Atmospheric Chemistry and Physics www.atmos-chem-phys.net 1680-7316 1680-7324 9 18 2009 10.5194/acp-9-7183-2009 http://www.atmos-chem-phys.net/9/7183/2009/ http://www.atmos-chem-phys.net/9/7183/2009/acp-9-7183-2009.html http://www.atmos-chem-phys.net/9/7183/2009/acp-9-7183-2009.pdf 7183 7212 2009-09-29 Modelling the impacts of ammonia emissions reductions on North American air quality P. A. Makar paul.makar@ec.gc.ca M. D. Moran Q. Zheng S. Cousineau M. Sassi A. Duhamel M. Besner D. Davignon L.-P. Crevier V. S. Bouchet Air Quality Research Division, Science and Technology Branch, Environment Canada, Toronto, Ontario, Canada Air Quality Model Applications Section, Meteorological Service of Canada, Environment Canada, Montreal, Quebec, Canada A unified regional air-quality modelling system (AURAMS) was used to investigate the effects of reductions in ammonia emissions on regional air quality, with a focus on particulate-matter formation. Three simulations of one-year duration were performed for a North American domain: (1) a base-case simulation using 2002 Canadian and US national emissions inventories augmented by a more detailed Canadian emissions inventory for agricultural ammonia; (2) a 30% North-American-wide reduction in agricultural ammonia emissions; and (3) a 50% reduction in Canadian beef-cattle ammonia emissions. The simulations show that a 30% continent-wide reduction in agricultural ammonia emissions lead to reductions in median hourly PM_2.5 mass of <1 μg m^&minus;3 on an annual basis. The atmospheric response to these emission reductions displays marked seasonal variations, and on even shorter time scales, the impacts of the emissions reductions are highly episodic: 95th-percentile hourly PM_2.5 mass decreases can be up to a factor of six larger than the median values. <br><br> A key finding of the modelling work is the linkage between gas and aqueous chemistry and transport; reductions in ammonia emissions affect gaseous ammonia concentrations close to the emissions site, but substantial impacts on particulate matter and atmospheric deposition often occur at considerable distances downwind, with particle nitrate being the main vector of ammonia/um transport. Ammonia emissions reductions therefore have trans-boundary consequences downwind. Calculations of critical-load exceedances for sensitive ecosystems in Canada suggest that ammonia emission reductions will have a minimal impact on current ecosystem acidification within Canada, but may have a substantial impact on future ecosystem acidification. The 50% Canadian beef-cattle ammonia emissions reduction scenario was used to examine model sensitivity to uncertainties in the new Canadian agricultural ammonia emissions inventory, and the simulation results suggest that further work is needed to improve the emissions inventory for this particular sector. It should be noted that the model in its current form neglects coarse mode base cation chemistry, so the predicted effects of ammonia emissions reductions shown here should be considered upper limits. Aber, J. D. and Magill, A. H.: Chronic nitrogen additions at the Harvard Forest (USA): the first 15 years of a nitrogen saturation experiment, Forest Ecol. Manage., 196, 1–5, 2004. Adema, E. H., Heeres, P., and Hulskotte, J.: On the dry deposition of NH₃, SO₂, and NO₂ on wet surfaces in a small scale wind tunnel. edited by: Hartman, H. F., Proceedings of the Seventh World Clean Air Congress, Clean Air Society of Australia and New Zealand, 2, 1–8, 1986. Anlauf, K. G., Lusis, M. A., and Wiebe, H. A.: Toronto Air Quality Study, Env Canada report ARQA-60-78, 1978. Ansari, A. S. and Pandis, S. N.: Response of inorganic PM to precursor concentrations, Environmental Science and Technology, 32, 2706–2714, 1998. Ansari, A. S. and Pandis, S. N. Prediction of multicomponent inorganic atmospheric aerosol behavior, Atmos. Environ., 33, 745–757, 1999. Ayres, J., Bittman, S., Girdhar, S., Sheppard, S., Niemi, D., Ratté, D., Smith, P.: Chapter 5: Sources of Ammonia Emissions. \textitIn Environment Canada. The 2008 Canadian Atmospheric Assessment of Agricultural Ammonia, Environment Canada, Gatineau, QC, Canada, in press, 2009. Binkowski F. S. and Shankar U.: The Regional Particulate Matter Model. 1. Model description and preliminary results, J. Geophys. Res., 100, 26, 191–26, 1995. Binkowski, F. S. and Roselle S. J.: Models-3 Community Multiscale Air Quality (CMAQ) model aerosol component 1. Model description, J. Geophys. Res. Atmos., 108, AAC 3-1–3-18, 2003. Bittman, S., Ayres, J., Sheppard, S., and Girdhar, S.: Chapter 4: Emission Inventory Development. \textitIn Environment Canada, The 2008 Canadian Atmospheric Assessment of Agricultural Ammonia (in press), Environment Canada, Gatineau, QC, Canada, 2008. Blanchard, C. L., Roth, P. M., Tanenbaum, S. J., Ziman, S. D., and Seinfeld, J. H.: The use of ambient measurements to identify which precursor species limit aerosol formation, J. Air Waste Manage. Assoc., 50, 2073–2084, 2000. Brosset, C.: Water-soluble sulphur compounds in aerosols, Atmos. Environ., 12, 25–38, 1978. Carolina Environmental Program (CEP): Sparse Matrix Operator Kernel Emission (SMOKE) modelling system, University of North Carolina, Carolina Environmental Programs, Chapel Hill, NC, online available at: http://www.smoke-model.org/index.cfm, 2003. Chang, J. S., Brost, R. A., Isaksen, I. S. A., Madronich, S., Middleton, P., Stockwell, W. R., Walcek, C. J.: A three-dimensional Eulerian acid deposition model: Physical concepts and formulation, J. Geophys. Res., 92, 14681–14700, 2003. Coste, J. H. and Courtier, G. B.: Sulphuric acid as a disperse phase in town air, T. Faraday Soc., 32, 1198–1202, 1936. Côté, J., Gravel, S., Méthot, A., Patoine, A., Roch, M., and Staniforth, A.: The operational CMC-MRB Global Environmental Multiscale (GEM) model. Part 1: Design considerations and formulation, Mon. Weather Rev., 126, 1373–1395, 1998. D'Ans, J.: Zur Kenntnis der Suaren Sulfate VII. Sulfate und Pyrosulfate des Natrium, Kalium und Ammonium. Z. Allg. Anorg, On the knowledge of acidic sulphate VII. Acid sulphate and pyro-sulphate of sodium, potassium and ammonium, Journal for Inorganic and General Chemistry Ch., 80, 235–245, 1913. Denman, K. L., Brasseur, G., Chidthaisong, A., Ciais, P., Cox, P.M., Dickinson, R. E., Hauglustaine, D., Heinze, C., Holland, E., Jacob, D., Lohmann, U., Ramachandran, S., da Silva, P. L., Wofsy, S. C., and Zhang, X. Couplings Between Changes in the Climate System and Biogeochemistry, in: Climate Change 2007: The Physical Science Basis. Contribution of Working Group I to the Fourth Assessment Report of the Intergovernmental Panel on Climate Change edited by: Solomon, S., Qin, D., Manning, M., Chen, Z., Marquis, M., Averyt, K. B., Tignor, M., Miller, H. L., Cambridge University Press, Cambridge, UK and New York, USA, 499–587, 2007. Dentener, F., Drevet, J., Lamarque, J. F., Bey, I., Eickhout, B., Fiore, A. M., Hauglustaine, D., Horowitz, L. W., Krol, M., Kulshrestha, U. C., Lawrence, M., Galy-Lacaux, C., Rast, S., Shindell, D., Stevenson, D., Van Noije, T., Atherton, C., Bell, N., Bergman, D., Butler, T., Cofala, J., Collins, B., Doherty, R., Ellingsen, K., Galloway, J., Gauss, M., Montanaro, V., Muller, J.-F., Pitari, G., Rodriguez, J., Sanderson, M., Solmon, F., Strahan, S., Schultz, M., Sudo, K., Szopa, S., and Wild, O. Nitrogen and sulfur deposition on regional and global scales: A multimodel evaluation, Global Biogeochem. Cy., 20, GB4003, doi:10.1029/2005GB002672, 2006. Eder, B. and Yu, S.: A performance evaluation of the 2004 release of Models-3 CMAQ, Atmos. Environ., 40, 4811–4824, 2006. Erisman, J. W., Vanelzakker, B. G., Mennen, M. G., Hogenkamp, H., Zwart, E., Van den Beld, L., Romer, F. G., Bobbink, R., Heil, G., Raessen, M., Duyzer, J. H., Verhage, H., Wyers, G. P., Otjes, R. P., and Möls, J. J.: The Elspeetsche Veldexperiment on surface exchange of trace gases: summary of results, Atmos. Environ., 28, 487–496, 1994a. Erisman, J.W., Mennen, M., Hogenkamp, J., Kemkers, E., Godhart, D., van Pul, A., Draaijers, G., Duyzer, J., Wyers, P.: Dry deposition monitoring of SO₂, NH₃ and NO₂ over a coniferous forest, in: Proceedings of EUROTRAC Symposium '94, edited by: Borrell, P. M., Borrell, P., Cvitas, T., and Seiler, W., The Hague, The Netherlands, 655–659, 1994b. Fenn, R. W., Gerber, H. E., and Wasshuasen, D.. Measurements of the sulphur and ammonium component of the arctic aerosol of the Greenland icecap, J. Atmos. Sci., 20, 466–468, 1963. Fenn, M. E., Jovan, S., Yuan, F., Geiser, L., Meixner, T., and Gimeno, B. S.: Empirical and simulated critical loads for nitrogen deposition in California mixed conifer forests, Environ. Poll., 155, 492–511, 2008. Fowler, D., Cape, J. N., Coyle, M., Smith, R. I., Hjellbrekke, A.-G., Simpson, D., Derwent, R. G., and Johnson, C. E.: Modelling photochemical oxidant formation, transport, deposition and exposure of terrestrial ecosystems, Environ. Poll., 100, 43–55, 1998. Fung, C. S., Misra, P. K., Bloxam, R., and Wong, S.: A numerical experiment on the relative importance of H₂O₂ and O₃ in aqueous conversion of SO₂ to SO₄, Atmos. Environ., 25A, 411–423, 1991. Gilliland, A. B., Appel, K. W., Pinder, R. W., and Dennis, R. L.: Seasonal NH₃ emissions for the continental United States: inverse model estimation and evaluation, Atmos. Environ., 40, 4986–4998, 2006. Gong, W., Dastoor, A. P. , Bouchet, V. S. , Gong, S. , Makar, P. A., Moran, M. D., Pabla, B. , Ménard, S. , Crevier, L.-P. , Cousineau, S., and Venkatesh, S.: Cloud processing of gases and aerosols in a regional air quality model (AURAMS), Atmos. Res., 82, 248–275, 2006. Gordon, R. J. and Bryan, R. J.: Ammonium nitrate in airborne particles in Los Angeles, Environmental Science and Technology, 7, 645–647, 1973. Hall, J., Hornung, M., Kennedy, F., Langan, S., Reynolds, B., and Aherne, J.: Investigating the uncertainties in the simple mass balance equation for acidity critical loads for terrestrial ecosystems. Water Air Soil Pollut. Focus, 1, 43–56, 2001. Heard, M. J. and Wiffen, R. D.: Electron microscopy of natural aerosols and the identification of particulate ammonium sulphate, Atmos. Environ., 3, 337-340, 1969. Herrmann, H., Ervens, B., Jacobi, H.-W., Wolke, R., Nowack, P., and Zellner, R.: CAPRAM2.3: A Chemical Aqueous Phase Radical Chemistry for Tropospheric Chemistry, J. Atmos. Chem., 36, 231–284, 2000. Herrmann, H., Tilgner, A., Barzaghi, P., Majdik, Z., Gligorovski, S., Poulain, L., and Monod, A.: Towards a more detailed description of tropospheric aqueous phase organic chemistry: CAPRAM 3.0., Atmos. Environ., 39, 4351–4363, 2005. Houyoux, M. R., Vukovich, J. M., Coats, C. J. Jr., and Wheeler, N. J. M.: Emission inventory development and processing for the Seasonal Model for Regional Air Quality (SMRAQ) project, J. Geophys. Res., 105, 9079–9090, 2000. Jeffries, D. S. and Ouimet, R.: Critical loads: are they being exceeded? [In] Chapter 8 of Canadian Acid Deposition Science Assessment 2004, Environment Canada, 4905 Dufferin Street, Downsview, Canada, 440 pp., online available at: http://www.msc-smc.ec.gc.ca/saib/acid/acid_e.html, 2005. Jeffries, D. S., Lam, D. C. L., Moran, M. D., and Wong, I.: The effect of SO₂ emission controls on critical load exceedances for lakes in southeastern Canada, Water Sci. Tech., 39, 165–171, 1999. Junge, C. E. and Ryan, T. G.: Study of the SO2 oxidation in solution and its role in atmospheric chemistry, Q. J. Roy. Meteor. Soc., 84, 46–55, 1958. Kaste, Ø, Henriksen, A., and Posch, M.: Present and potential nitrogen outputs from Norwegian soft water lakes – an assessment made by applying the steady-state First-order Acidity Balance (FAB) model, \textitHydrol. Earth Syst. Sci., 6, 101–112, 2002. Kusik, C. L. and Meissner, H. P.: Electrolyte activity coefficients in inorganic processing, A.I.Ch.E. Symposium 173, 14–20, 1978. Logan, J. A.: An analysis of ozonesonde data for the troposphere: Recommendations for testing 3-D models, and development of a gridded climatology for tropospheric ozone, J. Geophys. Res., 104, 16115–16149, 1998. Luo, C., Zender, C. S., Bian, H., and Metzger, S.: Role of ammonia chemistry and coarse mode aerosols in global climatological inorganic aerosol distributions, Atmos. Environ., 41, 2510–2533, 2007. MacDonald, A. M., Anlauf, K. G., Leaitch, W. R., and Liu, P. S.: Multi-year Chemistry of Particles and Selected Trace Gases at the Whistler High Elevation Site, EOS Trans., AGU 87(52), Fall Meet., Suppl., Abstract A53b-0179, 2006. Makar, P. A., Bouchet, V. S., and Nenes, A.: Inorganic chemistry calculations using HETV – a vectorized solver for the SO$_4^2-$-NO$_3^-$ -NH$_4^+$ system based on the ISORROPIA algorithms, Atmos. Environ., 37, 2279–2294, 2003. Mathur, R. and Dennis, R. L.: Seasonal and annual modeling of reduced nitrogen compounds over the eastern United States: Emissions, ambient levels, and deposition amounts, J. Geophys. Res. Atmos., 108, ACH 22-1–ACH 22-19 2003. McNulty, S. G., Cohen, E. C., Moore Myers, J. A., Sullivan, T. J., and Li, H.: Estimates of critical acid loads and exceedances for forest soils across the conterminous United States, Environ. Pollut., 149, 281–292, 2007. Moran, M. D., Zheng, Q., Samaali, M., Narayan, J., Pavlovic, R., Cousineau, S., Bouchet, V. S., Sassi, M., Makar, P. A., Gong, W., Gong, S., Stroud, C., and Duhamel, A.: Comprehensive surface-based performance evaluation of a size-and composition-resolved regional particulate-matter model for a one-year simulation. Proc. 29th NATO/SPS ITM on Air Pollution Modelling and Its Application, Aveiro, Portugal, 24–28 Sept., 9 pp., published in Air Pollution Modeling and its Application XIX, 2008, edited by: Borrego, C. and Miranda, A. I., Springer, Dordrecht, The Netherlands, 434–442, 2007. Moran, M. D., Zheng, Q., Pavlovic, R., Cousineau, S., Bouchet, V. S., Sassi, M., Makar, P. A., Gong, W., and Stroud, C.: Predicted acid deposition critical-load exceedances across Canada from a one-year simulation with a regional particulate-matter model. Proc. 15th Joint AMS/A&WMA Conf. on Applications of Air Pollution Meteorology, 21–24 January, New Orleans, American Meteorological Society, Boston, 20 pp., online available at: http://ams.confex.com/ams/pdfpapers/132916.pdf, 2008. Neirynck, J., Kowalski, A. S., Carrara, A., Ceulemans, R.: Driving forces for ammonia fluxes over mixed forest subjected to high deposition loads, Atmos. Environ., 39, 5013–5024, 2005. Pinder, R. W., Adams, P. J., and Pandis, S. N.: Ammonia emission controls as a costeffective strategy for reducing atmospheric particulate matter in the eastern United States, Environ. Sci. Technol., 41, 380–386, 2007. Phillips, S. B., Aneja, V. P., Kang, D., and Arya, S. P.: Modelling and analysis of the atmospheric nitrogen deposition in North Carolina, International Journal of Global Environmental Issues, 6, 231–252, 2006. Pinder, R. W., Gilliland, A. B., and Dennis, R. L.: Environmental impact of atmospheric NH3 emissions under present and future conditions in the eastern United States, Geophys. Res. Lett., 35, L12808, doi:10.1029/2008GL033732, 2008. Quan, J. and Zhang, X.: Assessing the role of ammonia in sulfur transformation and deposition in China, Atmos. Res., 88, 78–88, 2008. Robbins, R. C. and Cadle, R. D.: Kinetics of the reaction between gaseous ammonia and sulfuric acid droplets in an aerosol, J. Phys. Chem., 62, 469–471, 1958. Schwarze, P. E., Orevik, J., Lag, M., Refsnes, M., Nafstad, P., Hetland, R. B., and Dybing, E.: Particulate matter properties and health effects: Consistency of epidemiological and toxicological studies, Human and Experimental Toxicology, 25, 559–579, 2006. Scire, J. S., Lurmann, F. W., Karamchandani, P., Venkatram, A., Yamartino, R., Young, J., and Pleim, J.: ADOM/TADAP Model Development Program, Volume 9: User's Guide, Environmental Research and Technology, Inc., Newbury Park, California, USA, 1986. Seinfeld, J. H. and Pandis, S. N.: Atmospheric chemistry and physics: from air pollution to climate change, John Wiley and Sons, Inc., New York, USA, 1326 pp., 1998. Spranger, T., Hettelingh, J.-P., Slootweg, J., Posch, M.: Modelling and mapping long-term risks due to reactive nitrogen effects: An overview of LRTAP convention activities, Environ. Pollut., 154, 482–487, 2008. Spurny, K. and Heard, M. J.: Discussions: Electron microscopy of natural aerosols and the identification of particulate ammonium sulphate. Atmos. Environ., 3, 483, 1969. Stelson, A. W., Friedlander, S. K. and Seinfeld, J. H.: A note on the equilibrium relationship between ammonia and nitric acid and particulate ammonium nitrate, Atmos. Environ., 13, 369–371, 1979. Stilg, M.: World-wide limits for toxic and hazardous chemicals. Noyes Publications, NJ, USA, 792 pp., 1994. Stockwell, W. R. and Calvert, J. G.: The mechanism of the HO-SO₂ reaction, Atmos. Environ., 17, 2231–2235, 1983. Sutton, M. A., Asman, W. A. H., SchjoØrring, J. K.: Dry deposition of reduced nitrogen, Tellus 46, 255–273, 1994. Tanner, R. L.: An ambient experimental study of phase equilibrium in the atmospheric system: aerosol H$^+$, NH$_4^+$, SO$_4^2-$, NO$_3^-$, NH₃(g), HNO₃(g), Atmos. Environ., 16, 2935–2942, 1983. Tsimpidi, A. P., Karydis, V. A., and Pandis, S. N.: Response of Inorganic Fine Particulate Matter to Emission Changes of Sulfur Dioxide and Ammonia: The Eastern United States as a Case Study, J. Air Waste Manage. Assoc., 57, 1489–1498, 2007. Van Hove, L. W. A., Adema, E. H., Vredenberg, W. H., and Pieters, G. A.: A study of the adsorption of NH₃ and SO₂ on leaf surfaces. Atmos. Environ., 23, 1479–1486, 1989. Venkatram, A. and Karamchandani, P. K.: Testing a comprehensive acid deposition model. Atmospheric Environment, 22, 737–747, 1988. Wang, J., Deeter, M. N., Gille, J. C., and Bailey, P. L.: Retrieval of tropospheric carbon monoxide profiles from MOPITT: Algorithm description and retrieval simulation, Proc. SPIE – Int. Soc. Opt. Eng., 3756, 437–446, 1999. Wang, Z., Xie, F., Sakurai, T., Ueda, H., Han, Z., Carmichael, G. R., Streets, D., Engardt, M., Holloway, T., Hayami, H., Kajino, M., Thongboonchoo, N., Bennet, C., Park, S. U., Fung, C., Chang, A., Sartelet, K., and Amann, M.: MICS-Asia II: Model inter-comparison and evaluation of acid deposition, Atmos. Environ., 42, 3528–3542, 2008. West, J. J., Ansari, A. S., and Pandis, S. N.: Marginal PM$_2.5$: Nonlinear aerosol mass response to sulfate reductions in the eastern United States, J. Air Waste Manage. Assoc., 49, 1415–1424, 1999. Wright, R. F., Alewell, C., Cullen, J. M., Evans, C. D., Marchetto, A., Moldan, F., Prechtel, A., and Rogora, M.: Trends in nitrogen deposition and leaching in acid-sensitive streams in Europe, Hydrol. Earth Syst. Sci., 5, 299–310, 2001. Ying, Q. and Kleeman, M. J.: Source contributions to the regional distribution of secondary particulate matter in California. Atmos. Environ., 40, 736–752, 2006. Yu, S., Dennis, R., Roselle, S., Nenes, A., Walker, J., Eder, B., Schere, K., Swall, J., and Robarge, W.: An assessment of the ability of three-dimensional air quality models with current thermodynamic equilibrium models to predict aerosol NO$_3^-$. J. Geophys. Res., 110, doi:10.1029/2004JD004718, 22 pp., 2005. Zhang, L., Gong, S., Padro, J., and Barrie, L.: A size-segregated particle dry deposition scheme for an atmospheric aerosol module. Atmos. Environ., 35, 549–560, 2001. Zhang, L., Moran, M. D., Makar, P. A., Brook, J. R., and Gong, S.: Modelling gaseous dry deposition in AURAMS: a unified regional air-quality modelling system. Atmos. Environ., 36, 537–560, 2002.