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At least 253 records · Page 14

Screening Ionic Liquids Based on Ionic Volume and Electrostatic Potential Analyses

Ionic liquids are known to have tunable solvation properties, based on the pairing of different anions and cations, but the compositional landscape is vast and challenging to navigate efficiently. Some computational screening protocols are available, but they can be either time-consuming or difficult to implement. Herein, we perform a detailed investigation of the fundamental role of electrostatic interactions in these systems. We effectively develop a bridge between the previous volume-based approach (VBA) with a quantum structure–property relationship (QSPR) approach to create fast, simple screening guidelines. We propose a new parameter that is applicable to both monovalent and multivalent ions, the ionic polarity index (IPI), which is defined as the ratio of the average electrostatic surface potential ($\bar{V}$) of the ion to the net charge of the ion (q). The IPI correlation has been tested on a diverse dataset of 121 ions and reliable predictions can be obtained within a homologous series of ionic liquid compounds.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Validation of Methods for Computational Catalyst Design: Geometries, Structures, and Energies of Neutral and Charged Silver Clusters

We report a systematic study of small silver clusters, Agn, Agn+, and Agn–, n = 1–7. We studied all possible isomers of clusters with n = 5–7. We tested 42 exchange–correlation functionals, and we assess these functionals for their accuracy in three respects: geometries (quantitative prediction of internuclear distances), structures (the nature of the lowest-energy structure, for example, whether it is planar or nonplanar), and energies. We find that the ingredients of exchange–correlation functionals are indicators of their success in predicting geometries and structures: local exchange–correlation functionals are generally better than hybrid functionals for geometries; functionals depending on kinetic energy density are the best for predicting the lowest-energy isomer correctly, especially for predicting two-dimensional to three-dimenstional transitions correctly. The accuracy for energies is less sensitive to the ingredient list. Our findings could be useful for guiding the selection of methods for computational catalyst design.

Environmental Molecular Sciences Laboratory↗

Rational solvent molecule tuning for high-performance lithium metal battery electrolytes

Electrolyte engineering improved cycling of Li metal batteries and anode-free cells at low current densities; however, high-rate capability and tuning of ionic conduction in electrolytes are desirable yet less-studied. In this study, we design and synthesize a family of fluorinated-1,2-diethoxyethanes as electrolyte solvents. The position and amount of F atoms functionalized on 1,2-diethoxyethane were found to greatly affect electrolyte performance. Partially fluorinated, locally polar –CHF 2 is identified as the optimal group rather than fully fluorinated –CF 3 in common designs. Paired with 1.2 M lithium bis(fluorosulfonyl)imide, these developed single-salt-single-solvent electrolytes simultaneously enable high conductivity, low and stable overpotential, >99.5% Li||Cu half-cell efficiency (up to 99.9%, ±0.1% fluctuation) and fast activation (Li efficiency >99.3% within two cycles). Combined with high-voltage stability, these electrolytes achieve roughly 270 cycles in 50-μm-thin Li||high-loading-NMC811 full batteries and >140 cycles in fast-cycling Cu||microparticle-LiFePO 4 industrial pouch cells under realistic testing conditions. The correlation of Li + –solvent coordination, solvation environments and battery performance is investigated to understand structure–property relationships.

25 ENERGY STORAGE↗

The ITER pre-compression rings – A first in cryogenic composite technology

The ITER Pre-Compression Rings represent one of the heaviest composite structures ever manufactured as a single piece and the largest - the outer diameter will be above 5.5 meters - intended for use in a cryogenic environment. With a cross section of 337 mm × 288 mm, each item will weigh more than 3,000 kg. A development program, based on filament wound and dry wound S2 glass unidirectional fibers, the latter processed by VARTM, was completed on one fifth scale rings, and these materials and techniques were shown to be satisfactory. The paper describes how a technology applied to build up primary structures of European launchers is being accommodated to produce the ITER Pre-Compression Rings, fulfilling its extremely challenging requirements. In addition, we will describe how the structural analysis is correlated with the test results of scaled down rings, as well as how the pre-compression rings’ manufacturing process will be qualified.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Eddy current sensor for in-situ monitoring of swelling of Li-ion prismatic cells

In-situ monitoring an on-board rechargeable battery in hybrid cars can be used to ensure a long operating life of the battery and safe operation of the vehicle. Intercalations of ions in the electrode material during charge and discharge of a Lithium Ion battery cause periodic stress and strain of the electrode materials that can ultimately lead to fatigue resulting in capacity loss and potential battery failure. Currently this process is not monitored directly on the cells. This work is focused on development technologies that would quantify battery swelling and provide in-situ monitoring for onboard vehicle applications. Several rounds of tests have been performed to spatially characterize cell expansion of a 5 Ah cell with a nickel/manganese/cobalt-oxide cathode (Sanyo, Japan) used by Ford in their Fusion HEV battery pack. A collaborative team of researchers from GE and the University of Michigan has characterized the free expansion of these cells to be in the range of 100×125 microns (1% of total cell thickness) at the center point of the cell. GE proposed to use a thin eddy current (EC) coil to monitor these expansions on the cells while inside the package. The photolithography manufacturing process previously developed for EC arrays for detecting cracks in aircraft engine components was used to build test coils for gap monitoring. These sensors are thin enough to be placed safely between neighboring cells and capable of monitoring small variations in the gap between the cells. Preliminary investigations showed that these coils can be less than 100 micron thick and have sufficient sensitivity in a range from 0 to 2 mm. Laboratory tests revealed good correlation between EC and optical gap measurements in the desired range. Further technology development could lead to establishing a sensor network for a low cost solution for the in-situ monitoring of cell swelling during battery operation.

42 ENGINEERING↗

Coupled cluster benchmarks of large noncovalent complexes: The L7 dataset as well as DNA–ellipticine and buckycatcher–fullerene

In this work, benchmark binding energies for dispersion-bound complexes in the L7 dataset, the DNA–ellipticine intercalation complex, and the buckycatcher–C60 complex with 120 heavy atoms using a focal-point method based on the canonical form of second-order Møller−Plesset theory (MP2) and the domain based local pair natural orbital scheme for the coupled cluster with single, double, and perturbative triple excitations [CCSD(T)] extrapolated to the complete basis set (CBS) limit are reported. This work allows for increased confidence given the agreement with respect to values recently obtained using the local natural orbital CCSD(T) for L7 and the canonical CCSD(T)/CBS result for the coronene dimer (C2C2PD). Therefore, these results can be considered pushing the CCSD(T)/CBS binding benchmark to the hundred-atom scale. The disagreements between the two state-of-the-art methods, CCSD(T) and fixed-node diffusion Monte Carlo, are substantial with at least 2.0 (∼10%), 1.9 (∼5%), and 10.3 kcal/mol (∼25%) differences for C2C2PD in L7, DNA–ellipticine, and buckycatcher–C60, respectively. Such sizable discrepancy above “chemical accuracy” for large noncovalent complexes indicates how challenging it is to obtain benchmark binding interactions for systems beyond small molecules, although the three up-to-date density functionals, PBE0+D4, ωB97M-V, and B97M-V, agree better with CCSD(T) for these large systems. In addition to reporting these values, different basis sets and various CBS extrapolation parameters for Hartree–Fock and MP2 correlation energies were tested for the first time in large noncovalent complexes with the goal of providing some indications toward optimal cost effective routes to approach the CBS limit without substantial loss in quality.

Ballesteros, Francisco (ORCID:0000000325732307)↗

Herschel far-infrared photometry of the swift burst alert telescope active galactic nuclei sample of the local universe. I. PACS observations

Far-Infrared (FIR) photometry from the Photodetector Array Camera and Spectrometer on the Herschel Space Observatory is presented for 313 nearby, hard X-ray selected galaxies from the 58 month Swift Burst Alert Telescope (BAT) Active Galactic Nuclei catalog. The present data do not distinguish between the FIR luminosity distributions at 70 and 160 μm for Seyfert 1 and Seyfert 2 galaxies. This result suggests that if the FIR emission is from the nuclear obscuring material surrounding the accretion disk, then it emits isotropically, independent of orientation. Alternatively, a significant fraction of the 70 and 160 μm luminosity could be from star formation, independent of active galactic nucleus (AGN) type. Using a non-parametric test for partial correlation with censored data, we find a statistically significant correlation between the AGN intrinsic power (in the 14-195 keV band) and the FIR emission at 70 and 160 μm for Seyfert 1 galaxies. We find no correlation between the 14-195 keV and FIR luminosities in Seyfert 2 galaxies. The observed correlations suggest two possible scenarios: (1) if we assume that the FIR luminosity is a good tracer of star formation, then there is a connection between star formation and the AGN at sub-kiloparsec scales, or (2) dust heated by the AGN has a statistically significant contribution to the FIR emission. Using a Spearman rank-order analysis, the 14-195 keV luminosities for the Seyfert 1 and 2 galaxies are weakly statistically correlated with the F {sub 70}/F {sub 160} ratios.

79 ASTRONOMY AND ASTROPHYSICS↗

THE CHANDRA COSMOS SURVEY. III. OPTICAL AND INFRARED IDENTIFICATION OF X-RAY POINT SOURCES

The Chandra COSMOS Survey (C-COSMOS) is a large, 1.8 Ms, Chandra program that has imaged the central 0.9 deg{sup 2} of the COSMOS field down to limiting depths of 1.9 Multiplication-Sign 10{sup -16} erg cm{sup -2} s{sup -1} in the soft (0.5-2 keV) band, 7.3 Multiplication-Sign 10{sup -16} erg cm{sup -2} s{sup -1} in the hard (2-10 keV) band, and 5.7 Multiplication-Sign 10{sup -16} erg cm{sup -2} s{sup -1} in the full (0.5-10 keV) band. In this paper we report the i, K, and 3.6 {mu}m identifications of the 1761 X-ray point sources. We use the likelihood ratio technique to derive the association of optical/infrared counterparts for 97% of the X-ray sources. For most of the remaining 3%, the presence of multiple counterparts or the faintness of the possible counterpart prevented a unique association. For only 10 X-ray sources we were not able to associate a counterpart, mostly due to the presence of a very bright field source close by. Only two sources are truly empty fields. The full catalog, including spectroscopic and photometric redshifts and classification described here in detail, is available online. Making use of the large number of X-ray sources, we update the 'classic locus' of active galactic nuclei (AGNs) defined 20 years ago in soft X-ray surveys and define a new locus containing 90% of the AGNs in the survey with full-band luminosity >10{sup 42} erg s{sup -1}. We present the linear fit between the total i-band magnitude and the X-ray flux in the soft and hard bands, drawn over two orders of magnitude in X-ray flux, obtained using the combined C-COSMOS and XMM-COSMOS samples. We focus on the X-ray to optical flux ratio (X/O) and we test its known correlation with redshift and luminosity, and a recently introduced anti-correlation with the concentration index (C). We find a strong anti-correlation (though the dispersion is of the order of 0.5 dex) between X/O computed in the hard band and C and that 90% of the obscured AGNs in the sample with morphological information live in galaxies with regular morphology (bulgy and disky/spiral), suggesting that secular processes govern a significant fraction of the black hole growth at X-ray luminosities of 10{sup 43}-10{sup 44.5} erg s{sup -1}. We also investigate the degree of obscuration of the sample using the hardness ratio, and we compare the X-ray color with the near-infrared to optical color.

79 ASTRONOMY AND ASTROPHYSICS↗

Direction dependence of the power spectrum and its effect on the cosmic microwave background radiation

We study several anisotropic inflationary models and their implications for the observed violation of statistical isotropy in the CMBR data. In two of these models the anisotropy decays very quickly during the inflationary phase of expansion. We explicitly show that these models lead to violation of isotropy only for low l CMBR modes. Our primary aim is to fit the observed alignment of l = 2,3 multipoles to the theoretical models. We use two measures, based on the power tensor, which contains information about the alignment of each multipole, to quantify the anisotropy in data. One of the measures uses the dispersion in eigenvalues of the power tensor. We also define another measure which tests the overall correlation between two different multipoles. We perturbatively compute these measures of anisotropy and fix the theoretical parameters by making a best fit to l = 2,3 multipoles. We show that some of the models studied are able to consistently explain the observed violation of statistical isotropy.

79 ASTRONOMY AND ASTROPHYSICS↗

CoLoRe: fast cosmological realisations over large volumes with multiple tracers

We present CoLoRe, a public software package to efficiently generate synthetic realisations of multiple cosmological surveys.CoLoRe can simulate the growth of structure with different degrees of accuracy, with the current implementation supporting lognormal fields, first, and second order Lagrangian perturbation theory.CoLoRe simulates the density field on an all-sky light-cone up to a desired maximum redshift, and uses it to generate multiple 2D and 3D maps: galaxy positions and velocities, lensing (shear, magnification, convergence), integrated Sachs-Wolfe effect, line intensity mapping, and line of sight skewers for simulations of the Lyman-α forest. We test the accuracy of the simulated maps against analytical theoretical predictions, and showcase its performance with a multi-survey simulation including DESI galaxies and quasars, LSST galaxies and lensing, and SKA intensity mapping and radio galaxies. We expect CoLoRe to be particularly useful in studies aiming to characterise the impact of systematics in multi-experiment analyses, quantify the covariance between different datasets, and test cross-correlation pipelines for near-future surveys.

79 ASTRONOMY AND ASTROPHYSICS↗

Local-noise spectroscopy for nonequilibrium systems

Here, we introduce the notion, and develop the theory of, local-noise spectroscopy (LNS)—a tool to study the properties of systems far from equilibrium by means of flux density correlations. As a test bed, we apply it to biased molecular junctions. This tool naturally extends those based on local fluxes, while providing complementary information on the system. As examples of the rich phenomenology that one can study with this approach, we show that LNS can be used to yield information on microscopic properties of bias-induced light emission in junctions, provide local resolution of intrasystem interactions, and employed as a nanothermometry tool. Although LNS may, at the moment, be difficult to realize experimentally, it can nonetheless be used as a powerful theoretical tool to infer a wide range of physical properties on a variety of systems of present interest.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Data-driven model validation for neutrino-nucleus cross section measurements

Neutrino-nucleus cross section measurements are needed to improve interaction modeling to meet the precision needs of neutrino experiments in efforts to measure oscillation parameters and search for physics beyond the Standard Model. We review the difficulties associated with modeling neutrino-nucleus interactions that lead to a dependence on event generators in oscillation analyses and cross section measurements alike. We then describe data-driven model validation techniques intended to address this model dependence. The method relies on utilizing various goodness-of-fit tests and the correlations between different observables and channels to probe the model for defects in the phase space relevant for the desired analysis. These techniques shed light on relevant mismodeling, allowing it to be detected before it begins to bias the cross section results. We compare more commonly used model validation methods which directly validate the model against alternative ones to these data-driven techniques and show their efficacy with fake data studies. These studies demonstrate that employing data-driven model validation in cross section measurements represents a reliable strategy to produce robust results that will stimulate the desired improvements to interaction modeling.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Experimental Analysis of the Effects of Simulator Complexity on Human Performance

Human Reliability Analysis predicts accidents caused by human errors and is an important factor in Probabilistic Safety Assessment that comprehensively evaluates the safety of nuclear power plants. This study compares and analyzes the human performance of nuclear power plant operators according to the simulator complexity as part of the HRA data collection support method development project conducted by Idaho National Laboratory. This experiment was conducted by setting two types of simulators and scenarios as independent variables. The data collected by conducting the experiments in two different simulators were analyzed using an analysis of variance test and a correlation analysis, and four human performance charts were derived.

99 GENERAL AND MISCELLANEOUS↗

Development of a 300 MWe Utility Scale Oxy-Fuel sCO2 Turbine

A 300 MWe direct-fired supercritical carbon dioxide (sCO2) oxy-fuel turbine is being developed that will burn natural gas-fired, coal syngas and even hydrogen mixtures capable of 1,150ºC turbine inlet temperature at 300 bar. This design will significantly improve the state-of-the-art for thermal efficiency and results in a high-pressure stream of CO2 with 98%+ carbon capture, making the power plant near emission-free and more efficient than Natural Gas Combined Cycle (NGCC) plants with carbon capture. This power plant will be capable of burning coal through gasification and cleanup of the synthesis gas (syngas). sCO2 power cycles are a transformational technology for the energy industry, providing higher efficiency heat source energy conversion for conventional and alternative energy sources. This novel cycle significantly reduces capital costs because of smaller equipment footprints, design modularity, and allows for rapid cyclic load and source following to balance solar and wind energy power swings. Oxy-fuel sCO2 cycles take these advantages even further, utilizing higher firing temperatures, improved efficiency, and simpler carbon capture strategies. This turbine will require cooled turbine nozzles and blades as well as advanced thermal management systems to accommodate these high temperatures. The cooled blade heat transfer correlations required new test programs at higher Reynolds number than air-breathing gas turbines for impingement, serpentine, and pin-fin regions. Novel blade optimization was performed to maximize aerodynamic efficiency, while minimizing cooling flows. A turbine layout was generated utilizing individual combustor cans with cooled liners feeding into a 6-stage axial flow turbine with cooled stator nozzles and turbine blades. The case design and thermal management preliminary design will be described.

Moore, Jeffrey↗

TU-A-12A-08: Computing Longitudinal Material Changes in Bone Metastases Using Dual Energy Computed Tomography

Purpose: This study demonstrates a methodology for tracking changes in metastatic bone disease using trajectories in material basis space in serial dual energy computed tomography (DECT) studies. Methods: This study includes patients with bone metastases from breast cancer that had clinical surveillance CT scans using a General Electric CT750HD in dual energy mode. A radiologist defined regions-of-interested (ROI) for bone metastasis, normal bone, and marrow across the serial DECT scans. Our approach employs a Radon transform to forward-projection the basis images, namely, water and iodine, into sinogram space. This data is then repartitioned into fat/bone and effective density/Z image pairs using assumed energy spectrums for the x-ray energies. This approach both helps remove negative material densities and avoids adding spectrum-hardening artifacts. These new basis data sets were then reconstructed via filtered back-projection to create new material basis pair images. The trajectories of these pairs were then plotted in the new basis space providing a means to both visualize and quantitatively measure changes in the material properties of the tumors. Results: ROI containing radiologist defined metastatic bone disease showed well-defined trajectories in both fat/bone and effective density/Z space. ROI that contained radiologist defined normal bone and marrow did not exhibit any discernible trajectories and were stable from scan to scan. Conclusions: The preliminary results show that changes in material composition and effective density/Z image pairs were seen primarily in metastasis and not in normal tissue. This study indicates that by using routine clinical DECT it may be possible to monitor therapy response of bone metastases because healing or worsening bone metastases change material composition of bone. Additional studies are needed to further validate these results and to test for their correlation with outcome.

60 APPLIED LIFE SCIENCES↗

Uncertain of uncertainties? A comparison of uncertainty quantification metrics for chemical data sets

Abstract With the increasingly more important role of machine learning (ML) models in chemical research, the need for putting a level of confidence to the model predictions naturally arises. Several methods for obtaining uncertainty estimates have been proposed in recent years but consensus on the evaluation of these have yet to be established and different studies on uncertainties generally uses different metrics to evaluate them. We compare three of the most popular validation metrics (Spearman’s rank correlation coefficient, the negative log likelihood (NLL) and the miscalibration area) to the error-based calibration introduced by Levi et al. ( Sensors 2022 , 22 , 5540). Importantly, metrics such as the negative log likelihood (NLL) and Spearman’s rank correlation coefficient bear little information in themselves. We therefore introduce reference values obtained through errors simulated directly from the uncertainty distribution. The different metrics target different properties and we show how to interpret them, but we generally find the best overall validation to be done based on the error-based calibration plot introduced by Levi et al. Finally, we illustrate the sensitivity of ranking-based methods (e.g. Spearman’s rank correlation coefficient) towards test set design by using the same toy model ferent test sets and obtaining vastly different metrics (0.05 vs. 0.65).

Rasmussen, Maria H.↗

Site Characterization of the Highest-Priority Geologic Formations for CO2 Storage in Wyoming

The project Site Characterization of the Highest-Priority Geologic Formations for CO2 Storage in Wyoming is one of 9 site characterization projects that were implemented as part of ARRA (American Recovery and Reinvestment Act). Data from this project was used to improve resolution of data in NATCARB in the area of study. Data related to this study has already been incorporated in NATCARB Atlas. The Wyoming Carbon Underground Storage Project (WY-CUSP) consisted of CO2 storage site characterization and evaluation, focusing on Wyoming’s most promising CO2 storage reservoirs (the Pennsylvanian Weber/Tensleep Sandstone and Mississippian Madison Limestone) and premier CO2 storage site (Rock Springs Uplift). Results from the WY-CUSP project suggest the two reservoirs could store up to 17,000 million tons of CO2. The WY-CUSP team drilled a stratigraphic test well and acquired a 3-D seismic survey covering 25 square miles of the Rock Springs Uplift site. The team retrieved 916 feet of core from the 12,810-foot-deep well, along with a complete log suite, borehole images, fluid samples, and other data. Project partners (1) provided continuous visual documentation of the core, including grain size, mineralogy, facies distribution, and porosity; (2) performed continuous permeability and velocity scans of selected reservoir intervals; and (3) chemically analyzed the fluid samples. WY-CUSP scientists integrated seismic attributes with observations from log suites, a VSP survey, core, fluid samples, and laboratory analyses, including continuous permeability scans. From these integrations, researchers constructed 3-D spatial distribution volumes of reservoir and seal properties that represent geological heterogeneity at the targeted CO2 storage site. The WY-CUSP team used this data to perform new CO2 plume migration simulations. Baker Hughes, Inc., completed a series of small-scale, in-situ water injectivity measurements. A database was formed when observations, analyses, and experiments from the stratigraphic test well were integrated. Correlation of these data allowed petrophysical parameters to be extrapolated from the test well out into the storage domain (5x5 mile 3-D seismic survey volume). This resulted in an improved, realistic understanding of performance assessments for potential CO2 storage scenarios. The WY-CUSP team worked on (1) improving CO2 storage resource estimates, (2) establishing long-term integrity and permanence of confining layers, (3) designing a profitable strategy for pressure management, and (4) evaluating the utilization of stored CO2 at the Rock Spring Uplift. Finally, Baker Hughes developed a microseismic baseline for the test site using in-bore geophones to complete field operations.

3-D seismic↗

Impact of Standing Bleed Water on Saltstone Placement

The amount of water present during placement and subsequent curing of saltstone has the potential to impact several properties important for grout quality. An active drain water system can remove residual standing water and expose the surface of the placed saltstone to air. Oxidation of the saltstone may result in an increase in the leachability of redox sensitive elements. A dry surface can lead to cracking, causing an increase in hydraulic conductivity. An inactive drain water system can allow standing water that generates unnecessary hydrostatic head on the vault walls. Standing water that cannot be removed via the drain system will be available for potential incorporation into subsequent grout placements. The objective of this work is to study the impact of standing water on grout quality pertaining to disposal units. A series of saltstone mixes were prepared, and cured at ambient temperature to evaluate the impact of standing water on saltstone placement. The samples were managed to control drying effects on leachability by either exposing or capping the samples. The water to premix ratio was varied to represent a range of processing conditions. Samples were analyzed for density, leachability, and hydraulic conductivity. A monolith of each composition was cut into four sections to analyze the homogeneity of the sample with respect to vertical position within the sample. The density of each section was measured by two methods, helium pycnometry and by ASTM 642-06. The results show a trend of increasing density with increasing depth in the samples. This effect is more pronounced with the inclusion of excess bleed water and indicative of increased settling. The leachability of the eight different samples was analyzed by ANS/ANSI 16.1 method. These results indicate that drying of the saltstone during curing leads to decreased Leachability Indices (indicative of more release) for potassium, sodium, rhenium, nitrite, and nitrate. This may be caused by shrinkage cracking in the samples creating additional pathways for contaminant release. There was no noticeable effect on leachability by changing the water to premix ratio or by including excess bleed water. There was no detectable chromium release in any of the samples. Chromium and rhenium were added in equal amounts to determine whether rhenium might be an acceptable surrogate for chromium, a hazardous material. This testing shows no correlation between the behavior of the two elements, as chromium is not released at detectable levels and rhenium is released at a comparable rate to nitrate, the most prevalent and mobile species in saltstone.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗