References

ACP

Atmospheric Chemistry and Physics

ACP

Atmos. Chem. Phys.

1680-7324

Copernicus Publications

Göttingen, Germany

10.5194/acp-9-7657-2009

Reactive nitrogen in atmospheric emission inventories

Reis

¹ Pinder

R. W.

² Zhang

³ Lijie

⁴ Sutton

M. A.

Centre for Ecology & Hydrology (CEH), Bush Estate, Penicuik, EH26 0QB, UK

US Environmental Protection Agency, Atmospheric Modeling Division, 109 T W Alexander Drive, Research Triangle Park, NC 27711, USA

Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing, China

The College of Environmental Science and Engineering, Nankai University, Tianjin, 300071, China

15 10 2009

9 19 7657 7677

2009

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/9/7657/2009/acp-9-7657-2009.html

The full text article is available as a PDF file from https://acp.copernicus.org/articles/9/7657/2009/acp-9-7657-2009.pdf

Excess reactive Nitrogen (Nr) has become one of the most pressing environmental problems leading to air pollution, acidification and eutrophication of ecosystems, biodiversity impacts, leaching of nitrates into groundwater and global warming. This paper investigates how current inventories cover emissions of Nr to the atmosphere in Europe, the United States of America, and China. The focus is on anthropogenic sources, assessing the state-of-the-art of quantifying emissions of Ammonia (NH3), Nitrogen Oxides (NOx) and Nitrous Oxide (N2O), the different purposes for which inventories are compiled, and to which extent current inventories meet the needs of atmospheric dispersion modelling. The paper concludes with a discussion of uncertainties involved and a brief outlook on emerging trends in the three regions investigated is conducted. Key issues are substantial differences in the overall magnitude, but as well in the relative sectoral contribution of emissions in the inventories that have been assessed. While these can be explained by the use of different methodologies and underlying data (e.g. emission factors or activity rates), they may lead to quite different results when using the emission datasets to model ambient air quality or the deposition with atmospheric dispersion models. Hence, differences and uncertainties in emission inventories are not merely of academic interest, but can have direct policy implications when the development of policy actions is based on these model results. The level of uncertainty of emission estimates varies greatly between substances, regions and emission source sectors. This has implications for the direction of future research needs and indicates how existing gaps between modelled and measured concentration or deposition rates could be most efficiently addressed. The observed current trends in emissions display decreasing NOx emissions and only slight reductions for NH3 in both Europe and the US. However, in China projections indicate a steep increase of both.

References 1

Akimoto, H. and Narita, H.: Distribution of SO2, NOx and CO2 emission from fuel combustion and industrial activities in Asia with 1$^{\circ}{\times}$1° resolution, Atmos. Environ., 28, 213–225, 1994.

Bai, N. B.: The emission inventory of SO2, NOx and CO2 in China. The Atmospheric Ozone Variation and Its Effect on the Climate and Environment in China, China Meteorological Press, 145–150, 1996.

Bergamaschi, P., Krol, M., Dentener, F., Vermeulen, A., Meinhardt, F., Graul, R., Ramonet, M., Peters, W., and Dlugokencky, E. J.: Inverse modelling of national and European CH4 emissions using the atmospheric zoom model TM5, Atmos. Chem. Phys., 5, 2431–2460, 2005

Bishop, G. A., and Stedman, D. H.: A Decade of On-road Emission Measurements, Environ. Sci. Technol., 42, 1651–1656, 2008.

Blackall, T. D., Wilson, L. J., Theobald, M. R., Milford, C., Nemitz, E., Bull, J., Bacon, P. J., Hamer, K. C., Wanless, S., and Sutton, M. A.: Ammonia emissions from seabird colonies, Geophys. Res. Lett., 34, L10801, https://doi.org/10.1029/2006GL028928, 2007.

Bleeker, A., Sutton, M. A., Acherman, B., Alebic-Juretic, A., Aneja, V. P., Ellermann, T., Erisman, J. W., Fowler, D., Fagerli, H., Gauger, T., Harlen, K. S., Hole, L. R., Horváth, L., Mitosinkova, M., Smith, R. I., Tang, Y. S., and van Pul., A.: Linking ammonia emission trends to measured concentrations and deposition of reduced nitrogen at different scales, in: Atmospheric Ammonia: Detecting emission changes and environmental impacts, edited by: Sutton, M. A., S. R. a. S. B., Springer, New York, USA, 123–180, 2009.

Bouwman, A. F., Lee, D. S., Asman, W. A. H., Dentener, F. J., Van der Hoek, K. W., and Olivier, J. G. J.: A global high-resolution emission inventory for ammonia, Global Biogeochem. Cy., 11, 561–587, 1997.

Bradshaw, J., Davis, D., Grodzinsky, G., Smyth, S., Newell, R., Sandholm, S., and Liu, S.: Observed distribution of nitrogen oxides in the remote free troposphere from the NASA global tropospheric experiment programs, Rev. Geophys., 38, 111–116, 2000.

Brasseur, G. P., Orlando, J. J., and Tyndall, G. S.: Atmospheric Chemistry and Global Change, Oxford University Press, New York, USA, 1999.

Crutzen, P. J., Mosier, A. R., Smith, K. A., and Winiwarter, W.: N2O release from agro-biofuel production negates global warming reduction by replacing fossil fuels, Atmos. Chem. Phys., 8, 389–395, 2008.

Del Grosso, S. J., Parton, W. J., Mosier, A. R., Hartman, M. D., Brenner, J., Ojima, D. S., Schimel, D. S.: Simulated Interaction of Carbon Dynamics and Nitrogen Trace Gas Fluxes Using the DAYCENT Model, in: Modeling Carbon and Nitrogen Dynamics for Soil Management edited by: Schaffer, M., Ma, L., and Hansen, S., CRC Press. Boca Raton, FL, USA, 303–332. 2001.

Dragosits, U., Dore, A., Sheppard, L., Vieno, M., Tang, Y. S., Theobald, M., and Sutton, M.: Sources, dispersion and fate of atmospheric ammonia. edited by: Hatfield, J. L., Follett, R. F., Nitrogen in the Environment - Sources, Problems, and Management, Academic Press, 333–393, 61 pp., 2008

EDGAR: Emissions Database for Global Atmospheric Research (EDGAR): <a href="http://edgar.jrc.ec.europa.eu/">http://edgar.jrc.ec.europa.eu/</a>, EDGAR v4, EDGAR FT32, EDGAR Hyde datasets, last access: 20 August 2009, 2009.

EMEP Webdab emission data hosted by the Centre on Emission Inventories and Projections (CEIP): <a href="http://www.ceip.at/">http://www.ceip.at/</a>, last access: 20 August 2009, 2009.

Erisman, J. W., Mosquera, J., and Hensen, A.: Two options to explain the ammonia gap in The Netherlands, Environmental Science & Policy, 4(2–3), 97–105, 2001.

Erisman, J. W.: The Nanjing Declaration on Management of Reactive Nitrogen, BioScience, 54, 286–287, 2004.

Erisman, J. W., Spranger, T., Sutton, M. A., Akselsson, C., Amin-Hanjani, S., Anderson, H. V., ApSimon, H., Fagerli, H., Harmens, H., Havlikova, M., Hettelingh, J. P., Hcks, K., Horvath, L., Hutchings, N. J., Maasikimets, M., Maione, M., Reis, S., and Stenby, C.: Working Group 5: Nitrogen – integrated environmental policies. Proceedings of the UNECE/EC Saltsjobaden 3 Workshop, 2007.

Erisman, J. W., Sutton, M. A., Galloway, J. N., Klimont, Z., and Winiwarter, W.: 100 years of ammonia synthesis: how a single patent changed the world, Nature Geosci., 1, 636–639, 2008.

Fowler, D., O'Donoghue, M., Muller, J. B. A., Smith, R. I., Dragosits, U., Skiba, U., Sutton, M. A., and Brimblecombe, P.: A Chronology of Nitrogen Deposition in the UK between 1900 and 2000, Water, Air and Soil Pollution: Focus, 4, 9–23, 2004.

Friedrich, R.: Natural and biogenic emissions of environmentally relevant atmospheric trace constituents in Europe, Atmos. Environ., 43(7), 1377-1379, 2008.

Galloway, J. N.: The global nitrogen cycle: changes and consequences, Environ. Poll., 102, 15–24, 1998.

Galloway, J. N., Aber, J. D., Erisman, J. W., Seitzinger, S. P., W., H. R., Cowling, E. B., and Cosby, B. J.: The nitrogen cascade, BioScience, 53, 341–356, 2003.

Galloway, J. N., Dentener, F. J., Capone, D. G., Boyer, E. W., Howarth, R. W., Seitzinger, S. P., Asner, G. P., Cleveland, C. C., Green, P. A., Holland, E. A., Karl, D. M., Michaels, A. F., Porter, J. H., Townsend, A. R., and Vorosmarty, C. J.: Nitrogen cycles: past, present and future, Biogeochemistry, 70, 153–226, 2004.

Galloway, J. N., Townsend, A. R., Erisman, J. W., Bekunda, M., Cai, Z., Freney, J. R., Martinelli, L. A., Seitzinger, S. P., and Sutton, M. A.: Transformation of the Nitrogen Cycle: Recent Trends, Questions and Potential Solutions, Science, 320, 889–892, 2008.

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.

Godowitch, J. M., Hogrefe, C., and Rao, S. T.: Diagnostic Analyses of a Regional Air Quality Model: Changes in Modeled Processes Affecting Ozone and Chemical-Transport Indicators from NOx Point Source Emission Reductions, J. Geophys. Res., 113, D19303, https://doi.org/10.1029/2007JD009537, 2008.

Goebes, M. D., Strader, R., and Davidson, C.: An ammonia emission inventory for fertilizer application in the United States, Atmos. Environ., 37, 2539–2550, 2003.

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

Henze, D. K., Seinfeld, J. H., and Shindell, D. T.: Inverse modeling and mapping US air quality influences of inorganic PM2.5 precursor emissions using the adjoint of GEOS-Chem, Atmos. Chem. Phys., Discuss., 8, 15031–15099, 2008.

Hettelingh, J. P., Posch, M., and Slootweg, J. (eds.): CCE Status Report 2008, Coordination Centre for Effects (CCE), 2008.

Horváth, L. and Sutton, M. A.: Long term record of ammonia and ammonium concentrations at K-puszta, Hungary, Atmos. Environ., 32, 339–344, 1998.

IIASA, The online version of the GAINS Model, <a href="http://gains.iiasa.ac.at/index.php/home-page">http://gains.iiasa.ac.at/index.php/home-page</a>, last access: 20 August 2009, 2009.

IPCC: Guidelines for National Greenhouse Gas Inventories: Greenhouse Gas Inventory Reference Manual (Revised 1996), IPCC/OECD/IGES, Bracknell, UK, 1997.

IPCC: Good Practice Guidance, Uncertainty Management in National Greenhouse Gas Inventorie, IPCC/IGES, Kanagawa, Japan, 2000, <a href="http://www.ipcc-nggip.iges.or.jp/public/gp/english/">http://www.ipcc-nggip.iges.or.jp/public/gp/english/</a>, last access: 21 August 2009.

Kato, N., and Akimoto, H.: Anthropogenic emissions of SO2 and NOx in Asia: Emission inventories, Atmos. Environ., 26A, 2997–3017, 1992.

Kim, S. W., Heckel, A., McKeen, S. A., Frost, G. J., Hsie, E. Y., Trainer, M. K., Richter, A., Burrows, J. P., Peckham, S. E., and Grell, G. A.: Satellite-observed US power plant NOx emission reductions and their impact on air quality, Geophys. Res. Lett., 33, L22812, https://doi.org/10.1029/2006GL027749, 2006.

Kim, S.-W., Heckel, A., Frost, G. J., Richter, A., Gleason, J., Burrows, J. P., McKeen, S., Hsie, E.-Y., Granier, C., and Trainer, M.: NO2 columns in the western United States observed from space and simulated by a regional chemistry model and their implications for NOx emissions, J. Geophys. Res., 114, D11301, https://doi.org/10.1029/2008JD011343, 2009.

Klaassen, G.: Options and Costs of Controlling Ammonia Emissions in Europe, Agricult. Econom., 21, 219–240, 1994.

Klimont, Z.: Current and Future Emissions of Ammonia in China. 10th International Emission Inventory Conference – "One Atmosphere, One Inventory, Many Challenges", US EPA, <a href="http://www.epa.gov/ttn/chief/conference/ei10/ammonia/klimont.pdf">http://www.epa.gov/ttn/chief/conference/ei10/ammonia/klimont.pdf</a>, last access: 22 December 2008, 2001a.

Klimont, Z.: Ammonia Emissions, Abatement Technologies and Related Costs for Europe in the RAINS model, International Institute for Applied Systems Analysis (IIASA), Laxenburg, Austria, 2001b.

Lee, D. S., Köhler, I., Grobler, E., Rohrer, F., Sausen, R., Gallardo-Klenner, L., Olivier, J. G. J., Dentener, F. J., and Bouwman, A. F.: Estimations of global NOx emissions and their uncertainties, Atmos. Environ., 31, 1735–1749, 1997.

Lehmann, C. M. B., Bowersox, V. C., Larson, R. S., and Larson, S. M.: Monitoring long-term trends in sulphate and ammonium in US precipitation: results from the National Atmospheric Deposition Program/National Trends Network, Water Air Soil Pollut. Focus, 7, 1567–7230, 2007, <a href="http://bqs.usgs.gov/acidrain/Deposition_trends.pdf">http://bqs.usgs.gov/acidrain/Deposition_trends.pdf</a>, last access: 1 August 2007.

Li, Y. E. and Lin, E.: Emissions of N2O, NH3 and NOx from fuel combustion, industrial processes and the agricultural sectors in China, Nutr. Cycl. Agroecosyst., 57, 99–106, 2000.

Li, C., Zhuang, Y., and Cao, M.: Comparing a national inventory of N2O emissions from arable lands in China developed with a process-based agroecosystem model to the IPCC methodology, Nutr. Cycl. Agroecosyst., 60, 159–170, 2001.

Lu, Y. Y., Huang, Y., Zou, J. W., and Zheng, X. H.: An inventory of N2O emissions from agriculture in China using precipitation-rectified emission factor and background emission, Chemosphere, 65, 1915–1924, 2006.

Ma, J. and Zhou, X. J.: Development of a three dimensional inventory of aircraft NOx emissions over China, Atmos. Environ., 34, 389–396, 2000.

Mosier, A. R., Duxbury, J. M., Freney, J. R., Heinemeyer, O., and Minami, K.: Assessing and mitigating N2O emissions from agricultural soils, Clim. Change, 40, 7–38, 1998.

NARSTO: Improving Emission Inventories for Effective Air Quality Management across North America, 2005.

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.

Olivier, J. G. J., Bouwman, A. F., Berdowski, J. J. M., Veldt, C., Bloos, J. P. J., Visschedijk, A. J. H., Van der Maas, C. W. M., and Zandveld, P. Y. J.: Sectoral emission inventories of greenhouse gases for 1990 on a per country basis as well as on 1$^{\circ}{\times}$1°, Environ. Sci. Pol., 2, 241–264, 1999.

Olivier, J. G. J. and Berdowski, J. J. M.: Global emissions sources and sinks, in: The Climate System, edited by: Berdowski, J., Guicherit, R., and Heij, B. J., A. A. Balkema Publishers/Swets & Zeitlinger Publishers, Lisse, The Netherlands, 33–78, 2001.

Olivier, J. G. J., Van Aardenne, J. A., Dentener, F., Ganzeveld, L., and Peters, J. A. H. W.:. Recent trends in global greenhouse gas emissions: regional trends and spatial distribution of key sources, in: "Non-CO2 Greenhouse Gases (NCGG-4)", van Amstel, A. (coord.), Millpress, Rotterdam, The Netherlands, ISBN: 90-5966-043-9, 325–330, 2005.

Parrish, D. D.: Critical evaluation of US on-road vehicle emission inventories, Atmos. Environ., 40, 2288–2300, 2006.

Pinder, R. W., Adams, P. J., Pandis, S. N., and Gilliland, A. B.: Temporally Resolved Ammonia Emission Inventories: Current Estimates, Evaluation Tools, and Measurement Needs, J. Geophys. Res., 111, D16310, https://doi.org/10.1029/2005JD006603, 2006.

Press, A.: China Agricultural Yearbook (in Chinese), Agricultural Press, Beijing, China, 1996.

Ravishankara, A. R., Daniel, J. S., Portmann, R. W.: Nitrous Oxide (N2O): The Dominant Ozone-Depleting Substance Emitted in the 21st Century. Science, 123–125, https://doi.org/10.1126/science.1176985, 2009.

Reis, S., Pfeiffer, H., Scholz, Y., and Theloke, J.: Temporal and Spatial Distribution of Carbon Emissions, in: The Continental-Scale Greenhouse Gas Balance of Europe, edited by: Dolman, H., Springer Publishers, 2008

Richter, A., Burrows, J.P., Nü{ß}, H., Granier, C., and Niemeier, U.: Increase in tropospheric nitrogen dioxide levels over China observed from space, Nature, 437, 129–132, 2005

Rypdal, K. and Winiwarter, W.: Uncertainties in Greenhouse Gas Inventories – Evaluation, comparability and implications, Environ. Sci. Pol., 4, 107–116, 2001.

Skiba, U., Sozanska, M., Metcalfe, S., and Fowler, D.: Spatially disaggregated inventories of soil NO and N2O emissions for Great Britain., Water Air Soil Poll., 1, 109–118, 2001.

Streets, D. G. and Waldhoff, S. T.: Present and future emissions of air pollutants in China: SO2, NOx and CO, Atmos. Environ., 34, 363–374, 2000.

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, 8809, https://doi.org/10.1029/2002JD003093, 2003.

Sutton, M. A., Dragosits, U., Tang. Y. S., and Fowler, D.: Ammonia emissions from non agricultural sources in the UK, Atmos. Environ., 34(6), 855–869, 2000.

Sutton, M. A., Asman, W. A. H., Ellerman, T., van Jaarsveld, J. A., Acker, K., Aneja, V., Duyzer, J. H., Horvath, L., Paramonov, S., Mitosinkova, M., Tang, Y. S., Achermann, B., Gauger, T., Bartnicki, J., Neftel, A., and Erisman, J. W.: Establishing the link between ammonia emission control and measurements of reduced nitrogen concentrations and deposition, Environ. Monit. Assess., 82, 149–185, 2003.

Sutton, M. A., Nemitz, E., Erisman, J. W., Beier, C., Butterbach Bahl, K., Cellier, P., de Vries, W., Cotrufo, M. F., Skiba, U., et al.: Challenges in quantifying biosphere-atmosphere exchange of nitrogen species, Environ. Poll., 150, 125–139, 2007.

Sutton, M. A., Erisman, J. W., Dentener, F., and Moeller, D.: Ammonia in the environment: from ancient times to the present, Environ. Poll., 156, 583–604, 2008.

Tian, H. Z., Hao, J. M., Lu, Y. Q., and Zhu, T. L.: The NOx emission distribution and inventory in China, China Environ. Sci., 21, 493–497, 2001.

UNEP: The Nanjing Declaration on Nitrogen Management Presented to the United Nations Environment Programme, 16th of October 2004, UNEP, Nanjing, China, 2004.

UNFCCC: Greenhouse Gas Inventory Data: <a href="http://unfccc.int/ghg_data/items/3800.php">http://unfccc.int/ghg_data/items/3800.php</a>, last access: 20 August 2009, 2009.

USDA: Agricultural Projections to 2016, USDA 2007.

USEPA: National Emission Inventory Tier Summaries: <a href="http://www.epa.gov/ttn/chief/eiinformation.html">http://www.epa.gov/ttn/chief/eiinformation.html</a>, last access 14 August 2009, 2009a

USEPA: Inventory of US Greenhouse Gas Emissions and Sinks: 1990–2007, <a href="http://epa.gov/climatechange/emissions/usinventoryreport.html">http://epa.gov/climatechange/emissions/usinventoryreport.html</a> last access: 14 August 2009, 2009b.

Van Aardenne, J. A., Carmichael, G. R., Levy II, H., Streets, D., and Hordjik, L.: Anthropogenic NOx emissions in Asia in the period 1990–2020, Atmos. Environ., 33, 633–646, 1999.

Van Aardenne, J. A., Dentener, F. J., Olivier, J. G. J., Klein Goldewijk, C. G. M. and Lelieveld, J.: A 1×1 degree resolution dataset of historical anthropogenic trace gas emissions for the period 1890–1990, Global Biogeochem. Cy., 15(4), 909–928, 2001.

Van Aardenne, J. A., Dentener, F., Olivier, J. G. J., and Peters, J. A. H. W.: The EDGAR 3.2 Fast Track 2000 dataset (32FT2000), 2005.

van der A, R. J., Peters, D. H. M. U., Eskes, H., Boersma, K. F., Van Roozendael, M., De Smedt, I., and Kelder, H. M.: Detection of the trend and seasonal variation in tropospheric NO2 over China, J. Geophys. Res., 111, D12317, https://doi.org/10.1029/2005JD006594, 2006.

Velthof, G. L., Oudendag, D., Witzke, H. P., Asman, W. A. H., Klimont, Z., and Oenema, O.: Integrated assessment of nitrogen emissions from agriculture in EU-27 using MITERRA EUROPE, J. Environ. Qual., 38, 402–417, https://doi.org/10.2134/jeq2008.0108, 2009.

Vestreng, V., Ntziachristos, L., Semb, A., Reis, S., Isaksen, I. S. A., and Tarrasón, L.: Evolution of NOx emissions in Europe with focus on road transport control measures, Atmos. Chem. Phys. Discuss., 8, 10697–10747, 2008.

Wallace, J. M. and Hobbes, P. V.: Atmospheric Science – An Introductory Survey. 2nd Edition, Elsevier Publishers, 2006.

Winiwarter, W. and Rypdal, K.: Assessing the uncertainty associated with national greenhouse gas emission inventories: a case study for Austria, Atmos. Environ., 35, 5425–5440, 2001.

Xing, G. X.: N2O emission from cropland in China, Nutr. Cy. Agroecosyst., 52, 249–254, 1998.

Yan, X. Y., Akimoto, H., and Ohara, T.: Estimation of nitrous oxide, nitric oxide and ammonia emissions from croplands in East, Southeast and South Asia, Global Change Biol., 9, 1080–1096, 2003.

Zhao, D. and Wang, A.: Estimation of Anthropogenic Ammonia Emissions in Asia, Atmos. Environ., 28, 689–694, 1994.

Zheng, X. H., Han, S. H., Huang, Y., Wang, Y. S., and Wang, M. X.: Re-quantifying the emission factors based on field measurements and estimating the direct N2O emission from Chinese croplands, Global Biogeochem. Cy., 18, GB2018, https://doi.org/10.1029/2003GB002167, 2004.

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, https://doi.org/10.1029/2007JD008684, 2007.