Atmospheric Chemistry and Physics Discussions
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10.5194/acpd-9-23955-2009
http://www.atmos-chem-phys-discuss.net/9/23955/2009/
http://www.atmos-chem-phys-discuss.net/9/23955/2009/acpd-9-23955-2009.html
http://www.atmos-chem-phys-discuss.net/9/23955/2009/acpd-9-23955-2009.pdf
23955
23986
2009-11-11
Size-resolved aerosol water-soluble ionic compositions in the summer of Beijing: implication of regional secondary formation
S. Guo
M. Hu
minhu@pku.edu.cn
Z. B. Wang
J. Slanina
Y. L. Zhao
State Key Joint Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking University, 100871 Beijing, China
Department of Environmental Science, Policy and Management, University of California, 94720 Berkeley, CA, USA
To characterize aerosol pollution in Beijing, size-resolved aerosols
were collected by MOUDIs during CAREBEIJING-2006 field campaign at
Peking University (urban site) and Yufa (upwind rural site). Fine
particle concentrations (PM<sub>1.8</sub> by MOUDI) were
99.8±77.4 μg/m<sup>3</sup> and 78.2±58.4 μg/m<sup>3</sup>, with PM<sub>1.8</sub>/PM<sub>10</sub> ratios of 0.64±0.08 and
0.76±0.08 at PKU and Yufa, respectively, and secondary compounds
accounted for more than 50% in fine particles. PMF model was used
to resolve the particle modes. Three modes were resolved at Yufa,
representing condensation, droplet and coarse mode. However, one more
droplet mode with bigger size was resolved, which was considered
probably from regional transport. Condensation mode accounted for
10%–60% of the total mass at both sites, indicating it must be
taken into account in summer. The formation of sulfate was mainly
attributed to in-cloud or aerosol droplet process (PKU 80%, Yufa
70%) and gas condensation process (PKU 14%, Yufa
22%). According to the thermodynamic instability of
NH<sub>4</sub>NO<sub>3</sub>, size distributions of nitrate were classified as
three categories by RH. The existence of Ca(NO<sub>3</sub>)<sub>2</sub> in droplet
mode indicated the reaction of HNO<sub>3</sub> with crustal particles was
also important in fine particles. Linear regression gave a rough
estimation that 69% of the PM<sub>10</sub> and 87% of the PM<sub>1.8</sub>
at PKU were regional contributions. Sulfate, ammonium and oxalate were
formed regionally, with the regional contributions of 90%, 87%
and 95% to PM<sub>1.8</sub>. Nitrate formation was local dominant. In
summary regional secondary formation led to aerosol pollution in the
summer of Beijing.
Anlauf,~K., Li,~S M., Leaitch,~R., Brook,~J., Hayden,~K., Toom-Sauntry,~D., and Wiebe,~A.: Ionic composition and size characteristics of particles in the lower Fraser Vellay: Pacific 2001 field study, Atmos. Environ., 40, 2662–2675, 2006.
Chow,~J.: Critical review of measurement methods to determine compliance with ambient air quality standards for suspended particulates. J Air Waste Manage., 45, 320–382, 1995.
Frenich,~A G., Galera,~M M., Vidal,~J L M., Massart,~D L., Torres-Lapasio,~J R., De Braekeleer,~K., Wang,~J H., and Hopke,~P K.: Resolution of multicomponent peaks by orthogonal projection approach, positive matrix factorization and alternating least squares, Anal. Chim. Acta, 411, 145–155, 2000.
Han,~L H., Zhuang,~G S., Yele,~S., and Wang,~Z F.: Local and non-local sources of airborne particulate pollution at Beijing. Sci. China Ser B, 48(3), 253–264, 2005.
He,~K B., Yang,~F M., Ma,~Y L., Zhang,~Q., Yao,~X H., Chan,~C K., Cadle,~S., Chan,~T., and Mulawa,~P.: The characteristics of PM$_2.5$ in Beijing, China, Atmos. Environ., 35(29), 4959–4970, 2001.
Hu,~M., Zhao,~Y L., He,~L Y., Huang,~X F., Tang,~X Y., Yao,~X H., and Chan,~C K.: Mass size distribution of Beijing particulate matters and its inorganic water-soluble ions in winter and summer, China Environ. Sci., 26(4), 1–6, 2005a.
Hu,~M., Zhang,~J., and Wu,~Z J.: Chemical compositions of precipitation and scavenging of particles in Beijing, Sci. China Ser B, 48(3), 265, 2005b.
Huang,~X F., Yu,~J Z., He,~L Y., and Yuan,~Z B.: 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.
Jia,~Y. T, Rahn,~K A., He,~K B., Wen,~T X., and Wang,~Y S.: A~novel technique for quantifying the regional component of urban aerosol solely from its sawtooth cycles, J Geophys. Res., 113, D21309, doi:10.1029/2008JD010389, 2008.
Jones,~D L.: Organic acids in the rhizosphere-a~critical review, Plant Soil, 205, 25–44, 1998.
Kawamura,~K. and Kaplan,~I R.: Motor exhaust emission as a~primary source for dicarboxylic acids in Los Angeles ambient air, Environ. Sci. Technol., 21, 105–110, 1987.
Kawamura,~K., Kasukabe,~H., and Barrie,~L A.: Source and reaction pathways of dicarboxylic acids, ketoacids and dicarbonyls in Arctic aerosols: one year of observations, Atmos. Environ., 30, 1709–1722, 1996.
Kim,~E., Hopke,~P K., Larson,~T V., and Covert,~D S.: Analysis of ambient particle size distributions using UNMIX and positive matrix factorization, Environ. Sci. Technol., 38, 202–209, 2004.
Kleeman,~M J., Schauer,~J J., and Cass,~G R.: Size and composition distribution of fine particulate matter emitted from wood burning, meat charbroiling and cigarettes, Environ. Sci. Technol., 33, 3516–3523, 1999.
Liu,~S., Hu,~M., Slanina,~J., He,~L Y., Niu,~Y W., Bruegemann,~E., Gnauk,~T., and Herrmann,~H.: Size distribution and source analysis of ionic compositions of aerosols in polluted periods at Xinken in Pearl River Delta (PRD) of China, Atmos. Environ., 42(25), 6284–6295, 2008.
Michael,~M.: The dissociation constant of ammonium nitrate and its dependence on temperature, relative humidity and particle size, Atmos. Environ., 27A, 261–270, 1993.
Narukawa,~M., Kawamura,~K., Anlauf,~K G., and Barrie,~L A.: Fine and coarse modes of dicarboxylic acids in the Arctic aerosols collected during the Polar Sunrise Experiment 1997, J Geophys. Res., 108(D18), 4575, doi:10.1029/203JD003646, 2003.
Narukawa,~M., Kawamura,~K., Takeuchi,~N., and Nakajima,~T.: Distribution of dicarboxylic acids and carbon isopotic compositions in aerosols from 1997 Indonesian forest fires, Geophys. Res. Lett., 26, 3101–3104, 1999.
NBSC, National Bureau of Statistics of China: Bulletin of Statistics for Beijing, Part Two: Population, People life and social security, http://www.stats.gov.cn/tjsj/ndsj/2008 /indexeh.htm, 2009a.
NBSC, National Bureau of Statistics of China: Bulletin of Statistics for Beijing, Part Three: Resource, Energy and Environment, http://www.stats.gov.cn/tjsj/ndsj/2008/indexeh.htm, 2009b.
Ohta,~S. and Okita,~T.: A~chemical characterization of atmospheric aerosol in Sapporo, Atmos. Environ., 24A, 815–822. 1990.
Pakkanen,~T A., Kerminen,~V M., Hillamo,~R E., Makinen,~M., Makela,~T., and Virkkula,~A.: Distribution of nitrate over sea-salt and soil derived particles implications from a~field study, J. Atmos. Chem., 24, 189–205, 1996.
Peng,~C. and Chan,~C K.: The water cycles of water soluble organic salts of atmospheric importance, Atmos. Environ., 35, 1183–1192, 2001.
Seinfeld,~J H. and Pandis,~S N.: Atmospheric Chemistry and Physics-from Air Pollution to Climate Change, John Wiley & Sons, Inc., New York, 1998.
Shao,~M., Tang,~X Y., Zhang,~Y H., and Li,~W J.: City clusters in China: air and surface water pollution, Front. Ecol. Environ., 4(7), 353–361, 2006.
Slanina,~J., ten Brink,~H M., Otjes,~R P., Even,~A., Jongejan,~P., Khlystov,~A., Waijers-Ijpelaan,~A., Hu,~M., and Lu,~Y.: The continuous analysis of nitrate and ammonium in aerosols by the steam jet aerosol collector (SJAC): extension and validation of the methodology, Atmos. Environ., 35, 2319–2330, 2001.
Stelson,~A W. and Seinfeld,~J H.: Thermodynamic prediction of the water activity, \chemNH_4NO_3 dissociation-constant, density and refractive index for the \chemNH_4NO_3-\chem(NH_4)_2SO_4-\chemH_2O system at 25-degrees-C, Atmos. Environ., 16(10), 2507–2514, 1982.
Sun,~Y L., Zhuang,~G S., Tang,~A H., Wang,~Y., and An,~Z S.: Chemical characteristics of PM$_2.5$ and PM$_10$ in haze-fog episodes in Beijing, Environ. Sci. Technol., 40(10), 3148–3155, 2006.
van Pinxteren,~D., Brueggemann,~E., Gnauk,~T., Iinuma,~Y., Mueller,~K., Nowak,~A., Achtert,~P., Wiedensohler,~A., and Herrmann,~H.: Size- and time-resolved chemical particle characterization during CAREBeijing-2006: different pollution regimes and diurnal profiles, J Geophys. Res., 114, D00G09, doi:10.1029/2008JD010890, 2009.
Wang,~L T., Hao,~J M., He,~K B., Wang,~S X., Li,~J H., Zhang,~Q., Streets,~D G., Fu,~J S., Jang,~C J., Takekawa,~H., and Chatani,~S.: A~modeling study of coarse particulate matter pollution in Beijing: regional source contributions and control implications for the 2008 summer Olympics, J Air Waste Manage., 58(8), 1057–1069, 2008.
Yang,~F., He,~K., Ye,~B., Chen,~X., Cha,~L., Cadle,~S H., Chan,~T., and Mulawa,~P A.: One-year record of organic and elemental carbon in fine particles in downtown Beijing and Shanghai, Atmos. Chem. Phys., 5, 1449–1457, 2005.
Yao, X. H., Chan, C. K., Fang, M., Cadle, S., Chan, T., Mulawa, P., He, K. B., and Ye, B. M.: The water-soluble ionic composition of PM$_2.5$ in Shanghai and Beijing, China, Atmos. Environ, 36(26), 4223–4234, 2002.
Yao,~X H., Lau,~A P S., Fang,~M., Chan,~C K., and Hu,~M.: Size distributions and formation of ionic species in atmospheric particulate pollutants in Beijing, China: 1 – inorganic ions, Atmos. Environ., 37(21), 2991–3000, 2003.
Zhuang,~H., Chan,~C K., Fang,~M., and Wexler,~A S.: Formation of nitrate and non-sea-salt sulfate on coarse particles, Atmos. Environ., 33, 4223–4233, 1999.