Online Characterization of Organic Aerosol by Condensational Growth into Aqueous Droplets Coupled with Droplet-Assisted Ionization

2021 ◽  
Vol 93 (5) ◽  
pp. 2793-2801
Author(s):  
Devan E. Kerecman ◽  
Michael J. Apsokardu ◽  
Savannah L. Talledo ◽  
Michael S. Taylor ◽  
Devon N. Haugh ◽  
...  
Author(s):  
Weiqi Xu ◽  
Chun Chen ◽  
Yanmei Qiu ◽  
Conghui Xie ◽  
Yunle Chen ◽  
...  

Organic aerosol (OA), a large fraction of fine particles, has a large impact on climate radiative forcing and human health, and the impact depends strongly on size distributions. Here we...


2014 ◽  
Vol 48 (21) ◽  
pp. 12671-12678 ◽  
Author(s):  
Mohammad Safi Shalamzari ◽  
Ariane Kahnt ◽  
Reinhilde Vermeylen ◽  
Tadeusz E. Kleindienst ◽  
Michael Lewandowski ◽  
...  

2021 ◽  
Author(s):  
Anna K. Tobler ◽  
Alicja Skiba ◽  
Francesco Canonaco ◽  
Griša Močnik ◽  
Pragati Rai ◽  
...  

2021 ◽  
Vol 21 (10) ◽  
pp. 8067-8088
Author(s):  
Vincent Michoud ◽  
Elise Hallemans ◽  
Laura Chiappini ◽  
Eva Leoz-Garziandia ◽  
Aurélie Colomb ◽  
...  

Abstract. The characterization of the molecular composition of organic carbon in both gaseous and aerosol is key to understanding the processes involved in the formation and aging of secondary organic aerosol. Therefore a technique using active sampling on cartridges and filters and derivatization followed by analysis using a thermal desorption–gas chromatography–mass spectrometer (TD–GC–MS) has been used. It is aimed at studying the molecular composition of organic carbon in both gaseous and aerosol phases (PM2.5) during an intensive field campaign which took place in Corsica (France) during the summer of 2013: the ChArMEx (Chemistry and Aerosol Mediterranean Experiment) SOP1b (Special Observation Period 1B) campaign. These measurements led to the identification of 51 oxygenated (carbonyl and or hydroxyl) compounds in the gaseous phase with concentrations between 21 and 3900 ng m−3 and of 85 compounds in the particulate phase with concentrations between 0.3 and 277 ng m−3. Comparisons of these measurements with collocated data using other techniques have been conducted, showing fair agreement in general for most species except for glyoxal in the gas phase and malonic, tartaric, malic and succinic acids in the particle phase, with disagreements that can reach up to a factor of 8 and 20 on average, respectively, for the latter two acids. Comparison between the sum of all compounds identified by TD–GC–MS in the particle phase and the total organic matter (OM) mass reveals that on average 18 % of the total OM mass can be explained by the compounds measured by TD–GC–MS. This number increases to 24 % of the total water-soluble OM (WSOM) measured by coupling the Particle Into Liquid Sampler (PILS)-TOC (total organic carbon) if we consider only the sum of the soluble compounds measured by TD–GC–MS. This highlights the important fraction of the OM mass identified by these measurements but also the relative important fraction of OM mass remaining unidentified during the campaign and therefore the complexity of characterizing exhaustively the organic aerosol (OA) molecular chemical composition. The fraction of OM measured by TD–GC–MS is largely dominated by di-carboxylic acids, which represent 49 % of the PM2.5 content detected and quantified by this technique. Other contributions to PM2.5 composition measured by TD–GC–MS are then represented by tri-carboxylic acids (15 %), alcohols (13 %), aldehydes (10 %), di-hydroxy-carboxylic acids (5 %), monocarboxylic acids and ketones (3 % each), and hydroxyl-carboxylic acids (2 %). These results highlight the importance of polyfunctionalized carboxylic acids for OM, while the chemical processes responsible for their formation in both phases remain uncertain. While not measured by the TD–GC–MS technique, humic-like substances (HULISs) represent the most abundant identified species in the aerosol, contributing for 59 % of the total OM mass on average during the campaign. A total of 14 compounds were detected and quantified in both phases, allowing the calculation of experimental partitioning coefficients for these species. The comparison of these experimental partitioning coefficients with theoretical ones, estimated by three different models, reveals large discrepancies varying from 2 to 7 orders of magnitude. These results suggest that the supposed instantaneous equilibrium being established between gaseous and particulate phases assuming a homogeneous non-viscous particle phase is questionable.


2015 ◽  
Vol 15 (20) ◽  
pp. 11807-11833 ◽  
Author(s):  
W. W. Hu ◽  
P. Campuzano-Jost ◽  
B. B. Palm ◽  
D. A. Day ◽  
A. M. Ortega ◽  
...  

Abstract. Substantial amounts of secondary organic aerosol (SOA) can be formed from isoprene epoxydiols (IEPOX), which are oxidation products of isoprene mainly under low-NO conditions. Total IEPOX-SOA, which may include SOA formed from other parallel isoprene oxidation pathways, was quantified by applying positive matrix factorization (PMF) to aerosol mass spectrometer (AMS) measurements. The IEPOX-SOA fractions of organic aerosol (OA) in multiple field studies across several continents are summarized here and show consistent patterns with the concentration of gas-phase IEPOX simulated by the GEOS-Chem chemical transport model. During the Southern Oxidant and Aerosol Study (SOAS), 78 % of PMF-resolved IEPOX-SOA is accounted by the measured IEPOX-SOA molecular tracers (2-methyltetrols, C5-Triols, and IEPOX-derived organosulfate and its dimers), making it the highest level of molecular identification of an ambient SOA component to our knowledge. An enhanced signal at C5H6O+ (m/z 82) is found in PMF-resolved IEPOX-SOA spectra. To investigate the suitability of this ion as a tracer for IEPOX-SOA, we examine fC5H6O (fC5H6O= C5H6O+/OA) across multiple field, chamber, and source data sets. A background of ~ 1.7 ± 0.1 ‰ (‰ = parts per thousand) is observed in studies strongly influenced by urban, biomass-burning, and other anthropogenic primary organic aerosol (POA). Higher background values of 3.1 ± 0.6 ‰ are found in studies strongly influenced by monoterpene emissions. The average laboratory monoterpene SOA value (5.5 ± 2.0 ‰) is 4 times lower than the average for IEPOX-SOA (22 ± 7 ‰), which leaves some room to separate both contributions to OA. Locations strongly influenced by isoprene emissions under low-NO levels had higher fC5H6O (~ 6.5 ± 2.2 ‰ on average) than other sites, consistent with the expected IEPOX-SOA formation in those studies. fC5H6O in IEPOX-SOA is always elevated (12–40 ‰) but varies substantially between locations, which is shown to reflect large variations in its detailed molecular composition. The low fC5H6O (< 3 ‰) reported in non-IEPOX-derived isoprene-SOA from chamber studies indicates that this tracer ion is specifically enhanced from IEPOX-SOA, and is not a tracer for all SOA from isoprene. We introduce a graphical diagnostic to study the presence and aging of IEPOX-SOA as a triangle plot of fCO2 vs. fC5H6O. Finally, we develop a simplified method to estimate ambient IEPOX-SOA mass concentrations, which is shown to perform well compared to the full PMF method. The uncertainty of the tracer method is up to a factor of ~ 2, if the fC5H6O of the local IEPOX-SOA is not available. When only unit mass-resolution data are available, as with the aerosol chemical speciation monitor (ACSM), all methods may perform less well because of increased interferences from other ions at m/z 82. This study clarifies the strengths and limitations of the different AMS methods for detection of IEPOX-SOA and will enable improved characterization of this OA component.


2019 ◽  
Vol 19 (7) ◽  
pp. 5235-5249 ◽  
Author(s):  
Kuangyou Yu ◽  
Qiao Zhu ◽  
Ke Du ◽  
Xiao-Feng Huang

Abstract. Organic nitrates are important atmospheric species that significantly affect the cycling of NOx and ozone production. However, characterization of particulate organic nitrates and their sources in polluted atmosphere is a big challenge and has not been comprehensively studied in Asia. In this study, an aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) was deployed at an urban site in China from 2015 to 2016 to characterize particulate organic nitrates in total nitrates with a high time resolution. Based on the cross-validation of two different data processing methods, organic nitrates were effectively quantified to contribute a notable fraction of organic aerosol (OA), namely 9 %–21 % in spring, 11 %–25 % in summer, and 9 %–20 % in autumn, while contributing a very small fraction in winter. The good correlation between organic nitrates and fresh secondary organic aerosol (SOA) at night, as well as the diurnal trend of size distribution of organic nitrates, indicated a key role of nighttime local secondary formation of organic nitrates. Furthermore, theoretical calculations of nighttime SOA production of NO3 reactions with volatile organic compounds (VOCs) measured during the spring campaign were performed, resulting in three biogenic VOCs (α-pinene, limonene, and camphene) and one anthropogenic VOC (styrene) identified as the possible key VOC precursors to particulate organic nitrates. The comparison with similar studies in the literature implied that nighttime particulate organic nitrate formation is highly relevant to NOx levels. This study proposes that unlike the documented cases in the United States and Europe, modeling nighttime particulate organic nitrate formation in China should incorporate not only biogenic VOCs but also anthropogenic VOCs for urban air pollution, which needs the support of relevant smog chamber studies in the future.


Sign in / Sign up

Export Citation Format

Share Document