Atmospheric Chemistry and Physics www.atmos-chem-phys.net 1680-7316 1680-7324 9 18 2009 10.5194/acp-9-6983-2009 http://www.atmos-chem-phys.net/9/6983/2009/ http://www.atmos-chem-phys.net/9/6983/2009/acp-9-6983-2009.html http://www.atmos-chem-phys.net/9/6983/2009/acp-9-6983-2009.pdf 6983 7002 2009-09-22 Tempo-spatial variation of emission inventories of speciated volatile organic compounds from on-road vehicles in China H. Cai S. D. Xie sdxie@pku.edu.cn College of Environmental Science and Engineering, State Key Joint Laboratory of Environmental Simulation and Pollution Control, Peking University, Beijing, China Emission inventories of sixty-seven speciated non-methane volatile organic compounds (NMVOC) from on-road vehicles in China were estimated for the period of 1980–2005, using seven NMVOC emission profiles, which were summarized based on local and international measurements from published literatures dealing with specific vehicle categories running under particular modes. <br><br> Results show an exponential growth trend of China's historical emissions of alkanes, alkenes, alkines, aromatics and carbonyls during the period of 1980–2005, increasing from 63.9, 39.3, 6.9, 36.8 and 24.1 thousand tons, respectively, in 1980 to 2778.2, 1244.5, 178.7, 1351.7 and 406.0 thousand tons, respectively, in 2005, which coincided well with China's economic growth. Emission inventories of alkenes, aromatics and carbonyls were gridded at a high resolution of 40 km&times;40 km for air quality simulation and health risk evaluation, using the geographic information system (GIS) methodology. Spatial distribution of speciated NMVOC emissions shows a clear difference in emission densities between developed eastern and relatively underdeveloped western and inland China. Besides, the appearance and expansion of high-emission areas was another notable characteristic of spatial distribution of speciated NMVOC emissions during the period. <br><br> Emission contributions of vehicle categories to speciated NMVOC groups showed annual variation, due to the variance in the provincial emissions and in the relative fractions of the seven emission profiles adopted at the provincial level. Highly reactive and toxic compounds accounted for high proportions of emissions of speciated NMVOC groups. The most abundant compounds were isopentane, pentane and butane from alkanes; ethene, propene, 2-methyl-2-butene and ethyne from alkenes and alkines; benzene, toluene, ethylbenzene, o-xylene, and m,p-xylene (BTEX) and 1,2,4-trimethylbenzene from aromatics and formaldehyde, acetaldehyde, benzaldehyde and acetone from carbonyls. Atkinson, R.: Atmospheric chemistry of VOCs and NOx, Atmos. Environ., 34, 2063–2101, 2000. 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. Batterman, S. A., Yu, Y. D., Jia, C. R., and Godwin, C.: Non-methane hydrocarbon emissions from vehicle fuel caps, Atmos. Environ., 39, 1855–1867, 2005. Bo, Y., Cai, H., and Xie, S. D.: Spatial and temporal variation of historical anthropogenic NMVOCs emission inventories in China, Atmos. Chem. Phys., 8, 7297–7316, 2008. Cai, H. and Xie, S. D.: Estimation of vehicular emission inventories in China from 1980 to 2005, Atmos. Environ., 41, 8963–8979, 2007. Chan, C. K. and Yao, X. H.: Air pollution in mega cities in China, Atmos. Environ., 42, 1–42, 2008. Chan, L. Y., Lau, W. L., Zou, S. C., Cao, Z. X., and Lai, S. C.: Exposure level of carbon monoxide and respirable suspended particulate in public transportation modes while commuting in urban area of Guangzhou, China, Atmos. Environ., 36, 5831–5840, 2002. Conner, T. L., Lonneman, W. A., and Seila, R. L.: Transportation-related volatile hydrocarbon source profiles measured in Atlanta, JAPCA J. Air Waste Ma., 45, 383–394, 1995. Duffy, B. L., Nelson, P. F., Ye, Y., and Weeks, I. A.: Speciated hydrocarbon profiles and calculated reactivities of exhaust and evaporative emissions from 82 in-use light-duty Australian vehicles, Atmos. Environ., 33, 291–307, 1999. European Environment Agency: COPERT III-Computer programme to calculate emissions from road transport, methodology and emission factors (version~2.1), technical report No 49, 2000. Fu, X. Q., Weng, Y. B., Qian, F. Z., Ye, W. B., Jin, Y. X., and Chen, Y. Y.: Study of the VOC source profile and benzene compounds emission of various motor vehicles, Acta Scientiae Circumstantiae, 6, 1056–1062, 2008 \mbox(in Chinese). General Administration of Quality Supervision, Inspection and Quarantine of the People's Republic of China: National Standards of Unleaded Gasoline for Motor Vehicles (GB~17930–1999), 1999. He, C. Y. and Wang, Q. D.: Vehicle emission factors determination using CMEM in Beijing, Research of Environmental Sciences, 1, 109-112, 2006 \mbox(in Chinese). He, D. Q.: Study on urban vehicular pollution assessment system and emission control target, Ph.D thesis, Tsinghua University, China, 1999 \mbox(in Chinese). He, D. Q., Hao, J. M., He, K. B., and Fu, L. X.: Vehicle emission factors determination using model calculation, Environmental Science, 3, 9–12, 1998 (in Chinese). Hoekman, S. K.: Speciated measurements and calculated reactivities of vehicle exhaust emissions from conventional and reformulated gasolines, Environ. Sci. Technol., 26, 1206–1216, 1992. Hu, B. X., Zhu, H., and Tan, W. X.: A detailed list for exhaust in development models of automobile technology in China, Journal of Wuhan Automotive Polytechnic University, 2, 99–102, 2002 \mbox(in Chinese). Hurley, M. D., Chang, T. Y., Japar, S. M., and Wallington, T. J.: Measurement of VOC reactivities using a photochemical flow reactor, Environ. Sci. Technol., 32, 1913–1919, 1998. Hwa, M. Y., Hsieh, C. C., Wu, T. C., and Chang, L. F. W.: Real-world vehicle emissions and VOCs profile in the Taipei tunnel located at Taiwan Taipei area, Atmos. Environ., 36, 1993–2002, 2002. Jeffries, H. E., Yu, J., and Bartolotti, L.: Theoretical and analytical advances in understanding aromatic atmospheric oxidation mechanisms, Abstr. Pap. Am. Chem. S., 210, 15-Phys, 1995. Klimont, Z., Streets, D. G., Gupta, S., Cofala, J., Fu, L. X., and Ichikawa, Y.: Anthropogenic emissions of non-methane volatile organic compounds in China, Atmos. Environ., 36, 1309–1322, 2002. Kourtidis, K. A., Ziomas, I. C., Rappenglueck, B., Proyou, A., and Balis, D.: Evaporative traffic hydrocarbon emissions, traffic CO and speciated HC traffic emissions from the city of Athens, Atmos. Environ., 33, 3831–3842, 1999. Lei, W.: Study on the driving cycle and emission characteristics of Wuhan light-duty vehicle, MA~thesis, Wuhan Polytechnic University, 2007 \mbox(in Chinese). Li, W., Fu, L. X., Hao, J. M., Ma, H., Li, S. Q., and Hu, W.: Emission inventory of 10~kinds of air pollutants for road traffic vehicles in China, Urban Environment and Urban Ecology, 2, 36–38, 2003 \mbox(in Chinese). Liu, X. L. and Ding, Y.: Research of vehicle driving cycle on the road in China's cities, Research of Environmental Sciences, 1, 23–27, 2000 \mbox(in Chinese). Liu, L. H. and Wang, Z.: Characters analysis and planning of small and middle city transport in China, Urban Transport of China, 1, 21–24, 2004 \mbox(in Chinese). Liu, Y., Shao, M., Fu, L. L., Lu, S. H., Zeng, L. M., and Tang, D. G.: Source profiles of volatile organic compounds (VOCs) measured in China: Part i, Atmos. Environ., 42, 6247–6260, 2008. Lough, G. C., Schauer, J. J., Lonneman, W. A., and Allen, M. K.: Summer and winter nonmethane hydrocarbon emissions from on-road motor vehicles in the midwestern United States, JAPCA J. Air Waste Ma., 55, 629–646, 2005. Lu, S. H., Bai, Y. H., Zhang, G. S., and Ma, J.: Study on the characteristics of VOCs source profiles of vehicle exhaust and gasoline emission, Acta Scientiarum Naturalium, Universitatis Pekinensis, 4, 507–511, 2003 \mbox(in Chinese). Martin, R. S., Villanueva, I., Zhang, J. Y., and Popp, C. J.: Nonmethane hydrocarbon, monocarboxylic acid, and low molecular weight aldehyde and ketone emissions from vegetation in central new Mexico, Environ. Sci. Technol., 33, 2186–2192, 1999. McLaren, R., Gertler, A. W., Wittorff, D. N., Belzer, W., Dann, T., and Singleton, D. L.: Real-world measurements of exhaust and evaporative emissions in the cassiar tunnel predicted by chemical mass balance modeling, Environ. Sci. Technol., 30, 3001–3009, 1996. Ministry of Environmental Protection of the People's Republic of China: Technologies and policies on prevention and control of pollution related with vehicular emissions, 1999. Ministry of Environmental Protection of the People's Republic of China, available at: http://www.mep.gov.cn/tech/hjbz/sywbzgz/200703/t20070309_101474.htm, 2007. Ministry of Environmental Protection of the People's Republic of China, and General Administration of Quality Supervision, Inspection and Quarantine of the People's Republic of China: Limits and Measurement methods for evaporative pollutants from motorcycles and mopeds (GB 20998-2007), 2007. Ministry of Environmental Protection of the People's Republic of China, and General Administration of Quality Supervision, Inspection and Quarantine of the People's Republic of China: Limits and Measurement methods for the emissions of pollutants from motorcycles on the running mode (GB~14622-2007), 2007. Ministry of Environmental Protection of the People's Republic of China, and General Administration of Quality Supervision, Inspection and Quarantine of the People's Republic of China: Limits and Measurement methods for the emissions of pollutants from motorcycles on the running mode (GB~14622-2000), 2000. Mugica, V., Ruiz, M. E., Watson, J., and Chow, J.: Volatile aromatic compounds in Mexico city atmosphere: Levels and source apportionment, Atmosfera, 16, 15–27, 2003. Na, K., Kim, Y. P., Moon, I., and Moon, K. C.: Chemical composition of major VOC emission sources in the Seoul atmosphere, Chemosphere, 55, 585–594, Chemosphere, 2004. National Bureau of Statistics: China Statistical Yearbook [M], China Statistical Publishing House, Beijing, 2006. Nelson, P. F., Quigley, S. M., and Smith, M. Y.: Sources of atmospheric hydrocarbons in Sydney – a quantitative-determination using a source reconciliation technique, Atmos. Environ., 17, 439–449, 1983. Niedojadlo, A., Becker, K. H., Kurtenbach, R., and Wiesen, P.: The contribution of traffic and solvent use to the total NMVOC emission in a German city derived from measurements and CMB modelling, Atmos. Environ., 41, 7108–7126, 2007. Ntzaichristos, L. and Samaras, Z.: COPERT3 – computer programme to calculate emissions from road transport, methodology and emission factor (version~2.1), European Environment Agency, Copenhagen, 2000. Odum, J. R., Jungkamp, T. P. W., Griffin, R. J., Flagan, R. C., and Seinfeld, J. H.: The atmospheric aerosol-forming potential of whole gasoline vapor, Science, 276, 96–99, 1997. 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. Ossés, D. E., Zah, R., Trivino, R., and Hurni, H.: Spatial accuracy of a simplified disaggregation method for traffic emissions applied in seven mid-sized Chilean cities, Atmos. Environ., 42, 1491–1502, 2008. Sagebiel, J. C., Zielinska, B., Pierson, W. R., and Gertler, A. W.: Real-world emissions and calculated reactivities of organic species from motor vehicles, Atmos. Environ., 30, 2287–2296, 1996. Schauer, J. J., Kleeman, M. J., Cass, G. R., and Simoneit, B. R. T.: Measurement of emissions from air pollution sources. 5. C-1-C-32 organic compounds from gasoline-powered motor vehicles, Environ. Sci. Technol., 36, 1169–1180, 2002. Schmitz, T., Hassel, D., and Weber, F. J.: Determination of VOC-components in the exhaust of gasoline and diesel passenger cars, Atmos. Environ., 34, 4639–4647, 2000. Shi, L., Wang, Q. D., and Fu, M. L.: Application of situation of residents travel to estimate vehicles emissions in Beijing, Natural Science Edition, Journal of Beijing Technology and Business University, 2, 12–15, 2009 \mbox(in Chinese). Song, Y., Shao, M., Liu, Y., Lu, S. H., Kuster, W., Goldan, P., and Xie, S. D.: Source apportionment of ambient volatile organic compounds in Beijing, Environ. Sci. Technol., 41, 4348–4353, 2007. Staehelin, J., Locher, R., Monkeberg, S., and Stahel, W. A.: Contribution of road traffic emissions to ambient air concentrations of hydrocarbons: The interpretation of monitoring measurements in Switzerland by principal component analysis and road tunnel measurements, International Journal of Vehicle Design, 27, 161–172, 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, doi:10.1029/2002JD003093, 2003. Tang, J. H., Chan, L. Y., Chan, C. Y., Li, Y. S., Chang, C. C., Wang, X. M., Zou, S. C., Barletta, B., Blake, D. R., Wu., D.: Implications of changing urban and rural emissions on non-methane hydrocarbons in the Pearl River Delta region of China, Atmos. Environ., 42, 3780–3794, 2008. Tonooka, Y., Kannari, A., Higashino, H., and Murano, K.: NMVOCs and CO emission inventory in east Asia, Water Air Soil Poll., 130, 199–204, 2001. Tsai, W. Y., Chan, L. Y., Blake, D. R., and Chu, K. W.: Vehicular fuel composition and atmospheric emissions in South China: Hong Kong, Macau, Guangzhou, and Zhuhai, Atmos. Chem. Phys., 6, 3281–3288, 2006. Tuia, D., Ossés, D.E., Zah, R., Osses, M., Zarate, E., and Clappier, A.: Evaluation of a simplified top-down model for the spatial assessment of hot traffic emissions in mid-sized cities, Atmos. Environ., 41, 3658–3671, 2007. US Environmental Protection Agency: SPECIATE Version~3.2, available at http://www.epa.gov/ttn/chief/software/speciate/speciate32.html, 2000. US Environmental Protection Agency.: 1970–2007 Average annual emissions, all criteria pollutants in MS Excel, available at http://www.epa.gov/ttnchie1/trends, 2008. 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, 2007. Wadden, R. A., Uno, I., and Wakamatsu, S.: Source discrimination of short-term hydrocarbon samples measured aloft, Environ. Sci. Technol., 20, 473–483, 1986. Wang, L. Z., Sui, Q., Xie, Q., and Yu, Y. Q.: Definition of emission factor of vehicle in Jinan, Transportation Environmental Protection, 2, 18–20, 2002 (in Chinese). Wang, Q. D., He, K. B., Yao, Z. L., and Huo, H.: Research in motor vehicle driving cycle of Chinese cities, Environmental Pollution and Control, 10, 745–748, 2007 \mbox(in Chinese). Wei, W., Wang, S. X., Chatani, S., Klimont, Z., Cofala, J., and Hao, J. M.: Emission and speciation of non-methane volatile organic compounds from anthropogenic sources in China, Atmos. Environ., 42, 4976–4988, 2008. Xie, S. D., Song, X. Y., and Shen, X. H.: Calculating vehicular emission factors with COPERT III model in China, Environmental Science, 27, 3415–3419, 2006 \mbox(in Chinese). Yao, Z. L., Ma, Y. L., He, K. B., Huo, H., and Guo, T.: A study on the real-world vehicle emission characteristics in Ningbo, Acta Scientiae Circumstantiae, 26, 1229–1234, 2006 \mbox(in Chinese). Yao, Z. L., Wang, Q. D., and Hu, Y. X.: Study of vehicle driving cycle on realistic road in Chengdu city, Natural Science Edition, Journal of Beijing Technology and Business University, 1, 18–20, 2004 \mbox(in Chinese). Ye, S. B., Wang, Q. D., and He, X.: Tianjin on-road vehicle activity study, Natural Science Edition, Journal of Beijing Technology and Business University, 2, 28–31, 2007 \mbox(in Chinese). Yu, Y. C. and Yu, M. Y.: Estimation and forecast of for-hire motor vehicle emission volume, Journal of Highway and Transportation Research and Development, 6, 154–158, 2008 \mbox(in Chinese). Zhang, K. B. and Ruan, T. Y.: Statistical analysis of the measurement of vehicle driving cycles in China's six cities, Automobile Research and Development, 12, 33–36, 2005 \mbox(in Chinese). Zhang, T.: Analysis on characteristics of the resident trip and study on policy of the transport development in medium or small urban, Transportation Science & Technology, 3, 89–92, 2005 \mbox(in Chinese). Zhang, Y. H., Shao, M., and Yu, K. H.: Vehicle emissions, environmental impact and control, Chemical Industry Press, Beijing, 2004 \mbox(in Chinese). Zheng, J. Y., Che, W. W., and Wang, Z. L.: Traffic flow and road network-based spatial allocation of regional mobile source emission inventories, Acta Scientiae Circumstantiae, 29, 815–821, 2009 \mbox(in Chinese).