NO at low concentration can enhance the formation of highly oxygenated biogenic molecules in the atmosphere

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: June 8, 2023

The interaction between nitrogen monoxide (NO) and organic peroxy radicals (RO2) greatly impacts the formation of highly oxygenated molecules (HOM), key precursors secondary aerosols. It has been thought that HOM production can be significantly suppressed by NO even at low concentrations. Here, we perform dedicated experiments focusing on from monoterpenes concentrations (0 - 82 pptv). We demonstrate such enhance modulating RO2 loss favoring alkoxy continue to autoxidize through isomerization. These insights suggest yields typical boreal forest emissions vary 2.5%-6.5%, will not completely inhibited high Our findings challenge notion monotonically reduces extending knowledge RO2-NO interactions low-NO regime. This represents a major advance towards an accurate assessment budgets, especially in environments, which prevails pre-industrial atmosphere, pristine areas, upper boundary layer.

Language: Английский

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Aqueous-Phase Reactions of Anthropogenic Emissions Lead to the High Chemodiversity of Atmospheric Nitrogen-Containing Compounds during the Haze Event

Environmental Science & Technology, Journal Year: 2023, Volume and Issue: 57(43), P. 16500 - 16511

Published: Oct. 16, 2023

Nitrogen-containing organic compounds (NOCs), a type of important reactive-nitrogen species, are abundant in aerosols haze events observed Northern China. However, due to the complex nature NOCs, sources, formation, and influencing factors still ambiguous. Here, molecular composition matters (OMs) hourly PM2.5 samples collected during event China was characterized using Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS). We found that CHON (formulas containing C, H, O, N atoms) dominated OM fractions showed high chemodiversity transformability. Relying on newly developed revised-workflow oxidation-hydrolyzation knowledge for compounds, 64% major aromatic (>80%) could be derived from oxidization or hydrolyzation processes. Results FT-ICR MS data analysis further aerosol liquid water (ALW)-involved aqueous-phase reactions distribution aromatic-CHON besides coal combustion, ALW-involved compound formation daytime nighttime different. Our results improve understanding composition, potential which can help advance evolution, control haze.

Language: Английский

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Aerosol high water contents favor sulfate and secondary organic aerosol formation from fossil fuel combustion emissions

npj Climate and Atmospheric Science, Journal Year: 2023, Volume and Issue: 6(1)

Published: Oct. 27, 2023

Abstract Fine-particle pollution associated with high sulfate and secondary organic aerosol (SOA) contents still occurs in winter, despite considerable reductions precursor emissions China. The chemical mechanisms involved are consistently acknowledged to be linked water but remain poorly understood. Here, we present findings demonstrating that the synergistic effect of elevated content particles originating from fossil fuel combustion significantly enhanced rapid formation SOAs under humidity conditions during winter northern presence promoted aging process containing elemental carbon (EC) facilitated SOAs. Evidence single reveals an increased potential for SOA primary aerosols (POAs) combustion, increasing water. Under relative exceeding 85%, multiphase oxidation SO 2 by in-particle nitrite/nitrous acid, generated through reactions involving aged EC-containing iron-rich particles, as well aqueous-phase hydroxymethanesulfonate (HMS), led a substantial increase production. This study emphasizes critical role chemistry concerning SOAs, highlighting urgent necessity mitigate combustion.

Language: Английский

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Investigation on the budget of peroxyacetyl nitrate (PAN) in the Yangtze River Delta: Unravelling local photochemistry and regional impact

The Science of The Total Environment, Journal Year: 2024, Volume and Issue: 917, P. 170373 - 170373

Published: Jan. 27, 2024

Language: Английский

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Road Traffic Emissions Lead to Much Enhanced New Particle Formation through Increased Growth Rates

Environmental Science & Technology, Journal Year: 2024, Volume and Issue: 58(24), P. 10664 - 10674

Published: June 8, 2024

New particle formation (NPF) is a major source of atmospheric aerosol particles, including cloud condensation nuclei (CCN), by number globally. Previous research has highlighted that NPF less frequent but more intense at roadsides compared to urban background. Here, we closely examine both background and roadside sites in Central Europe. We show the concentration oxygenated organic molecules (OOMs) greater roadside, OOMs along with sulfuric acid onto new particles sufficient explain growth sites. identify hitherto unreported traffic-related OOM contributing 29% 16% total background, respectively. Critically, this undiscovered an essential component NPF. Without their contribution rates subsequent enhancements survival, >50 nm produced would be reduced factor 21 site. Reductions hydrocarbon emissions from road traffic may thereby reduce numbers CCN counts.

Language: Английский

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The GFDL Variable‐Resolution Global Chemistry‐Climate Model for Research at the Nexus of US Climate and Air Quality Extremes

Journal of Advances in Modeling Earth Systems, Journal Year: 2024, Volume and Issue: 16(4)

Published: April 1, 2024

Abstract We present a variable‐resolution global chemistry‐climate model (AM4VR) developed at NOAA's Geophysical Fluid Dynamics Laboratory (GFDL) for research the nexus of US climate and air quality extremes. AM4VR has horizontal resolution 13 km over US, allowing it to resolve urban‐to‐rural chemical regimes, mesoscale convective systems, land‐surface heterogeneity. With gradually reducing 100 Indian Ocean, we achieve multi‐decadal simulations driven by observed sea surface temperatures 50% computational cost 25‐km uniform‐resolution grid. In contrast with GFDL's AM4.1 contributing sixth Coupled Model Intercomparison Project resolution, features much improved mean patterns variability. particular, shows representation of: precipitation seasonal‐to‐diurnal cycles extremes, notably central dry‐and‐warm bias; western snowpack summer drought, implications wildfires; North American monsoon, affecting dust storms. exhibits excellent winter precipitation, pollution meteorology in California complex terrain, enabling skillful prediction both extreme ozone haze events Central Valley. also provides vast improvements process‐level representations biogenic volatile organic compound emissions, interactive emissions from land, removal pollutants terrestrial ecosystems. highlight value increased representing climate–air interactions through land‐biosphere feedbacks. offers novel opportunity study dimensions quality, especially role Earth system feedbacks changing climate.

Language: Английский

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Identification of highly oxygenated organic molecules and their role in aerosol formation in the reaction of limonene with nitrate radical

Atmospheric chemistry and physics, Journal Year: 2022, Volume and Issue: 22(17), P. 11323 - 11346

Published: Sept. 2, 2022

Abstract. Nighttime NO3-initiated oxidation of biogenic volatile organic compounds (BVOCs) such as monoterpenes is important for the atmospheric formation and growth secondary aerosol (SOA), which has significant impact on climate, air quality, human health. In SOA growth, highly oxygenated molecules (HOM) may be crucial, but their pathways role in have yet to clarified. Among monoterpenes, limonene particular interest its high emission globally yield. this work, HOM reaction with nitrate radical (NO3) was investigated SAPHIR chamber (Simulation Atmospheric PHotochemistry a large Reaction chamber). About 280 products were identified, grouped into 19 monomer families, 11 dimer 3 trimer families. Both closed-shell open-shell peroxy radicals (RO2⚫) observed, many them not been reported previously. Monomers dimers accounted 47 % concentrations, respectively, trimers making up remaining 6 %. most abundant C10H15−17NO6−14, carbonyl outnumbered hydroxyl products, indicating importance RO2⚫ termination by unimolecular dissociation. autoxidation alkoxy–peroxy found processes leading HOM. Time-dependent concentration profiles containing nitrogen showed mainly second-generation patterns. Dimers likely formed via accretion two RO2⚫, HOM-trimers between RO2⚫. Trimers are suggested play an new particle (NPF) observed our experiment. A yield 1.5%-0.7%+1.7% estimated considering only first-generation products. mass could reasonably explained condensation particles assuming irreversible uptake ultra-low volatility (ULVOCs), extremely low (ELVOCs), (LVOCs). This work provides evidence +NO3 NPF particles.

Language: Английский

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Seasonal characteristics and provenance of organic aerosols in the urban atmosphere of Liaocheng in the North China Plain: Significant effect of biomass burning

Particuology, Journal Year: 2022, Volume and Issue: 75, P. 185 - 198

Published: Aug. 7, 2022

Language: Английский

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Aqueous‐Phase Secondary Processes and Meteorological Change Promote the Brown Carbon Formation and Transformation During Haze Events

Journal of Geophysical Research Atmospheres, Journal Year: 2023, Volume and Issue: 128(16)

Published: Aug. 20, 2023

Abstract The evolution and the impacts of meteorological conditions on brown carbon (BrC) absorption are not understood, which hinders assessment BrC radiative forcing. To address this issue, 1‐hr time‐resolved PM 2.5 samples collected during three haze events in North China Plain prior to COVID‐19 pandemic were used measure optical properties BrC. By coupling excitation‐emission matrix spectroscopy, chemical tracer analysis with multiple model including positive factorization (PMF) a deweather‐random forest model, we found that higher proportion highly oxidized chromophoric components was present water‐soluble than methanol‐soluble BrC, indicating conversion low‐oxidized water‐insoluble into day. results PMF showed aqueous secondary processes major contributor (68% ± 38%), changes such as relative humidity (RH) could significantly lead light‐absorbing capacity especially enhancement for bleaching noon afternoon. We further increased RH increases maximum ∼65%, then decreased when >65%, highlighting important role generation

Language: Английский

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Impact of biogenic secondary organic aerosol (SOA) loading on the molecular composition of wintertime PM_2.5 in urban Tianjin: an insight from Fourier transform ion cyclotron resonance mass spectrometry

Atmospheric chemistry and physics, Journal Year: 2023, Volume and Issue: 23(3), P. 2061 - 2077

Published: Feb. 9, 2023

Abstract. Biomass burning is one of the key sources urban aerosols in North China Plain, especially during winter, when impact secondary organic (SOAs) formed from biogenic volatile compounds (BVOCs) generally considered to be minor. However, little known about influence SOA loading on molecular composition wintertime aerosols. Here, we investigated water-soluble fine particulate matter (PM2.5) Tianjin by ultrahigh-resolution Fourier transform ion cyclotron resonanc mass spectrometry (FT-ICR MS). Our results show that most CHO and CHON are derived biomass which poor oxygen contain aromatic rings probably contribute light-absorbing brown carbon (BrC) chromophores. Under moderate high SOA-loading conditions, nocturnal chemistry more efficient than photooxidation generate with content. low loading, content mainly photochemistry. Secondary oxidation monoterpenes. may productive sesquiterpene-derived compounds. In contrast, number- intensity-weight S-containing groups (CHOS CHONS) increased significantly increase agrees fact a majority identified as organosulfates (OSs) nitrooxy–organosulfates (nitrooxy–OSs) BVOCs. Terpenes potential major contributors nitrooxy–organosulfates. While beneficial formation under loading. The an important factor associated degree, nitrate group chemodiversity nitrooxy-organosulfates. Furthermore, our study suggests hydrolysis nitrooxy-organosulfates possible pathway for organosulfates.

Language: Английский

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