Effect of the Aerosol-Phase State on Secondary Organic Aerosol Formation from the Reactive Uptake of Isoprene-Derived Epoxydiols (IEPOX)

Zhang, Yue; Chen, Yuzhi; Lambe, Andrew T.; Olson, Nicole E.; Lei, Ziying; Craig, R. L.; Zhang, Zhenfa; Gold, Avram; Onasch, T. B.; Jayne, John T.; Worsnop, Douglas R.; Gaston, Cassandra J.; Thornton, Joel A.; Vizuete, William; Ault, Andrew P.; Surratt, Jason D.

doi:10.1021/acs.estlett.8b00044

Cited by 170 publications

(281 citation statements)

References 77 publications

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“…Thus, the reaction system by Nguyen et al (2011b) can be considered to be closer to the isoprene-H 2 O 2 system. In addition, some other previous studies (Gaston et al, 2014;Riedel et al, 2015;Zhang et al, 2018) showed that RH had a negative effect on the formation of SOA from isoprene-OH systems due to an acid dilution effect. In these studies, acidic sulfate seed particles were used and the acid-catalyzed effect was very obvious.…”

Section: Soa Yieldsmentioning

confidence: 81%

Different roles of water in secondary organic aerosol formation from toluene and isoprene

Jia

2018

Atmos. Chem. Phys.

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Abstract. Roles of water in the formation of secondary organic aerosol (SOA) from the irradiations of toluene-NO 2 and isoprene-NO 2 were investigated in a smog chamber. Experimental results show that the yield of SOA from toluene almost doubled as relative humidity increased from 5 to 85 %, whereas the yield of SOA from isoprene under humid conditions decreased by 2.6 times as compared to that under dry conditions. The distinct difference of RH effects on SOA formation from toluene and isoprene is well explained with our experiments and model simulations. The increased SOA from humid toluene-NO 2 irradiations is mainly contributed by O-H-containing products such as polyalcohols formed from aqueous reactions. The major chemical components of SOA in isoprene-NO 2 irradiations are oligomers formed from the gas phase. SOA formation from isoprene-NO 2 irradiations is controlled by stable Criegee intermediates (SCIs) that are greatly influenced by water. As a result, high RH can obstruct the oligomerization reaction of SCIs to form SOA.

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Section: Soa Yieldsmentioning

confidence: 81%

Different roles of water in secondary organic aerosol formation from toluene and isoprene

Jia

2018

Atmos. Chem. Phys.

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“…Recent studies have confirmed that organic aerosols, which comprise approximately half of the total submicron aerosol mass in the atmosphere, can change from liquid to glassy state at ambient humidity levels and temperatures (Zobrist et al, 2008;Virtanen et al, 2010;Shrestha et al, 2014;Zhang et al, 2015). The effect of temperature may be especially important when aerosol particles are lifted into the free troposphere, where the temperature change can rapidly alter their phase from liquid to glass .…”

Section: Introductionmentioning

confidence: 99%

“…Kuwata and Martin (2012) showed that the phase state of secondary organic aerosols (SOAs) affects the uptake of ammonia into the particles. Zhang et al (2018) provided experimental and modeling evidence that the reactive uptake of isoprene-derived epoxydiols (IEPOX) into acidic sulfate particles is influenced by the phase state, which can contribute to at least a 30 % reduction in isoprene-derived SOAs in the southeastern USA.…”

Section: Introductionmentioning

confidence: 99%

Kinetically controlled glass transition measurement of organic aerosol thin films using broadband dielectric spectroscopy

et al. 2018

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Abstract. Glass transitions from liquid to semi-solid and solid phase states have important implications for reactivity, growth, and cloud-forming (cloud condensation nuclei and ice nucleation) capabilities of secondary organic aerosols (SOAs). The small size and relatively low mass concentration of SOAs in the atmosphere make it difficult to measure atmospheric SOA glass transitions using conventional methods. To circumvent these difficulties, we have adapted a new technique for measuring glass-forming properties of atmospherically relevant organic aerosols. Aerosol particles to be studied are deposited in the form of a thin film onto an interdigitated electrode (IDE) using electrostatic precipitation. Dielectric spectroscopy provides dipole relaxation rates for organic aerosols as a function of temperature (373 to 233 K) that are used to calculate the glass transition temperatures for several cooling or heating rates. IDE-enabled broadband dielectric spectroscopy (BDS) was successfully used to measure the kinetically controlled glass transition temperatures of aerosols consisting of glycerol and four other compounds with selected cooling and heating rates. The glass transition results agree well with available literature data for these five compounds. The results indicate that the IDE-BDS method can provide accurate glass transition data for organic aerosols under atmospheric conditions. The BDS data obtained with the IDE-BDS technique can be used to characterize glass transitions for both simulated and ambient organic aerosols and to model their climate effects.

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“…Note that this relation is not accurate for predicting the bulk diffusivity of water and small molecules and it may also underestimate the diffusivity of organic molecules in a highly viscous matrix by a few orders of magnitudes (Champion et al, 2000;Shiraiwa et al, 2011;Power et al, 2013;Marshall et al, 2016;Bastelberger et al, 2017;Reid et al, 2018). The particle phase state, viscosity, and bulk diffusivity have been shown to affect the gas uptake and chemical transformation of organic compounds due to the kinetic limitations of bulk diffusion Abbatt et al, 2012;Zhou et al, 2013;Slade and Knopf, 2014;Arangio et al, 2015;Davies and Wilson, 2015;Wang et al, 2015;Berkemeier et al, 2016;Marshall et al, 2016;Liu et al, 2018;Pratap et al, 2018;Zhang et al, 2018), which may facilitate the long-range transport of organic compounds embedded in viscous or glassy particles (Shrivastava et al, 2017b;Mu et al, 2018). Molecular motion can be hindered in a highly viscous matrix, slowing down photochemical reactions in particles (Lignell et al, 2014;Hinks et al, 2016).…”

Section: Introductionmentioning

confidence: 99%

Predicting the glass transition temperature and viscosity of secondary organic material using molecular composition

et al. 2018

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Abstract. Secondary organic aerosol (SOA) accounts for a large fraction of submicron particles in the atmosphere. SOA can occur in amorphous solid or semi-solid phase states depending on chemical composition, relative humidity (RH), and temperature. The phase transition between amorphous solid and semi-solid states occurs at the glass transition temperature (T g ). We have recently developed a method to estimate T g of pure compounds containing carbon, hydrogen, and oxygen atoms (CHO compounds) with molar mass less than 450 g mol −1 based on their molar mass and atomic O : C ratio. In this study, we refine and extend this method for CH and CHO compounds with molar mass up to ∼ 1100 g mol −1 using the number of carbon, hydrogen, and oxygen atoms. We predict viscosity from the T g -scaled Arrhenius plot of fragility (viscosity vs. T g /T ) as a function of the fragility parameter D. We compiled D values of organic compounds from the literature and found that D approaches a lower limit of ∼ 10 (±1.7) as the molar mass increases. We estimated the viscosity of α-pinene and isoprene SOA as a function of RH by accounting for the hygroscopic growth of SOA and applying the Gordon-Taylor mixing rule, reproducing previously published experimental measurements very well. Sensitivity studies were conducted to evaluate impacts of T g , D, the hygroscopicity parameter (κ), and the Gordon-Taylor constant on viscosity predictions. The viscosity of toluene SOA was predicted using the elemental composition obtained by high-resolution mass spectrometry (HRMS), resulting in a good agreement with the measured viscosity. We also estimated the viscosity of biomass burning particles using the chemical composition measured by HRMS with two different ionization techniques: electrospray ionization (ESI) and atmospheric pressure photoionization (APPI). Due to differences in detected organic compounds and signal intensity, predicted viscosities at low RH based on ESI and APPI measurements differ by 2-5 orders of magnitude. Complementary measurements of viscosity and chemical composition are desired to further constrain RH-dependent viscosity in future studies.

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Effect of the Aerosol-Phase State on Secondary Organic Aerosol Formation from the Reactive Uptake of Isoprene-Derived Epoxydiols (IEPOX)

Cited by 170 publications

References 77 publications

Different roles of water in secondary organic aerosol formation from toluene and isoprene

Different roles of water in secondary organic aerosol formation from toluene and isoprene

Kinetically controlled glass transition measurement of organic aerosol thin films using broadband dielectric spectroscopy

Predicting the glass transition temperature and viscosity of secondary organic material using molecular composition

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