ACP Atmospheric Chemistry and Physics ACP 1680-7324 Copernicus GmbH Göttingen, Germany 10.5194/acp-13-487-2013 The effects of recent control policies on trends in emissions of anthropogenic atmospheric pollutants and CO<sub>2</sub> in China Zhao Y. 1 Zhang J. 2 Nielsen C. P. 3 State Key Laboratory of Pollution Control & Resource Reuse and School of the Environment, Nanjing University, 163 Xianlin Ave., Nanjing, Jiangsu 210023, China Jiangsu Provincial Academy of Environmental Science, 241 West Fenghuang St., Nanjing, Jiangsu 210036, China Harvard China Project, School of Engineering and Applied Sciences, Harvard University, 29 Oxford St, Cambridge, MA 02138, USA 16 01 2013 13 2 487 508 This is an open-access article ditributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited. This article is available from http://www.atmos-chem-phys.net/13/487/2013/acp-13-487-2013.html The full text article is available as a PDF file from http://www.atmos-chem-phys.net/13/487/2013/acp-13-487-2013.pdf

To examine the effects of China's national policies of energy conservation and emission control during 2005–2010, inter-annual emission trends of gaseous pollutants, primary aerosols, and CO<sub>2</sub> are estimated with a bottom-up framework. The control measures led to improved energy efficiency and/or increased penetration of emission control devices at power plants and other important industrial sources, yielding reduced emission factors for all evaluated species except NO<sub>x</sub>. The national emissions of anthropogenic SO<sub>2</sub>, CO, and total primary PM (particulate matter) in 2010 are estimated to have been 89%, 108%, and 87% of those in 2005, respectively, suggesting successful emission control of those species despite fast growth of the economy and energy consumption during the period. The emissions of NO<sub>x</sub> and CO<sub>2</sub>, however, are estimated to have increased by 47% and 43%, respectively, indicating that they remain largely determined by the growth of energy use, industrial production, and vehicle populations. Based on application of a Monte-Carlo framework, estimated uncertainties of SO<sub>2</sub> and PM emissions increased from 2005 to 2010, resulting mainly from poorly understood average SO<sub>2</sub> removal efficiency in flue gas desulfurization (FGD) systems in the power sector, and unclear changes in the penetration levels of dust collectors at industrial sources, respectively. While emission trends determined by bottom-up methods can be generally verified by observations from both ground stations and satellites, clear discrepancies exist for given regions and seasons, indicating a need for more accurate spatial and time distributions of emissions. Limitations of current emission control polices are analyzed based on the estimated emission trends. Compared with control of total PM, there are fewer gains in control of fine particles and carbonaceous aerosols, the PM components most responsible for damages to public health and effects on radiative forcing. A much faster decrease of alkaline base cations in primary PM than that of SO<sub>2</sub> may have raised the acidification risks to ecosystems, indicating further control of acid precursors is required. Moreover, with relatively strict controls in developed urban areas, air pollution challenges have been expanding to less-developed neighboring regions. There is a great need in the future for multi-pollutant control strategies that combine recognition of diverse environmental impacts both in urban and rural areas with emission abatement of multiple species in concert.

 References Andreae, M. O., Schmid, O., Yang, H., Chand, D., Yu, J. Z., Zeng, L. M., and Zhang, Y. H.: Optical properties and chemical composition of the atmospheric aerosol in urban Guangzhou, China, Atmos. Environ., 42, 6335–6350, 2008. Akimoto, H., Ohara, T., Kurokawa, J, and Horii, N.: Verification of energy consumption in China during 1996–2003, Atmos. Environ., 40, 7664–7667, 2006. Boersma, K. F., Eskes, H. J., Dirksen, R. J., van der A, R. J., Veefkind, J. P., Stammes, P., Huijnen, V., Kleipool, Q. L., Sneep, M., Claas, J., Leitão, J., Richter, A., Zhou, Y., and Brunner, D.: An improved tropospheric NO<sub>2</sub> column retrieval algorithm for the Ozone Monitoring Instrument, Atmos. Meas. Tech., 4, 1905–1928, http://dx.doi.org/10.5194/amt-4-1905-2011doi:10.5194/amt-4-1905-2011, 2011. 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 NO<sub>2</sub> from OMI, Atmos. Chem. Phys., 7, 2103–2118, http://dx.doi.org/10.5194/acp-7-2103-2007doi:10.5194/acp-7-2103-2007, 2007. Chen, W. M., Wang, J. X., and Shuai, S. J.: The effects of fuel properties on diesel engine emissions (in Chinese), Automot. Eng., 30, 657–663, 2008. China Iron and Steel Association (CISA): China Steel Yearbook 2005–2010, the Editorial Board of China Steel Yearbook, Beijing, 2011. Cofala, J., Amann, M., Klimont, Z., Kupiainen, K., and Hoglund-Isaksson, L.: Scenarios of global anthropogenic emissions of air pollutants and methane until 2030, Atmos. Environ., 41, 8486–8499, 2007. Gu, J. X., Bai, Z. P., Liu, A. X., Wu, L. P., Xie, Y. Y., Li, W. F., Dong, H. Y., and Zhang, X.: Characterization of Atmospheric Organic Carbon and Element Carbon of PM$_2.5$ and PM$_10$ at Tianjin, China, Aerosol. Air. Qual. Res., 10, 167–176, 2010. Guan, D. B., Liu, Z., Geng, Y., Lindner, S., and Hubacek, K.: The gigatonne gap in China's carbon dioxide inventories, Nature Clim. Change, 2, 672–675, 2012. Guo, H., Zhang, Q. Y., Yao, S., and Wang, D. H.: On-road remote sensing measurements and fuel-based motor vehicle emission inventory in Hangzhou, China, Atmos. Environ., 41, 3095–3107, 2007. Han, S., Kondo, K., Oshima, N., Takegawa, N., Miyazaki, Y., Hu, M., Lin, P., Deng, Z., Zhao, Y., Sugimoto, N., and Wu, Y.: Temporal variations of elemental carbon in Beijing, J. Geophys. Res., 114, D23202, http://dx.doi.org/10.1029/2009JD012027doi:10.1029/2009JD012027, 2009. Han, Y. M., Han, Z. W., Cao, J. J., Chow, J. C., Watson, J. G., An, Z. S., Liu, S. X., and Zhang, R. J.: Distribution and origin of carbonaceous aerosol over a rural high-mountain lake area, Northern China and its transport significance, Atmos. Environ., 42, 2405–2414, 2008. He, K. B., Yao, Z. L., and Zhang, Y. Z.: Characteristics of vehicle emissions in China based on portable emission measurement system, 19th Annual International Emission Inventory Conference "Emissions Inventories – Informing Emerging Issues", San Antonio, Texas, 27–30 September 2010. Available at: http://www.epa.gov/ttnchie1/conference/ei19/session6/he.pdf He, K. B., Huo, H., Zhang, Q., He, D. Q., An, F., Wang, M., and Walsh, M. P.: Oil consumption and CO<sub>2</sub> emissions in China's road transport: current status, future trends, and policy implications, Energ. Policy, 33, 1499–1507, 2005. Huo, H., He, K. B., Wang, M., and Yao, Z. L.: Vehicle technologies, fuel-economy policies, and fuel-consumption rates of Chinese vehicles, Energ. Policy, 43, 30–36, 2012a. Huo, H., Zhang, Q., He, K. B., Yao, Z. L., and Wang, M.: Vehicle-use intensity in China: Current status and future trend, Energ. Policy, 43, 6–16, 2012b. Huo, H., Yao, Z. L., He, K. B., and Yu, X.: Fuel consumption rates of passenger cars in China: Labels versus real-world, Energ. Policy, 39, 7130–7135, 2011. Klimont, Z., Cofala, J., Xing, J., Wei, W., Zhang, C. Y., Wang, S. X., Jiang, K. J., Bhandari, P., Mathur, R., Purohit, P., Rafaj, P., Chambers, A., and Amann, M: Projections of SO<sub>2</sub>, NO$_\mathrmx$, and carbonaceous aerosols emissions in Asia, Tellus Ser.B., 61B, 602–617, 2009. Klimont, Z., Cofala, J., Bertok, I., Amann, M., Heyes, C., and Gyarfas, F.: Modeling Particulate Emissions in Europe: A framework to estimate reduction potential and control costs, Interim report, IR-02-076, International Institute for Applied Systems Analysis, Laxenburg, Austria, 2002. Kondo, Y., Oshima, N., Kajino, M., Mikami, R., Moteki, N., Takegawa, N., Verma, R. L., Kajii, Y., Kato, S., and Takami, A.: Emissions of black carbon in East Asia estimated from observation at a remote site in the East China Sea, J. Geophys. Res., 116, D16201, http://dx.doi.org/10.1029/2011JD015637doi:10.1029/2011JD015637, 2011. Larssen, T., Lydersen, E., Tang, D. G., He, Y., Gao, J. X., Liu, H. Y., Duan, L., Seip, H. M., Vogt, R. D., Mulder, J., Shao, M., Wang, Y. H., Shang, H., Zhang, X. S., Solberg, S., Aas, W., Okland, T., Eilertsen, O., Angell, V., Liu, Q. R., Zhao, D. W., Xiang, R. J., Xiao, J. S., and Luo, J. H.: Acid rain in China. Environ. Sci. Technol., 40, 418–425, 2006. Lei, Y., Zhang, Q., He, K. B., and Streets, D. G.: Primary anthropogenic aerosol emission trends for China, 1990–2005, Atmos. Chem. Phys., 11, 931–954, http://dx.doi.org/10.5194/acp-11-931-2011doi:10.5194/acp-11-931-2011, 2011a. Lei, Y., Zhang, Q., Nielsen, C. P., and He, K. B.: An inventory of primary air pollutants and CO<sub>2</sub> emissions from cement industry in China, 1990–2020, Atmos. Environ., 45, 147–154, 2011b. Li, C., Zhang, Q., Krotkov, N. A., Streets, D. G., He, K. B., Tsay, S. C., and Gleason, J. F.: Recent large reduction in sulfur dioxide emissions from Chinese power plants observed by the Ozone Monitoring Instrument, Geophys. Res. Lett., 37, L08807, http://dx.doi.org/10.1029/2010GL042594doi:10.1029/2010GL042594, 2010. Li, C., Marufu, L. T., Dickerson, R. R., Li, Z. Q., Wen, T. X., Wang Y. S., Wang, P. C., Chen. H. B., and Stehr, J. W.: In situ measurements of trace gases and aerosol optical properties at a rural site in northern China during East Asian Study of Tropospheric Aerosols: An International Regional Experiment 2005, J. Geophys. Res., 112, D22S04, http://dx.doi.org/10.1029/2006JD007592doi:10.1029/2006JD007592, 2007. Likens, G. E., Driscoll, C. T., and Buso, D. C.: Long-term effects of acid rain: Response and recovery of a forest ecosystem, Science, 272, 244–246, 1996. Lin, J. T. and McElroy, M. B.: Detection from space of a reduction in anthropogenic emissions of nitrogen oxides during the Chinese economic downturn, Atmos. Chem. Phys., 11, 8171–8188, http://dx.doi.org/10.5194/acp-11-8171-2011doi:10.5194/acp-11-8171-2011, 2011. Lin, J. T., Nielsen, C. P., Zhao, Y., Lei, Y., Liu, Y., and McElroy, M. B.: Recent changes in particulate air pollution over China observed from space and the ground: effectiveness of emission control, Environ. Sci. Technol., 44, 7771–7776, 2010a. Lin, J. T., McElroy, M. B., and Boersma, K. F.: Constraint of anthropogenic NOx emissions in China from different sectors: a new methodology using multiple satellite retrievals, Atmos. Chem. Phys., 10, 63–78, http://dx.doi.org/10.5194/acp-10-63-2010doi:10.5194/acp-10-63-2010, 2010b. Lu, Z., Zhang, Q., and Streets, D. G.: Sulfur dioxide and primary carbonaceous aerosol emissions in China and India, 1996–2010, Atmos. Chem. Phys., 11, 9839–9864, http://dx.doi.org/10.5194/acp-11-9839-2011doi:10.5194/acp-11-9839-2011, 2011. Lu, Z., Streets, D. G., Zhang, Q., Wang, S., Carmichael, G. R., Cheng, Y. F., Wei, C., Chin, M., Diehl, T., and Tan, Q.: Sulfur dioxide emissions in China and sulfur trends in East Asia since 2000, Atmos. Chem. Phys., 10, 6311–6331, http://dx.doi.org/10.5194/acp-10-6311-2010doi:10.5194/acp-10-6311-2010, 22010. Ministry of Industry and Information Technology (MIIT): The direction of technology improvement and investment for automobile industry, available at: http://www.miit.gov.cn/n11293472/n11293832/n12843956/n13227851.files/n13226869.xls (last access: 15 Januar 2013), 2010. National Bureau of Statistics (NBS): China Statistical Yearbook 2005–2010, China Statistics Press, Beijing, China, 2011a. National Bureau of Statistics (NBS): China Industry Economy Statistical Yearbook 2005–2010, China Statistics Press, Beijing, China, 2011b. National Bureau of Statistics (NBS): China Statistical Yearbook 2005–2010, China Statistics Press, Beijing, 2011c. Ohara, T., Akimoto, H., Kurokawa, K., 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, http://dx.doi.org/10.5194/acp-7-4419-2007doi:10.5194/acp-7-4419-2007, 2007. Oliver, H. H.: In-use vehicle emissions in China-Tianjin Study, Discussion paper 2008-08, Harvard Kennedy School, available at: http://belfercenter.ksg.harvard.edu/files/2008_Oliver_In-use_Vehicle_Emissions_Tianjin.pdf (last access: 15 Januar 2013), 2008. Parrish, D. D. and Zhu, T.: Clean air for megacities, Science, 326, 674–675, 2009. 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, 2005. Shen, G. F., Wei, S. Y., Wei, W., Zhang, Y. Y., Wang, B., Wang, R., Li, W., Shen, H. Z., Huang, Y., Yang, Y. F., , Wang, X. L., Wang, X. J., and Tao, S.: Emission factors, size distributions and emission inventories of carbonaceous particulate matter from residential wood combustion in rural China, Environ. Sci. Technol., 46, 4207–4214, 2012. Shen, G. F., Yang, Y. F., Wang, W., Tao, S., Zhu, C., Min, Y. J., Xue, M., Ding, J .N., Wang, B., Wang R., Shen, H. Z., Li, W., Wang, X. L., and Russell, A. G.: Emission factors of particulate matter and elemental carbon for crop residues and coals burned in typical household stoves in China, Environ. Sci. Technol., 44, 7157–7162, 2010. Streets, D. G., Zhang, Q., Wang, L. T., He, K. B., Hao, J. M., Wu, Y., Tang, Y. H., and Carmichael, G. R.: Revisiting China's CO emissions after the Transport and Chemical Evolution over the Pacific (TRACE-P) mission: Synthesis of inventories, atmospheric modeling, and observations, J. Geophys. Res., 111, D14306, http://dx.doi.org/10.1029/2006JD007118doi:10.1029/2006JD007118, 2006. Tang, J., Xu, X. B., Ba, J., and Wang, S. F.: Trends of the precipitation acidity over China during 1992–2006, Chinese. Sci. Bull., 55, 1800–1807, 2010. US Environmental Protection Agency (USEPA): Emission inventory information, available at http://www.epa.gov/ttn/chief/trends/index.html (last access: 15 Januar 2013), 2012. van Donkelaar, A., Martin, R. V., Brauer, M., Kahn, R., Levy, R., Verduzco, C., and Villeneuve, P. J.: Global estimates of ambient fine particulate matter concentrations from satellite-based aerosol optical depth: development and application, Environ. Health. Persp., 118, 847–855, 2010. Verma, R. L., Sahu, L. K., Kondo, Y., Takegawa, N., Han, S., Jung, J. S., Kim, Y. J., Fan, S., Sugimoto, N., Shammaa, M. H., Zhang. Y. H., and Zhao, Y.: Temporal variations of black carbon in Guangzhou, China, in summer 2006, Atmos. Chem. Phys., 10, 6471–6485, http://dx.doi.org/10.5194/acp-10-6471-2010doi:10.5194/acp-10-6471-2010, 2010. Wang, S. W., Zhang, Q., Streets, D. G., He, K. B., Martin, R. V., Lamsal, L. N., Chen, D., Lei. Y., and Lu, Z.: Growth in NOx emissions from power plants in China: bottom-up estimates and satellite observations, Atmos. Chem. Phys., 12, 4429–4447, 2012. Wang, Y. X., Wang, X., Kondo, Y., Kajino, M., Munger, J. W., and Hao, J. M.: Black carbon and its correlation with trace gases at a rural site in Beijing: Top-down constraints from ambient measurements on bottom-up emissions, J. Geophys. Res., 116, D24304, http://dx.doi.org/10.1029/2011JD016575doi:10.1029/2011JD016575, 2011. Wang, Y. X., Munger, J. W., Xu, S., McElroy, M. B., Hao, J. M., Nielsen, C. P., and Ma, H.: CO<sub>2</sub> and its correlation with CO at rural site near Beijing: implications for combustion efficiency in China, Atmos. Chem. Phys., 10, 8881–8897, http://dx.doi.org/10.5194/acp-10-8881-2010doi:10.5194/acp-10-8881-2010, 2010a. Wang, S. X., Zhao, M., Xing, J., Wu, Y., Zhou, Y., Lei, Y., He, K. B., Fu, L. X., and Hao, J. M.: Quantifying the air pollutants emission reduction during the 2008 Olympic Games in Beijing, Environ. Sci. Technol., 44, 2490–2496, 2010b. Wu, Y., Zhang, S. J., Li, M. L., Ge, Y. S., Wu, J. W., Zhou, Y., Xu, Y. Y., Hu, J. N., Liu, H., Fu, L. X., He, K. B., and Hao, J. M.: The challenge to NO$_\mathrmx$ emission control for heavy-duty diesel vehicles in China, Atmos. Chem. Phys., 12, 9365–9379, http://dx.doi.org/10.5194/acp-12-9365-2012doi:10.5194/acp-12-9365-2012, 2012. Xu, M. and Wang, Y. J.: The potential and countermove of energy-saving and cutting pollution about brick and tile industry in China(in Chinese), Brick & Tile World, 7, 6–11, 2007. Xu, Y.: Improvements in the operation of SO<sub>2</sub> scrubbers in China's coal power plants, Environ. Sci. Technol., 45, 380–385, 2011. Xu, Y., Williams, R. H., and Socolow, R. H.: China's rapid deployment of SO<sub>2</sub> scrubbers, Energy. Environ. Sci., 2, 459–465, 2009. Yang, F., Huang, L., Duan, F., Zhang, W., He, K., Ma, Y., Brook, J. R., Tan, J., Zhao, Q., and Cheng, Y.: Carbonaceous species in PM2.5 at a pair of rural/urban sites in Beijing, 2005–2008, Atmos. Chem. Phys., 11, 7893–7903, http://dx.doi.org/10.5194/acp-11-7893-2011doi:10.5194/acp-11-7893-2011, 2011. Yao, Z. L., Huo, H., Zhang, Q., Streets, D. G., and He, K. B.: Gaseous and particulate emissions from rural vehicles in China, Atmos. Environ., 45, 3055–3061, 2011. Zhang, C. Y., Wang, S. X., Xing, J., Zhao, Y., and Hao, J. M.: Current status and future projections of NO$_\mathrmx$ emissions from energy related industries in China (in Chinese), Acta Scientiae Circumstantiae, 28, 2470–2479, 2008. Zhang, Q., He, K. B., and Huo, H.: Cleaning China's air, Nature, 484, 161–162, 2012a. Zhang, Q., Geng, G. N., Wang, S. W., Richter, A., and He, K. B.: Satellite remote sensing of changes in NO$_\text x$ emissions over China during 1996–2010, Chinese. Sci. Bull., 57, 2857–2864, 2012b. Zhang, Q., Streets, D. G., Carmichael, G. R., He, K., Huo, H., Kannari, A., Klimont, Z., Park, I., Reddy, S., Fu, J. S., Chen, D., Duan, L., Lei, Y., Wang, L., and Yao, Z.: Asian emissions in 2006 for the NASA INTEX-B mission, Atmos. Chem. Phys., 9, 5131–5153, http://dx.doi.org/10.5194/acp-9-5131-2009doi:10.5194/acp-9-5131-2009, 2009. 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.: NO$_\text x$ emission trends for China, 1995–2004: The view from the ground and the view from space, J. Geo. Res., 112, D22306, http://dx.doi.org/10.1029/2007jd008684doi:10.1029/2007jd008684, 2007. Zhao, Y., Nielsen, C. P., McElroy, M. B., Zhang, L., and Zhang, J.: CO emissions in China: uncertainties and implications of improved energy efficiency and emission control, Atmos. Environ., 49, 103–113, 2012a. Zhao, Y., Nielsen, C. P., and McElroy, M. B.: China's CO<sub>2</sub> emissions estimated from the bottom up: Recent trends, spatial distributions, and quantification of uncertainties, Atmos. Environ., 59, 214–223, 2012b. Zhao, Y., Nielsen, C. P., Lei, Y., McElroy, M .B., and Hao, J. M.: Quantifying the uncertainties of a bottom-up emission inventory of anthropogenic atmospheric pollutants in China, Atmos. Chem. Phys., 11, 2295–2308, http://dx.doi.org/10.5194/acp-11-2295-2011doi:10.5194/acp-11-2295-2011, 2011a. Zhao, Y., Duan, L., Lei, Y., Xing, J., Nielsen, C. P., and Hao, J. M.: Will PM control undermine China's efforts to reduce soil acidification, Environ. Pollut., 159, 2726–2732, 2011b. Zhao, Y., Wang, S. X., Nielsen, C. P., Li, X. H., and Hao, J. M.: Establishment of a database of emission factors for atmospheric pollutants from Chinese coal-fired power plants, Atmos. Environ., 44, 1515–1523, 2010. Zhao, Y., Duan, L., Xing, J., Larssen, T., Nielsen, C. P., and Hao, J. M.: Soil acidification in China: Is controlling SO<sub>2</sub> emissions enough, Environ. Sci. Technol., 43, 8021–8026, 2009. Zhao, Y., Wang, S. X., Duan, L., Lei, Y., Cao, P. F., and Hao, J. M.: Primary air pollutant emissions of coal-fired power plants in China: current status and future prediction, Atmos. Environ., 42, 8442–8452, 2008. Zhou, X.: New ways of energy saving and emission control for brick and tile industry (in Chinese), Brick Tile World, 3, 15–19, 2009. Zhou, X. H., Gao, J., Wang, T., Wu, W., and Wang, W. X.: Measurement of black carbon aerosols near two Chinese megacities and the implications for improving emission inventories, Atmos. Environ., 43, 3918–3924, 2009. Zhu, X. Y., Duan, L., Tang, G. G., Hao, J. M., and Dong, G.: Estimation of atmospheric emissions of base cations in China (in Chinese), J. Tsinghua Univ. Sci. Technol., 44, 1176–1179, 2004. Zielinska, B., Sagebiel, J., McDonald, J. D., Whitney, K., and Lawson, D. R.: Emission rates and comparative chemical composition from selected in-use diesel and gasoline-fueled vehicles, J. Air Waste Manage. Assoc., 54, 1138–1150, 2004.