Chemical composition of secondary organic aerosol particles formed from mixtures of anthropogenic and biogenic precursors DOI Creative Commons
Yunqi Shao, Aristeidis Voliotis, Mao Du

et al.

Atmospheric chemistry and physics, Journal Year: 2022, Volume and Issue: 22(15), P. 9799 - 9826

Published: Aug. 2, 2022

Abstract. A series of experiments was designed and conducted in the Manchester Aerosol Chamber (MAC) to study photo-oxidation single mixed biogenic (isoprene α-pinene) anthropogenic (o-cresol) precursors presence NOx ammonium sulfate seed particles. Several online techniques (HR-ToF-AMS, semi-continuous GC-MS, O3 analyser) were coupled MAC monitor gas particle mass concentrations. Secondary organic aerosol (SOA) particles collected onto a quartz-fibre filter at end each experiment analysed using liquid chromatography–ultrahigh-resolution spectrometry (LC-Orbitrap MS). The SOA chemical composition precursor systems investigated non-targeted accurate analysis measurements both negative positive ionization modes, significantly reducing data complexity time, thereby providing more complete assessment composition. This is not widely used environmental science has never been previously atmospheric simulation chamber studies. Products from α-pinene found dominate binary α-pinene–isoprene system terms signal contributed number components detected. Isoprene generate negligible under experimental conditions, isoprene-derived products made contribution system. No compounds uniquely this sufficiently be reliably considered tracer compound for mixture. Methyl-nitrocatechol isomers (C7H7NO4) methyl-nitrophenol (C7H7NO3) o-cresol oxidation dominant contributions o-cresol–isoprene o-cresol–α-pinene mode. In contrast, interactions mechanisms led formation o-cresol-containing C9H11NO C8H8O10 large molecular mode mainly driven by high-molecular-weight (e.g. C20H31NO4 C20H30O3) formed ternary complex. abundance are markedly similar those mode, with major

Language: Английский

NO at low concentration can enhance the formation of highly oxygenated biogenic molecules in the atmosphere DOI Creative Commons
Wei Nie, Chao Yan, Liwen Yang

et al.

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

Citations

22
Aqueous-Phase Reactions of Anthropogenic Emissions Lead to the High Chemodiversity of Atmospheric Nitrogen-Containing Compounds during the Haze Event DOI
Hongxing Jiang, Junjie Cai, Xinxin Feng

et al.

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

Citations

20
Characterization of organic vapors by a Vocus proton-transfer-reaction mass spectrometry at a mountain site in southeastern China DOI
Yi Zhang,

Weiqi Xu,

Wei Zhou

et al.

The Science of The Total Environment, Journal Year: 2024, Volume and Issue: 919, P. 170633 - 170633

Published: Feb. 9, 2024

Language: Английский

Citations

6
Toward Building a Physical Proxy for Gas-Phase Sulfuric Acid Concentration Based on Its Budget Analysis in Polluted Yangtze River Delta, East China DOI Creative Commons
Liwen Yang, Wei Nie, Yuliang Liu

et al.

Environmental Science & Technology, Journal Year: 2021, Volume and Issue: 55(10), P. 6665 - 6676

Published: May 7, 2021

Gaseous sulfuric acid (H2SO4) is a crucial precursor for secondary aerosol formation, particularly new particle formation (NPF) that plays an essential role in the global number budget of particles and cloud condensation nuclei. Due to technology challenges, global-wide long-term measurements gaseous H2SO4 are currently very challenging. Empirical proxies have been derived mainly based on short-term intensive campaigns. In this work, we performed comprehensive related parameters polluted Yangtze River Delta East China during four seasons developed physical proxy analysis H2SO4. Besides photo-oxidation SO2, found primary emissions can contribute considerably, at night. Dry deposition has potential be non-negligible sink, addition onto surfaces. Compared with empirical proxies, newly demonstrates extraordinary stability all widely used improve understanding NPF fundamentally.

Language: Английский

Citations

34
Field Detection of Highly Oxygenated Organic Molecules in Shanghai by Chemical Ionization–Orbitrap DOI
Yanjun Zhang, Dandan Li,

Yingge Ma

et al.

Environmental Science & Technology, Journal Year: 2022, Volume and Issue: 56(12), P. 7608 - 7617

Published: May 20, 2022

Secondary organic aerosol, formed through atmospheric oxidation processes, plays an important role in affecting climate and human health. In this study, we conducted a comprehensive campaign the megacity of Shanghai during 2019 International Import Expo (EXPO), with first deployment chemical ionization─Orbitrap mass spectrometer for ambient measurements. With ultrahigh resolving power Orbitrap analyzer (up to 140,000 Th/Th) capability dealing massive spectral data sets by positive matrix factorization, were able identify major gas-phase processes leading formation oxygenated molecules (OOM) Shanghai. Nine main factors from three independent sub-range analysis identified. More than 90% OOM are anthropogenic origin >60% nitrogen-containing molecules, mainly dominated RO2 + NO and/or NO3 chemistry. The emission control EXPO showed that even though restriction was effectual significantly lowering primary pollutants (20–70% decrease), secondary products responded less effectively (14% or increased (50 >200%) due enhancement ozone lowered condensation sink, indicating importance stricter multi-pollutant coordinated strategy pollution mitigation.

Language: Английский

Citations

26
Large Daytime Molecular Chlorine Missing Source at a Suburban Site in East China DOI
Qianjie Chen, Men Xia, Xiang Peng

et al.

Journal of Geophysical Research Atmospheres, Journal Year: 2022, Volume and Issue: 127(4)

Published: Jan. 29, 2022

Abstract Molecular chlorine (Cl 2 ) affects atmospheric oxidative capacity by generating radicals upon photolysis, but it is poorly simulated in chemistry models. In this study, we observed up to 40 ppt Cl around noon at a suburban site East China, and used box model with up‐to‐date comprehensive observational constraints investigate formation mechanisms. The standard run traditional mechanisms underestimates the almost one order of magnitude noon. daytime missing source was estimated, accounting for on average (69 ± 5)% production 1‐week study period. It likely caused photochemistry within aerosols, based its correlation environmental factors, such as sunlight intensity aerosol abundances. With implemented into model, radical abundance increases factor 4 afternoon, enhancing oxidation volatile organic compounds. A good understanding critical while assessing impacts air quality climate.

Language: Английский

Citations

21
Weather History-based Parameterization of the G-93 Isoprene Emission Formula for the Tropical Plant Ficus septica DOI
Ishmael Mutanda,

Masashi Inafuku,

Hirosuke Oku

et al.

Atmospheric Environment, Journal Year: 2025, Volume and Issue: unknown, P. 121102 - 121102

Published: Feb. 1, 2025

Language: Английский

Citations

0
Reply on RC1 DOI Creative Commons
Wenxin Zhang

Published: Jan. 8, 2025

Abstract. Organic aerosol (OA) is a major type of fine particulate matter. OA shows large variability influenced by anthropogenic emissions, vegetation, and meteorological changes. Understanding trends crucial for air quality climate studies, yet changes in over time China are poorly documented. This study applied the Community Atmosphere Model version 6 with comprehensive tropospheric stratospheric chemistry (CAM6-Chem) to investigate long-term from 1990 2019 identify driving factors. The simulations agreed well ground-based measurements 151 observational sites CAQRA reanalysis dataset. Although showed modest 5.6 % increase, this resulted significant -8.1 decrease primary organic aerosols (POA) substantial 32.3 increase secondary (SOA). Anthropogenic emissions POA volatile compounds (VOCs) were dominant contributors these trends. While biogenic VOCs (BVOCs) played role SOA formation, observed specific sub-species: isoprene-derived decreased -18.8 due sulfate reduction, while monoterpene-derived increased 12.3 driven enhanced rising temperatures. Our found through sensitivity experiments negligible response nitrogen oxides (NOx) as net effect multiple pathways. highlights complex interplay between reduction growth, revealing notable varying roles both emissions.

Language: Английский

Citations

0
Gaseous Sulfuric Acid Contributions to Sulfate Formation in Urban Atmosphere DOI
Zhenning Wang, Wei Nie, Yuliang Liu

et al.

Environmental Science & Technology Letters, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 9, 2025

Sulfate aerosols are critical atmospheric constituents, influencing air quality and climate. Their complex formation processes have been studied predominantly in the context of multiphase chemistry. However, substantial contribution gas-phase condensation sulfuric acid (SAcond) to sulfate aerosol has not fully recognized, primarily due challenges associated with long-term measurement gaseous (H2SO4). Using comprehensive data set from SORPES station, we elucidated influence H2SO4 on generation across different meteorological pollution contexts. Our analysis indicates a marked increase concentrations enhances its role formation, cumulative five-day production accounting for up 50% total levels. Detailed stable conditions revealed that SAcond initially increases then stabilizes higher levels PM2.5, while relative diminishes. This implies high-polluted environments, reactions drive formation. Given ongoing efforts reduce PM2.5 China, shaping profiles is anticipated become increasingly significant. underscores need renewed focus within broader

Language: Английский

Citations

0
Understanding the long-term trend of organic aerosol and the influences from anthropogenic emission and regional climate change in China DOI Creative Commons
Wenxin Zhang, Yaman Liu, Man Yue

et al.

Atmospheric chemistry and physics, Journal Year: 2025, Volume and Issue: 25(7), P. 3857 - 3872

Published: April 3, 2025

Abstract. Organic aerosol (OA) is a major type of fine particulate matter. OA shows large variability influenced by anthropogenic emissions, vegetation, and meteorological changes. Understanding trends crucial for air quality climate studies, yet changes in over time China are poorly documented. This study applied the Community Atmosphere Model version 6 with comprehensive tropospheric stratospheric chemistry (CAM6-Chem) to investigate long-term from 1990 2019 identify driving factors. The simulations agreed well ground-based measurements 151 observational sites CAQRA reanalysis dataset. Although showed modest 5.6 % increase, this resulted significant −8.1 decrease primary organic aerosols (POAs) substantial 32.3 increase secondary (SOAs). Anthropogenic emissions POA volatile compounds (VOCs) were dominant contributors these trends. While biogenic VOCs (BVOCs) played role SOA formation, observed specific subspecies: isoprene-derived decreased −18.8 due sulfate reduction, while monoterpene-derived increased 12.3 driven enhanced rising temperatures. Through sensitivity experiments, our found negligible response nitrogen oxide (NOx) as net effect multiple pathways. highlights complex interplay between reduction growth, revealing notable varying roles both emissions.

Language: Английский

Citations

0