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At least 217 records · Page 12

The impact of Los Angeles Basin pollution and stratospheric intrusions on the surrounding San Gabriel Mountains as seen by surface measurements, lidar, and numerical models

In this work, the impact of Los Angeles Basin pollution transport and stratospheric intrusions on the surface ozone levels observed in the San Gabriel Mountains is investigated based on a combination of surface and lidar measurements as well as WRF-Chem (Weather Research and Forecasting with Chemistry) and WACCM (Whole Atmosphere Community Climate Model) runs. The number of days with observed surface ozone levels exceeding the National Ambient Air Quality Standards exhibit a clear seasonal pattern, with a maximum during summer, when models suggest a minimum influence of stratospheric intrusions and the largest impact from Los Angeles Basin pollution transport. Additionally, measured and modeled surface ozone and PM10 were analyzed as a function of season, time of the day, and wind direction. Measurements and models are in good qualitative agreement, with maximum surface ozone observed for southwest and west winds. For the prevailing summer wind direction, slightly south of the ozone maximum and corresponding to south-southwest winds, lower ozone levels were observed. Back trajectories suggest that this is associated with transport from the central Los Angeles Basin, where titration limits the amount of surface ozone. A quantitative comparison of the lidar profiles with WRF-Chem and WACCM models revealed good agreement near the surface, with models showing an increasing positive bias as function of altitude, reaching 75 % at 15 km above sea level. Finally, three selected case studies covering the different mechanisms affecting the near-surface ozone concentration over the San Gabriel Mountains, namely stratospheric intrusions and pollution transport, are analyzed based on surface and ozone lidar measurements, as well as co-located ceilometer measurements and models.

Impact↗

Global Premature Mortality By Dust and Pollution PM 2.5 Estimated From Aerosol Reanalysis of the Modern-Era Retrospective Analysis for Research and Applications, Version 2

This study quantifies global premature deaths attributable to long-term exposure of ambient PM 2.5 , or PM 2.5 -attributable mortality, by dust and pollution sources. We used NASA’s Modern-Era Retrospective Analysis for Research and Applications, Version 2 (MERRA-2) aerosol reanalysis product for PM 2.5 and the cause-specific relative risk (RR) from the integrated exposure-response (IER) model to estimate global PM2.5-attributable mortality for five causes of deaths, namely ischaemic heart disease (IHD), cerebrovascular disease (CEV) or stroke, lung cancer (LC), chronic obstructive pulmonary disease (COPD), and acute lower respiratory infection (ALRI). The estimated yearly global PM 2.5 -attributable mortality in 2019 amounts to 2.89 (1.38–4.48) millions, which is composed of 1.19 (0.73–1.84) million from IHD, 1.01 (0.35–1.55) million from CEV, 0.29 (0.11–0.48) million from COPD, 0.23 (0.14–0.33) million from ALRI, and 0.17 (0.04–0.28) million from LC (the numbers in parentheses represent the estimated mortality range due corresponding to RR spread at the 95% confidence interval). The mortality counts vary with geopolitical regions substantially, with the highest number of deaths occurring in Asia. China and India account for 40% and 23% of the global PM 2.5 -attributable deaths, respectively. In terms of sources of PM 2.5 , about 22% of the global all-cause PM 2.5 -attributable deaths are caused by desert dust. The largest dust attribution is 37% for ALRI. The relative contributions of dust and pollution sources vary with the causes of deaths and geographical regions. Enforcing air pollution regulations to transfer areas from PM 2.5 nonattainment to PM2.5 attainment can have great health benefits. Being attainable with the United States air quality standard (AQS) of 15 μg/m 3 globally would have avoided nearly 40% or 1.2 million premature deaths. The most recent update of PM 2.5 guideline from 10 to 5 μg/m 3 by the World Health Organization (WHO) would potentially save additional one million lives. Our study highlights the importance of distinguishing aerodynamic size from geometric size in accurately assessing the global health burden of PM 2.5 and particularly for dust. A use of geometric size in diagnosing dust PM 2.5 from the model simulation, a common approach in current health burden assessment, could overestimate the PM 2.5 level in the dust belt by 40–170%, leading to an overestimate of global all-cause mortality by 1 million or 32%.

PM2.5↗

Assessing Potential Air Pollutant Emissions from Agricultural Feedstock Production using MOVES

Biomass feedstock production is expected to grow as demand for biofuels and bioenergy increases. The change in air pollutant emissions that may result from large-scale biomass supply has implications for local air quality and human health. We developed spatially explicit emissions inventories for corn grain and six cellulosic feedstocks through the extension of the National Renewable Energy Laboratory's Feedstock Production Emissions to Air Model (FPEAM). These inventories include emissions of seven pollutants (nitrogen oxides, ammonia, volatile organic compounds, particulate matter, sulfur oxides, and carbon monoxide) generated from biomass establishment, maintenance, harvest, transportation, and biofuel preprocessing activities. By integrating the EPA's MOtor Vehicle Emissions Simulator (MOVES) into FPEAM, we created a scalable framework to execute county-level runs of the MOVES-Onroad model for representative counties (i.e., those counties with the largest amount of cellulosic feedstock production in each state) on a national scale. We used these results to estimate emissions from the on-road transportation of biomass and combined them with county-level runs of the MOVES-Nonroad model to estimate emissions from agricultural equipment. We also incorporated documented emission factors to estimate emissions from chemical application and the operation of drying equipment for feedstock processing, and used methods developed by the EPA and the California Air Resources Board to estimate fugitive dust emissions. The model developed here could be applied to custom equipment budgets and is extensible to accommodate additional feedstocks and pollutants. Future work will also extend this model to analyze spatial boundaries beyond the county-scale (e.g., regional or sub-county levels).

54 ENVIRONMENTAL SCIENCES↗

Spatially Explicit Modeling of Criteria Air Pollutants from Agricultural and Forestry Feedstock Production

The Feedstock Production Emissions to Air Model (FPEAM) is a spatially explicit supply chain model that quantifies criteria air pollutants and precursors generated by biomass production, harvest and transportation to biorefineries. FPEAM was most recently used for the 2016 Billion Ton Study (BTS) published by the U.S. Department of Energy Bioenergy Technologies Office. This presentation describes several use cases for the model, and provides an overview of recent restructuring that increases FPEAM's usability and functionality. FPEAM currently estimates emissions of volatile organic compounds, particulate matter, nitrogen oxides, sulfur oxides, and carbon monoxide from on-farm equipment operation, on-farm fugitive dust, on-farm chemical (fertilizer, herbicide and insecticide) application, and biomass transportation. These calculations are implemented within FPEAM as modules, which independently perform calculations for each emissions category. This structure allows users to include or exclude emissions categories according to the goal and scope of their analysis. Each module's input data defines the activities taking place with information including fuel combusted, chemicals applied, and equipment used. Users can replace or augment the default input data to quantify additional pollutant types, emissions categories, farming practices and biomass types. Emissions from biomass transportation and on-farm equipment operation are by default calculated by the U.S. Environmental Protection Agency's Motor Vehicle Emission Simulator (MOVES) and NONROAD model, respectively. These models - which are computationally intensive but provide detailed results - can optionally be replaced with user-provided emissions factors for fuel combustion and vehicle operation. This approach reduces FPEAM's runtime and allows users to run sensitivity analyses around biomass production and transportation scenarios. Other enhancements currently under development are the use of farm-to-biorefinery route information to increase the spatial resolution of transportation emissions, and a module to connect FPEAM and the Intervention Model for Air Pollution (InMAP), which will enable the quantification of human health impacts.

09 BIOMASS FUELS↗

Air Pollutant Emissions and Regulatory Implications of Co-Processing Raw Bio-Oil in U.S. Petroleum Refineries

Pyrolysis oil, often referred as bio-oil or biocrude, has attracted considerable attention because it has higher energy density and carbon content compared to the raw biomass. Using pyrolysis oil derived from low cost and underutilized biomass to produce renewable hydrocarbon fuels provides a viable link between the agriculture/forestry and (petro-) chemical industry. Co-processing bio-oil with vacuum gas oil (VGO) in petroleum refinery is appealing due to the relatively low capital requirement to retrofit refinery and the compatibility of fuel products with existing infrastructure. In order to implement co-processing, a petroleum refinery would need to consider several process modifications and therefore could be subject to varying levels of air permitting requirements based on bio-oil co-processing ratio, co-processing capacity in existing units, the amount of regulated pollutants expected to be emitted, among other factors. This analysis considers co-processing 5% (by weight) of raw bio-oil with VGO in the fluidized catalytic cracking (FCC) unit(s) in a petroleum refinery. We estimate the potential increase in emissions of regulated air pollutants resulting from the modifications required to implement bio-oil co-processing and evaluate the regulatory and permitting implications for three FCC size categories in the U.S. refineries, which could co-processes raw bio-oil to produce partially renewable transportation fuels. We also assess technically feasible emission control options petroleum refineries could adopt to avoid being subject to major source permitting requirements if the estimated increase in regulated air pollutant emission exceeds the applicable threshold for major modifications. Insights from our analysis can help overcome challenges and risks associated with timely obtaining air permits required to implement bio-oil co-processing in existing refineries. Our analysis also provides needed information for decision makers (e.g., local air quality agencies) to understand the potential air quality implications for retrofitting refineries to co-process bio-oil, particularly in areas with high concentration of petroleum refineries.

09 BIOMASS FUELS↗

Superhydrophobic Phosphonium Modified Robust 3D Covalent Organic Framework for Preferential Trapping of Charge Dispersed Oxoanionic Pollutants

Abstract Charge dispersed and less hydrophilic anionic pollutants are often difficult to be preferentially captured by common cationic framework materials. A gamma radiation modification approach is employed to anchor a superhydrophobic phosphonium‐containing coating on a robust crystalline 3D covalent organic framework (COF). By regulating the surface hydrophobicity, the prepared 3DCOF‐ g ‐VBPPh 3 Cl is endowed with a strong affinity for charge dispersed and less hydrophilic oxoanions, such as MnO 4 − , TcO 4 − and ReO 4 − , to surmount the Hofmeister bias, which much favors remediation of oxoanionic pollutants in complex aqueous systems. Batch and column experiments with 3DCOF‐g‐VBPPh 3 Cl in both tap water and simulated groundwater are performed, and rapid sequestration is achieved with removal efficacy up to 99.995%, record‐high distribution coefficient of 1.0 × 10 8 mL g −1 , and desirable priority over competing anions such as Cl − , SO 4 2− , HCO 3 − , and NO 3 − , confirming promise for remediation of charge dispersed anionic pollutants. Theoretical calculations reveal a mechanism of preferential capture based on electrostatic and dispersion interaction between charge dispersed anions and 3DCOF‐g‐VBPPh 3 Cl that effectively competes with solvation of the aqueous anions.

Wang, Yue↗

Experimental and numerical investigation of flame stabilization and pollutant formation in matrix stabilized ammonia-hydrogen combustion

Ammonia (NH 3 ) is a carbon-free fuel that offers an attractive alternative for reducing greenhouse gas emissions. However, the slow flame speed, low heating value, and emissions of nitrogen-containing pollutants present significant issues for practical combustion applications. To address these issues, we investigate the use of matrix stabilized combustion. In this type of burner, combustion is performed within an inert porous ceramic foam, heat is recirculated by solid conduction and radiation, which enhances flame speed and combustion stabilization, thereby permitting combustion over a wide range of equivalence ratio conditions. We present a new porous media burner (PMB) capable of stabilizing NH 3 /air flames at ambient conditions. An extensive experimental characterization of the stability of this burner is conducted with up to 30% by volume of hydrogen (H 2 ) in the fuel stream. A 15:1 turndown ratio is demonstrated, with a high thermal power density of 62 MW m -3 . Concentrations of NO, unburnt NH 3 , and H 2 in the exhaust stream are measured. Two regimes are identified for low NO operation: rich and very lean. For rich conditions, NO emissions decrease with increasing equivalence ratio and decreasing H 2 blending. Unburnt NH 3 emissions follow opposite trends. These measurements are complemented by simulations in which the burner is represented by a coupled solid-gas reactor network. In conclusion, this model captures the burner’s pollutant emissions to good accuracy and is used to analyze the mechanisms of pollutant formation.

42 ENGINEERING↗

Win-win transportation strategies for India: Linking air pollution and climate mitigation

Here, this article analyzes road transport in India to explore linkages between air pollution and climate change policies in the transportation sector. Five teams modeled five policy scenarios – fuel efficiency, electrification, alternative fuels, modal shifts, and moderation in transport demand – to explore which policy brings the largest synergetic effects in reducing carbon dioxide (CO 2 ) and particulate matter (PM 2.5 ) emissions. The teams also modeled the comprehensive scenario which included policy measures from individual scenarios. The paper concludes that all of the measures provide strong co-benefits in reducing air pollutant and CO 2 emissions. The modeling results show that increased energy efficiency of passenger and freight vehicles has the largest protentional for reducing both CO 2 and PM 2.5 emissions. It is possible to reach even a larger reduction of air pollutants and CO 2 emissions by combining several policy measures in the comprehensive scenario.

54 ENVIRONMENTAL SCIENCES↗

Integrating population connectivity into pollution assessment: Overwintering mixing reveals flame retardant contamination in breeding areas in a migratory raptor

Highlights: • This multidisciplinary study integrates population connectivity into pollution assessment. • Flame retardants in inviable eggs of black kites were assessed in two populations. • A much higher occurrence and concentration of flame retardants were found in Madrid than Doñana. • Kites from Western Europe showed a strong winter intermixing in Africa. • Diffuse migratory connectivity reveals breeding areas as the main contamination grounds. Determining the exposure and magnitude at which various pollutants are differentially assimilated at the breeding and non-breeding grounds of migratory wildlife is challenging. Here, the possibility of applying the migratory connectivity framework to understanding contamination in birds is illustrated by considering flame retardants in inviable eggs of a migratory raptor, the black kite (Milvus migrans). The occurrence and concentration of legacy and emerging compounds in eggs from the southeastern peri-urban area of Madrid city, central Spain, were compared with those from Doñana National Park in southern Spain. A much higher occurrence and concentration of multiple polybrominated diphenyl ethers and Dechlorane 602 were found in Madrid than Doñana, but the opposite patterns were found for Dechlorane Plus. Individuals from these and other breeding areas in western Europe showed a strong intermixing pattern over widespread wintering areas in Africa, as assessed by ringing recoveries and movements tracked by satellite devices. This diffuse migratory connectivity reveals breeding areas as the main contamination grounds. High contamination burdens sequestered in eggs point to rapid assimilation of these compounds before laying, associated with important emission sources in Madrid, especially landfills of partially incinerated urban refuse, and other anthropogenic operations. Diet composition regarding aquatic vs. terrestrial prey, and bioaccumulation and biomagnification processes are suggested to explain differential assimilation of some compounds, especially Dechlorane Plus in Doñana, although a local emission source polluting this area cannot be ruled out. Insight from the migratory connectivity framework can help to disentangle large-scale patterns of contaminant uptake and refocus attention on key regions and potential causes of chemical hazards in declining migratory species and human populations.

54 ENVIRONMENTAL SCIENCES↗

Modeling atmospheric data and identifying dynamics Temporal data-driven modeling of air pollutants

Atmospheric modelling has recently experienced a surge with the advent of deep learning. Most of these models, however, predict concentrations of pollutants following a data-driven approach in which the physical laws that govern their behaviors and relationships remain hidden. Furthermore, with the aid of real-world air quality data collected hourly in different stations throughout Madrid, we present a case study using a series of data-driven techniques with the following goals: (1) Find systems of ordinary differential equations that model the concentration of pollutants and their changes over time; (2) assess the performance and limitations of our model using stability analysis; (3) reconstruct the time series of chemical pollutants not measured in certain stations using delay coordinate embedding results.

54 ENVIRONMENTAL SCIENCES↗

Persistent Heavy Winter Nitrate Pollution Driven by Increased Photochemical Oxidants in Northern China

Nitrate is an increasingly important component of fine particulate matter (PM2.5) during winter in northern China. Past emission control has been ineffective in reducing winter nitrate. Here, we use extensive observations and a model with state-of-theart nitrogen chemistry to identify the key factors that control the nitrate formation in the heavily polluted North China Plain (NCP). In contrast to the previous view of weak winter photochemistry, we show that the O3 and OH productions are sufficiently high in winter to facilitate fast gas-phase and heterogeneous conversion of NOX to nitrate over the NCP. Increasing O3 and OH productions from higher precursor levels and fast ROX cycling accelerate the nitrate generation during heavy pollution. We find that the 31.8% reduction of NOX emissions from 2010 to 2017 in the NCP lowers surface nitrate by only 0.2% and even increases nitrate in some polluted areas. This is mainly due to the increase of O3 and OH (by~30%), which has subsequently increased the conversion efficiency of NOX to HNO3 (by 38.7%). Future control strategies for the winter haze should also aim to lower photochemical oxidants, via larger and synchronized NOX and VOCs emissions reduction, to overcome the effects of nonlinear photochemistry and aerosol chemical feedback.

Fu, Xiao↗

Ultranano Titania: Selectively Ridding Water of Persistent Organic Pollutants

Persistent organic pollutants, including the EPA's “dirty dozen”, are difficult to remove from water supplies due to their chemical stability. Here, we report a stable oxide photocatalyst, ultranano titania (d < 2 nm) doped with iron, Fe•TiUNP, that efficiently mineralizes multiple persistent pollutants including aromatic compounds plus common troublesome, difficult-to-oxidize intermediates such as formaldehyde and acetone, netting mineralization of persistent pollutants. Efficiency stems from a direct charge-transfer pathway. The key role of iron doping is to lower the reduction potential of the photogenerated electron so that it is insufficient to reduce water, thus eliminating competition from the hydrogen evolution reaction. The reduction potential of the localized electron is similarly insufficient to reduce quinone, enabling breaking aromaticity. Specific results for degrading acetone, phenol, benzoic acid, and 1,4-benzoquinone are reported.

alcohols↗

A mesoporous cationic thorium-organic framework that rapidly traps anionic persistent organic pollutants

Many environmental pollutants inherently exist in their anionic forms and are therefore highly mobile in natural water systems. Cationic framework materials that can capture those pollutants are highly desirable but scarcely reported. Here we present a mesoporous cationic thorium-based MOF (SCU-8) containing channels with a large inner diameter of 2.2 nm and possessing a high surface area of 1360 m 2 g –1 . The anion-exchange properties of SCU-8 were explored with many anions including small oxo anions like ReO 4 – and Cr 2 O 7 2– as well as anionic organic dyes like methyl blue and the persistent organic pollutant, perfluorooctane sulfonate (PFOS). Both fast uptake kinetics and great sorption selectivity toward PFOS are observed. The underlying sorption mechanism was probed using quantum mechanical and molecular dynamics simulations. These computational results reveal that PFOS anions are immobilized in SCU-8 by driving forces including electrostatic interactions, hydrogen bonds, hydrophobic interactions, and van der Waals interactions at different adsorption stages.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Significant contributions of trimethylamine to sulfuric acid nucleation in polluted environments

Abstract As one of the least understood aerosol processes, nucleation can be a dominant source of atmospheric aerosols. Sulfuric acid (SA)-amine binary nucleation with dimethylamine (DMA) has been recognized as a governing mechanism in the polluted continental boundary layer. Here we demonstrate the importance of trimethylamine (TMA) for nucleation in the complex atmosphere and propose a molecular-level SA-DMA-TMA ternary nucleation mechanism as an improvement upon the conventional binary mechanism. Using the proposed mechanism, we could connect the gaseous amines to the SA-amine cluster signals measured in the atmosphere of urban Beijing. Results show that TMA can accelerate the SA-DMA-based new particle formation in Beijing by 50–100%. Considering the global abundance of TMA and DMA, our findings imply comparable importance of TMA and DMA to nucleation in the polluted continental boundary layer, with probably higher contributions from TMA in polluted rural environments and future urban environments with controlled DMA emissions.

54 ENVIRONMENTAL SCIENCES↗

Impact of truck electrification on air pollution disparities in the United States

Electrifying heavy-duty trucks reduces on-road diesel emissions but shifts the burden of supplying energy to power-generation facilities. The combined effect of Inflation Reduction Act investments in grid decarbonization and truck electrification will alter the magnitude and distribution of air pollution burdens across the United States. These investments are intended to facilitate a just energy transition, with 40% of the benefits flowing to disadvantaged communities per the Justice40 Initiative. Here we evaluate the combined effects of Inflation Reduction Act grid decarbonization and truck electrification investments on a national scale to determine whether the air pollution benefits would meet this 40% goal for both disadvantaged communities and the most exposed racial–ethnic groups. We find that truck electrification and decarbonization reduce air-pollution-related premature mortality in disadvantaged communities. However, the relative disparity between disadvantaged and non-disadvantaged communities increases, suggesting that a disproportionate share of benefits accrue to non-disadvantaged communities. Whereas absolute disparity in grid emissions decreases over time for all racial–ethnic groups, relative disparity remains largely unchanged, with Black populations being the most exposed. Electrifying drayage corridors would result in comparatively large health benefits for disadvantaged communities, suggesting that increasing targeted electrification investments in short-haul routes near urban areas (for example, ports) could be promising.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

Anthropogenic sulfate aerosol pollution in South and East Asia induces increased summer precipitation over arid Central Asia

Precipitation has increased across the arid Central Asia region over recent decades. However, the underlying mechanisms of this trend are poorly understood. Here, we analyze multi-model simulations from the Precipitation Driver and Response Model Intercomparison Project (PDRMIP) to investigate potential drivers of the observed precipitation trend. We find that anthropogenic sulfate aerosols over remote polluted regions in South and East Asia lead to increased summer precipitation, especially convective and extreme precipitation, in arid Central Asia. Elevated concentrations of sulfate aerosols over remote polluted Asia cause an equatorward shift of the Asian Westerly Jet Stream through a fast response to cooling of the local atmosphere at mid-latitudes. This shift favours moisture supply from low-latitudes and moisture flux convergence over arid Central Asia, which is confirmed by a moisture budget analysis. High levels of absorbing black carbon lead to opposing changes in the Asian Westerly Jet Stream and reduced local precipitation, which can mask the impact of sulfate aerosols. This teleconnection between arid Central Asia precipitation and anthropogenic aerosols in remote Asian polluted regions highlights long-range impacts of anthropogenic aerosols on atmospheric circulations and the hydrological cycle.

54 ENVIRONMENTAL SCIENCES↗

Isoprene photo-oxidation products quantify the effect of pollution on hydroxyl radicals over Amazonia

Nitrogen oxides (NO x ) emitted from human activities are believed to regulate the atmospheric oxidation capacity of the troposphere. However, observational evidence is limited for the low-to-median NO x concentrations prevalent outside of polluted regions. Directly measuring oxidation capacity, represented primarily by hydroxyl radicals (OH), is challenging, and the span in NO x concentrations at a single observation site is often not wide. Concentrations of isoprene and its photo-oxidation products were used to infer the equivalent noontime OH concentrations. The fetch at an observation site in central Amazonia experienced varied contributions from background regional air, urban pollution, and biomass burning. The afternoon concentrations of reactive nitrogen oxides (NO y ), indicative of NO x exposure during the preceding few hours, spanned from 0.3 to 3.5 parts per billion. Accompanying the increase of NO y concentration, the inferred equivalent noontime OH concentrations increased by at least 250% from 0.6 × 10 6 to 1.6 × 10 6 cm -3 . The conclusion is that, compared to background conditions of low NO x concentrations over the Amazon forest, pollution increased NO x concentrations and amplified OH concentrations, indicating the susceptibility of the atmospheric oxidation capacity over the forest to anthropogenic influence and reinforcing the important role of NO x in sustaining OH concentrations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

rfasst: An R tool to estimate air pollution impacts on health and agriculture

Existing scientific literature shows that health and agricultural impacts attributable to air pollution are significant and should be considered in the integrated analysis of human and Earth-system interactions. The implementation of policies that affect the power sector, the composition of the vehicle fleet or the investments and deployment of different energy sources will in turn result in different levels of air pollution. Even though the various methodologies for estimating the impacts of air pollution, such as exposure-response functions, are extensively applied by the scientific community, they are normally not included in integrated assessment modeling outputs.

97 MATHEMATICS AND COMPUTING↗