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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 181 records · Page 10

Meteorological Influences on Anthropogenic PM 2.5 in Future Climates: Species Level Analysis in the Community Earth System Model v2

Abstract Biomass and fossil fuel burning impact air quality by injecting fine particulate matter (PM 2.5 ) and its precursors into the atmosphere, which poses serious threats to human health. However, the surface concentration of PM 2.5 depends not only on the magnitude of emissions, but also secondary production, transport, and removal. For example, in response to greenhouse gas driven warming, meteorological conditions that govern aerosol removal, primarily through rainfall and wet deposition, could shift in pattern, frequency, and intensity. This climate change driven process can impact air quality even without changes in aerosol emissions. In this experiment, we conduct new simulations by fixing aerosol emissions at present‐day levels in the Community Earth System Model Version 2, but increasing greenhouse gases through the 21st century. In our results, the changes in patterns and intensity of PM 2.5 are found to be associated with precipitation (via aerosol removal), temperature (via secondary organic aerosol (SOA) formation), and moisture and clouds (via sulfate production). A decrease in wet day frequency (∼1.2% global mean) contributes to increases in the surface concentrations of black carbon, primary organic matter, and sulfate in many regions. This is offset in some regions by an upward vertical shift in the level where SOA forms, which contributes to higher column burden but lower surface concentration. These results highlight a need, using a variety of modeling tools, to continually reassess aerosol emissions regulations in response to anticipated climate changes.

54 ENVIRONMENTAL SCIENCES↗

PM 2.5 Is Insufficient to Explain Personal PAH Exposure

To understand how chemical exposure can impact health, researchers need tools that capture the complexities of personal chemical exposure. In practice, fine particulate matter (PM 2.5 ) air quality index (AQI) data from outdoor stationary monitors and Hazard Mapping System (HMS) smoke density data from satellites are often used as proxies for personal chemical exposure, but do not capture total chemical exposure. Silicone wristbands can quantify more individualized exposure data than stationary air monitors or smoke satellites. However, it is not understood how these proxy measurements compare to chemical data measured from wristbands. In this study, participants wore daily wristbands, carried a phone that recorded locations, and answered daily questionnaires for a 7-day period in multiple seasons. We gathered publicly available daily PM 2.5 AQI data and HMS data. We analyzed wristbands for 94 organic chemicals, including 53 polycyclic aromatic hydrocarbons. Wristband chemical detections and concentrations, behavioral variables (e.g., time spent indoors), and environmental conditions (e.g., PM 2.5 AQI) significantly differed between seasons. Machine learning models were fit to predict personal chemical exposure using PM 2.5 AQI only, HMS only, and a multivariate feature set including PM 2.5 AQI, HMS, and other environmental and behavioral information. On average, the multivariate models increased predictive accuracy by approximately 70% compared to either the AQI model or the HMS model for all chemicals modeled. This study provides evidence that PM 2.5 AQI data alone or HMS data alone is insufficient to explain personal chemical exposures. Our results identify additional key predictors of personal chemical exposure.

63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗

Reduced Sediment Settling in Turbulent Flows Due To Basset History and Virtual Mass Effects

The behavior of suspended particles in turbulent flows is a recalcitrant problem spanning wide-ranging fields including geomorphology, hydrology, and dispersion of particulate matter in the atmosphere. One key mechanism underlying particle suspension is the difference between particle settling velocity (w s ) in turbulence and its still water counterpart (w so ). This difference is explored here for a range of particle-to-fluid densities (1 – 10) and particle diameter to Kolmogorov micro-eddy sizes (0.1 – 10). Conventional models of particle fluxes that equate w s to w so result in eddy diffusivities and turbulent Schmidt numbers contradictory to laboratory experiments. Incorporating virtual mass and Basset history forces resolves these inconsistencies, providing clarity as to why w s /w so is sub-unity for the aforementioned conditions. The proposed formulation can be imminently used to model particle settling in turbulence, especially when sediment distribution outcomes over extended time scales far surpassing turbulence time scales are sought.

Geology↗

Long‐Term Impacts of Global Solid Biofuel Emissions on Ambient Air Quality and Human Health for 2000–2019

Globally, solid biofuels (SB) have been widely used for household cooking and energy production for decades due to electricity shortages and socio-economic barriers to adopting renewable energy alternatives. This has detrimental effects on air quality, human health, and climate through trace gas and aerosol emissions. Despite numerous studies, the long-term consequences of SB emissions remain poorly understood. Here, we use the Community Earth System Model and the Community Emissions Data System emission inventory to investigate the SB emission impacts on air quality and human health for 2000–2019. Global SB emission increased the ambient PM 2.5 (particulate matter with aerodynamic diameters ≤2.5 μm) and ozone (O 3 ) concentrations up to 23.61 μg/m 3 and 13.69 ppbv, with significant effects found in India, China, and the Rest of Asia (ROA). Our study estimates total annual premature deaths (APDs) associated with global SB-attributable PM 2.5 and O 3 exposure as 1.11 million [95% confidence interval (95% CI): 1.00–1.22 million] in 2000 up to 1.43 million (95% CI: 1.30–1.56 million) in 2019. China's SB emissions and associated APDs have reduced substantially, whereas India and ROA had a major leap in both estimates in 2019 compared to 2000. China's progress in cutting residential SB emissions accounts for its improvements. Our study urges the reduction of SB usage and emissions to potentially improve overall air quality and human health conditions, especially in highly populated, low- and middle-income countries, where the poor air quality and associated health burden attributable to SB emissions are estimated to be higher.

O 3↗

The Abundance and Sources of Ice Nucleating Particles Within Alaskan Ice Fog

Abstract The Alaskan Layered Pollution and Chemical Analysis (ALPACA) field campaign included deployment of a suite of atmospheric measurements in January–February 2022 with the goal of better understanding atmospheric processes and pollution under cold and dark conditions in Fairbanks, Alaska. We report on measurements of particle composition, particle size, ice nucleating particle (INP) composition, and INP size during an ice fog period (29 January–3 February). During this period, coarse particulate matter (PM 10 ) concentrations increased by 150% in association with a decrease in air temperature, a stronger temperature inversion, and relatively stagnant conditions. Results also show a 18%–78% decrease in INPs during the ice fog period, indicating that particles had activated into the ice fog via nucleation. Peroxide and heat treatments performed on INPs indicated that, on average, the largest contributions to the INP population were heat‐labile (potentially biological, 63%), organic (31%), then inorganic (likely dust, 6%). Measurements of levoglucosan and bulk and single‐particle composition corroborate the presence of dust and aerosols from combustion sources. Heat‐labile and organic INPs decreased during the peak period of the ice fog, indicating those were preferentially activated, while inorganic INPs increased, suggesting they remained as interstitial INPs. In general, INP concentrations were unexpectedly high in Fairbanks compared to other locations in the Arctic during winter. The fact that these INPs likely facilitated ice fog formation in Fairbanks has implications for other high latitude locations subject to the hazards associated with ice fog.

Meteorology & Atmospheric Sciences↗

Environmental Factors Associated With Fall Phytoplankton Blooms in the Northern Bering and Chukchi Seas

This study investigates environmental drivers of fall phytoplankton blooms in the Arctic, focusing on the northern Bering and Chukchi seas. Random Forests models were used to analyze covariates of fall phytoplankton blooms from 2013 to 2018, incorporating shipboard, remote sensing, and modeled environmental properties. Four regional models and one comprehensive all-station model considered fall as well as midsummer conditions. Midsummer properties included suspended particulate matter, chlorophyll-a, and the proportion of degraded pheophytin to chlorophyll-a used as a proxy for bloom stage. Open water duration was one of the highest ranked factors in predicting fall blooms. Open water duration also influences the stage of midsummer (July) blooms as indicated by pheophytin proportions, which in turn were the highest-ranked factor for predicting fall bloom events in the Chirikov Basin (northern Bering Sea between St. Lawrence Island and the Bering Strait) and the Chukchi Sea. Wind direction, specifically easterly winds, was an important predictor in the northern Bering Sea. Maximum wind speed ranked highly at stations located within the nutrient-poor Alaska Coastal Current in the Chukchi Sea. However, stormy days, average and maximum wind speeds generally ranked low in importance as a predictor of fall bloom events. Other parameters, including photosynthetic active radiation, modeled nutrient concentrations, mixed layer depth, and time since sea ice breakup date showed strong but regionally varying relationships with fall blooms. Altogether, results from these Random Forests models suggest that high wind events and storms in the absence of sea ice provide an incomplete narrative for initiating fall bloom events.

Gaffey, C. B. [Clark University, Worcester, MA (Un↗

Development of the United States GReenhouse Gas and Air Pollutants Emissions System (GRA 2 PES)

In the U.S., emissions of greenhouse gases and air pollutants are often developed independently. Here, we describe the GReenhouse gas And Air Pollutants Emissions System (GRA 2 PES), which provides gridded emissions of fossil-fuel carbon dioxide (ffCO 2 ) and 93 air quality (AQ) species for 17 combustion and non-combustion sectors at 4 km × 4 km spatial resolution across the contiguous US. We find that the AQ emissions most spatially correlated with ffCO 2 are nitrogen oxides (NO x , ρ = 0.67), followed by sulfur dioxide (SO 2 , ρ = 0.51), carbon monoxide (CO, ρ = 0.44), and fine particulate matter (PM 2.5 , ρ = 0.38). We evaluate GRA 2 PES ffCO 2 emissions with an ensemble of publicly available regional and global inventories at national (Normalized Mean Bias (NMB) = +1.4%), state (NMB = +1.5%, R 2 = 0.98), and urban (NMB = +11.5%, R 2 = 0.97) scales. Nationally, the differences of publicly available inventories from the ensemble average range from −10.0% to +5.7%, and consistency diverges at state and urban scales. We simulate GRA 2 PES ffCO 2 in a particle dispersion model and compare to measurements of radiocarbon ( 14 C)-derived ffCO 2 collected in Los Angeles (August 2021), with results suggesting that GRA 2 PES ffCO 2 may be low by 19% for this city, but well within model-observation differences for other publicly available inventories (−43% to +94%). GRA 2 PES AQ/ffCO 2 ratios converted to concentration space generally agree with field observations (NMB = +4%, log R 2 = 0.90). Lastly, we present a method by which to utilize GRA 2 PES to derive AQ emission fluxes from ffCO 2 emissions.

Lyu, Congmeng [National Oceanic and Atmospheric Ad↗

Air pollution control strategies directly limiting national health damages in the US

Exposure to fine particulate matter (PM 2.5 ) from fuel combustion significantly contributes to global and US mortality. Traditional air pollution control strategies typically focus on emission reductions for specific air pollutants or sectors to maintain air pollutant concentrations within acceptable levels. Here we directly set national PM 2.5 mortality cost reduction targets within a global human-earth system model with US state-level energy systems, identifying endogenously the control actions, sectors, and locations that most cost-effectively reduce PM 2.5 mortality. Our results show that substantial health benefits can be cost-effectively achieved by using electricity to replace sources with high primary PM 2.5 emission intensities, including industrial coal, building biomass, and industrial liquids. Increasing the stringency of PM 2.5 reduction targets expedites the phaseout of high emission intensity sources, leading to larger declines in major air pollutant emissions, but very limited co-benefits in reducing CO 2 emissions. Control strategies achieve the greatest mortality cost reductions in the East North Central and Middle Atlantic states.

54 ENVIRONMENTAL SCIENCES↗

Source sector and fuel contributions to ambient PM 2.5 and attributable mortality across multiple spatial scales

Ambient fine particulate matter (PM 2.5 ) is the world’s leading environmental health risk factor. Reducing the PM 2.5 disease burden requires specific strategies that target dominant sources across multiple spatial scales. We provide a contemporary and comprehensive evaluation of sector- and fuel-specific contributions to this disease burden across 21 regions, 204 countries, and 200 sub-national areas by integrating 24 global atmospheric chemistry-transport model sensitivity simulations, high-resolution satellite-derived PM 2.5 exposure estimates, and disease-specific concentration response relationships. Globally, 1.05 (95% Confidence Interval: 0.74–1.36) million deaths were avoidable in 2017 by eliminating fossil-fuel combustion (27.3% of the total PM 2.5 burden), with coal contributing to over half. Other dominant global sources included residential (0.74 [0.52–0.95] million deaths; 19.2%), industrial (0.45 [0.32–0.58] million deaths; 11.7%), and energy (0.39 [0.28–0.51] million deaths; 10.2%) sectors. Our results show that regions with large anthropogenic contributions generally had the highest attributable deaths, suggesting substantial health benefits from replacing traditional energy sources.

54 ENVIRONMENTAL SCIENCES↗

Economy-wide evaluation of CO 2 and air quality impacts of electrification in the United States

Adopting electric end-use technologies instead of fossil-fueled alternatives, known as electrification, is an important economy-wide decarbonization strategy that also reduces criteria pollutant emissions and improves air quality. In this study, we evaluate CO 2 and air quality co-benefits of electrification scenarios by linking a detailed energy systems model and a full-form photochemical air quality model in the United States. We find that electrification can substantially lower CO 2 and improve air quality and that decarbonization policy can amplify these trends, which yield immediate and localized benefits. In particular, transport electrification can improve ozone and fine particulate matter (PM 2.5 ), though the magnitude of changes varies regionally. However, growing activity from non-energy-related PM 2.5 sources—such as fugitive dust and agricultural emissions—can offset electrification benefits, suggesting that additional measures beyond CO 2 policy and electrification are needed to meet air quality goals. We illustrate how commonly used marginal emissions approaches systematically underestimate reductions from electrification.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗

Global organic and inorganic aerosol hygroscopicity and its effect on radiative forcing

The climate effects of atmospheric aerosol particles serving as cloud condensation nuclei (CCN) depend on chemical composition and hygroscopicity, which are highly variable on spatial and temporal scales. Here we present global CCN measurements, covering diverse environments from pristine to highly polluted conditions. We show that the effective aerosol hygroscopicity, κ, can be derived accurately from the fine aerosol mass fractions of organic particulate matter (ϵ org ) and inorganic ions (ϵ inorg ) through a linear combination, κ = ϵ org · κ org + ϵ inorg · κ inorg . In spite of the chemical complexity of organic matter, its hygroscopicity is well captured and represented by a global average value of κ org = 0.12 ± 0.02 with κinorg = 0.63 ± 0.01 as the corresponding value for inorganic ions. By showing that the sensitivity of global climate forcing to changes in κ org and κ inorg is small, we constrain a critically important aspect of global climate modelling.

54 ENVIRONMENTAL SCIENCES↗

Weakening aerosol direct radiative effects mitigate climate penalty on Chinese air quality

Future climate change may worsen air quality in many regions. However, evaluations of this ‘climate penalty’ on air quality have typically not assessed the radiative effects of changes in short-lived aerosols. Additionally, China’s clean air goals will decrease pollutant emissions and aerosol loadings, with concomitant weakening of aerosol feedbacks. In this work, we assess how such weakened aerosol direct effects alter the estimates of air pollution and premature mortality in China attributable to mid-century climate change under Representative Concentration Pathway 4.5. We found that weakening aerosol direct effects cause boundary layer changes that facilitate diffusion. This reduces air-pollution exposure (~4% in fine particulate matter) and deaths (13,800 people per year), which largely offset the additional deaths caused by greenhouse gas-dominated warming. These results highlight the benefits of reduced pollutant emissions through weakening aerosol direct effects and underline the potential of pollution control measures to mitigate climate penalties locked in by greenhouse gas emissions.

54 ENVIRONMENTAL SCIENCES↗

Attributing human mortality from fire PM 2.5 to climate change

Climate change intensifies fire smoke, emitting hazardous air pollutants that impact human health. However, the global influence of climate change on fire-induced health impacts remains unquantified. Here, in this study, we used three well-tested fire-vegetation models in combination with a chemical transport model and health risk assessment framework to attribute global human mortality from fire fine particulate matter (PM 2.5 ) emissions to climate change. Of the 46401 (1960s) –to 98748 (2010s) annual fire PM 2.5 mortalities, 669 (1.2%, 1960s) –to 12566 (12.8%, 2010s) were attributed to climate change. The most substantial influence of climate change on fire mortality occurred in South America, Australia, and Europe, coinciding with decreased relative humidity, and in boreal forests with increased air temperature. Increasing relative humidity lowered fire mortality in other regions, like South Asia. Our study highlights the role of climate change in fire mortality, aiding public health authorities in spatial targeting adaptation measures for sensitive fire-prone areas.

54 ENVIRONMENTAL SCIENCES↗

Jamming, fragility and pinning phenomena in superconducting vortex systems

Abstract We examine driven superconducting vortices interacting with quenched disorder under a sequence of perpendicular drive pulses. As a function of disorder strength, we find four types of behavior distinguished by the presence or absence of memory effects. The fragile and jammed states exhibit memory, while the elastic and pinning dominated regimes do not. In the fragile regime, the system organizes into a pinned state during the first pulse, flows during the second perpendicular pulse, and then returns to a pinned state during the third pulse which is parallel to the first pulse. This behavior is the hallmark of the fragility proposed for jamming in particulate matter. For stronger disorder, we observe a robust jamming state with memory where the system reaches a pinned or reduced flow state during the perpendicular drive pulse, similar to the shear jamming of granular systems. We show signatures of the different states in the spatial vortex configurations, and find that memory effects arise from coexisting elastic and pinned components of the vortex assembly. The sequential perpendicular driving protocol we propose for distinguishing fragile, jammed, and pinned phases should be general to the broader class of driven interacting particles in the presence of quenched disorder.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Single-particle chemical analysis reveals organic-rich detonation soot products

The detonation of high explosives produces a wide variety of particulate matter (PM) with distinct properties, not all of which are traditionally studied for chemical composition, formation processes, and forensic applications. We report particle-resolved measurements of Composition B detonation soot using soot particle aerosol mass spectrometry (SP-AMS), identifying carbonaceous species and metals not previously characterized on a single-particle basis. Results are combined with scanning electron microscopy with energy dispersive X-ray spectroscopy (SEM-EDS) to enhance source-dependent signatures. Black carbon, including graphitic carbon and detonation nanodiamonds, contributed 50.5-71.4% of PM 2.5 mass, while 22.5-43.4% was non-refractory organic carbon, a previously overlooked component that exhibited a complex and varying composition. Detonations were performed with and without PMMA confinement and under steady and overdriven conditions. Distinct particles enriched with polycyclic aromatic hydrocarbons (PAHs) were observed in experiments utilizing confinement, with quantities dependent on manufacturing method. SEM-EDS validated SP-AMS findings of metals internally mixed with carbonaceous species and extended the particle size range to 100 µm. This work makes detecting non-refractory organics using single-particle techniques more feasible for detonation forensics and understanding high-energy soot formation. While this analysis uses offline sample collection, SP-AMS could be deployed for in-situ measurements of detonation PM 2.5 transported in the atmosphere.

36 MATERIALS SCIENCE↗

The atmospheric importance of methylamine additions to Criegee intermediates

We report that Criegee intermediates are important targets for study in atmospheric chemistry because of their capacity to oxidize airborne species. Among these species, ammonia has received critical attention for its presence in polluted agricultural or industrial areas and its role in forming particulate matter and condensation nuclei. Although methylamine has been given less attention than ammonia, both theoretical and experimental studies have demonstrated that the additional methyl substitution on the ammonia derivatives increases the rate constants for some systems. This suggests that the methylamine addition to Criegee intermediates could be more significant to atmospheric processes. In this work, geometries are optimized at the DF-CCSD(T)/ANO1 level for the methylamine addition reactions to the simplest Criegee intermediate and the anti- and syn-methylated Criegee intermediates. Energies for each stationary point were computed at the CCSD(T)/CBS level with corrections from the CCSDT(Q) method. Rate constants are obtained for each reaction using canonical transition state theory. Although methylamine addition proved to be a more favorable reaction relative to ammonia addition, the significantly lower concentration of atmospheric methylamine limits the prevalence of these reactions, even in the most optimal conditions. It is unlikely that the methylamine addition to Criegee intermediates will contribute significantly to the consumption of Criegee intermediates in the atmosphere.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Near-canopy horizontal concentration heterogeneity of semivolatile oxygenated organic compounds and implications for 2-methyltetrols primary emissions

Semivolatile oxygenated organic compounds (SV-OVOCs) are important atmospheric species, in particular for the production and chemistry of atmospheric particulate matter and related impacts on air quality and climate. In this study, SV-OVOCs were collected in the horizontal plane of the roughness layer over the tropical forest in the central Amazon during the wet season of 2018. A sampler mounted to a copter-type, hovering unmanned aerial vehicle was used. Underlying the collection region, a plateau forest transitioned into a slope forest across several hundred meters. The concentrations of pinonic and pinic acids, which are monoterpene oxidation products, had no statistical difference over the two forests. By comparison, across the study period, differences in the concentration of 2-methyltetrols, which are products of isoprene oxidation, ranged from -70% to +480% over the two forests. The chemical lifetime of 2-methyltetrols in the atmosphere is sufficiently long that heterogeneity in the isoprene emission rate from the two forests followed by atmospheric oxidation does not explain the concentration heterogeneity of 2-methyltetrols. Standing waves and local meteorology also cannot account for the heterogeneity. Of the possibilities considered, the most plausible explanation is the direct emission from the forest of 2-methyltetrols produced through biological processes within the plants. Under this explanation, the rate of direct SV-OVOC emissions should be modulated by forest type and related environmental stressors. Direct emissions of SV-OVOCs should be more broadly considered for constraining and improving models of atmospheric composition, transport, and chemistry over tropical forests.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Failure modes of protection layers produced by atomic layer deposition of amorphous TiO 2 on GaAs anodes

Amorphous titanium dioxide (a-TiO 2 ) films formed by atomic layer deposition can serve as protective coatings for semiconducting photoanodes in water-splitting cells using strongly alkaline aqueous electrolytes. Herein, we experimentally examine the mechanisms of failure for p + -GaAs anodes coated with a-TiO 2 films (GaAs/a-TiO 2 ). Galvanic displacement of exposed GaAs by Au allowed imaging of pinholes in the a-TiO 2 coatings, and enabled collection of quantitative and statistical data associated with pinhole defects. A combination of imaging, electrochemical measurements, and quantitative analyses of corrosion products indicated that extrinsic pinholes were present in the a-TiO 2 films before electrochemical operation. During electrochemical operation these pinholes led to pitting corrosion of the underlying GaAs substrate. The dominant source of pinholes was the presence of atmospheric particulate matter on the GaAs surface during deposition of the a-TiO 2 layer. The pinhole density decreased substantially when the thickness of the a-TiO 2 coating increased beyond 45 nm, and approached zero when the thickness of the film exceeded 112 nm. The density of pinholes in films thinner than 45 nm decreased when the a-TiO 2 coating was deposited in an environmentally controlled cleanroom. Pinhole-free GaAs/a-TiO 2 devices were also tested via chronoamperometry to quantify the rate of pinhole formation during electrochemistry. The time-to-failure increased with thickness, suggesting that the failure mechanism may involve diffusion or migration through the film. However, other mechanisms may also contribute to the degradation of thicker films (>112 nm). Nevertheless, as previously hypothesized, extrinsic pinhole defects formed during deposition and testing control the short-term protective performance of the a-TiO 2 film for GaAs anodes evolving O 2 from water.

25 ENERGY STORAGE↗