The influence of semi-volatile and reactive primary emissions on the abundance and properties of global organic aerosol

Jathar, Shantanu H.; Farina, S. C.; Adams, P. J.; Robinson, Allen L.

doi:10.5194/acpd-11-5493-2011

Cited by 12 publications

(12 citation statements)

References 67 publications

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“…The compounds with volatilities between VOCs and OA (i.e., with saturation vapor concentrations from approximately 1 to 10 6 µg m −3 ) include semivolatile and intermediate volatility organic compounds (SVOCs and IVOCs, or S/IVOCs; Robinson et al, 2007), which are more difficult to quantify and speciate. There have been recent attempts to quantify bulk S/IVOCs Hunter et al, 2017), to speciate subsets of S/IVOCs (e.g., Zhao et al, 2014;Chan et al, 2016), and to model SOA formation from anthropogenic S/IVOCs from urban or aircraft emissions (Robinson et al, 2007;Dzepina et al, 2009;Hodzic et al, 2010;Jathar et al, 2011;Miracolo et al, 2011;Woody et al, 2015). The importance of biogenic S/IVOCs for SOA formation in ambient air was also recently demonstrated for the first time .…”

Section: Introductionmentioning

confidence: 99%

Secondary organic aerosol formation from ambient air in an oxidation flow reactor in central Amazonia

Palm¹,

Sá²,

Day³

et al. 2018

Atmos. Chem. Phys.

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Abstract. Secondary organic aerosol (SOA) formation from ambient air was studied using an oxidation flow reactor (OFR) coupled to an aerosol mass spectrometer (AMS) during both the wet and dry seasons at the Observations and Modeling of the Green Ocean Amazon (GoAmazon2014/5) field campaign. Measurements were made at two sites downwind of the city of Manaus, Brazil. Ambient air was oxidized in the OFR using variable concentrations of either OH or O 3 , over ranges from hours to days (O 3 ) or weeks (OH) of equivalent atmospheric aging. The amount of SOA formed in the OFR ranged from 0 to as much as 10 µg m −3 , depending on the amount of SOA precursor gases in ambient air. Typically, more SOA was formed during nighttime than daytime, and more from OH than from O 3 oxidation. SOA yields of individual organic precursors under OFR conditions were measured by standard addition into ambient air and were confirmed to be consistent with published environmental chamber-derived SOA yields. Positive matrix factorization of organic aerosol (OA) after OH oxidation showed formation of typical oxidized OA factors and a loss of primary Published by Copernicus Publications on behalf of the European Geosciences Union. OA factors as OH aging increased. After OH oxidation in the OFR, the hygroscopicity of the OA increased with increasing elemental O : C up to O : C∼1.0, and then decreased as O : C increased further. Possible reasons for this decrease are discussed. The measured SOA formation was compared to the amount predicted from the concentrations of measured ambient SOA precursors and their SOA yields. While measured ambient precursors were sufficient to explain the amount of SOA formed from O 3 , they could only explain 10-50 % of the SOA formed from OH. This is consistent with previous OFR studies, which showed that typically unmeasured semivolatile and intermediate volatility gases (that tend to lack C=C bonds) are present in ambient air and can explain such additional SOA formation. To investigate the sources of the unmeasured SOA-forming gases during this campaign, multilinear regression analysis was performed between measured SOA formation and the concentration of gas-phase tracers representing different precursor sources. The majority of SOA-forming gases present during both seasons were of biogenic origin. Urban sources also contributed substantially in both seasons, while biomass burning sources were more important during the dry season. This study enables a better understanding of SOA formation in environments with diverse emission sources.

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Section: Introductionmentioning

confidence: 99%

Secondary organic aerosol formation from ambient air in an oxidation flow reactor in central Amazonia

Palm¹,

Sá²,

Day³

et al. 2018

Atmos. Chem. Phys.

View full text Add to dashboard Cite

show abstract

“…Recent model improvements like consideration of marine OA components (e.g. Myriokefalitakis et al, 2010;Vignati et al, 2010), of the oxidation of intermediate VOC and the semivolatile character of primary OA (Pye and Seinfeld, 2010;Jathar et al, 2011), reduced the discrepancies with observations. Although underestimating OA, most models are actually able to simulate the order of magnitude of OA observations in the troposphere.…”

Section: Introductionmentioning

confidence: 99%

In-cloud oxalate formation in the global troposphere: a 3-D modeling study

et al. 2011

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Abstract. Organic acids attract increasing attention as contributors to atmospheric acidity, secondary organic aerosol mass and aerosol hygroscopicity. Oxalic acid is globally the most abundant dicarboxylic acid, formed via chemical oxidation of gas-phase precursors in the aqueous phase of aerosols and droplets. Its lifecycle and atmospheric global distribution remain highly uncertain and are the focus of this study. The first global spatial and temporal distribution of oxalate, simulated using a state-of-the-art aqueous-phase chemical scheme embedded within the global 3-dimensional chemistry/transport model TM4-ECPL, is here presented. The model accounts for comprehensive gas-phase chemistry and its coupling with major aerosol constituents (including secondary organic aerosol). Model results are consistent with ambient observations of oxalate at rural and remote locations (slope = 1.16 ± 0.14, r 2 = 0.36, N =114) and suggest that aqueous-phase chemistry contributes significantly to the global atmospheric burden of secondary organic aerosol. In TM4-ECPL most oxalate is formed in-cloud and less than 5 % is produced in aerosol water. About 62 % of the oxCorrespondence to: M. Kanakidou (mariak@chemistry.uoc.gr) alate is removed via wet deposition, 30 % by in-cloud reaction with hydroxyl radical, 4 % by in-cloud reaction with nitrate radical and 4 % by dry deposition. The in-cloud global oxalate net chemical production is calculated to be about 21-37 Tg yr −1 with almost 79 % originating from biogenic hydrocarbons, mainly isoprene. This condensed phase net source of oxalate in conjunction with a global mean turnover time against deposition of about 5 days, maintain oxalate's global tropospheric burden of 0.2-0.3 Tg, i.e. 0.05-0.1 Tg-C that is about 5-9 % of model-calculated water soluble organic carbon burden.

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“…Threedimensional model simulations implementing this scheme show increased mass concentrations of organics, yielding better agreement with observations over the United States, Europe, and at a global scale (e.g., Fountoukis et al, 2011;Jathar et al, 2011;Ahmadov et al, 2012;Barbet et al, 2016). Recently, the VBS scheme has been introduced into regional model simulations for East Asia (Matsui et al, 2014;Morino et al, 2014Morino et al, , 2015Han et al, 2016;Lin et al, 2016).…”

Section: Introductionmentioning

confidence: 84%

Observed and Modeled Mass Concentrations of Organic Aerosols and PM2.5 at Three Remote Sites around the East China Sea: Roles of Chemical Aging

Kanaya

Matsui

Taketani

et al. 2017

Aerosol Air Qual. Res.

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Severe PM 2.5 air pollution over the Asian continent is occasionally transported across the East China Sea by the westerly winds to Japan, continuing for long distances over the Pacific Ocean. Despite such polluted air masses causing health issues, conventional models tend to underestimate levels of organic aerosols (OA) and PM 2.5 . Here, PM 2.5 and its major components recorded during three field campaigns carried out at Fukue Island (32.75°N, 128.68°E), Japan (spring 2009), Rudong (32.25°N, 121.37°E), China (spring 2010), and Jeju (33.35°N, 126.39°E), Korea (autumn 2012) around the East China Sea were used to test the performance of the Weather Research and Forecasting-Chem/ATRAS-MOSAIC model. Overall, model performance was improved by introducing chemical aging represented by a volatility basis-set scheme, whereby median values of the model/observation ratio for OA were raised to 0.34-1.28 from 0.30-0.35 in the case of conventional settings. In particular, the levels of OA at the Fukue site and daytime buildup of the OA levels at all three sites were reproduced by the model. OA levels were still sometimes underestimated. This suggests that either emission rates of organic precursors are being underestimated or other pathways of OA formation are also important. Our analysis also indicates that this region is characterized by high OH concentrations, promoting chemical aging. The predictions of PM 2.5 levels in the model also improved, with median values of the model/observation ratio shifting from 0.67-0.91 to 0.68-0.95, when chemical aging of OA was taken into account.

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The influence of semi-volatile and reactive primary emissions on the abundance and properties of global organic aerosol

Cited by 12 publications

References 67 publications

Secondary organic aerosol formation from ambient air in an oxidation flow reactor in central Amazonia

Secondary organic aerosol formation from ambient air in an oxidation flow reactor in central Amazonia

In-cloud oxalate formation in the global troposphere: a 3-D modeling study

Observed and Modeled Mass Concentrations of Organic Aerosols and PM2.5 at Three Remote Sites around the East China Sea: Roles of Chemical Aging

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