References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-10-63-2010

Constraint of anthropogenic NOx emissions in China from different sectors: a new methodology using multiple satellite retrievals

Lin

J.-T.

¹ McElroy

M. B.

¹ Boersma

K. F.

School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138, USA

KNMI, Climate Observations Department, De Bilt, The Netherlands

07 01 2010

10 1 63 78

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A new methodology is developed to constrain Chinese anthropogenic emissions of nitrogen oxides (NOx) from four major sectors (industry, power plants, mobile and residential) in July 2008. It combines tropospheric NO2 column retrievals from GOME-2 and OMI, taking advantage of their different passing time over China (~10:00 a.m. LT (local time) versus ~02:00 p.m.) and consistent retrieval algorithms. The approach is based on the difference of NOx columns at the overpass times of the two instruments; it thus is less susceptible to the likely systematic errors embedded in individual retrievals that are consistent with each other. Also, it explicitly accounts for diurnal variations and uncertainties of NOx emissions for individual sources. Our best top-down estimate suggests a national budget of 6.8 TgN/yr (5.5 TgN/yr for East China), close to the a priori bottom-up emission estimate from the INTEX-B mission for the year of 2006. The top-down emissions are lower than the a priori near Beijing, in the northeastern provinces and along the east coast; yet they exceed the a priori over many inland regions. Systematic errors in satellite retrievals are estimated to lead to underestimation of top-down emissions by at most 17% (most likely 10%). Effects of other factors on the top-down estimate are typically less than 15% each, including lightning, soil emissions, mixing in planetary boundary layer, anthropogenic emissions of carbon monoxide and volatile organic compounds, magnitude of a priori emissions, assumptions on emission diurnal variations, and uncertainties in the four sectors. The a posteriori emission budget is 5.7 TgN/yr for East China.

References 1

Acarreta, J. R., De Haan, J. F., and Stammes, P.: Cloud pressure retrieval using the O2-O2 absorption band at 477 nm, J. Geophys. Res., 109, D05204, doi:10.1029/2003jd003915, 2004.

Boersma, K. F., Eskes, H. J., and Brinksma, E. J.: Error analysis for tropospheric NO2 retrieval from space, J. Geophys. Res., 109, D04311, doi:10.1029/2003jd003962, 2004.

Boersma, K. F., Eskes, H. J., Veefkind, J. P., Brinksma, E. J., van der A, R. J., Sneep, M., van den Oord, G. H. J., Levelt, P. F., Stammes, P., Gleason, J. F., and Bucsela, E. J.: Near-real time retrieval of tropospheric NO2 from OMI, Atmos. Chem. Phys., 7, 2103–2118, 2007.

Boersma, K. F., Jacob, D. J., Bucsela, E. J., Perring, A. E., Dirksen, R., van der A, R. J., Yantosca, R. M., Park, R. J., Wenig, M. O., Bertram, T. H., and Cohen, R. C.: Validation of OMI tropospheric NO2 observations during INTEX-B and application to constrain NOx emissions over the eastern United States and Mexico, Atmos. Environ., 42, 4480–4497, doi:10.1016/j.atmosenv.2008.02.004, 2008a.

Boersma, K. F., Jacob, D. J., Eskes, H. J., Pinder, R. W., Wang, J., and van der A, R. J.: Intercomparison of SCIAMACHY and OMI tropospheric NO2 columns: Observing the diurnal evolution of chemistry and emissions from space, J. Geophys. Res., 113, D16S26, doi:10.1029/2007jd008816, 2008b.

Boersma, K. F., Dirksen, R., Veefkind, J. P., Eskes, H. J., and van der A, R. J.: Dutch OMI~NO2 (DOMINO) data product HE5 data file user manual, 2009a.

Boersma, K. F., Jacob, D. J., Trainic, M., Rudich, Y., DeSmedt, I., Dirksen, R., and Eskes, H. J.: Validation of urban NO2 concentrations and their diurnal and seasonal variations observed from the SCIAMACHY and OMI sensors using in situ surface measurements in Israeli cities, Atmos. Chem. Phys., 9, 3867–3879, 2009.

Cao, J., Ho, M. S., Lei, Y., Nielsen, C. P., Wang, Y. X., and Zhao, Y.: Reconciling Control of Carbon and Air Pollution with Economic Growth in China: Interim Report on Carbon Tax, Report of the Harvard China Project to the China Sustainable Energy Program of the Energy Foundation, Tsinghua University, Harvard University, Cambridge, MA, US, 2009.

Chen, D., Wang, Y., McElroy, M. B., He, K., Yantosca, R. M., and Le Sager, P.: Regional CO pollution and export in China simulated by the high-resolution nested-grid GEOS-Chem model, Atmos. Chem. Phys., 9, 3825–3839, 2009.

Hains, J., Boersma, F., Kroon, M., Dirksen, R., Volten, H., Swart, D., Richter, A., Wittrock, F., Schoenhardt, A., Wagner, T., Ibrahim, O., Roozendael, M. V., Pinardi, G., Gleason, J., Veefkind, P., and Levelt, P.: Testing and improving OMI DOMINO tropospheric NO2 using observations from the DANDELIONS and INTEX-B validation campaigns, J. Geophys. Res., doi:10.1029/2009JD012399, in press, 2009.

Holtslag, A. A. M. and Boville, B. A.: Local versus nonlocal boundary-layer diffusion in a global climate model, J. Climate, 6, 1825–1842, 1993.

Jaégle, L., Steinberger, L., Martin, R. V., and Chance, K.: Global partitioning of NOx sources using satellite observations: Relative roles of fossil fuel combustion, biomass burning and soil emissions, Faraday Discuss., 130, 407–423, doi:10.1039/b502128f, 2005.

Lamsal, L., Martin, R., and Donkelaar, A. V.: Seasonal variation in nitrogen oxides at northern midlatitudes as inferred from ground-based and satellite-based observations, GEOS-Chem Meeting, 8~April, 2009a.

Lamsal, L. N., Martin, R. V., van Donkelaar, A., Celarier, E. A., Bucsela, E. J., Boersma, K. F., Dirksen, R., Luo, C., and Wang, Y.: Indirect Validation of Tropospheric Nitrogen Dioxide Retrieved from the OMI Satellite Instrument: Insight into the Seasonal Variation of Nitrogen Oxides at Northern Midlatitudes, J. Geophys. Res., doi:10.1029/2009JD013351, in press, 2009b.

Lin, J. T. and McElroy, M. B.: Impacts of boundary layer mixing on pollutant vertical profiles in the lower troposphere: Implications to satellite remote sensing, Atmos. Environ., submitted, 2009.

Lin, J. T., Wuebbles, D. J., and Liang, X. Z.: Effects of intercontinental transport on surface ozone over the United States: Present and future assessment with a global model, Geophys. Res. Lett., 35, L02805, doi:10.1029/2007gl031415, 2008a.

Lin, J. T., Youn, D., Liang, X. Z., and Wuebbles, D. J.: Global model simulation of summertime US ozone diurnal cycle and its sensitivity to PBL mixing, spatial resolution, and emissions, Atmos. Environ., 42, 8470–8483, doi:10.1016/j.atmosenv.2008.08.012, 2008b.

Martin, R. V., Jacob, D. J., Chance, K., Kurosu, T. P., Palmer, P. I., and Evans, M. J.: Global inventory of nitrogen oxide emissions constrained by space-based observations of NO2 columns, J. Geophys. Res., 108, 4537, doi:10.1029/2003jd003453, 2003.

Martin, R. V., Sioris, C. E., Chance, K., Ryerson, T. B., Bertram, T. H., Wooldridge, P. J., Cohen, R. C., Neuman, J. A., Swanson, A., and Flocke, F. M.: Evaluation of space-based constraints on global nitrogen oxide emissions with regional aircraft measurements over and downwind of eastern North America, J. Geophys. Res., 111, D15308, doi:10.1029/2005jd006680, 2006.

McElroy, M. B. and Wang, Y. X. X.: Human and animal wastes: Implications for atmospheric N2O and NOx, Global Biogeochem.l Cy., 19, GB2008, doi10.1029/2004gb002429, 2005.

Mijling, B., Boersma, K. F., Roozendael, M. V., DeSmedt, I., and Kelder, H. M.: Reductions of NO2 detected from space during the 2008 Beijing Olympic Games, Geophys. Res. Lett., 36, L13801, doi:10.1029/2009GL038943, 2009.

Pickering, K. E., Wang, Y. S., Tao, W. K., Price, C., and Muller, J. F.: Vertical distributions of lightning NOx for use in regional and global chemical transport models, J. Geophys. Res., 103, 31203–31216, 1998.

Price, C., Penner, J., and Prather, M.: NOx from lightning, 1 Global distribution based on lightning physics, J. Geophys. Res., 102, 5929–5941, 1997.

Richter, A. and Burrows, J. P.: Tropospheric NO2 from GOME measurements, Adv. Space Res., 29, 1673–1683, 2002.

Richter, A., Burrows, J. P., Nuss, H., Granier, C., and Niemeier, U.: Increase in tropospheric nitrogen dioxide over China observed from space, Nature, 437, 129–132, doi:10.1038/nature04092, 2005.

Sauvage, B., Martin, R. V., van Donkelaar, A., Liu, X., Chance, K., Jaeglé, L., Palmer, P. I., Wu, S., and Fu, T.-M.: Remote sensed and in situ constraints on processes affecting tropical tropospheric ozone, Atmos. Chem. Phys., 7, 815–838, 2007.

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, 8809, doi:10.1029/2002jd003093, 2003.

van der A, R. J., Eskes, H. J., Boersma, K. F., Van Noije, T. P. C., Van Roozendael, M., De Smedt, I., Peters, D., and Meijer, E. W.: Trends, seasonal variability and dominant NOx source derived from a ten year record of NO2 measured from space, J. Geophys. Res., 113, D04302, doi:10.1029/2007jd009021, 2008.

Wang, P., Stammes, P., van der A, R., Pinardi, G., and van Roozendael, M.: FRESCO+: an improved O2 A-band cloud retrieval algorithm for tropospheric trace gas retrievals, Atmos. Chem. Phys., 8, 6565–6576, 2008.

Wang, X. P., Mauzerall, D. L., Hu, Y. T., Russell, A. G., Larson, E. D., Woo, J. H., Streets, D. G., and Guenther, A.: A high-resolution emission inventory for eastern China in 2000 and three scenarios for 2020, Atmos. Environ., 39, 5917–5933, doi:10.1016/j.atmonsenv.2005.06.051, 2005.

Wang, Y. X., McElroy, M. B., Martin, R. V., Streets, D. G., Zhang, Q., and Fu, T. M.: Seasonal variability of NOx emissions over east China constrained by satellite observations: Implications for combustion and microbial sources, J. Geophys. Res., 112, D06301, doi:10.1029/2006jd007538, 2007.

Wang, Y. X. X., McElroy, M. B., Wang, T., and Palmer, P. I.: Asian emissions of CO and NOx: Constraints from aircraft and Chinese station data, J. Geophys. Res., 109, D24304, doi:10.1029/2004jd005250, 2004.

Wuebbles, D. J., Lei, H., and Lin, J. T.: Intercontinental transport of aerosols and photochemical oxidants from Asia and its consequences, Environ. Pollut., 150, 65–84, doi:10.1016/j.envpol.2007.06.066, 2007.

Yienger, J. J. and Levy, H.: Empirical-model of global soil-biogenis NO$_\rm x$ emissions, J. Geophys. Res., 100, 11447–11464, 1995.

Zhang, L., Jacob, D. J., Boersma, K. F., Jaffe, D. A., Olson, J. R., Bowman, K. W., Worden, J. R., Thompson, A. M., Avery, M. A., Cohen, R. C., Dibb, J. E., Flock, F. M., Fuelberg, H. E., Huey, L. G., McMillan, W. W., Singh, H. B., and Weinheimer, A. J.: Transpacific transport of ozone pollution and the effect of recent Asian emission increases on air quality in North America: an integrated analysis using satellite, aircraft, ozonesonde, and surface observations, Atmos. Chem. Phys., 8, 6117–6136, 2008.

Zhang, Q., Streets, D. G., He, K., Wang, Y., Richter, A., Burrows, J. P., Uno, I., Jang, C. J., Chen, D., Yao, Z., and Lei, Y.: NOx emission trends for China, 1995–2004: The view from the ground and the view from space, J. Geophys. Res., 112, D22306, doi:10.1029/2007jd008684, 2007.

Zhang, Q., Streets, D. G., and He, K.: Satellite observations of recent power plant construction in Inner Mongolia, China, Geophys. Res. Lett., 36, L15809, doi:10.1029/2009GL038984, 2009.

Zhang, Q., Streets, D. G., Carmichael, G. R., He, K. B., Huo, H., Kannari, A., Klimont, Z., Park, I. S., Reddy, S., Fu, J. S., Chen, D., Duan, L., Lei, Y., Wang, L. T., and Yao, Z. L.: Asian emissions in 2006 for the NASA INTEX-B mission, Atmos. Chem. Phys., 9, 5131–5153, 2009.

Zhao, C. and Wang, Y. H.: Assimilated inversion of NOx emissions over east Asia using OMI~NO2 column measurements, Geophys. Res. Lett., 36, L06805, doi:10.1029/2008gl037123, 2009.

Zhou, Y., Brunner, D., Boersma, K. F., Dirksen, R., and Wang, P.: An improved tropospheric NO2 retrieval for satellite observations in the vicinity of mountainous terrain, Atmos. Meas. Tech. Discuss., 2, 401–416, 2009.