Comment on ar-2023-21 DOI Creative Commons
Melinda K. Schueneman, Douglas A. Day, Dongwook Kim

et al.

Published: Jan. 30, 2024

Abstract. Obtaining quantitative information from real-time soft-ionization aerosol instruments such as an Extractive Electrospray time-of-flight Mass Spectrometer (EESI) can be challenging, due to many individual species having different, and often hard predict, sensitivities. Directly calibrating is time-consuming relevant standards are obtain. In addition, the molecular identities of sampled may ambiguous. Bulk OA sensitivities sometimes used estimate sensitivities, but different types have bulk that vary by a factor ~10. A system separate compounds present in complex samples enable their direct calibration. Here, high performance liquid chromatography (HPLC) followed formation via atomization was combined with online, 1 Hz measurements calibrate EESI High Resolution Aerosol (AMS) for secondary organic (SOA) mixture. Pure were test method characterize its uncertainties. compound calibration factors consistent within ±20 % vs. HPLC separation, which far superior orders magnitude sensitivity differences possible EESI. For not well separated chromatography, Positive Matrix Factorization (PMF) based on AMS spectra ability overlapping species. two cases, further separation achieved using PMF, derived calibrations varied up 2.

Language: Английский

Rapid night-time nanoparticle growth in Delhi driven by biomass-burning emissions DOI
Suneeti Mishra, S. N. Tripathi, Vijay P. Kanawade

et al.

Nature Geoscience, Journal Year: 2023, Volume and Issue: 16(3), P. 224 - 230

Published: March 1, 2023

Language: Английский

Citations

30
Elucidating Secondary Organic Aerosol Processes through High-Resolution Aerosol Mass Spectrometry in Beijing DOI

Weiqi Xu,

Chun Chen, Zhijie Li

et al.

Advances in Atmospheric Sciences, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 24, 2025

Language: Английский

Citations

1
Time-Resolved Molecular Characterization of Secondary Organic Aerosol Formed from OH and NO3Radical Initiated Oxidation of a Mixture of Aromatic Precursors DOI Creative Commons
Varun Kumar, Jay G. Slowik, Urs Baltensperger

et al.

Environmental Science & Technology, Journal Year: 2023, Volume and Issue: 57(31), P. 11572 - 11582

Published: July 27, 2023

Aromatic hydrocarbons (ArHCs) and oxygenated aromatic (ArHC–OHs) are emitted from a variety of anthropogenic activities important precursors secondary organic aerosol (SOA) in urban areas. Here, we analyzed compared the composition SOA formed oxidation mixture VOCs by OH NO3 radicals. The VOC was composed toluene (C7H8), p-xylene + ethylbenzene (C8H10), 1,3,5-trimethylbenzene (C9H12), phenol (C6H6O), cresol (C7H8O), 2,6-dimethylphenol (C8H10O), 2,4,6-trimethylphenol (C9H12O) proportion where were chosen to approximate day-time traffic-related emissions Delhi, alcohols make up 20% mixture. These prominent other cities as well, including those influenced biomass combustion. In experiments, large contributions CxHyOzN dimers (C15–C18) observed, corresponding fast formation within 15–20 min after start chemistry. Additionally, different combinations initial VOCs, highlighting importance exploring SOAs mixed systems. contrast, experiments with radicals yielded gradual mass formation, CxHyOz monomers (C6–C9) being dominant constituents. evolution time tracked degradation observed concurrent monomer species. rates dimer decomposition ∼2–3 times higher previously determined for α-pinene O3 SOA, dependence particle-phase reactions on oxidants. produced did not dramatically change over same frame. No measurable effects humidity SOA.

Language: Английский

Citations

11
Temporal Dynamics and Source Characteristics of Fine Particulate Matter using Positive Matrix Factorization (PMF) DOI
Vikas Kumar, Manoranjan Sahu, Basudev Biswal

et al.

Atmospheric Pollution Research, Journal Year: 2025, Volume and Issue: unknown, P. 102539 - 102539

Published: April 1, 2025

Language: Английский

Citations

0
Exploring the chemical composition and processes of submicron aerosols in Delhi using aerosol chemical speciation monitor driven factor analysis DOI Creative Commons
Upasana Panda,

Supriya Dey,

Amit Sharma

et al.

Scientific Reports, Journal Year: 2025, Volume and Issue: 15(1)

Published: April 24, 2025

Abstract Wintertime non-refractory submicron particulate matter (NR-PM 1 ) species were measured in Delhi with an Aerodyne Aerosol Chemical Speciation Monitor (ACSM) during February–March 2018. The average NR-PM mass concentration throughout the study was 58.0 ± 42.6 µg m −3 , where contribution of organic aerosol (OA) 69% total . In Delhi, chloride (10%) main inorganic contributor, followed by ammonium (8%), sulfate (7%), and nitrate (6%), contrasting prevalence most urban environments. Source apportionment analysis OA identified five major factors, including three primary contributors: hydrocarbon-like (HOA), biomass burning (BBOA), cooking-related (COA) two secondary oxygenated (OPOA), more-oxidized (MO-OOA). A 19% rise OPOA observed high episodes, suggesting potential role atmospheric chemical transformation OA. Traffic emissions significantly contribute to ambient OA, accounting for at least 41% mass. Furthermore, exhibited low oxidation levels regardless its source. f 44 : 43 revealed slower oxidization compared other locations worldwide. Further investigations, chamber experiments tailored atmosphere, are necessary elucidate oxidants genesis alongside emissions.

Language: Английский

Citations

0
Optical source apportionment of aqueous brown carbon (BrC) on a daytime and nighttime basis in the eastern Indo-Gangetic Plain (IGP) and insights from 13C and 15N isotopic signatures DOI Creative Commons

Supriya Dey,

Pronoy Ghosh,

Prashant Rawat

et al.

The Science of The Total Environment, Journal Year: 2023, Volume and Issue: 894, P. 164872 - 164872

Published: June 19, 2023

Language: Английский

Citations

9
Organic aerosol sources in the Milan metropolitan area – Receptor modelling based on field observations and air quality modelling DOI Creative Commons

Kaspar R. Daellenbach,

Manousos Ioannis Manousakas, Jianhui Jiang

et al.

Atmospheric Environment, Journal Year: 2023, Volume and Issue: 307, P. 119799 - 119799

Published: May 15, 2023

The Milan metropolitan area in Northern Italy experiences historically severe particulate matter pollution episodes characterized by high organic aerosol (OA) concentrations. However, the main sources of OA, especially atmospherically formed secondary OA (SOA) are not well understood. Here, we investigated emission contributing to directly emitted (Primary – POA) and SOA urban Milan, where such information is particularly lacking. We used advanced mass spectrometric analytical techniques for characterization archive samples, as statistical receptor modeling (positive matrix factorization, PMF) air quality modeling, establish a base case investigating time evolution source contributions. found that residential heating biomass burning POA (BBOA) were major detrimental factor during winter (37% under polluted conditions up 56% OA). Inefficient combustion identified BBOA/K+ ratios contributed relative contribution BBOA OA. Long-term tracer analyses suggest concentrations remained approximately constant over last decade (2012–2022), supporting conclusion emissions from driver winter-time pollution. Yet assessing changes other require future research. While most important contributor (62% OA), dominated summer Our combined spectral apportionment modelling indicated mostly affected related precursor emissions, while summer-time linked both remaining anthropogenic (industry, energy production, shipping, traffic) biogenic emissions. Altogether, this study quantified thus provides crucial about baseline comparison present situation which needed tackling one hotspots Europe. Overall, presents transferable framework combining chemical with bottom-up order better understand formation SOA.

Language: Английский

Citations

8
A 1-year aerosol chemical speciation monitor (ACSM) source analysis of organic aerosol particle contributions from anthropogenic sources after long-range transport at the TROPOS research station Melpitz DOI Creative Commons
Samira Atabakhsh, Laurent Poulain, Gang Chen

et al.

Atmospheric chemistry and physics, Journal Year: 2023, Volume and Issue: 23(12), P. 6963 - 6988

Published: June 23, 2023

Abstract. Atmospheric aerosol particles are a complex combination of primary emitted sources (biogenic and anthropogenic) secondary resulting from aging processes such as condensation, coagulation, cloud processing. To better understand their sources, investigations have been focused on urban areas in the past, whereas rural-background stations normally less impacted by surrounding anthropogenic sources. Therefore, they predisposed for studying impact long-range transport aerosols. Here, chemical composition organic (OA) submicron measured an speciation monitor (ACSM) multi-angle absorption photometer (MAAP) were investigated at Melpitz September 2016 to August 2017. The location station frontier between western eastern Europe makes it ideal place investigate over Europe. Indeed, is under influence polluted air masses westerly directions more continental OA dominated particle mass concentration showed strong seasonal variability ranging 39 % (in winter) 58 summer). It was followed sulfate (15 20 %) nitrate (24 11 %). source identification performed using rolling positive matrix factorization (PMF) approach account potential temporal changes profile. possible split into five factors with distinct spectral signature. Three associated (POA) sources: hydrocarbon-like (HOA; 5.2 winter 6.8 summer), biomass burning (BBOA; 10.6 6.1 coal combustion (CCOA; 23 8.7 Another two processed oxygenated (OOA) oxidized OOA (LO-OOA; 28.4 36.7 (MO-OOA; 32.8 41.8 Since equivalent black carbon (eBC) clearly identified POA (sum HOA, BBOA, CCOA; R2= 0. 87), eBC's contribution each achieved multilinear regression model. Consequently, CCOA represented main carbonaceous eBC) not only during (56 but also summer (13 BBOA (29 69 summer, respectively) HOA 18 respectively). A cluster analysis used geographical origins different types that both time, PM1 (PM aerodynamic diameter smaller than 1 µm) always highest fraction. wintertime domestic heating power plant emissions, emphasizes critical importance emissions aerosols its quality, through transportation.

Language: Английский

Citations

8
Quantification of primary and secondary organic aerosol sources by combined factor analysis of extractive electrospray ionisation and aerosol mass spectrometer measurements (EESI-TOF and AMS) DOI Creative Commons
Yandong Tong, Lu Qi, Giulia Stefenelli

et al.

Atmospheric measurement techniques, Journal Year: 2022, Volume and Issue: 15(24), P. 7265 - 7291

Published: Dec. 20, 2022

Abstract. Source apportionment studies have struggled to quantitatively link secondary organic aerosols (SOAs) their precursor sources due largely instrument limitations. For example, aerosol mass spectrometer (AMS) provides quantitative measurements of the total SOA fraction but lacks chemical resolution resolve most sources. In contrast, instruments based on soft ionisation techniques, such as extractive electrospray spectrometry (EESI, e.g. EESI time-of-flight spectrometer, EESI-TOF), demonstrated identify specific provide only a semi-quantitative uncertainties in dependence sensitivity molecular identity. We address this challenge by presenting method for positive matrix factorisation (PMF) analysis single dataset which includes from both AMS and EESI-TOF instruments, denoted “combined PMF” (cPMF). Because each factor profile components, cPMF maintains source capability while also providing concentrations. Therefore, bulk can be directly determined analysis. present metrics ensuring that are well represented solution, optionally constraining profiles factors detectable one or protocol uncertainty As proof concept, was applied summer winter Zurich, Switzerland. Factors related biogenic wood-burning-derived SOAs quantified, POA wood burning, cigarette smoke, cooking, traffic. The retrieved factor-dependent sensitivities consistent with laboratory model precursors parameterisations ion formulae. shows that, standalone PMF, not accounted for, some significantly under- overestimated. when considered dataset, is underestimated ∼25 % high components primary biomass burning levoglucosan. where OA dominated monoterpene oxidation products, uncorrected underestimates daytime relative nighttime (in organonitrates less oxygenated CxHyOz molecules enhanced). Although here an pairing, suitable general case multi-instrument thereby framework exploiting semi-quantitative, high-resolution instrumentation apportionment.

Language: Английский

Citations

14
New Insights Into the Sources of Atmospheric Organic Aerosols in East China: A Comparison of Online Molecule‐Level and Bulk Measurements DOI
Dafeng Ge, Wei Nie, Yuliang Liu

et al.

Journal of Geophysical Research Atmospheres, Journal Year: 2024, Volume and Issue: 129(16)

Published: Aug. 26, 2024

Abstract Organic aerosols (OA) significantly contribute to haze pollution, threaten human health, and affect the radiation balance. However, real‐time tracking of OA evolution at molecular level is limited, hindering a comprehensive understanding their origins behaviors. In this study, we investigated wintertime in megacity East China by combining simultaneous measurements from an extractive electrospray ionization time‐of‐flight mass spectrometer (EESI‐TOF) high‐resolution aerosol (AMS) (HR‐TOF‐AMS). AMS results indicate that accounts for about 27% non‐refractory submicron particulate matter (NR‐PM 1 ) on average. EESI‐TOF data reveal C x H y O z N 1–2 are predominant components, contributing over 70% 20%, respectively. Factorization analysis shows while traffic, cooking, biomass burning major primary sources, most (>70% EESI‐TOF, >55% AMS) originate secondary production. although missing hydrocarbon‐like OA, excels providing information oxygenated identifying aromatics aliphatics as possible key precursors. It further differentiates less oxidized organic (SOA) into two factors with distinct compositions, likely due diverse source regions. Importantly, identifies additional factors: one possibly related plasticizers another representing SOA formation monoterpene oxidation NO 3 radicals. conclusion, complements offering valuable insights chemical processes underlying formation, especially complex urban environments.

Language: Английский

Citations

2