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At least 199 records · Page 11

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NASA NTRS1978

Determination of oxygen in silicon and carbide by activation with 27.2 meV alpha particles

The Si sample was polished on one side, and on the other side Ni was applied chemically and soldered with Pb to a water cooled Cu substrate. Optical quartz standard was fixed from the other side. Si carbide samples were soldered to a substrated with In. The prepared samples were irradiated in a cyclotron with a 27.2 MeV alpha particle beam. The layers were removed from the Si and Si carbide samples by grinding and the positron activity of F-18(t sub 1/2 110 min) was measured by using a gamma, gamma coincidence spectrometer with two NaI(TI) crystals. For analysis of Si carbide, the activity decay curve of the samples was recorded to find the contribution of the positron activity of Cu-65(t sub 1/2 12.9 hr) which formed from Ni impurity on irradiation.

Dolgolenko, A. P.↗

DOE OSTI2021

Effects of short-term over-discharge cycling on the performance of commercial 21,700 lithium-ion cells and the identification of degradation modes

In this paper, short-term over-discharge cycling was performed on commercially available 21,700 lithium-ion cells to investigate its effects on cell performance; the degradation modes were also identified and analyzed in detail using both in-situ and ex-situ methods. Results show that observable capacity loss occurs when the cell is over-discharged to 112.5% depth of discharge. Moreover, the negative impact of the depth of discharge on cell performance (or cell aging) is more serious than the number of cycles, and continuous over-discharge cycling will accumulate such impact. The loss of Li inventory related to the decomposition and reformation of solid electrolyte interphase film is an important cause of the irreversible capacity loss/degradation of Li-ion cells during over-discharge cycling testing. Furthermore, the dissolution of copper current collector can greatly reduce the mechanical stability of the anode, and further, the deposition of Cu, the exfoliation and the cracking of active material particles can influence the transfer of ions and lead to the loss of Li inventory and the loss of active material within Li-ion cells. Additionally, when the depth of discharge exceeds 108.3%, deposition of Cu is observed on the ceramic-covered side of separators.

25 ENERGY STORAGE↗

DOE OSTI2024

Cloud Condensation Nuclei Particle Counter (CCN) Instrument Handbook

The Cloud Condensation Nuclei Counter—CCN (Figure 1) is a U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Climate Research Facility instrument for measuring the concentration of aerosol particles that can act as cloud condensation nuclei [1, 2]. The CCN draws the sample aerosol through a column with thermodynamically unstable supersaturated water vapor that can condense onto aerosol particles. Particles that are activated, i.e., grown larger in this process, are counted (and sized) by an Optical Particle Counter (OPC). Thus, activated ambient aerosol particle number concentration as a function of supersaturation is measured. Models CCN-100 and CCN-200 differ only in the number of humidifier columns and related subsystems: CCN-100 has one column and CCN-200 has two columns along with dual flow systems and electronics.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1974

The measurement of the size distribution of artificial fogs

The size-distribution of the fog droplets at various fog particle concentrations in fog chamber was determined by two methods: (1) the Stokes' velocity photographic method and (2) using the active scattering particle spectrometer. It is shown that the two techniques are accurate in two different ranges of particle size - the former in the radii range (0.1 micrometers to 10.0 micrometers), and the latter for radii greater than 10.0 micrometers. This was particularly true for high particle concentration, low visibility fogs.

Deepak, A.↗

DOE OSTI2023

Influence of electronic transport on electrochemical performance of (Cu,Mn) 3 O 4 solid oxide fuel cell cathodes

Alkaline Earth free spinel oxides provide a potential benefit over Sr-doped perovskite-based materials commonly used as electrodes in high-temperature electrochemical energy conversion devices, e.g., solid oxide fuel cells (SOFCs). Sr-segregation is a known issue leading to performance degradation. In this study, Cu x Mn 3-x O 4 (x = 1, 1.2, and 1.5) porous electrodes were examined as SOFC cathodes using electrochemical impedance spectroscopy to investigate the oxygen reduction reaction (ORR) kinetics in relation to the material's intrinsic conductivity, the extrinsic electrode structure, and the cell test design. Similar to the electronic conducting (La,Sr)MnO 3 SOFC cathodes, the ORR kinetics of Cu x Mn 3-x O 4 spinel electrodes was governed by the oxygen adsorption and diffusion at the particle surface as well as the charge transfer at the triple phase boundaries. The overall electrode polarization resistance was highly dependent on contact density with the metallic current collector, active material particle connectivity, electrode thickness, and the intrinsic electronic materials conductivity. Here, we describe the importance of effective electronic charge transport parallel to the electrode surface in maximizing the electrochemically active electrode volume and enhancing electrode performance. We discuss an approach to optimize cell and electrode design with respect to active materials properties. This aspect is critical to ensure reliable evaluation of new materials, since laboratory-scale button-cells typically exhibit a high degree of electrode microstructure (e.g. porosity, thickness) and electrical contact density variation from sample to sample.

(Cu,Mn)3O4↗

DOE OSTI2022

Nuclear and Chemical Sciences Division: Investment Strategy 2023

The mission of the Nuclear and Chemical Sciences (NACS) Division within the Physical and Life Sciences (PLS) Directorate is to advance scientific understanding, capabilities, and technologies in nuclear and particle physics, radiochemistry, forensic science, and isotope systems to support LLNL’s national security mission. NACS Division personnel conduct a diverse range of research activities in particle physics, nuclear physics, radiation detection, nuclear measurements, chemical and nuclear forensic science, nuclear and radiochemistry, isotope geochemistry, and environmental science. These areas are leveraged to address evolving national security challenges. Scientific research provides the foundation for addressing these challenges, and it is also the principal means of attracting, training, and retaining staff scientists who can deliver solutions across the Laboratory’s mission space. The overarching strategy is to position the NACS Division at the nexus between fundamental nuclear and chemical science research and nuclear security applications. This approach will support efforts to recruit, train, and retain top-flight scientists and engineers who will play a key role in executing the Laboratory’s core nuclear security missions, while also enhancing LLNL’s reputation as a center for innovative scientific research. This document describes the strategic vision that will be used to guide key investments aimed at enabling NACS scientists to lead new efforts and meet future challenges.

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2024

Hydrogen Spillover Is Regulating Minority Rh 1 Active Sites on TiO 2 in Room-Temperature Ethylene Hydrogenation

The complicated dynamics of active sites on single-atom catalysts under reducing conditions limits their applications in hydrogenation reactions and mechanistic understanding. Herein, we report that on Rh 1 /TiO 2 , *H spillover during room-temperature ethylene hydrogenation hydroxylates and reduces TiO 2 , enhancing the intrinsic activity of Rh 1 by 9-fold. Spectroscopic and kinetic evidence suggests that the spillover of *H is suppressed by their facile reaction with C 2 H 4 , most of the spilled *H are nonreactive spectators, and >99% turnovers occur on a small subset (<20%) of exposed “active Rh 1 ”. Steady-state kinetics indicates competitive adsorption between H and C 2 H 4 , H 2 dissociation is the rate-determining step, and the apparent activation barrier (E a,app ) of the reaction is ~48 kJ/mol. The evolution of Rh 1 under H 2 was further tracked by spectroscopic and microscopic techniques at elevated temperatures. At 200 °C, more Rh 1 are exposed, but these Rh 1 are at least 5-fold less active than that of the “active Rh 1 ”. At 300 °C, Rh clusters derived from Rh 1 become the main active sites, shifting E a,app to 62 kJ/mol, characteristic of Rh nanoparticles. At ≥400 °C, larger and more active Rh particles in the strong metal–support interaction state are created. In conclusion, this work revealed the unexpected regulation effects of *H spillover on M 1 active sites under ambient conditions, differentiated the minority active M 1 sites, and demonstrated how the stability of M 1 under reducing atmospheres affects hydrogenation catalysis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1993

Research in cosmic and gamma ray astrophysics: Cosmic physics portion

Research in particle astrophysics at the Space Radiation Laboratory (SRL) of the California Institute of Technology is supported under NASA Grant NAGW-1919. A three-year proposal for continuation of support was submitted a year ago and put into effect 1 October 1992. This report is the combined progress report and continuation application called for under the Federal Demonstration Project. Gamma-ray Astrophysics at SRL is separately supported under NAGW-1919 and will be separately summarized and proposed. This report will document progress and plans for our particle spectroscopy activities and for related data analysis, calibration, and community service activities. A bibliography and a budget will be attached as appendices. The Caltech SRL research program includes a heavy emphasis on elemental and isotopic spectroscopy of energetic particles in the cosmic radiation; in solar, interplanetary, and anomalous 'cosmic' radiation; and in planetary magnetospheres as discussed.

Stone, Edward C.↗

DOE OSTI2021

Nanowire-based hydrodesulfurization catalysts for hydrocarbon fuels

The present development is a metal particle coated nanowire catalyst for use in the hydrodesulfurization of fuels and a process for the production of the catalyst. The catalyst comprises titanium(IV) oxide nanowires wherein the nanowires are produced by exposure of a TiO2—KOH paste to microwave radiation. Metal particles selected from the group consisting of molybdenum, nickel, cobalt, tungsten, or a combination thereof, are impregnated on the metal oxide nanowire surface. The metal impregnated nanowires are sulfided to produce catalytically-active metal particles on the surface of the nanowires The catalysts of the present invention are intended for use in the removal of thiophenic sulfur from liquid fuels through a hydrodesulfurization (HDS) process in a fixed bed reactor. The presence of nanowires improves the HDS activity and reduces the sintering effect, therefore, the sulfur removal efficiency increases.

Sunkara, Mahendra Kumar↗

DOE OSTI2022

Nanowire-based hydrodesulfurization catalysts for hydrocarbon fuels

Sunkara, Mahendra K.↗

NASA NTRS1990

Particle injection and acceleration at earth's bow shock - Comparison of upstream and downstream events

The injection and acceleration of thermal solar wind ions at the quasi-parallel earth's bow shock during radial interplanetary magnetic field conditions is investigated. Active Magnetospheric Particle Tracer Explorers/Ion Release Module satellite observations of complete proton spectra, and of heavy ion spectra above 10 keV/Q, made on September 12, 1984 near the nose of the shock, are presented and compared to the predictions of a Monte Carlo shock simulation which includes diffusive shock acceleration. It is found that the spectral observations are in good agreement with the predictions of the simulation when it is assumed that all accelerated ions originate in the solar wind and are injected into the acceleration mechanism by thermal leakage from the downstream plasma. The efficiency, which is determined directly from the downstream observations, is high, with at least 15 percent of the solar wind energy flux going into accelerated particles. The comparisons allow constraints to be placed on the rigidity dependence of the scattering mean free path and suggest that the upstream solar wind must be slowed substantially by backstreaming accelerated ions prior to undergoing a sharp transition in the viscous subshock.

Ellison, Donald C.↗

DOE OSTI2024

Baselining the Indirect Effect by Improving Quantification of Sea Spray and Marine Sources at Ascension Island (Final Report)

Oceans cover two-thirds of the Earth and understanding the interactions of aerosols with clouds in these large marine regions requires quantifying the man-made contributions to the budget of cloud-drop forming particles (known as cloud condensation nuclei, or CCN) relative to the non-manmade “baseline” conditions and understanding the meteorology of boundary layer clouds. Modeling studies have shown substantial uncertainties and sensitivities to natural marine CCN sources, meaning that to reduce uncertainties in indirect effects we must be able to better quantify the CCN budget in ocean regions. While models provide important constraints on these uncertainties, actually reducing uncertainties requires substantial observations in open-ocean and coastal regions in order to establish the baseline on which manmade emissions are added. The tropical South Atlantic Ocean is one of the least-sampled regions of the planet, making the comprehensive measurements of the Department of Energy Atmospheric Radiation Measurement Layered Atlantic Smoke Interactions with Clouds (LASIC) campaign provides the longest record of aerosol size distribution measurements from a differential mobility analyzer in a cloud-influenced marine location in the ARM database, with 17 months of ground-based aerosol size distribution measurements. This project addressed the research topic of Aerosol-Cloud Interactions (ACI) by supporting three publications from the LASIC measurements: 1. The ARM measurements were combined with a new value-added technique that was pioneered by the Russell group for quantifying sea salt. This quantification of sea salt uses supermicron scattering measurements for retrieving reasonable sea spray mass concentrations, providing the best-available, observationally-constrained estimate of the sea spray mode properties when supermicron size distribution measurements are not available. 2. The fitted modes of the distribution were used to investigate the signatures of cloud processing for very clean to very smoky aerosol conditions, revealing not only differences in the particles that activate in clouds but also in the mechanisms that control that droplet formation process. In clean air, the size required to form a cloud droplet is influenced by the number of particles, as well as how quickly particles take up water during growth in cloud. 3. Building on this aerosol characterization, cloud and meteorological conditions were used to evaluate aerosol-related changes in cloud albedo and optical depth. We introduced a new method of decomposing the impact of aerosols on clouds known as the Twomey effect by incorporating retrieved supersaturation from two independent sets of observations to constrain the feedback of aerosol particles on cloud properties. The method quantifies the reduction of the Twomey effect at high aerosol concentrations, which has never been explained quantitatively by observations. In addition, the results provide the first direct validation for the conditions observed in the tropical South Atlantic of a parcel-based approach that is embedded in many climate models. Together these findings illustrate how ARM extended field campaigns in stratocumulus-covered regions can be used to constrain ACI processes with direct observations, providing specific radiative effects without models. By making such process-specific constraints available to improve ACI in global climate models, ARM observations play a key role in supporting model development.

58 GEOSCIENCES↗

NASA NTRS1994

Microphysical growth state of ice particles and large-scale electrical structure of clouds

Cloud temperature, liquid water content, and vertical air velocity are all considered in evaluating the microphysical growth state of ice phase precipitation particles in the atmosphere. The large-scale observations taken together with in situ measurements indicated that the most prevalent growth condition for large ice particles in active convection is sublimation during riming, whereas the most prevalent growth condition in stratiform precipitation is vapor deposition. The large-scale electrical observations lend further support to the idea that particles warmed by riming into sublimation charge negatively and particles in vapor deposition charge positively in collisions with small ice particles.

Williams, Earle↗

DOE OSTI2024

The Abundance and Sources of Ice Nucleating Particles Within Alaskan Ice Fog

Abstract The Alaskan Layered Pollution and Chemical Analysis (ALPACA) field campaign included deployment of a suite of atmospheric measurements in January–February 2022 with the goal of better understanding atmospheric processes and pollution under cold and dark conditions in Fairbanks, Alaska. We report on measurements of particle composition, particle size, ice nucleating particle (INP) composition, and INP size during an ice fog period (29 January–3 February). During this period, coarse particulate matter (PM 10 ) concentrations increased by 150% in association with a decrease in air temperature, a stronger temperature inversion, and relatively stagnant conditions. Results also show a 18%–78% decrease in INPs during the ice fog period, indicating that particles had activated into the ice fog via nucleation. Peroxide and heat treatments performed on INPs indicated that, on average, the largest contributions to the INP population were heat‐labile (potentially biological, 63%), organic (31%), then inorganic (likely dust, 6%). Measurements of levoglucosan and bulk and single‐particle composition corroborate the presence of dust and aerosols from combustion sources. Heat‐labile and organic INPs decreased during the peak period of the ice fog, indicating those were preferentially activated, while inorganic INPs increased, suggesting they remained as interstitial INPs. In general, INP concentrations were unexpectedly high in Fairbanks compared to other locations in the Arctic during winter. The fact that these INPs likely facilitated ice fog formation in Fairbanks has implications for other high latitude locations subject to the hazards associated with ice fog.

Meteorology & Atmospheric Sciences↗

DOE OSTI2021

Ice Nucleating Particle Connections to Regional Argentinian Land Surface Emissions and Weather During the Cloud, Aerosol, and Complex Terrain Interactions Experiment

Abstract Here, we present a multi‐season study of ice‐nucleating particles (INPs) active via the immersion freezing mechanism, which took place in north‐central Argentina, a worldwide hotspot for mesoscale convective storms. INPs were measured untreated, after heating to 95°C, and after hydrogen peroxide digestion. No seasonal cycle of INP concentrations was observed. Heat labile INPs, which we define as “biological” herein, dominated the population active at −5 to −20°C, while non‐heat‐labile organic INPs (decomposed by peroxide) dominated at lower temperatures, from −20 to −28°C. Inorganic INPs (remaining after peroxide digestion), were minor contributors to the overall INP activity. Biological INP concentration active around −12°C peaked during rain events and under high relative humidity, reflecting emission mechanisms independent of the background aerosol concentration. The ratio of non‐heat‐labile organic and inorganic INPs was generally constant, suggesting they originated from the same source, presumably from regional arable topsoil based on air mass histories. Single particle mass spectrometry showed that soil particles aerosolized from a regionally common agricultural topsoil contained known mineral INP sources (K‐feldspar and illite) as well as a significant organic component. The INP activity observed in this study correlates well with agricultural soil INP activities from this and other regions of the world, suggesting that the observed INP spectra might be typical of many arable landscapes. These results demonstrate the strong influence of regional continental landscapes, emitting INPs of types that are not yet well represented in global models.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

A new method for operating a continuous-flow diffusion chamber to investigate immersion freezing: assessment and performance study

Abstract. Glaciation in mixed-phase clouds predominantly occurs through the immersion-freezing mode where ice-nucleating particles (INPs) immersed within supercooled droplets induce the nucleation of ice. Model representations of this process currently are a large source of uncertainty in simulating cloud radiative properties, so to constrain these estimates, continuous-flow diffusion chamber (CFDC)-style INP devices are commonly used to assess the immersion-freezing efficiencies of INPs. This study explored a new approach to operating such an ice chamber that provides maximum activation of particles without droplet breakthrough and correction factor ambiguity to obtain high-quality INP measurements in a manner that previously had not been demonstrated to be possible. The conditioning section of the chamber was maintained at −20 ∘C and water relative humidity (RHw) conditions of 113 % to maximize the droplet activation, and the droplets were supercooled with an independently temperature-controlled nucleation section at a steady cooling rate (0.5 ∘C min−1) to induce the freezing of droplets and evaporation of unfrozen droplets. The performance of the modified compact ice chamber (MCIC) was evaluated using four INP species: K-feldspar, illite-NX, Argentinian soil dust, and airborne soil dusts from an arable region that had shown ice nucleation over a wide span of supercooled temperatures. Dry-dispersed and size-selected K-feldspar particles were generated in the laboratory. Illite-NX and soil dust particles were sampled during the second phase of the Fifth International Ice Nucleation Workshop (FIN-02) campaign, and airborne soil dust particles were sampled from an ambient aerosol inlet. The measured ice nucleation efficiencies of model aerosols that had a surface active site density (ns) metric were higher but mostly agreed within 1 order of magnitude compared to results reported in the literature.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Dynamics of Liquid–Liquid Phase Separation in Submicrometer Aerosol

Nanoscale materials, when compared to their bulk components, possess unique properties. In particular, shifts in phase transitions can occur for submicron particles. For instance, small particles do not undergo the process of liquid-liquid phase separation (LLPS). LLPS has applications in emulsions such as Janus particles, controllable morphology to create drug-rich phases during drug delivery, and is often observed in atmospheric aqueous aerosol particles. In atmospheric particles, LLPS is tracked as a function of particle water activity, which is equivalent to the relative humidity (RH) at equilibrium. We probed three organic/inorganic aerosol systems in the range of RH over which phase separation occurs (SRH). Our findings indicate that SRH for submicron aerosol particles is lower than for micron-sized droplets. These findings show that it may be necessary to update the representation of phase transitions in aerosol particles in climate models. The vast majority of organic/inorganic aerosol particles have submicron diameters, and a decrease in SRH for submicron particles indicates that the current estimation of phase separated aerosols may be overestimated. Furthermore, understanding the properties of LLPS at the nanoscale can provide key parameters to describe these systems and may lead to better control of phase separation in submicron particles.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

A new method for operating a continuous flow diffusion chamber to investigate immersion freezing: assessment and performance study

Glaciation in mixed-phase clouds predominately occurs through the immersion freezing mode where ice nucleating particles (INPs) immersed within supercooled droplets induce nucleation of ice. Currently, model representations of this process are a large source of uncertainty in simulating cloud radiative properties, and to constrain these estimates, continuous flow diffusion chamber (CFDC)-style INP devices are commonly used to assess the immersion freezing efficiencies of INPs. In this study, a new approach was explored to operating such an ice chamber that provides maximum activation of particles without droplet breakthrough and correction factor ambiguity to obtain high-quality INP measurements in a manner that has not been demonstrated as possible previously. The conditioning section of the chamber was maintained at ~ –20 °C and water relative humidity (RH w ) ~ 113 % conditions to maximize the droplet activation, and the droplets were supercooled with an independently temperature-controlled nucleation section at a steady cooling rate (0.5 °C min –1 ) to induce the freezing of droplets and evaporation of unfrozen droplets. The performance of the modified ice chamber was evaluated using four INP species: K-feldspar, illite-NX, Argentinian soil dust, and airborne arable dust that had shown ice nucleation over a wide span of supercooled temperatures. Dry dispersed and size-selected K-feldspar particles were generated in the laboratory. Illite-NX and soil dust particles were sampled during the second phase of the Fifth International Ice Nucleation Workshop (FIN-02) campaign, and airborne arable dust particles were sampled from the aerosol inlet located on the rooftop of the laboratory. The measured ice nucleation efficiencies of model aerosols with a surface active site density (n s ) metric were higher, but mostly agreed within one order of magnitude compared to literature results.

54 ENVIRONMENTAL SCIENCES↗