Comment on egusphere-2023-1355 DOI Creative Commons
Alexandre Albinet

Published: Sept. 26, 2023

Abstract. Secondary organic aerosols (SOA) formed by oxidation of typical precursors largely emitted biomass burning, such as PAHs and furans, are still poorly characterized in terms formation yields, physical light absorption properties, particularly those generated at night following reaction with nitrate radicals (NO3). In the present study, we evaluated compared effective density (ρeff), Ångström exponent (α), mass coefficient (MAC) laboratory-generated SOA from three furan compounds (furan, 2-methylfuran, 2,5-dimethylfuran) four (naphthalene, acenaphthylene, fluorene, phenanthrene). were an flow reactor between hydroxyl (OH; 0.1–20 equivalent aging days) or NO3 (0.05–6 nights 14 h) single PAH. The ρeff, α, MAC varied depending on precursor oxidant considered. ρeff OH tended to increase particle size before reaching a “plateau”. This was evident for nighttime chemistry experiments (1.2 1.6 average particles > 100 nm). Such results highlighted potential differences chemical composition SOA, well probably their morphology, according size. Three times lower yields obtained OH. PAH (18 76 %) 5 6 higher than furans (3–12 %). While showed low negligible found have significant impact UV-Visible region, implying contribution atmospheric brown carbon (BrC). No values observed processes, due nitrogen-containing chromophores through homogeneous gas phase processes only (without NOx). Overall, this work demonstrated that both, day- substantial aerosol properties so climate.

Language: Английский

Secondary Brown Carbon Formation From Photooxidation of Furans From Biomass Burning DOI Creative Commons
Taekyu Joo, Jo Machesky, Linghan Zeng

et al.

Geophysical Research Letters, Journal Year: 2024, Volume and Issue: 51(1)

Published: Jan. 4, 2024

Abstract Furans are a major class of volatile organic compounds emitted from biomass burning. Their high reactivity with atmospheric oxidants leads to the formation secondary aerosol (SOA), including brown carbon (BrC) that can affect global climate via interactions solar radiation. Here, we investigate optical properties and chemical composition SOA generated photooxidation furfural, 2‐methylfuran, 3‐methylfuran under dry (RH < 5%) humid ∼ 50%) conditions in presence nitrogen oxides (NO x ) ammonium sulfate seed aerosol. Dry furfural oxidation has greatest BrC formation, reduced nitrogen‐containing (NOCs) SOA, which dominated by amines amides formed reactions between carbonyls ammonia/ammonium. Based on products detected, propose novel pathways NOCs photooxidation, contribute accretion during photochemical aging burning plumes.

Language: Английский

Citations

9
Emissions and Atmospheric Chemistry of Furanoids from Biomass Burning: Insights from Laboratory to Atmospheric Observations DOI Creative Commons
Manolis N. Romanías, Matthew M. Coggon,

Fatima Al Ali

et al.

ACS Earth and Space Chemistry, Journal Year: 2024, Volume and Issue: 8(5), P. 857 - 899

Published: April 8, 2024

Furanoids are a class of reactive volatile organic compounds that major products from the pyrolysis and combustion biomass polymers, including cellulose, hemicellulose, lignin. Biomass burning is an atmospheric source furanoids increasing in frequency intensity throughout regions world. Once emitted to atmosphere, may react with oxidants form secondary pollutants hazardous human health, ozone (O3) aerosol (SOA). This review comprehensive assessment literature between 1977 present describing emissions fate wild, prescribed, domestic fires. The organized by presenting physical properties key first, followed summary biopolymer reactions lead furanoid formation. Next, factors compiled across typical fuels consumed highlight species smoke. We next available kinetic degradation mechanism data characterize reaction rates, gas-phase products, SOA formed as result OH, NO3, O3, Cl radicals. then describe studies have focused on evaluating chemistry their impacts air quality using combination field observations model simulations. conclude perspective identifies future research directions would address gaps improve understanding processes.

Language: Английский

Citations

8
Contribution of Carbonyl Chromophores in Secondary Brown Carbon from Nighttime Oxidation of Unsaturated Heterocyclic Volatile Organic Compounds DOI Creative Commons
Kunpeng Chen, Raphael Mayorga, Caitlin Hamilton

et al.

Environmental Science & Technology, Journal Year: 2023, Volume and Issue: 57(48), P. 20085 - 20096

Published: Nov. 20, 2023

The light absorption properties of brown carbon (BrC), which are linked to molecular chromophores, may play a significant role in the Earth's energy budget. While nitroaromatic compounds have been identified as strong chromophores wildfire-driven BrC, other types remain be investigated. Given electron-withdrawing nature carbonyls ubiquitous atmosphere, we characterized carbonyl BrC samples from nighttime oxidation furan and pyrrole derivatives, important but understudied precursors secondary organic aerosols primarily found wildfire emissions. Various were quantified samples, their ultraviolet-visible spectra simulated by using time-dependent density functional theory. Our findings suggest that with bonded nitrogen (i.e., imides amides) derived N-containing heterocyclic substantially contribute absorption. contributed over 40% total at wavelengths below 350 nm above 430 BrC. contributions differed significantly wavelength, highlighting divergent importance different wavelength ranges. Overall, our highlight significance underscore need for further investigation.

Language: Английский

Citations

16
Relative Humidity Modulates the Physicochemical Processing of Secondary Brown Carbon Formation from Nighttime Oxidation of Furan and Pyrrole DOI Creative Commons
Kunpeng Chen, Caitlin Hamilton,

B. Ries

et al.

ACS ES&T Air, Journal Year: 2024, Volume and Issue: 1(5), P. 426 - 437

Published: April 9, 2024

Light-absorbing secondary organic aerosols (SOAs), also known as brown carbon (BrC), are major components of wildfire smoke that can have a significant impact on the climate system; however, how environmental factors such relative humidity (RH) influence their formation is not fully understood, especially for heterocyclic precursors. We conducted chamber experiments to investigate BrC from nighttime oxidation furan and pyrrole, two primary precursors in wildfires, presence pre-existing particles at RH < 20% ∼ 50%. Our findings revealed increasing significantly affected size distribution dynamics both SOAs, with pyrrole SOA showing stronger potential generate ultrafine via intensive nucleation processes. Higher led increased mass fractions oxygenated compounds suggesting enhanced gas-phase and/or multiphase under humid conditions. Moreover, higher reduced absorption coefficients BrC, contrasting those homocyclic precursors, due non-absorbing high-molecular-weight decreasing molecular chromophores. Overall, our demonstrate unique dependence which may critically modulate radiative effects change.

Language: Английский

Citations

6
Light Absorption of Black and Brown Carbon in Eastern China DOI
Rongzhi Tang,

Weizhen Cui,

Xiuli Zhang

et al.

Journal of Hazardous Materials, Journal Year: 2025, Volume and Issue: 489, P. 137530 - 137530

Published: Feb. 8, 2025

Language: Английский

Citations

0
Insights into secondary organic aerosol formation from the day- and nighttime oxidation of polycyclic aromatic hydrocarbons and furans in an oxidation flow reactor DOI Creative Commons
Abd El Rahman El Mais, Barbara D’Anna, Luka Drinovec

et al.

Atmospheric chemistry and physics, Journal Year: 2023, Volume and Issue: 23(23), P. 15077 - 15096

Published: Dec. 7, 2023

Abstract. Secondary organic aerosols (SOAs) formed by oxidation of typical precursors largely emitted biomass burning, such as polycyclic aromatic hydrocarbons (PAHs) and furans, are still poorly characterized. We evaluated compared the formation yields, effective density (ρeff), absorption Ångström exponent (α), mass coefficient (MAC) laboratory-generated SOAs from three furan compounds four PAHs. were generated in an flow reactor under day- (OH radicals) or nighttime (NO3 conditions. The ρeff, α, MAC varied depending on precursor oxidant considered. ρeff with OH NO3 tended to increase particle size before reaching a “plateau”, highlighting potential differences SOA chemical composition and/or morphology, according size. Three times lower yields obtained OH. PAH (18 %–76 %) five six higher than those for furans (3 %–12 %). While showed low negligible light properties, had significant impact UV–visible region, implying contribution atmospheric brown carbon. No values was observed processes, probably due nitrogen-containing chromophores only (without NOx). results demonstrated that PAHs through both, have substantial aerosol properties.

Language: Английский

Citations

7
Insights into secondary organic aerosol formation from the day- and nighttime oxidation of PAHs and furans in an oxidation flow reactor DOI Creative Commons
Abd El Rahman El Mais, Barbara D’Anna, Luka Drinovec

et al.

Published: July 4, 2023

Abstract. Secondary organic aerosols (SOA) formed by oxidation of typical precursors largely emitted biomass burning, such as PAHs and furans, are still poorly characterized in terms formation yields, physical light absorption properties, particularly those generated at night following reaction with nitrate radicals (NO3). In the present study, we evaluated compared effective density (ρeff), Ångström exponent (α), mass coefficient (MAC) laboratory-generated SOA from three furan compounds (furan, 2-methylfuran, 2,5-dimethylfuran) four (naphthalene, acenaphthylene, fluorene, phenanthrene). were an flow reactor between hydroxyl (OH; 0.1–20 equivalent aging days) or NO3 (0.05–6 nights 14 h) single PAH. The ρeff, α, MAC varied depending on precursor oxidant considered. ρeff OH tended to increase particle size before reaching a “plateau”. This was evident for nighttime chemistry experiments (1.2 1.6 average particles > 100 nm). Such results highlighted potential differences chemical composition SOA, well probably their morphology, according size. Three times lower yields obtained OH. PAH (18 76 %) 5 6 higher than furans (3–12 %). While showed low negligible found have significant impact UV-Visible region, implying contribution atmospheric brown carbon (BrC). No values observed processes, due nitrogen-containing chromophores through homogeneous gas phase processes only (without NOx). Overall, this work demonstrated that both, day- substantial aerosol properties so climate.

Language: Английский

Citations

1
Overlooked Trace Molecules in Organic Aerosol Revealed by Gas Chromatography–Orbitrap Mass Spectrometry DOI
Ting Wang, Ru‐Jin Huang, Jing Miao

et al.

Environmental Science & Technology, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 2, 2024

Molecular characterization of organic aerosol (OA) is crucial for understanding its sources and atmospheric processes. However, the chemical components OA remain not well constrained. This study used gas chromatography–Orbitrap mass spectrometry (GC-Orbitrap MS) GC-Quadrupole MS (GC-qMS) to investigate composition in PM2.5 from Xi'an, Northwest China. GC-Orbitrap identified 335 tracers, including overlooked isomers low-concentration molecules, approximately 1.6 times more than GC-qMS. The "molecular corridor" assessment shows superior capability identifying an expansive range compounds with higher volatility oxidation states, such as furanoses/pyranoses, di/hydroxy/ketonic acids, di/poly alcohols, aldehydes/ketones, amines/amides. Seasonal variations reflect diverse sources: increased alcohols winter are derived indoor emissions, furanoses/pyranoses heterocyclics spring summer might be biogenic emissions secondary formation, amides autumn probably biomass burning. Integrating partial least squares discriminant analysis (PLS-DA) potential source contribution function (PSCF) models, similarities differences further elucidated, highlighting role local transport southern cities. offers new insights into aided by high resolution sensitivity MS.

Language: Английский

Citations

0
Chemical Fate of Particulate Sulfur from Nighttime Oxidation of Thiophene DOI
Michael Lum, Kunpeng Chen,

B. Ries

et al.

ACS ES&T Air, Journal Year: 2024, Volume and Issue: 1(12), P. 1637 - 1649

Published: Nov. 27, 2024

Sulfur-containing volatile organic compounds emitted during wildfire events, such as dimethyl sulfide, are known to form secondary aerosols containing inorganic sulfate (SO42–) and surfactant-like compounds; however, little is about the fate of sulfur in other reduced organosulfur species. This study aimed determine sulfurous product distribution resulting from nighttime oxidation thiophene a model system. Ion chromatography (IC) aerosol mass spectrometry (a mini spectrometer, mAMS) were used constrain proportions produced under wildfire-relevant conditions ([NO2]/[O3] = 0.1). With constraints IC, results indicated that particle consisted 30.3 ± 6.6% SO42–, while mAMS fractionation attributed 24.5 1.6% total signal 15.4 1.9% organosulfates, 60.1 0.9% sulfonates. Empirical formulas products identified C1–C8 organosulfates sulfonates using complementary techniques. highlights its derivatives source SO42– particulate compounds, which have important implications for atmospheric budget aerosol/droplet physical chemical properties.

Language: Английский

Citations

0
Comment on egusphere-2023-1355 DOI Creative Commons
Abd El Rahman El Mais, Barbara D’Anna, Luka Drinovec

et al.

Published: July 21, 2023

Abstract. Secondary organic aerosols (SOA) formed by oxidation of typical precursors largely emitted biomass burning, such as PAHs and furans, are still poorly characterized in terms formation yields, physical light absorption properties, particularly those generated at night following reaction with nitrate radicals (NO3). In the present study, we evaluated compared effective density (ρeff), Ångström exponent (α), mass coefficient (MAC) laboratory-generated SOA from three furan compounds (furan, 2-methylfuran, 2,5-dimethylfuran) four (naphthalene, acenaphthylene, fluorene, phenanthrene). were an flow reactor between hydroxyl (OH; 0.1–20 equivalent aging days) or NO3 (0.05–6 nights 14 h) single PAH. The ρeff, α, MAC varied depending on precursor oxidant considered. ρeff OH tended to increase particle size before reaching a “plateau”. This was evident for nighttime chemistry experiments (1.2 1.6 average particles > 100 nm). Such results highlighted potential differences chemical composition SOA, well probably their morphology, according size. Three times lower yields obtained OH. PAH (18 76 %) 5 6 higher than furans (3–12 %). While showed low negligible found have significant impact UV-Visible region, implying contribution atmospheric brown carbon (BrC). No values observed processes, due nitrogen-containing chromophores through homogeneous gas phase processes only (without NOx). Overall, this work demonstrated that both, day- substantial aerosol properties so climate.

Language: Английский

Citations

0