gas. Although, to date, little is known about the effectiveness of these caps, SIMS results showed that they were effective in limiting contamination arising from the furnace environment. Inspection of sample surfaces by SEM showed a lack of nitrides present on contaminated specimens. TEM with energy dispersive spectroscopy performed on these samples revealed that a carbon-rich layer now existed, indicating that a relatively high contaminant load prevents the nucleation and growth of surface nitrides, while thus inhibiting interstitial nitrogen uptake. Except in extreme cases, subsequent removal of the top several micrometers of the surface via electropolishing appears to effectively eliminate any strong influence on the subsequent SRF cavity performance. With the absence of furnace cleaning, carbon contamination was found to be nearly 10× higher for protected nitrogen-doped and electropolished samples, with minimal metallic contamination detected for both processes. SIMS analysis was also performed to compare the cleanliness of samples fully prepared by such nitrogen “doping” with those prepared by a related process, involving the dissolution of niobium surface oxide and diffusion of oxygen into the surface. This oxygen doping or alloying process offers attractive advantages.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗