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DOE OSTI2025

Signatures of aerosol-cloud interactions in GiOcean: a coupled global reanalysis with two-moment cloud microphysics

Aerosols influence the Earth's radiative balance through direct interactions with radiation and by affecting cloud properties. Anthropogenic aerosols have led to cooling during the industrial era through aerosol–cloud interactions (ACI), including aerosol effects on cloud microphysical properties and the subsequent adjustments. However, large uncertainties remain in Earth system models (ESMs) regarding the magnitude of this cooling. In part, ESMs substantially disagree on cloud properties, thermodynamics, the hydrological cycle, and general circulation. Reanalysis provides a useful avenue for exploring the impact of ACI on clouds and radiation because its atmosphere is forced to match realistic conditions through the assimilation of observations. Here, we explore the impact of ACI on clouds in the GiOcean reanalysis – the first to incorporate aerosol-cloud interactions. We contrast variables important for ACI between GiOcean and satellite observations and develop 2-dimensional lookup tables of ACI for both using a source-sink budget perspective to attribute the changes in cloud droplet number (Nd) and liquid water path (LWP) to aerosol and meteorology. A compositing analysis using lookup tables shows that GiOcean captures key aspects of aerosol–cloud–precipitation interactions, including (1) activation of aerosol into cloud droplets, (2) effective precipitation scavenging of Nd, (3) suppression of precipitation by high Nd in regions with heavy aerosol emissions. In contrast, satellite observations do not exhibit clear patterns for processes (2) and (3). Random Forest analysis shows that interannual variability in Nd and LWP over the Northern Hemisphere ocean in GiOcean is primarily driven by precipitation, consistent with satellite observations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

A general flame aerosol route to high-entropy nanoceramics

High-entropy ceramics are an emerging class of materials with fascinating characteristics. However, elemental immiscibility and crystal complexity limit the development of a general synthesis strategy, and common methods yield bulk materials. Here, we introduce a transformative non-equilibrium flame aerosol technique for synthesizing high-entropy nanoceramics. This scalable, one-step process enables the production of high-entropy oxide nanoceramics with an unprecedented diversity of crystal structures, including fluorite-phase materials that integrate up to 22 distinct cation elements. The method’s capacity for entropic stabilization and grain refinement significantly improves the thermal stability of these nanostructures. In a representative application, a Pt-(MgCoNiCuZn)O high-entropy single-atom catalyst showed superior activity and long-term stability, maintaining constant CO 2 conversion over 670 h and dramatically outperforming conventional catalysts. Finally, the general approach opens a vast composition and structure space for the creation of high-entropy oxide nanomaterials for application across diverse fields, including catalysis, energy storage, sensing, and thermal management.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Open cells exhibit weaker entrainment of free-tropospheric biomass burning aerosol into the south-east Atlantic boundary layer

This work presents synergistic satellite, airborne and surface-based observations of a pocket of open cells (POC) in the remote south-east Atlantic. The observations were obtained over and upwind of Ascension Island during the CLouds and Aerosol Radiative Impacts and Forcing (CLARIFY) and the Layered Smoke Interacting with Clouds (LASIC) field experiments. A novel aspect of this case study is that an extensive free-tropospheric biomass burning aerosol plume that had been transported from the African continent was observed to be in contact with the boundary layer inversion over the POC and the surrounding closed cellular cloud regime. The in situ measurements show marked contrasts in the boundary layer thermodynamic structure, cloud properties, precipitation and aerosol conditions between the open cells and surrounding overcast cloud field. The data demonstrate that the overlying biomass burning aerosol was mixing down into the boundary layer in the stratocumulus cloud downwind of the POC, with elevated carbon monoxide, black carbon mass loadings and accumulation-mode aerosol concentrations measured beneath the trade-wind inversion. The stratocumulus cloud in this region was moderately polluted and exhibited very little precipitation falling below cloud base. A rapid transition to actively precipitating cumulus clouds and detrained stratiform remnants in the form of thin quiescent veil clouds was observed across the boundary into and deep within the POC. The subcloud layer in the POC was much cleaner than that in the stratocumulus region. The clouds in the POC formed within an ultra-clean layer (accumulation-mode aerosol concentrations of approximately a few cm -3 ) in the upper region of the boundary layer, which was likely to have been formed via efficient collision–coalescence and sedimentation processes. Enhanced Aitken-mode aerosol concentrations were also observed intermittently in this ultra-clean layer, suggesting that new particle formation was taking place. Across the boundary layer inversion and immediately above the ultra-clean layer, accumulation-mode aerosol concentrations were ~1000 cm -3 . Importantly, the air mass in the POC showed no evidence of elevated carbon monoxide over and above typical background conditions at this location and time of year. As carbon monoxide is a good tracer for biomass burning aerosol that is not readily removed by cloud processing and precipitation, it demonstrates that the open cellular convection in the POC is not able to entrain large quantities of the free-tropospheric aerosol that was sitting directly on top of the boundary layer inversion. This suggests that the structure of the mesoscale cellular convection may play an important role in regulating the transport of aerosol from the free troposphere down into the marine boundary layer. We then develop a climatology of open cellular cloud conditions in the south-east Atlantic from 19 years of September Moderate Resolution Imaging Spectroradiometer (MODIS) Terra imagery. This shows that the maxima in open cell frequency (> 0.25) occurs far offshore and in a region where subsiding biomass burning aerosol plumes may often come into contact with the underlying boundary layer cloud. If the results from the observational case study applied more broadly, then the apparent low susceptibility of open cells to free-tropospheric intrusions of additional cloud condensation nuclei could have some important consequences for aerosol–cloud interactions in the region.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2026

Investigating the Impacts of Aqueous-Phase Processing on Organic Aerosol Chemical Climatology Using ARM and ASR Observations

This project improved understanding of how atmospheric aerosol particles form and evolve, with a focus on the role of water-driven (aqueous-phase) chemical reactions in the atmosphere. These processes occur in clouds, fog, and humid air and can significantly change the composition and properties of airborne particles, known as aerosols, which influence air quality and climate. By combining field measurements, laboratory experiments, and advanced analytical techniques, the project identified key chemical signatures that allow scientists to distinguish particles formed through aqueous processes from those formed in the gas phase. Observations from multiple environments, including wildfire smoke, urban regions, and cloud-influenced areas, show that aqueous chemistry is an important pathway for particle formation and aging. The project also developed new measurement approaches using uncrewed aerial systems (UAS) to capture how aerosol composition varies with altitude, providing critical insights into how particles interact with clouds. In addition, new data analysis frameworks were created to better interpret long-term aerosol measurements and improve characterization of particle sources and transformations. These results have been integrated into a global database of aerosol measurements and used to support atmospheric modeling efforts. Overall, the project provides important tools and knowledge to improve predictions of how aerosols affect climate and air quality, particularly through their interactions with radiation and clouds.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Aerosol Deposition Inside a Spent Fuel Transportation and Storage Canister (Interim Report)

This report documents the progress in preparing the ANSYS/Fluent ® and MELCOR models to perform characterization studies of aerosols dispersal and deposition within a select spent fuel cask system. Steady state thermal-hydraulic cask response is modeled with both codes, at present, while the MELCOR source code is being modified to allow imposed thermal-hydraulic conditions with aerosol physics calculations. This will allow the MELCOR model to assume the thermal-hydraulic calculation from the ANSYS/Fluent ® , while only computing the aerosol physics. Detailed results are presented on the thermal-hydraulic analysis of the MAGNASTOR ® cask for the current ANSYS/Fluent ® model, with convergent conditions observed over two fidelities. While the MELCOR computation computes the steady state conditions, they differ sufficiently from that computed with ANSYS/Fluent ® . The MELCOR analysis include a set of UO 2 sources to investigate system response for interim reporting. The airborne concentrations and evolving distributions are presented. Model development is anticipated to continue as additional components impacting flow conditions or aerosol deposition within the MAGNASTOR ® cask and Westinghouse fuel assemblies are identified.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2023

Novel Calibration Approach for Monitoring Aerosol Hydrogen Isotopes Using Laser-Induced Breakdown Spectroscopy for Molten Salt Reactor Off-Gas Streams

Online monitoring is a key challenge for the continued development of molten salt reactor (MSR) technology. Laser-induced breakdown spectroscopy (LIBS) has previously been demonstrated to be a viable tool for monitoring aerosolized species and noble gases in real time, but the ability to discern varying isotopes in these streams has not yet been investigated for MSR applications. Tritium will form in MSRs from ternary fission and from (n,α)-reactions occurring in lithium-containing salts. This study compares three spectrometers of varying resolutions and types for measuring hydrogen isotope shifts in LIBS spectra of wetted filter paper. For each spectrometer, multivariate models were built (i.e., principal component regression, partial least squares regression, and multivariate curve resolution) to quantify the isotope ratio. The top models were then modified and corrected to apply the models to aerosol samples with varying isotope ratios. This novel calibration strategy offers an 82% reduction in volume of the calibration samples needed and is a more viable pathway for calibrating deployable LIBS systems. Lastly, this calibration model was compared with an all-aerosol trained model for monitoring hydrogen isotopes during a real-time test where the protium/deuterium ratio, along with representative salt species (i.e., lithium, sodium, and potassium) were adjusted dynamically. Results of this test validated the predictive capabilities of the transferred model and highlighted the capabilities of LIBS for real-time monitoring of MSR effluent streams.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2023

Long-range transported continental aerosol in the eastern North Atlantic: three multiday event regimes influence cloud condensation nuclei

Abstract. The eastern North Atlantic (ENA) is a region dominated by pristine marine environment and subtropical marine boundary layer clouds. Under unperturbed atmospheric conditions, the regional aerosol regime in the ENA varies seasonally due to different seasonal surface-ocean biogenic emissions, removal processes, and meteorological regimes. However, during periods when the marine boundary layer aerosol in the ENA is impacted by particles transported from continental sources, aerosol properties within the marine boundary layer change significantly, affecting the concentration of cloud condensation nuclei (CCN). Here, we investigate the impact of long-range transported continental aerosol on the regional aerosol regime in the ENA using data collected at the U.S. Department of Energy's (DOE) Atmospheric Radiation Measurement (ARM) user facility on Graciosa Island in 2017 during the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) campaign. We develop an algorithm that integrates number concentrations of particles with optical particle dry diameter (Dp) between 100 and 1000 nm, single scattering albedo, and black carbon concentration to identify multiday events (with duration >24 consecutive hours) of long-range continental aerosol transport in the ENA. In 2017, we detected nine multiday events of long-range transported particles that correspond to ∼ 7.5 % of the year. For each event, we perform HYSPLIT 10 d backward trajectories analysis, and we evaluate CALIPSO aerosol products to assess, respectively, the origins and compositions of aerosol particles arriving at the ENA site. Subsequently, we group the events into three categories, (1) mixture of dust and marine aerosols, (2) mixture of marine and polluted continental aerosols from industrialized areas, and (3) biomass burning aerosol from North America and Canada, and we evaluate their influence on aerosol population and cloud condensation nuclei in terms of potential activation fraction and concentrations at supersaturation of 0.1 % and 0.2 %. The arrival of plumes dominated by the mixture of dust and marine aerosol in the ENA in the winter caused significant increases in baseline Ntot. Simultaneously, the baseline particle size modes and CCN potential activation fraction remained almost unvaried, while cloud condensation nuclei concentrations increased proportionally to Ntot. Events dominated by a mixture of marine and polluted continental aerosols in spring, fall, and winter led to a statistically significant increase in baseline Ntot, a shift towards larger particular sizes, a higher CCN potential activation fractions, and cloud condensation nuclei concentrations of >170 % and up to 240 % higher than during baseline regime. Finally, the transported aerosol plumes characterized by elevated concentration of biomass burning aerosol from continental wildfires detected in the summertime did not statistically contribute to increase baseline aerosol particle concentrations in the ENA. However, particle diameters were larger than under baseline conditions, and CCN potential activation fractions were >75 % higher. Consequentially, cloud concentration nuclei concentrations increased by ∼ 115 % during the period affected by the biomass burning events. Our results suggest that, through the year, multiday events of long-range continental aerosol transport periodically affect the ENA and represent a significant source of CCN in the marine boundary layer. Based on our analysis, in 2017, the multiday aerosol plume transport dominated by a mixture of dust and marine aerosol, a mixture of marine and polluted continental aerosols, and biomass burning aerosols caused increases in the NCCN baseline regime of, respectively, 6.6 %, 8 %, and 7.4 % at SS 0.1 % (and, respectively, 6.5 %, 8.2 %, and 7.3 % at SS 0.2 %) in the ENA.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Developing a Vaccine Platform for a Balanced Mucosal Immune Response (CB11446), Project Report: Year 1

Mucosal vaccines can elicit protective immune responses at the infection site of respiratory or aerosolized pathogens. Achieving balanced mucosal and systemic responses is a key challenge in the design of mucosal vaccines, especially in terms of developing a broadly applicable vaccine delivery platform amenable to a wide range of subunit vaccine antigens. The overarching goal of the project entitled “Developing a Vaccine Platform for a Balanced Mucosal Immune Response” is to develop a pathogen-agnostic vaccine platform that elicits robust and balanced mucosal immune responses upon intranasal vaccination, in the context of a nanolipoprotein particle (NLP) platform. In year one, we investigated NLP-based vaccine formulations incorporating select immune adjuvants (Monophosphoryl Lipid A (MPLA), FSL-1, L18-muramyl dipeptide (MDP), and cholesterol-tagged ODN2006 (cCpG)) along with antigens relevant to plague (LcrV), tularemia (IglC), and Ebola virus (GP). We demonstrated the ability to prepare, characterize, and quantify these formulations. We then carried out studies in vivo using a BALB/c mouse model, comparing intranasal and intramuscular administration and systematically evaluated the resulting mucosal and systemic immune responses using ELISpot and ELISAs. All proposed tasks (Table 1) were completed within the twelve-month base period, and the established go/no go metric was successfully achieved. Numerous adjuvant:LcrV:NLP formulations were found to have statistically significant increases in IgA titers in serum and/or lung upon IN administration (compared to IM administration), while also producing robust IgG responses in serum. Some formulations also showed significant IFNγ responses using restimulated splenocytes. The data collected during the base period provide valuable insights for the future design of safe and effective mucosal subunit vaccines while also highlighting areas of research that merit further investigation.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2024

High Precision, High Frequency Printed Antennas

An emerging trend in advanced manufacturing is printed electronics and sensors. The ability to print customized electronics and sensors integrated into functional packages is a growing need within a variety of growing markets such as smart manufacturing, internet of things (IoT), and the small satellite industry. Both Oak Ridge National Laboratory (ORNL) and the MITRE Corporation have seedling research efforts evaluating the potential for future printed electronic systems. High frequency, wide-bandwidth phased array antennas (i.e. >45 GHz) open the door to new applications. However, such sensors require currently prohibitively small feature sizes for commercial 3D printing technologies along with increasing challenges with connecting the driving electronics to such features. An additional finding with related advanced manufacturing challenges is the rapid production of 3D additive connectors for integration with commercial printed circuit boards (PCBs), primarily for advanced in-circuit inspection techniques. This work is developing additive manufacturing processes for producing connected and conductive fine scale 3D features. The primary focus was on aerosol-jet printing (AJP), which has a small minimum resolution (<50 µm) but is traditionally printed flat with small height/width aspect ratios <<1, and developing controls to enable fully 3D, high aspect ratio, and unsupported features. In Phase 1 of this effort, baselines of process performance were characterized, and test coupons produced for both ultra-high frequency antennas and microstructures to support reverse engineering of PCBs. In Phase 2, these efforts will be extended for system demonstration of ultra-high frequency antenna arrays, as well as reverse engineering circuitry for dense PCBs.

42 ENGINEERING↗

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↗

DOE OSTI2024

Assessing the sensitivity of aerosol mass budget and effective radiative forcing to horizontal grid spacing in E3SMv1 using a regional refinement approach

Abstract. Atmospheric aerosols have important impacts on air quality and the Earth–atmospheric energy balance. However, as computing power is limited, Earth system models generally use coarse spatial grids and parameterize finer-scale atmospheric processes. These parameterizations and the simulation of atmospheric aerosols are often sensitive to model horizontal resolutions. Understanding the sensitivities is necessary for the development of Earth system models at higher resolutions with the deployment of more powerful supercomputers. Using the Energy Exascale Earth System Model (E3SM) version 1, this study investigates the impact of horizontal grid spacing on the simulated aerosol mass budget, aerosol–cloud interactions, and the effective radiative forcing of anthropogenic aerosols (ERFaer) over the contiguous United States. We examine the resolution sensitivity by comparing the nudged simulation results for 2016 from the low-resolution model (LR) and the regional refinement model (RRM). As expected, the simulated emissions of natural dust, sea salt, and marine organic matter are substantially higher in the RRM than in the LR. In addition, RRM simulates stronger aqueous-phase production of sulfate through the enhanced oxidation of sulfur dioxide by hydrogen peroxide due to increased cloud liquid water content. In contrast, the gas-phase chemical production of sulfate is slightly suppressed. The RRM resolves more large-scale precipitation and produces less convective precipitation than the LR, leading to increased (decreased) aerosol wet scavenging by large-scale (convective) precipitation. Regarding aerosol effects on clouds, RRM produces larger temporal variabilities in the large-scale liquid cloud fractions than LR, resulting in increased microphysical cloud processing of aerosols (more interstitial aerosols are converted to cloud-borne aerosols via aerosol activation) in RRM. Water vapor condensation is also enhanced in RRM compared to LR. Consequently, the RRM simulation produces more cloud droplets, a larger cloud droplet radius, a higher liquid water path, and a larger cloud optical depth than the LR simulation. A comparison of the present-day and pre-industrial simulations indicates that, for this contiguous United States domain, the higher-resolution increases ERFaer at the top of the model by about 12 %, which is mainly attributed to the strengthened indirect effect associated with aerosol–cloud interactions.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Strong Local Evaporative Cooling Over Land Due to Atmospheric Aerosols

Abstract Aerosols can enhance terrestrial productivity through increased absorption of solar radiation by the shaded portion of the plant canopy—the diffuse radiation fertilization effect. Although this process can, in principle, alter surface evaporation due to the coupling between plant water loss and carbon uptake, with the potential to change the surface temperature, aerosol‐climate interactions have been traditionally viewed in light of the radiative effects within the atmosphere. Here, we develop a modeling framework that combines global atmosphere and land model simulations with a conceptual diagnostic tool to investigate these interactions from a surface energy budget perspective. Aerosols increase the terrestrial evaporative fraction, or the portion of net incoming energy consumed by evaporation, by over 4% globally and as much as ∼40% regionally. The main mechanism for this is the increase in energy allocation from sensible to latent heat due to global dimming (reduction in global shortwave radiation) and slightly augmented by diffuse radiation fertilization. In regions with moderately dense vegetation (leaf area index >2), the local surface cooling response to aerosols is dominated by this evaporative pathway, not the reduction in incident radiation. Diffuse radiation fertilization alone has a stronger impact on gross primary productivity (+2.18 Pg C y −1 or +1.8%) than on land evaporation (+0.18 W m −2 or +0.48%) and surface temperature (−0.01 K). Our results suggest that it is important for land surface models to distinguish between quantity (change in total magnitude) and quality (change in diffuse fraction) of radiative forcing for properly simulating surface climate.

Chakraborty, TC↗

DOE OSTI2024

Formation of secondary organic aerosol from wildfire emissions enhanced by long-time ageing

Wildfire smoke, consisting primarily of organic aerosols, has profound impacts on air quality, climate and human health. Wildfire organic aerosol evolves over long-time photochemical oxidation due to the formation and ageing of secondary organic aerosol, which substantially changes its magnitude and properties. However, there are large uncertainties in the long-time ageing of wildfire organic aerosol because of the distinct ageing behaviours of the complex organic emissions. Here we developed an oxidation model that simulates the ageing of wildfire organic emissions in the full volatility range on a precursor level and integrated insights from single-species ageing and wildfire emissions ageing experiments and field plume observations to constrain the long-time ageing of wildfire organic aerosol. The model captured the enhancement of organic aerosol mass (2–8 times) and oxygen-to-carbon ratio (1–4 times) in the wildfire ageing experiments. It also reconciled a long-standing discrepancy between field and laboratory observations of the magnitude of secondary organic aerosol formation. The model indicated large emissions-driven variations in precursor contributions to secondary organic aerosol, which further evolve with long-time ageing. In conclusion, the estimated global wildfire secondary organic aerosol production (139 ± 34 Tg per year) was much higher than previous studies omitting or under-constraining long-time ageing.

58 GEOSCIENCES↗

DOE OSTI2021

Final Report on Aerosol Pretreatment Technology Performance and Benchmarking

Solvent-based post-combustion CO 2 capture (PCC) technology remains one of the leading methods to combat global CO 2 emissions produced from large-scale coal-fired power production. Advanced solventbased PCC technology has made significant improvements in design and performance that reduce capital and operating costs to enable its commercial use. Key to low cost, manageable logistics, and environmentally safe operation of solvent-based PCC technology are minimal solvent losses from the process through the treated gas stream exiting PCC plant absorbers. High flue gas aerosol particle concentrations (>10 5 particles/cm 3 ) for particles in the range of 70-200 nm have been shown to cause significant amine solvent losses for solvent-based PCC processes through several mechanisms including absorption of solvent and water into growing aerosol particles. Flue gas aerosol pretreatment technology is the only realistic and economically attractive method to reduce very high aerosol particle concentrations (>10 7 particles/cm 3 ) to enable solvent-based PCC for existing power plants lacking sufficient particle removal systems, such as baghouses. The overall goal of this project was to design, construct, independently test, and evaluate three flue gas aerosol pretreatment technologies identified to significantly reduce high aerosol particle concentrations (>10 7 particles/cm 3 ) in the 70-200 nm particle size range: (1) a novel, high-velocity water injection spray concept developed by RWE and tested by Linde, (2) an innovative electrostatic precipitator (ESP) device with optimized operating conditions developed by Washington University in St. Louis (WUSTL), and (3) a non-regenerative sorbent-based filter technology developed by InnoSepra for SO x and NO x removal from coal-fired power plant flue gas. Each technology has been validated with tests on 500-1000 scfm of actual coal-fired flue gas and evaluated in terms of particle removal efficiency (%), cost competitiveness, and environmental impact. Aerosol measurements were performed upstream and downstream of each aerosol reduction unit during independent testing of each technology using advanced instrumentation and analytical methods provided by WUSTL. To perform aerosol measurements, isokinetic probes were inserted into flanged pipes attached to the flue gas piping, and a small suction pump was used to sample gas containing aerosol particles. Aerosol particle number concentrations (# particles/cm 3 ) and size distributions were then measured using a scanning mobility particle sizer (SMPS, TSI Inc.) for very fine particles (<1,000 nm) and a particle counter manufactured by GRIMM for particles larger than 1,000 nm. This report summarizes the aerosol removal performance results from pilot scale testing of each technology. Performance results have been benchmarked against pre-defined targets and other flue gas aerosol pretreatment technologies with documented performance. Linde Gas North America LLC has been the prime contractor to DOE responsible for overall project management and provided the design for the high-velocity water spray-based aerosol removal technology based on a design concept developed by the German utility company RWE.

20 FOSSIL-FUELED POWER PLANTS↗

DOE OSTI2025

Enhanced Convective Microphysics Scheme and Its Impacts on Mean Climate in E3SM

Abstract To improve the representation of microphysical processes in convective clouds and their interaction with aerosol and stratiform clouds, a two‐moment convective microphysics parameterization (CMP) scheme developed by Song and Zhang (2011, https://doi.org/10.1029/2010jd014833 ) is upgraded and implemented in E3SM. The new developments include: (a) implementing a parameterization for graupel to enhance the representation of ice‐phase microphysical processes; (b) representing the impact of spatial inhomogeneity of cloud droplets in cumulus ensembles on autoconversion and accretion processes to improve the representation of warm‐rain microphysical processes; (c) implementing a comprehensive Bergeron process parameterization to better represent mixed‐phase microphysical processes; and (d) representing the interactions between ice‐phase microphysics and cloud thermodynamics. Simulations show that the cloud microphysical properties simulated by the CMP are generally in good agreement with observations. It reasonably simulates the changes in droplets effective radius related to precipitation formation in convective clouds, as identified from satellite observations. It also successfully simulates the contrast in these processes between maritime and continental clouds, demonstrating its capability to simulate the impact of aerosols on convection. Analyses of the impact of CMP on climate mean state simulation demonstrate that the CMP slightly improves the simulations of precipitation, cloud macrophysical properties, longwave cloud radiative forcing, zonal wind, and temperature. However, a degradation in shortwave cloud radiative forcing occurs.

GCM↗

DOE OSTI2022

A Kinetic Model for Predicting Trace Gas Uptake and Reaction

A model is developed to describe trace gas uptake and reaction with applications to aerosols and microdroplets. Gas uptake by the liquid is formulated as a coupled equilibria that links gas, surface, and bulk regions of the droplet or solution. Previously, this framework was used in explicit stochastic reaction-diffusion simulations to predict the reactive uptake kinetics of ozone with droplets containing aqueous aconitic acid, maleic acid, and sodium nitrite. With the use of prior data and simulation results, a new equation for the uptake coefficient is derived, which accounts for both surface and bulk reactions. Lambert W functions are used to obtain closed form solutions to the integrated rate laws for the multiphase kinetics; similar to previous expressions that describe Michaelis-Menten enzyme kinetics. Together these equations couple interface and bulk processes over a wide range of conditions and do not require many of the limiting assumptions needed to apply resistor model formulations to explain trace gas uptake and reaction.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Forest Breeze–Cold Pool Interactions Drive Convective Organization over Heterogeneous Vegetation

Heterogeneous landscapes can influence the development of convection through the generation of thermally driven mesoscale circulations. To assess the impacts of these circulations and their interaction with sea breezes, we simulated convection in an idealized coastal environment using the Regional Atmospheric Modeling System (RAMS). We compared simulations with striped patterns of surface vegetation to those of uniform vegetation to identify the importance of vegetation heterogeneity in impacting convective development. Under dry soil conditions representative of those during the Tracking Aerosol Convection Interactions Experiment (TRACER) and Experiment of Sea Breeze Convection, Aerosols, Precipitation, and Environment (ESCAPE) campaigns in June 2022, we found that these vegetation-induced circulations, referred to in the literature as “forest breezes,” are more important than the sea breeze in determining the location of convection initiation. Convection and precipitation are also found to be favored over forests and suppressed over pasture and suburban landscapes as a result of greater surface sensible heat flux over the forest. Our findings also indicate that forest breezes are important for initiating convection along the boundaries of the forest, but that cold pools may play a key role in propagating the forest breezes toward the center of the forest stripe. In our simulations, the collisions of these breezes in the center of the forest stripe lead to uplift and strong convection there; however, a different width of the forest stripe would alter when the forest breezes collide or whether they collide at all. The presence of these cold pools may therefore impact the “ideal stripe width,” the width of each vegetation stripe which maximizes domain-wide precipitation.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Ventilation in Residential Care Environments

The purpose of this study was to evaluate the effect of ventilation rate, directional airflow (e.g. pressure relationships) and airflow barriers on bioaerosol concentration and movement within assisted-living and residential care environments. Included within this report is a comprehensive literature review, field data collection test plan and, an evaluation of commercially available mitigation technologies related to the transmission of COVID-19 in LTC environments. Additionally, this report includes aerosol testing in an actual LTC facility using the test plan developed herein. Nearly 1.5 million people live in 16,000 nursing homes in the U.S. As of December 20, 2020 the Centers for Medicare and Medicaid Services (CMS) identified a total of 662,549 confirmed and suspected COVID-19 cases in these and other long-term care (LTC) facilities resulting in 92,373 deaths. At this time, COVID-19 cases in LTC facilities accounted for only 3% of the U.S. total of 21M confirmed cases yet nearly a third of the 350,000 total U.S. deaths. Preliminary studies have found little correlation between the quality of care and transmission of COVID-19 in these facilities, suggesting that even the best infection control practices may not be effective in containing the spread of this potentially airborne disease. As a result, many LTC facilities have implemented quarantine procedures and other measures to isolate infectious residents from the general population. Unfortunately, most LTC facilities were not designed for airborne infection control and guidance for retrofitting existing LTC spaces for airborne isolation is limited.

42 ENGINEERING↗