References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-8-91-2008

The interaction of N2O5 with mineral dust: aerosol flow tube and Knudsen reactor studies

Wagner

¹ Hanisch

¹ ² Holmes

¹ ³ de Coninck

¹ ⁴ Schuster

¹ Crowley

J. N.

Max-Planck-Institut für Chemie, Mainz, Germany

now at: Bayerisches Staatsministerium für Umwelt, Gesundheit und Verbraucherschutz, Rosenkavalierplatz 2, 81925 München, Germany

now at: International Laboratory for Air Quality and Health, QUT Gardens Point, 2 George Street, Brisbane, 4001 QLD, Australia

now at: Unit Policy Studies of the Energy research Centre of the Netherlands, (ECN), VU University of Amsterdam (IVM), Radarweg 60, 1040 AW Amsterdam, The Netherlands

14 01 2008

8 1 91 109

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The interaction of mineral dust with N2O5 was investigated using both airborne mineral aerosol (using an aerosol flow reactor with variable relative humidity) and bulk samples (using a Knudsen reactor at zero humidity). Both authentic (Saharan, SDCV) and synthetic dust samples (Arizona test dust, ATD and calcite, CaCO3) were used to derive reactive uptake coefficients (γ). The aerosol experiments (Saharan dust only) indicated efficient uptake, with e.g. a value of γ(SDCV)=(1.3±0.2)×10−2 obtained at zero relative humidity. The values of γ obtained for bulk substrates in the Knudsen reactor studies are upper limits due to assumptions of available surface area, but were in reasonable agreement with the AFT measurements, with: γ(SDCV)=(3.7±1.2)×10−2, γ(ATD)=(2.2±0.8)×10−2 and γ(CaCO3=(5±2)×10−2. The errors quoted are statistical only. The results are compared to literature values and assessed in terms of their impact on atmospheric N2O5.

References 1

Aldener, M., Brown, S. S., Stark, H., Williams, E. J., Lerner, B. M., Kuster, W. C., Goldan, P. D., Quinn, P. K., Bates, T. S., Fehsenfeld, F. C., and Ravishankara, A. R.: Reactivity and loss mechanisms of NO3 and N2O$_5$ in a polluted marine environment: Results from in situ measurements during New England Air Quality Study 2002, J. Geophys. Res., 111, D23S73, doi:10.1029/2006JD007252, 2006.

Alfaro, S. C., Gomes, L., Rajot, J. L., Lafon, S., Gaudichet, A., Chatenet, B., Maille, M., Cautenet, G., Lasserre, F., Cachier, H., and Zhang, X. Y.: Chemical and optical characterization of aerosols measured in spring 2002 at the ACE-Asia supersite, Zhenbeitai, China, J. Geophys. Res., 108, 8461, doi:10.1029/2002JD003214, 2003.

Ansmann, A., Mattis, I., Muller, D., Wandinger, U., Radlach, M., Althausen, D., and Damoah, R.: Ice formation in Saharan dust over central Europe observed with temperature/humidity//aerosol Raman lidar, J. Geophys. Res., 110, D18S12, doi:10.1029/2004JD005000, 2005.

Bauer, S. E., Balkanski, Y., Schulz, M., Hauglustaine, D. A., and Dentener, F.: Global modeling of heterogeneous chemistry on mineral aerosol surfaces: Influence on tropospheric ozone chemistry and comparison to observations, J. Geophys. Res., 109, D02304, doi:10.1029/2003JD003868, 2004.

Bian, H. S. and Zender, C. S.: Mineral dust and global tropospheric chemistry: Relative roles of photolysis and heterogeneous uptake, J. Geophys. Res., 108, 4672, doi:10.1029/2002JD003143, 2003.

Boulter, J. E. and Marschall, J.: Measurement of effective Knudsen diffusion coefficients for powder beds used in heterogeneous uptake experiments, J. Phys. Chem. A, 110, 10 444–10 455, 2006.

Brown, R. L.: Tubular flow reactors with first-order kinetics, J. Res. Nat. Bur. Standards, 83, 1–8, 1978.

Carmichael, G. R., Zhang, Y., Chen, L.-L., Hong, M.-S., and Ueda, H.: Seasonal variation of aerosol composition at Cheju island, Korea, Atmos. Environ., 30, 2407–2416, 1996.

Carstens, T.: Labormessungen kinetischer Parameter zur Beschreibung der Spurengasaufnahme in atmosphphärische Wassertröpfchen, University of Bonn, 1998.

Chartrand, D. J. and McConnell, J. C.: Heterogeneous chemistry and the O3 budget in the lower mid- latitude stratosphere, J. Atmos. Chem., 35, 109–149, 1999.

Chester, R. and Johnson, L. R.: Atmospheric dusts collected off West African coast, Nature, 229, 105–107, 1971.

Curtis, A. R. and Sweetenham, W. P.: Facsimile, AERE, Report R-12805, 1987.

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., 101, 22 869–22 889, 1996.

Dentener, F. J. and Crutzen, P. J.: Reaction of N2O$_5$ on tropospheric aerosols – Impact on the global distributions of NOx, O3, and OH, J. Geophys. Res., 98, 7149–7163, 1993.

Evans, M. J. and Jacob, D. J.: Impact of new laboratory studies of N2O$_5$ hydrolysis on global model budgets of tropospheric nitrogen oxides, ozone, and OH, Geophys. Res. Lett., 32, L09813, doi:10.1029/2005GL022469, 2005.

Fahey, D. W., Eubank, C. S., Hübler, G., and Fehsenfeld, F. C.: A calibrated source of N2O$_5$, Atmos. Environ., 19, 1883–1890, 1985.

Fried, A., Henry, B. E., Calvert, J. G., and Mozurkewich, M.: The Reaction Probability of N2O5 With Sulfuric-Acid Aerosols At Stratospheric Temperatures and Compositions, J. Geophys. Res., 99, 3517–3532, 1994.

Fuchs, N. A. and Sutugin, A. G.: Higly dispersed aerosols, Ann Arbor Sci., Ann Arbor, 1970.

Gobbi, G. P., Barnaba, F., Giorgi, R., and Santacasa, A.: Altitude-resolved properties of Saharan dust event over the mediterranean, Atmos. Environ., 34, 5119–5127, 2000.

Gomes, L. and Gillette, D. A.: A comparison of characteristics of aerosol from dust storms in central Asia with soil-derived dust from other regions, Atmos. Environ., 27A, 2539–2544, 1993.

Grim, R. E.: Clay Mineralogy, McGraw-Hill, New York, 1953.

Gustafsson, R. J., Orlov, A., Badger, C. L., Griffiths, P. T., Cox, R. A., and Lambert, R. M.: A comprehensive evaluation of water uptake on atmospherically relevant mineral surfaces: DRIFT spectroscopy, thermogravimetric analysis and aerosol growth measurements, Atmos. Chem. Phys., 5, 3415–3421, 2005.

Hanisch, F. and Crowley, J. N.: Heterogeneous reactivity of gaseous nitric acid on Al2O3, CaCO3, and atmospheric dust samples: A Knudsen cell study, J. Phys. Chem., 105, 3096–3106, 2001a.

Hanisch, F. and Crowley, J. N.: The heterogeneous reactivity of gaseous nitric acid on authentic mineral dust samples, and on individual mineral and clay mineral components, Phys. Chem. Chem. Phys., 3, 2474–2482, 2001b.

Hanisch, F. and Crowley, J. N.: heterogeneous reactivity of NO and HNO3 on mineral dust in the presence of ozone, Phys. Chem. Chem. Phys., 5, 883–887, 2003a.

Hanisch, F. and Crowley, J. N.: Ozone destruction on Saharan dust: An experimental investigation, Atmos. Chem. Phys., 3, 119–130, 2003b.

Heintz, F., Platt, U., Flentje, H., and Dubois, R.: Long-term observation of nitrate radicals at the Tor station, Kap Arkona (Ruegen), J. Geophys. Res., 101, 22 891–22 910, 1996.

Hendricks, J., Lippert, E., Petry, H., and Ebel, A.: Heterogeneous reactions on and in sulfate aerosols: Implications for the chemistry of the midlatitude tropopause region, J. Geophys. Res., 104, 5531–5550, 1999.

Hinds, W. C.: Aerosol Technology, John Wiley & Sons, New York, 1999.

Hu, J. H. and Abbatt, J. P. D.: Reaction probabilities for N2O$_5$ hydrolysis on sulfuric acid and ammonium sulfate aerosols at room temperature, J. Phys. Chem. A, 101, 871–878, 1997.

Hwang, H. J. and Ro, C. U.: Single-particle characterization of four aerosol samples collected in ChunCheon, Korea, during Asian dust storm events in 2002, J. Geophys. Res., 110, D23201, doi:10.1029/2005JD006050, 2005.

Immler, F. and Schrems, O.: Vertical profiles, optical and microphysical properties of Saharan dust layers determined by a ship-borne lidar, Atmos. Chem. Phys., 3, 1353–1364, 2003.

Karagulian, F. and Rossi, M.J.: The heterogeneous chemical kinetics of NO3 on atmospheric mineral dust surrogates, Phys. Chem. Chem. Phys., 7, 3150–3162, 2005.

Karagulian, F., Santschi, C., and Rossi, M. J.: The heterogeneous chemical kinetics of N2O$_5$ on CaCO3 and other atmospheric mineral dust surrogates, Atmos. Chem. Phys., 6, 1373–1388, 2006.

Keyser, L. F., Moore, S. B., and Leu, M.-T.: Surface-Reaction and Pore Diffusion in Flow-Tube Reactors, J. Phys. Chem., 95, 5496–5502, 1991.

Levin, Z., Price, C., and Ganor, E.: The contribution of sulfate and desert aerosols to the acidification of clouds and rain in Israel, Atmos. Environ., 24A, 1143–1151, 1990.

Lovejoy, E. R. and Hanson, D. R.: Measurement of the kinetics of reactive uptake by submicron sulfuric-acid particles, J. Phys. Chem., 99, 2080–2087, 1995.

Loy\"e-Pilot, M. D., Martin, J. M., and Morelli, J.: Influence of Saharan dust on the rain acidity and atmospheric input to the Mediterranean, Nature, 321, 427–428, 1986.

Lunt, D. J. and Valdes, P. J.: The modern dust cycle: Comparison of model results with observations and study of sensitivities, J. Geophys. Res., 107, 4669, doi:10.1029/2002JD002316, 2002.

Luo, C., Mahowald, N. M., and del Corral, J.: Sensitivity study of meteorological parameters on mineral aerosol mobilization, transport, and distribution, J. Geophys. Res., 108, 4447, doi:10.1029/2003JD003483, 2003.

Martinez, M., Perner, D., Hackenthal, E. M., Kulzer, S., and Schutz, L.: NO3 at Helgoland during the NORDEX campaign in October 1996, J. Geophys. Res., 105, 22 685–22 695, 2000.

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:10.1029/2005GL0244176, 2005.

Meskhidze, N., Chameides, W. L., and Nenes, A.: Dust and pollution: A recipe for enhanced ocean fertilization?, J. Geophys. Res., 110, D03301, doi:10.1029/JD005082, 2005.

Monchick, L. and Mason, E. A.: Transport properties of polar gases, J. Chem. Phys., 35, 1676–1697, 1961.

Mori, I., Nishikawa, M., Tanimura, T., and Quan, H.: Change in size distribution and chemical composition of kosa (Asian dust) aerosol during long-range transport, Atmos. Environ., 37, 4253–4263, 2003.

Nishikawa, M. and Kanamori, S.: Chemical composition of kosa aerosol (yellow sand dust) collected in Japan, Anal. Sci., 7, 1127–1130, 1991.

Okada, K., Kobayashi, A., Iwasaka, Y., Naruse, H., Tanaka, T., and Nemoto, O.: Features of individual Asian dust storm particles collected at Nagoya, Japan, J. Met. Soc. Japan, 65, 515–521, 1987.

Phadnis, M. J. and Carmichael, G. R.: Numerical investigation of the influence of mineral dust on the tropospheric chemistry of East Asia, J. Atmos. Chem., 36, 285–323, 2000.

Prospero, J. M.: Mineral and sea-salt concentrations in various ocean regions, J. Geophys. Res., 84, 725–731, 1979.

Prospero, J. M. and Nees, R. T.: Impact of the North African drought and El Niño on mineral dust in the Barbados trade winds, Nature, 320, 735–738, 1986.

Reus, D. M., Dentener, F., Thomas, A., Borrmann, S., Strom, J., and Lelieveld, J.: Airborne observations of dust aerosol over the North Atlantic Ocean during ACE 2: Indications for heterogeneous ozone destruction, J. Geophys. Res., 105, 15 263–15 275, 2000.

Sander, S. P., Friedl, R. R., Golden, D. M., Kurylo, M. J., Huie, R. E., Orkin, V. L., Moortgat, G. K., Ravishankara, A. R., Kolb, C. E., Molina, M. J., and Finlayson-Pitts, B. J., Chemical kinetics and photochemical data for use in atmospheric studies: Evaluation Number 15, Jet Propulsion Laboratory, National Aeronautics and Space Administration/Jet Propulsion Laboratory/California Institute of Technology, Pasadena, CA, 2006.

Sassen, K., DeMott, P. J., Prospero, J. M., and Poellot, M. R.: Saharan dust storms and indirect aerosol effects on clouds: CRYSTAL-FACE results, Geophys. Res. Lett., 30, 1633, doi:10.1029/2003GL017371, 2003.

Seisel, S., Borensen, C., Vogt, R., and Zellner, R.: Kinetics and mechanism of the uptake of N2O$_5$ on mineral dust at 298 K, Atmos. Chem. Phys., 5, 3423–3432, 2005.

Shon, Z. H., Kim, K. H., Bower, K. N., Lee, G., and Kim, J.: Assessment of the photochemistry of OH and NO3 on Jeju Island during the Asian-dust-storm period in the spring of 2001, Chemosphere, 55, 1127–1142, 2004.

Silva, P. J., Carlin, R. A., and Prather, K. A.: Single particle analysis of suspended soil dust from Southern California, Atmos. Environ., 34, 1811–1820, 2000.

Song, C. H. and Carmichael, G. R.: Gas-particle partitioning of nitric acid modulated by alkaline aerosol, J. Atmos. Chem., 40, 1–22, 2001.

Tegen, I., Harrison, S. P., Kohfeld, K., Prentice, I. C., Coe, M., and Heimann, M.: Impact of vegetation and preferential source areas on global dust aerosol: Results from a model study, J. Geophys. Res., 107, 4567, doi:10.1026/2001JD000963, 2002.

Twomey, S. A., Piepgrass, M., and Wolfe, T.: An assessment of the impact of pollution on global cloud albedo, Tellus, 36B, 243–249, 1984.

Wayne, R. P., Barnes, I., Biggs, P., Burrows, J. P., Canosa-Mas, C. E., Hjorth, J., Le Bras, G., Moortgat, G. K., Perner, D., Poulet, G., Restelli, G., and Sidebottom, H.: The nitrate radical: Physics, chemistry, and the atmosphere, Atmos. Environ., 25A, 1–206, 1991.

Wood, E. C., Bertram, T. H., Wooldridge, P. J., and Cohen, R. C.: Measurements of N2O$_5$, NO2 and O3 east of the San Francisco Bay, Atmos. Chem. Phys., 5, 483–491, 2005.

Zasypkin, A. Y., Grigoreva, V. M., Korchak, V. N., and Gershenson, Y. M.: A formula for summing of kinetic resistances for mobile and stationary media: 1. Cylindrical reactor, Kinet. Catal., 38, 772–781, 1997.

Zhang, Y., Sunwoo, Y., Kotamarthi, V., and Carmichael, G. R.: Photochemical oxidant processes in the presence of dust: An evaluation of the impact of dust on particulate nitrate and ozone formation, J. Appl. Met., 33, 813–824, 1994.