Abstract
Saturated n-dicarboxylic acids (C2-C7, C9), unsaturated dicarboxylic acids (maleic, fumaric, phthalic acid), ketocarboxylic acids (pyruvic, glyoxylic acid), and dicarbonyls (glyoxal, methylglyoxal) were determined in size-segregated samples with a high-volume Andersen air sampler at a suburban site in Saitama, Japan, May 12–17 and July 24–27, 2007 and January 22–31, 2008. The seasonal average concentrations of these detected organic acids were 670 ng/m3, accounting for about 4.4–5.7% (C/C) of water-soluble organic carbon (WSOC) and 2.3–3.6% (C/C) of organic carbon (OC). The most abundant species of dicarboxylic acids was oxalic acid, followed by malonic, phthalic, or succinic acids. Glyoxylic acid and methyglyoxal were most abundant ketocarboxylic acid and dicarbonyl, respectively. Seasonal differences, sizesegregated concentrations, and the correlations of these acids with ambient temperatures, oxidants, elemental carbon (EC), OC, WSOC, and ionic components were also discussed in terms of their corresponding sources and possible secondary formation pathways. The results suggested that photochemical reactions contributed more to the formation of particulate organic acids in Saitama suburban areas than did direct emissions from anthropogenic and natural sources. However, direct emissions of vehicles were also important sources of several organic acids in particles, such as phthalic and adipic acids, especially in winter.
References
Abbatt J.P.D., K. Broekhuizen, and P. Pradeep Kumar (2005) Cloud condensation nucleus activity of internally mixed ammonium sulfate/organic acid aerosol particles. Atmospheric Environment, 39(26), 4767–4778.
Blando J.D. and B.J. Turpin (2000) Secondary organic aerosol formation in cloud and fog droplets: a literature evaluation of plausibility. Atmospheric Environment, 34(10), 1623–1632.
Chebbi A. and P. Carlier (1996) Carboxylic acids in the troposphere, occurrence, sources, and sinks: a review. Atmospheric Environment, 30(24), 4233–4249.
Chow J.C. and J.G. Watson (2002) PM2.5 carbonate concentrations at regionally representative interagency monitoring of protected visual environment sites. Journal of Geophysical Research, 107(D21), 8344, doi: https://doi.org/10.1029/2001JD000574.
Cruz C.N. and S.N. Pandis (1998) The effect of organic coatings on the cloud condensation nuclei activation of inorganic atmospheric aerosol. Journal of Geophysical Research, 103(D11), 13111–13123.
Falkovich A.H., E.R. Graber, G. Schkolnik, Y. Rudich, W. Maenhaut, and P. Artaxo (2005) Low molecular weight organic acids in aerosol particles from Rondonia, Brazil, during the biomass-burning, transition and wet periods. Atmospheric Chemistry and Physics, 5, 781–797.
Graham B., O.L. Mayol-Bracero, P. Guyon, G.C. Roberts, S. Decesari, M.C. Facchini, P. Artaxo, W. Maenhaut, P. Koll, and M.O. Andreae (2002) Water-soluble organic compounds in biomass burning aerosols over Amazonia 1. Characterization by NMR and GC-MS. Journal of Geophysical Research, 107(D20), 1–15.
Hatakeyama S., M. Ohno, J. Weng, H. Takagi, and H. Akimoto (1987) Mechanism for the formation of gaseous and particulate products from ozone-cycloalkene reactions in air. Environmental Science and Technology, 21(1), 52–57.
Ho K.F., S.C. Lee, J.J. Cao, K. Kawamura, T. Watanabe, Y. Cheng, and J.C. Chow (2006) Dicarboxylic acids, ketocarboxylic acids and dicarbonyls in the urban roadside area of Hong Kong. Atmospheric Environment, 40(17), 3030–3040.
Hsieh L.Y., S.C. Kuo, C.L. Chen, and Y.I. Tsai (2007) Origin of low-molecular-weight dicarboxylic acids and their concentration and size distribution variation in suburban aerosol. Atmospheric Environment, 41(31), 6648–6661.
Jiang Z.W., Q.Y. Wang, K. Sekiguchi, and K. Sakamoto (2006) Investigation of variations in suspended particulate matter with enforcement of regulations on diesel vehicle exhaust in suburban Japan. JSME International Journal, 49(1), 2–7.
Jaffrezo J.L., G. Aymoz, C. Delaval, and J. Cozic (2005) Seasonal variations of the water soluble organic carbon mass fraction of aerosol in two valleys of the French Alps. Atmospheric Chemistry and Physics, 5, 3999–4036.
Kawamura K. (1993a) Identification of C2-C10 ω-Oxocarboxylic acids, pyruvic acid, and C2-C3 α-dicarbonyls in wet precipitation and aerosol samples by capillary GC and GC/MS. Anal. Chem., 65(23), 3505–3511.
Kawamura K. and K. Ikushima (1993b) Seasonal changes in the distribution of dicarboxylic acids in the urban atmosphere. Environmental Science and Technology, 27(10), 2227–2235.
Kawamura K., H. Kasukabe, and L.A. Barrie (1996) Source and reaction pathways of dicarboxylic acids, ketoacids and dicarbonyls in Arctic aerosols: one year of observations. Atmospheric Environment, 30, 1709–1722.
Kawamura K. and F. Sakaguchi (1999) Molecular distribution of water soluble dicarboxylic acids in marine aerosols over the Pacific Ocean including tropics. Journal of Geophysical Research, 104(D3), 3501–3509.
Kawamura K. and O. Yasuib (2005) Diurnal changes in the distribution of dicarboxylic acids, ketocarboxylic acids and dicarbonyls in the urban Tokyo atmosphere. Atmospheric Environment, 39(10), 1945–1960.
Kerminen V.-M., K. Teinila, R. Hillamo, and T. Makela (1999) Size-segregated chemistry of particulate dicarboxylic acids in the Arctic atmosphere. Atmospheric Environment, 33(13), 2089–2100.
Kerminen V.-M., C. Ojanen, T. Pakkanen, R. Hillamo, M. Aurela, and J. Merilaien (2000) Low-molecularweight dicarboxylic acids in an urban and rural atmosphere. Journal of Aerosol Science, 31(3), 349–362.
Limbeck A., H. Puxbaum, L. Otter, and M.C. Scholes (2001) Semivolatile behavior of dicarboxylic acids and other polar organic species at a rural background site (Nylsvley, RSA). Atmospheric Environment, 35(10), 1853–1862.
Li Y.C. and J.Z. Yu (2005) Simultaneous determination of mono and dicarboxylic acids, ω-oxo-carboxylic acids, midchain ketocarboxylic acids and aldehydes in atmospheric aerosol samples. Environmental Science and Technology, 39(19), 7616–7624.
Narukawa M., K. Kawamura, N. Takeuchi, and T. Nakajima (1999) Distribution of dicarboxylic acids and carbon isotopic compositions in aerosols from 1997 Indonesian forest fires. Geophysical Research Letters, 26(20), 3101–3104.
Ortiz R., H. Hagino, K. Sekiguchi, Q.Y. Wang, and K. Sakamoto (2006) Ambient air measurements of six bifunctional carbonyls in a suburban area. Atmospheric Research, 82, 709–718.
Peng C., M.N. Chan, and C.K. Chan (2001) The hygroscopic properties of dicarboxylic and multifunctional acids: measurements and UNIFAC predictions. Environmental Science and Technology, 35(22), 4495–4501.
Ray J. and S.R. McDow (2005) Dicarboxylic acid concentration trends and sampling artifacts. Atmospheric Environment, 39(40), 7906–7919.
Rohrl A. and G. Lammel (2001) Low-molecular weight dicarboxylic acids and glyoxylic acid: seasonal and air mass characteristics. Environmental Science and Technology, 35(1), 95–101.
Saxena P. and L.M. Hildemann (1996) Water-soluble organics in atmospheric particles: A critical review of the literature and application of thermodynamics to identify candidate compounds. Journal of Atmospheric Chemistry, 24(1), 57–109.
Wang G., S. Niu, C. Liu, and L. Wang (2002) Identification of dicarboxylic acids and aldehydes of PM10 and PM2.5 aerosols in Nanjing, China. Atmospheric Environment, 36(12), 1941–1950.
Yao X.H., M. Fang, and C.K. Chan (2002) Size distributions and formation of dicarboxylic acids in atmospheric particles. Atmospheric Environment, 36(13), 2099–2107.
Yu J.Z., J. Xu, and H. Yang (2002) Charring characteristics of atmospheric organic particulate matter in thermal analysis. Environmental Science and Technology, 36(4), 754–761.
Yu J.Z., X.-F. Huang, J. Xu, and M. Hu (2005) When aerosol sulfate goes up, so does oxalate: Implication for the formation mechanisms of oxalate. Environmental Science and Technology, 39(1), 128–133.
Acknowledgements
This work was supported in part by Grants-in-Aid from Saitama University.
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
Bao, L., Sakamoto, K. Chemical Characterization of Water-Soluble Organic Acids in Size-Segregated Particles at a Suburban Site in Saitama, Japan. Asian J. Atmos. Environ 3, 42–51 (2009). https://doi.org/10.1007/BF03654864
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/BF03654864