Atmospheric Chemistry and Physics Discussions
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10.5194/acpd-10-7185-2010
http://www.atmos-chem-phys-discuss.net/10/7185/2010/
http://www.atmos-chem-phys-discuss.net/10/7185/2010/acpd-10-7185-2010.html
http://www.atmos-chem-phys-discuss.net/10/7185/2010/acpd-10-7185-2010.pdf
7185
7214
2010-03-17
HULIS in emissions of fresh rice straw burning and in ambient aerosols in the pearl river delta region, China
P. Lin
G. Engling
J. Z. Yu
chjianyu@ust.hk
Division of Environment, Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong, China
Research Center for Environmental Changes, Academia Sinica, Taipei, Taiwan
Department of Chemistry, Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong, China
Atmospheric Research Center, HKUST Fok Ying Tung Graduate School, Nansha, Guangzhou 511458, China
HUmic-LIke Substances (HULIS) are an abundant unresolved mixture of organic
compounds present in atmospheric samples. Biomass burning (BB) has been
recognized as an important primary source of HULIS, but measurements of
HULIS in various fresh BB particles are lacking. In this work, HULIS in
emissions of rice straw burning in a number of field and chamber experiments
was measured. The HULIS/OC ratio was 0.34±0.05 in μg/μgC,
showing small variance among emissions under different burning conditions.
The influence of BB on ambient HULIS levels was investigated by examining
the spatial and temporal variation of HULIS and other aerosol constituents
and interspecies relations in ambient PM<sub>2.5</sub> collected at an urban and a
suburban location in the Pearl River Delta (PRD), China over a period of one
year. The HULIS concentrations in the ambient PM<sub>2.5</sub> were significantly
higher in air masses originating from regions influenced by BB. Significant
correlations between HULIS and water-soluble K<sup>+</sup> concentrations at both
sites further support that BB was an important source of HULIS. HULIS also
correlated well with sulfate, oxalate, and oxidant (the sum of O<sub>3</sub> and
NO<sub>2</sub>). The HULIS/OC ratios in BB-influenced ambient aerosols (~0.6) were much higher than those in the fresh BB emissions (0.34), implying
that secondary formation was also an important source of HULIS in the
atmosphere. The annual average HULIS concentrations were 4.9 μg m<sup>−3</sup> at the urban site and 7.1 μg m<sup>−3</sup> at the suburban site
while the annual average concentrations of elemental carbon were
3.3 μg m<sup>−3</sup> and 2.4 μg m<sup>−3</sup>, respectively. The urban-suburban spatial
gradient of HULIS was opposite to that of elemental carbon, negating
vehicular emissions as a significant source of HULIS.
Allen, A. G. and Miguel, A. H.: Biomass burning in the Amazon: Characterization of the ionic component of aerosols generated from flaming and smoldering rainforest and Savannah, Environ. Sci. Technol., 29, 486–493, 1995.
Altieri, K. E., Seitzinger, S. P., Carlton, A. G., Turpin, B. J., Klein, G. C., and Marshall, A. G.: Oligomers formed through in-cloud methylglyoxal reactions: Chemical composition, properties, and mechanisms investigated by ultra-high resolution FT-ICR mass spectrometry, Atmos. Environ., 42, 1476–1490, 2008.
Andreae, M. O. and Merlet, P.: Emission of trace gases and aerosols from biomass burning, Global Biogeochem. Cy., 15(4), 955–966, 2001.
Bey, I., Jacob, D. J., Logan, J. A., and Yantosca, R. M.: Asian chemical outflow to the pacific in spring: Origins, pathways, and budgets, J. Geophys. Res., 116(D19), 23097–23113, 2001.
Cavalli, F., Facchini, M. C., Decesari, S., Mircea, M., Emblico, L., Fuzzi, S., Ceburnis, D., Yoon, Y. J., O'Dowd, C. D., Putaud, J.-P., and Dell'Acqua, A.: Advances in characterization of size-resolved organic matter in marine aerosol over the North Atlantic, J. Geophys. Res., 109, D24215, doi:10.1029/2004JD005137, 2004.
Chan, C. Y., Chan, L. Y., Zheng, Y. G., Harris, J. M., Oltmans, S. J., and Christopher, S.: Effects of 1997 Indonesian forest fires on tropospheric ozone enhancement, radiative forcing, and temperature change over the Hong Kong region, J. Geophys. Res., 106, 14875–14885, 2001.
Chen, X. and Yu, J. Z.: Measurement of organic mass to organic carbon ratio in ambient aerosol samples using a gravimetric technique in combination with chemical analysis, Atmos. Environ., 42, 8857–8864, 2007.
Dinar, E., Taraniuk, I., Graber, E. R., Katsman, S., Moise, T., Anttila, T., Mentel, T. F., and Rudich, Y.: Cloud Condensation Nuclei properties of model and atmospheric HULIS, Atmos. Chem. Phys., 6, 2465–2482, 2006.
Duarte, R., Santos, E., Pio, C. A., and Duarte, A. C.: Comparison of structural features of water-soluble organic matter from atmospheric aerosols with those of aquatic humic substances, Atmos. Environ., 41, 8100–8113, 2007.
D'Anna, B., Jammoul, A., George, C., Stemmler, K., Fahrni, S., Ammann, M., and Wisthaler, A.: Light-induced ozone depletion by humic acid films and submicron aerosol particles, J. Geophys. Res., 114, D12301, doi:10.1029/2008JD001237, 2009.
Echalar, F., Gaudichet, A., Cachier, H., and Artaxo P.: Aerosol emissions by tropical forest and savanna biomass burning: Characteristic trace elements and fluxes, Geophys. Res. Lett., 22(22), 3039–3042, 1995.
Engling, G., Lee, J. J., Tsai, Y. W., Lung, S. C., Chou, C. C.-K., and Chan C. Y.: Size-resolved anhydrosugar composition in smoke aerosol from controlled field burning of rice straw, Aerosol Sci. Technol., 43, 662–672, 2009.
Feczko, T., Puxbaum, H., Kasper-Giebl, A., Handler, M., Limbeck, A., Gelencser, A., Pio, C., Preunkert, S., and Legrand, M.: Determination of water and alkaline extractable atmospheric humic-like substances with the TU Vienna HULIS analyzer in samples from six background sites in Europe, J. Geophys. Res., 112, D23S10, doi:10.1029/2006JD008331, 2007.
Fermo, P., Piazzalunga, A., Tuccillo, F., Brambilla, L., Cazzuli, O., Vecchi, R., and Valli, G.: Analytical methods for quantificantion and characterization of HULIS (HUmic Like Substances) in atmospheric aerosol, European Aerosol Conference 2009, Karlsruhe, Germany, 6–11~September~2009, Abstract T022A18, 2009.
Gao, S., Hegg, D. A., Hobbs, P. V., Kirchstetter, T. W., Magi, B. I., and Sadilek, M.: Water-soluble organic components in aerosols associated with savanna fires in southern Africa: Identification, evolution, and distribution, J. Geophys. Res., 108(D13), 8491, doi:10.1029/2002JD002324, 2003.
Gelencser, A., Hoffe, A., Kiss, G., Tombacz, E., Kurdi, R., and Bencze, L.: In-situ formation of light-absorbing organic matter in cloud water, J. Atmos. Chem. 45, 25–33, 2003.
Graber, E. R. and Rudich, Y.: Atmospheric HULIS: How humic-like are they? A comprehensive and critical review, Atmos. Chem. Phys., 6, 729–753, 2006.
Gysel, M., Weingartner, E., Nyeki, S., Paulsen, D., Baltensperger, U., Galambos, I., and Kiss, G.: Hygroscopic properties of water-soluble matter and humic-like organics in atmospheric fine aerosol, Atmos. Chem. Phys., 4, 35–50, 2004.
Hagler, G. S. W., Bergin, M. H., Salmon, L. G., Yu, J. Z., Wan, E. C. H., Zheng, M., Zeng, L. M., Kiang, C. S., Zhang, Y. H., Lau, A. K. H., and Schauer, J. J.: Source areas and chemical composition of fine particulate matter in the Pearl River Delta region of China, Atmos. Environ., 40, 3802–3815.
Hays, M. D., Fine, P. M., Geron, C. D., Kleeman, M. J., and Gullett, B. K.: Open burning of agricultural biomass: Physical and chemical properties of particle-phase emissions, Atmos. Environ., 39, 6747–6764, 2005.
Hobbs, P. V., Sinha, P., Yokelson, R. J., Christian, T. J., Blake, D. R., Gao, S., Krichstetter, T. W., Novakov, T., and Pilewskie, P.: Evolution of gases and particles from a savanna fire in South Africa, J. Geophys. Res., 108(D13), 8485, doi:10.1029/2002JD002352, 2003.
Hoffer, A., Kiss, G., Blazsó, M., and Gelencsér, A.: Chemical characterization of humic-like substances (HULIS) formed from a lignin-type precursor in model cloud water, Geophys. Res. Lett., 31, L06115, doi:10.1029/2003GL018962, 2004.
Hoffer, A., Gelencsér, A., Guyon, P., Kiss, G., Schmid, O., Frank, G. P., Artaxo, P., and Andreae, M. O.: Optical properties of humic-like substances (HULIS) in biomass-burning aerosols, Atmos. Chem. Phys., 6, 3563–3570, 2006.
Holmes, B. J. and Petrucci, G. A.: Water-soluble oligomer formation from acid-catalyzed reactions of levoglucosan in proxies of atmospheric aqueous aerosols, Environ. Sci. Technol., 40, 4983–4989, 2006.
Holmes, B. J. and Petrucci, G. A.: Oligomerization of levoglucosan by Fenton chemistry in proxies of biomass burning aerosols, J. Atmos. Chem., 58, 151–166, 2007.
Huang, X. F., Yu, J. Z., He, L. Y., and Yuan, Z.: Water-soluble organic carbon and oxalate in aerosols at a coastal urban site in China: Size distribution characteristics, sources, and formation mechanisms, J. Geophys. Res., 111, D22212, doi:10.1029/2006JD007408, 2006.
Jang, M. S., Czoschke, N. M., Lee, S., and Kamens, R. M.: Heterogeneous atmospheric aerosol production by acid-catalyzed particle-phase reactions, Science, 298, 814–817, 2002.
Jang, M. S., Carroll, B., Chandramouli, B., and Kamens, R. M.: Particle growth by acid-catalyzed heterogeneous reactions of organic carbonyls on preexisting aerosols, Environ. Sci. Technol., 37, 3828–3837, 2003.
Kalberer, M., Paulsen, D., Sax, M., Steinbacher, M., Dommen, J., Prevot, A. S. H., Fisseha, R., Weingartner, E., Frankevich, V., Zenobi, R., and Baltensperger, U.: Identification of polymers as major components of atmospheric organic aerosols, Science, 303, 1659–1662, 2004.
Khalil, M. A. K. and Rasmussen, R. A.: Tracers of wood smoke, Atmos. Environ., 37, 1211–1222, 2003.
Kiss, G., Varga, B., Galambos, I., and Ganszky, I.: Characterization of water-soluble organic matter isolated from atmospheric fine aerosol. J. Geophys. Res., 107(D21), 8339, doi:10.1029/2001JD000603, 2002.
Krivácsy, Z., Kiss, G., Ceburnis, D., Jennings, G., Maenhaut, W., Salma, I., and Shooter, D.: Study of water-soluble atmospheric humic matter in urban and marine environments. Atmos. Res., 87, 1–12, 2008.
Lee, C. T., Lin, N. H., Hou, Y. H., and Chang, S. Y.: Humic-like substances in the transported biomass burning plume at Mt. Lulin in Taiwan, European Aerosol Conference 2009, Karlsruhe, Germany, 6–11~September~2009, Abstract T057A08, 2009.
Lemieux, P. M., Lutes, C. C., and Santoianni, D. A.: Emissions of organic air toxics from open burning: a comprehensive review, Prog. Energ. Combust., 30, 1–32, 2004.
Lin, P., Huang, X. F., He, L. Y., and Yu, J. Z.: Abundances and size distribution of HULIS in ambient aerosols at a rural site in South China, J. Aerosol Sci., 41, 74–87, doi:10.1016/j.jaerosci.2009.09.001, 2010.
Lukács, H., Gelencser, A., Hammer, S., Puxbaum, H., Pio, C., Legrand, M., Kasper-Giebl, A., Handler, M., Limbeck, A., Simpson, D., and Preunker, S.: Seasonal trends and possible sources of brown carbon based on 2-year aerosol measurements at six sites in Europe, J. Geophys. Res., 112, D23S18, doi:10.1029/2006JD008151, 2007.
Marion, T., Perros, P. E., Losno, R., and Steiner, E.: Ozone production in savanna and forested areas during the EXPRESSO experiment, J. Atmos. Chem., 38, 3–30, 2001.
Mayol-Bracero, O. L., Guyon, P., Graham, B., Roberts, G., Andreae, M. O., Decesari, S., Facchini, M. C., Fuzzi, S., and Artaxo, P.: Water-soluble organic compounds in biomass burning aerosols over Amazonia, 2, Apportionment of the chemical composition and importance of the polyacidic fraction, J. Geophys. Res., 107(D20), 8091, doi:10.1029/2001JD000522, 2002.
Mazzoleni L. R., Zielinska B., and Moosmüller, H.: Emissions of Levoglucosan, Methoxy Phenols, and Organic Acids from Prescribed Burns, Laboratory Combustion of Wildland Fuels, and Residential Wood Combustion, Environ. Sci. Technol., 41, 2115–2122, 2007.
McKeen, S. A., Wotawa, G., Parrish, D. D., Holloway, J. S., Buhr, M. P., Hubler, G., Fehsenfeld, F. C., and Maegher, J. F.: Ozone production from Canadian wildfires during June and July of 1995, J. Geophys. Res., 107(D14), 4192, doi:10.1029/2001JD000697, 2002.
McMeeking, G. R., Kreidenweis, S. M., Baker, S., Carrico, C. M., Chow, J. C., Collett Jr., J. L., Hao, W. M., Holden, A. S., Kirchstetter, T. W., Malm, W. C., Moosmuller, H., Sullivan, A. P., and Wold, C. E.: Emissions of trace gases and aerosols during the open combustion of biomass in the laboratory, J. Geophys. Res., 114, D19210, doi:10.1029/2009JD011836, 2009.
Moonshine, M., Rudich, Y., Katsman, S., and Graber, E. R.: Atmospheric HULIS enhance pollutant degradation by promoting the dark Fenton reaction, Geophys. Res. Lett., 35, L20807, doi:10.1029/2008GL035285, 2008.
Mukai, H. and Ambe, Y., Characterization of a humic acid-like brown substance in airborne particulate matter and tentative identification of its origin, Atmos. Environ., 20, 813–819, 1986.
Nguyen, B., Mihalopoulos, N., and Putaud, J.-P.: Rice straw burning in Southeast Asia as a source of CO and COS to the atmosphere, J. Geophys. Res., 99, 16435–16439, 1994.
Rogers, F. C., Hudson, J. G., Zielinska, B., Tanner, R. L., Hallett, J., and Watson, J. G.: Cloud condensation nuclei from Biomass Burning, in: Global Biomass Burning: Atmospheric, Climatic and Biospheric Implications, edited by: Levine, J. S., MIT Press, Cambridge, England, 431–438, 1991.
Samburova, V., Szidat, S., Hueglin, C., Fisseha, R., Baltensperger, U., Zenobi, R., and Kalberer, M.: Seasonal variation of high-molecular-weight compounds in the water-soluble fraction of organic urban aerosols, J. Geophys. Res., 110, D23210, doi:10.1029/2005JD005910, 2005.
Sannigrahi, P., Sullivan, A. P., Weber, R. J., and Ingall, E. D.: Characterization of Water-Soluble Organic Carbon in Urban Atmospheric Aerosols Using Solid-State $^13$C NMR Spectroscopy, Environ. Sci. Technol., 40, 666–672, 2006.
Simoneit, B. R. T.: Biomass burning-a review of organic tracers for smoke from incomplete combustion, Appl. Geochem., 17, 129–162, 2002.
Streets, D. G., Yarber, K. F., Woo, J. H., and Carmichael, G. R.: Biomass burning in Asia: annual and seasonal estimates and atmospheric emissions, Global Biogeochem. Cy., 17(4), 1099, doi:10.1029/2003GB002040, 2003.
Thompson, A. M., Witte, J. C., Hudson, R. D., Guo, H., Herman, J. R., and Fujiwara, M.: Tropical tropospheric ozone and biomass burning, Science, 291, 2128–2132, 2001.
Wai, K. M., Lin, N.-H., Wang, S.-H., and Dokiya, Y.: Rainwater chemistry at a high-altitude station, Mt. Lulin, Taiwan: Comparison with a background station, Mt. Fuji, J. Geophys. Res., 113, D06305, doi:10.1029/2006JD008248, 2008.
Yang, H., Yu, J. Z., Ho, S. S. H., Xu, J., Wu, W. S., Wan, C. H., Wang, X. D., Wang, X. R., and Wang, L. S.: The chemical composition of inorganic and carbonaceous materials in PM$_2.5$ in Nanjing, China, Atmos. Environ., 39, 3735–3749, 2005.
Yu, J. Z., Tung, J. W. T., Wu, A. W. M., Lau, A. K. H., Louie, P. K. K., and Fung, J. C. H.: Abundance and seasonal characteristics of elemental and organic carbon in Hong Kong PM$_10$, Atmos. Environ., 38, 1511–1521, 2004a.
Yu, J. Z., Yang, H., Zhang, H. Y., and Lau, A. K. H.: Size distributions of water-soluble organic carbon in ambient aerosols and its size-resolved thermal characteristics, Atmos. Environ., 38, 1061–1071, 2004b.
Yu, J. Z., Huang, X. F., Xu, J. H., and Hu, M.: When aerosol sulfate goes up, so does oxalate: Implication for the formation mechanism of oxalate, Environ. Sci. Technol., 39, 128–133, 2005.
Yuan, Z. B., Lau, A. K. H.,Zhang, H. Y., Yu, J. Z., Louie, P. K. K., and Fung, J. C. H.: Identification and spatial distribution of dominant sources of PM$_10$ in Hong Kong, Atmos. Environ., 40, 1803–1815, 2006.
Zappoli, S., Andracchio, A., Fuzzi, S., Facchini, M. C., Gelencser, A., Kiss, G., Krivacsy, Z., Molnar, A., Meszaros, E., Hansson, H. C., Rosman, K., and Zebuhr, Y.: Inorganic, organic and macromolecular components of fine aerosol in different areas of Europe in relation to their water solubility, Atmos. Environ., 33, 2733–2743, 1999.
Zheng, M., Hagler, G. S. W., Ke, L., Bergin, M. H., Wang, F., Louie, P. K. K., Salmon, L., Sin, D. W. M., Yu, J. Z., and Schauer, J. J.: Composition and sources of carbonaceous aerosols at three contrasting sites in Hong Kong, J. Geophys. Res., 111, D20313, doi:10.1029/2006JD007074, 2006.