Aerosol Liquid Water Driven by Anthropogenic Nitrate: Implications for Lifetimes of Water-Soluble Organic Gases and Potential for Secondary Organic Aerosol Formation

Hodas, Nathan O.; Sullivan, A.; Skog, Kate; Keutsch, Frank N.; Collett, Jeffrey L.; Decesari, Stefano; Facchini, M. C.; Carlton, Annmarie G.; Laaksonen, A.; Turpin, Barbara J.

doi:10.1021/es5025096

Cited by 107 publications

(128 citation statements)

References 95 publications

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“…For example, water in particles facilitates the partitioning of water-soluble gas species into the condensed phase (Blando and Turpin, 2000;Surratt et al, 2006;Ervens et al, 2008;Hennigan et al, 2008;Galloway et al, 2009;Asa-Awuku et al, 2010;Carlton and Turpin, 2013;Hodas et al, 2014). In this study, the growth of nanoparticles (here, the accumulation of the dry species) was simulated with the MABNAG model Hodshire et al, 2016), in which RH was varied in the range of 30-95 % while concentrations of the dry, gaseous species were kept constant (Fig.…”

Section: Atmospheric Implicationsmentioning

confidence: 99%

Vertically resolved concentration and liquid water content of atmospheric nanoparticles at the US DOE Southern Great Plains site

et al. 2018

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Abstract. Most prior field studies of new particle formation (NPF) have been performed at or near ground level, leaving many unanswered questions regarding the vertical extent of NPF. To address this, we measured concentrations of 11-16 nm diameter particles from ground level to 1000 m during the 2013 New Particle Formation Study at the Atmospheric Radiation Measurement Southern Great Plains site in Lamont, Oklahoma. The measurements were performed using a tethered balloon carrying two condensation particle counters that were configured for two different particle cut-off diameters. These observations were compared to data from three scanning mobility particle sizers at the ground level. We observed that 11-16 nm diameter particles were generated at the top region of the boundary layer, and were then rapidly mixed throughout the boundary layer. We also estimate liquid water content of nanoparticles using ground-based measurements of particle hygroscopicity obtained with a Humidified Tandem Differential Mobility Analyzer and vertically resolved relative humidity (RH) and temperature measured with a Raman lidar. Our analyses of these observations lead to the following conclusions regarding nanoparticles formed during NPF events at this site: (1) ground-based observations may not always accurately represent the timing, distribution, and meteorological conditions associated with the onset of NPF; (2) nanoparticles are highly hygroscopic and typically contain up to 50 % water by volume, and during conditions of high RH combined with high particle hygroscopicity, particles can be up to 95 % water by volume; (3) increased liquid water content of nanoparticles at high RH greatly enhances the partitioning of water-soluble species like organic acids into ambient nanoparticles.

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Section: Atmospheric Implicationsmentioning

confidence: 99%

Vertically resolved concentration and liquid water content of atmospheric nanoparticles at the US DOE Southern Great Plains site

et al. 2018

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“…Nitrate is more hygroscopic than sulfate (Kreidenweis et al, 2008) and was the main inorganic component during the sampling period with an average molar ratio NO 3 -/SO 4 2-= 4.5. Nitrate is expected to increase its importance not just in China but worldwide because of the generalized trend in policies aimed at reducing SO 2 emissions and the increasing emissions of NO x itself (Hodas et al, 2014).…”

Section: Daass Measured Water and Isorropia Estimationsmentioning

confidence: 99%

Continuous Measurement of Ambient Aerosol Liquid Water Content in Beijing

Fajardo

Jiang

Hao

2016

Aerosol Air Qual. Res.

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The amount of liquid water present on ambient aerosol particles influences its radiative properties, the partitioning of gas-phase organic and inorganic compounds to the condensed phase, and the assessment of particle health effects upon inhalation. An improved home-made Dry-Ambient Aerosol Size Spectrometer (DAASS) was implemented and deployed at a sampling site in Beijing to measure water content and volumetric growth factor of fine ambient aerosol during clean and polluted days. Aerosol chemical composition was characterized by an aerosol chemical speciation monitor (ACSM). Meteorological conditions were also assessed to trace origin of the air masses arriving at the site. A thermodynamic model, ISORROPIA II, was used to predict aerosol water content based on inorganic compositions measured by ACSM. It was then compared with the aerosol water content measured by DAASS. During the two-week sampling period, an aerosol efflorescence behavior was observed around 50% relative humidity (RH). Aerosol at the sample location was predominantly alkaline, with an average acidity ratio of 1.3 during the polluted days but very variable during the clean days. This fact coupled with generally low ambient RH resulted in low amounts of liquid water detected during the campaign. When RH reached its maximum of 87% and aerosol appeared to be more acidic, the maximum amount of aerosol water content measured was 1.3 µg m -3 (44.9% wt of DAASS measured ambient aerosol). Measured aerosol water content and model predictions seem to show a better agreement during the more polluted days, but during the clean days aerosol organic fraction appears to have an important contribution in the water content. We argue that the organicassociated water is comparable with that associated with inorganic compositions during the clean periods at low ambient RH conditions.

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“…For example, the major sink of nitrate radicals in the aqueous phase is the formation of HNO 3 (Kirkland et al, 2013). However, it should be noted that organonitrates are commonly observed in rainwater (Altieri et al, 2009), clouds (Boone et al, 2015), and wet aerosols (Hodas et al, 2014). Are organonitrates formed in the aqueous phase?…”

Section: Introductionmentioning

confidence: 99%

Photochemical organonitrate formation in wet aerosols

Lim

Kim

et al. 2016

Atmos. Chem. Phys.

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Abstract. Water is the most abundant component of atmospheric fine aerosol. However, despite rapid progress, multiphase chemistry involving wet aerosols is still poorly understood. In this work, we report results from smog chamber photooxidation of glyoxal-and OH-containing ammonium sulfate or sulfuric acid particles in the presence of NO x and O 3 at high and low relative humidity. Particles were analyzed using ultra-performance liquid chromatography coupled to quadrupole time-of-flight mass spectrometry (UPLC-Q-TOF-MS).During the 3 h irradiation, OH oxidation products of glyoxal that are also produced in dilute aqueous solutions (e.g., oxalic acids and tartaric acids) were formed in both ammonium sulfate (AS) aerosols and sulfuric acid (SA) aerosols. However, the major products were organonitrogens (CHNO), organosulfates (CHOS), and organonitrogen sulfates (CHNOS). These were also the dominant products formed in the dark chamber, indicating non-radical formation. In the humid chamber (> 70 % relative humidity, RH), two main products for both AS and SA aerosols were organonitrates, which appeared at m / z − 147 and 226. They were formed in the aqueous phase via non-radical reactions of glyoxal and nitric acid, and their formation was enhanced by photochemistry because of the photochemical formation of nitric acid via reactions of peroxy radicals, NO x and OH during the irradiation.

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Aerosol Liquid Water Driven by Anthropogenic Nitrate: Implications for Lifetimes of Water-Soluble Organic Gases and Potential for Secondary Organic Aerosol Formation

Cited by 107 publications

References 95 publications

Vertically resolved concentration and liquid water content of atmospheric nanoparticles at the US DOE Southern Great Plains site

Vertically resolved concentration and liquid water content of atmospheric nanoparticles at the US DOE Southern Great Plains site

Continuous Measurement of Ambient Aerosol Liquid Water Content in Beijing

Photochemical organonitrate formation in wet aerosols

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