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DOE OSTI2021

Examining Nuisance Aerosol Detections in Light of the Origin of the Screening Process (November 2021)

The evolution of philosophy and computations in the International Data Center (IDC) related to aerosol samples have had profound impacts on the number of recorded detections in the network since routine operations began in 2000. Key decisions from policymakers have been the list of triggering radionuclides, the scheme for categorizing these into interest levels 1-5, and an algorithm for determining when an anthropogenic isotope is seen so often that it is no longer interesting, known as the Exponential Weighted Moving Average (EWMA). These are described in the Operations Manual of the IDC. Key parameters that are controlled by the IDC but for which the IDC receives occasional input from policymakers include the constants in EWMA and the peak significance threshold for individual gamma rays, the latter of which directly leads to determination of the presence or absence of a radionuclide in a sample. There are also changes in computations which the IDC makes and informs policy makers about, such as changes in how background is computed, which could also affect the ease of detecting a peak – real or false. Rather than focus on the quantitative changes due to computation changes, this work records some thinking on how isotopes and peak significance levels were chosen, and the resulting detections seen over 18 years during the buildup of the International Monitoring System (IMS). These detections are considered on a global scale to try to determine the relative impact on monitoring, and in some cases, the nature of their existence. Repeated detections of 131I and 133I are the most troublesome, but they are not so frequent to be a major problem for the Verification Regime. These detections could probably be handled adequately using scientific methods currently under development for xenon backgrounds. It is also somewhat problematic that top-level analysis of aerosol backgrounds has not been reported previous to this. The steep increase in the rate of detections after 2016 are a concern, either in the actual backgrounds or from changes in the calculations methods used to generate the Reviewed Radionuclide Report (RRR.) Final conclusions of the authors are that the computational stability of the RRR is very important. With computational stability, changes can be usefully analyzed as being due to changes in radioactivity in Earth’s atmosphere This report is a distillation into text of a talk given in the Radionuclide Experts Group (RNEG) in Vienna during Working Group B (WGB) in February of 2019. This report does not directly contain any IDC data, only summaries by year, or by isotope, or by location. No specific IDC detection by time, location, or isotope is included.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2023

Impact of Wildfires on Solar Resource Availability in California in a Changing Climate

Wildfires can emit large amounts of atmospheric particulate matters and influence not only air quality but also availability of photovoltaic (PV) generation due to scattering and absorption of solar radiation. Under anthropogenic changing climate, wildfire activity is projected to increase over western North America due to drier and warmer climate, implying increasing impact on solar resource and larger uncertainty in solar generation especially in regions with faster PV penetration. This study focuses on quantifying the impact of wildfires on aerosol optical depth (AOD) and thus solar resource over California using National Solar Radiation Database (NSRDB), developed by the National Renewable Energy Laboratory (NREL). This assessment includes historical analysis and estimation of solar resource under wildfire scenarios (2020 wildfire and an enhanced wildfire scenario based on 2020 wildfires). Historical analysis for the period of July-October 2019/2020 (low/high fire activity period) shows that the averaged global horizontal irradiance (GHI) and direct normal irradiance (DNI) are reduced by about 30 and 90 W m-2 (5.6 and 15.3%), respectively, during high fire activity period. To create AOD dataset for enhanced fire scenario, 165% increase in burn area (in around 2050) is selected based on comprehensive literature review, which is further applied to the Fire INventory from NCAR (FINN) fire emission. WRF-Chem model with the enhanced FINN emissions is used to simulate and represent a preserving spatial distribution of burned areas and wildfire-emitted aerosols. Our initial analysis suggests that the"enhanced 2020 wildfire" AOD can increase by a factor of 1.3 - 2, which can significantly reduce solar irradiance and increase uncertainty in generation and reliability of power system in extreme wildfire events under a high solar penetration scenario. Overall, this study provides an estimate of the impacts of wildfires on solar resource to make informed decisions on reserve planning, generation scheduling, and reliability investments.

aerosol optical depth↗

DOE OSTI2020

Revisiting particle dry deposition and its role in radiative effect estimates

Wet and dry deposition remove aerosols from the atmosphere, and these processes control aerosol lifetime and thus impact climate and air quality. Dry deposition is a significant source of aerosol uncertainty in global chemical transport and climate models. Dry deposition parameterizations in most global models were developed when few particle deposition measurements were available. However, new measurement techniques have enabled more size-resolved particle flux observations. We combined literature measurements with data that we collected over a grassland in Oklahoma and a pine forest in Colorado to develop a dry deposition parameterization. We find that relative to observations, previous parameterizations overestimated deposition of the accumulation and Aitken mode particles, and underestimated in the coarse mode. These systematic differences in observed and modeled accumulation mode particle deposition velocities are as large as an order of magnitude over terrestrial ecosystems. As accumulation mode particles form most of the cloud condensation nuclei (CCN) that influence the indirect radiative effect, this model-measurement discrepancy in dry deposition alters modeled CCN and radiative forcing. We present a revised observationally driven parameterization for regional and global aerosol models. Using this revised dry deposition scheme in the Goddard Earth Observing System (GEOS)-Chem chemical transport model, we find that global surface accumulation-mode number concentrations increase by 62% and enhance the global combined anthropogenic and natural aerosol indirect effect by −0.63 W m −2 . Our observationally constrained approach should reduce the uncertainty of particle dry deposition in global chemical transport models.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

ARM Aerosol Measurement Science Group 2019 Strategic Planning Workshop Report

This report summarizes the results of a U.S. Department of Energy Atmospheric Radiation Measurement (ARM) user facility workshop held in November 2019 to advance a science-based strategy for ARM’s aerosol measurement program. This was the second such workshop since the Aerosol Measurement Science Group (AMSG) was chartered in 2015 to enhance coordination of ARM observations of aerosols and atmospheric trace gases with the needs of ARM users. The results presented here reflect the AMSG’s focus in recent years on science-based strategies that will contribute to the increased use of ARM data to fulfill its mission of improving process representations and predictability in climate models. Sessions held during the workshop range from interfacing with models through aerosol sampling strategies to calibration protocols and data products. The AMSG workshops have been designed to recommend actions that will enable ARM to evolve and continue to meet its mission. To that end, the AMSG will develop an actionable plan from the recommendations outlined here. Some are well defined and can reasonably be accomplished in the short term. Others are less definite or of a larger scope that calls for a longer-term implementation. Further discussion will be required to develop and prioritize actionable items related to such areas. Task teams comprising the appropriate expertise and perspective from the AMSG and other members of the community will be formed to achieve this outcome. Some particular topics are recognized as high priority, so plans are underway to develop task teams and to hold follow-on discussions to address them. Four areas currently being considered for short, focused discussion are 1) aerosol measurements on the North Slope of Alaska, 2) improving data usability for modeling, 3) strategies for advancing remote sensing, vertical profiling, and distributed measurements of aerosols, and 4) aerosol sampling strategies at existing ARM sites to provide intensive modes of operation to promote data usage for process and modeling studies.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Improving Predictability of Mixed-Phase Clouds and Aerosol Interactions in the Community Earth System Model (CESM) with ARM Measurements

The objective of this project is to improve the simulation and predictability of mixed-phase clouds and aerosol interactions in the Community Earth System Model (CESM) through comparisons with the DOE ARM observations. There are four major goals of the proposed study: (1) Improve the representation of ice microphysical processes in mixed-phase clouds; (2) Develop a long-term multi-sensor mixed-phase cloud dataset; (3) Test the performance of improved ice microphysics in CESM-CAM5 with the ARM data; and (4) Examine mixed-phase cloud microphysics-aerosol-dynamics-radiation interactions in CESM-CAM5. In this project, we have (1) Improved the representation of ice microphysical processes in mixed-phase clouds that include ice nucleation, ice depositional growth through the Wegener–Bergeron–Findeisen (WBF) process, feedbacks between cloud microphysics, dynamics and radiation, and provides links to aerosol properties in the Community Earth System Model (CESM)-Community Atmosphere Model version 5 (CAM5); (2) Developed a long-term multi-sensor mixed-phase cloud dataset. The mixed-phase cloud retrieval algorithms are improved by refining the phase determinations and ice number concentration retrievals. A multi-year mixed-phase cloud observation dataset (1999-2004; October 2013-February 2017) is regenerated at the ARM Barrow site with the improved algorithms. The dataset has been used in the global model evaluation to improve the model parameterizations; (3) Tested the performance of improved ice microphysics in CESM-CAM5 with the ARM data. CESM-CAM5 is run in the DOE Cloud-Associated Parameterizations Testbed (CAPT) and in the single-column model (SCM) mode to facilitate comparison with ARM observations. Multi-year CAPT simulations of seasonal variations of cloud microphysical properties, cloud liquid water path (LWP) and ice water path (IWP), cloud longwave and shortwave forcings, cloud occurrence frequency are evaluated against the ARM multi-sensor mixed-phase cloud retrievals; and (4) Examined mixed-phase cloud microphysics-aerosol-dynamics-radiation interactions in CESM-CAM5 that include the impacts of different ice nucleation mechanisms, sensitivity to dust IN concentration, treatment of the WBF process on mixed-phase cloud properties. Aerosol effect on mixed-phase clouds through the liquid phase (droplet activation) and ice phase processes (e.g., the glaciation indirect effect) is investigated.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Aerosol Inlets for a Mid-Sized Uncrewed Aerial System (UAS)

The purpose of this technical report is to document the efforts to design and test two inlet systems for aerosol sampling suitable for deployment on a medium-sized fixed-wing Uncrewed Aerial System (UAS). This work, which was supported by the U.S. Department of Energy’s Atmospheric Radiation Measurement (ARM) user facility, was conducted at the Pacific Northwest National Laboratory (PNNL) for the ARM Aircraft Facility (AAF) starting in November 2017. The current work is a part of AAF efforts to instrument the ArcticShark (a mid-sized UAS owned and operated by the AAF) for atmospheric research and develop a scientific payload for deployment on a similar-sized UAS with minimal adaptation and integration. An aerosol inlet system is necessary to sample and transport ambient air sample to the scientific instrumentation with minimal distortions to the aerosols. Two isokinetic aerosol inlets were designed: the first is a simple passive system for a single instrument suitable to be installed in a wing pylon; the second is a system with active control designed to sample and distribute air among several heterogeneous instruments and to provide basic humidity control of the air sample so that the measured aerosol parameters should correspond to “dry” conditions (a common requirement). Both systems could be easily adapted for deployment on another platform and/or with a different set of instrumentation. Several conducted flight tests showed that the inlets’ performance met our design goals.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Aerosol Inlets for a Mid-Sized Uncrewed Aerial System (UAS)

42 ENGINEERING↗

DOE OSTI2022

Regularized inversion of aerosol hygroscopic growth factor probability density function: application to humidity-controlled fast integrated mobility spectrometer measurements

Abstract. Aerosol hygroscopic growth plays an important role in atmospheric particle chemistry and the effects of aerosol on radiation and hence climate. The hygroscopic growth is often characterized by a growth factor probability density function (GF-PDF), where the growth factor is defined as the ratio of the particle size at a specified relative humidity to its dry size. Parametric, least-squares methods are the most widely used algorithms for inverting the GF-PDF from measurements of the humidified tandem differential mobility analyzer (HTDMA) and have been recently applied to the GF-PDF inversion from measurements of the humidity-controlled fast integrated mobility spectrometer (HFIMS). However, these least-squares methods suffer from noise amplification due to the lack of regularization in solving the ill-posed problem, resulting in significant fluctuations in the retrieved GF-PDF and even occasional failures of convergence. In this study, we introduce nonparametric, regularized methods to invert the aerosol GF-PDF and apply them to HFIMS measurements. Based on the HFIMS kernel function, the forward convolution is transformed into a matrix-based form, which facilitates the application of the nonparametric inversion methods with regularizations, including Tikhonov regularization and Twomey's iterative regularization. Inversions of the GF-PDF using the nonparameteric methods with regularization are demonstrated using HFIMS measurements simulated from representative GF-PDFs of ambient aerosols. The characteristics of reconstructed GF-PDFs resulting from different inversion methods, including previously developed least-squares methods, are quantitatively compared. The result shows that Twomey's method generally outperforms other inversion methods. The capabilities of Twomey's method in reconstructing the pre-defined GF-PDFs and recovering the mode parameters are validated.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Coupled Air Quality and Boundary-Layer Meteorology in Western U.S. Basins during Winter: Design and Rationale for a Comprehensive Study

The wintertime episodes of high aerosol concentrations occur frequently in urban and agricultural basins and valleys worldwide. These episodes often arise following development of persistent cold-air pools (PCAPs) that limit mixing and modify chemistry. While field campaigns targeting either basin meteorology or wintertime pollution chemistry have been conducted, coupling between interconnected chemical and meteorological processes remains an insufficiently studied research area. Gaps in understanding the coupled chemical–meteorological interactions that drive high-pollution events make identification of the most effective air-basin specific emission control strategies challenging. To address this, a September 2019 workshop occurred with the goal of planning a future research campaign to investigate air quality in western U.S. basins. Approximately 120 people participated, representing 50 institutions and five countries. Workshop participants outlined the rationale and design for a comprehensive wintertime study that would couple atmospheric chemistry and boundary layer and complex-terrain meteorology within western U.S. basins. Participants concluded the study should focus on two regions with contrasting aerosol chemistry: three populated valleys within Utah (Salt Lake, Utah, and Cache Valleys) and the San Joaquin Valley in California. This paper describes the scientific rationale for a campaign that will acquire chemical and meteorological datasets using airborne platforms with extensive range, coupled to surface-based measurements focusing on sampling within the near-surface boundary layer, and transport and mixing processes within this layer, with high vertical resolution at a number of representative sites. No prior wintertime basin-focused campaign has provided the breadth of observations necessary to characterize the meteorological–chemical linkages outlined here, nor to validate complex processes within coupled atmosphere–chemistry models.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

The Surface Atmosphere Integrated Field Laboratory (SAIL) Campaign

The science of mountainous hydrology spans the atmosphere through the bedrock and inherently crosses physical and disciplinary boundaries: land-atmosphere interactions in complex terrain enhance clouds and precipitation, while watersheds retain and release water over a large range of spatial and temporal scales. Limited observations in complex terrain challenge efforts to improve predictive models of the hydrology in the face of rapid changes. The Upper Colorado River exemplifies these challenges, especially with ongoing mismatches between precipitation, snowpack, and discharge. Consequently, the U.S. Department of Energy’s (DOE) Atmospheric Radiation Measurement (ARM) user facility has deployed an observatory to the East River Watershed near Crested Butte, Colorado between September 2021 and June 2023 to measure the main atmospheric drivers of water resources, including precipitation, clouds, winds, aerosols, radiation, temperature and humidity. This effort, called the Surface Atmosphere Integrated Field Laboratory (SAIL), is also working in tandem with DOE-sponsored surface and subsurface hydrologists and other federal, state, and local partners. SAIL data can be benchmarks for model development by producing a wide range of observational information on precipitation and its associated processes, including those processes that impact snowpack sublimation and redistribution, aerosol direct radiative effects in the atmosphere and in the snowpack, aerosol impacts on clouds and precipitation, and processes controlling surface fluxes of energy and mass. Preliminary data from SAIL’s first year showcase the rich information content in SAIL’s many data-streams and support testing hypotheses that will ultimately improve scientific understanding and predictability of Upper Colorado River hydrology in 2023 and beyond.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Review and Assessment of Available Data Regarding the Behavior of Sodium Aerosols

Recently, there has been a resurgence of interest in advanced (non-light water) reactor designs, including sodium fast reactors (SFRs). In parallel, multiple efforts are underway to develop risk informed, performance-based licensing pathways for advanced reactors. However, such licensing approaches depend on the accuracy of the associated safety assessments, including mechanistic source term (MST) analyses. Unlike historical source term assessments, which utilizes bounding estimates of radionuclide release, MSTs attempt to realistically estimate the transport and retention of radionuclides for specific transient scenarios. For SFR MST analyses, the behavior of radionuclide aerosols is a key factor, as noted in recent studies. Due to the use of sodium as the primary coolant, many potential transient scenarios involve the release of radionuclide aerosols in conjunction with sodium aerosols. For such scenarios, sodium may be the dominant aerosol species, compared to that of released radionuclides. Therefore, understanding the behavior of sodium aerosols is particularly important to an accurate assessment of aerosol transport. Although many approaches to aerosol modeling exist, it is vital to establish their capabilities in evaluating sodium aerosol behavior for SFR analyses.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2021

Subtask 2.6 – Optimization of Aerosol Mitigation Technology for Postcombustion CO 2 Capture

Growing concerns over the impact of CO 2 emissions from combustion sources on global climate change have prompted numerous research and development projects aimed at developing cost-effective technologies for CO 2 capture. One family of technologies being demonstrated at pilot and full scale globally is postcombustion CO 2 capture (PCCC) systems that employ amine-based solvents. The captured CO 2 can be compressed and permanently stored underground or used for enhanced oil recovery (EOR). The proximity of North Dakota’s lignite-fired fleet of power plants to potential CO 2 storage options creates a unique atmosphere for PCCC within the state. However, the aerosols present in lignite flue gas present a challenge for large-scale PCCC at North Dakota power plants. Aerosols can negatively impact the long-term performance of amine-based solvents for CO 2 capture. Amine-based solvents are volatile, and aerosols provide nucleation sites where amine vapors can condense. Because aerosols cannot be easily captured at the column outlet using conventional technologies, the amine-laden aerosols escape the system and lead to accelerated solvent losses. Moreover, aerosol components can chemically react with amines to form degradation products that can permanently deactivate the amine, cause fouling, and lead to hazardous emissions. Many of the elements that have been shown to catalyze solvent degradation are present in lignite coals and can exacerbate solvent replacement economics. Understanding this issue is critical to the implementation of solvent-based CO 2 capture systems as applied to lignite-fired generation systems. The Energy & Environmental Research Center (EERC) designed and carried out this project to optimize aerosol mitigation technology for PCCC at a lignite-fired power plant. To meet the goal of this project, the following objectives were identified: Determine the effectiveness of a wet electrostatic precipitator (WESP) on collection of aerosols at a low-rank coal-fired power station. Determine the impact of aerosols on the efficiency and degradation products of amine-based carbon capture systems fired with low-rank fuels. Work was conducted at Minnkota Power Cooperative’s (MPC’s) Milton R. Young (MRY) Station Unit 2 using a slipstream of flue gas from the outlet of the plant’s flue gas desulfurization (FGD) unit. To gather initial data for sizing and specifying a WESP for this system, a temporary pilot-scale WESP was rented and installed on-site. Several different conditions were tested to examine the impact of flow rate, voltage, and current on WESP performance. The WESP was effective at removing large particulate (>200 nm) but caused an increase in fine particulate (<75 nm). Fine particulate material at the inlet and outlet of the WESP was collected, analyzed, and showed that crystalline sulfates carried over from the plant’s FGD unit were being converted to fine aerosols and SO 2 was being converted to SO 3 through the WESP. Additionally, the high moisture content of the flue gas stream at this sample location also contributed to an overall increase in aerosol mass under some of the test conditions. Using the results from the rented WESP, the project team installed a smaller-scale WESP upstream of the EERC’s slipstream CO 2 capture system. Flue gas was routed through a pilot-scale FGD unit to remove SO 2 to very low levels (~1 ppm) and then through a direct contact cooler (DCC) to further cool the gas and to remove moisture. The gas exiting the DCC was then routed through the new WESP before passing to the CO 2 absorber columns. Fluor’s amine-based solvent was used to scrub CO 2 from the slipstream through a set of two absorber columns. The rich solvent was regenerated in a stripper column by heating to drive off captured CO 2 . The system operated using a catch-and-release method where the CO 2 was separated to provide data on the process, but the captured CO 2 was released back into the host site stack. Aerosols and sulfur species were measured at multiple locations throughout the pilot-scale system. The inlet FGD and DCC removed much of the particulate matter and gaseous sulfur upstream of the WESP. With this configuration, the WESP achieved >95% particulate capture. The new WESP did not show any of the increases in SO 3 or other aerosol species that had been consistently observed with the larger-scale WESP installed immediately downstream of the plant’s full-scale FGD unit. Particulate samples captured and analyzed from the WESP inlet did not show any presence of crystalline sulfate materials, indicating that the pilot-scale FGD and DCC were efficient at reducing carryover from the plant’s full-scale FGD unit. A set of parametric tests were conducted on the new WESP to assess the impacts of flow rate, voltage, number of online WESP fields, and gas-phase sulfur content on aerosol and sulfur transformations. The results showed that the WESP performed similarly well at all sets of conditions. Sulfur and particulate matter exiting the WESP were further reduced through the absorber column as the amine-based solvent captured some of the residual contaminants. Solvent analysis showed that these species were slowly concentrating in the solvent over the duration of the test. When the WESP was taken offline and the sulfur slip through the FGD allowed to rise, the sulfate content in the solvent rose sharply, showing that the extra FGD and WESP were effective at reducing sulfate and cation uptake. This would be expected to extend amine-based solvent life by slowing the formation of heat-stable salts and other degradation products. This subtask was cofunded through the EERC–U.S. Department of Energy Joint Program on Research and Development for Fossil Energy-Related Resources Cooperative Agreement No. DE-FE0024233. Nonfederal funding was provided by the North Dakota Industrial Commission and MPC.

01 COAL, LIGNITE, AND PEAT↗

DOE OSTI2021

Topical Report – Findings on Subtask 2.7 – Wet ESP and Aerosol Testing at Coal Creek Station

Growing concerns over the impact of CO 2 emissions from combustion sources on global climate change have prompted numerous research and development projects aimed at developing cost-effective technologies for CO 2 capture. One family of technologies being demonstrated at pilot and full scale globally is postcombustion carbon capture (PCCC) systems that employ amine-based solvents. The captured CO 2 can be compressed and permanently stored underground or used for enhanced oil recovery. The proximity of North Dakota’s lignite-fired fleet of power plants to potential CO 2 storage options creates a unique atmosphere for PCCC within the state. However, the unique components present in lignite flue gas present a challenge for large-scale PCCC at North Dakota power plants by contributing to aerosol formation. Aerosols can negatively impact the long-term performance of amine-based solvents for CO 2 capture. Amine-based solvents are volatile, and flue gas particulate provides nucleation sites where amine vapors can condense as aerosols. Because aerosols cannot be easily captured at the column outlet using conventional technologies, the amine-laden aerosols escape the system and lead to accelerated solvent losses. Moreover, particulate components can chemically react with amines to form degradation products that can permanently deactivate the amine, cause fouling, and lead to hazardous emissions. Many of the elements that have been shown to catalyze solvent degradation are present in lignite coals and can exacerbate solvent replacement economics. Understanding this issue is critical to the implementation of solvent-based CO 2 capture systems as applied to lignite-fired generation systems. The Energy & Environmental Research Center (EERC) designed and carried out this project to fully characterize aerosol behavior with various control technologies installed to better optimize aerosol mitigation technology for CO 2 capture. To meet the goal of this project, the following objectives were identified: Determine the effectiveness of a wet electrostatic precipitator (WESP) on mitigating formation of problematic aerosols at Great River Energy’s Coal Creek Station, upstream of the PCCC system. Determine the effectiveness of the Mitsubishi Heavy Industries (MHI) proprietary amine emission reduction unit (AERU) as a postcapture solvent recovery system for reducing aerosol emissions and extending solvent life downstream of the PCCC system. Determine the impact of aerosols on the efficiency and degradation products of both commercial and advanced solvents within the PCCC system. Work was conducted at Coal Creek Station Unit 1 using a slipstream of flue gas from the outlet of the plant’s flue gas desulfurization (FGD) unit. Flue gas was routed through a pilot-scale FGD unit to remove SO 2 to very low levels (~1 ppm) and then through a direct contact cooler (DCC) to further cool the gas and to remove moisture. The gas exiting the DCC was then optionally routed through a WESP before passing to the CO 2 absorber columns. The MHI solvent was used to scrub CO 2 from the slipstream through a set of two absorber columns. The rich solvent was regenerated in a stripper column by heating to drive off captured CO 2 . Flue gas exiting the absorber column was routed to MHI’s proprietary AERU to recover entrained solvent. The system operated using a catch-and-release method where the CO 2 was separated to provide data on the process, but the captured CO 2 was released back into the host site stack. Particulate was measured, collected, and analyzed from multiple locations throughout the pilot-scale system. Unlike the performance observed in prior work, the inlet FGD and DCC did not remove significant particulate matter from the flue gas. This appears to be due to a difference in the nature of the particulate. The DCC seemed to increase particulate size and count, most likely owing to water condensing onto the surfaces of fly ash particles. When the WESP was operated, it achieved >95% particulate capture. Very little particulate matter or indications of solvent were detected at the AERU outlet. When operating with advanced KS 21 solvent, the particulate material at the AERU outlet was even further decreased. Solvent analysis showed that some species derived from flue gas and ash were slowly concentrating in the solvent over the duration of the test. The levels observed were reported to be within expected ranges and were not of concern to MHI. A high-level techno-economic assessment of installing CO 2 capture at Coal Creek Station suggested that, when using a standard monoethanolamine (MEA)-based solution with simple heat integration, the energy penalty to net generation would be 34%. The bulk of this was due to steam losses for regenerating solvent, followed by parasitic electrical demand for CO 2 compression and then by increased parasitic load for pushing flue gas through the absorber column. These demands could be decreased with a more advanced solvent that exhibits lower heat of regeneration and lower pressure drop than does a simple MEA solution. Further energy could be saved with more thorough heat integration to recover useful energy from the steam used for solvent regeneration. Installing a WESP was predicted to increase the cost of electricity by nearly $5/MWh. This would become cost-effective if solvent losses were roughly 10 times the baseline estimate when not using a WESP but could be returned to baseline by installing the WESP. Piping CO 2 for storage in more favorable geology could help with carbon capture and storage economics. Although storing off-site would necessitate construction of a CO 2 transport pipeline, the cost of this pipeline might be more than offset by reducing the number of wells required, the depths of the wells required, and the electrical demand for the CO 2 compressor. Additional factors that favor off-site storage costs include smaller expected CO 2 plume sizes, which translates to less monitoring and fewer landowner agreements. More detailed assessment of the specific geology in the region under and around Coal Creek Station would be needed to accurately assess the costs and benefits of different storage site options. This subtask was cofunded through the Energy & Environmental Research Center–U.S. Department of Energy Joint Program on Research and Development for Fossil Energy-Related Resources Cooperative Agreement No. DE-FE0024233. Nonfederal funding was provided by the North Dakota Industrial Commission.

Strege, Joshua↗

DOE OSTI2026

Strong Sensitivity of Simulated Biomass Burning Aerosol Transport and Radiative Effects Over the South Atlantic to Carbonaceous Aerosol Aging and Particle Density

Biomass burning aerosol (BBA) impacts climate through aerosol‐cloud‐radiation interactions, but models disagree on the sign and magnitude of BBA radiative effects. We quantify the sensitivity of BBA radiative effects and transport to three BBA‐relevant processes and properties: parameterized oxidative aging of organic aerosol (OA), a combined change to black carbon (BC) density and the method for calculating aerosol refractive index, and reduction in OA density. We evaluate Unified Model simulations against two aircraft campaigns from summer 2017 over the Southeast Atlantic. The model generally performs well, such that discrepancies between the observational data sets may sometimes limit the precision of the evaluation. Our newly developed aging parameterization reproduces observed OA:BC mass ratios well and allows modeled OA:BC to decrease with smoke age, but increases bias in aerosol extinction and changes the BBA radiative effect little (+0.12 W m -2 ). We calculate aerosol refractive index using either a volume‐weighted component average or the Maxwell‐Garnett (MG) mixing assumption, which represents BC as small inclusions in a host material. Compared to MG mixing, the volume‐weighted average refractive index and reduced BC density increase aerosol absorption, substantially increasing the total BBA radiative effect (+2.66 W m -2 ) and amount of BBA transported across the ocean through BC self‐lofting. Reducing OA density to better match literature values changes the total BBA radiative effect by −1.96 W m -2 . Changes to direct radiative effects exceed changes to cloud radiative effects. Our findings emphasize the sensitivity of aerosol radiative effects and transport to these processes and properties, which we suggest could be improved in climate models.

Southeast Atlantic↗

DOE OSTI2025

Coupling of Lipid Peroxidation and Criegee Intermediate Mediated Autoxidation in the Heterogeneous Oxidation of Linoleic Acid Aerosols

Autoxidation is an established mechanism for the degradation of organic molecules, which is relevant in the atmosphere, combustion processes, the environment, and the rancidification of lipids (commonly known as lipid peroxidation). Autoxidation proceeds via radical chain reactions involving hydroxyl (•OH), peroxy (RO2•), and alkoxy radicals, which are also prominent oxidants in the atmosphere. Recent reports have provided evidence for an alternative autoxidation mechanism driven instead by Criegee intermediates (CIs), which are produced from the reaction of β-hydroxy peroxy radicals (β-OH-RO2•). This work evaluates the contributions of these two mechanisms in the •OH initiated heterogeneous oxidation of linoleic acid (LA) aerosols. Reaction kinetics and product distributions are monitored using a vacuum ultraviolet photoionization aerosol time-of-flight mass spectrometer. To explain the observed kinetics, a kinetic model is developed that incorporates both the conventional peroxidation and alternative CI-mediated autoxidation mechanisms. We observe that the CI-mediated autoxidation pathways enhance the heterogeneous autoxidation rate, while the peroxidation reactions, although present, contributes less to the overall oxidation rate. α-Acyloxyalkyl hydroperoxides (AAHPs) are identified as key indicators for bimolecular reactions of CI with LA, highlighting the role of LA as a CI scavenger. Moreover, the measured functionalized LA products with hydroxyl or carbonyl group(s), serve as markers for the peroxidation reactions. In summary, this work presents a quantitative framework to understand the coupled reaction network of •OH, RO2•, β-OH-RO2• radicals, and CI in driving heterogeneous autoxidation, which is crucial for understanding degradation mechanisms of organic molecules in the environment and atmosphere.

Criegee intermediate↗

DOE OSTI2025

Location generalizability of image-based air quality models

This paper is to be submitted at the IEEE/CVF Winter Conference on Applications of Computer Vision (WACV) Computer Vision for Earth Observation workshop. The full paper abstract is below: The ability to rapidly quantify atmospheric pollutants is important both for global emissions monitoring and for mitigating the adverse effects that follow a hazardous chemical release. In the aftermath of a chemical release, imagery is often the only available resource to assess local conditions. Recent work has demonstrated initial success in predicting particulate matter pollution from imagery; however, these results are tied to a specific site and do not generalize to new geographic locations. In this work, we seek to understand how easily deep learning models generalize to new locations in the context of image-based air quality assessments, targeting two distinct tasks: (1) broad measures of particulate matter pollution, and (2) the mass of a given chemical released in hazardous plumes. For the latter, we focus on sulfur dioxide, a toxic aerosol and a major component of particulate matter pollution caused by industrial fossil fuel consumption. To develop a model that operates in the widest possible range of environments, we test different training strategies, including the use of new geolocation foundation models. The best performing models achieve >80% accuracy when evaluating unseen imagery at previously seen sites, but we find significant drops in performance when evaluating imagery from unseen sites, at best 65%. Additionally, we present the public release of the National Parks Air Quality Index Dataset, a new medium-sized dataset that pairs imagery with sensor-based air quality measurements at 15 different national parks.

Byler, Eleanor B. [BATTELLE (PACIFIC NW LAB)]↗

DOE OSTI2023

Deep Learning Parameterization of Vertical Wind Velocity Variability via Constrained Adversarial Training

Atmospheric models with typical resolution in the tenths of kilometers cannot resolve the dynamics of air parcel ascent, which varies on scales ranging from tens to hundreds of meters. Small-scale wind fluctuations are thus characterized by a subgrid distribution of vertical wind velocity W with standard deviation σ W . The parameterization of σ W is fundamental to the representation of aerosol–cloud interactions, yet it is poorly constrained. Using a novel deep learning technique, this work develops a new parameterization for σ W merging data from global storm-resolving model simulations, high-frequency retrievals of W , and climate reanalysis products. The parameterization reproduces the observed statistics of σ W and leverages learned physical relations from the model simulations to guide extrapolation beyond the observed domain. Incorporating observational data during the training phase was found to be critical for its performance. The parameterization can be applied online within large-scale atmospheric models, or offline using output from weather forecasting and reanalysis products.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Cold-Air Outbreaks in the Marine Boundary Layer Experiment (COMBLE) Field Campaign Report

The Cold-Air Outbreaks in the Marine Boundary Layer Experiment (COMBLE) was conducted successfully between 1 December 2019 and 31 May 2020 around the Norwegian Sea. COMBLE deployed the U.S. Department of Energy Atmospheric Radiation Measurement (ARM) first Mobile Facility (AMF1) along the coast of northern Scandinavia, at an arctic latitude (70°N), and an array of additional instruments on Bear Island (75°N) in the Norwegian Sea. The instruments deployed at these two sites collected a large array of in situ and remote-sensing observations of atmospheric conditions, clouds, precipitation, and aerosol. The main objective of COMBLE is to quantify the properties of shallow convective clouds that develop as part of an air-mass transformation process when cold air blows over open water. The two COMBLE sites are located at ~1,200 km and ~500 km from the cold source, i.e., arctic ice edge, respectively.

54 ENVIRONMENTAL SCIENCES↗