Observations and Modeling of NOx Photochemistry and Fate in Fresh Wildfire Plumes DOI
Qiaoyun Peng, Brett B. Palm, Carley D. Fredrickson

et al.

ACS Earth and Space Chemistry, Journal Year: 2021, Volume and Issue: 5(10), P. 2652 - 2667

Published: Sept. 13, 2021

With large primary emissions of nitrogen-containing compounds, wildfires impact the tropospheric oxidizing capacity, ozone (O3), and formation secondary organic inorganic aerosol. The fate reactive nitrogen in daytime fresh wildfire plumes was examined using airborne measurements over western U.S. during Wildfire Experiment for Cloud chemistry, Aerosol absorption, Nitrogen (WE-CAN) campaign summer 2018 together with a photochemical box model. For four sampled pseudo-Lagrangian manner, model predicts that majority emitted NOx (96 ± 2%) is converted into peroxyacetyl nitrate (PAN) (27 8%) sum gas particulate HNO3 (29 5%) within few hours plume evolution. In two highest initial HONO, default significantly underestimates observed dilution-normalized decay rate age. We investigated several potential causes this discrepancy found likely does not accurately represent suite oxidized species such as alkyl acyl peroxynitrates these fire plumes, consistent compounds measured by chemical ionization mass spectrometry. This reservoir can be similar magnitude to PAN thus represents an important uncertain impacts on downwind O3 aerosol depending whether are (APNs), nitrates (RONO2), or nitro-aromatics.

Language: Английский

Aging Effects on Biomass Burning Aerosol Mass and Composition: A Critical Review of Field and Laboratory Studies DOI
Anna L. Hodshire, Ali Akherati, M. J. Alvarado

et al.

Environmental Science & Technology, Journal Year: 2019, Volume and Issue: 53(17), P. 10007 - 10022

Published: July 31, 2019

Biomass burning is a major source of atmospheric particulate matter (PM) with impacts on health, climate, and air quality. The particles vapors within biomass plumes undergo chemical physical aging as they are transported downwind. Field measurements the evolution PM plume age range from net decreases to increases, most showing little no change. In contrast, laboratory studies tend show significant mass increases average. On other hand, similar effects average composition (e.g., oxygen-to-carbon ratio) reported for lab field studies. Currently, there consensus mechanisms that lead these observed similarities differences. This review summarizes available observations aging-related aerosol concentrations markers, discusses four broad hypotheses explain variability between campaigns: (1) in emissions chemistry, (2) differences dilution/entrainment, (3) losses chambers lines, (4) timing initial measurement, baseline which changes estimated. We conclude concise set research needs advancing our understanding aerosol.

Language: Английский

Citations

248

Aging of Atmospheric Brown Carbon Aerosol DOI
Rachel F. Hems, Elijah G. Schnitzler, Carolyn Liu-Kang

et al.

ACS Earth and Space Chemistry, Journal Year: 2021, Volume and Issue: 5(4), P. 722 - 748

Published: April 5, 2021

Emitted by numerous primary sources and formed secondary sources, atmospheric brown carbon (BrC) aerosol is chemically complex. As BrC ages in the atmosphere via a variety of chemical physical processes, its composition optical properties change significantly, altering impacts on climate. Research past decade has considerably expanded our understanding reactions both gas condensed phases. We review these recent advances aging chemistry with focus phase leading to formation, aqueous in-cloud particle reactions. Connections are made between single component proxies more complex mixtures as well laboratory field measurements chemistry. General conclusions that can darken particles over short time scales hours close source considerable photobleaching oxidative whitening will occur when day or removed from source.

Language: Английский

Citations

242

Formation of Secondary Brown Carbon in Biomass Burning Aerosol Proxies through NO3 Radical Reactions DOI

Chunlin Li,

Quanfu He, Anusha P. S. Hettiyadura

et al.

Environmental Science & Technology, Journal Year: 2019, Volume and Issue: 54(3), P. 1395 - 1405

Published: Nov. 15, 2019

Atmospheric brown carbon (BrC) is an important contributor to the radiative forcing of climate by organic aerosols. Because molecular diversity BrC compounds and their dynamic transformations, it challenging predictively understand optical properties. OH radical O3 reactions, together with photolysis, lead diminished light absorption lower warming effects biomass burning BrC. The night-time aging on properties aerosols are less known. To address this knowledge gap, NO3 chemistry tar from wood pyrolysis was investigated in a flow reactor. This study shows that change because transformations driven reactions form new absorbing species significant enhancement over ultraviolet–visible (UV-vis) range. overnight increases mass coefficients factor 1.3–3.2 between 380 nm 650 nm. Nitrated compounds, particularly nitroaromatics, were identified as main products contribute enhanced secondary Night-time represents source can have pronounced effect atmospheric air pollution.

Language: Английский

Citations

159

Rapid dark aging of biomass burning as an overlooked source of oxidized organic aerosol DOI Creative Commons
John K. Kodros, Dimitrios K. Papanastasiou, Marco Paglione

et al.

Proceedings of the National Academy of Sciences, Journal Year: 2020, Volume and Issue: 117(52), P. 33028 - 33033

Published: Dec. 14, 2020

Significance To quantify the full implications of biomass burning emissions on atmosphere, it is essential to accurately represent emission plume after has undergone chemical aging in atmosphere. Atmospheric models typically consider predominant pathway take place presence sunlight (via OH radical); however, this mechanism leads consistent underpredictions oxidized organic aerosol wintertime urban areas. Here, we show, through a combination laboratory experiments, ambient field measurements, and transport modeling, that plumes exposed NO 2 O 3 age rapidly without requiring any sunlight, thus providing an overlooked source previously not accounted for models.

Language: Английский

Citations

155

Fire Influence on Regional to Global Environments and Air Quality (FIREX‐AQ) DOI Creative Commons
C. Warneke, Joshua P. Schwarz, Jack E. Dibb

et al.

Journal of Geophysical Research Atmospheres, Journal Year: 2022, Volume and Issue: 128(2)

Published: Dec. 30, 2022

Abstract The NOAA/NASA Fire Influence on Regional to Global Environments and Air Quality (FIREX‐AQ) experiment was a multi‐agency, inter‐disciplinary research effort to: (a) obtain detailed measurements of trace gas aerosol emissions from wildfires prescribed fires using aircraft, satellites ground‐based instruments, (b) make extensive suborbital remote sensing fire dynamics, (c) assess local, regional, global modeling fires, (d) strengthen connections observables the ground such as fuels fuel consumption satellite products burned area radiative power. From Boise, ID western were studied with NASA DC‐8 two NOAA Twin Otter aircraft. high‐altitude ER‐2 deployed Palmdale, CA observe some these in conjunction overpasses other Further conducted three mobile laboratories sites, 17 different forecast analyses for fire, air quality climate implications. Salina, KS investigated 87 smaller Southeast in‐situ data collection. Sampling by all platforms designed measure gases aerosols multiple transects capture chemical transformation perform observations smoke plumes under day night conditions. linked consumed power orbital collected during overflights sampling fuels.

Language: Английский

Citations

82

The formation and mitigation of nitrate pollution: comparison between urban and suburban environments DOI Creative Commons

Suxia Yang,

Bin Yuan, Yuwen Peng

et al.

Atmospheric chemistry and physics, Journal Year: 2022, Volume and Issue: 22(7), P. 4539 - 4556

Published: April 8, 2022

Abstract. Ambient nitrate has been of increasing concern in PM2.5, while there are still large uncertainties quantifying the formation aerosol. The pathways aerosol at an urban site and a suburban Pearl River Delta (PRD) investigated using observation-constrained box model. Throughout campaigns, pollution episodes were constantly accompanied with increase concentrations fractions both sites. simulations demonstrate that chemical reactions daytime night contributed significantly to boundary layer two However, nighttime predominantly occurred aloft residual site, downward transport from morning is important source (53 %) for surface whereas similar amounts produced nocturnal which results little ground site. We show was volatile-organic-compound-limited (VOC-limited) regime transition identical response ozone reduction VOC emissions can be efficient approach mitigate areas through influencing hydroxyl radical (OH) N2O5 production, will also beneficial synergistic control regional pollution. highlight relative importance site-specific, quantitative understanding various provide insights developing mitigation strategies.

Language: Английский

Citations

76

Effects of Fire Diurnal Variation and Plume Rise on U.S. Air Quality During FIREX‐AQ and WE‐CAN Based on the Multi‐Scale Infrastructure for Chemistry and Aerosols (MUSICAv0) DOI Creative Commons
Wenfu Tang, L. K. Emmons, Rebecca R. Buchholz

et al.

Journal of Geophysical Research Atmospheres, Journal Year: 2022, Volume and Issue: 127(16)

Published: Aug. 12, 2022

Abstract We analyze the effects of diurnal cycle fire emissions (DCFE) and plume rise on U.S. air quality using MUSICAv0 (Multi‐Scale Infrastructure for Chemistry Aerosols Version 0) model during FIREX‐AQ (Fire Influence Regional to Global Environments Air Quality) WE‐CAN (Western wildfire Experiment Cloud chemistry, Aerosol absorption Nitrogen) field campaigns. To include DCFE in model, we employ two approaches: a climatology derived from satellite radiative power product. also implemented sets plume‐rise climatologies, parameterizations. evaluate performance with airborne measurements, EPA Quality System surface products. Overall, including improves agreement observations such as aircraft CO NO x WE‐CAN. Applying performance, PM 2.5 fire‐impacted regions. The impact is larger than DCFE. Plume can greatly enhance modeled long‐range transport fire‐emitted pollutants. simulations parameterizations generally perform better climatologies FIREX‐AQ, but not 2019 Williams Flats Fire case study demonstrates that change impacts because are subject different meteorology chemistry when emitted at times day altitudes. Moreover, local‐to‐regional chemical reaction rates. will be included future MUSICA versions.

Language: Английский

Citations

76

Shortwave absorption by wildfire smoke dominated by dark brown carbon DOI Creative Commons
Rajan K. Chakrabarty, Nishit Shetty, Arashdeep Singh Thind

et al.

Nature Geoscience, Journal Year: 2023, Volume and Issue: 16(8), P. 683 - 688

Published: Aug. 1, 2023

Wildfires emit large amounts of black carbon and light-absorbing organic carbon, known as brown into the atmosphere. These particles perturb Earth's radiation budget through absorption incoming shortwave radiation. It is generally thought that loses its absorptivity after emission in atmosphere due to sunlight-driven photochemical bleaching. Consequently, atmospheric warming effect exerted by remains highly variable poorly represented climate models compared with relatively nonreactive carbon. Given wildfires are predicted increase globally coming decades, it increasingly important quantify these radiative impacts. Here we present measurements ensemble-scale particle-scale smoke plumes from western United States. We find a type dark contributes three-quarters short visible light half long absorption. This strongly absorbing aerosol species water insoluble, resists daytime photobleaching increases night-time processing. Our findings suggest parameterizations need be revised improve estimation forcing associated warming.

Language: Английский

Citations

63

A newly developed Lagrangian chemical transport scheme: Part 1. Simulation of a boreal forest fire plume DOI
Yayong Liu, Yufei Huang, John Liggio

et al.

The Science of The Total Environment, Journal Year: 2023, Volume and Issue: 880, P. 163232 - 163232

Published: April 4, 2023

Language: Английский

Citations

43

Molecular Characterization of Water- and Methanol-Soluble Organic Compounds Emitted from Residential Coal Combustion Using Ultrahigh-Resolution Electrospray Ionization Fourier Transform Ion Cyclotron Resonance Mass Spectrometry DOI
Jianzhong Song,

Meiju Li,

Xingjun Fan

et al.

Environmental Science & Technology, Journal Year: 2019, Volume and Issue: 53(23), P. 13607 - 13617

Published: Nov. 4, 2019

Water-soluble organic compounds (WSOC) and methanol-soluble (MSOC) in smoke particles emitted from residential coal combustion were characterized by ultrahigh-resolution mass spectrometry. The results showed that the molecular compositions of WSOC MSOC are different. S-containing (CHOS CHONS) found to be dominant components (65-87%) WSOC, whereas CHO CHON make a great contribution (79-96%) samples. It is worth noting greater abundance was produced compared biomass burning atmospheric also varied significantly depending on maturity coal. derived low-maturity contained higher proportion oxidized functional groups but with lower degree aromaticity than high-maturity Our findings suggest molecules high modified index, low O/C ratio, polarity stronger light absorption. This study suggests contributed absorption may stronger.

Language: Английский

Citations

126