Diurnal Variations in Partitioning of Atmospheric Glyoxal and Methylglyoxal between Gas and Particles at the Ground Level and in the Free Troposphere

Kasumi Mitsuishi, Masakazu Iwasaki, Masaki Takeuchi, Hiroshi Okochi, Shungo Kato, Shin Ichi Ohira, Kei Toda

    Research output: Contribution to journalArticle

    Abstract

    This work presents diurnal variations of gas- and particle-phase dicarbonyls (glyoxal (Gly) and methylglyoxal (Mgly)) in the atmosphere, which are important compounds that contribute to the formation and growth of atmospheric particulate matter. To obtain variations in partitioning, continuous collection of gaseous dicarbonyls was performed using a parallel plate wet denuder, and at the same time, the dicarbonyls in particle were collected using a spray-type particle collector downstream. Hourly samples were analyzed by high performance liquid chromatography-electrospray ionization-tandem mass spectrometry. This method is advantageous to monitor the gaseous and particulate carbonyls separately without loss during sampling. Sampling was performed in summer and winter in a midsize city (Kumamoto, Japan). The concentrations of the dicarbonyls increased in the summer daytime, which suggests that they are mostly formed by secondary production in the local atmosphere. The dicarbonyls and formaldehyde (HCHO) were found in both gas and particle phases, and partitioning to the particle phase was highest for Gly, followed by Mgly and HCHO. It was observed that the compounds moved to the particle phase in the midnight and early morning hours according to the growth of hygroscopic aerosols in summer. The particle/gas ratio also increased in the presence of high PM2.5, which is transported from the Chinese Continent in winter. The dicarbonyls were also observed on Mt. Fuji (3776 m) in the free troposphere. From back trajectory data and information on volatile organic compounds, they were most likely produced from relatively long-lifetime organic compounds from the Chinese Continent and biogenic volatile organic compounds emitted in the Japan Alps mountain range. Higher particle/gas ratios at the Mt. Fuji station indicate that low temperatures and high humidity precede the partition. The estimated effective Henry's law constants for the dicarbonyls, 108 order in mol/kgH2O/atm for summer data, were much higher than those for ideal liquid/vapor equilibrium but close to reported results obtained by chamber experiments. In the proposed method, oligomers in particle were also counted as the compounds. The dicarbonyl compounds existed up to submolar levels in real atmospheric aerosols, which suggests they undergo further reactions in the particle phase.

    Original languageEnglish
    Pages (from-to)915-924
    Number of pages10
    JournalACS Earth and Space Chemistry
    Volume2
    Issue number9
    DOIs
    Publication statusPublished - 2018 Sep 20

    Fingerprint

    Glyoxal
    Pyruvaldehyde
    Troposphere
    diurnal variations
    troposphere
    diurnal variation
    partitioning
    Gases
    Volatile Organic Compounds
    gases
    gas
    summer
    Sampling
    Atmospheric aerosols
    Electrospray ionization
    Particulate Matter
    High performance liquid chromatography
    Aerosols
    Organic compounds
    Oligomers

    Keywords

    • dinitrophenylhydrazine derivatization
    • glyoxal
    • high performance liquid chromatography?tandem mass spectrometry
    • methylglyoxal
    • Mt. Fuji
    • parallel plate wet denuder
    • particulate matter
    • partition

    ASJC Scopus subject areas

    • Atmospheric Science
    • Geochemistry and Petrology
    • Space and Planetary Science

    Cite this

    Diurnal Variations in Partitioning of Atmospheric Glyoxal and Methylglyoxal between Gas and Particles at the Ground Level and in the Free Troposphere. / Mitsuishi, Kasumi; Iwasaki, Masakazu; Takeuchi, Masaki; Okochi, Hiroshi; Kato, Shungo; Ohira, Shin Ichi; Toda, Kei.

    In: ACS Earth and Space Chemistry, Vol. 2, No. 9, 20.09.2018, p. 915-924.

    Research output: Contribution to journalArticle

    Mitsuishi, Kasumi ; Iwasaki, Masakazu ; Takeuchi, Masaki ; Okochi, Hiroshi ; Kato, Shungo ; Ohira, Shin Ichi ; Toda, Kei. / Diurnal Variations in Partitioning of Atmospheric Glyoxal and Methylglyoxal between Gas and Particles at the Ground Level and in the Free Troposphere. In: ACS Earth and Space Chemistry. 2018 ; Vol. 2, No. 9. pp. 915-924.
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    abstract = "This work presents diurnal variations of gas- and particle-phase dicarbonyls (glyoxal (Gly) and methylglyoxal (Mgly)) in the atmosphere, which are important compounds that contribute to the formation and growth of atmospheric particulate matter. To obtain variations in partitioning, continuous collection of gaseous dicarbonyls was performed using a parallel plate wet denuder, and at the same time, the dicarbonyls in particle were collected using a spray-type particle collector downstream. Hourly samples were analyzed by high performance liquid chromatography-electrospray ionization-tandem mass spectrometry. This method is advantageous to monitor the gaseous and particulate carbonyls separately without loss during sampling. Sampling was performed in summer and winter in a midsize city (Kumamoto, Japan). The concentrations of the dicarbonyls increased in the summer daytime, which suggests that they are mostly formed by secondary production in the local atmosphere. The dicarbonyls and formaldehyde (HCHO) were found in both gas and particle phases, and partitioning to the particle phase was highest for Gly, followed by Mgly and HCHO. It was observed that the compounds moved to the particle phase in the midnight and early morning hours according to the growth of hygroscopic aerosols in summer. The particle/gas ratio also increased in the presence of high PM2.5, which is transported from the Chinese Continent in winter. The dicarbonyls were also observed on Mt. Fuji (3776 m) in the free troposphere. From back trajectory data and information on volatile organic compounds, they were most likely produced from relatively long-lifetime organic compounds from the Chinese Continent and biogenic volatile organic compounds emitted in the Japan Alps mountain range. Higher particle/gas ratios at the Mt. Fuji station indicate that low temperatures and high humidity precede the partition. The estimated effective Henry's law constants for the dicarbonyls, 108 order in mol/kgH2O/atm for summer data, were much higher than those for ideal liquid/vapor equilibrium but close to reported results obtained by chamber experiments. In the proposed method, oligomers in particle were also counted as the compounds. The dicarbonyl compounds existed up to submolar levels in real atmospheric aerosols, which suggests they undergo further reactions in the particle phase.",
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    AU - Takeuchi, Masaki

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    AU - Ohira, Shin Ichi

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    N2 - This work presents diurnal variations of gas- and particle-phase dicarbonyls (glyoxal (Gly) and methylglyoxal (Mgly)) in the atmosphere, which are important compounds that contribute to the formation and growth of atmospheric particulate matter. To obtain variations in partitioning, continuous collection of gaseous dicarbonyls was performed using a parallel plate wet denuder, and at the same time, the dicarbonyls in particle were collected using a spray-type particle collector downstream. Hourly samples were analyzed by high performance liquid chromatography-electrospray ionization-tandem mass spectrometry. This method is advantageous to monitor the gaseous and particulate carbonyls separately without loss during sampling. Sampling was performed in summer and winter in a midsize city (Kumamoto, Japan). The concentrations of the dicarbonyls increased in the summer daytime, which suggests that they are mostly formed by secondary production in the local atmosphere. The dicarbonyls and formaldehyde (HCHO) were found in both gas and particle phases, and partitioning to the particle phase was highest for Gly, followed by Mgly and HCHO. It was observed that the compounds moved to the particle phase in the midnight and early morning hours according to the growth of hygroscopic aerosols in summer. The particle/gas ratio also increased in the presence of high PM2.5, which is transported from the Chinese Continent in winter. The dicarbonyls were also observed on Mt. Fuji (3776 m) in the free troposphere. From back trajectory data and information on volatile organic compounds, they were most likely produced from relatively long-lifetime organic compounds from the Chinese Continent and biogenic volatile organic compounds emitted in the Japan Alps mountain range. Higher particle/gas ratios at the Mt. Fuji station indicate that low temperatures and high humidity precede the partition. The estimated effective Henry's law constants for the dicarbonyls, 108 order in mol/kgH2O/atm for summer data, were much higher than those for ideal liquid/vapor equilibrium but close to reported results obtained by chamber experiments. In the proposed method, oligomers in particle were also counted as the compounds. The dicarbonyl compounds existed up to submolar levels in real atmospheric aerosols, which suggests they undergo further reactions in the particle phase.

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