Atmospheric Chemistry and Physics Discussions www.atmos-chem-phys-discuss.net 1680-7367 1680-7375 8 4 2008 10.5194/acpd-8-13159-2008 http://www.atmos-chem-phys-discuss.net/8/13159/2008/ http://www.atmos-chem-phys-discuss.net/8/13159/2008/acpd-8-13159-2008.html http://www.atmos-chem-phys-discuss.net/8/13159/2008/acpd-8-13159-2008.pdf 13159 13195 2008-07-10 Regional-scale modeling of near-ground ozone in the Central East China, source attributions and an assessment of outflow to East Asia – The role of regional-scale transport during MTX2006 J. Li lijie8074@jamstec.go.jp Z. Wang H. Akimoto K. Yamaji M. Takigawa P. Pochanart Y. Liu Y. Kanaya Frontier Research Center for Global Change, Japan Agency for Marine-Earth Science and Technology, Japan State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry(LAPC), Nansen-Zhu International Research Center (NZC), Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing, People's Republic of China A 3-D regional chemical transport model, the Nested Air Quality Prediction Model System (NAQPMS), with an on-line tracer tagging module was applied to study the source of the near-ground (<1.5 km above ground level) ozone at Mt. Tai (36.25°N, 117.10°E, 1534 m a.s.l.) in Central East China (CEC) during the Mount Tai eXperiment 2006 (MTX2006): regional ozone photochemistry and aerosol studies in Central East China in June, 2006. The model reproduced the temporal and spatial variations of near-ground ozone and other pollutants. In particular, the model captured highly polluted and clean cases well. The simulated near-ground ozone over CEC is 60–85 ppbv (parts per billion by volume), higher than those (20–50 ppbv) in Japan and over the North Pacific. The simulated tagged tracer indicates that the regional-scale transport of chemically produced ozone over other areas in CEC contributes to the most fractions (49%) of the near-ground mean ozone at Mt. Tai in June, rather than the in-situ photochemistry (12%). Due to high anthropogenic and biomass burning emissions, the contributions of the ground ozone from the southern part of CEC plays the most important role (32.4 ppbv, 37.9% of total ozone) in the monthly mean ozone concentration at Mt. Tai, which even reached 59 ppbv (62%) on 6–7 June 2006. The monthly mean horizontal distribution of chemically produced ozone from various source regions indicates that the spatial distribution of O₃ over CEC is controlled by the photochemical reactions. In addition, the regional-scale transport of pollutants also plays an important role in the spatial and temporal distribution of ozone over CEC. The chemically produced ozone from the southern part of the study region can be transported northeastwardly to the northern rim of CEC. The mean contribution is 5–10 ppbv, and it can reach 25 ppbv during high ozone events. This work also studied the outflow of CEC ozone and its precursors, as well as their influences and contributions to the ozone level over adjacent regions/countries. It shows that the contribution of CEC ozone to mean ozone mixing ratios over Korea Peninsula and Japan is 5–15 ppbv, of which about half was due to the direct transport of ozone from CEC and half was contributed by the ozone produced locally by the transported ozone precursors from CEC. Akimoto, H., Ohara, T., Kurokawa, J., and Horii, N.: Verification of energy consumption in China during 1996–2003 by using satellite observational data, Atmos. Environ., 40, 7663–7667, 2006. Brasseur, G., Orlannd, J. J., and Tyndal, G. S.: Atmospheric chemistry and global change, Oxford University Press, New York, USA, 1999. Cao, G., Zhang, X., Wang, D., and Zheng, F.: Inventory of atmospheric pollutants discharged from biomass burning in China continent (in Chinese), China Environmental Science, 25(4), 389–393, 2005. Cheung, V. and Wang, T.: Observational study of ozone pollution at a rural site in the Yangtze Delta of China, Atmos. Environ., 35, 4947–4958, 2001 Crutzen, P. J. and Lawrence, M. G., Poschl, U.: On the background photochemistry of tropospheric ozone, Tellus B, 51A, 126–146, 1999. Davis, D. D., Chen, G., Grawford, J. H., Liu, S., Tan, D., Sandholm, S. T., Jiang, P., Cunnold, D. M., Dinunno, B., Browell, E. V., Grant, W. B., Fenn, M. A., Anerson, B. E., Barrick, J. D., Sachse, G. W., Vay, S. A., Hudgins, H., Avery, M. A., Lefer., B., Shetter, R. E., Heikes, B. G., Blake, D. R., Kondo., Y., and Oltmans, S.: An assessment of western North Pacific ozone photochemistry based on spring obsevations from NASA's PEM-West B (1994) and TRACE-P (2001) field studies, J. Geophys. Res., 108(D21), 8829, doi:10.1029/2002JD003-232, 2003. Derwent, R. G., Stevenson, D. S., Collins, W. J., and Johnson, C. E.: Intercontinental transport and the origins of the ozone observed at surface sites in Europe, Atmos. Environ., 38, 1891–1901, 2004. Ding, A., Wang, T., Thouret, V., Cammas, J.-P., and Nédélec, P.: Tropospheric ozone climatology over Beijing: analysis of aircraft data from the MOZAIC program, Atmos. Chem. Phys., 8, 1–13, 2008. Fu, T. M., Jacob, D. J., Palmer, P. I., Chance, K., Wang, Y. X., Barletta, B., Balke, D. R., Stanton, J. C., and Pilling, M.: Space-based formaldehyde measurements as constraints on volatile organic compound emissions in east and south Asia and implications for ozone, J. Geophys. Res., 112, D06312, doi:10.1029/2006JD007853, 2007. Gao, J., Wang, T., Ding, A., and Liu, C.: Observational study of ozone and carbon monoxide at the summit of mount Tai (1534 m a.s.l.) in central-eastern China, Atmos. Environ., 39, 4779–4791, 2005. Giglio L., Descloitres J., Justice, C. O., and Kaufman, Y. J.: An enhanced contextual fire detection algorithm for MODIS, Remote Sens. Environ, 87(2–3), 273–282, 2003. Grell, G. A., Dudhia, J., and Stauffer, D. R.: A description of the Fifth-Generation Penn State/NCAR Mesoscale Model (MM5), Technical Note: NCAR/TN-398+STR, Natl. Cent. For Atmos. Res., Boulder, CO, USA, 122 pp., 1994. Guenther, A., Hewitt, C. N., Erickson, D., Fall, R., Geron, C., Graedel, T., Harley, P., Klinger, L., Lerdau, M., McKay, W. A., Scholes, B., Steinbrecher, R., Tallamraju, R., Taylor, J., and Zimmerman, P.: A global model of natural volatile organic compound emissions, J. Geophys. Res., 100(D5), 8873–8892, 1995. He, Y., Uno, I., Wang, Z., Ohara, T., Sugimoto, N., Shimizu, A., Richter, and A., Burrows, J.: Variations of the increasing trend of tropospheric NO₂ over central east China during the past decade, Atmos. Environ., 41, 4865–4876, 2007. Intergovernmental Panel on Climate Change (IPCC): Climate Change 1995: the Science of Climate Change, edited by: Houghton, J. T., Ding, Y., Griggs, D. J., Noguer, M., van der Linden, P. J., Dai, X., Maskell, K., and Johnson, C. A., Cambridge Univ. Press, New York, USA, 1996. Kondo, Y., Nakamyra, K., Chen, G., Takega, N., Koike, M., Miyazaki, Y., Kita, K., Crawford, J., Ko, M., Kawakami, S., Shirai, T., Liley, Wang, Y., and Ogawa, T.: Photochemistry of ozone over western Pacific from winter to spring, J. Geophys. Res., 109, D23S02, doi:10.1029/2004JD004871, 2004. Li, J., Wang, Z., Akimoto, H., Gao, C., Pochanart, P., and Wang, X.: Modeling study of ozone seasonal cycle in lower troposphere over East Asia, J. Geophys. Res., 112, D22S25, doi:10.1029/2006JD008209, 2007. Liu, H., Jacob, D., Bey, I., Yantosca, R. M., and Duncan, B.: Transport pathways for Asian pollution outflow over the Pacific: Interannual and seasonal variations, J. Geophys. Res., 108(D20), 8786, doi:10.1029/2002-JD003102, 2003. Liu, H., Jacob, D., Bey, I., Yantosca, R. M., and Duncan, B.: Transport pathways for Asian pollution outflow over the Pacific: Interannual and seasonal variations, J. Geophys. Res., 108(D20), 8786, doi:10.1029/2002-JD003102, 2003. Naja, M., Akimoto, H.: Contribution of regional pollution and long-range transport to the Asia-Pacific region: Analysis of long-term ozonesonde data over Japan, J. Geophys. Res., 109(D2), D21306, doi:10.1029/2004JD004687, 2004. Ohara, T., Akimoto, H., Kurokawa, J., Horii, N., Yamaji, K., Yan, X., and Hayasaka, T.: An Asian emission inventory of anthropogenic emission sources for the period 1980–2020, Atmos. Chem. Phys., 7, 4419–4444, 2007. Pochanart, P., Hirokawa, J., Kajii, Y., and Akimoto, H.: Influence of regional-scale anthropogenic activity in northeast Asia on seasonal variations of surface ozone and carbon monoxide observed at Oki, Japan, J. Geophys. Res., 109(D3), 3621–3631, 1999. Pochanart, P., Kato, N., Katsuno, T., and Akimoto, H.: Eurasian continental background and regionally polluted levels of ozone and CO observed in northeast Asia, Atmos. Environ., 38, 1325–1336, 2004. Richter, A., Burrows, J. P., Nüß, H., Granier, C., and Niemeier, U.: Increase in tropospheric nitrogen dioxide over China observed from space, Nature, 437, 129–132, 2005. 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., 108(D21), 8809, doi:10.1029/2002JD003093, 2003. Streets, D. G. and Waldhoff, S. T.: Present and future emissions of air pollutants in China: SO₂, NO_x, and CO, Atmos. Environ., 34, 363–374, 2000. Sudo, K. and Akimoto, H.: Global source attribution of tropospheric ozone: long-range transport from various source regions, J. Geophys. Res., 112, D12302, doi:10.1029/2006JD007992, 2007. Sudo, K., Takahashi, M., Kurokawa, J., Akimoto, H.: Chaser: A global chemical model of the troposphere, 1: model description, J. Geophys. Res., 107(D17), 4339, doi:10.1029/2001JD-001113, 2002. Tanimoto H., Wild, O., Kato, S., Furutani, H., Makide, Y., Komazaki, Y., Hashimoto, S., Tanaka, S., and Akimoto, H.: Seasonal cycles of ozone and oxidized nitrogen species in northeast Asia, 2: a model analysis of the roles of chemistry and transport, J. Geophys. Res., 107(D23), 4706, doi:10.1029/2001JD001497, 2002. Van der Werf, G. R., Randerson, J. T., Giglio, L., Collatz, G. J., and Kasibhatla, P. S.: Interannual variability in global biomass burning emission from 1997 to 2004, Atmos. Chem. Phys., 6, 3423–3441, 2006. Waleck, C. J. and Aleksic, N. M.: A simple but accurate mass conservative peak-preserving, mixing ratio bounded advection algorithm with Fortran code, Atmos. Environ., 32, 3863–3880, 1998. Wang, T., Ding, A., Gao, J., and Wu, W.: Strong ozone production in urban plumes from Beijing, China, Geophys. Res. Lett., 33, L21806, doi:10.1029/2006-GL027689, 2006a. Wang, T., Vincent, T. F., Cheung, M. A., and Li, Y. S.: Ozone and related gaseous pollutants in the boundary layer of eastern China: overview of the recent measurements at a rural site, Geophys. Res. Lett., 28, 2373–2376, 2001a. Wang, Y., Jacob, D., and Logan, J.: Global simulation of tropospheric O₃-NO_x-hydrocarbon chemistry, 3: origin of tropospheric ozone and effects of nonmethane hydrocarbons, J. Geophys. Res., 103(D9), 10 757–10 768, 1998. Wang, Y., McElroy, M. B., Wang, T., and Palmer, P.: Asian emissions of CO and NO_x constraints from aircraft and Chinese station data, J. Geophys. Res., 109, D24304, doi:610.1029/2004JD005250, 2004. Wang, Z., Akimoto, H., and Uno, I.: Neutralization of soil aerosol and its impact on the distribution of acid rain over East Asia: observations and model results, J. Geophys. Res., 107(D19), 4389, doi:10.1029/2001JD-001040, 2002. Wang, Z., Huang, M., He, D., Xu, H., and Zhou, L.: Sulfur distribution and transport studies in East Asia using Eulerian model, Advance of Atmospheric Science, 13, 399–409, 1996. Wang, Z., Li, J., Wang, X., Pochanart, P., and Akimoto, H.: Modeling of regional high ozone episode observed at two mountain sites (Mt. Tai and Huang) in East China, J. Atmos. Chem., 55(3), 253–272, 2006b. Wang Z., Maeda, T., Hayashi, M., Hsiao, L. F., and Liu, K. Y.: A nested air quality prediction modeling system for urban and regional scales, application for high-ozone episode in Taiwan, Water, Air, and Soil Pollut., 130, 391–396, 2001b. Wang Z., Ueda, H., and Huang, M.: A deflation module for use in modeling long-range transport of yellow sand over East Asia, J. Geophys. Res., 104, 26 947–26 960, 2000. Wesely, M. L.: Parameterization of surface resistances to gaseous dry deposition in regional-scale numerical models, Atmos. Environ., 23, 1293–1304, 1989. Xu, X., Lin, W., Wang, T., Yan, P., Tang, J., Meng, Z., and Wang, Y.: Long-term trend of surface ozone at a regional background station in eastern China 1991–2006: enhanced variability, Atmos. Chem. Phys., 8, 2595–2607, 2008. Yamaji, K., Ohara, T., Uno, I., Tanimoto, H., Kurokawa, J., and Akimoto, H.: Analysis of the seasonal variation of ozone in the boundary layer in East Asia using the Community Multi-scale Air Quality model: what controls surface ozone levels over Japan?, Atmos. Environ., 40, 1856–1868, 2006. Zaveri, R. A. and Peters, L. K.: A new lumped structure photochemical mechanism for large-scale applications, J. Geophys. Res., 104, 30 387–30 415, 1999. Zhang, M., Uno, I., Carmichael, G. R, Akimoto, H., Wang, Z. F., Tang, Y. H., Woo, J. H., Streets, D. J., Sachse, G.W., Avery, M. A., Weber, R. J., and Talbot, R. W.: Large-scale structure of trace gas and aerosol distributions over the western Pacific Ocean during the Transport and Chemical Evolution Over the Pacific (TRACE-P) experiment, J. Geophys. Res., 108(D21), 8820, doi:610.1029/2002JD002946, 2003. Zhu, B., Akimoto, H., Wang, Z., Sudo, K., Tang, J., and Uno, I.: Why does surface ozone peak in summertime at Waliguan?, Geophys. Res. Lett., 31, L17104, doi:10.1029/2004GL020609, 2004.