Characteristics, seasonality and sources of carbonaceous and ionic components in the tropical aerosols from Indian region

Copernicus GmbH - Tập 11 Số 15 - Trang 8215-8230
Chandra Mouli Pavuluri1, Kimitaka Kawamura1, Shankar G. Aggarwal1,2, T. Swaminathan3
1Institute of Low Temperature Science, Hokkaido University, N19 W8, Kita-Ku, Sapporo 060-0819, Japan
2National Physical Laboratory, Council of Scientific and Industrial Research, Dr. K.S. Krishnan Road, New Delhi 110012, India
3Department of Chemical Engineering, Indian Institute of Technology Madras, Chennai 600036, India

Tóm tắt

Abstract. To better characterize the tropical aerosols in Indian region, PM10 samples collected from Chennai, India (13.04° N; 80.17° E) were analyzed for carbonaceous and water-soluble ionic components. Concentration ranges of elemental carbon (EC) and organic carbon (OC) were 2.4–14 μg m−3 (ave. 6.5 μg m−3) and 3.2–15.6 μg m−3 (ave. 9.1 μg m−3) in winter samples whereas they were 1.1–2.5 μg m−3 (ave. 1.6 μg m−3) and 4.1–17.6 μg m−3 (ave. 9.7 μg m−3) in summer samples, respectively. Concentration of secondary organic carbon (SOC) retrieved from EC-tracer method was 4.6±2.8 μg m−3 in winter and 4.3±2.8 μg m−3 in summer. OC accounted for 38.5±14 % (n = 49) of combined concentrations of carbonaceous and ionic components in PM10. We also found that OC concentrations are generally higher than those of SO42− (8.8±2.5 μg m−3 and 4.1±2.7 μg m−3 in winter and summer, respectively), which was the most abundant ionic species (57 %) followed by NH4+ (15 %) >NO3−>Cl−>K+>Na+> Ca2+>MSA−>Mg2+. The mass fractions of EC, organic matter (OM) and ionic species varied seasonally, following the air mass trajectories and corresponding source strength. Based on mass concentration ratios of selected components and relations of EC and OC to marker species, we found that biofuel/biomass burning is a major source of atmospheric aerosols in South and Southeast Asia. The high concentrations of SOC and WSOC/OC ratios (ave. 0.45; n = 49) as well as good correlations between SOC and WSOC suggest that the secondary production of organic aerosols during long-range atmospheric transport is also significant in this region. This study provides the baseline data of carbonaceous aerosols for southern part of the Indian subcontinent.

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Ackerman, A. S., Toon, O. B., Stevens, D. E., Heymsfield, A. J., Ramanathan, V., and Welton, E. J.: Reduction of tropical cloudiness by soot, Science, 288, 1042–1047, 2000.

Aggarwal, S. G. and Kawamura, K.: Molecular distributions and stable carbon isotopic compositions of dicarboxylic acids and related compounds in aerosols from Sapporo, Japan: implications for photochemical aging during long-range atmospheric transport, J. Geophys. Res., 113, D14301, https://doi.org/10.1029/2007JD009365, 2008.

Aggarwal, S. G. and Kawamura, K.: Carbonaceous and inorganic composition in long-range transported aerosols over northern Japan: implication for aging of water-soluble organic fraction, Atmos. Environ., 43, 2532–2540, 2009.

Ali-Mohamed, A. Y.: Estimation of inorganic particulate matter in the atmosphere of Isa town, Bahrain, by dry deposition, Atmos. Environ., 25B, 397–405, 1991.

Andreae, M. O.: Soot carbon and excess fine potassium: long-range transport of combustion-derived aerosols, Science, 220, 1148–1151, 1983.

Andreae, M. O. and Merlet, P.: Emission of trace gases and aerosols from biomass burning, Global Biogeochem. Cy., 15, 955–966, 2001.

Babu, S. S. and Moorthy, K. K.: Aerosol black carbon over a tropical coastal station in India, Geophys. Res. Lett., 29(23), 2098, https://doi.org/10.1029/2002GL015662, 2002.

Babu, S. S., Satheesh, S. K., and Moorthy, K. K.: Aerosol radiative forcing due to enhanced black carbon at an urban site in India, Geophys. Res. Lett., 29(18), 1880, https://doi.org/10.1029/2002GL015826, 2002.

Cao, J. J., Lee, S. C., Ho, K. F., Zhang, X. Y., Zou, S. C., Fung, K., Chow, J. C., and Watson, J. G.: Characteristics of carbonaceous aerosol in Pearl River Delta region, China during 2001 winter period, Atmos. Environ., 37, 1451–1460, 2003.

Carrico, C. M., Bergin, M. H., Shrestha, A. B., Dibb, J. E., Gomes, L., and Harris, J. M.: The importance of carbon and mineral dust to seasonal aerosol properties in the Nepal Himalaya, Atmos. Environ., 37, 2811–2824, 2003.

Castro, L. M., Pio, C. A., Harrison, R. M., and Smith, D. J. T.: Carbonaceous aerosol in urban and rural European atmosphere: estimation of secondary organic carbon concentrations, Atmos. Environ., 33, 2771–2781, 1999.

Cavalli, F., C. Facchini, S. Decesari, M. Mircea, L. Emblico, S. Fuzzi, D. Ceburnis, Y. J. Yoon, C. D. O'Dowd, J.-P. Putaud, and Dell'Acqua, A.: Advances in characterization of size-resolved organic matter in marine aerosol over the North Atlantic, J. Geophys. Res., 109, D24215, https://doi.org/10.1029/2004JD005137, 2004.

Chow, J. C., Watson, J. G., Fujita, E. M., Lu, Z., and Lawson, D. R.: Temporal and spatial variations of PM2.5 and PM10 aerosols in the Southern California air quality study, Atmos. Environ., 28, 2061–2080, 1994.

Fu, P. Q., Kawamura, K., Pavuluri, C. M., Swaminathan, T., and Chen, J.: Molecular characterization of urban organic aerosol in tropical India: contributions of primary emissions and secondary photooxidation, Atmos., Chem. Phys., 10, 2663–2689, https://doi.org/10.5194/acp-10-2663-2010, 2010.

Garg, A., Bhattacharya, S., Shukla, P. R., and Dadhwal, V. K.: Regional and sectoral assessment of greenhouse gas emissions in India, Atmos. Environ., 35, 2679–2695, 2001.

Gillies, J. A., Gertler, A. W., Sagebiel, J. C., and Dippel, W. A.: On-road particulate matter (PM2.5 and PM10) emissions in the Sepulveda tunnel, Los Angels, California, Environ. Sci. Technol., 35, 1054–1063, 2001.

Guazzotti, S. A., Suess, D. T., Coffee, K. R., Quinn, P. K., Bates, T. S., Wisthler, A., Hansel, A., Ball., W. P., Dickerson, R. R., Neusü{ß}, C., Crutzen, P. J., and Prather, K. A.: Characterization of carbonaceous aerosols outflow from India and Arabia: biomass/biofuel burning and fossil fuel combustion, J. Geophys. Res., 108(D15), 4485, https://doi.org/10.1029/2002JD003277, 2003.

Gustafsson, Ö., Krusa, M., Zencak, Z., Sheesley, R. J., Granat, L., Engstöm, E., Praveen, P. S., Rao, P. S. P., Leck, C., and Rodhe, H.: Brown clouds over South Asia: biomass or fossil fuel combustion?, Science, 323, 495–498, 2009.

Habib, G., Venkataraman, C., Bond, T. C., and Schauer, J. J.: Chemical, microphysical and optical properties of primary particles from the combustion of biomass fuels, Environ. Sci. Technol., 42, 8829–8834, 2008.

Hara, K., Osada, K., Kido, M., Hayashi, M., Matsunaga, K., Iwasaka, Y., Yamanouchi, T., Hashida, G., and Fukatsu, T.: Chemistry of sea-salt particles and inorganic halogen species in Antarctic regions: compositional differences between coastal and inland stations, J. Geophys. Res., 109, D20208, https://doi.org/10.1029/2004JD004713, 2004.

Heywood, J. M. and Ramaswamy, V.: Global sensitivity studies of the direct radiative forcing due to anthropogenic sulfate and black carbon aerosols, J. Geophys. Res., 103(D6), 6043–6058, 1998.

Jacobson, M. Z.: Strong radiative heating due to the mixing of black carbon in atmospheric aerosols, Nature, 409, 695–697, 2001.

Kanakidou, M., Seinfeld, J. H., Pandis, S. N., Barnes, I., Dentener, F. J., Facchini, M. C., Van Dingenen, R., Ervens, B., Nenes, A., Nielsen, C. J., Swietlicki, E., Putaud, J. P., Balkanski, Y., Fuzzi, S., Horth, J., Moortgat, G. K., Winterhalter, R., Myhre, C. E. L., Tsigaridis, K., Vignati, E., Stephanou, E. G., and Wilson, J.: Organic aerosol and global climate modelling: a review, Atmos. Chem. Phys., 5, 1053–1123, https://doi.org/10.5194/acp-5-1053-2005, 2005.

Kawamura, K. and Usukura, K.: Distributions of low molecular weight dicarboxylic acids in the North Pacific aerosol samples, J. Oceanogr., 49, 271–283, 1993.

Keene, W. C., Lobert, J. M., Crutzen, P. J., Maben, J. R., Scharffe, D. H., Landmann, T., Hely, C., and Brain, C.: Emissions of major gaseous and particulate species during experimental burns of southern African biomass, J. Geophys. Res., 111, D04301, https://doi.org/10.1029/2005JD006319, 2006.

Khemani, L. T., Momin, G. A., Naik, M. S., Kumar, R. V., and Murthy, B. H. V. R.: Chemical composition and size distribution of atmospheric aerosols over the Deccan Plateau, India, Tellus, 34, 151–158, 1982.

Kiehl, J. T. and Briegleb, B. P.: The relative roles of sulfate aerosols and greenhouse gases in climate forcing, Science, 260, 311–314, 1993.

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, https://doi.org/10.1029/2001JD000603, 2002.

Kondo, Y., Miyazaki, Y., Takegawa, N., Miyakawa, T., Weber, R. J., Jimenez, J. L., Zhang, Q., and Worsnop, D. R.: Oxygenated and water-soluble organic aerosols in Tokyo, J. Geophys. Res., 112, D01203, https://doi.org/10.1029/2006JD007056, 2007.

Latha, K. M. and Badrinath, K. V. S.: Black carbon aerosols over tropical urban environment-a case study, Atmos. Res., 69, 125–133, 2003.

Lelieveld, J., Crutzen, P. J., Ramanathan, V., Andreae, M. O., Brenninkmeijer, C. A. M., Campos, T., Cass, G. R., Dickerson, R. R., Fischer, H., de Gouw, J. A., Hansel, A., Jefferson, A., Kley, D., de Laat, A. T. J., Lal, S., Lawrence, M. G., Lobert, J. M., Mayol-Bracero, O. L., Mitra, A. P., Novakov, T., Oltmans, S. J., Prather, K. A., Reiner, T., Rodhe, H., Scheeren, H. A., Sikka, D., and Williams, J.: The Indian Ocean experiment: widespread air pollution from South and Southeast Asia, Science, 291, 1031–1036, 2001.

Lim, H.-J. and Turpin, B. J.: Origins of primary and secondary organic aerosol in Atlanta: results of time-resolved measurements during the Atlanta supersite experiment, Environ. Sci. Technol., 36, 4489–4496, 2002.

Lu, R. and Turco, R. P.: Air pollutant transport in a coastal environment. Part I: two-dimensional simulations of sea-breeze and mountain effects, J. Atmos. Sci., 51(15), 2285–2308, 1994.

Mayol-Bracero, O. L., Gabriel, R., Andreae, M. O., Kirchstetter, T. W., Novakov, T., Ogren, J., Sheridan, P., and Streets, D. G.: Carbonaceous aerosols over the Indian Ocean during the Indian Ocean Experiement (INDOEX): chemical characterization, optical properties, and probable sources, J. Geophys. Res., 107(D19), 8030, https://doi.org/10.1029/2000JD000039, 2002.

Meinardi, S., Simpson, I. J., Blake, N. J., Blake, D. R., and Rowland, F. S.: Dimethyl disulfide (DMDS) and dimethyl sulfide (DMS) emissions from biomass burning in Australia, Geophys. Res. Lett., 30(9), 1454, https://doi.org/10.1029/2003GL016967, 2003.

Menon, S., Hansen, J., Nazarenko, L., and Luo, Y.: Climate effects of black carbon aerosols in China and India, Science, 297, 2250–2253, 2002.

Miller, S. T. K., Keim, B. D., Talbot, R. W., and Mao, H.: Sea breeze: structure, forecasting, and impacts, Rev. Geophys., 41(3), 1011, https://doi.org/10.1029/2003RG000124, 2003.

Miyazaki, Y., Kondo, Y., Takegawa, N., Komazaki, Y., Fukuda, M., Kawamura, K., Mochida, M., Okuzawa, K., and Weber, R. J.: Time-resolved measurements of water-soluble organic carbon in Tokyo, J. Geophys. Res., 111, D23206, https://doi.org/10.1029/2006JD007125, 2006.

Miyazaki, Y., Aggarwal, S. G., Singh, K., Gupta, P. K., and Kawamura, K.: Dicarboxylic acids and water-soluble organic carbon in aerosols in New Delhi, India in winter: Characteristics and formation processes, J. Geophys. Res., 114, D19206, https://doi.org/10.1029/2009JD011790, 2009.

Mouli, P. C., Mohan, S. V., and Reddy, S. J.: Chemical composition of atmospheric aerosol (PM10) at asemi-arid urban site: influence of terrestrial sources, Environ. Monitor. Assess., 117, 291–305, 2006.

Negi, B. S., Sadasivan, S., and Mishra, U. C.: Aerosol composition and sources in urban areas in India, Atmos. Environ., 21, 1259–1266, 1987.

Novakov, T., Andreae, M. O., Gabriel, R., Kirchstetter, T. W., Mayol-Bracero, O. L., and Ramanathan, V.: Origin of carbonaceous aerosols over the tropical Indian Ocean: biomass burning or fossil fuels?, Geophys. Res. Lett., 27(24), 4061–4064, 2000.

Olivier, J. G. J., Bouwman, A. F., Van der Hoek, K. W., and Berdowski, J. J. M.: Global air emission inventories for anthropogenic sources of NO$_{\\rm x}$, NH3 and N2O in 1990, Environ. Pollut., 102(S1), 135–148, 1998.

Padhy, P. K. and Varshney, C. K.: Emission of volatile organic compounds (VOC) from tropical plant species in India, Chemosphere, 59, 1643–1653, 2005.

Parmar, R. S., Satsangi, G. S., Kumari, M., Lakhani, A., Srivastava, S. S., and Prakash, S.: Study of size distribution of atmospheric aerosol at agra, Atmos. Environ., 35, 693–702, 2001.

Pavuluri, C. M., Kawamura, K., and Swaminathan,T.: Water-soluble organic carbon, dicarboxylic acids, ketoacids and α-dicarbonyls in the tropical Indian aerosols, J. Geophys., Res., 115, D11302, https://doi.org/10.2019/2009JD012661, 2010a.

Pavuluri, C. M., Kawamura, K., Tachibana, E., and Swaminathan, T.: Elevated nitrogen isotope ratios of tropical Indian aerosols from Chennai: implication for the origins of aerosol nitrogen in South and Southeast Asia, Atmos. Environ., 44, 3597–3604, 2010b.

Ram, K., Sarin, M. M., and Hegde, P.: Atmospheric abundances of primary and secondary carbonaceous species at two high-altitude sites in India: sources and temporal variability, Atmos. Environ., 42, 6785–6796, 2008.

Ram, K., Sarin, M. M., and Tripathi, S. N.: A 1 year record of carbonaceous aerosols from urban site in the Indo-Gangetic plain: characterization, sources and temporal variability, J. Geophys. Res., Res., 115, D24313, https://doi.org/10.1029/2010JD014188, 2010.

Ramanathan, V., Crutzen, P. J., Kiehl, J. T., and Rosenfeld, D.: Aerosols, Climate, and the hydrological cycle, Science, 294, 2119–2124, 2001.

Reddy, M. S. and Venkataraman, C.: Inventory of aerosol and sulphur dioxide emissions from India: I-fossil fuel combustion, Atmos. Environ., 36, 677–697, 2002a.

Reddy, M. S. and Venkataraman, C.: Inventory of aerosol and sulphur dioxide emissions from India. Part II – biomass combustion, Atmos. Environ., 36, 699–712, 2002b.

Rengarajan, R., Sarin, M. M., and Sudheer, A. K.: Carbonaceous and inorganic species in atmospheric aerosols during wintertime over urban and high-altitude sites in North India, J. Geophys. Res., 112, D21307, https://doi.org/10.1029/2006JD008150, 2007.

Salam, A., Bauer, H., Kassin, K., Ullah, S. M., and Puxbaum, H.: Aerosol chemical characteristics of a mega-city in Southeast Asia (Dhaka-Bangladesh), Atmos. Environ., 37, 2517–2528, 2003.

Satheesh, S. K. and Ramanathan, V.: Large differences in tropical aerosol forcing at the top of the atmosphere and Earth's surface, Nature, 405, 60–63, 2000.

Saxena, P. and Hildemann, L. M.: Water-soluble organics in atmospheric particles: a critical review of the literature and application of thermodynamics to identify candidate compounds, J. Atmos. Chem., 24, 57–109, 1996.

Saxena, P., Hildemann, L. M., McMurry, P. H., and Seinfeld, J. H.: Organics alter hygroscopic behavior of atmospheric particles, J. Geophys. Res., 100(D9), 18755–18770, 1995.

Sharma, V. K. and Patil, R. S.: Size distribution of atmospheric aerosol and their source identification using factor analysis in Bombay, India, Atmos. Environ., 26, 135–141, 1992.

Sillanpää, M., Frey, A., Hillamo, R., Pennanen, A. S., and Salonen, R. O.: Organic, elemental and organic carbon in particulate of six urban environments in Europe, Atmos. Chem. Phys., 5, 2869–2879, https://doi.org/10.5194/acp-5-2869-2005, 2005.

Smith, D. J. T., Harrison, R. M., Luhana, L., Pio, C. A., Castro, L. M., Tariq, M. N., Hayat, S., and Quraishi, T.: Concentrations of particulate airborne polycyclic aromatic hydrocarbons and metals collected in Lahore, Pakistan, Atmos. Environ., 30(23), 4031–4040, 1996.

Srinivas, C. V., Venkatesan, R., Somayaji, K. M., and Singh, A. B.: A numerical study of sea breeze circulation observed at a tropical site Kalpakkam on the east coast of Inda under different synoptic flow situations, J. Earth Syst. Sci., 115(5), 557–574, 2006.

Srinivas, C. V., Venkatesan, R., and Singh, A. B.: Sensitivity of mesoscale simulations of land-sea breeze to boundary layer turbulence parameterization, Atmos. Environ., 41, 2534–2548, 2007.

Stone, E. A., Schauer, J. J., Pradhan, B. B., Dangol, P. M., Habib, G., Venkataraman, C., and Ramanathan, V.: Characterization of emissions from South Asian biofuels and application to source apportionment of carbonaceous aerosol in the Himalayas, J. Geophys. Res., 115, D06301, https://doi.org/10.1029/2009JD011881, 2010.

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, https://doi.org/10.1029/2003GB002040, 2003.

Sudheer, A. K. and Sarin, M. M.: Carbonaceous aerosols in MABL of Bay of Bengal: influence of continental outflow, Atmos. Environ., 42, 4089–4100, 2008.

Sun, J. and Ariya, P. A.: Atmospheric organic and bio-aerosols as cloud condensation nuclei (CCN): a review, Atmos. Environ., 40, 795–820, 2006.

Tata Energy Research Institute, Tata energy directory and data yearbook 1996–1997, New Delhi, India, 1997.

Turpin, B. J. and Huntzicker, J. J.: Identification of secondary organic aerosol episodes and quantification of primary and secondary organic aerosol concentrations during SCAQS, Atmos. Environ., 29(23), 3527–3544, 1995.

Venkataraman, C., Reddy, C. K., Josson, S., and Reddy, M. S.: Aerosol size and chemical characteristics at Mumbai, India, during the INDOEX-IFP (1999), Atmos. Environ., 36, 1979–1991, 2002.

Venkataraman, C., Habib, G., Eiguren-Fernandez, A., Miguel, A. H., and Friedlander, S. K.: Residential biofuels in South Asia: carbonaceous aerosol emissions and climate impacts, Science, 307, 1454–1456, 2005.

von Glasow, R. and Crutzen, P. J.: Model study of multiphase DMS oxidation with a focus on halogens, Atmos. Chem. Phys., 4, 589–608, https://doi.org/10.5194/acp-4-589-2004, 2004.

Wang, H., Kawamura, K., and Shooter, D.: Carbonaceous and ionic components in wintertime atmospheric aerosols from two New Zealand cities: implications for solid fuel combustion, Atmos. Environ., 39, 5865–5875, 2005.

Watson, J. G., Chow, J., and Houk, J. E.: PM2.5 source profile for vehicle exhaust, vegetative burning, geological material, and coal burning in Northwestern Colorado during 1995, Chemosphere, 43, 1141–1151, 2001.

World Bank: World development report 1999/2000: entering into the 21st century, Washington, DC, USA, 2000.

Yamasoe, M. A., Artaxo, P., Miguel, A. H., and Allen, A. G.: Chemical composition of aerosol particles from direct emissions of vegetation fires in the Amazon Basin: water-soluble species and trace elements, Atmos. Environ., 34, 1641–1653, 2000.

Yang, H., Xu, J., Wu, W.-S., Wan, C. H., and Yu, J. Z.: Chemical characterization of water-soluble organic aerosols at Jeju Island collected during ACE-Asia, Environ. Chem., 1, 13–17, https://doi.org/10.1071/EN04006, 2004.

Yang, H., Yu, J. Z., Ho, S. S. H., Xu, J., Wu, W.-S., Wan, C. H., Wang, X., Wang, X., and Wang, L.: The chemical composition of inorganic and carbonaceous materials in PM2.5 in Nanjing, China, Atmos. Environ., 39, 3735–3749, 2005.

Yu, S., Dennis, R. L., Bhave, P. V., and Eder, B. K.: Primary and secondary organic aerosols over the United States: estimates on the basis of observed organic carbon (OC) and elemental carbon (EC), and air quality modeled primary OC/EC ratios, Atmos. Environ., 38, 5257–5268, 2004.