Reactions of Atmospheric Particulate Stabilized Criegee Intermediates Lead to High-Molecular-Weight Aerosol Components

Wang, Mingyi; Yao, Lei; Zheng, Jun; Wang, XinKe; Chen, Jianmin; Yang, Xin; Worsnop, Douglas R.; Donahue, Neil M.; Wang, Lin

doi:10.1021/acs.est.6b02114

Cited by 64 publications

(75 citation statements)

References 45 publications

(82 reference statements)

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“…The corresponding mass loadings and sampling times (particle collection on filter) for the four experiments are listed in Table 2. For experiment CD, the C10H16O4I1 -thermograms exhibited a multi-modal shape, indicative of contributions from isomers having different vapor pressures, or thermal decomposition of larger molecules. Based on previous FIGAERO data analyses (Lopez-Hilfiker et al, 2015;D'Ambro et al, 2017;Wang et al, 2016), we can safely presume that the first mode corresponds 310 to the monomer. Figure 6A−B shows that Tmax of an individual compound varied by up to 20 °C, depending on experimental conditions.…”

Section: Thermograms: Variation In Tmax Of Soa Compounds For Differenmentioning

confidence: 66%

α-pinene secondary organic aerosol at low temperature: Chemical composition and implications for particle viscosity

Huang¹,

Saathoff²,

Pajunoja³

et al. 2017

Preprint

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Abstract. Chemical composition and viscosity of secondary organic aerosol (SOA) from α-pinene (C10H16) ozonolysis were investigated for low temperature conditions (223 K). Two types of experiments were performed using two simulation chambers at the Karlsruhe Institute of Technology, the Aerosol Preparation and Characterization chamber (APC), and the Aerosol Interaction and Dynamics in the Atmosphere chamber (AIDA). Experiment type 1 simulated SOA formation at upper tropospheric conditions: SOA was generated in the AIDA chamber directly at 223 K, 61 % relative humidity (RH) (experiment 15 termed "cold humid", CH), or for comparison at 6 % RH (experiment termed "cold dry", CD) conditions. Experiment type 2 simulated SOA uplifting: SOA was formed in the APC chamber at room temperature (296 K), <1 % RH (experiment termed "warm dry", WD) or 21 % RH (experiment termed "warm humid", WH) conditions, and then partially transferred to the AIDA chamber kept at 223 K, and 61 % RH (WDtoCH) or 30 % RH (WHtoCH), respectively. Precursor concentrations varied between 0.7 and 2.2 ppm α-pinene, and 2.3 and 1.8 ppm ozone for type 1 and type 2 experiments, respectively. Among other 20 instrumentation, a chemical ionization mass spectrometer (CIMS) with filter inlet for gases and aerosols (FIGAERO), deploying I -as reagent ion, was used for SOA chemical composition analysis.For type 1 experiments with lower α-pinene concentration and cold SOA formation temperature (223 K), smaller particles of 100−300 nm vacuum aerodynamic diameter (dva) and higher mass fractions (>40 %) of adducts (molecules with more than 10 carbon atoms) of α-pinene oxidation products were observed. For type 2 experiments with higher α-pinene concentration 25 and warm SOA formation temperature (296 K), larger particles (~500 nm dva) with smaller mass fractions of adducts (<35 %) were produced.We also observed differences (up to 20 ºC) in maximum desorption temperature (Tmax) of individual compounds desorbing from the particles deposited on the FIGAERO Teflon filter for different experiments, indicating that Tmax is not purely a function of a compound's vapor pressure or volatility, but is also influenced by diffusion limitations within the particles 30 (particle viscosity), interactions between particles deposited on the filter (particle matrix), and/or particle mass on the filter.Highest Tmax were observed for SOA under dry conditions and with higher adduct mass fraction; lowest Tmax for SOA under humid conditions and with lowest adduct mass fraction. The observations indicate that particle viscosity may be influenced by intra-and inter-molecular hydrogen bonding between oligomers, and particle water uptake, even under such low temperature conditions. 35 Our results suggest that particle physicochemical properties such as viscosity and oligomer content mutually influence each other, and that variation in Tmax of particle desorptions may provide implications for particle viscosity and particle matrix effects. The differences in particle physicochemical properties ...

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Section: Thermograms: Variation In Tmax Of Soa Compounds For Differenmentioning

confidence: 66%

α-pinene secondary organic aerosol at low temperature: Chemical composition and implications for particle viscosity

Huang¹,

Saathoff²,

Pajunoja³

et al. 2017

Preprint

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“…Several mechanisms for oligomer product formation in SOA arising from VOC oxidation have been proposed: (i) self-and cross-reactions of the peroxy radicals (RO 2 ) (Zhang et al, 2015); (ii) reaction of ozonolysis products in the condensed-phase, such as aldol condensation, esterification, hemiacetal and peroxyhemiacetal formation (Ziemann, 2003;Tolocka et al, 2004;Kristensen et al, 2014;Docherty et al, 2005;Muller et al, 2009;Yasmeen et al, 2010;Hall and Johnston, 2012;Witkowski and Gierczak, 2014;DePalma et al, 2013;Lim and Turpin, 2015); (iii) dimer cluster formation from carboxylic acids (Hoffmann et al, 1998;Tobias and Ziemann, 2000;Claeys et al, 2009;Camredon et al, 2010;DePalma et al, 2013); (iv) reactions of Criegee intermediates (CIs) with VOCs oxidation products (Bonn et al, 2002;Lee and Kamens, 2005;Tolocka et al, 2006;Heaton et al, 2007;Witkowski and Gierczak, 2012;Kristensen et al, 2016;Wang et al, 2016); reactions of RO 2 radicals with Cis (Sadezky et al, 2008;Zhao et al, 2015). Among them, the reactions of CIs with protic substances (water, alcohols, acids and hydroperoxides) can form ROOH.…”

Section: Identification Of Rooh In Soa Materialsmentioning

confidence: 99%

Identification of organic hydroperoxides and peroxy acids using atmospheric pressure chemical ionization–tandem mass spectrometry (APCI-MS/MS): application to secondary organic aerosol

et al. 2018

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Abstract. Molecules with hydroperoxide functional groups are of extreme importance to both the atmospheric and biological chemistry fields. In this work, an analytical method is presented for the identification of organic hydroperoxides and peroxy acids (ROOH) by direct infusion of liquid samples into a positive-ion atmospheric pressure chemical ionization-tandem mass spectrometer ((+)-APCI-MS/MS). Under collisional dissociation conditions, a characteristic neutral loss of 51 Da (arising from loss of H 2 O 2 +NH 3 ) from ammonium adducts of the molecular ions ([M + NH 4 ] + ) is observed for ROOH standards (i.e. cumene hydroperoxide, isoprene-4-hydroxy-3-hydroperoxide (ISOPOOH), tertbutyl hydroperoxide, 2-butanone peroxide and peracetic acid), as well as the ROOH formed from the reactions of H 2 O 2 with aldehydes (i.e. acetaldehyde, hexanal, glyoxal and methylglyoxal). This new ROOH detection method was applied to methanol extracts of secondary organic aerosol (SOA) material generated from ozonolysis of α-pinene, indicating a number of ROOH molecules in the SOA material. While the full-scan mass spectrum of SOA demonstrates the presence of monomers (m/z = 80-250), dimers (m/z = 250-450) and trimers (m/z = 450-600), the neutral loss scan shows that the ROOH products all have masses less than 300 Da, indicating that ROOH molecules may not contribute significantly to the SOA oligomeric content. We anticipate this method could also be applied to biological systems with considerable value.

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“…Several mechanisms for oligomer product formation in SOA arising from VOC oxidation have been proposed: i) self-and cross-reactions of the peroxy radicals (RO 2 ) (Zhang et al, 2016), ii) reaction of ozonolysis products in the condensed-phase, such as aldol condensation, esterification, hemiacetal and peroxyhemiacetal formation (Ziemann, 2003;Tolocka et al, 2004;Kristensen et al, 2014;Docherty et al, 2005;Muller et al, 2009;Yasmeen et al, 2010;Hall and Johnston, 2012;Witkowski and Gierczak, 2012;DePalma et al, 2013;Lim and Turpin, 2015), iii) dimer cluster formation from carboxylic acids 15 (Hoffmann et al, 1998;Tobias and Ziemann, 2000;Claeys et al, 2009;Camredon et al, 2010;DePalma et al, 2013), iv) reactions of Criegee intermediates (CIs) with VOCs oxidation products (Bonn et al, 2002;Lee and Kamens, 2005;Tolocka et al, 2006;Heaton et al, 2007;Witkowski and Gierczak, 2012;Kristensen et al, 2016;Wang et al, 2016), and vi) reactions of RO 2 radicals with Cis (Sadezky et al, 2008;Zhao et al, 2015). Among them, the reactions of CIs with protic substances (water, alcohols, acids and hydroperoxides) can form ROOH.…”

Section: (A)mentioning

confidence: 99%

Identification of Organic Hydroperoxides and Peroxy Acids Using Atmospheric Pressure Chemical Ionization – Tandem Mass Spectrometry (APCI-MS/MS): Application to Secondary Organic Aerosol

Zhou¹,

Rivera-Rios²,

Keutsch³

et al. 2018

Preprint

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Abstract.Molecules with hydroperoxide functional groups are of extreme importance to both the atmospheric and biological 10 chemistry fields. In this work, an analytical method is presented for the identification of organic hydroperoxides and peroxy and peracetic acid), as well as the ROOH formed from the reactions of H 2 O 2 with aldehydes (i.e. acetaldehyde, hexanal, glyoxal and methylglyoxal). This new ROOH detection method was applied to methanol extracts of secondary organic aerosol (SOA) material generated from ozonolysis of α-pinene, indicating a number of ROOH molecules in the SOA material. While the full scan mass spectrum of SOA demonstrates the presence of monomers (m/z=80-250), dimers (m/z=250-450) and trimers (m/z=450-600), the neutral loss scan shows that the ROOH products all have masses less than 20 300 Da, indicating that ROOH molecules may not contribute significantly to the SOA oligomeric content. We anticipate this method could also be applied to biological systems with considerable value.

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Reactions of Atmospheric Particulate Stabilized Criegee Intermediates Lead to High-Molecular-Weight Aerosol Components

Cited by 64 publications

References 45 publications

α-pinene secondary organic aerosol at low temperature: Chemical composition and implications for particle viscosity

α-pinene secondary organic aerosol at low temperature: Chemical composition and implications for particle viscosity

Identification of organic hydroperoxides and peroxy acids using atmospheric pressure chemical ionization–tandem mass spectrometry (APCI-MS/MS): application to secondary organic aerosol

Identification of Organic Hydroperoxides and Peroxy Acids Using Atmospheric Pressure Chemical Ionization – Tandem Mass Spectrometry (APCI-MS/MS): Application to Secondary Organic Aerosol

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