Volatile chemical product emissions enhance ozone and modulate urban chemistry

Proceedings of the National Academy of Sciences, Journal Year: 2021, Volume and Issue: 118(32)

Published: Aug. 2, 2021

Significance Recent work in Los Angeles has shown that urban volatile organic compound (VOC) emissions from consumer and industrial products—termed chemical products (VCPs)—are now an important source of ozone precursors. Using advancements VOC instrumentation, we show VCP are ubiquitous regions can be identified via unique fingerprints. Through detailed modeling, VCPs as to production fossil fuel VOCs the chemistry have significant impacts on model simulations key atmospheric processes. Consequently, air quality models must updated account for both order capture their full impact quality.

Language: Английский

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The Community Multiscale Air Quality (CMAQ) model versions 5.3 and 5.3.1: system updates and evaluation

Geoscientific model development, Journal Year: 2021, Volume and Issue: 14(5), P. 2867 - 2897

Published: May 20, 2021

The Community Multiscale Air Quality (CMAQ) model version 5.3 (CMAQ53), released to the public in August 2019 and followed by 5.3.1 (CMAQ531) December 2019, contains numerous science updates, enhanced functionality, improved computation efficiency relative previous of model, 5.2.1 (CMAQ521). Major advances new include a aerosol module (AERO7) with significant updates secondary organic (SOA) chemistry, updated chlorine detailed bromine iodine simple halogen addition dimethyl sulfide (DMS) chemistry CB6r3 chemical mechanism, M3Dry bidirectional deposition Surface Tiled Aerosol Gaseous Exchange (STAGE) model. In addition, support for Weather Research Forecasting (WRF) model's hybrid vertical coordinate (HVC) was added CMAQ53 Meteorology-Chemistry Interface Processor (MCIP) 5.0 (MCIP50). Enhanced functionality includes Detailed Emissions Scaling, Isolation Diagnostic (DESID) system scaling incoming emissions CMAQ reading multiple gridded input emission files. Evaluation CMAQ531 performed comparing monthly seasonal mean daily 8 h average (MDA8) O3 PM2.5 values from several simulations similarly configured CMAQ521 simulation encompassing 2016. For MDA8 O3, has higher winter versus CMAQ521, due primarily reduced dry snow, which strongly reduces wintertime bias (2-4 ppbv average). is lower throughout rest year, particularly spring, part lateral boundary conditions (BCs), generally increases spring fall ( 0.5 μg m-3). 24 PM2.5, concentrations on fall, summer, similar slightly summer. Comparisons were also isolate specific aspects modeling system, namely BCs, meteorology version, used. Transitioning hemispheric (HCMAQ) HCMAQ provide BCs contributes mixing ratios regional latitudes during (due decreased snow CMAQ53) middle year-round over ocean CMAQ53). WRF 3.8 4.1.1 HVC resulted consistently (1.0-1.5 ppbv) (0.1-0.25 m-3) year. Finally, comparisons STAGE models showed that outside while differences assumptions particle velocities non-vegetated surfaces land use short vegetation (e.g., grasslands) between two models. ambient NH3, smaller winter, but larger error correlation

Language: Английский

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Secondary organic aerosol association with cardiorespiratory disease mortality in the United States

Nature Communications, Journal Year: 2021, Volume and Issue: 12(1)

Published: Dec. 16, 2021

Abstract Fine particle pollution, PM 2.5 , is associated with increased risk of death from cardiorespiratory diseases. A multidecadal shift in the United States (U.S.) composition towards organic aerosol as well advances predictive algorithms for secondary (SOA) allows novel examinations role components on mortality. Here we show SOA strongly county-level rates U.S. independent total mass association largest associations located southeastern Compared to variability across 3.5× greater per capita On a basis, 6.5× higher rate mortality than and biogenic anthropogenic carbon sources both play overall Our results suggest reducing health impacts requires consideration SOA.

Language: Английский

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Evaluating the Impact of Chemical Complexity and Horizontal Resolution on Tropospheric Ozone Over the Conterminous US With a Global Variable Resolution Chemistry Model

Journal of Advances in Modeling Earth Systems, Journal Year: 2022, Volume and Issue: 14(6)

Published: May 21, 2022

A new configuration of the Community Earth System Model (CESM)/Community Atmosphere with full chemistry (CAM-chem) supporting capability horizontal mesh refinement through use spectral element (SE) dynamical core is developed and called CESM/CAM-chem-SE. Horizontal in CESM/CAM-chem-SE unique novel that pollutants such as ozone are accurately represented at human exposure relevant scales while also directly including global feedbacks. down to ∼14 km over conterminous US (CONUS) beginning Multi-Scale Infrastructure for Chemistry Aerosols (MUSICAv0). Here, MUSICAv0 evaluated used better understand how resolution chemical complexity impact precursors CONUS compared measurements from five aircraft campaigns, which occurred 2013. This field campaign analysis demonstrates importance using finer simulate nitrogen oxides carbon monoxide. In general, more complex on other oxidation products pronounced when where a larger number regimes resolved. Large model biases near surface remain Southeast observations even updated resolution. suggests need adding replacing sections emission inventories regional inventories, increasing vertical planetary boundary layer, reducing meteorological variables temperature clouds.

Language: Английский

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A synergistic ozone-climate control to address emerging ozone pollution challenges

One Earth, Journal Year: 2023, Volume and Issue: 6(8), P. 964 - 977

Published: Aug. 1, 2023

Tropospheric ozone threatens human health and crop yields, exacerbates global warming, fundamentally changes atmospheric chemistry. Evidence has pointed toward widespread increases in the troposphere, particularly surface is chemically complex difficult to abate. Despite past successes some regions, a solution new challenges of pollution warming climate remains unexplored. In this perspective, by compiling measurements at ∼4,300 sites worldwide between 2014 2019, we show emerging challenge pollution, featuring unintentional rise due uncoordinated emissions reduction increasing penalty. On basis shared emission sources, interactive chemical mechanisms, synergistic effects propose ozone-climate control strategy incorporating joint fine particulate matter. This presents an opportunity alleviate tropospheric forthcoming low-carbon transition.

Language: Английский

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Volatile organic compounds: A threat to the environment and health hazards to living organisms – A review

Journal of Biotechnology, Journal Year: 2024, Volume and Issue: 382, P. 51 - 69

Published: Jan. 17, 2024

Language: Английский

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Substantially underestimated global health risks of current ozone pollution

Nature Communications, Journal Year: 2025, Volume and Issue: 16(1)

Published: Jan. 2, 2025

Existing assessments might have underappreciated ozone-related health impacts worldwide. Here our study assesses current global ozone pollution using the high-resolution (0.05°) estimation from a geo-ensemble learning model, with key focuses on population exposure and all-cause mortality burden. Our model demonstrates strong performance, achieving mean bias of less than -1.5 parts per billion against in-situ measurements. We estimate that 66.2% is exposed to excess for short term (> 30 days year), 94.2% suffers long-term exposure. Furthermore, severe levels are observed in Cropland areas, particularly over Asia. Importantly, ozone-attributable deaths significantly surpass previous recognition specific diseases Notably, mid-latitude Asia (30°N) western United States show high burden, contributing substantially deaths. highlights significant risks may benefit ozone-exposed future. This reveals O₃-related risks, model.

Language: Английский

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Simulation of organic aerosol formation during the CalNex study: updated mobile emissions and secondary organic aerosol parameterization for intermediate-volatility organic compounds

Atmospheric chemistry and physics, Journal Year: 2020, Volume and Issue: 20(7), P. 4313 - 4332

Published: April 14, 2020

Abstract. We describe simulations using an updated version of the Community Multiscale Air Quality model 5.3 (CMAQ v5.3) to investigate contribution intermediate-volatility organic compounds (IVOCs) secondary aerosol (SOA) formation in southern California during CalNex study. first derive a model-ready parameterization for SOA from IVOC emissions mobile sources. To account both diesel and gasoline sources, has six lumped precursor species that resolve volatility molecular structure (aromatic versus aliphatic). also implement new mobile-source emission profiles quantify all IVOCs based on direct measurements. The have been released SPECIATE 5.0. By incorporating comprehensive semivolatile (SVOCs) experimentally constrained yields, this CMAQ configuration best represents sources urban regional ambient (OA). In Los Angeles region, emit 4 times more non-methane gases (NMOGs) than but emits roughly 3 absolute basis. revised predicts (including on- off-road gasoline, aircraft, diesel) contribute ∼1 µg m−3 daily peak concentration Pasadena. This ∼70 % increase predicted compared base CMAQ. Therefore, almost as much traditional precursors such single-ring aromatics. However, accounting these does not reproduce measurements either or IVOCs. potential other we performed two exploratory with varying amounts nonmobile close mass balance primary hydrocarbon IVOCs, would need 12 NMOG (or equivalently 30.7 t d−1 Angeles–Pasadena region), value is well within reported range content volatile chemical products. explain mildly oxygenated Pasadena, additional 14.8 nonmobile-source be (assuming yields apply IVOCs). IVOC-to-NMOG ratio 26.8 68.5 region) likely unrealistically high. Our results highlight important production region underscore uncertainties must addressed (multigenerational aging, aqueous chemistry vapor wall losses) balance. research highlights effectiveness regulations reduce emissions, which turn increased relative importance

Language: Английский

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Reactive organic carbon emissions from volatile chemical products

Atmospheric chemistry and physics, Journal Year: 2021, Volume and Issue: 21(6), P. 5079 - 5100

Published: March 31, 2021

Volatile chemical products (VCPs) are an increasingly important source of anthropogenic reactive organic carbon (ROC) emissions. Among these sources everyday items, such as personal care products, general cleaners, architectural coatings, pesticides, adhesives, and printing inks. Here, we develop VCPy, a new framework to model emissions from VCPs throughout the United States, including spatial allocation regional local scales. Evaporation species VCP mixture in VCPy is function compound-specific physiochemical properties that govern volatilization timescale relevant for product evaporation. We introduce two terms describe processes: evaporation use timescale. Using this framework, predicted national per capita 9.5 kg person year (6.4 C year) 2016, which translates 3.05 Tg (2.06 C), making dominant States. Uncertainty associated with sensitivity select parameters were characterized through Monte Carlo analysis, resulting 95 % confidence interval 2016 2.61-3.53 (1.76-2.38 C). This nationwide total broadly consistent U.S. EPA's 2017 National Emission Inventory (NEI); however, county-level categorical estimates can differ substantially NEI values. predicts higher than approximately half all counties, 5 counties having greater 55 Categorically, application yields (150 %) paints coatings (25 when compared NEI, whereas pesticides (-54 inks (-13 feature lower An observational evaluation indicates key reproduced high fidelity using (normalized mean bias -13 r =0.95). Sector-wide, effective secondary aerosol yield maximum incremental reactivity 5.3 by mass 1.58 gO3 g-1, respectively, indicating important, likely date underrepresented, pollution urban environments.

Language: Английский

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Modeling secondary organic aerosol formation from volatile chemical products

Atmospheric chemistry and physics, Journal Year: 2021, Volume and Issue: 21(24), P. 18247 - 18261

Published: Dec. 16, 2021

Volatile chemical products (VCPs) are commonly-used consumer and industrial items that an important source of anthropogenic emissions. Organic compounds from VCPs evaporate on atmospherically relevant time scales include many species secondary organic aerosol (SOA) precursors. However, the chemistry leading to SOA, particularly intermediate volatility (IVOCs), has not been fully represented in regional-scale models such as Community Multiscale Air Quality (CMAQ) model, which tend underpredict SOA concentrations urban areas. Here we develop a model represent formation VCP The incorporates new emissions inventory employs three classes emissions: siloxanes, oxygenated IVOCs, nonoxygenated IVOCs. estimated produce 1.67 μg m-3 noontime doubling current predictions reducing mass concentration bias -75% -58% when compared observations Los Angeles 2010. While emitted similar quantities, is dominated by Formaldehyde show relationships temperature signatures indicating common sources and/or chemistry. This work suggests contribute up half must better precursors predict enhancement SOA.

Language: Английский

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