References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-10-5107-2010

Size distributions of elemental carbon and its contribution to light extinction in urban and rural locations in the pearl river delta region, China

¹ ² Wu

¹ ³ Wu

⁴ Yu

J. Z.

¹ ²

Division of Environment, Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong, China

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

Institute of Tropical and Marine Meteorology, China Meteorological Administration, Guangzhou 510080, China

08 06 2010

10 11 5107 5119

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Elemental carbon (EC) in size-segregated aerosol samples were determined at five urban, one suburban, and one rural locations in the Pearl River Delta region in South China during 2006–2008 period. The size modal characteristics of EC were different at the urban and suburban/rural locations. The urban EC had a dominant condensation mode with a mass median aerodynamic diameter (MMAD) in the 0.36–0.43 μm range and a slightly less abundant mode in the droplet mode size (MMAD: 0.8–1.1 μm), while the suburban/rural EC had a prominent mode in the droplet mode size (MMAD: 0.7–1.1 μm) and a minor condensation mode (MMAD: 0.22–0.33 μm). Calculations using Mie theory and the measured size distributions of EC, organic carbon, and major inorganic ions indicate that EC-containing particles contributed 76±20% of the observed light extinction at the urban sites. Among the EC-containing particles, EC mass alone contributed 21±11% of the observed light extinction while non-EC materials on the EC particles (i.e., organic matter, ammonium sulfate, and water) contributed 55±15%. At the suburban/rural locations, EC-containing particles contributed 37–48% of the measured light extinction, with EC mass contributing 4–10% and non-EC coating materials contributing the remaining light extinction. Our results suggest that EC-containing particles were important to the overall light extinction in the urban atmospheres due to their more abundant presence from vehicular emissions. The EC-containing particles in the suburban/rural locations had a reduced but still significant contribution to light extinction budget.

References 1

Andreae, M. O., Schmid, O., Yang, H., Chand, D., Yu, J. Z., Zeng, L. M., and Zhang, Y. H.: Optical properties and chemical composition of the atmospheric aerosol in urban Guangzhou, China, Atmos. Environ., 42, 6335–6350, 2008.

Bergin, M. H., Cass, G. R., Xu, J., Fang, C., Zeng, L. M., Yu, T., Salmon, L. G., Kiang, C. S., Tang, X. Y., Zhang, Y. H., and Chameides, W. L.: Aerosol radiative, physical, and chemical properties in Beijing during June 1999, J. Geophys. Res.-Atmos., 106(D16), 17969–17980, 2001.

Birch, M. E. and Cary, R. A.: Elemental carbon-based method for monitoring occupational exposures to particulate diesel exhaust, Aerosol Sci. Technol., 25, 221–241, 1996.

Bohren, C. F. and Huffman D. R.: Absorption and scattering of light by small particles, John Wiley, Hoboken, N. J., 1983.

Bond, T. C. and Bergstrom, R. W.: Light absorption by carbonaceous particles: An investigative review, Aerosol Sci. Technol., 40, 27–67, 2006.

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.

Cao, J. J., Lee, S. C., Ho, K. F., Zou, S. C., Fung, K., Li, Y., Watson, J. G., and Chow, J. C.: Spatial and seasonal variations of atmospheric organic carbon and elemental carbon in Pearl River Delta Region, China, Atmos. Environ., 38, 4447–4456, 2004.

Chang, W. L. and Koo, E.: A study of visibility trends in Hong Kong (1968–1982), Atmos. Environ., 20, 1847–1858, 1986.

Cheng, Y. F., Eichler, H., Wiedensohler, A., Heintzenberg, J., Zhang, Y. H., Hu, M., Herrmann, H., Zeng, L. M., Liu, S., Gnauk, T., Bruggemann, E., and He, L. Y.: Mixing state of elemental carbon and non-light-absorbing aerosol components derived from in situ particle optical properties at Xinken in Pearl River Delta of China, J. Geophys. Res., 111, D20204, doi:10.1029/2005JD006929, 2006.

Cheng, Y. F., Wiedensohler, A., Eichler, H., Su, H., Gnauk, T., Bruggemann, E., Herrmann, H., Heintzenberg, J., Slanina, J., Tuch, T., Hu, M., and Zhang, Y.H.: Aerosol optical properties and related chemical apportionment at Xinken in Pearl River Delta of China, Atmos. Environ., 42, 6351–6372, 2008.

China Meteorology Administration: Specifications for Surface Meteorological Observation, China Meteorological Press, 2003.

Chow, J. C., Watson, J. G., Louie, P. K. K., Chen, L.-W. A., and Sin, D.: Comparison of PM$_2.5$ carbon measurement methods in Hong Kong, China, Environ. Pollut., 137, 334–344, 2005.

Clegg, S. L., Brimblecombe, P., and Wexler, A. S.: A thermodynamic model of the system H$^+$-NH$_4^+$-SO$_4^2-$-NO$_3^-$-H<sub>2</sub>O at tropospheric temperatures, J. Phys. Chem. A, 102, 2137–2154, 1998.

Duan, J., Tan, J., Cheng, D., Bi, X., Deng, W., Sheng, G., Fu, J., and Wong, M.H.: Sources and characteristics of carbonaceous aerosol in two largest cities in Pearl River Delta Region, China, Atmos. Environ., 41, 2895–2903, 2007.

Dong, Y., Hays, M. D., Smith, N. D., and Kinsey, J. S.: Inverting cascade impactor data for size-resolved characterization of fine particulate source emissions, J. Aerosol. Sci., 35, 1497–1512, 2004.

Eldering, A., Cass, G. R., and Moon, K. C.: Monitoring network using continuous particle size distribution monitors: Connecting pollutant properties to visibility via Mie scattering calculations, Atmos. Environ., 28(16), 2733–2749, 1994.

Fung, J. C. H., Lau, A. K. H., Lam, J. S. L., and Yuan, Z.: Observational and modeling analysis of a severe air pollution episode in western Hong Kong, J. Geophys. Res., 110, D09105, doi:10.1029/2004JD005105, 2005.

Garland, R. M., Yang, H., Schmid, O., Rose, D., Nowak, A., Achtert, P., Wiedensohler, A., Takegawa, N., Kita, K., Miyazaki, Y., Kondo, Y., Hu, M., Shao, M., Zeng, L. M., Zhang, Y. H., Andreae, M. O., and Pöschl, U.: Aerosol optical properties in a rural environment near the mega-city Guangzhou, China: implications for regional air pollution, radiative forcing and remote sensing, Atmos. Chem. Phys., 8, 5161–5186, doi:10.5194/acp-8-5161-2008, 2008.

Gnauk, T., Müller, K., van Pinxteren, D., He, L. Y., Niu, Y., Hu, M., and Herrmann, H.: Size-segregated particulate chemical composition in Xinken, Pearl River Delta, China: OC/EC and organic compounds, Atmos. Environ., 42, 6296–6309, 2008.

Groblicki, P. J., Wolff, G. T., and Countess, R. J.: Visibility-reducing species in the Denver "brown cloud" – I. Relationship between extinction and chemical composition, Atmos. Environ., 15, 2473–2484, 1981.

Guangzhou Transport Planning Research Institute: Annual report on transport development of Guangzhou, 2006. http://www.gztpri.com/journal-viewer.asp?id=3, last accessed on August 21, 2009.

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, 2006.

Hale, G. M. and Querry, M. R.: Optical Constants of Water in the 200-nm to 200-\unit\mum Wavelength Region, Appl. Optics, 12(3), 555–563, doi:10.1364/AO.12.000555, 1973.

Hasan, H. and Dzubay, T. G.: Apportioning light extinction coefficients to chemical species in atmospheric aerosol, Atmos. Environ., 17(8), 1573–1581, 1983.

Hitzenberger, R., Jennings, S. G., Larson, S. M., Dillner, A., Cachier, H., Galambos, Z., Rouc, A., and Spain, T. G.: Intercomparison of measurement methods for black carbon aerosols, Atmos. Environ., 33, 2823–2833, 1999.

Ho, K. F., Lee, S. C., Cao, J. J., Li, Y. S., Chow, J. C., Watson, J. G., and Fung, K.: Variability of organic and elemental carbon, water soluble organic carbon, and isotopes in Hong Kong, Atmos. Chem. Phys., 6, 4569–4576, doi:10.5194/acp-6-4569-2006, 2006.

Ho, K. F., Lee, S. C., Yu, J. C., Zou, S. C., and Fung, K.: Carbonaceous characteristics of atmospheric particulate matter in Hong Kong, Sci. Total Environ., 300, 59–67, 2002.

Horvath, H.: Atmospheric light absorption – a review, Atmos. Environ., 27A, 293–317, 1993.

Horvath H.: Size segregated light absorption coefficient of the atmospheric aerosol, Atmos. Environ., 29(8), 875–883, 1995.

Huang, X.-F. and Yu, J. Z.: Size distributions of elemental carbon in the atmosphere of a coastal urban area in South China: characteristics, evolution processes, and implications for the mixing state, Atmos. Chem. Phys., 8, 5843–5853, doi:10.5194/acp-8-5843-2008, 2008.

Huang, X. F., Yu, J. Z., He, L.Y., and Hu, M.: Size distribution characteristics of elemental carbon emitted from Chinese vehicles: Results of a tunnel study and atmospheric implications, Environ. Sci. Technol., 40, 5355–5360, 2006.

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

Kim, K. W., Kim, Y. J., and Bang, S. Y.: Summer time haze characteristics of the urban atmosphere of Gwangju and the rural atmosphere of Anmyon, Korea, Environ. Monit. Assess., 141, 89–199, 2008.

Lai, L. Y. and Sequeira, R.: Visibility degradation across Hong Kong: its components and their relative contributions, Atmos. Environ., 35(34), 5861–5872, 2001.

Lowenthal, D. H., Rogers, C. F., Saxena, P., Watson, J. G., and Chow, J. C.: Sensitivity of estimated light extinction coefficients to model assumptions and measurement errors, Atmos. Environ., 29(7), 751–766, 1995.

Maenhaut, W., Cafmeyer, J., Dubtsov, S., and Chi, X. G.: Detailed mass size distributions of elements and species, and aerosol chemical mass closure during fall 1999 at Gent, Belgium, Nucl. Instrum. Methods Phys. Res. Sect. B-Beam Interact. Mater. Atoms., 189, 238–242, 2002.

Mallet, M., Roger, J. C., Despiaua, S., Dubovik, C., and Putaud, J. P.: Microphysical and optical properties of aerosol particles in urban zone during ESCOMPTE, Atmos. Res., 69, 73–97, 2003.

Malm, W. C., Gebhart, K. A., Molenar, J., Cahill, T., Eldred, R., and Huffman, D.: Examining the Relationship between Atmospheric Aerosols and Light Extinction at Mount Rainier and North Cascades National Parks, Atmos. Environ., 28(2), 347–360, 1994.

Miguel, A. H., Eiguren-Fernandez, A., Jaques, P. A., Froines, J. R., Grant, B. L., Mayo, P. R., and Sioutas, C.: Seasonal variation of the particle size distribution of polycyclic aromatic hydrocarbons and of major aerosol species in Claremont, California, Atmos. Environ., 38, 3241–3251, 2004.

Miyazaki, Y., Kondo, Y., Shiraiwa, M., Takegawa, N., Miyakawa, T., Han, S., Kita, K., Hu, M., Deng, Z. Q., Zhao, Y., Sugimoto, N., Blake, D. R., and Weber, R. J.: Chemical characterization of water-soluble organic carbon aerosols at a rural site in the Pearl River Delta, China, in the summer of 2006, J. Geophys. Res., 114, D14208, doi:10.1029/2009JD011736, 2009.

Pitchford, M., Malm, W. C., Schichtel, B., Kumar, N., Lowenthal, D., and Hand, J.: Revised algorithm for estimating light extinction from IMPROVE particle speciation data, J.Air and Waste Manage. Assoc., 57, 1326–1336, doi:10.3155/1047-3289.57.11.1326, 2007.

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

Seinfeld, J. H. and Pandis, S. N.: Atmospheric Chemistry and Physics – From Air Pollution to Climate Change (2nd Edition),~John Wiley and Sons, p 362, p 905, 2006.

Sloane, C. S., Watson, J., Chow, J., Pritchett, L., and Richards, L.W.: Size-segregated fine particle measurements by chemical species and their impact on visibility impairment in Denver, Atmos. Environ. – Part A General Topics, 25(5–6), 1013–1024, 1991.

Tang, A. N.: Chemical and size effects of hygroscopic aerosols on light scattering coefficients, J. Geophys. Res., 101, 19245–19250, 1996.

Van de Hulst, H. C.: Light Scattering by Small Particles, New York, Dover, 470pp., 1981.

Vanderlei, M. J., Artaxo, P., Liousse, C., Reid, J. S., Hobbs, P. V., and Kaufman, Y. J.: Effects of black carbon content, particle size, and mixing on light absorption by aerosols from biomass burning in Brazil, J. Geophys. Res., 103(D4), 32041–32050, 1998.

Venkataraman, C. and Friedlander, S. K.: Size distributions of polycyclic aromatic hydrocarbons and elemental carbon: 2. Ambient measurements and effects of atmospheric processes, Environ. Sci. Technol., 28, 563–572, 1994.

Wang, T.: Study of Visibility Reduction and its Causes in Hong Kong, final report to Air Services Group of The Environmental Protection Department of HKSAR, March 2003.

Wu, D., Bi, X. Y., Deng, X. J., Li, F., Tan, H.B., Liao, G. L., and Huang, J.: Effect of atmospheric haze on the deterioration of visibility over the Pearl River Delta, Acta Meteor. Sinica, 21, 215–223, 2007.

Xiao, R., Takegawa, N., Kondo, Y., Miyazaki, Y., Miyakawa, T., Hua, M., Shao, M., Zeng, L. M., Hofzumahaus, A., Holland, F., Lu, K., Sugimoto, N., Zhao, Y., and Zhang, Y. H.: Formation of submicron sulfate and organic aerosols in the outflow from the urban region of the Pearl River Delta in China, Atmos. Environ., 43, 3754–3763, doi:10.1016/j.atmosenv.2009.04.028, 2009.

Yang, H., Yu, J. Z., Ho, S. S. H., Xu, J. H., 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(20), 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, 2004.

Yu, H. and Yu, J. Z.: Modal Characteristics of Elemental and Organic Carbon in an Urban Location in Guangzhou, China, Aerosol Sci. Technol., 43, 1108–1118, 2009.

Zhang, X., Turpin, B. J., McMurry, P. H., Hering, S. V., and Stolzenburg, M. R.: Mie theory evaluation of species contributions to 1990 wintertime visibility reduction in the Grand Canyon, J. Air and Waste Manage. Assoc., 44(2), 153–162, 1994.

Zhang, Q. Y. and Zhang, Y. H.: Research on atmospheric boundary layer and pollution in Chinese cities, Research Progress on Urban Environmental Meteorology in China and Overseas, issue 2, 2001. Available at http://library.cma.gov.cn/publications/973environment/cshj0102.htm.