References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-11-7319-2011

Chemical characterization of aerosols at the summit of Mountain Tai in Central East China

Deng

¹ Zhuang

¹ Huang

¹ Li

¹ Zhang

¹ Wang

¹ Liu

¹ Sun

² Guo

¹ Fu

J. S.

³ Wang

The Center for Atmospheric Chemistry Study, Department of Environmental Science & Engineering, Fudan University, Shanghai 200433, China

The Institute of Atmospheric Physics, Chinese Academy of Science, LAPC, Beijing 100029, China

Department of Civil and Environmental Engineering, The University of Tennessee, Knoxville, TN 37996, USA

25 07 2011

11 14 7319 7332

This is an open-access article ditributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited.

This article is available from http://www.atmos-chem-phys.net/11/7319/2011/acp-11-7319-2011.html

The full text article is available as a PDF file from http://www.atmos-chem-phys.net/11/7319/2011/acp-11-7319-2011.pdf

PM2.5 and TSP samples were collected at the summit of Mountain Tai (MT) (1534 m a.s.l.) in spring 2006/2007 and summer 2006 to investigate the characteristics of aerosols over central eastern China. For comparison, aerosol samples were also collected at Tazhong, Urumqi, and Tianchi in Xinjiang in northwestern China, Duolun and Yulin in northern China, and two urban sites in the megacities, Beijing and Shanghai, in 2007. Daily mass concentrations of TSP and PM2.5 ranged from 39.6–287.6 μg m−3 and 17.2–235.7 μg m−3 respectively at the summit of MT. Averaged concentrations of PM2.5 showed a pronounced seasonal variation with higher concentration in summer than spring. 17 water-soluble ions (SO42−, NO3−, Cl−, F−, PO43−, NO2−, CH3COO−, CH2C2O42−, C2H4C2O42−, HCOO−, MSA, C2O42−, NH4+, Ca2+, K+, Mg2+, Na+), and 19 elements of all samples were measured. SO42−, NO3−, and NH4+ were the major water-soluble species in PM2.5, accounting for 61.50 % and 72.65 % of the total measured ions in spring and summer, respectively. The average ratio of PM2.5/TSP was 0.37(2006) and 0.49(2007) in spring, while up to 0.91 in summer, suggesting that aerosol particles were primarily comprised of fine particles in summer and of considerable coarse particles in spring. Crustal elements (e.g., Ca, Mg, Al, Fe, etc.) showed higher concentration in spring than summer, while most of the pollution species (SO42−, NO3−, K+, NO2−, NH4+, Cl−, organic acids, Pb, Zn, Cd, and Cr) from local/regional anthropogenic emissions or secondary formation presented higher concentration in summer. The ratio of Ca/Al suggested the impact of Asian dust from the western deserts on the air quality in this region. The high concentration of K+ in PM2.5 (4.41 μg m−3) and its good correlation with black carbon (r = 0.90) and oxalic acid (r = 0.87) suggested the severe pollution from biomass burning, which was proved to be a main source of fine particles over central eastern China in summer. The contribution of biomass burning to the fine particle at MT accounted for 7.56 % in spring and 36.71 % in summer, and even reached to 81.58 % on a day. As and Pb were two of the most enriched elements. The long-range transport of aerosols spread the heavy pollution from coal-mining/coal-ash to everywhere over China. Anthropogenic air-pollution was evidently rather severe at MT, though it has been declared by UNESCO to be a World Heritage site.

References 1

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

Ariel, F. S. and Lamb, D.: The sensitivity of sulfer wet deposition to atmospheric oxidants, Atmos, Environ., 34, 1681–1690, 2000.

Arimoto, R.: Eolian dust and Climate: Relationship to sources, tropospheric chemistry, transport and deposition, Earth Sci. Rev., 54, 29–42, 2001.

Arimoto R., Duce R. A., and Savoie D. L.: Relationships among aerosol constituents from Asia and the North Pacific during PEM-West, J. Geophys. Res. Atmos., 101(D1), 2011–2023, 1996.

Cao, G., Zhang, X., Wang, D., and Zheng, F.: Inventory of atmospheric pollutants discharged from biomass burning in China continent, China Environ. Sci., 25(4), 389–393, 2005 (in Chinese).

Cao, G., Zhang, X., Wang, Y., and Zheng, F.: Estimation of the emission from open burning of crop residues in China continent, Chin. Sci. Bull., 52(18), 1826–1831, 2007 (in Chinese).

Cao, G., Zhang, X., Gong, S., and Zheng, F.: Investigation on emission factors of particulate matter and gaseous pollutants from crop residue burning, Environ. Sci., 20, 50–55, 2008a.

Cao, J. J., Chow, J. C., Watson, J. G., Wu, F., Han, Y. M., Jin, Z. D., Shen, Z. X., and An, Z. S.: Size-differentiated source profiles for fugitive dust in the Chinese Loess Plateau, Atmos. Environ., 42(10), 2261–2275, 2008b.

Chan, Y. C., Simpson, R. W., Mctainsh, G. H., Vowles, P. D., Cohen, D. D., and Bailey, G. M.: Source apportionment of visibility degradation problems in Brisbane (Australia) using the multiple linear regression technique, Atmos. Environ., 33, 3237–3250, 1999.

Chester, R.: Marine Geochemistry, Unwin Hyman, London, 698~pp., 1990.

Dentener, F. J., Carmichael, G. R., and Zhang, Y.: Role of mineral aerosol as a reactive surface in the global troposphere, J. Geophys. Res. Atmos., 101(D17), 22869–22889, 1996.

Dockery, D. W., Pope, A. C., Xu, X., Spengler, J. D., Ware, J. H., Fay, M. E., Ferris Jr., B. G., and Speizer, F. E.: An association between air pollution and mortality in six US cities, New Engl. J. Med., 1753–1759, 1993.

Facchini, M. C. S., Decesari, M., Mircea, S., Fuzzi, and Loglio, G.: Surface tension of atmospheric wet aerosol and cloud/fog droplets in relation to their organic carbon content and chemical composition, Atmos. Environ., 34, 4853–4857, 2000.

Gao, J., Wang, T., Ding, A., and Liu, C.: Observational study of ozone and carbon monoxide at the summit of mount Tai (1534 m a.s.l.) in central-eastern China, Atmos. Environ., 39(20), 4779–4791, 2005.

Guo, J., Kenneth, A., Rahn, and Zhuang, G.: A mechanism for the increase of pollution elements in dust storms in Beijing, Atmos. Environ., 38, 855–862, 2004.

Han, L., Zhuang G., Sun Y., and Wang, Z. F.: Local and non-local sources of airborne particulate pollution at Beijing, Science in China Ser. B Chemistry, 48(4), 1–12, 2005.

Jill, E. R., Oliver, V. R., Katharine, F. M., Christopher J., Eli, D. S., Vincent, A. D., Sonia, M. K., Liaquat, H., and Collett Jr., J.: Drop size-dependent S (IV) oxidation in chemically heterogeneous radiation fogs, Atmos. Environ., 35, 5717–5728, 2001.

Kaufman, Y. J., Tanre, D., and Boucher, O.: A satellite view of aerosols in the climate system, Nature, 419, 215–223, 2002.

Li, X., Wang, S., Duan, L., Hao, J., Li, C., Chen, Y., and Yang, L.: Particulate and Trace Gas Emissions from Open Burning of Wheat Straw and Corn Stover in China, Environ. Sci. Technol., 41(17), 6052–6058, 2007.

Liu, C. L., Zhang, J., and Liu, S. M.: Physical and chemical characters of materials from several mineral aerosol sources in China, Environ. Sci., 23, 28–32, 2002.

Matsumoto, K., Tanaka, H., Nagao, I., and Ishizaka, Y.: Contribution of particulate sulfate and organic carbon to cloud condensation nuclei in the marine atmosphere, Geophys. Res. Lett., 24, 655–658, 1997.

Novakov, T. and Penner, J. E.: Large condensation of organic aerosols to cloud-condensation nuclei concentration, Nature, 365, 823–826, 1993.

Novelli, P. C., Masarie, K. A., Tans, P. P., and Lang, P. M.: Recent changes in atmospheric carbon monoxide, Science, 263, 1587–1590, 1994.

Novelli, P. C., Masarie, K. A., and Lang, P. M.: Distributions and recent changes of carbon monoxide in the lower troposphere, J. Geophys. Res., 103(D51), 19015–19033, 1998.

Ohta, S. and Okita, T.: A chemical characterization of atmospheric aerosol in Sapporo, Atmos. Environ., 24A, 815–822, 1990.

Pierson, W. R., Brachaczek, W. W., and Mckee, D. E.: Sulfate emissions from catalyst equipped automobiles on the highway, J. Air Pollut. Control Assoc., 29, 255–257, 1979.

Rastogi, N. and Sarin M. M.: Long-term characterization of ionic species in aerosols from urban and high altitude sites in western India: Role of mineral dust and anthropogenic sources, Atmos. Environ, 39, 5541–5554, 2005.

Rastogi, N. and Sarin, M. M.: Chemistry of aerosols over a semi-arid region: Evidence for acid neutralization by mineral dust, J. Geophys. Res. Lett., 33, L23815, http://dx.doi.org/10.1029/2006GL027708doi:10.1029/2006GL027708, 2006.

Ren, Y., Ding, A., Wang, T., Shen, X., Guo, J., Zhang, J., Wang, Y., Xu, P., Wang, X., Gao, J., Jeffrey, L., and Collett, J.: Measurement of gas-phase total peroxides at the summit of Mount Tai in China, Atmos. Environ., 43, 1702–1711, 2009.

Sacoby, M. W. and Marc, L.: Examination of atmospheric ammonia levels near hog CAFOs, homes, and schools in Eastern North Carolina, Atmos. Environ., 41, 4977–4987, 2007.

Shen, Z. X., Cao, J. J., Li, X. X., Wang, Y. Q., Jie, D. M., and Zhang, X. Y.: Chemical characteristics of aerosol particles (PM$_2.5)$ at a site of Horqin Sand-land in northeast China, Environmental Sciences-China, 18(4), 701–707, 2006.

Song, C. H. and Carmichael, G. R.: A three-dimensional modeling investigation of the evolution processes of dust and sea-salt particles in East Asia, J. Geophys. Res.-Atmos., 106(D16), 18131–18154, 2001.

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, http://dx.doi.org/10.1029/2003GB002040doi:10.1029/2003GB002040, 2003.

Sun, Y., Zhuang, G., Wang, Y., Han, L., Guo, J., Dan, M., Zhang, W., Wang, Z., and Hao, Z.: The air-borne particulate pollution in Beijing-concentration, composition, distribution and sources, Atmos. Environ., 38, 5991–6004, 2004.

Sun, Y., Zhuang, G., Wang, Y., Zhao, X., Li, J., Wang, Z., and An, Z.: Chemical composition of dust storms in Beijing and implications for the mixing of mineral aerosol with pollution aerosol on the pathway, J. Geophys. Res., 110, D24209, http://dx.doi.org/10.1029/2005JD006054doi:10.1029/2005JD006054, 2005.

Sun, Y., Zhuang, G., Huang K., Li J., Wang, Q., Wang Y., Lin, Y., Fu, J., Zhang, W., Tang, A., and Zhao, X.: Asian dust over northern China and its impact on the downstream aerosol chemistry in 2004, J. Geophys. Res., 115, D00K09, http://dx.doi:10.1029/2009JD012757doi:10.1029/2009JD012757, 2010.

Suthawaree, J., Kato, S., Okuzawa, K., Kanaya, Y., Pochanart, P., Akimoto, H., Wang, Z., and Kajii, Y.: Measurements of volatile organic compounds in the middle of Central East China during Mount Tai Experiment 2006 (MTX2006): observation of regional background and impact of biomass burning, Atmos. Chem. Phys., 10, 1269–1285, http://dx.doi.org/10.5194/acp-10-1269-2010doi:10.5194/acp-10-1269-2010, 2010.

Tegen, I., Lacis, A. A., and Fung, I.: The influence of climate forcing of mineral aerosols from disturbed soils, Nature, 380(4), 419–422, 1996.

Truex, T. J., Pierson, W. R., and Mckee, D. E.: Sulfate in diesel exhaust. Environ. Sci. Technol., 14, 1118–1121, 1980.

Tsai, Y. I. and Cheng, M. T.: Visibility and aerosol chemical compositions near the coastal area in central Taiwan, Sci. Total Environ., 231, 37–51, 1999.

Underwood, G. M., Li, P., Al-Abadleh, H., and Grassian, V. H.: A Knudsen cell study of the heterogeneous reactivity of nitric acid on oxide and mineral dust particles, J. Phys. Chem. A., 105(27), 6609–6620, 2001.

Virkkula, A., Teinilä, K., Hillamo, R., Kerminen, V.-M., Saarikoski, S., Aurela, M., Viidanoja, J., Paatero, J., Koponen, I. K., and Kulmala, M.: Chemical composition of boundary layer aerosol over the Atlantic Ocean and at an Antarctic site, Atmos. Chem. Phys., 6, 3407–3421, http://dx.doi.org/10.5194/acp-6-3407-2006doi:10.5194/acp-6-3407-2006, 2006.

Wang, T., Cheung, A., Vincent, T. F., Anson, M., and Li, Y. S.: Ozone and related gaseous pollutants in the boundary layer of eastern China: overview of the recent measurements at a rural site, Geophys. Res. Lett., 28(12), 2373–2376, 2001.

Wang, Y., Zhuang, G., Sun, Y., and An, Z.: Water-soluble part of the aerosol in the dust storm season – evidence of the mixing between mineral and pollution aerosols, Atmos. Environ., 39, 7020–7029, 2005.

Wang, Y., Zhuang, G., Sun Y., and An, Z.: The variation of characteristics and formation mechanisms of aerosols in dust, haze, and clear days in Beijing, Atmos. Environ., 40, 6579–6591, 2006a.

Wang, Y., Zhuang, G., Zhang, X., Huang, K., Xu, C., Tang, A., Chen, J., and An, Z.: The ion chemistry, seasonal cycle, and sources of PM$_2.5$ and TSP aerosol in Shanghai, Atmos. Environ., 40, 2935–2952, 2006b.

Wang, Y., Ge, F., Liu, X., Wang, W., Jia, H., and Wang, D.: Analysis of the ionic characteristics for wet droplets at Mountain Tai, China Environ. Sci., 26(4), 422–426, 2006c (in Chinese).

Wang, Y., Wai, K., Gao, J., Liu, X., Wang, T., and Wang, W.: The impacts of anthropogenic emissions on the precipitation chemistry at an elevated site in North-eastern China, Atmos. Environ., 42, 2959–2970, 2008.

Wedepohl, K. H.: The compositions of the continental crust, Geochim. Cosmochim. Acta, 59, 1217–1232, 1995.

Yaacov, M. and Judith, G.: Heterogeneous reactions of minerals with sulfur and nitrogen oxides, J. Aerosol Sci., 20(3), 303–311, 1989.

Yuan, H., Wang, Y., and Zhuang, G.: The simultaneous determination of organic acid, MSA with inorganic anions in aerosol and rainwater by ion chromatography, J. Inst. Anal., 6, 12–16, 2003 (in Chinese).

Zhang, X. Y., Zhuang, G. Y., Zhu, G. H., Zhang, D., An, Z. S., Chen, T., and Huang, X. P.: Element tracers for Chinese source dust, Science in China (Series D), 39(5), 512–521, 1996.

Zhang, X. Y., Arimoto, R., and An, Z. S.: Dust emission from Chinese desert sources linked to variations in atmospheric circulation, J. Geophys. Res.-Atmos., 102(D23), 28041–28047, 1997.

Zhang, D., Zang, J., Shi, G., Iwasaka, Y., Matsuki, A., and Trochkine, D.: Mixture state of individual Asian dust particles at a coastal site of Qingdao, China, Atmos. Environ., 37(28), 3895–3901, 2003.

Zhu, B., Zhu, X., Zhang, Y., Zeng, L., and Zhang, Y.: Emission factors of PM$_2.5$ from crop straw burning, Res. Environ. Sci., 18(2), 29–33, 2005 (in Chinese).

Zhuang, G., Guo, J., Yuan, H., and Zhao, C.: The compositions, sources, and size distribution of the dust storm from China in spring of 2000 and its impact on the global environment, Chin. Sci. Bull., 46(11), 895–900, http://dx.doi.org/10.1007/BF02900460doi:10.1007/BF02900460, 2001.