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DOE OSTI2022

Turbulent Flux Measurements of the Near‐Surface and Residual‐Layer Small Particle Events

Abstract According to recent field studies, almost half of the New Particle Formation (NPF) events occur aloft, in a residual layer, near the top of the boundary layer. Therefore, measurements of the meteorological parameters, precursor gas concentrations, and aerosol loadings conducted at the ground level are often not representative of the conditions where the NPFs take place. This paper presents new measurements obtained during the Turbulent Flux Measurements of the Residual Layer Nucleation Particles, conducted at the Southern Great Plains research site. Vertical turbulent fluxes of 3–10 nm‐sized particles were measured using a sonic anemometer and two condensation particle counters with nominal cutoff diameters of 3 nm and 10 nm mounted at the top of the 10‐m telescoping tower. Aerosol number size distribution (5–300 nm) was determined through the ground‐based Scanning Mobility Particle Sizers. The size selected (15–50 nm) particle hygroscopicity was derived with the Humidified Tandem Differential Mobility Analyzer. The ground level observations were supplemented by vertically‐resolved measurements of horizontal and vertical wind speeds and aerosol backscatter. The data analysis suggests that (a) turbulent flux measurements of 3–10 nm particles can distinguish between near‐surface and residual‐layer small particle events; (b) sub‐50 nm particles had a hygroscopicity value of 0.2, suggesting that organic compounds dominate atmospheric nanoparticle chemical composition at the site; and (c) current methodologies are inadequate for estimating the dry deposition velocity of sub‐10 nm particles because it is not feasible to measure particle concentration very near the surface, in the diffusion sublayer.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Critical Shear Stress for Erosion Under Laminar Jet Flow

Particle erosion is an important process in both natural and manmade environments. For example, in natural environments particle or sediment erosion rates determine the course of rivers, depth of streams, and fate of deltas. The interplay between erosion rates and flow patterns can have dramatic impact on shorelines. Where hydrodynamic jet flows or rip currents change direction, sediments may accumulate or disperse altering the shape of coastlines and the ecosystems and economies that rely on them. In man-made systems, jet flows may be used to mobilize particles from surfaces or within industrial scale mixing tanks. For example, in the nuclear industry, impinging jet mixers may be used to mobilize and suspend sludges at the bottom of waste tanks. In each of these examples, the Shields diagram is useful to determine the conditions under which erosion occurs. This diagram plots the scaled critical shear stress for erosion as a function of the particle size as embedded in particle Reynolds numbers, Archimedes numbers, or their equivalents. Although the data, that carries a large spread, is largely in agreement with mathematical models, for the smallest particles, model predictions diverge from each other and from experimental data. Indeed, there is substantial uncertainty about the Shields diagrams at relatively small particle sizes and flow rates. Here we evaluate critical shear stresses for erosion under laminar jet flow. To date critical shear stresses for erosion, as embodied in Shields diagrams, have largely been developed for turbulent flow both experimental and mathematically. However, curves on the Shields diagrams diverge among various models at lower particle Reynolds numbers. Indeed, how critical shear stresses for erosion develop under fully laminar jet flow conditions (not simply laminar boundary layers under turbulent flow) remains unclear. Here we address this gap, which is particularly important for mobilization of the smallest particles. We find the Shields parameter to be inversely proportional to the particle Reynolds numbers under laminar jet flow conditions similar to turbulent conditions.

critical shear stresses, erosion rates, effective ↗

DOE OSTI2019

Quantifying aerosol size distributions and their temporal variability in the Southern Great Plains, USA

A quality-controlled, 5-year dataset of aerosol number size distributions (particles with diameters (Dp) from 7 nm through 14 µm) was developed using observations from a scanning mobility particle sizer, aerodynamic particle sizer, and a condensation particle counter at the Department of Energy's Southern Great Plains (SGP) site. This data set was used for two purposes. First, typical characteristics of the aerosol size distribution (number, surface area, and volume) were calculated for the SGP site, both for the entire dataset and on a seasonal basis, and size distribution lognormal fit parameters are provided. While the median size distributions generally had similar shapes (four lognormal modes) in all the seasons, there were some significant differences between seasons. These differences were most significant in the smallest particles(Dp<30 nm) and largest particles (Dp>800 nm).Second, power spectral analysis was conducted on this long-term dataset to determine key temporal cycles of total aerosol concentrations, as well as aerosol concentrations in specified size ranges. The strongest cyclic signal was associated with a diurnal cycle in total aerosol number concentrations that was driven by the number concentrations of the smallest particles(Dp<30 nm). This diurnal cycle in the smallest particles occurred in all seasons in ~50% of the observations,suggesting a persistent influence of new particle formation events on the number concentrations observed at the SGP site. This finding is in contrast with earlier studies that suggest new particle formation is observed primarily in the springtime at this site. The timing of peak concentrations associated with this diurnal cycle was shifted by several hours depending on the season,which was consistent with seasonal differences in insolation and boundary layer processes. Significant diurnal cycles in number concentrations were also found for particles with Dp between 140 and 800 nm, with peak concentrations occurring in the overnight hours, which were primarily associated with both nitrate and organic aerosol cycles. Weaker cyclic signals were observed for longer timescales (days to weeks) and are hypothesized to be related to the timescales of synoptic weather variability. The strongest periodic signals (3.5–5 and 7 d cycles) for these longer timescales varied depending on the season, with no cyclic signals and the lowest variability in the summer.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2016

Nucleation and structural growth of cluster crystals

We study the nucleation of crystalline cluster phases in the generalized exponential model with exponent n = 4. Due to the finite value of this pair potential for zero separation, at high densities the system forms cluster crystals with multiply occupied lattice sites. Here, we investigate the microscopic mechanisms that lead to the formation of cluster crystals from a supercooled liquid in the low-temperature region of the phase diagram. Using molecular dynamics and umbrella sampling, we calculate the free energy as a function of the size of the largest crystalline nucleus in the system, and compare our results with predictions from classical nucleation theory. Employing bond-order parameters based on a Voronoi tessellation to distinguish different crystal structures, we analyze the average composition of crystalline nuclei. We find that even for conditions where a multiply occupied fcc crystal is the thermodynamically stable phase, the nucleation into bcc cluster crystals is strongly preferred. Furthermore, we study the particle mobility in the supercooled liquid and in the cluster crystal. In the cluster crystal, the motion of individual particles is captured by a simple reaction-diffusion model introduced previously to model the kinetics of hydrogen bonds.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2019

Mixing state evolution of agglomerating particles in an aerosol chamber: Comparison of measurements and particle-resolved simulations

This article introduces a validation study of the stochastic particle-resolved aerosol model PartMC with experimental data from an aerosol chamber experiment. For the experiment, a scanning mobility particle sizer and a single-particle soot photometer were used to monitor the aerosol mixing state evolution of two initially externally-mixed aerosol populations of ammonium sulfate and black carbon particles undergoing agglomeration. We applied an efficient optimization algorithm (ProSRS) to determine several unconstrained simulation parameters and were able to successfully reproduce number concentrations and size distributions of mixed particles that formed by agglomeration. The PartMC modeling method in conjunction with the optimization procedure provides a tool for detailed comparisons of chamber experiments and modeling, where aerosol mixing state is the focus of investigation.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Second ARM Aerosol Chemical Speciation Monitor Users’ Meeting Report

The aerosol chemical speciation monitor (ACSM) was developed to adapt the technology of the aerosol mass spectrometer (AMS) to routine, long-term, standalone monitoring. The calculation of particulate mass concentration from ACSM data requires the measurement of the response of the instrument to aerosol of specific size and composition as well as assumptions about the instrument response based on laboratory measurements and field experience acquired over more than two decades of operation of AMS and a decade of operation of the ACSM. Three parameters in the concentration calculations that are particularly important are the NO3 response factor (RFNO3), relative ionization efficiency (RIE), and the collection efficiency (CE). The values of RFNO3 and RIEs are determined from calibration, however the jump calibration method previously used in calibration can result in errors in the RIE for sulfate. This has been corrected by implementing a continuous calibration method. The default collection efficiency is 0.5. This has been shown to result in mass loadings that do not agree with mass determinations from other instruments because of effects of composition on the vaporization of the particles. The previous work of investigators addressing this issue is discussed. After preliminary work on ACSM and scanning mobility particle sizer (SMPS) data from the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) user facility Southern Great Plains (SGP) observatory collected in late 2016 and 2017 produced a parameterization of composition dependent collection efficiency very different from the results of previous studies, SMPS data were examined and we determined that there was significant mass that the instrument did not capture because the particles with diameters larger than 465 nm are not counted by this instrument. Data for the ultra-high-sensitivity aerosol spectrometer (UHSAS), SMPS, and ACSM are available for nearly all of 2019. The data from UHSAS and SMPS collected in 2019 were compared. We found that the UHSAS data has particle counts and total volumes significantly less than measured by the condensation particle counter (CPC) and SMPS. The SMPS data were extended by fitting the average volume distribution with a log normal curve and using this relationship to estimate a mass value for the SMPS over extended diameter range. The extended SMPS mass values result in a CDCE parameterization that is in better agreement with the results of other investigators, but is still different from other formulations. The working group recommends that the ACSM data be processed with a collective efficiency (CE)=1, that this be documented clearly in the metadata, and the use of the default CE of 0.5 or a formulation of composition-dependent collection efficiencies (CDCE) chosen by the user should be implemented based on the ammonium nitrate mass fraction. This is clearly necessary for the wintertime SGP ACSM data because of the high nitrate concentrations.

47 OTHER INSTRUMENTATION↗

DOE OSTI2026

Development of a Flow-through Cell for Ultrasonic Extraction (UE)─Single Particle (SP)─ICP-MS─an Approach for Nano/Microparticle Elemental and Isotopic Analysis

Nanotechnology is a salient part of the scientific landscape, and analytical approaches are rapidly evolving to enable small-scale characterization of nano- and microparticle compositions and impurities. Here, a flow-through sonicating cell was developed for direct particle extraction from a silicon wafer and integrated with an inductively coupled plasma–mass spectrometer (ICP-MS) for subsequent elemental and isotopic characterization of the released particles. Ultrasonic extraction (UE)─single particle (SP)─ICP-MS offers controlled particle mobilization from solid substrates and allows for increased sample throughput by eliminating the need for pre-extraction of particles and decreasing sample preparation steps. Coupling this device to an ICP-MS with a time-of-flight (TOF) mass analyzer, it is possible to distinguish unique isotopic compositions of the particles. Both tungsten and nickel isotopically tagged particles, which were deposited on Si wafers, are presented here with analysis via UE─SP─ICP-MS. This approach could support efforts in the fields of particle synthesis, nuclear safeguards and forensics, environmental monitoring, and semiconductor industries in which the detection of particles from substrates and wafers is critical.

Paul, Molly [ORNL] (ORCID:0009000009672055)↗

DOE OSTI2023

Biological toxicity and environmental hazards associated with PLGA nanoparticles

There have been tremendous advances in nanotechnology. More recently, the use of nanoparticles has expanded to applications including materials, packaging, energy, and medical uses such as drug delivery, diagnostics, and therapeutics. The American Society for Testing and Materials (ASTM) and the International Organization for Standardization (ISO) define nanoparticles as particles with at least one dimension measuring between 1 and 100 nm (2), but this view is generally too limited, and recommendations have been made to consider all materials with a dimension measuring under 1,000 nm as nanoparticles. The biomedical uses of nanoparticles are particularly promising because of their ability to reach and target various sites and organs. However, some nanoparticles can be composed of toxic materials or are limited by issues of biodistribution and bioaccumulation, which have hampered their use in biomedicine. The copolymer poly lactic-co-glycolic acid (PLGA) has gained use in biomedical applications as a delivery system because it is considered biocompatible and can be formulated with controlled degradation in physiological environments. PLGA has a history in biomedicine that dates to the 1970s when biodegradable sutures were developed using PLGA. In addition, the United States (US) Food and Drug Administration (FDA) and the European Medicine Agency (EMA) have approved various PLGA particle formulations as therapeutic delivery vehicles. Interest in biocompatible materials to deliver a range of therapeutic drugs, proteins, nucleic acids, and other molecules has risen recently. In addition to drug delivery, sustained drug release can be achieved by tuning the physical properties of PLGA, such as the molecular weight, ratio of lactic to glycolic acid, drug concentration, stabilizing molecules, and particle size. Given the rise of nanoparticles, human and environmental exposure to them is inevitable as more applications use free, unbound, and highly mobile particles. Although PLGA is generally considered safe, a detailed understanding of how PLGA and the other components used to help formulate this copolymer into a nanoparticle delivery vehicle is useful for assessing potential harmful effects. Despite recent advances in PLGA nanoparticle formulations, residual stabilizing molecules, inconsistent preparations, and batch-to-batch variations can lead to toxicity. Poor preparations of PLGA can lead to common mechanisms of toxicity observed with nanoparticles, such as inflammation and oxidative stress. Consistency in PLGA formulations and accurate methods to evaluate nanoparticle toxicity are needed to ensure safety. In order to better assess PLGA nanoparticles as non-toxic delivery systems, it is critical to understand their physical and chemical properties and the formulation protocols that may introduce toxic components into particles.

Biology, nanoparticle, toxicity↗

DOE OSTI2018

Theory of activated glassy dynamics in randomly pinned fluids

We generalize the force-level, microscopic, Nonlinear Langevin Equation (NLE) theory and its elastically collective generalization [elastically collective nonlinear Langevin equation (ECNLE) theory] of activated dynamics in bulk spherical particle liquids to address the influence of random particle pinning on structural relaxation. The simplest neutral confinement model is analyzed for hard spheres where there is no change of the equilibrium pair structure upon particle pinning. As the pinned fraction grows, cage scale dynamical constraints are intensified in a manner that increases with density. This results in the mobile particles becoming more transiently localized, with increases of the jump distance, cage scale barrier, and NLE theory mean hopping time; subtle changes of the dynamic shear modulus are predicted. The results are contrasted with recent simulations. Similarities in relaxation behavior are identified in the dynamic precursor regime, including a roughly exponential, or weakly supra-exponential, growth of the alpha time with pinning fraction and a reduction of dynamic fragility. However, the increase of the alpha time with pinning predicted by the local NLE theory is too small and severely so at very high volume fractions. The strong deviations are argued to be due to the longer range collective elasticity aspect of the problem which is expected to be modified by random pinning in a complex manner. A qualitative physical scenario is offered for how the three distinct aspects that quantify the elastic barrier may change with pinning. ECNLE theory calculations of the alpha time are then presented based on the simplest effective-medium-like treatment for how random pinning modifies the elastic barrier. The results appear to be consistent with most, but not all, trends seen in recent simulations. Key open problems are discussed with regard to both theory and simulation.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Transient pattern formation in an active matter contact poisoning model

Abstract One of the most notable features in repulsive particle based active matter systems is motility-induced-phase separation (MIPS) where a dense, often crystalline phase and low density fluid coexist. Most active matter studies involve time-dependent activity; however, there are many active systems where individual particles transition from living or moving to dead or nonmotile due to lack of fuel, infection, or poisoning. Here we consider an active matter particle system at densities where MIPS does not occur. When we add a small number of infected particles that can poison other particles, rendering them nonmotile, we find a rich variety of time dependent pattern formation, including MIPS, a wetting phase, and a fragmented state formed when mobile particles plow through a nonmotile packing. We map the patterns as a function of time scaled by epidemic duration, and show that the pattern formation is robust for a wide range of poisoning rates and activity levels. We also show that pattern formation does not occur in a random death model, but requires the promotion of nucleation by contact poisoning. Our results should be relevant to biological and active matter systems where there is some form of poisoning, death, or transition to nonmotility.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2020

Perpendicular magnetofluid theory for magnetically confined plasmas in the collisionless limit

Note that the magnetically confined plasmas in thermonuclear fusion turn to be collisionless. Some particles are trapped by the inhomogeneous equilibrium field or by the waves, while some others keep circulating. One cannot expect the charged particles to be collectively localized in space by collisions along the magnetic field lines. Consequently, the fluid parameters relating to the parallel motion, such as parallel fluid velocity, become inadequate. In this paper, the perpendic- ular magnetofluid theory for magnetically confined plasmas in the collisionless limit is developed. It revises Braginskii’s transport theory by releasing the collisional dominance assumption. In the perpendicular direction, the particle spatial localization is solo resulted from the strong magnetic field, while the finite Larmor radius (FLR) effects are taken into account in the next order. In the parallel direction, the particle mobility feature is fully retained by constructing only the per- pendicular moments. Therefore, besides the FLR effects till order O($k$ $^{2}_{⊥}$ $ρ$ $^{2}_{i}$ ), the Landau damping, the trapped particle effects, and other parallel kinetic effects are all kept in the current formalism. Here, k ⊥ is the perpendicular wave number and ρ i is the ion Larmor radius. Here, the theory can be used both for the analytical and numerical studies of magnetically confined plasmas.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2020

Reactive particle-tracking solutions to a benchmark problem on heavy metal cycling in lake sediments

Geochemical systems are known to exhibit highly variable spatiotemporal behavior. This may be observed both in non-smooth concentration curves in space for a single sampling time and also in variability between samples taken from the same location at different times. However, most models that are designed to simulate these systems provide only single-solution smooth curves and fail to capture the noise and variability seen in the data. We apply a recently developed reactive particle-tracking method to a system that displays highly complex geochemical behavior. When the method is made to most closely resemble a corresponding Eulerian method, in its unperturbed form, we see near-exact match between solutions of the two models. More importantly, we consider two approaches for perturbing the model and find that the spatially-perturbed condition is able to capture a greater degree of the variability present in the data. This method of perturbation is a task to which particle methods are uniquely suited and Eulerian models are not well-suited. Additionally, because of the nature of the algorithm, noisy spatial gradients can be highly resolved by a large number of mobile particles, and this incurs negligible computational cost, as compared to expensive chemistry calculations.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2015

Reaction of Chlorine Molecules with Unsaturated Submicron Organic Particles

Here, the reaction of closed shell Cl 2 molecules with sub-micron droplets composed of unsaturated molecules, oleic acid (OA), linoleic acid (LA), linolenic acid (LNA), or squalene (Sqe), are investigated in an atmospheric pressure flow tube reactor in conjunction with a vacuum ultraviolet photoionization aerosol mass spectrometer and a scanning mobility particle sizer. Cl 2 is found to react with all particles, and the reactive uptake coefficients depend on the number of unsaturated reaction sites, e.g., γ Cl2 Sqe = (0.66 ± 0.03) × 10 –4 versus γ Cl2 OA = (0.23 ± 0.01) × 10 –4 . In addition, the chemical evolution of squalene and its chlorinated products reveal that the reaction becomes slower for higher chlorinated products.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2018

Summertime Aerosol across the North Slope of Alaska Field Campaign Report

The Summertime Aerosol across the North Slope of Alaska U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Climate Research Facility field campaign, a collaborative effort between the University of Michigan and Baylor University, was focused on chemically characterizing sources of summertime aerosol impacting the Utqiagvik (Barrow, NSA) and the Oliktok Point (AMF3) ARM sites. This campaign was co-funded by a grant from the National Oceanic and Atmospheric Administration (NOAA, PI: Kerri Pratt, Co-I: Rebecca Sheesley) titled “Assessment of Atmospheric Aerosols Resulting from Oil and Gas Extraction Activities near the North Slope of Alaska”. The ARM field campaign took place on the North Slope of Alaska (NSA) from August 21 to September 30, 2015 and August 12 to September 20, 2016, with filter sampling occurring both years at both the NSA Barrow and AMF3 Oliktok Point sites. Online intensive measurements occurred at Barrow in 2015 and at Oliktok Point in 2016, coordinated with the arrival of the ARM Aerosol Observing System (AOS) in August 2016 at Oliktok Point. During 2015, the University of Michigan deployed the newly constructed aerosol time-of-flight mass spectrometer (ATOFMS), as well as a microanalysis particle sampler (MPS) to collect particles for offline analysis by computer-controlled scanning electron microscopy with energy-dispersive x-ray spectroscopy (CCSEM-EDX). Unfortunately, an issue with the time-of-flight mass spectrometer on the ATOFMS limited the number of particles that produced mass spectra during the 2015 study. This issue was subsequently fixed for the 2016 deployment. During 2016, the ATOFMS was deployed to the AMF3 at the Oliktok Point field site, in addition to a micro-orifice uniform deposition impactor (MOUDI) to collect particles for offline analysis by CCSEM-EDX. Notably, these measurements, to our knowledge, represent the first real-time, single-particle chemical characterization (aerosol mixing state) measurements at Utqiagvik and Oliktok Point. Online aerosol measurements also included: PM2.5 (particulate matter <2.5 μm) black carbon mass concentrations (aethalometer; Baylor) and size-resolved (0.013-20 μm) number concentrations (scanning mobility particle sizer, SMPS, and aerodynamic particle sizer, APS; Michigan). Baylor conducted filter sampling at both the Utqiagvik and Oliktok Point locations during both intensive operational periods (IOPs). Baylor deployed a total suspended particulate matter (TSP) sampler to Oliktok Point, and continuous one-week samples were collected in 2015 for a total of seven samples; during 2016, continuous 3-7 day samples were collected, for a total of 13 filters. Baylor deployed a TSP sampler and a PM1.0 sampler at Utqiagvik, Alaska; continuous 4-7 day filter samples were collected in 2015 for a total of eight samples. To supplement this campaign, PI Sheesley had a simultaneous DOE ARM field campaign at Utqiagvik and Oliktok Point (https://www.arm.gov/research/ campaigns/amf2016bbc), the goal of which was to collected continuous one-week TSP samples at both sites from June 2016 to September 2017. These results provide better context in terms of annual trends and for year-to-year variability and a final report with data was already submitted by PI Sheesley for that project. Analysis by Baylor focuses on TSP samples because of the extremely low PM loading on the PM1.0 sampler. Michigan deployed a three-stage impactor (0.07-5 μm PM collection) at Utqiagvik and a 10-stage impactor (0.056-10 μm PM collection) at Oliktok Point, during the 2015 and 2016 campaigns, respectively.

Arctic processes, North Slope of Alaska, Barrow, O↗

NASA NTRS1996

A proof of concept investigation: A unique mobility spectrometer for In Situ diagnostics of positive and negative ion distributions in the mesosphere and lower ionosphere

We have carried out a proof-of-concept development and test effort that not only promises the reduction of parasitic effects of surface contamination (therefore increasing the integrity of 'in situ' measurements in the 60-130 km regime), but promises a uniquely expanded measurement set that includes electron densities, plasma conductivities, charged-particle mobilities, and mass discrimination of positive and negative ion distributions throughout the continuum to free-molecular-flow regimes. Three different sensor configurations were designed, built and tested, along with specialized driving voltage, electrometer and channeltron control electronics. The individual systems were tested in a variety of simulated space environments ranging from pressures near the continuum limit of 100 mTorr to the collisionless regime at 10(exp -6) Torr. Swept modes were initially employed to better understand ion optics and ion 'beam' losses to end walls and to control electrodes. This swept mode also helped better understand and mitigate the influences of secondary electrons on the overall performance of the PIMS design concept. Final results demonstrated the utility of the concept in dominant single-ion plasma environments. Accumulated information, including theoretical concepts and laboratory data, suggest that multi-ion diagnostics are fully within the instrument capabilities and that cold plasma tests with minimized pre-aperture sheath acceleration are the key ingredients to multi-ion success.

Szuszczewicz, Edward P.↗

NASA NTRS1995

The Effect of Altitude Conditions on the Particle Emissions of a J85-GE-5L Turbojet Engine

Particles from a J85-GE-5L turbojet engine were measured over a range of engine speeds at simulated altitude conditions ranging from near sea level to 45,000 ft and at flight Mach numbers of 0.5 and 0.8. Samples were collected from the engine by using a specially designed probe positioned several inches behind the exhaust nozzle. A differential mobility particle sizing system was used to determine particle size. Particle data measured at near sea-level conditions were compared with Navy Aircraft Environmental Support Office (AESO) particle data taken from a GE-J85-4A engine at a sea-level static condition. Particle data from the J85 engine were also compared with particle data from a J85 combustor at three different simulated altitudes.

Rickey, June Elizabeth↗

DOE OSTI2025

Morphological Characterization of Uranyl Fluoride Particles via Atomic Force Microscopy

Uranium hexafluoride (UF 6 ) undergoes a rapid hydrolysis reaction when exposed to atmospheric water. In addition to producing hazardous HF gas, the hydrolysis reaction produces uranyl fluoride (UO 2 F 2 ), a radioactive solid phase particulate material. Because of the technological utility of UF 6 in the nuclear fuel cycle, understanding the transport properties of UO 2 F 2 aerosol produced via UF 6 hydrolysis is important for accident scenarios. Moreover, the fundamental chemical and physical properties of the UF 6 hydrolysis reaction are not completely understood. Recently, several experiments on the aerosol phase properties of UO 2 F 2 produced in this way have shown that under most relevant conditions, the particle size distribution (PSD) of UO 2 F 2 can be extremely small, approximately 3 to 5 nm, which is well below the threshold that can be routinely observed via scanning electron microscopy (SEM). Although readily observable in the aerosol phase, observation of nanometer-sized particles in the condensed phase (i.e. deposited on surfaces) remains a challenge. Here, in this study, we have used atomic force microscopy (AFM) to study the PSD and morphological characteristics of UO 2 F 2 deposited at low and high concentrations under different humidity conditions, a primary variable in the hydrolysis reaction. Here, we find strong agreement between PSD measured in the aerosol phase via scanning mobility particle sizing and PSD measured via AFM, with particle sizes peaked below 4 nm for low-humidity conditions. At higher humidity, the distribution is centered around 5 to 10 nm but extends up to 20 nm. These results are in stark contrast to previous measurements using SEM that show PSD on the order of 300- to 1000-nm particle sizes; moreover, these are the first direct measurements of individual particles of UO 2 F 2 having been produced via UF 6 hydrolysis deposited on surfaces. These measurements, therefore, open a new avenue for collecting and detecting UO 2 F 2 in the condensed phase and further refine the PSD, which is critical for environmental transport determinations.

Uranium hexafluoride↗

DOE OSTI2025

Tuning transition metal nanoparticles on a non-traditional support via experimental design

The ability to control metal nanoparticle size and morphology on supported catalysts is crucial for optimizing catalytic performance in targeted applications. Here, this work presents a systematic approach for tuning Ni particle and crystallite size on an unconventional, low-porosity silica fume support through select thermal treatments. The catalyst was synthesized via the deposition of nickelocene onto silica fume, resulting in well-dispersed Ni nanoparticles. A face-centered central composite design was employed to systematically assess the effects of time, temperature, and sintering gas environment on metal particle growth. The results demonstrate that the sintering gas environment is the primary factor governing particle and crystallite evolution, with temperature as the next most significant influence. Nickel nanoparticles sintered at temperatures of 650 °C and above under inert conditions exhibited substantial growth and polycrystalline structures, whereas samples treated in oxidative environments formed NiO, restricting particle mobility. Minimally oxidative (500 ppm O₂) environments facilitated rapid sintering while effectively removing residual ligands from the one-step nickelocene deposition process. Extensive structural characterization via a combination of scanning transmission electron microscopy, X-ray diffraction, hydrogen temperature programmed reduction, and small-angle X-ray scattering revealed that oxidative treatments enhanced metal-support interactions, as evidenced by increased reduction temperatures and narrower particle size distributions. These findings establish quantitative relationships between sintering parameters and Ni nanoparticle characteristics, providing a framework for rational catalyst design through controlled thermal treatments. This methodology is broadly applicable to other catalytic systems and provides a quantitative foundation for catalyst design.

CVD↗