Non-linear effects of secondary organic aerosol formation and properties in multi-precursor systems

Nature Communications, Journal Year: 2022, Volume and Issue: 13(1)

Published: Dec. 22, 2022

Abstract Secondary organic aerosol (SOA) contributes significantly to ambient fine particulate matter that affects climate and human health. Monoterpenes represent an important class of biogenic volatile compounds (VOCs) their oxidation by nitrate radicals poses a substantial source SOA globally. Here, we investigate the formation properties from radical two common monoterpenes, α-pinene limonene. When monoterpenes are oxidized simultaneously, observe ~50% enhancement in ~20% reduction limonene formation. The change yields is accompanied pronounced changes chemical composition volatility. These non-linear effects not observed sequential experiment. Our results highlight unlike currently assumed atmospheric models, interaction products formed individual VOCs should be accounted for accurately describe its health impacts.

Language: Английский

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Photooxidation and ozonolysis of α-pinene and limonene mixtures: Mechanisms of secondary organic aerosol formation and cross-dimerization

Journal of Environmental Sciences, Journal Year: 2025, Volume and Issue: unknown

Published: April 1, 2025

Language: Английский

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The importance of burning conditions on the composition of domestic biomass-burning organic aerosol and the impact of atmospheric ageing

Atmospheric chemistry and physics, Journal Year: 2025, Volume and Issue: 25(8), P. 4367 - 4389

Published: April 22, 2025

Abstract. Domestic biomass burning is a significant source of organic aerosol (OA) to the atmosphere; however, understanding OA composition under different conditions and after oxidation largely unknown. Compositional analysis often limited by lack analytical standards available for quantification; semi-quantitative non-target (NTA) can overcome these limitations enabling detection thousands compounds quantification via surrogate standards. A series controlled-burn experiments were conducted at Manchester Aerosol Chamber investigate domestic biomass-burning (BBOA) impact atmospheric ageing. Insights into chemical fresh aged from flaming-dominated smouldering-dominated combustion obtained newly developed NTA approach using ultra-high-performance liquid chromatography high-resolution mass spectrometry. burns contained carbon content, whereas it was primarily black carbon. The detectable both dominated oxygenated (CHO) (≈ 90 %) with smaller contributions organonitrogen species. Primary (POA) had high concentration C8–C17CHO compounds, exhibiting peak between C8–C11. However, POA exhibited greater contribution C13–C17 CHO More than 50 % in determined as aromatic aromaticity index, form functionalised monoaromatic compounds. After ageing, total decreased loss smouldering (−53 flaming (−16 due increased reduction polyaromatic conditions. O:C ratios consistent those (0.57–1.00), suggesting that compositional changes upon ageing driven aromaticity. there probability ≥ 0.8 OA, indicating presence more oxidised This study presents first reported quantitative BBOA retention window scaling demonstrates burn phase may have important consequences exposure such emissions residential settings.

Language: Английский

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Controlled particle coating from β -caryophyllene photo-oxidation: An aerosol dynamics modeling–assisted chamber method

Aerosol Science and Technology, Journal Year: 2025, Volume and Issue: unknown, P. 1 - 14

Published: May 8, 2025

Language: Английский

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Gas-Phase Water-Soluble Organic Carbon: CMAQ Model Evaluation in Baltimore County

ACS Earth and Space Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: May 9, 2025

Language: Английский

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Characteristics, formation, and sources of PM2.5 in 2020 in Suzhou, Yangtze River Delta, China

Environmental Research, Journal Year: 2022, Volume and Issue: 212, P. 113545 - 113545

Published: May 31, 2022

Language: Английский

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Combined application of online FIGAERO-CIMS and offline LC-Orbitrap mass spectrometry (MS) to characterize the chemical composition of secondary organic aerosol (SOA) in smog chamber studies

Atmospheric measurement techniques, Journal Year: 2022, Volume and Issue: 15(14), P. 4385 - 4406

Published: July 29, 2022

Abstract. A combination of online and offline mass spectrometric techniques was used to characterize the chemical composition secondary organic aerosol (SOA) generated from photooxidation α-pinene in an atmospheric simulation chamber. The filter inlet for gases aerosols (FIGAERO) coupled with a high-resolution time-of-flight iodide ionization spectrometer (I−-ToF-CIMS) employed track evolution gaseous particulate components. Extracts particles sampled onto at end each experiment were analysed using ultra-performance liquid chromatography ultra-high-resolution tandem spectrometry (LC-Orbitrap MS). Each technique investigate major SOA elemental group contributions system. CIMS particle-phase measurements show that species containing exclusively carbon, hydrogen, oxygen (CHO group) dominate contribution ion signals products, broadly consistent LC-Orbitrap MS negative mode analysis, which better able identify sulfur-containing fraction. An increased abundance high-carbon-number (nC≥16) compounds additionally nitrogen (CHON detected positive mode, indicating fraction missed by negative-mode measurements. Time series gas-phase oxidation products provided allowed investigation chemistry those hierarchical clustering analysis assess phase partitioning individual molecular compositions. inform selection components targeted structural samples. Saturation concentrations derived nearly simultaneous same ions FIGAERO-CIMS compared estimated structure based on interpret component behaviour. This paper explores insight brought interpretation combined application analytical techniques.

Language: Английский

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On the evolution of sub- and super-saturated water uptake of secondary organic aerosol in chamber experiments from mixed precursors

Atmospheric chemistry and physics, Journal Year: 2022, Volume and Issue: 22(6), P. 4149 - 4166

Published: March 31, 2022

Abstract. To better understand the chemical controls of sub- and super-saturated aerosol water uptake, we designed conducted a series chamber experiments to investigate evolution secondary organic (SOA) particle physicochemical properties during photo-oxidation single mixed biogenic (α-pinene, isoprene) anthropogenic (o-cresol) volatile compounds (VOCs) in presence ammonium sulfate seeds. During 6 h experiments, cloud condensation nuclei (CCN) activity at super-saturation (0.1 %–0.5 %), hygroscopic growth factor 90 % relative humidity (RH), non-refractory PM1 composition were recorded concurrently. Attempts use hygroscopicity parameter κ reconcile uptake ability below above saturation from various VOC precursor systems made, aiming predict CCN sub-saturated hygroscopicity. The thermodynamic model AIOMFAC (aerosol inorganic-organic mixtures functional groups coefficients) was used simulate values compound compare with observation isolate controlling factors different RHs. (in terms both κHTDMA κCCN) mainly controlled by SOA mass fraction, which depended on production rate precursors, played second-order role. For reconciliation κCCN, κHTDMA/κCCN ratio increased fraction this observed all investigated systems, independent initial concentrations sources. mean particles ∼25 lower than κCCN beginning inorganic With increase condensed seed throughout discrepancy became weaker (down ∼0 %) finally ∼60 higher average when approached ∼0.8. As indicated simulations, non-ideality alone cannot fully explain high (0.8). A good agreement between achieved doubling molecular weight or reducing dry size counter. This indicates that evaporation semi-volatile organics counter together could have led discrepancy. result, predicted number distribution ∼10 measurement beginning, further even turned an overestimation ∼20 composition-dependent performances κ-Köhler approach prediction can introduce variable uncertainty predicting droplet numbers influence models still needs be investigated.

Language: Английский

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Interaction between marine and terrestrial biogenic volatile organic compounds: Non-linear effect on secondary organic aerosol formation

Atmospheric Environment, Journal Year: 2024, Volume and Issue: 338, P. 120868 - 120868

Published: Oct. 11, 2024

Language: Английский

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Interaction between marine and terrestrial biogenic volatile organic compounds: Non-linear effect on secondary organic aerosol formation

Published: March 6, 2024

Abstract. Biogenic volatile organic compounds (BVOCs) are the largest source of secondary aerosols (SOA) globally. However, complex interactions between marine and terrestrial BVOCs remain unclear, inhibiting our in-depth understanding SOA formation in coastal areas its environmental impacts. Here, we performed smog chamber experiments with mixed α-pinene (a typical monoterpene) dimethyl sulfide (DMS, a emission BVOC) to investigate their possible subsequent formation. It is found that DMS has non-linear effect on generation: mass concentration yield show an increasing then decreasing trend increase initial DMS. The can be attributed OH regeneration together acid-catalyzed heterogeneous reactions by oxidation DMS, while explained high reactivity inhibits low volatility products. results from infrared spectra reveal contribution sulfur-containing molecules system. Moreover, indicate acidic products generated photooxidation enhance O:C ratio, organosulfates produced contribute SOA. In addition, trends relative abundance highly oxygenated (HOMs) C8-C10 multiple functional groups different systems agree well turning point yield. findings this study have significant implications for binary or more atmosphere areas.

Language: Английский

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