Atmospheric Chemistry and Physics Discussions www.atmos-chem-phys-discuss.net 1680-7367 1680-7375 8 2 2008 10.5194/acpd-8-5537-2008 http://www.atmos-chem-phys-discuss.net/8/5537/2008/ http://www.atmos-chem-phys-discuss.net/8/5537/2008/acpd-8-5537-2008.html http://www.atmos-chem-phys-discuss.net/8/5537/2008/acpd-8-5537-2008.pdf 5537 5561 2008-03-18 Source-receptor relationships between East Asian sulfur dioxide emissions and Northern Hemisphere sulfate concentrations J. Liu D. L. Mauzerall mauzeral@princeton.edu L. W. Horowitz Woodrow Wilson School of Public and Int. Affairs, Princeton Univ., Princeton, NJ, USA Geophysical Fluid Dynamics Laboratory, Princeton, NJ, USA We analyze the effect of varying East Asian (EA) sulfur emissions on sulfate concentrations in the Northern Hemisphere, using a global coupled oxidant-aerosol model (MOZART-2). We conduct a base and five sensitivity simulations, in which sulfur emissions from each continent are tagged, to establish the source-receptor (S-R) relationship between EA sulfur emissions and sulfate concentrations over source and downwind regions. We find that from west to east across the North Pacific, EA sulfate contributes approximately 80%–20% of sulfate at the surface, but at least 50% at 500 hPa. In addition, EA SO₂ emissions account for approximately 30%–50% and 10%–20% of North American background sulfate over the western and eastern US, respectively. The contribution of EA sulfate to the western US at the surface is highest in MAM and JJA, but is lowest in DJF. Reducing EA SO₂ emissions will significantly decrease the spatial extent of the EA sulfate influence over the North Pacific both at the surface and at 500 mb in all seasons, but the extent of influence is insensitive to emission increases, particularly in DJF and JJA. We find that EA sulfate concentrations over most downwind regions respond nearly linearly to changes in EA SO₂ emissions, but sulfate concentrations over the EA source region increase more slowly than SO₂ emissions, particularly at the surface and in winter, due to limited availability of oxidants (mostly H₂O₂). We find that similar estimates of the S-R relationship for trans-Pacific transport of EA sulfate would be obtained using either sensitivity or tagging techniques. Our findings suggest that future changes in EA sulfur emissions may cause little change in the sulfate induced health impact over downwind continents but SO₂ emission reductions may significantly reduce the sulfate related climate cooling over the North Pacific and the United States. Berglen, T. F., Berntsen, T. K., Isaksen, I. S. A., and Sundet, J. K.: A global model of the coupled sulfur/oxidant chemistry in the troposphere: The sulfur cycle, J. Geophys. Res.-Atmos., 109, D19310, doi:10.1029/2003JD003948, 2004. Brasseur, G. P., Orlando, J. J., Tyndall, G. S., and National Center for Atmospheric Research (US): Atmospheric chemistry and global change, Topics in environmental chemistry, Oxford University Press, New York, xviii, 654 pp., 1999. Carlson, C., Burtraw, D., Cropper, M., and Palmer, K. L.: Sulfur dioxide control by electric utilities: What are the gains from trade?, J. Polit. Econ., 108, 1292–1326, 2000. Chin, M., Diehl, T., Ginoux, P., and Malm, W.: Intercontinental transport of pollution and dust aerosols: Implications for regional air quality, Atmos. Chem. Phys., 7, 5501–5517, 2007. Conrad, K. and Kohn, R. E.: The US market for SO₂ permits – policy implications of the low price and trading volume, Energ. Policy, 24, 1051–1059, 1996. Dutkiewicz, V. A., Das, M., and Husain, L.: The relationship between regional SO₂ emissions and downwind aerosol sulfate concentrations in the northeastern US, Atmos. Environ., 34, 1821–1832, 2000. Feichter, J., Kjellstrom, E., Rodhe, H., Dentener, F., Lelieveld, J., and Roelofs, G. J.: Simulation of the tropospheric sulfur cycle in a global climate model, Atmos. Environ., 30, 1693–1707, 1996. Ginoux, P., Horowitz, L. W., Ramaswamy, V., Geogdzhayev, I. V., Holben, B. N., Stenchikov, G., and Tie, X.: Evaluation of aerosol distribution and optical depth in the geophysical fluid dynamics laboratory coupled model CM2.1 for present climate, J. Geophys. Res.-Atmos., 111, D22210, doi:10.1029/2005JD006707, 2006. Giorgi, F., Bi, X. Q., and Qian, Y.: Indirect vs. Direct effects of anthropogenic sulfate on the climate of east Asia as simulated with a regional coupled climate-chemistry/aerosol model, Climatic Change, 58, 345–376, 2003. Gunther, A. J.: A chemical survey of remote lakes of the Alagnak and Aaknek river systems, southwest Alaska, USA, Arctic Alpine Res., 24, 64–68, 1992. Hao, J. M., Wang, S. X., Liu, B. J., and He, K. B.: Plotting of acid rain and sulfur dioxide pollution control zones and integrated control planning in china, Water Air Soil Poll., 130, 259–264, 2001. Heald, C. L., Jacob, D. J., Park, R. J., Alexander, B., Fairlie, T. D., Yantosca, R. M., and Chu, D. A.: Transpacific transport of Asian anthropogenic aerosols and its impact on surface air quality in the United States, J. Geophys. Res.-Atmos., 111, D14310, doi:10.1029/2005JD006847, 2006. Hilst, G. R.: Proportionality between SO₂ emissions and wet SO$_4^2-$ concentrations – the effect of area of averaging, Atmos. Environ. A-Gen., 26, 1413–1420, 1992. Horowitz, L. W., Walters, S., Mauzerall, D. L., Emmons, L. K., Rasch, P. J., Granier, C., Tie, X. X., Lamarque, J. F., Schultz, M. G., Tyndall, G. S., Orlando, J. J., and Brasseur, G. P.: A global simulation of tropospheric ozone and related tracers: Description and evaluation of MOZART, version 2, J. Geophys. Res.-Atmos., 108(D24), 4784, doi:10.1029/2002JD002853, 2003. Horowitz, L. W.: Past, present, and future concentrations of tropospheric ozone and aerosols: Methodology, ozone evaluation, and sensitivity to aerosol wet removal, J. Geophys. Res.-Atmos., 111, D22211, doi:10.1029/2005JD006937, 2006. Jaffe, D., Tamura, S., and Harris, J.: Seasonal cycle and composition of background fine particles along the west coast of the US, Atmos. Environ., 39, 297–306, 2005. Klimont, Z., Cofala, J., Schopp, W., Amann, M., Streets, D. G., Ichikawa, Y., and Fujita, S.: Projections of SO₂, NO_x, NH₃ and VOC emissions in east Asia up to 2030, Water Air Soil Poll., 130, 193–198, 2001. Koch, D., Bond, T. C., Streets, D., and Unger, N.: Linking future aerosol radiative forcing to shifts in source activities, Geophys. Res. Lett., 34, L05821, doi:10.1029/2006GL028360, 2007a. Koch, D., Bond, T. C., Streets, D., Unger, N., and van der Werf, G. R.: Global impacts of aerosols from particular source regions and sectors, J. Geophys. Res.-Atmos., 112, D02205, doi:10.1029/2005JD007024, 2007b. Liu, J. F. and Mauzerall, D. L.: Estimating the average time for inter-continental transport of air pollutants, Geophys. Res. Lett., 32, L11814, doi:10.1029/2005GL022619, 2005. Liu, J. F., Mauzerall, D. L., and Horowitz, L. W.: Analysis of seasonal and inter-annual variability in transpacific transport, J. Geophys. Res.-Atmos., 110, D04302, doi:10.1029/2004JD005207, 2005. Liu, J. F., and Mauzerall, D. L.: Potential influence of inter-continental transport of sulfate aerosols on air quality, Environ. Res. Lett., 2, 045029, doi:10.1088/1748-9326/1082/1084/045029, 2007. Marmer, E., Langmann, B., Fagerli, H., and Vestreng, V.: Direct shortwave radiative forcing of sulfate aerosol over Europe from 1900 to 2000, J. Geophys. Res.-Atmos., 112, D23S17, doi:10.1029/2006JD008037, 2007. Martin, L. R. and Damschen, D. E.: Aqueous oxidation of sulfur-dioxide by hydrogen-peroxide at low ph, Atmos. Environ., 15, 1615–1621, 1981. Moldan, F., Wright, R. F., Lofgren, S., Forsius, M., Ruoho-Airola, T., and Skjelkvale, B. L.: Long-term changes in acidification and recovery at nine calibrated catchments in Norway, Sweden and Finland, Hydrol. Earth Syst. Sc., 5, 339–349, 2001. NAPAP: National acid precipitation assessment program report to congress: An integrated assessment, Washington, DC, 2005. Olivier, J. G. J., Bouwman, A. F., Van der Maas, C. W. M., Berdowski, J. J. M., Veldt, C., Bloos, J. P. J., Visschedijk, A. J. H., Zandveld, P. Y. J., and Haverlag, J. L.: Description of edgar version 2.0: A set of global emission inventories of greenhouse gases and ozone-depleting substances for all anthropogenic and most natural sources on a per country basis and on 1$^\circ\times$1° grid. National institute of public health and the environment, (RIVM) report no. 771060 771002 / TNO-MEP report no. R771096/771119, 1996. Oppenheimer, M., Epstein, C. B., and Yuhnke, R. E.: Acid deposition, smelter emissions, and the linearity issue in the western united-states, Science, 229, 859–862, 1985. Park, R. J., Jacob, D. J., Field, B. D., Yantosca, R. M., and Chin, M.: Natural and trans-boundary pollution influences on sulfate-nitrate-ammonium aerosols in the United States: Implications for policy, J. Geophys. Res.-Atmos., 109, D15204, doi:10.1029/2003JD004473, 2004. Pope, C., Burnett, R., Thun, M., Calle, E., Krewski, D., Ito, K., and Thurston, G.: Lung cancer, cardiopulmonary mortality, and long-term exposure to fine particulate air pollution, Jama – J. Am. Med. Assoc., 287, 1132–1141, 2002. Pope, C., Burnett, R., Thurston, G., Thun, M., Calle, E., Krewski, D., and Godleski, J.: Cardiovascular mortality and long-term exposure to particulate air pollution – epidemiological evidence of general pathophysiological pathways of disease, Circulation, 109, 71–77, 2004. Prospero, J. M.: The atmospheric transport of particles to the ocean, in particle flux in the ocean, edited by Ittekkot, V., Schäfer, P., Honjo, S., and Depetris, P. J., Scope, 57, 19–52, 1996. Prospero, J. M., Savoie, D. L., and Arimoto, R.: Long-term record of nss-sulfate and nitrate in aerosols on midway island, 1981–2000: Evidence of increased (now decreasing?) anthropogenic emissions from Asia, J. Geophys. Res.-Atmos., 108, 4019, doi:10.1029/2001JD001524, 2003. Seinfeld, J. H. and Pandis, S. N.: Atmospheric chemistry and physics: From air pollution to climate change, Wiley, New York, xxvii, 1326 pp., 1998. Streets, D. G.: Dissecting future aerosol emissions: Warming tendencies and mitigation opportunities, Climatic Change, 81, 313–330, 2007. Tie, X. X., Madronich, S., Walters, S., Edwards, D. P., Ginoux, P., Mahowald, N., Zhang, R. Y., Lou, C., and Brasseur, G.: Assessment of the global impact of aerosols on tropospheric oxidants, J. Geophys. Res.-Atmos., 110, D03204, doi:10.1029/2004JD005359, 2005.