Gas phase precursors to anthropogenic secondary organic aerosol: detailed observations of 1,3,5-trimethylbenzene photooxidation

Wyche, Kevin; Monks, Paul S.; Ellis, Andrew M.; Cordell, Rebecca; Parker, Alison E.; Whyte, Christopher; Metzger, Axel; Dommen, Josef; Duplissy, Jonathan; Prévôt, Andrê S. H.; Baltensperger, Urs; Rickard, Andrew R.; Wülfert, Florian

doi:10.5194/acpd-8-11685-2008

Cited by 3 publications

(6 citation statements)

References 65 publications

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“…The mass fraction (4.8%) of ON groups under high-NO x and high-RH conditions (28 March) matched the mass fraction (3.2 ± 2.0%) measured at coastal Southern California (Day et al 2010), a site that was significantly influenced by anthropogenic emissions (from the Los Angeles Basin) and associated with high RH. The OM yield, quantified by FTIR and defined as the ratio of OM to the mass of reacted TMB (Odum et al 1996), spanned from 1.7 to 5.9% in agreement with reported SOA yields for TMB (Odum et al 1996;Cocker et al 2001;Wyche et al 2009). …”

Section: On Group Mass Fractionmentioning

confidence: 58%

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Hydrolysis of Organonitrate Functional Groups in Aerosol Particles

Liu

Shilling

Song

et al. 2012

Aerosol Science and Technology

181

204

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Organonitrate (ON) groups are thought to be important substituents in secondary organic aerosols (SOAs). Model simulations and laboratory studies indicate a large fraction of ON groups in aerosol particles, but much lower quantities are observed in the atmosphere. Hydrolysis of ON groups in aerosol particles has been proposed recently to account for this discrepancy. To test this hypothesis, we simulated formation of ON molecules in a reaction chamber under a wide range of relative humidity (RH) (0 to 90%). The mass fraction of ON groups (5 to 20% for high-NO x experiments) consistently decreased with increasing RH, which was best explained by hydrolysis of ON groups at a rate of 4 day −1 (lifetime of 6 h) for reactions under RH greater than 20%. In addition, we found that secondary nitrogen-containing molecules absorb light, with greater absorption under dry and high-NO x conditions. This work provides the first evidence for particle-phase hydrolysis of ON groups, a process that could substantially reduce ON group concentration in atmospheric SOAs.

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Section: On Group Mass Fractionmentioning

confidence: 58%

“…According to Wyche et al (2009), one likely product of 1,2,4-TMB and OH reaction system is molecule A (Figure 7), which contains a tertiary ON group and is sufficiently nonvolatile to partition into particle phase (Johnson et al 2004(Johnson et al , 2005Wyche et al 2009).…”

Section: Fig 3 Time-dependence Of (A) Rh (B) Temperature (C) Tmbmentioning

confidence: 99%

Hydrolysis of Organonitrate Functional Groups in Aerosol Particles

Liu

Shilling

Song

et al. 2012

Aerosol Science and Technology

181

204

View full text Add to dashboard Cite

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“…(Sato et al, 2012;Kleindienst et al, 1999;Wyche et al, 2009;Odum et al, 1997;Paulsen et al, 2005;Cocker et al, 2001). Only Cao and Jang (2007) investigated SOA yields in the absence of NO x and reported values between 7.1 and 13.8 %.…”

Section: Influence Of Heating Temperaturementioning

confidence: 99%

“…Oxidation products of 1,3,5-TMB were investigated in a number of studies (e.g. Huang et al, 2015;Kalberer et al, 2004Kalberer et al, , 2006Paulsen et al, 2005;Healy et al, 2008;Cocker et al, 2001;Metzger et al, 2008;Wyche et al, 2009;Yu et al, 1997). Methylglyoxal was found as one of the most important oxidation product Healy et al, 2008;Cocker et al, 2001;Wyche et al, 2009;Rickard et al, 2010;Kalberer et al, 2004;Yu et al, 1997;Müller et al, 2012;Nishino et al, 2010;Hamilton et al, 2003;Tuazon et al, 1986;Bandow and Washida, 1985;Lim and Turpin, 2015) contributing with a fraction of up to 2 % to the particle mass (Healy et al, 2008;Cocker et al, 2001).…”

Section: Introductionmentioning

confidence: 99%

A quantification method for heat-decomposable methylglyoxal oligomers and its application on 1,3,5-trimethylbenzene SOA

2017

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Abstract. Methylglyoxal forms oligomeric compounds in the atmospheric aqueous particle phase, which could establish a significant contribution to the formation of aqueous secondary organic aerosol (aqSOA). Thus far, no suitable method for the quantification of methylglyoxal oligomers is available despite the great effort spent for structure elucidation. In the present study a simplified method was developed to quantify heat-decomposable methylglyoxal oligomers as a sum parameter. The method is based on the thermal decomposition of oligomers into methylglyoxal monomers. Formed methylglyoxal monomers were detected using PFBHA (o-(2,3,4,5,6-pentafluorobenzyl)hydroxylamine hydrochloride) derivatisation and gas chromatography-mass spectrometry (GC/MS) analysis. The method development was focused on the heating time (varied between 15 and 48 h), pH during the heating process (pH = 1-7), and heating temperature (50, 100 • C). The optimised values of these method parameters are presented.The developed method was applied to quantify heatdecomposable methylglyoxal oligomers formed during the OH-radical oxidation of 1,3,5-trimethylbenzene (TMB) in the Leipzig aerosol chamber (LEipziger AerosolKammer, LEAK). Oligomer formation was investigated as a function of seed particle acidity and relative humidity. A fraction of heat-decomposable methylglyoxal oligomers of up to 8 % in the produced organic particle mass was found, highlighting the importance of those oligomers formed solely by methylglyoxal for SOA formation. Overall, the present study provides a new and suitable method for quantification of heatdecomposable methylglyoxal oligomers in the aqueous particle phase.

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“…Previous (NH 4 ) 2 SO 4 seed studies emphasize the effect on SOA mass yields in the smog chamber. Wyche et al [29] found that (NH 4 ) 2 SO 4 seeds with low concentrations (0.2~40 μg m -3 ) had no detectable influence on mass yields of aromatic SOA. By contrast, mass yields of m-xylene SOA were clearly raised with high concentrations (40~100 μg m ) of (NH 4 ) 2 SO 4 seeds [30].…”

Section: Introductionmentioning

confidence: 99%

Mass Spectral Analysis of the Aged 1,3,5-Trimethylbenzene Secondary Organic Aerosol in the Presence of Ammonium Sulfate Seeds

Huang

Cai

et al. 2017

Pol. J. Environ. Stud.

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The ammonium sulfate ((NH 4 ) 2 SO 4 ) seed aerosols commonly found in the Chinese urban atmosphere could affect the formation and aging of secondary organic aerosols (SOA). Aging of aromatic SOA is performed using UV-irradiation of 1,3,5-trimethylbenzene (135-TMB)/CH 3 ONO/NO/air mixtures with high concentrations (~100 μg/m 3 ) of (NH 4 ) 2 SO 4 seeds in the laboratory chamber in this study. The particulate products of SOA were measured using an aerosol laser time-of-flight mass spectrometer (ALTOFMS) in real-time, and fuzzy c-means (FCM) was applied to the mass spectra organic species for clusters. Experimental results indicated that methylglyxoal, 2-methyl-4-oxo-2-pentenal, 4-methyl-1H-imidazole, 4-methyl-imidazole-2-acetaldehyde, and other imidazole derivative compounds are the principal products in the aged particles. Imidazole compounds that can absorb solar radiation effectively were newly detected in the aged 135-TMB SOA with high concentrations of (NH 4 ) 2 SO 4 seed aerosols. These would provide new information for discussing the 135-TMB SOA aging mechanism.

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Gas phase precursors to anthropogenic secondary organic aerosol: detailed observations of 1,3,5-trimethylbenzene photooxidation

Cited by 3 publications

References 65 publications

Hydrolysis of Organonitrate Functional Groups in Aerosol Particles

Hydrolysis of Organonitrate Functional Groups in Aerosol Particles

A quantification method for heat-decomposable methylglyoxal oligomers and its application on 1,3,5-trimethylbenzene SOA

Mass Spectral Analysis of the Aged 1,3,5-Trimethylbenzene Secondary Organic Aerosol in the Presence of Ammonium Sulfate Seeds

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