Atmospheric Chemistry and Physics www.atmos-chem-phys.net 1680-7316 1680-7324 8 9 2008 10.5194/acp-8-2387-2008 http://www.atmos-chem-phys.net/8/2387/2008/ http://www.atmos-chem-phys.net/8/2387/2008/acp-8-2387-2008.html http://www.atmos-chem-phys.net/8/2387/2008/acp-8-2387-2008.pdf 2387 2403 2008-05-06 Experimental studies on particle emissions from cruising ship, their characteristic properties, transformation and atmospheric lifetime in the marine boundary layer A. Petzold andreas.petzold@dlr.de J. Hasselbach P. Lauer R. Baumann K. Franke C. Gurk H. Schlager E. Weingartner Dt. Zentrum für Luft- und Raumfahrt, Inst. für Physik der Atmosphäre, Oberpfaffenhofen, 82234 Wessling, Germany MAN Diesel SE, Stadtbachstr. 1, 86135 Augsburg, Germany Institute for Environmental Physics, University of Bremen, Otto-Hahn-Allee 1, 28359 Bremen, Germany Max-Planck-Institute for Chemistry, Johann-Joachim-Becher-Weg 27, 55128 Mainz, Germany Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, CH-5232 Villigen PSI, Switzerland Particle emissions from ship engines and their atmospheric transformation in the marine boundary layer (MBL) were investigated in engine test bed studies and in airborne measurements of expanding ship plumes. During the test rig studies, detailed aerosol microphysical and chemical properties were measured in the exhaust gas of a serial MAN B&W seven-cylinder four-stroke marine diesel engine under various load conditions. The emission studies were complemented by airborne aerosol transformation studies in the plume of a large container ship in the English Channel using the DLR aircraft Falcon 20 E-5. Observations from emission studies and plume studies combined with a Gaussian plume dispersion model yield a consistent picture of particle transformation processes from emission to atmospheric processing during plume expansion. Particulate matter emission indices obtained from plume measurements are 8.8±1.0×1015(kg fuel)−1 by number for non-volatile particles and 174±43 mg (kg fuel)−1 by mass for Black Carbon (BC). Values determined for test rig conditions between 85 and 110% engine load are of similar magnitude. For the total particle number including volatile compounds no emission index can be derived since the volatile aerosol fraction is subject to rapid transformation processes in the plume. Ship exhaust particles occur in the size range Dp<0.3 μm, showing a bi-modal structure. The combustion particle mode is centred at modal diameters of 0.05 μm for raw emissions to 0.10 μm at a plume age of 1 h. The smaller-sized volatile particle mode is centred at Dp≤0.02 μm. From the decay of ship exhaust particle number concentrations in an expanding plume, a maximum plume life time of approx. 24 h is estimated for a well-mixed marine boundary layer. Andreae, M. O. and Gelencser, A.: Black carbon or brown carbon?, Atmos. Chem. Phys., 6, 3131–3148, 2006. Beirle, S., Platt, U., von Glasow, R., Wenig, M., and Wagner, T.: Estimate of nitrogen oxide emissions from shipping by satellite remote sensing, Geophys. Res. Lett., 31, L18102, doi:10.1029/2004GL020312, 2004. Bond, T. C., Anderson, T. L., and Campbell, D.: Calibration and intercomparison of filter-based measurements of visible light absorption by aerosols, Aerosol Sci. Technol., 30, 582–600, 1999. Bond, T. C. and Bergstrom, R. W.: Light absorption by carbonaceous particles: An investigative review, Aerosol Sci. Technol., 40, 27–67, 2006. Burtscher, H., Baltensperger, U., Bukowiecki, N., Cohn, P., Hüglin, C., Mohr, M., Matter, M., Nyeki, S., Schmatloch, V., Streit, N., and Weingartner, E.: Separation of volatile and non-volatile aerosol fractions by thermodesorption: Instrument development and applications, J. Aerosol Sci., 32, 427–442, 2001. Capaldo, K., Corbett, J. J., Kasibhatla, P., Fischbeck, P. S. and Pandis, S. N.: Effects of ship emissions on sulfur cycling and radiative climate forcing over the ocean, Nature, 400, 743–746, 1999. Chen, G., Huey, G., Trainer, M., et al.: An investigation of the chemistry of ship emission plumes during ITCT 2002, J. Geophys. Res. 110, doi:10.1029/2004JD005236, 2005. Cooper, D. A.: Exhaust emissions from ships at berth, Atmos. Environ., 37, 3817–3830, 2003. Corbett, J. J.: New directions: Designing ship emissions and impacts research to inform both science and policy, Atmos. Environ., 37, 4719–4721, 2003. Corbett, J. J. and Fischbeck, P. S.: Emissions from ships, Science 278, 3723–3731, 1997. Devasthale, A., Krüger, O., and Gragl, H.: Impact of ship emissions n cloud properties over coastal areas, Geophys. Res. Lett., 33, L02811, doi:10.1029/2005GL024470, 2006. Durkee, P. A., Noone, K. J., and Bluth, R. T.: The Monterey Area ship track experiment, J. Atmos. Sci., 57, 2523–2541, 2000a. Durkee, P. A., Chartier, R. E., Brown, A., Trehubenko, E. J., Rogerson, S. D., Skupniewicz, C., Nielsen, K. E., Platnick, S., and King, M. D.: Composite ship track characteristics, J. Atmos. Sci., 57, 2542–2553, 2000b. Dusek, U., Frank, G. P., Hildebrandt, L., Curtius, J., Schneider, J., Walter, S., Chand, D., Drewnick, F., Hungs, S., Jung, D., Borrmann, S., and Andreae, M. O.: Size matters more than chemistry for cloud-nucleating ability of aerosol particles, Science, 312, 1375–1378, 2006. Endresen, Ø., Sørgård, E., Sundet, J. K., Dalsøren, S. B., Isaksen, I. S. A., Berglen, T. F., and Gravir, G.: Emission from international sea transportation and environmental impact, J. Geophys. Res. 108, 4560, doi:10.1029/2002JD002898, 2003. Eyring V., Köhler, H. W., van Aardenne, J., and Lauer, A.: Emissions from international shipping: 1. The last 50 years, J. Geophys. Res., 110, D17305, doi:10.1029/2004JD005619, 2005a. Eyring V., Köhler, H. W., Lauer, A., and Lemper, B.: Emissions from international shipping: 2. Impact of future technologies on scenarios until 2050, J. Geophys. Res., 110, D17306, doi:10.1029/2004JD005620, 2005b. Eyring, V., Stevenson, D S., Lauer, A., et al.: Multi-model simulations of the impact of international shipping on Atmospheric Chemistry and Climate in 2000 and 2030 Atmos. Chem. Phys., 7, 757–780,~2007. Feldpausch, P., Fiebig, M., Fritzsche, L., and Petzold, A.: Measurement of ultrafine aerosol size distributions by a combination of diffusion screen separators and condensation particle counters, J. Aerosol Sci., 37, 577–597, doi:10.1016/j.jaerosci.2005.04.009, 2006. Fiebig, M., Stein, C., Schröder, F., Feldpausch, P., and Petzold, A.: Inversion of data containing information on the aerosol particle size distribution using multiple instruments, J. Aerosol Sci.,36, 1353–1372, 2005. Frick, G. M. and Hoppel, W. A.: Airship measurements of ship's exhaust plumes and their effect on marine boundary layer clouds, J. Atmos. Sci., 57, 2625–2648, 2000. Gopalakrishnan, V., Pawar, S. D., Siinggh, D., and Kamra, A. K.: Intermediate ion formation in ship's exhaust, Geophys. Res. Lett., 32, L11806, doi:10.1029/2005GL022613, 2005. Hobbs, P. V., Garrett, T. J., Ferek, R. J., Strader, S. R., Hegg, D. A., Frick, G. M., Hoppel, W. A., Gasparovic, R. F., Russell, L. M., Johnson, D. W., O'Dowd, C., Durkee, P. A., Nielsen, K. E., and Innis, G.: Emissions from ships with respect to their effects on cloud, J. Atmos. Sci., 57, 2570–2590, 2000. Kasper, A., Aufdenblatten, S., Forss, A., Mohr, M., and Burtscher, H.: Particulate emissions from a low-speed marine diesel engine, Aerosol Sci. Technol., 41, 24–32, 2007. Köhler, H. W.: Worldwide NOx emissions from merchant shipping, paper presented at 24th Annual Marine Propulsion Conference, 10–11 April, Copenhagen, Denmark, 2002. Köhler, H. W.: NOx emissions from ocean-going ships: Calculation and evaluation, paper presented at Spring Technical Conference, Internal Combust. Engine Div., Am. Soc. of Automotive Eng., Salzburg, Austria, 11–14 May, 2003. Lawrence, M. G. and Crutzen, P. J.: Influence of NOx emissions from ships on tropospheric photochemistry and climate, Nature, 402, 167–170, 1999. Lyyränen, J., Jokiniemi, J., Kauppinen, E. I., and Joutsensaari, J.: Aerosol characterisation in medium-speed diesel engines operating with heavy fuel oils, J. Aerosol Sci., 30, 771–784, 1999. Noone K. J., Öström, E., Ferek, R. J., et al.: A case study of ships forming and not forming tracks in moderately polluted clouds, J. Atmos. Sci., 57, 2729–2747, 2000. Osborne, S. O., Johnson, D. W., Bower, K. N., and Wood, R.: Modification of the aerosol size distribution within exhaust plumes produced by diesel-powered ships, J. Geophys. Res., 106, 9827–9842, 2001. Petzold, A., Feldpausch, P., Fritzsche, L., Minikin, A., Lauer, P., Kurok, C., and Bauer, H.: Particle emissions from ship engines, J. Aerosol Sci., Abstracts of the European Aerosol Conference, S1095–S1096, 2004. Petzold, A. and Schönlinner, M.: Multi-angle absorption photometry – a new method for the measurement of aerosol light absorption and atmospheric black carbon, J. Aerosol Sci., 35, 421–441, 2004. Petzold, A., Gysel, M. , Vancassel, X. , Hitzenberger, R. , Puxbaum, H., Vrochticky, S., Weingartner, E. , Baltensperger, U., and Mirabel, P.: On the effects of organic matter and sulphur-containing compounds on the CCN activation of combustion particles, Atmos. Chem. Phys., 5, 3187–3203, 2005. Petzold, A., Weinzierl, B., Fiebig, M., Lichtenstern, M., Lauer, P., Gurk, C., Franke, K., and Weingartner, E.: Particle Emissions from Ship Engines: Emission Properties and Transformation in the Marine Boundary Layer, Proceedings of the International Conference on Transport, Atmosphere and Climate, Oxford, June 2006, TAC Extended Abstracts, 2007. Petzold, A., Weinzierl, B., Huntrieser, H., Stohl, A., Real, E., Cozic, J., Fiebig, M., Hendricks, J., Lauer, A., Law, K., Minikin, A., Roiger, A., Schlager, H., and Weingartner, E.: Perturbation of European Free Troposphere Aerosol by North American Forest Fire Plumes during the ICARTT-ITOP Experiment in Summer 2004, Atmos. Chem. Phys., 7, 5105–5127, 2007. Schlager, H., Baumann, R., Lichtenstern, M., Petzold, A., Arnold, F. , Speidel, M., Gurk, C., and Fischer, H.: Aircraft-based Trace Gas Measurements in a Primary European Ship Corridor, Proceedings of the International Conference on Transport, Atmosphere and Climate, Oxford, June 2006, TAC Extended Abstracts, 2007 Schmid, H., Laskus, L., Abraham, H. J., Baltensperger, U., Lavanchy, V., Bizjak, M., Burba, P., Cachier, H., Crow, D., Chow, J., et al.: Results of the "carbon conference" international aerosol carbon round robin test stage I., Atmos. Environ., 35, 2111–2121, 2001. Schröder, F. P. and Ström, J.: Aircraft measurements of sub micrometer aerosol particles ($>$7 nm) in the midlatitude free troposphere and tropopause region, Atmos. Res., 44, 333–356, 1997. Sinha, P., Hobbs, P. V., Yokelson, R. J., Christian, T. J., Kirchstetter, T. W., and Bruintjes, R.: Emission of trace gases and particles from two ships in the southern Atlantic Ocean, Atmos. Environ., 37, 2139–2148, 2003. Song, C. H., Chen, G., Hanna, S. R., Crawford, J., Davis, D. D.: Dispersion and chemical evolution of ship plumes in the marine boundary layer: Investigation of O3/NOy/HOx chemistry, J. Geophys. Res. 108, 4143, doi:10.1029/2002JD002216, 2003. Ulrich, E. W.: Entwicklung eines thermografischen Verfahrens zur Analyse von Dieselpartikelemissionen (Development of a thermographic method for the analysis of diesel particulate matter), PhD Thesis, Technical University of Berlin, Berlin 1994. VDI Guideline 2465 – 2: Measurement of soot (ambient air) – Thermographical determination of elemental carbon after thermal desorption of organic carbon, VDI/DIN – Reinhaltung der Luft, Beuth, Berlin, 2005. von Glasow, R., Lawrence, M. G., Sander, R., and Crutzen, P. J.: Modelling the chemical effects of ship exhaust in the cloud-free marine boundary layer, Atmos. Chem. Phys., 3, 233–250, 2003. Williams, E., Lerner, B., Quinn, P., and Bates, T.: Measurements of gas and particle emissions from commercial marine vessels, Eos Trans. AGU, 86(52), Fall Meet. Suppl., Abstract A51E-0130, 2005.