Distributions and diurnal changes of low molecular weight organic acids and ^|^alpha;-dicarbonyls in suburban aerosols collected at Mangshan, North China

He, Nannan; Kawamura, Kimitaka

doi:10.2343/geochemj.1.0093

Cited by 24 publications

(16 citation statements)

References 28 publications

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“…These observations are consistent with the diurnal distributions of glyoxylic acid in the time-resolved aerosols from Tokyo, whose concentrations showed a positive correlation with ambient temperature and ozone (Kawamura and Yasui, 2005). In the late afternoon or night to early morning, when relative humidity increases, ωC 2 can be oxidized to oxalic acid possibly in the aerosol aqueous phase (Warneck, 2003;Miyazaki et al, 2009;He and Kawamura, 2010).…”

Section: Compositional Changes Of Dicarboxylic Acidssupporting

confidence: 75%

High abundances of water-soluble dicarboxylic acids, ketocarboxylic acids and α-dicarbonyls in the mountaintop aerosols over the North China Plain during wheat burning season

et al. 2013

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Aerosol (TSP) samples were collected at the summit of Mount Tai (elevation: 1534 m a.s.l., 36.25° N, 117.10° E) located in the North China Plain using a high-volume air sampler and pre-combusted quartz filters. Sampling was conducted on day/night or 3 h basis in the period from 29 May to 28 June 2006 during the field burning of wheat straw residue and the post-burning season. The filter samples were analyzed for low-molecular-weight dicarboxylic acids, ketoacids and α-dicarbonyls using capillary gas chromatography (GC) and GC-MS employing water extraction and butyl ester derivatization. Molecular distributions of dicarboxylic acids (C₂-C₁₁, 220–6070 ng m⁻³) were characterized by a predominance of oxalic (C₂) acid (105–3920 ng m⁻³) followed by succinic (C₄) or malonic (C₃) acid. Unsaturated aliphatic diacids, including maleic (M), isomaleic (iM) and fumaric (F) acids, were also detected together with aromatic diacids (phthalic, isophthalic and terephthalic acids). ω-oxocarboxylic acids (C₂-C₉, 24–610 ng m⁻³) were detected as the second most abundant compound class with the predominance of glyoxylic acid (11–360 ng m⁻³), followed by α-ketoacid (pyruvic acid, 3–140 ng m⁻³) and α-dicarbonyls (glyoxal, 1–230 ng m⁻³ and methylglyoxal, 2–120 ng m⁻³). We found that these levels (>6000 ng m⁻³ for diacids) are several times higher than those reported in Chinese megacities at ground levels. The concentrations of diacids increased from late May to early June, showing a maximum on 7 June, and then significantly decreased during the period 8–11 June, when the wind direction shifted from southerly to northerly. Similar temporal trends were found for ketocarboxylic acids and α-dicarbonyls as well as total carbon (TC) and water-soluble organic carbon (WSOC). The temporal variations of water-soluble organics were interpreted by the direct emission from the field burning of agricultural wastes (wheat straw) in the North China Plain and the subsequent photochemical oxidation of volatile and semi-volatile organic precursors emitted from field burning as well as dark ozonolysis of volatile organic compounds and other organics, accretion reactions and oxidation of nonvolatile organics such as unsaturated fatty acids. This study demonstrates that the field burning of agricultural wastes in early summer strongly influenced the air quality of the free troposphere over the North China Plain

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Section: Compositional Changes Of Dicarboxylic Acidssupporting

confidence: 75%

High abundances of water-soluble dicarboxylic acids, ketocarboxylic acids and α-dicarbonyls in the mountaintop aerosols over the North China Plain during wheat burning season

et al. 2013

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“…Although the differences in the ratios are not significant, wetter conditions under strong solar radiation may enhance the photochemical aging of organic aerosols in the tropical atmosphere. Based on the filed experiments, aqueous aerosol phase production of oxalic acid was reported in urban and suburban sites (Miyazaki et al, 2009;He and Kawamura, 2010). However, when compared to literature values, our C 3 /C 4 ratios are slightly lower than those (1.5) reported in Tokyo (Kawamura and Ikushima, 1993) and 1.4 in Chennai but comparable to those (0.84) in Nainital, India (Hegde and Kawamura, 2012) and those (1.3) in Jeju Island in the East China Sea .…”

Section: Comparison Of Molecular Composition Of Diacids and Related Ccontrasting

confidence: 53%

Molecular composition of dicarboxylic acids, ketocarboxylic acids, α-dicarbonyls and fatty acids in atmospheric aerosols from Tanzania, East Africa during wet and dry seasons

Mkoma

Kawamura

2013

Atmos. Chem. Phys.

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Atmospheric aerosol samples of PM2.5 and PM10 were collected during the wet and dry seasons in 2011 from a rural site in Tanzania and analysed for water-soluble dicarboxylic acids, ketocarboxylic acids, α-dicarbonyls, and fatty acids using a gas chromatography/flame ionization detector (GC/FID) and GC/mass spectrometry. Here we report the molecular composition and sources of diacids and related compounds for wet and dry seasons. Oxalic acid (C2) was found as the most abundant diacid species followed by succinic and/or malonic acids whereas glyoxylic acid and glyoxal were the dominant ketoacid and α-dicarbonyl, respectively in both seasons in PM2.5 and PM10. Mean concentration of C2 in PM2.5 (121 ± 47 ng m−3) was lower in wet season than dry season (258 ± 69 ng m−3). Similarly, PM10 samples showed lower concentration of C2 (169 ± 42 ng m−3) in wet season than dry season (292 ± 165 ng m−3). Relative abundances of C2 in total diacids were 65% and 67% in PM2.5 and 65% and 64% in PM10 in the wet and dry seasons, respectively. Total concentrations of diacids (289–362 ng m−3), ketoacids (37.8–53.7 ng m−3), and α-dicarbonyls (5.7–7.8 ng m−3) in Tanzania are higher than those reported at a rural background site in Nylsvley (South Africa) but comparable or lower than those reported from sites in Asia and Europe. Diacids and ketoacids were found to be present mainly in PM2.5 in both seasons (total α-dicarbonyls in the dry season), suggesting a production of organic acids from pyrogenic sources and photochemical oxidations. Averaged contributions of total diacids to aerosol total carbon were 1.4% in PM2.5 and 2.1% in PM10 during wet season and 3.3% in PM2.5 and 3.9% in PM10 during dry season whereas those to water-soluble organic carbon were 2.2% and 4.7% in PM2.5 during wet season and 3.1% and 5.8% in PM10 during dry season. The higher ratios in dry season suggest an enhanced photochemical oxidation of organic precursors probably via heterogeneous reactions on aerosols under strong solar radiation. Strong positive correlations were found among diacids and related compounds as well as good relations to source tracers in both seasons, suggesting a mixed source from natural biogenic emissions, biomass burning, biofuel combustion, and photochemical production

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“…He and Kawamura (2010) have shown that nighttime observations of oxalic acid over polluted areas are about 1.3 times higher than the daytime ones. However, most of the data used for Fig.…”

Section: Comparison With Observationsmentioning

confidence: 99%

In-cloud oxalate formation in the global troposphere: a 3-D modeling study

et al. 2011

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Abstract. Organic acids attract increasing attention as contributors to atmospheric acidity, secondary organic aerosol mass and aerosol hygroscopicity. Oxalic acid is globally the most abundant dicarboxylic acid, formed via chemical oxidation of gas-phase precursors in the aqueous phase of aerosols and droplets. Its lifecycle and atmospheric global distribution remain highly uncertain and are the focus of this study. The first global spatial and temporal distribution of oxalate, simulated using a state-of-the-art aqueous-phase chemical scheme embedded within the global 3-dimensional chemistry/transport model TM4-ECPL, is here presented. The model accounts for comprehensive gas-phase chemistry and its coupling with major aerosol constituents (including secondary organic aerosol). Model results are consistent with ambient observations of oxalate at rural and remote locations (slope = 1.16 ± 0.14, r 2 = 0.36, N =114) and suggest that aqueous-phase chemistry contributes significantly to the global atmospheric burden of secondary organic aerosol. In TM4-ECPL most oxalate is formed in-cloud and less than 5 % is produced in aerosol water. About 62 % of the oxCorrespondence to: M. Kanakidou (mariak@chemistry.uoc.gr) alate is removed via wet deposition, 30 % by in-cloud reaction with hydroxyl radical, 4 % by in-cloud reaction with nitrate radical and 4 % by dry deposition. The in-cloud global oxalate net chemical production is calculated to be about 21-37 Tg yr −1 with almost 79 % originating from biogenic hydrocarbons, mainly isoprene. This condensed phase net source of oxalate in conjunction with a global mean turnover time against deposition of about 5 days, maintain oxalate's global tropospheric burden of 0.2-0.3 Tg, i.e. 0.05-0.1 Tg-C that is about 5-9 % of model-calculated water soluble organic carbon burden.

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Distributions and diurnal changes of low molecular weight organic acids and ^|^alpha;-dicarbonyls in suburban aerosols collected at Mangshan, North China

Cited by 24 publications

References 28 publications

High abundances of water-soluble dicarboxylic acids, ketocarboxylic acids and α-dicarbonyls in the mountaintop aerosols over the North China Plain during wheat burning season

High abundances of water-soluble dicarboxylic acids, ketocarboxylic acids and α-dicarbonyls in the mountaintop aerosols over the North China Plain during wheat burning season

Molecular composition of dicarboxylic acids, ketocarboxylic acids, α-dicarbonyls and fatty acids in atmospheric aerosols from Tanzania, East Africa during wet and dry seasons

In-cloud oxalate formation in the global troposphere: a 3-D modeling study

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