Chemical composition of gas and particle–phase products of OH–initiated oxidation of 1,3,5–trimethylbenzene

Huang, Mingqiang; Hu, Changjin; Guo, Xiaoyong; Gu, Xuejun; Zhao, Weixiong; Wang, Zhenya; Li, Fang; Zhang, Weijun

doi:10.5094/apr.2014.009

Cited by 16 publications

(7 citation statements)

References 29 publications

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“…According to the literature, other carbonyl compounds can be expected as particle-phase products, e.g. propionaldehyde (Cocker et al, 2001), glyoxal (Cocker et al, 2001;Huang et al, 2015), 2-methyl-4-oxo-2-pentenal (Healy et al, 2008;Huang et al, 2014), glycolaldehyde (Cocker et al, 2001) and 3,5-dimethylbenzaldehyde (Huang et al, 2014). Noticeably, no carbonyl compounds other than methylglyoxal were identified, which showed an increase after thermal decomposition.…”

Section: Influence Of Heating Temperaturementioning

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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Section: Influence Of Heating Temperaturementioning

confidence: 99%

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

2017

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“…In this study we investigate a range of isomers of C 9 aromatics to evaluate this effect in more detail. Of the aromatics studied in these experiments, molecular understanding of SOA products is most well developed for the trimethylbenzene isomers (Huang et al, 2014;Li and Wang, 2014;Sato et al, 2012Sato et al, , 2019. Though other aromatics have been studied, these have either lacked molecular-level detail or focused on gas-phase oxidation and lacked detailed characterisation of SOA (Chan et al, 2009;Li et al, 2016;Molteni et al, 2018;Ping, 2013).…”

Section: Introductionmentioning

confidence: 99%

Evaluation of the chemical composition of gas- and particle-phase products of aromatic oxidation

et al. 2020

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Abstract. Aromatic volatile organic compounds (VOCs) are key anthropogenic pollutants emitted to the atmosphere and are important for both ozone and secondary organic aerosol (SOA) formation in urban areas. Recent studies have indicated that aromatic hydrocarbons may follow previously unknown oxidation chemistry pathways, including autoxidation that can lead to the formation of highly oxidised products. In this study we evaluate the gas- and particle-phase ions measured by online mass spectrometry during the hydroxyl radical oxidation of substituted C9-aromatic isomers (1,3,5-trimethylbenzene, 1,2,4-trimethylbenzene, propylbenzene and isopropylbenzene) and a substituted polyaromatic hydrocarbon (1-methylnaphthalene) under low- and medium-NOx conditions. A time-of-flight chemical ionisation mass spectrometer (ToF-CIMS) with iodide–anion ionisation was used with a filter inlet for gases and aerosols (FIGAERO) for the detection of products in the particle phase, while a Vocus proton-transfer-reaction mass spectrometer (Vocus-PTR-MS) was used for the detection of products in the gas phase. The signal of product ions observed in the mass spectra were compared for the different precursors and experimental conditions. The majority of mass spectral product signal in both the gas and particle phases comes from ions which are common to all precursors, though signal distributions are distinct for different VOCs. Gas- and particle-phase composition are distinct from one another. Ions corresponding to products contained in the near-explicit gas phase Master Chemical Mechanism (MCM version 3.3.1) are utilised as a benchmark of current scientific understanding, and a comparison of these with observations shows that the MCM is missing a range of highly oxidised products from its mechanism. In the particle phase, the bulk of the product signal from all precursors comes from ring scission ions, a large proportion of which are more oxidised than previously reported and have undergone further oxidation to form highly oxygenated organic molecules (HOMs). Under the perturbation of OH oxidation with increased NOx, the contribution of HOM-ion signals to the particle-phase signal remains elevated for more substituted aromatic precursors. Up to 43 % of product signal comes from ring-retaining ions including HOMs; this is most important for the more substituted aromatics. Unique products are a minor component in these systems, and many of the dominant ions have ion formulae concurrent with other systems, highlighting the challenges in utilising marker ions for SOA.

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“…A box model run was performed to test the impact of this chemistry in this study. The α-pinene scheme from the Master Chemical Mechanism version v3.3.1 (MCMv3.3.1;Jenkin et al, 1997; http://mcm.york.ac.uk, last access: 27 January 2022) was incorporated into the AtChem box model (Sommariva et al, 2020), and an OH yield of 0.5 was assigned to the reaction of HO 2 with the initial β-ONO 2 -RO 2 radicals formed from the α-pinene+NO 3 reaction. The model was initiated with A further potential interference with the current experimental set-up is the reaction of NO 2 with the compounds used.…”

Section: Ln ([Vocmentioning

confidence: 99%

“…Oxidation of furans in the atmosphere has been shown to produce 2-furanones (monounsaturated five-membered cyclic esters) both via OH (notably hydroxy-furan-2-ones; Aschmann et al, 2014) and NO 3 (Berndt et al, 1997) reactions. Furan-2-ones are also produced from the OH oxidation of six-membered aromatic compounds (Smith et al, 1998(Smith et al, , 1999Hamilton et al, 2005;Bloss et al, 2005;Wyche et al, 2009;Huang et al, 2014). In both cases, the initial product is thought to be an unsaturated dicarbonyl, with production of the 2-furanone formed via photoisomerisation of the dicarbonyl to a ketene-enol (Newland et al, 2019), followed by ring closure of this molecule.…”

Section: Introductionmentioning

confidence: 99%

NO<sub>3</sub> chemistry of wildfire emissions: a kinetic study of the gas-phase reactions of furans with the NO<sub>3</sub> radical

et al. 2022

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Abstract. Furans are emitted to the atmosphere during biomass burning from the pyrolysis of cellulose. They are one of the major contributing volatile organic compound (VOC) classes to OH and NO3 reactivity in biomass burning plumes. The major removal process of furans from the atmosphere at night is reaction with the nitrate radical, NO3. Here, we report a series of relative rate experiments in the 7300 L indoor simulation chamber at Institut de Combustion Aérothermique Réactivité et Environnement, Centre national de la recherche scientifique (ICARE-CNRS), Orléans, using a number of different reference compounds to determine NO3 reaction rate coefficients for four furans, two furanones, and pyrrole. In the case of the two furanones, this is the first time that NO3 rate coefficients have been reported. The recommended values (cm3 molec.−1 s−1) are as follows: furan, (1.49 ± 0.23) × 10−12; 2-methylfuran, (2.26 ± 0.52) × 10−11; 2,5-dimethylfuran, (1.02 ± 0.31) × 10−10; furfural (furan-2-aldehyde), (9.07 ± 2.3) × 10−14; α-angelicalactone (5-methyl-2(3H)-furanone), (3.01 ± 0.45) × 10−12; γ-crotonolactone (2(5H)-furanone), <1.4 × 10−16; and pyrrole, (6.94 ± 1.9) × 10−11. The furfural + NO3 reaction rate coefficient is found to be an order of magnitude smaller than previously reported. These experiments show that for furan, alkyl-substituted furans, α-angelicalactone, and pyrrole, reaction with NO3 will be the dominant removal process at night and may also contribute during the day. For γ-crotonolactone, reaction with NO3 is not an important atmospheric sink.

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Chemical composition of gas and particle–phase products of OH–initiated oxidation of 1,3,5–trimethylbenzene

Cited by 16 publications

References 29 publications

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

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

Evaluation of the chemical composition of gas- and particle-phase products of aromatic oxidation

NO<sub>3</sub> chemistry of wildfire emissions: a kinetic study of the gas-phase reactions of furans with the NO<sub>3</sub> radical

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Chemical composition of gas and particle–phase products of OH–initiated oxidation of 1,3,5–trimethylbenzene

Cited by 16 publications

References 29 publications

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

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

Evaluation of the chemical composition of gas- and particle-phase products of aromatic oxidation

NO&lt;sub&gt;3&lt;/sub&gt; chemistry of wildfire emissions: a kinetic study of the gas-phase reactions of furans with the NO&lt;sub&gt;3&lt;/sub&gt; radical

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NO<sub>3</sub> chemistry of wildfire emissions: a kinetic study of the gas-phase reactions of furans with the NO<sub>3</sub> radical