Atmospheric Chemistry and Physics www.atmos-chem-phys.net 1680-7316 1680-7324 7 15 2007 10.5194/acp-7-4015-2007 http://www.atmos-chem-phys.net/7/4015/2007/ http://www.atmos-chem-phys.net/7/4015/2007/acp-7-4015-2007.html http://www.atmos-chem-phys.net/7/4015/2007/acp-7-4015-2007.pdf 4015 4025 2007-08-01 GEM/POPs: a global 3-D dynamic model for semi-volatile persistent organic pollutants – Part 2: Global transports and budgets of PCBs P. Huang S. L. Gong T. L. Zhao L. Neary L. A. Barrie Air Quality Research Division, Science & Technology Branch, Environment Canada, 4905 Dufferin Street, Toronto, Ontario M3H 5T4, Canada Dept. of Chemical Engineering and Applied Chemistry, University of Toronto, 200 College Street, Toronto, Ontario, Canada, M5S 3E5, Canada Dept. of Earth and Space Science and Engineering, York University, 4700 Keele Street, Toronto, Ontario, M3J 1P3, Canada Atmospheric Research and Environment Program, World Meteorological Organization, 7 bis, avenue de la Paix, BP2300, 1211 Geneva 2, Switzerland Global transports and budgets of three PCBs were investigated with a 3-D dynamic model for semi-volatile persistent organic pollutants – GEM/POPs. Dominant pathways were identified for PCB transports in the atmosphere with a transport flux peaking below 8 km for gaseous and 14 km for particulate PCB28, and peaking below 4 km for gaseous and 6 km for particulate PCB180. The inter-continental transports of PCBs in the Northern Hemisphere (NH) are dominated in the zonal direction with their route changes regulated seasonally by the variation of westerly jet. The transport pathways from Europe and North Atlantic contributed the most PCBs to the Arctic. Inter-hemispheric transports of PCBs originated from the regions of Europe, Asia and North America in three different flow-paths, accompanying with easterly jet, Asian monsoon winds and trade winds. PCBs from the Southern Hemisphere (SH) could also be exported into the NH. According to the PCB emissions of year 2000, Europe, North America and Asia are the three largest sources of the three PCBs, contributing to the global background concentrations in the atmosphere, soil and water. Globally, PCB28 in soil and water has become a comparable source to the anthropogenic emissions while heavier PCBs such as PCB153 and 180 are still transporting into soil and water. For all three congeners, particulate PCBs are concentrated in the higher levels than gaseous PCBs. More than half of the particulate PCB28 could reach up to the stratosphere, while most of the heavier counter-parts (PCB153 and PCB180) are stored in the troposphere including boundary layer with more than 99% gaseous PCB180 below 6 km. Breivik, K., Sweetman, A., Pacyna, J. M., and Jones, K. C.: Towards a global historical emission inventory for selected PCB congeners – a mass balance approach 2. Emissions, Sci. Total Environ., 290, 199–224, 2002. Côté, J., Gravel, S., Méthot, A., Patoine, A., Roch, M., and Staniforth, A.: The operational CMC-MRB Global Environmental Multiscale (GEM) model: Part I – Design considerations and formulation, Mon. Wea. Rev., 126, 1373–1395, 1998. Gong, S. L., Barrie, L. A., Blanchet, J.-P., Salzen, K. v., Lohmann, U., Lesins, G., Spacek, L., Zhang, L. M., Girard, E., Lin, H., Leaitch, R., Leighton, H., Chylek, P., and Huang, P.: Canadian Aerosol Module: A size-segregated simulation of atmospheric aerosol processes for climate and air quality models 1. Module development, J. Geophys. Res., 108, 4007, doi:10.1029/2001JD002002, 2003. Gong, S. L., Huang, P., Zhao, T. L., Sahsuvar, L., Barrie, L. A., Kaminski, J. W., Li, Y. F., and Niu, T.: GEM/POPs: A Global 3-D Dynamic Model for Semi-volatile Persistent Organic Pollutants 1. Model description and evaluations, Atmos. Chem. Phys., 2007. \blackbox\bf Will be updated by the Production Office. Hansen, K. M., Christensen, J. H., Brandt, J., Frohn, L. M., and Geels, C.: Modelling atmospheric transport persistent organic pollutants in Northern Hemisphere with a 3-D dynamical model: DEHM-POP, Atmos. Chem. Phys., 4, 1339–1369, 2005. Harrad, S. J., Sewart, A. P., Alcock, R., Boumphrey, R., Burnett, V., Duarte-Davidson, R., Halsall, C., Sanders, G., Waterhouse, K., Wild, S. R., and Jones, K.: Polychlorinated Biphenyls (PCBs) in the British Environment: Sinks, Sources and Temporal Trends, Environ. Pollut., 85, 131–146, 1994. Hung, H., Blanchard, P., Halsall, C. J., Bidleman, T. F., Stern, G. A., Fellin, P., Muir, D. C. G., Barrie, L. A., Jantunen, L. M., Helm, P. A., Ma, J., and Konoplev, A.: Temporal and spatial variabilities of atmospheric polychlorinated biphenyls (PCBs), organochlorine (OC) pesticides and polycyclic aromatic hydrocarbons (PAHs) in the Canadian Arctic: Results from a decade of monitoring, Sci. Total Environ., 342, 119–144, 2005a. Hung, H., Lee, S. C., Wania, F., Blanchard, P., and Brice, K.: Measuring and simulating atmospheric concentration trends of polychlorinated biphenyls in the Northern Hemisphere, Atmos. Environ., 39, 6502–6512, 2005b. Jaward, F. M., Barber, J. L., Booij, K., Dachs, J., Lohmann, R., and Jones, K. C.: Evidence for dynamic air-water coupling and cycling of persistent organic pollutants over the open Atlantic Ocean, Environ. Sci. Technol., 38, 2617–2625, 2004. Jurado, E., Jaward, F., Lohmarm, R., Jones, K. C., Simo, R., and Dachs, J.: Wet deposition of persistent organic pollutants to the global oceans, Environ. Sci. Technol., 39, 2426–2435, 2005. Jurado, E., Jaward, F. M., Lohmann, R., Jones, K. C., Simo, R., and Dachs, J.: Atmospheric dry deposition of persistent organic pollutants to the Atlantic and inferences for the global oceans, Environ. Sci. Technol., 38, 5505–5513, 2004. Koziol, A. S. and Pudykiewicz, J. A.: Global-scale environmental transport of persistent organic pollutants, Chemosphere, 45, 1181–1200, 2001. Ma, J., Daggupaty, S., Harner, T., and Li, Y.-F.: Impacts of Lindane usage in the Canadian prairies on the Great Lakes ecosystem, 1. Coupled atmospheric transport model and modeled concentrations in air and soil, Environ. Sci. Technol., 37(17), 3774–3781, 2003. Mackay, D.: Multimedia Environmental Models: The Fugacity Approach, CRC Press, New York, 2001. Mackay, D., Webster, E., and Gouin, T.: Partitioning, Persistence and Long-Range Transport, in: Chemicals in the Environment: Assessing and Managing Risk, edited by: Hester, R. E. and Harrison, R. M., Royal Society of Chemistry, Cambridge, UK, 2006. MacLeod, M., Riley, W. J., and McKone, T.: Assessing the Influence of Climate Variability on Atmospheric Concentrations of Polychlorinated Biphenyls Using a Global-Scale Mass Balance Model (BETR-Global), Environ. Sci. Technol., 39, 6749–6756, 2005. Malanichev, A., Mantseva, E., Shatalov, V., Strukov, B., and Vulykh, N.: Numerical evaluation of the PCBs transport over the Northern Hemisphere, Environ. Pollut., 128, 279–289, 2004. Semeena, V. S. and Lammel, G.: The significance of the grasshopper effect on the atmospheric distribution of president organic substances, Geophys. Res. Lett., 32, L07804, doi:10.1029/2004GL022229, 2005. Strand, A. and Hov, Ø.: A model strategy for the simulation of chlorinated hydrocarbon distributions in the global environment, Water Air Soil Poll., 86, 283–316, 1996. van Jaarsveld, J. A., van Pul, W. A. J., and de Leeuw, F. A. A. M.: Modelling transport and deposition of persistent organic pollutants in the European region, Atmos. Environ., 31, 1011–1024, 1997. Wania, F.: Assessing the potential of persistent organic chemicals for long-range transport and accumulation in polar regions, Environ. Sci. Technol., 37, 1344–1351, 2003. Wania, F. and Daly, G. L.: Estimating the contribution of degradation in air and deposition to the deep sea to the global loss of PCBs, Atmos. Environ., 36, 5581–5593, 2002. Wania, F., Mackay, D., Li, Y.-F., Bidleman, T. F., and Strand, A.: Global chemical fate of alpha-hexachlorocyclohexane. 1. Evaluation of a global distribution model, Environ. Toxicol. Chem., 18, 1390–1399, 1999. Wania, F. and Su, Y.: Quantifying the Global Fractionation of Polychlorinated Biphenyls, Ambio, 33, 161–168, 2004.