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DOE OSTI2025

Chemical imaging of individual stratospheric particles sampled over North America

The increasing size, severity, and frequency of wildfires have led to dramatic increases in particulate matter concentrations in the troposphere. Severe wildfires can generate intense convective systems capable of transporting large quantities of biomass burning organic aerosols (BBOA) to the upper troposphere and lower stratosphere (UTLS). Chemically complex organic matter and light-absorbing carbonaceous material is introduced into stratospheric regions that were historically isolated from direct surface emissions. In this study, stratospheric particles were sampled over North America during the Dynamics and Chemistry of the Summer Stratosphere (DCOTSS) campaign, an aircraft-based research project designed to characterize convective perturbation in the UTLS. Particle samples collected from six research flights during summer 2022 were analyzed using Computer-Controlled Scanning Electron Microscopy and Scanning Transmission X-ray Microscopy to investigate particle size distributions, morphology, chemical composition, and mixing state of stratospheric particles along transects across the continental United States and adjacent Pacific Ocean airspace. Analysis revealed that all sampled particles contained detectable levels of carbon, with most exhibiting organic volume fractions of 0.37 ± 0.20. Notably, about 5% of the particles also contained soot inclusions, which indicates the presence of refractory black carbon transported to stratospheric altitudes and provides direct evidence of wildfire-derived black carbon reaching the UTLS. Typical particle morphology exhibits organic shells over soot and inorganic cores and suggests secondary processing and aging of BBOA during transport to and within the UTLS. These findings provide compelling evidence that wildfire emissions play a critical role in affecting the long-term composition and radiative properties of stratospheric particles.

Sharpe, Steven [Purdue Univ., West Lafayette, IN (↗

DOE OSTI2023

Source apportionment of soot particles and aqueous-phase processing of black carbon coatings in an urban environment

Abstract. The impacts of soot particles on climate and human health depend on the concentration of black carbon (BC) as well as the thickness and composition of the coating material, i.e., organic and inorganic compounds internally mixed with BC. In this study, the size-resolved chemical composition of BC-containing aerosol was measured using a high-resolution soot particle aerosol mass spectrometer (SP-AMS) during wintertime in Fresno, California, a location influenced by abundant combustion emissions and frequent fog events. Concurrently, particle optical properties were measured to investigate the BC absorption enhancement. Positive matrix factorization (PMF) analysis was performed on the SP-AMS mass spectral measurements to explore the sources of soot particles and the atmospheric processes affecting the properties of BC coatings. The analysis revealed that residential woodburning and traffic are the dominant sources of soot particles. Alongside primary soot particles originating from biomass burning (BBOABC) and vehicles (HOABC) two distinct types of processed BC-containing aerosol were identified: fog-related oxidized organic aerosol (FOOABC) and winter-background OOABC (WOOABC). Both types of OOABC showed evidence of having undergone aqueous processing, albeit with differences. The concentration of FOOABC was substantially elevated during fog events, indicating the formation of aqueous secondary organic aerosol (aqSOA) within fog droplets. On the other hand, WOOABC was present at a relatively consistent concentration throughout the winter and was likely related to the formation of secondary organic aerosol (SOA) in both the gas phase and aerosol liquid water. By comparing the chemical properties and temporal variations in FOOABC and WOOABC, we gain insights into the key aging processes of BC aerosol. It was found that aqueous-phase reactions facilitated by fog droplets had a significant impact on the thickness and chemical composition of BC coatings, thereby affecting the light absorption and hygroscopic properties of soot particles. These findings underscore the important role of chemical reactions occurring within clouds and fogs and influencing the climate forcing of BC aerosol in the atmosphere.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

A numerical investigation of coal particle modeling for the inlet section of a pressurized oxy-combustion burner

Concerns over climate change have led to numerous efforts to develop low-carbon technologies, and pressurized oxy-combustion (POC) is a promising candidate to reduce carbon emissions in the power industry. Designing an effective burner for such technologies is vital for the development of these and other coal combustion technologies. Because of the high pressure, the volume fraction of coal particles at the fuel inlet of the pressurized oxy-combustor burner is close to or even higher than the maximum limit for commercial CFD codes (e.g., ANSYS FLUENT). At these high particle volume fractions, the interactions among particles, fluid flow and wall need to be re-evaluated. The present computational work is a first step in a systematic analysis of the influence of various parameters, like method of particle release, release location, and particle size, in a pilot-scale POC combustor, developed at Washington University in St. Louis (WUSTL). In the POC process, pulverized coal is burned under elevated pressure in an O2-CO2 environment. Specifically, a 15-bar, 100 kWth, POC combustor is modeled employing Ansys FLUENT commercial sodtware using the Reynolds-Averaged Navier-Stokes (RANS) approach. It is revealed that for this pilot-scale, pressurized burner, velocity profiles in the near-wall region exhibit some anomalies. In order to investigate the influence of particle loading in the near-wall region, particle release location was investigated. The numerical simulations incorporate the coupling between the turbulent flow and the particles. A sensitivity investigation of particle release location found that by tuning the release location, the velocity profile can be consistent with the pure gas flow velocity profile. More importantly, the particle releasing location also affects flame stability. Particle size was also found to have a significant impact on particle trajectory, flame stability and temperature. Finally, Large Eddy Simulations (LES) were performed and compared with the results from two-dimensional RANS.

Li, Lei↗

DOE OSTI2024

Experimental Investigation of the Effect of Air-Handling and DME-Propane Blends on the Performance and Emissions of a 4-Cylinder CI Engine

Dimethyl ether (DME) is considered an excellent alternative to diesel because of its higher cetane number and lower carbon content. Additionally, DME can be blended with abundantly available propane with minimal modifications to the propane infrastructure. This paper focuses on an experimental investigation of the effect of air-handling i.e., boost pressure and exhaust gas recirculation (EGR), and DME-propane blends on the combustion and emissions performance of a light-duty, four-cylinder, compression ignition (CI) engine. Here, the boost pressure and EGR sweeps were carried out and showed that higher boost pressures resulted in increased brake thermal efficiencies (BTE) at the expense of higher NOx emissions which could be reduced by an increase in EGR. The fuel sweeps were carried out at 0, 15 and 25% propane (neat, 85% and 75% DME) with 0% and 25% EGR. The fuel sweeps indicated that the ignition delay (ID) increased and burn duration (BD) decreased monotonically when the blend increased to 25% propane/75% DME. The results suggest optimum engine performance with neat DME at 105 kPa boost pressure and 25% EGR with propane addition improving the BTE with negligible increase in emissions. Higher contents of Propane, up to 25%, did not affect the variability of combustion, with standard deviations of burn duration and peak cylinder pressures below 1% for all test cases.

air-handling↗

DOE OSTI2023

AmeriFlux FLUXNET-1F US-Wi6 Pine barrens #1 (PB1)

This is the AmeriFlux Management Project (AMP) created FLUXNET-1F version of the carbon flux data for the site US-Wi6 Pine barrens #1 (PB1). This is the FLUXNET version of the carbon flux data for the site US-Wi6 Pine barrens #1 (PB1) produced by applying the standard ONEFlux (1F) software. Site Description - The Wisconsin Pine Barrens site is located in the Washburn Ranger District of the northeastern section of Chequamegon National Forest. A member of the northern coniferous-deciduous biome, surveys from the mid-19th century indicate the region consisted of a mixed stand of red, white, and jack pines. After extensive timber harvesting, wildfires, and farming activity, the region turned into a fragmented mosaic of stands of various ages and composition. As an assemblage, the ten Wisconsin sites are indicative of the successional stages of development in the predominant stand types of a physically homogeneous landscape. In order to establish and maintain both natural and plantation jack pine stands, pine barrens undergo prescribed burns and harvesting rotations. Pine Barrens occupy 17% of the region in 2001.

Chen, Jiquan↗

DOE OSTI2020

Reactor and fuel cycle performance of light water reactor fuel with 235 U enrichments above 5%

Recent advances in nuclear fuel materials research, particularly on the topic of accident-tolerant fuels, have brought up potential opportunities for expanding the operating envelope of existing light water reactors. As many of the performance improvements offered by these technologies may be most fully realized by increasing fuel enrichment beyond the standard 5% limit, this paper examines the potential reactor performance and fuel cycle performance of low-enriched uranium oxide fueled light water reactors by generically considering pressurized water reactors with 235 U enrichment from 5 to 7%. Advanced cladding, including accident-tolerant cladding, has the potential to increase fuel burnup limits related to hydrogen in the cladding that coincide with those limits associated with end-of-life reactivity. Therefore, higher enrichment will be necessary in order to realize the higher fuel burnups. This work includes evaluation of the fuel cycle length, discharge burnup, reactivity coefficients, and fuel cycle performance, including radioactive waste and environmental impact metrics per unit energy generated. The analysis was performed using the evaluation metrics from the US Department of Energy Office of Nuclear Energy Fuel Cycle Evaluation and Screening Study. The reactor performance and safety analysis show that enrichments between 5 and 7% would have similar fuel temperature and moderator temperature coefficients. However, the soluble boron coefficient would decrease in magnitude, requiring more corrosive boric acid in the coolant or other methods of reactivity control during the fuel cycle. At these higher enrichments the maximum burnup at the rim of the fuel pellet would increase by almost a factor of two, which is expected to impact the formation of high-burnup structure in the fuel and the corresponding thermo-mechanical fuel properties. The fuel cycle performance assessment shows that increasing enrichment reduces the quantity of high-level waste disposed per unit energy generated, but it increases the natural resource requirements normalized to a gigawatt-electricity-per-year basis. Another impact is the slightly higher discharge burnup, resulting in somewhat different activity levels of the spent nuclear fuel and high-level waste radioactivity at 100 and 100,000 years after fuel discharge. The environmental impacts—including land use, water use, carbon emission, and radiological exposure—are of the same magnitude per unit energy generated. Finally, however, the impacts are distributed differently. Less than 5% enrichment has marginally more impact on the back-end of the fuel cycle, and greater than 5% enrichment has marginally more impact on the front-end of the fuel cycle. Ultimately, no neutronic or reactor safety hindrances to employing light water reactor fuel with enrichments greater than 5% are identified; given the achievable reactor performance benefits with advanced fuels, further practical exploration of increased enrichment fuel is recommended.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2026

Observations of Nocturnal Sulfuric Acid Formation in Pittsburgh, PA

Measurements of sulfuric acid (H 2 SO 4 ) and sulfur trioxide (SO 3 ) were conducted in Pittsburgh, Pennsylvania, during field campaigns in Fall 2023 and Fall 2024. These measurements identified nocturnal concentrations of H 2 SO 4 comparable to those of daytime values. Nocturnal H 2 SO 4 concentrations were observed to increase by 5 × 10 5 to 5 × 10 7 molecules cm –3 above background on 16 of the 31 measurement nights. The median peak concentration during events was 6.5 × 10 6 molecules cm –3 , with a maximum of 1.0 × 10 8 molecules cm –3 , exceeding previously reported nighttime concentrations. Increases in H 2 SO 4 concentrations were positively correlated with the anomalously high SO 3 concentrations and condensation sink rates, indicating that the formation of H 2 SO 4 increased to overcome the loss rates to particles. Increases in particulate mass and the mass fraction of metals commonly emitted from coal combustion and steel production were also observed. The air masses were traced back to the southeast of Pittsburgh, a region home to a steel mill, coke plant, and a steel processing plant. The observations indicate a previously unrecognized nighttime formation pathway for H 2 SO 4 , potentially from heterogeneous catalysis with metal or black carbon, originating from steel and coke plant emissions. Further measurements are needed to identify key compounds and chemical processes driving these increases in nocturnal H 2 SO 4 concentrations.

aerosols↗

DOE OSTI2020

AmeriFlux US-xSB NEON Ordway-Swisher Biological Station (OSBS)

This is the AmeriFlux version of the carbon flux data for the site US-xSB NEON Ordway-Swisher Biological Station (OSBS). Site Description - The Ordway-Swisher Biological Station (OSBS) is operated by the University of Florida and comprises over 9,300 acres. It is a year-round field station established for the long-term study and conservation of unique ecosystems through management, research and education. The Station is located approximately 20 miles east of Gainesville in Melrose (Putnam County, Florida). There are two aquatic arrays at Ordway-Swisher, representing the two dominant aquatic features on the landscape: 1) Suggs lake, a shallow surface water lake that is rich in taxa and biologically active in structure and function; and 2) Barco lake, a deep lake connected to ground water. The forest is maintained by fire and has a relatively open structure: it is managed with prescribed burns at a frequency of 3-4 years.

Network), NEON (National Ecological Observatory↗

DOE OSTI2023

Biomass-burning smoke's properties and its interactions with marine stratocumulus clouds in WRF-CAM5 and southeastern Atlantic field campaigns

Abstract. A large part of the uncertainty in climate projections comes from uncertain aerosol properties and aerosol–cloud interactions as well as the difficulty in remotely sensing them. The southeastern Atlantic functions as a natural laboratory to study biomass-burning smoke and to constrain this uncertainty. We address these gaps by comparing the Weather Research and Forecasting with Chemistry Community Atmosphere Model (WRF-CAM5) to the multi-campaign observations ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS), CLARIFY (CLoud–Aerosol–Radiation Interaction and Forcing), and LASIC (Layered Atlantic Smoke Interactions with Clouds) in the southeastern Atlantic in August 2017 to evaluate a large range of the model's aerosol chemical properties, size distributions, processes, and transport, as well as aerosol–cloud interactions. Overall, while WRF-CAM5 is able to represent smoke properties and transport, some key discrepancies highlight the need for further analysis. Observations of smoke composition show an overall decrease in aerosol mean diameter as smoke ages over 4–12 d, while the model lacks this trend. A decrease in the mass ratio of organic aerosol (OA) to black carbon (BC), OA:BC, and the OA mass to carbon monoxide (CO) mixing ratio, OA:CO, suggests that the model is missing processes that selectively remove OA from the particle phase, such as photolysis and heterogeneous aerosol chemistry. A large (factor of ∼2.5) enhancement in sulfate from the free troposphere (FT) to the boundary layer (BL) in observations is not present in the model, pointing to the importance of properly representing secondary sulfate aerosol formation from marine dimethyl sulfide and gaseous SO2 smoke emissions. The model shows a persistent overprediction of aerosols in the marine boundary layer (MBL), especially for clean conditions, which multiple pieces of evidence link to weaker aerosol removal in the modeled MBL than reality. This evidence includes several model features, such as not representing observed shifts towards smaller aerosol diameters, inaccurate concentration ratios of carbon monoxide and black carbon, underprediction of heavy rain events, and little evidence of persistent biases in modeled entrainment. The average below-cloud aerosol activation fraction (NCLD/NAER) remains relatively constant in WRF-CAM5 between field campaigns (∼0.65), while it decreases substantially in observations from ORACLES (∼0.78) to CLARIFY (∼0.5), which could be due to the model misrepresentation of clean aerosol conditions. WRF-CAM5 also overshoots an observed upper limit on liquid cloud droplet concentration around NCLD= 400–500 cm−3 and overpredicts the spread in NCLD. This could be related to the model often drastically overestimating the strength of boundary layer vertical turbulence by up to a factor of 10. We expect these results to motivate similar evaluations of other modeling systems and promote model development to reduce critical uncertainties in climate simulations.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Shrub Seedling Experiment: Environmental Conditions, Vegetation Composition, and Seedling Recruitment, Seward Peninsula, Alaska, 2018-2019

In June 2018, a manipulative seed-addition experiment was established at the Council Mile Marker 71 (CN_MM71), Quartz Creek Burn Area (Kougarok Mile Marker 86), and Quartz Creek Unburned (Kougarok Mile Marker 80) sites on the Seward Peninsula, Alaska. At each site, 5 replicate blocks were established in disturbed and intact upland tussock tundra (a total of 40 plots). Disturbed plots at Council were located on thermo-erosional (thermokarst) slopes, while disturbed plots in Quartz Creek were in burned areas affected by the Mingvk Lake fire in 2015. Using a split-plot design, an additional manual disturbance treatment (scraping to remove the surface bryophyte layer) was implemented across all blocks in June 2018. Seeds of five erect, deciduous shrubs were broadcast seeded into each plot in June 2018, and seedlings were censused in August 2018 and August 2019. The dataset includes ancillary measurements of plot-level environmental conditions (soil temperature, moisture, chemistry, thaw depth, microtopography, substrate thickness) and vegetation composition (NDVI and estimated percent cover by species and plant functional type). Dataset contains 10 csv data files (five data files with corresponding data dictionaries and one file-level metadata file) and one pdf user guide. The Next-Generation Ecosystem Experiments: Arctic (NGEE Arctic), was research effort to reduce uncertainty in Earth System Models by developing a predictive understanding of carbon-rich Arctic ecosystems and feedbacks to climate. NGEE Arctic was supported by the Department of Energy's Office of Biological and Environmental Research. The NGEE Arctic project had two field research sites: 1) located within the Arctic polygonal tundra coastal region on the Barrow Environmental Observatory (BEO) and the North Slope near Utqiagvik (Barrow), Alaska and 2) multiple areas on the discontinuous permafrost region of the Seward Peninsula north of Nome, Alaska. Through observations, experiments, and synthesis with existing datasets, NGEE Arctic provided an enhanced knowledge base for multi-scale modeling and contributed to improved process representation at global pan-Arctic scales within the Department of Energy's Earth system Model (the Energy Exascale Earth System Model, or E3SM), and specifically within the E3SM Land Model component (ELM).

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Cryogenic Carbon Capture™ (CCC) Status Report

The Cryogenic Carbon Capture™ (CCC) process separates CO2 from light gases in essentially any continuous process. CCC cools the gases to the frost or desublimation point of CO2 (-100 to -135 °C), separates and pressurizes the solids, and warms all streams to produce a CO2-depleted stream at ambient pressure and a pure (99+%) pressurized liquid CO2 stream typically to about 150 bar, both at ambient temperature. The process also recovers all gas moisture and most gas impurities less volatile than CO2 (NOx, SOx, Hg, PM, UHC, CCC, etc.) in separable streams. CCC nearly eliminates refrigeration energy for sensible temperature changes through heat integration. CCC does require energy to change the CO2 phase from a mixed vapor to a pressurized fluid, which represents the minimum energy required of any process for this separation. CCC uses additional energy for turbomachinery inefficiencies, heat losses, moisture removal and overall process pressure drop. Aside from these real-world energy demands, CCC operates near the minimum energy required to perform this gas separation by minimizing stream recycling. CCC compresses CO2 as a liquid, which is one of several reasons it costs about about half as much and consumes about half as much energy as an amine process when using flue gases with about 15% CO2. The process also has several major additional advantages, including (a) it is a bolt-on retrofit technology that does not need steam or any modification of existing equipment, (b) it recovers water and nearly all pollutants in addition to CO2 from the flue gas, (c) it enables highly efficient and cost effective energy storage at grid scale and on time scales of minutes, (d) it enables NG storage if the energy storage option is used, and (d) it has a small footprint and is minimally disruptive to existing plants, requiring only electrical power and a gas source to operate. Sustainable Energy Solutions (SES) has scaled this technology through several levels, the largest of which captures nominally 1 tonne of CO2/day and is called the skid system. Skid system field tests include utility-scale power plants, cement plants, heating plants, and other utility or industrial sites that burn natural gas, biomass, coal, shredded tires, municipal waste, and combinations of these fuels. These field tests produced 95-99% CO2 capture with CO2 purities of 99+% and initial CO2 contents that range from 4 to 28%. SES currently seeks to scale the system to merchant scale (10-80 tonnes of CO2 per day). In the process of doing so, SES has demonstrated the potential for CCC to contribute to energy storage and direct air capture in innovative and cost-effective ways. This presentation discusses the overall process and highlights results from field and in-house tests. These include (a) measured CO2 capture rates and operating conditions from in-house and field tests, and (b) predicted utility-scale costs and energy demands. This discussion also includes the application of the CCC technology to energy storage and direct air capture.

20 FOSSIL-FUELED POWER PLANTS↗

DOE OSTI2026

Sunlight can turn smoldering pine wood smoke into a glass

Wildfires inject biomass burning organic aerosols (BBOA) into the atmosphere. During their lifetimes of weeks to months, they are exposed to ultraviolet (UV) irradiation. Viscosity and phase behaviour are essential properties for understanding their chemical and climate impacts. Here, we quantify changes in viscosity and phase behavior after UV exposure. After an atmospheric equivalent of 8.7 days of boundary layer UV exposure, BBOA develop a highly viscous (glassy) outer phase with a viscosity at least five orders of magnitude higher than unaged BBOA, which persists up to at least 58% relative humidity. High-resolution mass spectrometry indicates that UV-aging increases oxidation and molecular weight. Using our viscosity results, we predict that UV-aged BBOA are frequently glassy above ~2.5 km and can have viscosities up to eight orders of magnitude higher than unaged particles in some atmospheric regions, which may influence lifetimes of pollutants and brown carbon, and impact stratospheric ozone chemistry.

Golay, Zoe↗

DOE OSTI2023

Gold Nanoparticles AuNP Decorated on Fused Graphene-like Materials for Application in a Hydrogen Generation

The search for a sustainable, alternative fuel source to replace fossil fuels has led to an increased interest in hydrogen fuel. This combustible gas is not only clean-burning but can readily be produced via the hydrolysis of sodium borohydride. The main drawback of this reaction is that the reaction occurs relatively slowly and requires a catalyst to improve efficiency. This study explored a novel composite material made by combining gold nanoparticles and fused graphene-like materials (AuFGLM) as a catalyst for generating hydrogen via sodium borohydride. The novel fused graphene-like material (FGLM) was made with a sustainable dextrose solution and by using a pressure-processing method. Imaging techniques showed that FGLM appears to be an effective support template for nanoparticles. Transmission electron microscopy (TEM), scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDS), Fourier-transform infrared spectroscopy (FTIR), X-ray diffraction (XRD) and Raman spectroscopy were used to characterize and determine the size, shape, and structure of nanoparticles and composites. The TEM study characterized the fused carbon backbone as it began to take on a rounder shape. The TEM images also revealed that the average diameter of the gold nanoparticle was roughly 23 nm. The FTIR study confirmed O-H, C-C, and C=O as functional groups in the materials. The EDS analysis showed that the composite contained approximately 6.3% gold by weight. The crystal structures of FGLM and AuFGLM were identified via P-XRD analysis. Various reaction conditions were used to test the catalytic ability of AuFGLM, including various solution pHs, temperatures, and doses of NaBH 4 . It was observed that optimal reaction conditions included high temperature, an acidic solution pH, and a higher dose of NaBH 4 . The activation energy of the reaction was determined to be 45.5 kJ mol -1 , and it was found that the catalyst could be used multiple times in a row with an increased volume of hydrogen produced in ensuing trials. The activation energy of this novel catalyst is competitive compared to similar catalysts and its ability to produce hydrogen over multiple uses makes the material an exciting choice for catalyzing the hydrolysis of NaBH 4 for use as a hydrogen fuel source.

08 HYDROGEN↗

DOE OSTI2021

Exploring the elevated water vapor signal associated with the free tropospheric biomass burning plume over the southeast Atlantic Ocean

In southern Africa, widespread agricultural fires produce substantial biomass burning (BB) emissions over the region. The seasonal smoke plumes associated with these emissions are then advected westward over the persistent stratocumulus cloud deck in the southeast Atlantic (SEA) Ocean, resulting in aerosol effects which vary with time and location. Much work has focused on the effects of these aerosol plumes, but previous studies have also described an elevated free tropospheric water vapor signal over the SEA. Water vapor influences climate in its own right, and it is especially important to consider atmospheric water vapor when quantifying aerosol-cloud interactions and aerosol radiative effects. Here we present airborne observations made during the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) campaign over the SEA Ocean. In observations collected from multiple independent instruments on the NASA P-3 aircraft (from near-surface to 6-7 km), we observe a strongly linear correlation between pollution indicators (carbon monoxide (CO) and aerosol loading) and atmospheric water vapor content, seen at all altitudes above the boundary layer. The focus of the current study is on the especially strong correlation observed during the ORACLES-2016 deployment (out of Walvis Bay, Namibia), but a similar relationship is also observed in the August 2017 and October 2018 ORACLES deployments. Using reanalyses from the European Centre for Medium-Range Weather Forecasts (ECMWF) and Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2), and specialized WRF-Chem simulations, we trace the plume-vapor relationship to an initial humid, smoky continental source region, where it mixes with clean, dry upper tropospheric air and then is subjected to conditions of strong westward advection, namely the southern African easterly jet (AEJ-S). Our analysis indicates that air masses likely left the continent with the same relationship between water vapor and carbon monoxide as was observed by aircraft. This linear relationship developed over the continent due to daytime convection within a deep continental boundary layer (up to ~5-6 km) and mixing with higher-altitude air, which resulted in fairly consistent vertical gradients in CO and water vapor, decreasing with altitude and varying in time, but this water vapor does not originate as a product of the BB combustion itself. Due to a combination of conditions and mixing between the smoky, moist continental boundary layer and the dry and fairly clean upper-troposphere air above (~6 km), the smoky, humid air is transported by strong zonal winds and then advected over the SEA (to the ORACLES flight region) following largely isentropic trajectories. Hybrid Single-Particle Lagrangian Integrated Trajectory model (HYSPLIT) back trajectories support this interpretation. This work thus gives insights into the conditions and processes which cause water vapor to covary with plume strength. Better understanding of this relationship, including how it varies spatially and temporally, is important to accurately quantify direct, semi-direct, and indirect aerosol effects over this region.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Estimating the influence of field inventory sampling intensity on forest landscape model performance for determining high-severity wildfire risk

Abstract Historically, fire has been essential in Southwestern US forests. However, a century of fire-exclusion and changing climate created forests which are more susceptible to uncharacteristically severe wildfires. Forest managers use a combination of thinning and prescribed burning to reduce forest density to help mitigate the risk of high-severity fires. These treatments are laborious and expensive, therefore optimizing their impact is crucial. Landscape simulation models can be useful in identifying high risk areas and assessing treatment effects, but uncertainties in these models can limit their utility in decision making. In this study we examined underlying uncertainties in the initial vegetation layer by leveraging a previous study from the Santa Fe fireshed and using new inventory plots from 111 stands to interpolate the initial forest conditions. We found that more inventory plots resulted in a different geographic distribution and wider range of the modelled biomass. This changed the location of areas with high probability of high-severity fires, shifting the optimal location for management. The increased range of biomass variability from using a larger number of plots to interpolate the initial vegetation layer also influenced ecosystem carbon dynamics, resulting in simulated forest conditions that had higher rates of carbon uptake. We conclude that the initial forest layer significantly affects fire and carbon dynamics and is dependent on both number of plots, and sufficient representation of the range of forest types and biomass density.

Science & Technology - Other Topics↗

DOE OSTI2023

AmeriFlux FLUXNET-1F US-xSB NEON Ordway-Swisher Biological Station (OSBS)

This is the AmeriFlux Management Project (AMP) created FLUXNET-1F version of the carbon flux data for the site US-xSB NEON Ordway-Swisher Biological Station (OSBS). This is the FLUXNET version of the carbon flux data for the site US-xSB NEON Ordway-Swisher Biological Station (OSBS) produced by applying the standard ONEFlux (1F) software. Site Description - The Ordway-Swisher Biological Station (OSBS) is operated by the University of Florida and comprises over 9,300 acres. It is a year-round field station established for the long-term study and conservation of unique ecosystems through management, research and education. The Station is located approximately 20 miles east of Gainesville in Melrose (Putnam County, Florida). There are two aquatic arrays at Ordway-Swisher, representing the two dominant aquatic features on the landscape: 1) Suggs lake, a shallow surface water lake that is rich in taxa and biologically active in structure and function; and 2) Barco lake, a deep lake connected to ground water. The forest is maintained by fire and has a relatively open structure: it is managed with prescribed burns at a frequency of 3-4 years.

Network), NEON (National Ecological Observatory↗

DOE OSTI2024

Chemical properties and single-particle mixing state of soot aerosol in Houston during the TRACER campaign

Abstract. A high-resolution soot particle aerosol mass spectrometer (SP-AMS) was used to selectively measure refractory black carbon (rBC) and its associated coating material using both the ensemble size-resolved mass spectral mode and the event trigger single particle (ETSP) mode in Houston, Texas, in summer 2022. This study was conducted as part of the Department of Energy Atmospheric Radiation Measurement (ARM) program's TRacking Aerosol Convection interactions ExpeRiment (TRACER) field campaign. The study revealed an average (±1σ) rBC concentration of 103 ± 176 ng m−3. Additionally, the coatings on the BC particles were primarily composed of organics (59 %; 219 ± 260 ng m−3) and sulfate (26 %; 94 ± 55 ng m−3). Positive matrix factorization (PMF) analysis of the ensemble mass spectra of BC-containing particles resolved four distinct types of soot aerosol, including an oxidized organic aerosol (OOABC,PMF) factor associated with processed primary organic aerosol, an inorganic sulfate factor (SO4,BC,PMF), an oxidized rBC factor (O-BCPMF), and a mixed mineral dust–biomass burning aerosol factor with significant contribution from potassium (K-BBBC,PMF). Additionally, K-means clustering analysis of the single-particle mass spectra identified eight different clusters, including soot particles enriched in hydrocarbon-like organic aerosol (HOABC,ETSP), sulfate (SO4,BC,ETSP), two types of rBC, OOA (OOABC,ETSP), chloride (ClBC,ETSP), and nitrate (NO3,BC,ETSP). The single-particle measurements demonstrate substantial variation in BC coating thickness with coating-to-rBC mass ratios ranging from 0.1 to 100. The mixing state index (χ), which denotes the degree of homogeneity of the soot aerosol, varied from 4 % to 94 % with a median of 40 %, indicating that the aerosol population lies in between internal and external mixing but has large temporal and source type variability. In addition, a significant fraction of BC-containing particles, a majority enriched with oxidized organics and sulfate, exhibit sufficiently high κ values and diameters conducive to activation as cloud nuclei under atmospherically relevant supersaturation conditions. This finding bears significance in comprehending the aging processes of rBC-containing particles and their activation into cloud droplets. Our analysis highlights the complex nature of soot aerosol and underscores the need to comprehend its variability across different environments for accurate assessment of climate change.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Biofuels as Heavy Fuel Oil Substitutes in the Maritime Sector: Findings and Potential Pathways

The United States Department of Energy has commissioned four national laboratories to evaluate the feasibility of biofuels in the maritime sector. This effort is briefly described including the overall project goals, structure and aims. The large two-stroke crosshead engines used to power large merchant vessels were of particular interest since they can burn lower combustion quality fuels relative to four-stroke engines. This characteristic allows for consideration of pyrolysis oils and hydrothermal liquefaction (HTL) oils which are feedstock agnostic and, in the raw state, are more economical compared to distillate drop-in fuels. Pyrolysis and HTL oils are collectively known as bio-intermediates since they require additional processing for use in distillate fuel systems. The key limiting feature is that these bio-intermediate fuels will cause asphaltene precipitation when blended with heavy fuel oils (HFOs) such as very low sulfur fuel oil (VLSFO) unless they are upgraded to remove water and oxygenates. Economics are the key driver at this point in time, and preliminary techno-economic analyses (TEAs) indicate that bio-intermediates have potentially lower cost relative to other biofuels such as biodiesel and renewable diesel. Additionally, life cycle analyses (LCAs) of feedstocks and pathways show the life cycle carbon reduction benefit relative to heavy fuel oils. In addition to TEA and LCA results, we also present on the technical feasibility of these fuels. These studies have focused on the properties of biofuel blends with VLSFO that are critical to the fuel systems of maritime vessels fueled with HFOs. These properties include the compatibility with fuel system metals, viscosity, and blend stability. Aging studies with blends of VLSFO with biodiesel, HTL, and pyrolysis oils are also presented. Future efforts being planned to conduct additional biofuel testing, including the use of biofuels as pilot fuels in zero carbon shipping options fueled with ammonia and methanol, ship-based demonstrations, and bioresource competition studies.

Kass, Michael↗