Top-down estimates of benzene and toluene emissions in the Pearl River Delta and Hong Kong, China

Copernicus GmbH - Tập 16 Số 5 - Trang 3369-3382
Xuekun Fang1, Min Shao2, A. Stohl3, Qiang Zhang4, Junyu Zheng5, Hai Guo6, Chen Wang7,2, Ming Wang2, Jiamin Ou8, Rona L. Thompson3, Ronald G. Prinn1
1Center for Global Change Science, Massachusetts Institute of Technology, Cambridge, Massachusetts, USA,
2State Key Joint Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing, China
3Norwegian Institute for Air Research, Kjeller, Norway
4Ministry of Education Key Laboratory for Earth System Modeling, Center for Earth System Science, Tsinghua University, Beijing, China
5College of Environment and Energy, South China University of Technology, University Town, Guangzhou, China
6Air Quality Studies, Department of Civil and Environmental Engineering, The Hong Kong Polytechnic University, Hong Kong, China
7College of Environmental Engineering and Science, Qilu University of Technology, Jinan, Shandong, China
8Institute of Space and Earth Information Science, The Chinese University of Hong Kong, Hong Kong, China

Tóm tắt

Abstract. Benzene (C6H6) and toluene (C7H8) are toxic to humans and the environment. They are also important precursors of ground-level ozone and secondary organic aerosols and contribute substantially to severe air pollution in urban areas in China. Discrepancies exist between different bottom-up inventories for benzene and toluene emissions in the Pearl River Delta (PRD) and Hong Kong (HK), which are emission hot spots in China. This study provides top-down estimates of benzene and toluene emissions in the PRD and HK using atmospheric measurement data from a rural site in the area, Heshan, an atmospheric transport model, and an inverse modeling method. The model simulations captured the measured mixing ratios during most pollution episodes. For the PRD and HK, the benzene emissions estimated in this study for 2010 were 44 (12–75) and 5 (2–7) Gg yr−1 for the PRD and HK, respectively, and the toluene emissions were 131 (44–218) and 6 (2–9) Gg yr−1, respectively. Temporal and spatial differences between the inversion estimate and four different bottom-up emission estimates are discussed, and it is proposed that more observations at different sites are urgently needed to better constrain benzene and toluene (and other air pollutant) emissions in the PRD and HK in the future.

Từ khóa


Tài liệu tham khảo

Ait-Helal, W., Borbon, A., Sauvage, S., de Gouw, J. A., Colomb, A., Gros, V., Freutel, F., Crippa, M., Afif, C., Baltensperger, U., Beekmann, M., Doussin, J. F., Durand-Jolibois, R., Fronval, I., Grand, N., Leonardis, T., Lopez, M., Michoud, V., Miet, K., Perrier, S., Prévôt, A. S. H., Schneider, J., Siour, G., Zapf, P., and Locoge, N.: Volatile and intermediate volatility organic compounds in suburban Paris: variability, origin and importance for SOA formation, Atmos. Chem. Phys., 14, 10439–10464, https://doi.org/10.5194/acp-14-10439-2014, 2014.

Baker, A. K., Beyersdorf, A. J., Doezema, L. A., Katzenstein, A., Meinardi, S., Simpson, I. J., Blake, D. R., and Sherwood Rowland, F.: Measurements of nonmethane hydrocarbons in 28 United States cities, Atmos. Environ., 42, 170–182, 2008.

Barletta, B., Meinardi, S., Simpson, I. J., Khwaja, H. A., Blake, D. R., and Rowland, F. S.: Mixing ratios of volatile organic compounds (VOCs) in the atmosphere of Karachi, Pakistan, Atmos. Environ., 36, 3429–3443, 2002.

Barletta, B., Meinardi, S., Rowland, F. S., Chan, C. Y., Wang, X. M., Zou, S. C., Chan, L. Y., and Blake, D. R.: Volatile organic compounds in 43 Chinese cities, Atmos. Environ., 39, 5979–5990, 2005.

Barletta, B., Meinardi, S., Simpson, I. J., Zou, S., Sherwood Rowland, F., and Blake, D. R.: Ambient mixing ratios of nonmethane hydrocarbons (NMHCs) in two major urban centers of the Pearl River Delta (PRD) region: Guangzhou and Dongguan, Atmos. Environ., 42, 4393–4408, 2008.

Chan, L.-Y., Chu, K.-W., Zou, S.-C., Chan, C.-Y., Wang, X.-M., Barletta, B., Blake, D. R., Guo, H., and Tsai, W.-Y.: Characteristics of nonmethane hydrocarbons (NMHCs) in industrial, industrial-urban, and industrial-suburban atmospheres of the Pearl River Delta (PRD) region of south China, J. Geophys. Res.-Atmos., 111, D11304, https://doi.org/10.1029/2005JD006481, 2006.

Donald, J. M., Hooper, K., and Hopenhayn-Rich, C.: Reproductive and Developmental Toxicity of Toluene: A Review, Environ. Health Perspect., 94, 237–244, https://doi.org/10.2307/3431317, 1991.

Fang, X., Thompson, R. L., Saito, T., Yokouchi, Y., Kim, J., Li, S., Kim, K. R., Park, S., Graziosi, F., and Stohl, A.: Sulfur hexafluoride (SF6) emissions in East Asia determined by inverse modeling, Atmos. Chem. Phys., 14, 4779–4791, https://doi.org/10.5194/acp-14-4779-2014, 2014.

Fang, X., Stohl, A., Yokouchi, Y., Kim, J., Li, S., Saito, T., Park, S., and Hu, J.: Multiannual Top-Down Estimate of HFC-23 Emissions in East Asia, Environ. Sci. Technol., 49, 4345–4353, https://doi.org/10.1021/es505669j, 2015.

Guo, H., Jiang, F., Cheng, H. R., Simpson, I. J., Wang, X. M., Ding, A. J., Wang, T. J., Saunders, S. M., Wang, T., Lam, S. H. M., Blake, D. R., Zhang, Y. L., and Xie, M.: Concurrent observations of air pollutants at two sites in the Pearl River Delta and the implication of regional transport, Atmos. Chem. Phys., 9, 7343–7360, https://doi.org/10.5194/acp-9-7343-2009, 2009.

Guo, H., Ling, Z. H., Cheung, K., Jiang, F., Wang, D. W., Simpson, I. J., Barletta, B., Meinardi, S., Wang, T. J., Wang, X. M., Saunders, S. M., and Blake, D. R.: Characterization of photochemical pollution at different elevations in mountainous areas in Hong Kong, Atmos. Chem. Phys., 13, 3881–3898, https://doi.org/10.5194/acp-13-3881-2013, 2013.

Guo, S., Hu, M., Zamora, M. L., Peng, J., Shang, D., Zheng, J., Du, Z., Wu, Z., Shao, M., Zeng, L., Molina, M. J., and Zhang, R.: Elucidating severe urban haze formation in China, P. Natl. Acad. Sci. USA, 111, 17373–17378, https://doi.org/10.1073/pnas.1419604111, 2014.

Henze, D. K., Seinfeld, J. H., Ng, N. L., Kroll, J. H., Fu, T. M., Jacob, D. J., and Heald, C. L.: Global modeling of secondary organic aerosol formation from aromatic hydrocarbons: high- vs. low-yield pathways, Atmos. Chem. Phys., 8, 2405–2420, https://doi.org/10.5194/acp-8-2405-2008, 2008.

Kurokawa, J., Ohara, T., Morikawa, T., Hanayama, S., Janssens-Maenhout, G., Fukui, T., Kawashima, K., and Akimoto, H.: Emissions of air pollutants and greenhouse gases over Asian regions during 2000–2008: Regional Emission inventory in ASia (REAS) version 2, Atmos. Chem. Phys., 13, 11019–11058, https://doi.org/10.5194/acp-13-11019-2013, 2013.

Lamarque, J. F., Bond, T. C., Eyring, V., Granier, C., Heil, A., Klimont, Z., Lee, D., Liousse, C., Mieville, A., Owen, B., Schultz, M. G., Shindell, D., Smith, S. J., Stehfest, E., Van Aardenne, J., Cooper, O. R., Kainuma, M., Mahowald, N., McConnell, J. R., Naik, V., Riahi, K., and van Vuuren, D. P.: Historical (1850–2000) gridded anthropogenic and biomass burning emissions of reactive gases and aerosols: methodology and application, Atmos. Chem. Phys., 10, 7017–7039, https://doi.org/10.5194/acp-10-7017-2010, 2010.

Langford, B., Nemitz, E., House, E., Phillips, G. J., Famulari, D., Davison, B., Hopkins, J. R., Lewis, A. C., and Hewitt, C. N.: Fluxes and concentrations of volatile organic compounds above central London, UK, Atmos. Chem. Phys., 10, 627–645, https://doi.org/10.5194/acp-10-627-2010, 2010.

Lau, A. K. H., Yuan, Z., Yu, J. Z., and Louie, P. K. K.: Source apportionment of ambient volatile organic compounds in Hong Kong, Sci. Total Environ., 408, 4138–4149, 2010.

Liu, Y., Shao, M., Lu, S., Chang, C.-c., Wang, J.-L., and Chen, G.: Volatile Organic Compound (VOC) measurements in the Pearl River Delta (PRD) region, China, Atmos. Chem. Phys., 8, 1531–1545, https://doi.org/10.5194/acp-8-1531-2008, 2008.

Liu, Z., Wang, Y. H., Vrekoussis, M., Richter, A., Wittrock, F., Burrows, J. P., Shao, M., Chang, C. C., Liu, S. C., Wang, H. L., and Chen, C. H.: Exploring the missing source of glyoxal (CHOCHO) over China, Geophys. Res. Lett., 39, L10812, https://doi.org/10.1029/2012gl051645, 2012.

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, https://doi.org/10.5194/acp-7-4419-2007, 2007.

Ou, J., Zheng, J., Li, R., Huang, X., Zhong, Z., Zhong, L., and Lin, H.: Speciated OVOC and VOC emission inventories and their implications for reactivity-based ozone control strategy in the Pearl River Delta region, China, Sci. Total Environ., 530–531, 393–402, 2015.

Ran, L., Zhao, C., Geng, F., Tie, X., Tang, X., Peng, L., Zhou, G., Yu, Q., Xu, J., and Guenther, A.: Ozone photochemical production in urban Shanghai, China: Analysis based on ground level observations, J. Geophys. Res.-Atmos., 114, D15301, https://doi.org/10.1029/2008JD010752, 2009.

Saha, S., Moorthi, S., Pan, H.-L., Wu, X., Wang, J., Nadiga, S., Tripp, P., Kistler, R., Woollen, J., Behringer, D., Liu, H., Stokes, D., Grumbine, R., Gayno, G., Wang, J., Hou, Y.-T., Chuang, H.-Y., Juang, H.-M. H., Sela, J., Iredell, M., Treadon, R., Kleist, D., Van Delst, P., Keyser, D., Derber, J., Ek, M., Meng, J., Wei, H., Yang, R., Lord, S., van den Dool, H., Kumar, A., Wang, W., Long, C., Chelliah, M., Xue, Y., Huang, B., Schemm, J.-K., Ebisuzaki, W., Lin, R., Xie, P., Chen, M., Zhou, S., Higgins, W., Zou, C.-Z., Liu, Q., Chen, Y., Han, Y., Cucurull, L., Reynolds, R. W., Rutledge, G., and Goldberg, M.: NCEP Climate Forecast System Reanalysis (CFSR) 6-hourly Products, January 1979 to December 2010, Research Data Archive at the National Center for Atmospheric Research, Computational and Information Systems Laboratory, Boulder, CO, 2010.

Schultz, M., Rast, S., van het Bolscher, M., Pulles, T., Brand, R., Pereira, J., Mota, B., Spessa, A., Dalsøren, S., van Nojie, T., and Szopa, S.: Emission data sets and methodologies for estimating emissions, RETRO project report D1-6, Hamburg, http://retro-archive.iek.fz-juelich.de/data/documents/reports/D1-6_final.pdf (last access: 10 March 2016), 2007.

Seibert, P. and Frank, A.: Source-receptor matrix calculation with a Lagrangian particle dispersion model in backward mode, Atmos. Chem. Phys., 4, 51–63, https://doi.org/10.5194/acp-4-51-2004, 2004.

Seibert, P., Kristiansen, N. I., Richter, A., Eckhardt, S., Prata, A. J., and Stohl, A.: Uncertainties in the inverse modelling of sulphur dioxide eruption profiles, Geomat. Nat. Hazards Risk, 2, 201–216, https://doi.org/10.1080/19475705.2011.590533, 2011.

Seila, R. L., Lonneman, W. A., Meeks, S. A., and Atmospheric Research and Exposure Assessment Laboratory (U.S.): Determination of C2 to C12 ambient air hydrocarbons in 39 U.S. cities, from 1984 though 1986, EPA/600/S3-89/058, Research Triangle Park, NC, US Environmental Protection Agency, Atmospheric Research and Exposure Assessment Laboratory, 1989.

Simpson, I. J., Blake, N. J., Barletta, B., Diskin, G. S., Fuelberg, H. E., Gorham, K., Huey, L. G., Meinardi, S., Rowland, F. S., Vay, S. A., Weinheimer, A. J., Yang, M., and Blake, D. R.: Characterization of trace gases measured over Alberta oil sands mining operations: 76 speciated C2–C10 volatile organic compounds (VOCs), CO2, CH4, CO, NO, NO2, NOy, O3 and SO2, Atmos. Chem. Phys., 10, 11931–11954, https://doi.org/10.5194/acp-10-11931-2010, 2010.

Song, Y., Shao, M., Liu, Y., Lu, S., Kuster, W., Goldan, P., and Xie, S.: Source Apportionment of Ambient Volatile Organic Compounds in Beijing, Environ. Sci. Technol., 41, 4348–4353, https://doi.org/10.1021/es0625982, 2007.

Stohl, A. and Thomson, D.: A Density Correction for Lagrangian Particle Dispersion Models, Bound.-Lay. Meteorol., 90, 155–167, https://doi.org/10.1023/A:1001741110696, 1999.

Stohl, A., Hittenberger, M., and Wotawa, G.: Validation of the Lagrangian particle dispersion model FLEXPART against large-scale tracer experiment data, Atmos. Environ., 32, 4245–4264, 1998.

Stohl, A., Forster, C., Frank, A., Seibert, P., and Wotawa, G.: Technical note: The Lagrangian particle dispersion model FLEXPART version 6.2, Atmos. Chem. Phys., 5, 2461–2474, https://doi.org/10.5194/acp-5-2461-2005, 2005.

Stohl, A., Seibert, P., Arduini, J., Eckhardt, S., Fraser, P., Greally, B. R., Lunder, C., Maione, M., Mühle, J., O'Doherty, S., Prinn, R. G., Reimann, S., Saito, T., Schmidbauer, N., Simmonds, P. G., Vollmer, M. K., Weiss, R. F., and Yokouchi, Y.: An analytical inversion method for determining regional and global emissions of greenhouse gases: Sensitivity studies and application to halocarbons, Atmos. Chem. Phys., 9, 1597–1620, https://doi.org/10.5194/acp-9-1597-2009, 2009.

Stohl, A., Kim, J., Li, S., O'Doherty, S., Mühle, J., Salameh, P. K., Saito, T., Vollmer, M. K., Wan, D., Weiss, R. F., Yao, B., Yokouchi, Y., and Zhou, L. X.: Hydrochlorofluorocarbon and hydrofluorocarbon emissions in East Asia determined by inverse modeling, Atmos. Chem. Phys., 10, 3545–3560, https://doi.org/10.5194/acp-10-3545-2010, 2010.

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 Perspect., 118, 847–855, 2010.

van Vuuren, D., den Elzen, M. J., Lucas, P., Eickhout, B., Strengers, B., van Ruijven, B., Wonink, S., and van Houdt, R.: Stabilizing greenhouse gas concentrations at low levels: an assessment of reduction strategies and costs, Climatic Change, 81, 119–159, https://doi.org/10.1007/s10584-006-9172-9, 2007.

Velasco, E., Lamb, B., Westberg, H., Allwine, E., Sosa, G., Arriaga-Colina, J. L., Jobson, B. T., Alexander, M. L., Prazeller, P., Knighton, W. B., Rogers, T. M., Grutter, M., Herndon, S. C., Kolb, C. E., Zavala, M., de Foy, B., Volkamer, R., Molina, L. T., and Molina, M. J.: Distribution, magnitudes, reactivities, ratios and diurnal patterns of volatile organic compounds in the Valley of Mexico during the MCMA 2002 & 2003 field campaigns, Atmos. Chem. Phys., 7, 329–353, https://doi.org/10.5194/acp-7-329-2007, 2007.

Wang, M., Zeng, L., Lu, S., Shao, M., Liu, X., Yu, X., Chen, W., Yuan, B., Zhang, Q., Hu, M., and Zhang, Z.: Development and validation of a cryogen-free automatic gas chromatograph system (GC-MS/FID) for online measurements of volatile organic compounds, Anal. Methods, 6, 9424–9434, https://doi.org/10.1039/C4AY01855A, 2014.

Weiss, R. F. and Prinn, R. G.: Quantifying greenhouse-gas emissions from atmospheric measurements: a critical reality check for climate legislation, Philos. T. Roy. Soc. A, 369, 1925–1942, https://doi.org/10.1098/rsta.2011.0006, 2011.

White, M. L., Russo, R. S., Zhou, Y., Ambrose, J. L., Haase, K., Frinak, E. K., Varner, R. K., Wingenter, O. W., Mao, H., Talbot, R., and Sive, B. C.: Are biogenic emissions a significant source of summertime atmospheric toluene in the rural Northeastern United States?, Atmos. Chem. Phys., 9, 81–92, https://doi.org/10.5194/acp-9-81-2009, 2009.

Xue, L. K., Wang, T., Gao, J., Ding, A. J., Zhou, X. H., Blake, D. R., Wang, X. F., Saunders, S. M., Fan, S. J., Zuo, H. C., Zhang, Q. Z., and Wang, W. X.: Ground-level ozone in four Chinese cities: precursors, regional transport and heterogeneous processes, Atmos. Chem. Phys., 14, 13175–13188, https://doi.org/10.5194/acp-14-13175-2014, 2014.

Yin, S., Zheng, J., Lu, Q., Yuan, Z., Huang, Z., Zhong, L., and Lin, H.: A refined 2010-based VOC emission inventory and its improvement on modeling regional ozone in the Pearl River Delta Region, China, Sci. Total Environ., 514, 426–438, 2015.

Yoshino, A., Nakashima, Y., Miyazaki, K., Kato, S., Suthawaree, J., Shimo, N., Matsunaga, S., Chatani, S., Apel, E., Greenberg, J., Guenther, A., Ueno, H., Sasaki, H., Hoshi, J.-Y., Yokota, H., Ishii, K., and Kajii, Y.: Air quality diagnosis from comprehensive observations of total OH reactivity and reactive trace species in urban central Tokyo, Atmos. Environ., 49, 51–59, 2012.

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

Zheng, J., Shao, M., Che, W., Zhang, L., Zhong, L., Zhang, Y., and Streets, D.: Speciated VOC Emission Inventory and Spatial Patterns of Ozone Formation Potential in the Pearl River Delta, China, Environ. Sci. Technol., 43, 8580–8586, https://doi.org/10.1021/es901688e, 2009.

Thông tin
Thông tin xuất bản

Copernicus GmbH

Tập 16 Số 5

3369-3382

Thông tin tác giả