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At least 91 records · Page 5

Aerosol Activation in Radiation Fog at the Atmospheric Radiation Program Southern Great Plains Site

Environmental supersaturation is a key parameter in the formation of fog and clouds, yet it cannot be measured directly and must be inferred. Calculating the ambient supersaturation in fog requires knowledge of the aerosol hygroscopicity as well as particle size distribution, and relatively few values have been reported in the literature. Here we use κ-Köhler theory to derive aerosol activation properties based on particle hygroscopicity and dry particle size distributions, and then estimate the effective peak supersaturation during eight cases of radiative fog at the Southern Great Plains site in rural north-central Oklahoma, USA. The mean hygroscopicity parameter κ of particles likely to act as cloud condensation nuclei varied from 0.14 to 0.43. Ambient effective peak supersaturation during the fog episodes was between 0.01%–0.07%, with most values below 0.04%. Furthermore, the minimum 50% dry activation diameter generally ranged between 300–400 nm with little activation of particles with diameters below 300 nm.

54 ENVIRONMENTAL SCIENCES↗

Characterization of Virgin, Re-used, and Oxygen-reduced Copper Powders processed by the Plasma Spheroidization Process

We report that fabrication of parts with high mechanical properties heavily depend on the quality of powder deployed in the fabrication process. Copper powder in three different powder types were spheroidized using radio-frequency inductively coupled plasma (ICP) spheroidization process (TekSphero-15 system). The characterized powders include virgin powder as purchased from the powder manufacturer, powder used in electron beam powder bed fusion (EB-PBF) process, and reconditioned powder, which was used powder that underwent an oxygen-reduction treatment. The goal of spheroidizing these powder types was to evaluate the change in powder morphology, the possibility of enhancing the powder properties back to their as-received conditions, and assess oxygen reduction of the powder lots given their initial oxygen contents. Also, to investigate the impact of re-spheroidization on powder properties, the second round of spheroidization was performed on the already used-spheroidized powder. The impact of powder type on powder sphericity and particle size distribution was evaluated using the image analysis of scanning electron microscope (SEM) micrographs and laser diffraction, respectively. The spheroidized powder showed higher sphericity and more uniform particle size distribution overall. Depending on the powder collection bin, second round of spheroidization affected the powder sphericity differently. The possibility of deploying the plasma spheroidization process as an alternative oxygen-reduction technique was also investigated through tracking the powders’ oxygen content using inert gas fusion method before and after the spheroidization. The plasma spheroidized powder showed less oxygen content than the hydrogen-treated powder. The second round of spheroidization caused no change in oxygen content. The correlation between oxygen-reduction and created cracks was discussed and compared between plasma spheroidization and hydrogen-treatment. The plasma spheroidization process created a powder with higher sphericity, uniform particle size, and less oxygen content.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

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Merged aerosol particle size distributions for the Aerodynamic Particle Sizer (APS) and Scanning Mobility Particle Sizer (SMPS) instruments with Machine Learning Quality Checks Applied

54 ENVIRONMENTAL SCIENCES↗

TGA Study of the Reaction Kinetics of a CuFeMnAlO 4+δ Oxygen Carrier for Methane Chemical Looping Combustion under High Pressure and Atmospheric Pressure Conditions

Reduction and oxidation kinetics of a CuFeMnAlO 4+δ oxygen carrier for methane were studied using an atmospheric thermogravimetric analyzer (TGA) and a pressurized TGA. Important parameters such as temperature (500–900 °C), particle size distribution (150–650 μm), and partial pressures of reactants (methane and oxygen) were evaluated. Results showed that the reduction of the oxygen carrier was not affected by particle size distribution studied in this work, and that above 750 °C, the effect of the temperature on oxygen carrier reduction started to diminish. The reaction time approaches an asymptotic limit as methane partial pressure increases. For oxygen carrier oxidation, it was found that the rate of oxidation increased with increasing oxygen concentration. The effect of the oxygen concentration was more noticeable when the oxygen concentration was below 7.5%. Because of the inherent feature of the oxygen carrier, its chemical looping with oxygen uncoupling property was also assessed. A phase boundary-controlled shrinking sphere model was used to model the test data from the TGAs. Modeling results showed that the oxygen carrier reduction had a reaction order of 1 with an activation energy of ∼46 kJ/mol. Oxygen carrier oxidation demonstrated a reaction order of 1.1 with an activation energy of ∼55 kJ/mol. Additionally, the differences of the experimental results between the atmospheric pressure TGA and the pressurized TGA were discussed in detail and the limitations of the pressurized TGA were highlighted.

Hydrocarbons↗

Cesium Removal and Hydraulic Performance Comparisons of CST Ion Exchange Media Batches in Support of the Tank Closure Cesium Removal Project - 20522

Three batches of Crystalline Silicotitanate (CST) ion exchange media have been evaluated for cesium removal efficiency from a Savannah River Site (SRS) High Level Waste (HLW) supernate simulant in support of the Tank Closure Cesium Removal (TCCR) Project, which involves at-tank column waste treatment. Results will be utilized to select the CST media batch to be added to the next TCCR unit columns. Two of the CST media samples were recent production batches and the third was an archived batch studied extensively at SRS nearly two decades ago. The archived CST batch had a significantly smaller average particle diameter than more recent batches. Small-scale (∼23 mL), side-by-side column tests were conducted at 35 deg. C with each of the CST batches using the same simulant at flow rates near 1.2 mL/min (3.0-3.4 CST bed volumes/hr). The cesium ion exchange column performance results were lower than expected for all three CST batches, but the data indicated that 30% more simulant volume and 40% more equivalent CST bed volumes of solution can be processed with the older CST batch prior to reaching the 50% cesium breakthrough point than can be processed with the newer CST batches. Hydraulic evaluations of the CST columns were also conducted in simulant at 24 deg. C to determine the impact of the different particle size distributions and associated bed porosities on frictional pressure drop under dynamic flow conditions. Higher differential pressure drops were observed with the archived CST batch relative to recent production batches, due to the smaller particle size distribution and the packing characteristics of the archived batch. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Portable Optical Particle Spectrometer aboard an Airborne Platform (POPS_AIR) Instrument Handbook

The U.S. Department of Energy Atmospheric Radiation Measurement (ARM) user facility portable optical particle spectrometer (POPS) is a lightweight particle spectrometer designed for aerosol particle size distribution measurement. Several POPS of different versions have been procured to serve as routine instruments for the ARM Aerial Facility (AAF) unmanned aerial systems (UAS) and tethered balloon system (TBS) deployment since 2018. POPS measures the aerosol particle size distribution approximately between 0.13 and 3 μm.

54 ENVIRONMENTAL SCIENCES↗

U Metal Oxidation with Steam (U)

The Savannah Rive National Laboratory 9SRNL) is evaluating a method to produce uranium oxide (UO 2 ) from uranium metal using steam. The typical methods for making UO 2 yield powders with particle-size ranges of 1 to 50 micron. The goal of the steam oxidation is to produce a depleted uranium (DU) product with a larger particle size that can be used as a surrogate for testing physical and mechanical process techniques to refine uranium and/or plutonium bearing residues. Several studies in the literature indicated that reactions between uranium metal and steam will yield UO 2 as fine powders in the 160 to 500 °C range, but granular materials form above 500°C. Above 880 °C, a hard compact scale forms on the U metal. Furthermore, sintering of UO 2 occurs at about 1300 °C, but it has been stated that the presence of steam enhances the sintering characteristics of UO 2 . Initial studies into the oxidation of DU metal in an atmosphere of argon and steam have been completed. Oxidation of depleted uranium metal in Ar/steam at 600, 710, 700, and 830 °C yielded at UO 2 product with little or no impurity at each temperature. Although not enough sample was available to perform sieve analysis for particle size distribution, SEM images reveal that a significant volume fraction of the products at 710, 770, and 830 °C exceeds 100 microns. The material produced at 600 °C was too fine for programmatic needs. Questions associated with the UO 2 include morphology of product, mechanical strength of the particles, and performance in milling operations. The size of the samples produced in these tests did not allow for quantitative assessment of particle size of mechanical strength. A qualitative assessment of the particles formed at 710, 770, and 830 °C was that the samples produced at 710 and 770 °C were friable, and the sample produced 830 °C had more mechanical strength. Sintering of the samples in Ar/steam at 970 °C appeared to increase the strength of the particles without changing their general particle size characteristics. Due to the small sample sizes, the increase in strength could not be quantified. If the sintering at 970 °C is inadequate, higher sintering temperatures in Ar/steam can be evaluated. Future work will increase scale of the steam oxidation conditions which yield the most-favorable particle-size distributions with sufficient mechanical strength for programming usage. Further consideration will be given to oxidation temperature, steam addition to the reaction vessel, U metal pretreatment, and sintering conditions after oxidation. The UO 2 production could involve a two-step process where particles are formed in steam at lower temperatures (700-850 °C) and then sintered in Ar/steam at elevated temperatures (950-1200 °C). Larger samples (50-100 g each) will provide sufficient UO 2 product for sieve analysis and assessment of mechanical strength relatives to subsequent milling operations.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Estimating reaction parameters in mechanism-enabled population balance models of nanoparticle size distributions: A Bayesian inverse problem approach

In order to quantitatively predict nano- as well as other particle-size distributions, one needs to have both a mathematical model and estimates of the parameters that appear in these models. Here, we show how one can use Bayesian inversion to obtain statistical estimates for the parameters that appear in recently derived mechanism-enabled population balance models (ME-PBM) of nanoparticle growth. The Bayesian approach addresses the question of “how well do we know our parameters, along with their uncertainties?.” The results reveal that Bayesian inversion statistical analysis on an example, prototype $\mathrm{lr(0)_n}$ nanoparticle formation system allows one to estimate not just the most likely rate constants and other parameter values, but also their SDs, confidence intervals, and other statistical information. Moreover, knowing the reliability of the mechanistic model's parameters in turn helps inform one about the reliability of the proposed mechanism, as well as the reliability of its predictions. Importantly, the paper can also be seen as a tutorial with the additional goal of achieving a “Gold Standard” Bayesian inversion ME-PBM benchmark that others can use as a control to check their own use of this methodology for other systems of interest throughout nature. Overall, the results provide strong support for the hypothesis that there is substantial value in using a Bayesian inversion methodology for parameter estimation in particle formation systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Polarimetric Radar Variables in Snowfall at Ka- and W-Band Frequency Bands: A Comparative Analysis

Dual-frequency millimeter-wavelength radar observations in snowfall are analyzed in order to evaluate differences in conventional polarimetric radar variables such as differential reflectivity (ZDR) specific differential phase shift (K DP ) and linear depolarization ratio (LDR) at traditional cloud radar frequencies at Ka and W bands (~35 and ~94 GHz, correspondingly). Low radar beam elevation (~5°) measurements were performed at Oliktok Point, Alaska, with a scanning fully polarimetric radar operating in the horizontal–vertical polarization basis. This radar has the same gate spacing and very close beam widths at both frequencies, which largely alleviates uncertainties associated with spatial and temporal data matching. It is shown that observed Ka- and W-band Z DR differences are, on average, less than about 0.5 dB and do not have a pronounced trend as a function of snowfall reflectivity. The observed Z DR differences agree well with modeling results obtained using integration over nonspherical ice particle size distributions. For higher signal-to-noise ratios, KDP data derived from differential phase measurements are approximately scaled as reciprocals of corresponding radar frequencies indicating that the influence of non-Rayleigh scattering effects on this variable is rather limited. This result is also in satisfactory agreement with data obtained by modeling using realistic particle size distributions. Observed Ka- and W-band LDR differences are strongly affected by the radar hardware system polarization “leak” and are generally less than 4 dB. Smaller differences are observed for higher depolarizations, where the polarization “leak” is less pronounced. Realistic assumptions about particle canting and the system polarization isolation lead to modeling results that satisfactorily agree with observational dual-frequency LDR data.

42 ENGINEERING↗

ADVANCED TECHNIQUES FOR ENERGY INPUT REDUCTION IN GYPSUM WALLBOARD DRYING

Gypsum has been used for thousands of years in building and construction applications, starting with the pyramids in ancient Egypt, to “Plaster of Paris” in the midcenturies, and to the now-ubiquitous drywall in modern-day houses. Production of gypsum drywall boards takes several steps with high energy and water consumption. The current state of the art in industry is a process that begins by mining gypsum and reducing its particle size by milling. These gypsum particles undergo calcination to convert the gypsum (calcium sulfate dihydrate) into stucco (calcium sulfate hemihydrate). The stucco is mixed with additives and enough water to form a slurry that can be poured onto a conveyor belt and molded into the desired geometry. The stucco reacts with the water, converting back into gypsum. The remaining water is then dried from the board to form the final product. While only ~20 wt. % of water is needed for the conversion of stucco to gypsum, significant excess water is needed to ensure sufficient fluidity of the slurry for processibility. This is due to the low quality of the stucco particles produced in high throughput calcination units, which disintegrate upon mixing with water, thereby reducing the fluidity and processability of the slurry. This project aims to produce high-quality stucco particles by dielectric calcination. In doing so, particle integrity can be maintained through the slurry formulation step, and particle size distribution of the stucco can be adjusted to increase fluidity with less excess water. With less water remaining unreacted in the board, significant energy can be saved in drying the product. The project aims to 1) develop a dielectric calcination method to TRL 3, 2) determine optimal and practical particle size distributions to minimize excess water in the slurry, and 3) reduce the energy consumption of the drying process.

Conforti, Kameron↗

A novel flow cell for optical particle analyzers—application to measurements of Malvern Insitec under high pressure and temperature

A flow cell is a necessary measurement interface for some important optical analyzers. In our application of the flow cell, we utilize a state-of-the-art optical analyzer (Malvern Insitec) to measure particle size distribution and concentration in-situ in a sampled flow from a novel pressurized oxygen-fuel combustion process. However, since this sampling flow is a flow of moist flue gas under high temperature and pressure, and the flow contains particles and corrosive acid gases, it is an extreme challenge to obtain a flow cell with a high optical quality that does not perturb the measurement. To address this challenge, we propose a new design for an optical flow cell. By using a unique flow field in the proposed flow cell, the measurement zone can be well defined by the sampling flow, minimizing the influence of purge flow. To demonstrate this flow cell, we have built a test system, and conduct measurements utilizing polydisperse-particle standards (10-100 µm and 1-10 µm). The results reveal that the optical windows are well protected by the purge flow field, without risk of deposition from the sampling flow, and the Malvern Insitec can measure the particle size distribution by using this flow cell, without generating sample bias.

Cheng, Mao↗

Prognostic simulations of mixed-phase clouds with model AC-1D v1.0: the impact of aerosol types and freezing parameterizations on ice crystal budgets

Mixed-phase clouds at high latitudes contribute to the uncertainty in predicting cloud feedbacks and climate sensitivity, mainly due to the complexity of microphysical processes that influence the partitioning between the supercooled liquid and ice phases, and hence, cloud radiative effects on regional scales. Particularly in Arctic mixed-phase clouds, the activation of ice-nucleating particles (INPs) from various aerosol populations remains a leading source of uncertainty. We developed an aerosol-cloud one-dimensional (AC-1D) model, which provides a novel framework to prognostically treat INP and ice crystal budgets while explicitly accounting for polydisperse and multicomponent aerosol that activate INPs following different freezing parameterizations. The AC-1D model is informed by large-eddy simulations to probe the impact of INP representation on predicted ice crystal number concentrations (N i ) and ice crystal budgets in mixed-phase Arctic stratus. We apply three immersion freezing (IMF) parameterizations, two time-independent (singular) and one time-dependent (classical nucleation theory), to predict the evolution of the INP reservoir and resulting ice crystal budget from polydisperse mineral dust, organic (humic-like substances), and sea spray aerosol particle size distributions. Our analysis focuses on how variations in aerosol number concentration and cloud system parameters such as cloud cooling rate, cloud-top entrainment rate, and ice crystal fall speed influence the INP reservoir and ice crystal budgets. Furthermore, this study investigates the competitive ice nucleation dynamics in mixed aerosol environments and provides a process-level quantification of the INP budget terms, which directly controls ice crystal budgets. For all studied case scenarios, the aerosol types and associated particle size distributions significantly impact INP and N i , and the choice between a time-dependent and a singular freezing description yields orders-of-magnitude differences in the predicted INP and N i over the 10 h simulation time, reflecting typical cloud lifetimes. Our results show that the influence of cloud cooling, INP entrainment, and sedimentation varies significantly depending on the chosen freezing parameterization. These findings underscore the critical need for robust IMF parameterizations and precise cloud system observations to enhance the accuracy of models in predicting mixed-phase cloud structure and evolution.

Arctic clouds↗

Optimization models for integrated biorefinery operations

Variations of physical and chemical characteristics of biomass lead to an uneven flow of biomass in a biorefinery, which reduces equipment utilization and increases operational costs. Uncertainty of biomass supply and high processing costs increase the risk of investing in the US’s cellulosic biofuel industry. We propose a stochastic programming model to streamline processes within a biorefinery. A chance constraint models system’s reliability requirement that the reactor is operating at a high utilization rate given uncertain biomass moisture content, particle size distribution, and equipment failure. The model identifies operating conditions of equipment and inventory level to maintain a continuous flow of biomass to the reactor. Furthermore, the sample average approximation method approximates the chance constraint and a bisection search-based heuristic solves this approximation. A case study is developed using real-life data collected at Idaho National Laboratory’s biomass processing facility. An extensive computational analysis indicates that sequencing of biomass bales based on moisture level, increasing storage capacity, and managing particle size distribution, increases utilization of the reactor and reduces operational costs.

09 BIOMASS FUELS↗

Characterization of Iron and Organic Carbon Colloids in Boreal Rivers and Their Fate at High Salinity

Riverine colloids are important carriers of macronutrients, trace metals, and pollutants into marine waters. The aim of the current study was to extend the understanding of iron (Fe) and organic carbon (OC) colloids in boreal rivers and their fate at higher salinities. X-ray absorbance spectroscopy (XAS) and dynamic light scattering (DLS) were combined to explore Fe speciation and colloidal characteristics such as size and surface charge and how these are affected at increasing salinity. XAS confirmed the presence of two Fe phases in the river waters—Fe-organic matter (OM) complexes and Fe(oxy)hydroxides. From DLS measurements on filtered and unfiltered samples, three particle size distributions were identified. The smallest particles (10–40 nm) were positively charged and suggested to consist of essentially bare Fe (oxy)hydroxide nanoparticles. The largest particles (300–900 nm) were dominated by Fe(oxy)hydroxides associated with chromophoric molecular matter. An intermediate size distribution (100–200 nm) with a negative surface charge was presumably dominated by OM and containing Fe-OM complexes. Increasing the salinity resulted in a removal of the smallest distribution. Unexpectedly, both the intermediate and largest size distributions were still detected at high salinity. The collective results suggest that Fe(oxy) hydroxides and Fe-OM complexes are both found across the wide size range studied and that colloidal size does not necessarily reflect either Fe speciation or stability toward salinity-induced aggregation. The findings further demonstrate that also particles beyond the typically studied <0.45-μm size range should be considered to fully understand the riverine transport and fate of macronutrients, trace metals, and pollutants.

54 ENVIRONMENTAL SCIENCES↗

Paper or Plastic? Multiscale Material Handling Properties of Two Model Municipal Solid Waste Streams

Purpose: Municipal Solid Waste (MSW) is a potentially valuable sustainable feedstock for fuel and chemical production due to its carbon-rich content and low cost. This study aims to assess the material handling properties of paperand plastic-rich MSW feedstocks to mitigate equipment failure and processing downtime. Methods: The material handling properties of crumbled MSW feedstocks were measured using apowder rheometer with mass flow hopper calculations to assess handling performance. Inverse gas chromatography was use to measure the surface energy differences between feedstocks. Electron microscopy and Raman spectroscopy was used to evaluate microscale features that may contribute to material handling differences. Results: Plastic and paper rich feedstocks crumbled to a nominal 2 mm particle size were observed to have similar flow and handling characteristics with reasonable hopper outlets. 2 mm plastic rich crumbles, with their higher bulk density, exhibited superior flow performance. By contrast, 4 mm material required significantly larger hopper outlets, indicating poor flowability. Paper rich and 4 mm plastic rich samples displayed broad particle size distributions, which contributed to particle interlocking, jamming, and other flow issues. Electron microscopy revealed that plastic rich samples were significantly smoother, enhancing their flowability compared to the rougher, paper rich materials. Conclusions: This study establishes critical material handling baselines for processing MSW as a viable feedstock for fuel and chemical production. The findings highlight the importance of optimizing particle size and feedstock composition to improve flowability and handling performance.

09 BIOMASS FUELS↗

CFD-DEM Modeling of Autothermal Pyrolysis of Corn Stover with a Coupled Particle- and Reactor-Scale Framework

Autothermal operation of fast pyrolysis is an efficient process-intensification technique wherein exothermic oxidation reactions are used to overcome the heat-transfer bottleneck of conventional pyrolysis. The development of accurate, reliable modeling toolsets is imperative to generating a deeper understanding of biomass autothermal pyrolysis systems to support scale-up and industrial deployment. This modeling effort describes the development of single-particle and reactor models which incorporate detailed reaction schemes and simultaneous exothermic oxidation reactions. The particle-scale model was parameterized for corn stover feedstock with particle morphology, density, ash content, and biopolymer composition, all of which impact the emergent conversion characteristics during pyrolysis. Results were then used to parameterize a reactor-scale autothermal pyrolysis model, which was developed using a coarse-grained computational fluid dynamic-discrete element method. The simulation results compared well with experimental results, with the predicted bio-oil, light gas, and biochar yield within 3.0 wt% of the experimental yields. Further analyses were performed to test the influence of equivalence ratio, biomass injection position, and particle size distribution on autothermal pyrolysis. The analysis of the physio-chemical properties of the fluid and solid phase inside the reactor and at the reactor outlet help reveal important process interactions of autothermal pyrolysis.

BIOMASS FUELS,INORGANIC, ORGANIC, PHYSICAL, AND AN↗