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All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Soil Particulate Organic Matter is Related to Ericoid Mycorrhizal Shrubs, not Ectomycorrhizal Trees, in a Temperate Forest

Mycorrhizal associations are key drivers of soil biogeochemistry, but previous studies have focused almost exclusively on ectomycorrhizal (EcM) and arbuscular mycorrhizal (AM) associations. Ericoid mycorrhizal (ErM) shrubs frequently occur in forest understories and are expanding in response to disturbance, but are rarely considered in biogeochemical frameworks. We investigated the relationships of understory ErM shrubs and overstory trees on carbon (C) and nitrogen (N) in soil organic matter fractions in a southern Appalachian temperate forest. We sampled the 0–10 cm mineral soil layer from 43 plots at the Coweeta Hydrologic Laboratory, across gradients in overstory EcM dominance and understory ErM shrub biomass. Soil C:N ratios increased with both increasing EcM dominance and increasing ErM shrub biomass. However, total particulate organic matter (POM) C, and the proportion of C and N held in POM increased with increasing ErM shrub biomass, but not with increasing EcM dominance. In contrast, mineral-associated organic matter (MAOM) C and N were negatively associated with EcM dominance, but were not related to ErM shrubs. Our findings suggest that ErM shrubs facilitate POM formation while AM trees promote MAOM formation. Because ErM shrub biomass represents a small fraction of total forest biomass, our work provides evidence that ErM shrubs have an outsized effect on soil organic matter, which advocates for their inclusion in mechanistic studies and biogeochemical frameworks.

Bonilla, Kayla A. [University of Georgia, Athens, ↗
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

Investigation of Lubricant Additive Interactions on Gasoline Particulate Filters

To understand how the composition of novel lubricant additives and their ash interact with gasoline particulate filters (GPFs), an accelerated aging protocol was conducted using three lubricant additive formulations and two GPF types. The additive packages (adpaks) consisted of Ca+Mg detergent in a 3:1 or 0:1 ratio and an anti-wear component—either zinc dialkyl dithiophosphate (ZDDP) or a novel phosphonium-phosphinate ionic liquid (IL) substitute. The particulate sampling captured amount/compositions of particulate matter (PM) generated, total particulate number, and size distribution. Five ash loadings were completed. GPF position and adpak composition affected the backpressure, ash composition, ash morphology, and captured mass. The particulate sampling indicated that the ash component consisted primarily of particles less than 50 nm in size and that the Mg-only adpak resulted in more particulate of 50–400 nm in size. Postmortem materials characterization indicated GPFs in the underfloor position had deeper penetration of ash into the walls compared to the close-coupled position. Additionally, the Mg-only adpak had a higher filter collection efficiency (>90%) and the ash particles consisted of a higher concentration of dense ash material. In contrast, four of the 3:1 Ca:Mg lubricant adpaks resulted in a collection efficiency of only 40–50%. Although the collection efficiency was higher with the Mg-only adpak, the ash layer in the GPF was not thicker, nor was the penetration into the wall more significant, and surprisingly the full useful life (FUL) backpressure was lower than with Ca:Mg adpaks. The higher density of the Mg-derived ash was the only detectable difference. A possible explanation of this observation is that Mg ash has a lower melting point and is more susceptible to densification during combustion or GPF regeneration. The substitution of IL in place of the ZDDP did not lead to any notable changes in collection efficiency or location of the ash.

42 ENGINEERING↗
DOE OSTI2020

Constructing a spatiotemporally coherent long-term PM2.5 concentration dataset over China during 1980–2019 using a machine learning approach

The lack of long-term observations and satellite retrievals of health-damaging fine particulate matter in China has demanded the estimates of historical PM 2.5 (particulate matter less than 2.5 µm in diameter) concentrations. This study constructs a gridded near-surface PM 2.5 concentration dataset across China covering 1980–2019 using the space-time random forest model with atmospheric visibility observations and other auxiliary data. The modeled daily PM2.5 concentrations are in excellent agreement with ground measurements during 2015–2019, with a coefficient of determination of 0.95 and mean relative error of 12%. Besides the atmospheric visibility which explains 30% of total importance of variables in the model, both emissions and meteorological conditions are also essential factors affecting PM2.5 predictions. From 1980 to 2014, the model-predicted PM2.5 concentrations increased constantly with the maximum growth rate of 5–10 µg/m3/decade over eastern China. Due to the clean air actions, PM 2.5 concentrations have decreased effectively at a rate over 50 µg/m 3 /decade in the North China Plain and 20–50 µg/m 3 /decade over eastern China during 2014–2019. The newly generated dataset of 1-degree gridded PM 2.5 concentrations for the past 40 years across China provides a useful means for investigating interannual and decadal environmental and climate impacts related to aerosols.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Cooled Spray Technology for Particulate Reduction in a Heavy-Duty Engine

Cooled spray (CS) technology passively reduces particulate matter (PM) emissions from diesel engines compared to non-CS-equipped diesel engines. CS inserts are mounted near the injector nozzle and control mixing so that the fuel and air can premix while limiting combustion near fuel-rich zones, thereby reducing the formation of particulate matter. CS components contain no moving parts and could be installed as a retrofit or built into new engines. However, CS technology is early in its development, and further investigations are needed to understand the overall performance implications and practicality of the technology. In this paper, we investigate several important aspects of CS, providing a clearer picture of some challenges and potential benefits of CS. Two alignment techniques are used to characterize measurement ease and bias, namely, an optical alignment and spray-plug impact alignment. While the optical technique facilitates alignment more easily, a bias was measured between the optical and spray-plug techniques, suggesting the optical technique may have insufficient accuracy without additional corrections. We also evaluate the engine performance of a well-aligned and poorly aligned CS insert, compared to the baseline configuration. The poorly aligned insert shows slower combustion than the baseline and mixed overall performance. However, the well-aligned insert shows faster combustion than the baseline and PM emission reduction at most operating conditions, with some conditions showing PM reduction up to 80%. Furthermore, the results of this paper highlight the alignment challenges of CS technology as well as the potential PM reduction benefit of the technology.

33 ADVANCED PROPULSION SYSTEMS↗
DOE OSTI2025

Biochemical Conversion of Herbaceous Biomass to Renewable Diesel: Net Greenhouse Gas and Air Pollutant Trade-offs

This study examines greenhouse gas (GHG) and criteria air pollutant (CAP) emissions trade-offs for renewable diesel across 12 scenarios, involving different biochemical conversion designs, biorefinery scales, and feedstocks. A conventional design uses lignin for on-site heat and power, which exports excess power to the grid. An alternative design exports lignin pellets, offsetting other pellet production methods but requiring grid electricity to meet biorefinery power demands. Net emissions were quantified in Iowa and Georgia, selected considering feedstock availability, coproduct displacement, and regional power grids, assuming grid-exported power avoids coal or low-carbon electricity. Results for the conventional design remained consistent across the electricity displacement scenarios. When comparing lignin utilization strategies, pelletizing lignin reduces sulfur dioxide, carbon monoxide, nitrogen oxides, and volatile organic compounds (net emissions –0.66 mg MJ –1 , 25 mg MJ –1 , 25 mg MJ –1 , 7.8 mg MJ –1 , respectively). However, lignin pelletization increases net particulate matter (fine and coarse) and ammonia (net emissions of 4.7 mg MJ –1 , 13 mg MJ –1 , and 0.26 mg MJ –1 , respectively), alongside indirect GHG emissions due to grid electricity dependence. Additionally, processing 2000 tonnes corn stover daily minimizes emissions for both designs. Only lignin pelletization with renewable electricity and additional particulate matter and ammonia controls reduces all CAP and GHG emissions simultaneously.

09 BIOMASS FUELS↗
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 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 OSTI2022

Ambient Aerosol Is Physically Larger on Cloudy Days in Bondville, Illinois

Particle chemical composition affects aerosol optical and physical properties in ways important for the fate, transport, and impact of atmospheric particulate matter. For example, hygroscopic constituents take up water to increase the physical size of a particle, which can alter the extinction properties and atmospheric lifetime. At the collocated AERosol RObotic NETwork (AERONET) and Interagency Monitoring of PROtected Visual Environments (IMPROVE) network monitoring stations in rural Bondville, Illinois, we employ a novel cloudiness determination method to compare measured aerosol physicochemical properties on predominantly cloudy and clear sky days from 2010 to 2019. On cloudy days, aerosol optical depth (AOD) is significantly higher than on clear sky days in all seasons. Measured angstrom ngstro''m exponents are significantly smaller on cloudy days, indicating physically larger average particle size for the sampled populations in all seasons except winter. Mass concentrations of fine particulate matter that include estimates of aerosol liquid water (ALW) are higher on cloudy days in all seasons but winter. More ALW on cloudy days is consistent with larger particle sizes inferred from angstrom ngstro''m exponent measurements. Aerosol chemical composition that affects hygroscopicity plays a determining impact on cloudy versus clear sky differences in AOD, angstrom ngstro''m exponents, and ALW. This work highlights the need for simultaneous collocated, high-time-resolution measurements of both aerosol chemical and physical properties, in particular at cloudy times when quantitative understanding of tropospheric composition is most uncertain.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

A Laboratory Comparison of a Nephelometer and the Cavity-Attenuated Phase Shift Instrument (CAPS)

The interaction of incoming solar radiation (light) with particulate matter in the atmosphere impacts Earth’s radiation budget and thus is of great importance to climate and climate change. This particulate matter consists of particles, an aerosol referring to the ensemble of these particles. All particles scatter incoming solar radiation, sending some of it back to space and providing a cooling influence on the climate. Some particles additionally absorb incoming solar radiation, causing the particle, and the surrounding atmosphere, to heat, and thus altering atmospheric stability and evaporating water and other substances in the particles, which in turn affect the scattering and absorption of light by the particle.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

A Multi-Instrument Cloud Condensation Nuclei Spectrum Product (Final Technical Report)

A wealth of observational data exists on the characteristics of atmospheric particulate matter, over multiple years, at the DOE ARM Southern Great Plains (SGP) Central Facility site. This site is located in a region of the country that frequently experiences weather extremes, and that is removed from many local sources of pollution but is affected by transported smoke, dust, and urban emissions. The relationships between particulate matter, cloud formation and evolution, and precipitation are therefore of strong interest, and are being explored via modeling on a variety of scales. These models require as input detailed information on the characteristics of particles capable of serving as the nuclei for cloud formation. Sufficient data exist to be able to put together a picture of the nature of the total aerosol and the cloud condensation nuclei (CCN) subset, and their variability, through merged data products. This study was aimed at exploiting the multiple measurement types at SGP to develop the first such multi-year estimates. Further, the resulting data were analyzed to understand temporal patterns ranging from hourly to seasonal, thereby gaining insights into the particle sources affecting the atmosphere in this region. DOE-funded datasets that were analyzed in this study include total particle number concentrations, submicron aerosol scattering coefficients, dry aerosol size distributions, and more recently, time-resolved submicron aerosol chemical composition. Data are also available for the number concentrations of particles that are activated in a cloud condensation nucleus instrument at a series of setpoint supersaturations, providing direct observations of the number concentrations of “CCN”. This variable is the quantity that is generally desired for inclusion in numerical models that seek to represent and predict the impacts of varying aerosol characteristics on the formation and microphysical properties of clouds. One limitation of the use of direct CCN observations is that they are not available for supersaturations larger than about 1%, which is insufficient for deep convection and may be insufficient even for shallow convection, depending on the nature of the available CCN and the dynamics of the cloud. We developed a data-based approach to representing the full aerosol size spectrum with size-dependent hygroscopicity, and used this to extrapolate CCN spectra beyond the limited measurements. Five years of SGP aerosol data (2009 -2013) were analyzed. As a side product of our work, we identified and communicated several previously-unflagged data quality issues. The resulting merged aerosol distributions, along with fits for seasonal averages, were published and submitted to the ARM archive as a special value-added product (VAP; submitted as a PI product). CCN spectra were computed for the same data period and will similarly be published and submitted to the archive for use by the community. We also note that our methodologies and findings have been discussed at several Joint ARM User Facility/Atmospheric System Research (ASR) Principal Investigators Meetings and that recent ARM/ASR aerosol data reporting strategies have included similar ideas for data merging, indicating that this work has had a lasting impact on ARM aerosol data acquisition and reporting. The proposed work advances the science of the interactions of aerosols, clouds and precipitation, with direct application to improve representation of such interactions for clouds in regional and global climate models. The archived data will continue to serve research studies in the future.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Development and Optimization of a Multi-Functional SCR-DPF Aftertreatment System for Heavy-Duty NOX and Soot Emission Reduction

The objective of this project is to develop a strategy for the integration of catalytic NOX emission control and particulate matter emission control into a single device for the successful application to heavy-duty on-road diesel engine exhaust aftertreatment. The critical attributes of such a device, for successful application to PACCAR fleet, are as follows: 1. Must have sufficient filtration efficiency and successfully demonstrate soot management strategies (i.e., oxidation) to be economically attractive and regulatory compliant for particulate matter abatement. 2. In particular, the integrated device must retain sufficiently high soot oxidation capacity with NO2 (i.e., passive soot oxidation) across an applicable engine test cycle to be economically attractive. 3. Must exhibit sufficient catalytic NOX reduction activity in an economically-attractive fashion that is regulatory compliant.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Industrial emission inventories of iron and phosphorus for past, present and future

Global emission inventories of aerosol iron by species, and of phosphorus, were developed for inclusion in Earth system modeling that includes atmospheric transport. The time period covered was 1850-2010 to evaluate human influence. A variety of approaches to compare measured and modeled values of aerosol iron was synthesized to estimate how well anthropogenic emissions are known. Anthropogenic emissions are constrained within a factor of two and if there is a bias, it is an overestimation. The exception is shipping emissions, which may be underestimated. Direct radiative forcing by iron aerosol is small in the global average (0.02 W m -2 ) but reaches 0.25 W m -2 around source regions. Regions of high direct radiative forcing are poorly constrained by observations. The central value of change in oceanic net primary productivity due to iron deposition is about 0.26 PgC yr -1 , also highly localized. This leads to a decrease in atmospheric CO2 accumulation that corresponds to a forcing of 0.008 W m -2 since 1850 (0.003-0.18 W m -2 ). Emissions of particulate matter to 2050 were estimated in response to different policy scenarios, including the need for renewable energy installations under decarbonization scenarios. Under the business-as-usual scenario, the total metal demand is 195 Mt/yr in 2020, peaking at 270 Mt/yr in years 2040-2045; under the Rapid Decarbonization scenario, total metal demand is nearly doubled at its peak: 480 Mt/yr in year 2040. Primary particulate matter emissions attributable to processing metals for renewable energy are also amplified under rapid decarbonization, but total atmospheric emissions are much lower because of the shift away from combustion.

58 GEOSCIENCES↗
DOE OSTI2026

Persistent Elevated Soot Emissions Induced by Clustered Stochastic Preignition Events

Stochastic Preignition (SPI) is an abnormal combustion phenomenon that can occur in spark-ignition engines particularly under high-load operation. SPI is characterized by uncontrolled initiation of combustion prior to spark discharge, an abnormal combustion process that can lead to severe knock events and significant engine damage. SPI has been associated with fuel properties, lubricant composition, and engine design and operation. Here, in this work, a single-cylinder test engine with a dry-sump oil system was utilized to study the SPI response of E10 and E25 fuels with a range of Reid Vapor Pressure (RVP). An automated test procedure was employed, consisting of ten square-waved load profile segments, with each segment composed of 5 min of low-load operation followed by 25 min of sustained high-load operation. These tests were replicated across multiple days of testing including a lubricant triple flush between tests, and an online Fuel in Oil diagnostic measurement. Exhaust particulate emissions were continuously measured by an AVL microsoot sensor (MSS). Elevated particulate matter emissions were observed to occur concurrently with SPI events as blooms of soot. Particularly after clustered events (i.e., multiple SPI cycles occurring within 10 consecutive engine cycles), high soot emissions were observed to persist over several days of sequential operation despite daily lubricant changes, a complete warm-up procedure, and sustained low-load operation between test segments. This result implies that the particulate emissions trends may be dominated by deposit-based effects, where higher load operation is needed to alter deposition and formation processes. The observed soot blooms were also found to correspond to a reduction in the engine fueling and the fuel engine oil dilution rate despite the engine exhaust remaining at stoichiometric exhaust operation. These observations suggest that post-SPI events, pathways for lubricant migration and consumption into the combustion chamber may occur until these pathways are closed from deposit formation or ring dynamics during extended operation. These observed sooting propensity persisted with all fuels tests, but a linear correlation was observed between the summation of soot and particulate matter index (PMI) value for each fuel as well as SPI events, proving that PMI is a crucial fuel property for reducing SPI.

Splitter, Derek [Oak Ridge National Laboratory (OR↗
DOE OSTI2026

Adverse Neurological Effects of Wildfire Smoke

The respiratory and cardiovascular effects of smoke exposure are well documented from cigarette smoking and particulate matter (PM) associated with air-pollution studies, but epidemiological data also suggests exposure to high levels of woodsmoke correlate with central-nervous-system (CNS) dysfunction, including elevated rates of Alzheimer’s disease (AD) and dementia. Neuro-inflammation is believed to initiate the majority of Alzheimer’s and other neurodegenerative diseases attributed to environmental factors. We investigated whether inhaled PM and specific classes of compounds in wildfire smoke condensate extract (WSE) reach the brain and cause neuro-inflammation that can lead to progressive neurological degeneration, using isotope tracing of labeled particulate matter and major compound classes, biomarkers of blood-brain barrier (BBB) integrity, and biomarkers of neuro-inflammation. This project showed that inhalation exposure to PM and major compound classes present in WSE reached the brain through absorption in the nasal cavity and systemic circulation across the BBB. Twenty-four exposures of WSE to brain endothelial cells that form the main physical barrier of the BBB produced dose-dependent increases in biomarkers of inflammation and decreases in tight junction markers between cells. Intranasal exposure to WSE caused inflammatory disfunction in lung and brain. Biomarkers of inflammation increased and an enzyme inhibiting inflammation decreased. Similar patterns of chemical-induced changes in the lung and brain suggest either: (1) chemicals may act through shared molecular pathways upon entering lung and brain, or (2) that mediators originating in the lung circulate systemically to the brain and drive neuroinflammation. These findings warrant further mechanistic studies to delineate the temporal sequence of events to establish the lung-brain axis.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Chemical changes in thirdhand smoke associated with remediation using an ozone generator

Ozonation is a common remediation approach to eliminate odors from mold, tobacco and fire damage in buildings. Little information exists to: 1) assess its effectiveness; 2) provide guidance on operation conditions; and 3) identify potential risks associated with the presence of indoor ozone and ozonation byproducts. The goal of this study is to evaluate chemical changes in thirdhand smoke (THS) aerosols induced by high levels of ozone, in comparison with THS aerosols aged under similar conditions in the absence of ozone. Samples representing different stages of smoke aging in the absence of ozone, including freshly emitted secondhand smoke (SHS) and THS, were collected inside an 18-m 3 room-sized chamber over a period of 42 h after six cigarettes were consumed. The experiments involved collection and analysis of gas phase species including volatile organic compounds (VOCs), volatile carbonyls, semivolatile organic compounds (SVOCs), and particulate matter. VOC analysis was carried out by gas chromatography/mass spectrometry with a thermal desorption inlet (TD-GC/MS), and volatile carbonyls were analyzed by on-line derivatization with dinitrophenylhydrazine (DNPH), followed by liquid chromatography with UV/VIS detection. SVOCs were extracted from XAD-coated denuders and Teflon-coated fiberglass filters in the absence of ozone. In those extracts, tobacco-specific nitrosamines (TSNAs) and other SVOCs were analyzed by gas chromatography with positive chemical ionization-triple quadrupole mass spectrometric detection (GC/PCI-QQQ-MS), and polycyclic aromatic hydrocarbons (PAHs) were quantified by gas chromatography with ion trap mass spectrometric detection (GC/IT-MS) in selected ion monitoring mode. Particulate matter concentration was determined gravimetrically. In a second experiment, a 300 mg h -1 commercial ozone generator was operated during 1 h, one day after smoke was generated, to evaluate the remediation of THS by ozonation. VOCs and volatile carbonyls were analyzed before and after ozonation. Extracts from fabrics that were exposed in the chamber before and after ozonation as surrogates for indoor furnishings were analyzed by GC/IT-MS, and aerosol size distribution was studied with a scanning mobility particle sizer. Ozone concentration was measured with a photometric detector. An estimated 175 mg ozone reacted with THS after 1 h of treatment, corresponding to 58% of the total O 3 released during that period. Fabric-bound nicotine was depleted after ozonation, and the surface concentration of PAHs adsorbed to fabric specimens decreased by an order of magnitude due to reaction with ozone, reaching pre-smoking levels. These results suggest that ozonation has the potential to remove harmful THS chemicals from indoor surfaces. However, gas phase concentrations of volatile carbonyls, including formaldehyde, acetaldehyde and acetone were higher immediately after ozonation. Ultrafine particles (UFP, in most cases with size <60 nm) were a major ozonation byproduct. UFP number concentrations peaked shortly after ozonation ended, and remained at higher-than background levels for several hours. Based on these results, minimum re-entry times after ozone treatment were predicted for different indoor scenarios. Clearly defining re-entry times can serve as a practical measure to prevent acute exposures to ozone and harmful ozonation byproducts after treatment. This study evaluated potential benefits and risks associated with THS remediation using ozone, providing insights into this technology.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Measured indoor PM2.5, black carbon, and oxidative potential before and after replacing gas with induction cooking in asthmatic households

Cooking is a major source of fine particulate matter (PM) in homes and evidence to date is inconclusive about the impact of cooking fuel on measures of residential PM exposure. The Cooking Energy and Ventilation Impacts on Children's Asthma (CEVICA) study measured cooking frequency, range hood use, indoor air quality (IAQ) and respiratory health indicators of children with asthma living in homes with gas stoves in California's San Joaquin Valley. Intensive measurements occurred over three 2-week intensive periods: at baseline and at the end of two consecutive 3-month study phases. Participants were randomly assigned to have their gas stoves replaced with electric induction at the start of Phase 1 or Phase 2. As part of the IAQ assessment, we collected particulate matter on Teflon filters using ultrasonic personal air samplers (UPAS). The filters were analyzed to quantify time-integrated PM 2.5 mass concentration, black carbon (BC) oxidative potential (OP). OP was measured using the SLF-OH assay, an acellular chemical assay that quantifies production of OH radicals in simulated lung fluid (SLF). Across all comparisons, PM 2.5 mass tended to be higher during gas cooking than induction electric cooking, although only one transition (Baseline to Phase 1) was statistically discernible at p<0.05. BC and mass-normalized OP showed no measurable differences across stove types or across phases. These preliminary findings suggest that stove fuel alone may not be the dominant determinant of indoor PM 2.5 concentrations in this sample, as previous studies have reported that indoor PM 2.5 during cooking can also be influenced by factors such as cooking practices, food and oil type, kitchen ventilation, and outdoor infiltration.

Lin, Zhuoying↗
DOE OSTI2021

Biofuel Options for Marine Applications: Technoeconomic and Life-Cycle Analyses

This study performed technoeconomic and life-cycle analyses to assess the economic feasibility and emission benefits and tradeoffs of various biofuel production pathways as an alternative to conventional marine fuels. We analyzed production pathways for (1) Fischer-Tropsch diesel from biomass and cofeeding biomass with natural gas or coal, (2) renewable diesel via hydroprocessed esters and fatty acids from yellow grease and cofeeding yellow grease with heavy oil, and (3) bio-oil via fast pyrolysis of low-ash woody feedstock. We also developed a new version of the Greenhouse gases, Regulated Emissions, and Energy use in Transportation (GREET) marine fuel module for the estimation of life-cycle greenhouse gas (GHG) and criteria air pollutant (CAP) emissions of conventional and biobased marine fuels. The alternative fuels considered have a minimum fuel selling price between 2.36 and 4.58 $/heavy fuel oil gallon equivalent (HFOGE), and all exhibit improved life-cycle GHG emissions compared to heavy fuel oil (HFO), with reductions ranging from 40 to 93%. The alternative fuels also exhibit reductions in sulfur oxides and particulate matter emissions. Additionally, when compared with marine gas oil and liquified natural gas, they perform favorably across most emission categories except for cases where carbon and sulfur emissions are increased by the cofed fossil feedstocks. The pyrolysis bio-oil offers the most promising marginal CO2 abatement cost at less than $100/tonne CO2e for HFO prices >$1.09/HFOGE followed by Fischer-Tropsch diesel from biomass and natural gas pathways, which fall below $100/tonne CO2e for HFO prices >$2.25/HFOGE. Pathways that cofeed fossil feedstocks with biomass do not perform as well for marginal CO2 abatement cost, particularly at low HFO prices. This study indicates that biofuels could be a cost-effective means of reducing GHG, sulfur oxide, and particulate matter emissions from the maritime shipping industry and that cofeeding biomass with natural gas could be a practical approach to smooth a transition to biofuels by reducing alternative fuel costs while still lowering GHG emissions, although marginal CO2 abatement costs are less favorable for the fossil cofeed pathways.

Greenhouse gas, life cycle assessment, techno-econ↗