References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-11-2295-2011

Quantifying the uncertainties of a bottom-up emission inventory of anthropogenic atmospheric pollutants in China

Zhao

¹ ² Nielsen

C. P.

¹ Lei

¹ ³ McElroy

M. B.

¹ Hao

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

School of Environment, Tsinghua University, Beijing 100084, China

Key Laboratory of Environmental Planning and Policy Simulation, Chinese Academy for Environmental Planning, Beijing 100012, China

14 03 2011

11 5 2295 2308

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/11/2295/2011/acp-11-2295-2011.html

The full text article is available as a PDF file from http://www.atmos-chem-phys.net/11/2295/2011/acp-11-2295-2011.pdf

The uncertainties of a national, bottom-up inventory of Chinese emissions of anthropogenic SO2, NOx, and particulate matter (PM) of different size classes and carbonaceous species are comprehensively quantified, for the first time, using Monte Carlo simulation. The inventory is structured by seven dominant sectors: coal-fired electric power, cement, iron and steel, other industry (boiler combustion), other industry (non-combustion processes), transportation, and residential. For each parameter related to emission factors or activity-level calculations, the uncertainties, represented as probability distributions, are either statistically fitted using results of domestic field tests or, when these are lacking, estimated based on foreign or other domestic data. The uncertainties (i.e., 95% confidence intervals around the central estimates) of Chinese emissions of SO2, NOx, total PM, PM10, PM2.5, black carbon (BC), and organic carbon (OC) in 2005 are estimated to be −14%~13%, −13%~37%, −11%~38%, −14%~45%, −17%~54%, −25%~136%, and −40%~121%, respectively. Variations at activity levels (e.g., energy consumption or industrial production) are not the main source of emission uncertainties. Due to narrow classification of source types, large sample sizes, and relatively high data quality, the coal-fired power sector is estimated to have the smallest emission uncertainties for all species except BC and OC. Due to poorer source classifications and a wider range of estimated emission factors, considerable uncertainties of NOx and PM emissions from cement production and boiler combustion in other industries are found. The probability distributions of emission factors for biomass burning, the largest source of BC and OC, are fitted based on very limited domestic field measurements, and special caution should thus be taken interpreting these emission uncertainties. Although Monte Carlo simulation yields narrowed estimates of uncertainties compared to previous bottom-up emission studies, the results are not always consistent with those derived from satellite observations. The results thus represent an incremental research advance; while the analysis provides current estimates of uncertainty to researchers investigating Chinese and global atmospheric transport and chemistry, it also identifies specific needs in data collection and analysis to improve on them. Strengthened quantification of emissions of the included species and other, closely associated ones – notably CO2, generated largely by the same processes and thus subject to many of the same parameter uncertainties – is essential not only for science but for the design of policies to redress critical atmospheric environmental hazards at local, regional, and global scales.

References 1

Akimoto, H., Ohara, T., Kurokawa, J, and Horii, N.: Verification of energy consumption in China during 1996–2003, Atmos. Environ., 40, 7664–7667, 2006.

Andreae, M. O., and Merlet, P.: Emission of trace gases and aerosols from biomass burning, Global. Biogeochem. Cy., 15, 955–966, 2001.

Anshan Iron and Steel Group Corporation (AISGC): Description on developing emission standard of air pollutants for iron and steel industry-sintering, internal report, 2007(in Chinese).

Bond, T. C., Streets, D. G., Yarber, K. F., Nelson, S. M., Woo, J-H., and Klimont, Z.: A technology-based global inventory of black and organic carbon emissions from combustion, J. Geophys. Res., 109, D14203, http://dx.doi.org/10.1029/2003jd003697doi:10.1029/2003jd003697, 2004.

Carmichael, G. R., Tang, Y., Kurata, G., Uno, I., Streets, D., Woo, J.-H., Huang, H., Yienger, J., Lefer, B., Shetter, R., Blake, D., Atlas, E., Fried, A., Apel, E., Eisele, F., Cantrell, C., Avery, M., Barrick, J., Sachse, G., Brune, W., Sandholm, S., Kondo, Y., Singh, H., Talbot, R., Bandy, A., Thorton, D., Clarke, A., and Heikes, B.: Regional-scale chemical transport modeling in support of the analysis of observations obtained during the TRACE-P experiment, J. Geophys. Res., 108(D21), 8823, http://dx.doi.org/10.1029/2002jd003117doi:10.1029/2002jd003117, 2003a.

Carmichael, G. R., Tang, Y., Kurata, G., Uno, I., Streets, D. G., Thongboonchoo, N., Woo, J.-H., Guttikunda, S., White, A., Wang, T., Blake, D. R., Atlas, E., Fried, A., Potter, B., Avery, M. A., Sachse, G. W., Sandholm, S. T., Kondo, Y., Talbot, R. W., Bandy, A., Thorton, D., and Clarke, A. D.: Evaluating regional emission estimates using the TRACE-P observations, J. Geophys. Res., 108 (D21), 8810, http://dx.doi.org/10.1029/2002jd003116doi:10.1029/2002jd003116, 2003b.

Cao, G. L., Zhang, X. Y., and Zheng, F. C.: Inventory of black carbon and organic carbon emissions from China, Atmos. Environ., 40, 6516–6527, 2006.

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, http://dx.doi.org/10.5194/acp-9-3825-2009doi:10.5194/acp-9-3825-2009, 2009.

Chen, Y. J., Sheng, G. Y., Bi, X. H., Feng, Y. L., Mai, B. X., and Fu, J. M.: Emission factors for carbonaceous particles and polycyclic aromatic hydrocarbons from residential coal combustion in China, Environ. Sci. Technol., 39, 1861–1867, 2005.

Chen, Y. J., Zhi, G. R., Feng, Y. L., Fu, J. M., Feng, J. L., Sheng, G. Y., and Simoneit, B. R. T.: Measurements of emission factors for primary carbonaceous particles from residential raw-coal combustion in China, Geophys. Res. Lett., 33, L20815, http://dx.doi.org/10.1029/2006gl026966doi:10.1029/2006gl026966, 2006.

China Association of Automobile Manufacturers (CAAM) and China Automotive Technology & Research Center (CATRA): Evaluation report of automobile energy saving in China, available at: http://caam.org.cn/files/file/0906/zhyh.pdf, 2009(in Chinese).

Chinese Research Academy of Environm. Scis (CRAES): Description on developing emission standard of air pollutants for cement industry , internal report, Beijing, 2003(in Chinese).

Frey, H. C. and Zhao, Y. C.: Quantification of variability and uncertainty for air toxic emission inventories with censored emission factor data, Environ. Sci. Technol., 38, 6094–6100, 2004.

Frey, H. C. and Li, S.: Methods for quantifying variability and uncertainty in AP-42 emission factors: case studies for natural gas-fueled engines, J. Air Waste Manage., 53, 1436–1447, 2003.

Frey, H. C. and Zheng, J. Y.: Quantification of variability and uncertainty in air pollutant emission inventories: method and case study for utility NOx emissions, J. Air Waste Manage., 52, 1083–1095, 2002.

Hao, J. M., Tian, H. Z., and Lu, Y. Q.: Emission inventories of NOx from commercial energy consumption in China, 1995–1998, Environ. Sci. Technol., 36, 552–560, 2002.

He, K. B., Huo, H., Zhang, Q., He, D. Q., An, F., Wang, M., and Walsh, M. P.: Oil consumption and CO2 emissions in China's road transport: current status, future trends, and policy implications, Energ. Policy, 33, 1499–1507, 2005.

He, Y. J., Uno, I., Wang, Z. F., Ohara, T., Sugimoto, N., Shimizu, A., Richter, A., and Burrows, J. P.: Variations of the increasing trend of tropospheric NO2 over central east China during the past decade, Atmos. Environ., 41, 4865–4876, 2007.

Huang, J. Y. and Xia, J. X.: General situation of industrial boiler industry in China and product trend, Energ. Environ., 1, 21–23, 2004(in Chinese).

Intergovernmental Panel on Climate Change (IPCC): 2006 IPCC Guidelines for National Greenhouse Gas Inventories, IPCC National Greenhouse Gas Inventories Programme, 2006.

Karvosenoja, N., Tainio, M., Kupiainen, K., Tuomisto, J. T., Kukkonen, J., and Johansson, M.: Evaluation of the emissions and uncertainties of PM$_2.5$ originated from vehicular traffic and domestic wood combustion in Finland, Boreal Env. Res., 13, 465–474, 2008.

Kean, A. J., Sawyer, R. F., and Harley, R. A.: A fuel-based assessment of off-road diesel engine emissions, J. Air Waste Manage. Assoc., 50, 1929–1939, 2000.

Kioutsioukis, I., Tarantola, S., Saltelli, A., and Debora, G.: Uncertainty and global sensitivity analysis of road transport emission estimates, Atmos. Environ., 38, 6609–6620, 2004.

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, Institute for Applied Systems Analysis, Laxenburg, Austria, 2002.

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 SO2, NOx, and carbonaceous aerosols emissions in Asia, Tellus Ser.B., 61B, 602–617, 2009.

Lal, R.: World crop residues production and implications of its use as a biofuel, Environ. Int., 31, 575–584, 2005.

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, 2011.

Lei, Y., Zhang, Q., Nielsen, C. P., and He, K. B.: An inventory of primary air pollutants and CO2 emissions from cement industry in China, 1990–2020, Atmos. Environ., 45, 147–154, 2011b.

Li, X. H., Duan, L., Wang, S. X., Duan, J. C., Guo, X. M., Yi, H. H., Hu, J. N., Li, C., and Hao, J. M.: Emission characteristics of particulate matter from rural household biofuel combustion in China, Energ. Fuel, 21, 845–851, 2007a.

Li, X. H., Wang, S. X., Duan, L., Hao, J. M., Li C., Chen, Y. S., and Yang, L.: Particulate and trace gas emissions from open burning of wheat straw and corn stover in China, Environ. Sci. Technol., 41, 6052–6058, 2007b.

Li, C., Li, X. H., Duan, L., Zhao, M., Duan, J. C., and Hao, J. M.: Emission characteristics of PM$_10$ from coal-fired industrial boiler, Environm. Sci., 30, 650–655, 2009a(in Chinese).

Li, X. H., Wang, S. X., Duan, L., Hao, J. M., and Nie, Y. F.: Carbonaceous aerosol emissions from household biofuel combustion, Environ. Sci. Technol., 43, 6076–6081, 2009b.

Liu, H., He, K. B., Lents, J. M., Wang, Q. D., and Tolvett, S.: Characteristics of diesel truck emission in China based on portable emissions measurement systems, Environ. Sci. Technol., 43, 9507–9511, 2009.

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, 2010.

Ma, J. Z., Richter, A., Burrows, J. P., Nuss, H., and van Aardenne, J.A.: Comparison of model-simulated tropospheric NO2 over China with GOME-satellite data, Atmos. Environ., 40, 593–604, 2006.

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, 2007.

Qu, L. F.: Economical operation analysis of industrial boilers in China 2007, China Electrical Equipment Industry, 6, 24–29, 2008(in Chinese).

Saikawa, E., Naik, V., Horowitz, L. W., Liu, J. F., and Mauzerall, D. L.: Present and potential future contributions of sulfate, black and organic carbon aerosols from China to global air quality, premature mortality and radiative forcing, Atmos. Environ., 43, 2814–2822, 2009.

State Environmental Protection Administration (SEPA): Handbook of Industrial Pollution Emission Factors, China Environm. Sci. Press, 1–262, Beijing, 1996(in Chinese).

Streets, D. G., Gupta, S., Waldhoff, S. T., Wang, M. Q., Bond, T. C., and Bo, Y. Y.: Black carbon emissions in China, Atmos. Environ., 35, 4281–4296, 2001.

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, http://dx.doi.org/10.1029/2002jd003093doi:10.1029/2002jd003093, 2003.

U.S. Environmental Protection Agency (USEPA): Compilation of Air Pollutant Emission Factors, available at: http://www.epa.gov/ttn/chief/ap42/index.html, 2002.

Wang, H. K., Chen, C. H., Huang, C., and Fu, L. X.: On-road vehicle emission inventory and its uncertainty analysis for Shanghai, China, Sci. Total. Environ, 398, 60–67, 2008.

Wang, M., Huo, H., Johnson, L., and He, D. Q.: Projection of Chinese motor vehicle growth, oil demand, and CO2 emissions through 2050, Argon National Laboratory, ANL/ESD/06-6, 2006.

Wang, S. X. and Zhang, C. Y.: Spatial and temporal distribution of air pollutant emission from open burning of crop residues in China, Sciencepaper online, 3, 329–333, 2008(in Chinese).

Wang, S. X., Zhao, X. J., Li, X. H., Wei, W., and Hao, J. M.: Emission characteristics of fine particles from grate firing boilers, Environm. Sci., 30, 963–968, 2009(in Chinese).

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, http://dx.doi.org/10.1029/2006jd007538doi:10.1029/2006jd007538, 2007.

Wang, Y. 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, http://dx.doi.org/10.1029/2004jd005250doi:10.1029/2004jd005250, 2004.

Wu, Y., Streets, D. G., Wang, S. X., and Hao, J. M.: Uncertainties in estimating mercury emissions from coal-fired power plants in China, Atmos. Chem. Phys., 10, 2937–2946, http://dx.doi.org/10.5194/acp-10-2937-2010doi:10.5194/acp-10-2937-2010, 2010.

Xu, Y., Williams, R. H., and Socolow, R. H.: China's rapid deployment of SO2 scrubbers, Energy. Environ. Sci., 2, 459–465, 2009.

Zhang, J. F. and Smith, K. R.: Greenhouse gases and other airborne pollutants from household stoves in China: a database for emission factors, Atmos. Environ., 34, 4537–4549, 2000.

Zhang, M. G., Uno, I., Yoshida, Y., Xu, Y. F., Wang, Z. F., Akimoto, H., Bates, T., Quinn, T., Bandy, A., and Blomquist, B.: Transport and transformation of sulfur compounds over East Asia during the TRACE-P and ACE-Asia campaigns, Atmos. Environ., 38, 6947–6959, 2004.

Zhang, C. Y., Wang, S. X., Zhao, Y., and Hao, J. M.: Current status and future prospects of anthropogenic particulate matter emissions in China, Environm. Sci., 30, 1881–1887, 2009a(in Chinese).

Zhang, J., He, K. B., Shi, X. Y., and Zhao, Y.: Effect of SME biodiesel blends on PM$_2.5$ emission from a heavy-duty engine, Atmos. Environ., 43, 2442–2448, 2009b.

Zhang, J., He, K. B., Ge, Y. S., and Shi, X. Y.: Influence of fuel sulfur on the characterization of PM$_10$ from a diesel engine, Fuel, 88, 504–510, 2009c.

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, http://dx.doi.org/10.5194/acp-9-5131-2009doi:10.5194/acp-9-5131-2009, 2009.

Zhang, C. Y., Wang, S. X., Xing, J., Zhao, Y., and Hao, J. M.: Current status and future projections of NOx emissions from energy related industries in China, Acta Scientiae Circumstantiae, 28, 2470–2479, 2008a(in Chinese).

Zhang, Y. X., Schauer, J. J., Zhang, Y. H., Zeng, L. M., Wei, Y. J., Liu, Y., and Shao, M.: Characteristics of particulate carbon emissions from real-world Chinese coal combustion, Environ. Sci. Technol., 42, 5068–5073, 2008b.

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, http://dx.doi.org/10.1029/2007jd008684doi:10.1029/2007jd008684, 2007a.

Zhang, Q., Streets, D. G., He, K. B., and Klimont, Z.: Major components of China's anthropogenic primary particulate emissions, Environ. Res. Lett., 2, 045027, http://dx.doi.org/10.1088/1748-9326/2/4/045027doi:10.1088/1748-9326/2/4/045027, 2007b.

Zhao, C. and Wang, Y. H.: Assimilated inversion of NOx emissions over east Asia using OMI NO2 column measurements, Geophys. Res. Lett., 36, L06805, http://dx.doi.org/10.1029/2008gl037123doi:10.1029/2008gl037123, 2009.

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 SO2 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.

Zheng, J. Y., Zhang, L. J., Che, W. W., Zheng, Z, Y., and Yin, S. S.: A highly resolved temporal and spatial air pollutant emission inventory for the Pearl River Delta region, China and its uncertainty assessment, Atmos. Environ., 43, 5112–5122, 2009.