ACP Atmospheric Chemistry and Physics ACP Atmos. Chem. Phys. 1680-7324 Copernicus Publications Göttingen, Germany 10.5194/acp-10-3545-2010 Hydrochlorofluorocarbon and hydrofluorocarbon emissions in East Asia determined by inverse modeling Stohl A. 1 Kim J. 2 Li S. 2 O'Doherty S. 3 Mühle J. 4 Salameh P. K. 4 Saito T. 5 Vollmer M. K. 6 Wan D. 7 Weiss R. F. 4 Yao B. 8 Yokouchi Y. 5 Zhou L. X. 8 Norwegian Institute for Air Research, Kjeller, Norway School of Earth and Environmental Sciences, Seoul National University, Seoul, Korea School of Chemistry, University of Bristol, Bristol, UK Scripps Institution of Oceanography, University of California, San Diego, California, USA National Institute for Environmental Studies, Tsukuba, Japan Swiss Federal Laboratories for Materials Testing and Research (Empa), Duebendorf, Switzerland State Key Joint Laboratory for Environmental Simulation and Pollution Control, Peking University, Beijing, China Centre for Atmosphere Watch and Services, Key Laboratory for Atmospheric Chemistry, Chinese Academy of Meteorological Sciences, Beijing, China 16 04 2010 10 8 3545 3560 Copyright: © 2010 A. Stohl et al. 2010 This work is licensed under the Creative Commons Attribution 3.0 Unported License. To view a copy of this licence, visit https://creativecommons.org/licenses/by/3.0/ This article is available from https://acp.copernicus.org/articles/10/3545/2010/acp-10-3545-2010.html The full text article is available as a PDF file from https://acp.copernicus.org/articles/10/3545/2010/acp-10-3545-2010.pdf

The emissions of three hydrochlorofluorocarbons, HCFC-22 (CHClF<sub>2</sub>), HCFC-141b (CH<sub>3</sub>CCl<sub>2</sub>F) and HCFC-142b (CH<sub>3</sub>CClF<sub>2</sub>) and three hydrofluorocarbons, HFC-23 (CHF<sub>3</sub>), HFC-134a (CH<sub>2</sub>FCF<sub>3</sub>) and HFC-152a (CH<sub>3</sub>CHF<sub>2</sub>) from four East Asian countries and the Taiwan region for the year 2008 are determined by inverse modeling. The inverse modeling is based on in-situ measurements of these halocarbons at the Japanese stations Cape Ochi-ishi and Hateruma, the Chinese station Shangdianzi and the South Korean station Gosan. For every station and every 3 h, 20-day backward calculations were made with the Lagrangian particle dispersion model FLEXPART. The model output, the measurement data, bottom-up emission information and corresponding uncertainties were fed into an inversion algorithm to determine the regional emission fluxes. The model captures the observed variation of halocarbon mixing ratios very well for the two Japanese stations but has difficulties explaining the large observed variability at Shangdianzi, which is partly caused by small-scale transport from Beijing that is not adequately captured by the model. Based on HFC-23 measurements, the inversion algorithm could successfully identify the locations of factories known to produce HCFC-22 and emit HFC-23 as an unintentional byproduct. This lends substantial credibility to the inversion method. We report national emissions for China, North Korea, South Korea and Japan, as well as emissions for the Taiwan region. Halocarbon emissions in China are much larger than the emissions in the other countries together and contribute a substantial fraction to the global emissions. Our estimates of Chinese emissions for the year 2008 are 65.3&plusmn;6.6 kt/yr for HCFC-22 (17% of global emissions extrapolated from Montzka et al., 2009), 12.1&plusmn;1.6 kt/yr for HCFC-141b (22%), 7.3&plusmn;0.7 kt/yr for HCFC-142b (17%), 6.2&plusmn;0.7 kt/yr for HFC-23 (>50%), 12.9&plusmn;1.7 kt/yr for HFC-134a (9% of global emissions estimated from Velders et al., 2009) and 3.4&plusmn;0.5 kt/yr for HFC-152a (7%).

 References Ashford, P., Clodic, D., McCulloch, A., and Kuijpers, L.: Emission profiles from the foam and refrigeration sectors comparison with atmospheric concentrations. Part 2: Results and discussion, Intern. J. Refrigeration, 27, 701–716, 2004. Barletta, B., Meinardi, S., Simpson, I. J., Rowland, F. S., Chan, C.-Y., et al.: Ambient halocarbon mixing ratios in 45 Chinese cities, Atmos. Environ., 40, 7706–7719, 2006. Blake N. J. Blake, D. R., Simpson, I. J., Meinardi, S., Swanson, A. L., et al.: NMHCs and halocarbons in Asian continental outflow during the Transport and Chemical Evolution over the Pacific (TRACE-P) Field Campaign: Comparison With PEM-West B, J. Geophys. Res., 108, 8806, https://doi.org/10.1029/2002JD003367, 2003. Chan, C. Y., Tang, J. H., Li, Y. S., and Chan, L. Y.: Mixing ratios and sources of halocarbons in urban, semi-urban and rural sites of the Pearl River Delta, South China, Atmos. Environ., 40, 7331–7345, 2006. Center for International Earth Science Information Network (CIESIN): Gridded Population of the World: Future Estimates, Socioeconomic Data and Applications Center (SEDAC), Columbia University, Palisades, NY, USA,available online at: <a href="http://sedac.ciesin.columbia.edu/gpw">http://sedac.ciesin.columbia.edu/gpw</a> (downloaded on 22 April 2008), 2005. Dunse, B., Steele, P., Wilson, S., Fraser, P., and Krummel, P.: Trace gas emissions from Melbourne Australia, based on AGAGE observations at Cape Grim, Tasmania, 1995–2000, Atmos. Environ., 39, 6334–6344, 2005. European Commission, Joint Research Centre (JRC)/Netherlands Environmental Assessment Agency (PBL): Emission Database for Global Atmospheric Research (EDGAR), release version 4.0, available from <a href="http://edgar.jrc.ec.europa.eu">http://edgar.jrc.ec.europa.eu</a>, 2009. Eckhardt, S., Prata, A. J., Seibert, P., Stebel, K., and Stohl, A.: Estimation of the vertical profile of sulfur dioxide injection into the atmosphere by a volcanic eruption using satellite column measurements and inverse transport modeling, Atmos. Chem. Phys., 8, 3881–3897, 2008. Greenhouse Gas Inventory Office of Japan (GIO): National Greenhouse Gas Inventory Report of JAPAN, Ministry of the Environment, Japan, 2009. Guo, H., Ding, A. J., Wang, T., Simpson, I. J., Blake, et al.: Source origins, modeled profiles, and apportionments of halogenated hydrocarbons in the greater Pearl River Delta region, southern China, J. Geophys. Res., 114, D11302, https://doi.org/10.1029/2008JD010360, 2009. Hartley, D. and Prinn, R.: Feasibility of determining surface emissions of trace gases using an inverse method in a three-dimensional chemical transport model, J. Geophys. Res., 98, 5183–5197, 1993. Hu, J., Wan, D., Li, C., Zhang, J., and Yi, X.: Forecasting of consumption and emission of HFC-134a used in automobile air conditioner sector in China, Adv. Clim. Change Res., 5, 1–6, (in Chinese), 2009. Kim, J., Li, S., Kim, K.-R. Stohl, A., Mühle, J. M., et al.: Regional atmospheric emissions determined from measurements at Jeju Island: Halogenated compounds from China, submitted, Geophys. Res. Lett., 2010. Manning, A. J., Ryall, D. B., Derwent, R. G., Simmonds, P. G., and O'Doherty, S.: Estimating European emissions of ozone-depleting and greenhouse gases using observations and a modeling back-attribution technique, J. Geophys. Res., 108, 4405, https://doi.org/10.1029/2002JD002312, 2003. McCulloch, A., Midgley, P. M., and Ashford, P.: Releases of refrigerant gases (CFC-12, HCFC-22 and HFC-134a) to the atmosphere, Atmos. Environ., 37, 889–902, 2003. McCulloch, A., Midgley, P. M., and Lindley, A. A.: Recent changes in the production and global atmospheric emissions of chlorodifluoromethane (HCFC-22), Atmos. Environ., 40, 936–942, 2006. McCulloch, A., Lindley, A. A.: Global emissions of HFC-23 estimated to the year 2015, Atmos. Environ., 41, 1560–1566, 2007. Miller, B. R., Weiss, R. F., Salameh, P. K., Tanhua, T., Greally, B. R., Mühle, J., and Simmonds, P. G.: Medusa: A sample preconcentration and GC/MS detector system for in situ measurements of atmospheric trace halocarbons, hydrocarbons, and sulfur compounds, Anal. Chem., 80, 1536–1545, 2008. Millet, D. B., Atlas, E. L., Blake, D. R., Blake, N. J., Diskin, G. S., et al. (2009): Halocarbon emissions from the United States and Mexico and their Global Warming Potential, Environ. Sci. Technol., 43, 1055–1060, 2009. Molina, M., Zaelke, D., Sarma, K. M., Andersen, S. O., Ramanathan, V., and Kaniaru, D. (2009): Reducing abrupt climate change risk using the Montreal Protocol and other regulatory actions to complement cuts in CO<sub>2</sub> emissions, Proc. Natl. Acad. Sci. USA, Early Edition, <a href="http://www.pnas.org/content/early/2009/10/09/0902568106.full.pdf">http://www.pnas.org/content/early/2009/10/09/0902568106.full.pdf</a>, 2009. Montzka, S. A., Hall, B. D., and Elkins, J. W.: Accelerated increases observed for hydrochlorofluorocarbons since 2004 in the global atmosphere, Geophys. Res. Lett., 36, L03804, https://doi.org/10.129/2008GL036475, 2009. Montzka, S. A., Kuijpers, L., Battle, M. O., Aydin, M., Verhulst, K., Saltzman, E. S., and Fahey, D. W.: Recent increases in global HFC-23 emissions, Geophys. Res. Lett., 37, L02808, https://doi.org/10.1029/2009GL041195, 2010. O'Doherty, S., Cunnold, D. M., Manning, A., Miller, B. R., Wang, R. H. J., et al.: Rapid growth of hydrofluorocarbon 134a and hydrochlorofluorocarbons 141b, 142b, and 22 from Advanced Global Atmospheric Gases Experiment (AGAGE) observations at Cape Grim, Tasmania, and Mace Head, Ireland, J. Geophys. Res., 109, D06310, https://doi.org/10.1029/2003JD004277, 2004. O'Doherty, S., Cunnold, D. M., Miller, B. R., Mühle, J., McCulloch, A., et al.: Global and regional emissions of HFC-125 (CHF<sub>2</sub>CF<sub>3</sub>) from in situ and air archive atmospheric observations at AGAGE and SOGE observatories, J. Geophys. Res., 114, D23304, https://doi.org/10.1029/2009JD012184. Palmer, P. I., Jacob, D. J., Mickley, L. J., Blake, D. R., Sachse, G. W., et al.: Eastern Asian emissions of anthropogenic halocarbons deduced from aircraft concentration data, J. Geophys. Res., 108, 4753, https://doi.org/10.1029/2003JD003591, 2003. Prinn, R. G., Weiss, R. F., Fraser, P. J., Simmonds, P. G., Cunnold, D. M., et al: A history of chemically and radiatively important gases in air deduced from ALE/GAGE/AGAGE, J. Geophys. Res., 105, 17751–17792, 2000. PRTR: Pollutant Release and Transfer Register Data, FY 2007, Ministry of Economy, Trade and Industry, and Ministry of the Environment (in Japanese), 2009. Seibert, P.: Inverse modelling of sulfur emissions in Europe based on trajectories, In: Inverse Methods in Global Biogeochemical Cycles, edited by :Kasibhatla, P., Heimann, M., Rayner, P., Mahowald, N., Prinn, R. G., and Hartley, D. E., Geophysical Monograph 114, American Geophysical Union, ISBN: 0-87590-097-6, 147–154, 2000. 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, 2005. Stohl, A., Seibert, P., Arduini, J., Eckhardt, S., Fraser, P., et al.: 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, 2009. Tsai, W. T.: Energy and environmental policies relating to hydrofluorocarbons (HFCs) emissions mitigation and energy conservation in Taiwan, Energy Conversion and Management, 47, 2308–2318, 2006. Tsai, W. T. and Chou, Y.-H.: Governmental policies on hydrochlorofluorocarbons (HCFCs) mitigation and its cleaner production measures – case study in Taiwan, J. Cleaner Production, 16, 646–654, 2008. United Nations Environment Programme (UNEP): Ozone Secretariat Data Access Centre, <a href="http://ozone.unep.org/Data_Reporting/Data_Access/">http://ozone.unep.org/Data_Reporting/Data_Access/</a>, UNEP, Nairobi, Kenya, accessed on 26 September 2009, 2009. Velders, G. J. M., Fahey, D. W., Daniel, J. S., McFarland, M., and Andersen, S. O.: The large contribution of projected HFC emissions to future climate forcing, Proc. Natl. Acad. Soc., 106, 10949–10954, 2009. Vollmer, M. K., Zhou, L. X., Greally, B. R., Henne, S., Yao, B., et al.: Emissions of ozone-depleting halocarbons from China, Geophys. Res. Lett., 36, L15823, https://doi.org/10.1029/2009GL038659, 2009. Wan, D., Xu, J., Zhang, J., Tong, X., and Hu, J.: Historical and projected emissions of major halocarbons in China, Atmos. Environ., 43, 5822–5829, 2009. Yokouchi, Y., Inagaki, T., Yazawa, K., Tamaru, T., Enomoto, T., and Izumi, K.: Estimates of ratios of anthropogenic halocarbon emissions from Japan based on aircraft monitoring over Sagami Bay, Japan, J. Geophys. Res., 110, D06301, https://doi.org/10.1029/2004JD005320, 2005. Yokouchi, Y., Taguchi, S., Saito, T., Tohjima, Y., Tanimoto, H., and Mukai, H.: High-frequency measurements of HFCs at a remote site in east Asia and their implications for Chinese emissions, Geophys. Res. Lett., 33, L21814, https://doi.org/10.1029/2006GL026403, 2006.