<?xml version="1.0" encoding="utf-8" standalone="no"?>
<!DOCTYPE article SYSTEM "http://www.atmos-chem-phys-discuss.net/inc/acpd/copernicus.dtd">
<article language="en">
	<journal>
		<journal_title>Atmospheric Chemistry and Physics Discussions</journal_title>
		<journal_url>www.atmos-chem-phys-discuss.net</journal_url>
		<issn>1680-7367</issn>
		<eissn>1680-7375</eissn>
		<volume_number>8</volume_number>
		<issue_number>6</issue_number>
		<publication_year>2008</publication_year>
	</journal>
	<doi>10.5194/acpd-8-19249-2008</doi>
	<article_url>http://www.atmos-chem-phys-discuss.net/8/19249/2008/</article_url>
	<abstract_html>http://www.atmos-chem-phys-discuss.net/8/19249/2008/acpd-8-19249-2008.html</abstract_html>
	<fulltext_pdf>http://www.atmos-chem-phys-discuss.net/8/19249/2008/acpd-8-19249-2008.pdf</fulltext_pdf>
	<start_page>19249</start_page>
	<end_page>19272</end_page>
	<publication_date>2008-11-14</publication_date>
	<article_title content_type="html">Observation of nitrate coatings on atmospheric mineral dust particles</article_title>
	<authors>
		<author numeration="1" affiliations="1,2">
			<name>W. J. Li</name>
		</author>
		<author numeration="2" affiliations="1">
			<name>L. Y. Shao</name>
		</author>
	</authors>
	<affiliations>
		<affiliation numeration="1" content_type="html">State Key Laboratory of Coal Resources and Safe Mining &amp; Department of Resources and Earth Science, China University of Mining and Technology, Beijing, China</affiliation>
		<affiliation numeration="2" content_type="html">School of Earth and Space Exploration &amp; Department of Chemistry and Biochemistry, Arizona State University, Tempe, AZ, USA</affiliation>
	</affiliations>
	<abstract content_type="html">Nitrate compounds have recently received much attention because of their
ability to alter the hygroscopic properties and cloud condensation nuclei
(CCN) activity of mineral dust particles in the atmosphere. However, very
little is known about specific characteristics of nitrate-coated mineral
particles in an individual particle scale in field study. The sample
collection was conducted during brown haze and dust episodes occurred
between 24 May and 21 June 2007 in Beijing, northern China. The sizes,
morphologies, and compositions of mineral dust particles together with their
coatings were analyzed using transmission electron microscopy (TEM). 92%
of the internally mixed mineral particles analyzed are covered with Ca-,
Mg-, and Na-rich coatings, and 8% are associated with K- and S-rich
coatings. The major coatings contain Ca, Mg, O, and N with minor amounts of
S and Cl, suggesting that they are possibly nitrates mixed with less
sulfates and chlorides. These nitrate coatings strongly relate with the
presence of alkaline mineral components (e.g., calcite and dolomite) within
individual mineral particles. Calcium sulfate particles with the diameter
from 10 to 500 nm were also detected within Ca(NO&lt;sub&gt;3&lt;/sub&gt;)&lt;sub&gt;2&lt;/sub&gt; and
Mg(NO&lt;sub&gt;3&lt;/sub&gt;)&lt;sub&gt;2&lt;/sub&gt; coatings. Our results indicate that mineral particles in
brown haze episodes were involved in atmospheric heterogeneous reactions
with two or more acidic gases (e.g., SO&lt;sub&gt;2&lt;/sub&gt;, NO&lt;sub&gt;2&lt;/sub&gt;, HCl, and
HNO&lt;sub&gt;3&lt;/sub&gt;). Mineral particles that acquire hygroscopic coatings tend to be
more spherical and larger. Such changes enhance their light scattering and
CCN activity, both of which have cooling effects on the climate.</abstract>
	<references>
		<reference numeration="1" content_type="text"> Al-Hosney, H. A. and Grassian, V. H.: Water, sulfur dioxide and nitric acid adsorption on calcium carbonate: A transmission and ATR-FTIR study, Phys. Chem. Chem. Phys., 7, 1266–1276, 2005. </reference>
		<reference numeration="2" content_type="text"> Andreae, M. O.: Climatic effects of changing atmospheric aerosol levels, in: Future Climates of the World: A Modeling Perspective, World Survey of Climatology, edited by: Henderson, A., Elsevier, New York, 1620–1623, 1995. </reference>
		<reference numeration="3" content_type="text"> 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, 17 969–17 980, 2001. </reference>
		<reference numeration="4" content_type="text"> Borensen, C., Kirchner, U., Scheer, V., Vogt, R., and Zellner, R.: Mechanism and kinetics of the reactions of NO&lt;sub&gt;2&lt;/sub&gt; or HNO&lt;sub&gt;3&lt;/sub&gt; with alumina as a mineral dust model compound, J. Phys. Chem. A, 104, 5036–5045, 2000. </reference>
		<reference numeration="5" content_type="text"> Buseck, P. R. and Posfai, M.: Airborne minerals and related aerosol particles: Effects on climate and the environment, P. Natl. Acad. Sci. USA, 96, 3372–3379, 1999. </reference>
		<reference numeration="6" content_type="text"> Buseck, P. R., Jacob, D. J., Posfai, M., Li, J., and Anderson, J. R.: Minerals in the air: An environmental perspective, Int. Geol. Rev., 42, 577–593, 2000. </reference>
		<reference numeration="7" content_type="text"> Chan, C. K. and Yao, X.: Air pollution in mega cities in China, Atmos. Environ., 42, 1–42, 2008. </reference>
		<reference numeration="8" content_type="text"> DeMott, P. J., Cziczo, D. J., Prenni, A. J., Murphy, D. M., Kreidenweis, S. M., Thomson, D. S., Borys, R., and Rogers, D. C.: Measurements of the concentration and composition of nuclei for cirrus formation, P. Natl. Acad. Sci. USA, 100, 14 655–14 660, doi:10.1073/pnas.2532677100, 2003. </reference>
		<reference numeration="9" content_type="text"> Dentener, F. J., Carmichael, G. R., Zhang, Y., Lelieveld, J., and Crutzen, P. J.: Role of mineral aerosol as a reactive surface in the global troposphere, J. Geophys. Res.-Atmos., 101, 22 869–22 889, 1996. </reference>
		<reference numeration="10" content_type="text"> Draxler, R. R. and Rolph, G. D.: HYbrid Single-Particle Lagrange Integrated Trajectory, Model access via NOAA ARL READY Website: http://www.arl.noaa.gov/ready/hysplit4.html, NOAA Air Resources Laboratory, Silver Spring, MD, 2003. </reference>
		<reference numeration="11" content_type="text"> Fairlie, T. D., Jacob, D. J., and Park, R. J.: The impact of transpacific transport of mineral dust in the United States, Atmos. Environ., 41, 1251–1266, 2007. </reference>
		<reference numeration="12" content_type="text"> Fountoukis, C. and Nenes, A.: ISORROPIA II: a computationally efficient thermodynamic equilibrium model for K$^+$-Ca$^2+$-Mg$^2+$-NH$_4^+$-Na$^+$-SO$_4^2-$-NO$_3^-$-Cl$^-$-H&lt;sub&gt;2&lt;/sub&gt;O aerosols, Atmos. Chem. Phys., 7, 4639–4659, 2007. </reference>
		<reference numeration="13" content_type="text"> Gibson, E. R., Hudson, P. K., and Grassian, V. H.: Aerosol chemistry and climate: Laboratory studies of the carbonate component of mineral dust and its reaction products, Geophys. Res. Lett., 33, L13811, doi:10.1029/2006GL026386, 2006a. </reference>
		<reference numeration="14" content_type="text"> Gibson, E. R., Hudson, P. K., and Grassian, V. H.: Physicochemical properties of nitrate aerosols: Implications for the atmosphere, J. Phys. Chem. A, 110, 11 785–11 799, 2006b. </reference>
		<reference numeration="15" content_type="text"> Guinot, B., Cachier, H., Sciare, J., Tong, Y., Xin, W., and, Jianhua, Y.: Beijing aerosol: Atmospheric interactions and new trends, J. Geophys. Res.-Atmos., 112, 16, D14314, doi:10.1029/2006JD008195, 2007. </reference>
		<reference numeration="16" content_type="text"> Ha, Z. Y. and Chan, C. K.: The water activities of MgCl&lt;sub&gt;2&lt;/sub&gt;, Mg(NO$_3)_2$, MgSO&lt;sub&gt;4&lt;/sub&gt;, and their mixtures, Aerosol Sci. Tech., 31, 154–169, 1999. </reference>
		<reference numeration="17" content_type="text"> Hanisch, F. and Crowley, J. N.: Heterogeneous reactivity of gaseous nitric acid on Al&lt;sub&gt;2&lt;/sub&gt;O&lt;sub&gt;3&lt;/sub&gt;, CaCO&lt;sub&gt;3&lt;/sub&gt;, and atmospheric dust samples: A Knudsen cell study, J. Phys. Chem. A, 105, 3096–3106, doi:10.1021/jp001254, 2001. </reference>
		<reference numeration="18" content_type="text"> Haywood, J. and Boucher, O.: Estimates of the direct and indirect radiative forcing due to tropospheric aerosols: A review, Rev. Geophys., 38, 513–543, 2000. </reference>
		<reference numeration="19" content_type="text"> Husar, R. B., Tratt, D. M., Schichtel, B. A., Falke, S. R., Li, F., Jaffe, D., Gasso, S., Gill, T., Laulainen, N. S., Lu, F., Reheis, M. C., Chun, Y., Westphal, D., Holben, B. N., Gueymard, C., McKendry, I., Kuring, N., Feldman, G. C., McClain, C., Frouin, R. J., Merrill, J., DuBois, D., Vignola, F., Murayama, T., Nickovic, S., Wilson, W. E., Sassen, K., Sugimoto, N., and Malm, W. C.: Asian dust events of April 1998, J. Geophys. Res.-Atmos., 106, 18 317–18 330, 2001. </reference>
		<reference numeration="20" content_type="text"> Hwang, H. J. and Ro, C. U.: Direct observation of nitrate and sulfate formations from mineral dust and sea-salts using low-Z particle electron probe X-ray microanalysis, Atmos. Environ., 40, 3869–3880, 2006. </reference>
		<reference numeration="21" content_type="text"> Jacob, D. J.: Heterogeneous chemistry and tropospheric ozone, Atmos. Environ., 34, 2131–2159, 2000. </reference>
		<reference numeration="22" content_type="text"> Johnson, K. S., Zuberi, B., Molina, L. T., Molina, M. J., Iedema, M. J., Cowin, J. P., Gaspar, D. J., Wang, C., and Laskin, A.: Processing of soot in an urban environment: case study from the Mexico City Metropolitan Area, Atmos. Chem. Phys., 5, 3033–3043, 2005. </reference>
		<reference numeration="23" content_type="text"> Kelly, J. T. and Wexler, A. S.: Thermodynamics of carbonates and hydrates related to heterogeneous reactions involving mineral aerosol, J. Geophys. Res.-Atmos., 110, D11201 doi:10.1029/2004jd005583, 2005. </reference>
		<reference numeration="24" content_type="text"> Kelly, J. T., Chuang, C. C., and Anthony, S. W.: Influence of dust composition on cloud droplet formation, Atmos. Environ., 41, 2904–2904, 2007. </reference>
		<reference numeration="25" content_type="text"> Knopf, D. A. and Koop, T.: Heterogeneous nucleation of ice on surrogates of mineral dust, J. Geophys. Res.-Atmos., 111, 10, D12201, doi:10.1029/2005JD006894, 2006. </reference>
		<reference numeration="26" content_type="text"> Kojima, T., Buseck, P. R., Iwasaka, Y., Matsuki, A., and Trochkine, D.: Sulfate-coated dust particles in the free troposphere over Japan, Atmos. Res., 82, 698–708, 2006. </reference>
		<reference numeration="27" content_type="text"> Krueger, B. J., Grassian, V. H., Cowin, J. P., and Laskin, A.: Heterogeneous chemistry of individual mineral dust particles from different dust source regions: the importance of particle mineralogy, Atmos. Environ., 38, 6253–6261, doi:10.1016/j.atmosenv.2004.07.010, 2004. </reference>
		<reference numeration="28" content_type="text"> Krueger, B. J., Grassian, V. H., Laskin, A., and Cowin, J. P.: The transformation of solid atmospheric particles into liquid droplets through heterogeneous chemistry: Laboratory insights into the processing of calcium containing mineral dust aerosol in the troposphere, Geophys. Res. Lett., 30(3)1148, doi:10.1029/2002gl016563, 2003. </reference>
		<reference numeration="29" content_type="text"> Laskin, A., Iedema, M. J., Ichkovich, A., Graber, E. R., Taraniuk, I., and Rudich, Y.: Direct observation of completely processed calcium carbonate dust particles, Faraday Discuss., 130, 453–468, doi:10.1039/b417366j, 2005a. </reference>
		<reference numeration="30" content_type="text"> Laskin, A., Wietsma, T. W., Krueger, B. J., and Grassian, V. H.: Heterogeneous chemistry of individual mineral dust particles with nitric acid: A combined CCSEM/EDX, ESEM, and ICP-MS study, J. Geophys. Res.-Atmos., 110, D10208, doi:10.1029/2004jd005206, 2005b. </reference>
		<reference numeration="31" content_type="text"> Li, X. H., Zhao, L. J., Dong, J. L., Xiao, H. S., and Zhang, Y. H.: Confocal Raman studies of Mg(NO$_3)_2$ aerosol particles deposited on a quartz substrate: Supersaturated structures and complicated phase transitions, J. Phys. Chem. B, 112, 5032–5038, doi:10.1021/jp709938x, 2008. </reference>
		<reference numeration="32" content_type="text"> Li, Z. Q., Chen, H., Cribb, M., Dickerson, R., Holben, B., Li, C., Lu, D., Luo, Y., Maring, H., Shi, G., Tsay, S. C., Wang, P., Wang, Y., Xia, X., Zheng, Y., Yuan, T., and Zhao, F.: Preface to special section on east Asian studies of tropospheric aerosols: An international regional experiment (EAST-AIRE), J. Geophys. Res.-Atmos., 112, D22S00, doi:10.1029/2007JD008853, 2007. </reference>
		<reference numeration="33" content_type="text"> Matsuki, A., Iwasaka, Y., Shi, G. Y., Zhang, D. Z., Trochkine, D., Yamada, M., Kim, Y. S., Chen, B., Nagatani, T., Miyazawa, T., Nagatani, M., and Nakata, H.: Morphological and chemical modification of mineral dust: Observational insight into the heterogeneous uptake of acidic gases, Geophys. Res. Lett., 32, L22806, doi:10.1029/2005GL024176, 2005. </reference>
		<reference numeration="34" content_type="text"> Middlebrook, A. M., Murphy, D. M., Lee, S. H., Thomson, D. S., Prather, K. A., Wenzel, R. J., Liu, D. Y., Phares, D. J., Rhoads, K. P., Wexler, A. S., Johnston, M. V., Jimenez, J. L., Jayne, J. T., Worsnop, D. R., Yourshaw, I., Seinfeld, J. H., and Flagan, R. C.: A comparison of particle mass spectrometers during the 1999 Atlanta Supersite Project, J. Geophys. Res.-Atmos., 108(D7)13, 8424, doi:10.1029/2001JD000660, 2003. </reference>
		<reference numeration="35" content_type="text"> Murphy, D. M., Cziczo, D. J., Froyd, K. D., Hudson, P. K., Matthew, B. M., Middlebrook, A. M., Peltier, R. E., Sullivan, A., Thomson, D. S., and Weber, R. J.: Single-particle mass spectrometry of tropospheric aerosol particles, J. Geophys. Res.-Atmos., 111, D23S32, doi:10.1029/2006jd007340, 2006. </reference>
		<reference numeration="36" content_type="text"> Niemi, J. V., Saarikoski, S., Tervahattu, H., Mäkelä, T., Hillamo, R., Vehkamäki, H., Sogacheva, L., and Kulmala, M.: Changes in background aerosol composition in Finland during polluted and clean periods studied by TEM/EDX individual particle analysis, Atmos. Chem. Phys., 6, 5049–5066, 2006. </reference>
		<reference numeration="37" content_type="text"> Okada, K. and Hitzenberger, R. M.: Mixing properties of individual submicrometer aerosol particles in Vienna, Atmos. Environ., 35, 5617–5628, 2001. </reference>
		<reference numeration="38" content_type="text"> Ooki, A. and Uematsu, M.: Chemical interactions between mineral dust particles and acid gases during Asian dust events, J. Geophys. Res.-Atmos., 110, 3201–3201, 2005. </reference>
		<reference numeration="39" content_type="text"> Pandis, S. N. and Seinfeld, J. H.: Sensitivity analysis of a chemical mechanism for aqueous-phase atmospheric chemistry, J. Geophys. Res.-Atmos., 94, 1105–1126, 1989. </reference>
		<reference numeration="40" content_type="text"> Posfai, M., Anderson, J. R., Buseck, P. R., and Sievering, H.: Compostioinal variations of sea-salt-mode aerosol-particles from the North-Atlantic, J. Geophys. Res.-Atmos., 100, 23 063–23 074, 1995. </reference>
		<reference numeration="41" content_type="text"> Ravishankara, A. R.: Heterogeneous and multiphase chemistry in the troposphere, Science, 276, 1058–1065, 1997. </reference>
		<reference numeration="42" content_type="text"> Seinfeld, J. H., Carmichael, G. R., Arimoto, R., Conant, W. C., Brechtel, F. J., Bates, T. S., Cahill, T. A., Clarke, A. D., Doherty, S. J., Flatau, P. J., Huebert, B. J., Kim, J., Markowicz, K. M., Quinn, P. K., Russell, L. M., Russell, P. B., Shimizu, A., Shinozuka, Y., Song, C. H., Tang, Y. H., Uno, I., Vogelmann, A. M., Weber, R. J., Woo, J. H., and Zhang, X. Y.: ACE-ASIA – Regional climatic and atmospheric chemical effects of Asian dust and pollution, B. Am. Meteorol. Soc., 85, 367–380, 2004. </reference>
		<reference numeration="43" content_type="text"> Shao, L. Y., Li, W. J., Xiao, Z. H., and Sun, Z. Q.: The mineralogy and possible sources of spring dust particles over Beijing, Adv. Atmos. Sci., 25, 395–403, doi:10.1007/s00376-008-0395-8, 2008. </reference>
		<reference numeration="44" content_type="text"> Sokolik, I. N. and Toon, O. B.: Direct radiative forcing by anthropogenic airborne mineral aerosols, Nature, 381, 681–683, 1996. </reference>
		<reference numeration="45" content_type="text"> Streets, D. G., Bond, T. C., Carmichael, G. R., Fernandes, S. D., Fu, Q., He, D., Klimont, Z., Nelson, S. M., Tsai, N. Y., Wang, M. Q., Woo, J. H., and Yarber, K. F.: An inventory of gaseous and primary aerosol emissions in Asia in the year 2000, J. Geophys. Res.-Atmos., 108(D21)doi:10.1029/2002JD003093, 2003. </reference>
		<reference numeration="46" content_type="text"> Sullivan, R. C., Guazzotti, S. A., Sodeman, D. A., and Prather, K. A.: Direct observations of the atmospheric processing of Asian mineral dust, Atmos. Chem. Phys., 7, 1213–1236, 2007. </reference>
		<reference numeration="47" content_type="text"> 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, 3148–3155, 2006. </reference>
		<reference numeration="48" content_type="text"> Tang, I. N. and Fung, K. H.: Hydration and Raman scattering studies of levitated microparticles: Ba(NO$_3)_2$, Sr(NO$_3)_2$, and Ca(NO$_3)_2$, J. Phys. Chem., 106, 1653–1660, 1997. </reference>
		<reference numeration="49" content_type="text"> Tegen, I., Koch, D., Lacis, A. A., and Sato, M.: Trends in tropospheric aerosol loads and corresponding impact on direct radiative forcing between 1950 and 1990: A model study, J. Geophys. Res.-Atmos., 105, 26 971–26 989, 2000. </reference>
		<reference numeration="50" content_type="text"> Ullerstam, M., Johnson, M. S., Vogt, R., and Ljungström, E.: DRIFTS and Knudsen cell study of the heterogeneous reactivity of SO&lt;sub&gt;2&lt;/sub&gt; and NO&lt;sub&gt;2&lt;/sub&gt; on mineral dust, Atmos. Chem. Phys., 3, 2043–2051, 2003. </reference>
		<reference numeration="51" content_type="text"> Underwood, G. M., Song, C. H., Phadnis, M., Carmichael, G. R., and Grassian, V. H.: Heterogeneous reactions of NO&lt;sub&gt;2&lt;/sub&gt; and HNO&lt;sub&gt;3&lt;/sub&gt; on oxides and mineral dust: A combined laboratory and modeling study, J. Geophys. Res.-Atmos., 106, 18 055–18 066, 2001. </reference>
		<reference numeration="52" content_type="text"> Usher, C. R., Michel, A. E., and Grassian, V. H.: Reactions on mineral dust, Chem. Rev., 103, 4883–4939, 2003. </reference>
		<reference numeration="53" content_type="text"> Vlasenko, A., Sjogren, S., Weingartner, E., Stemmler, K., Gäggeler, H. W., and Ammann, M.: Effect of humidity on nitric acid uptake to mineral dust aerosol particles, Atmos. Chem. Phys., 6, 2147–2160, 2006. </reference>
		<reference numeration="54" content_type="text"> Wang, Y., Zhuang, G. S., Sun, Y. L., and An, Z. S.: The variation of characteristics and formation mechanisms of aerosols in dust, haze, and clear days in Beijing, Atmos. Environ., 40, 6579–6591, 2006. </reference>
		<reference numeration="55" content_type="text"> Xu, J., Bergin, M. H., Greenwald, R., Schauer, J. J., Shafer, M. M., Jaffrezo, J. L., and Aymoz, G.: Aerosol chemical, physical, and radiative characteristics near a desert source region of northwest China during ACE-Asia, J. Geophys. Res.-Atmos., 109, D19S03, doi:10.1029/2003JD004239, 2004. </reference>
		<reference numeration="56" content_type="text"> Zhang, D. Z. and Iwasaka, Y.: Nitrate and sulfate in individual Asian dust-storm particles in Beijing, China in spring of 1995 and 1996, Atmos. Environ., 33, 3213–3223, 1999. </reference>
		<reference numeration="57" content_type="text"> Zhang, D. Z., Shi, G. Y., Iwasaka, Y., and Hu, M.: Mixture of sulfate and nitrate in coastal atmospheric aerosols: individual particle studies in Qingdao (36 degrees 04&apos; N, 120 degrees 21&apos; E), China, Atmos. Environ., 34, 2669–2679, 2000. </reference>
		<reference numeration="58" content_type="text"> Zhang, Q., Streets, D. G., He, K., Wang, Y., Richter, A., Burrows, J. P., Uno, I., Jang, C. J., Chen, D., Yao, Z., and Lei, Y.: NO&lt;sub&gt;x&lt;/sub&gt; emission trends for China, 1995–2004: The view from the ground and the view from space, J. Geophys. Res.-Atmos., 112, D22306, doi:10.1029/2007JD008684, 2007. </reference>
		<reference numeration="59" content_type="text"> Zhang, X. Y., Gong, S. L., Shen, Z. X., Mei, F. M., Xi, X. X., Liu, L. C., Zhou, Z. J., Wang, D., Wang, Y. Q., and Cheng, Y.: Characterization of soil dust aerosol in China and its transport and distribution during 2001 ACE-Asia: 1. Network observations, J. Geophys. Res.-Atmos., 108(D9)4261, doi:10.1029/2002JD002632, 2003. </reference>
	</references>
</article>

