References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-11-6139-2011

Characteristics of atmospheric ammonia over Beijing, China

Meng

Z. Y.

¹ Lin

W. L.

¹ ⁴ Jiang

X. M.

² Yan

¹ ⁴ Wang

¹ Zhang

Y. M.

¹ Jia

X. F.

³ Yu

X. L.

Key Laboratory for Atmospheric Chemistry, Center for Atmospheric Watch and Services, Chinese Academy of Meteorological Sciences, Beijing, China

Tsinghua University, Beijing, China

Department of Environmental Engineering, School of Civil and Environmental Engineering, University of Science and Technology Beijing, Beijing, China

Meteorological Observation Centre, China Meteorological Administration, Beijing, China

29 06 2011

11 12 6139 6151

This is an open-access article ditributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited.

This article is available from http://www.atmos-chem-phys.net/11/6139/2011/acp-11-6139-2011.html

The full text article is available as a PDF file from http://www.atmos-chem-phys.net/11/6139/2011/acp-11-6139-2011.pdf

Continuous measurements of atmospheric ammonia (NH3) were conducted using Ogawa passive samplers from February 2008 to July 2010 at an urban site and from January 2007 to July 2010 at a rural site in Beijing, China. NH4+ in fine particles was also collected at the rural site during 2008–2009. The field comparison between the Ogawa passive samplers and an active analyzer for NH3 conducted at the urban site assures the quality and accuracy of the measurements. The concentrations of NH3 at the urban site ranged from 0.7 to 85.1 ppb, with the annual average of 18.5 ± 13.8 and 23.5 ± 18.0 ppb in 2008 and 2009, respectively. The NH3 concentrations at the rural site were lower than those at urban site, and varied from 0.8 to 42.9 ppb, with the annual average of 4.5 ± 4.6, 6.6 ± 7.0 and 7.1 ± 3.5 ppb in 2007, 2008 and 2009, respectively. The data showed marked seasonal variations at both sites. The results emphasized traffic to be a significant source of NH3 concentrations in winter in urban areas of Beijing. This was illustrated by the strong correlations of NH3 with the traffic related pollutants (NOx and CO) and also by the bimodal diurnal cycle of NH3 concentrations that was synchronized with traffic. Similar patterns were not observed during the summer, suggesting other non-traffic sources became more important. At the rural site, the daily NH4+ concentrations ranged from 0.10 to 36.53 μg m−3, with an average of 7.03 μg m−3 from June 2008 to December 2009. Monthly NH3 were significantly correlated with NH4+ concentrations. Average monthly NH3/NH4+ ratios varied from 0.13 to 2.28, with an average of 0.73. NH4+ in PM2.5 was primarily associated with SO4−2 at the rural site.

References 1

% vor jede Referenz Alebic-Juretic, A.: Airborne ammonia and ammonium within the Northern Adriatic area, Croatia, Environ. Pollut., 154, 439–447, 2008.

Aneja, V. P., Chauhan, J. P., and Walker, J. T.: Characterization of Atmospheric Ammonia Emissions from Swine Waste Storage and Treatment Lagoons, J. Geophys. Res., 105, 11535–11545, 2000.

Asman, W. A., Sutton, M. A., and Schjørring, J. K.: Ammonia: Emission, atmospheric transport and deposition, New Phytol., 139, 27–48, 1998.

Bai, Z., Dong, Y., Wang, Z., and Zhu, T.: Emission of ammonia from indoor concrete wall and assessment of human exposure, Environ. Int., 32, 303–311, 2006.

Bari, A., Ferraro, V., Wilson, L. R., Luttinger, D., and Husain, L.: Measurements of gaseous HONO, HNO3, SO2, HCl, NH3, particulate sulfate and PM$_2.5$ in New York, NY, Atmos. Environ., 37, 2825–2835, 2003.

Biswas, K. F., Ghauri, B. M., and Husain, L.: Gaseous and Aerosol Pollutants During Fog and Clear Episodes in South Asian Urban, Atmos. Environ., 42, 7775–7785, 2008.

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

Brunekreef, B. and Holgate, S. T.: Air pollution and health, Lancet, 360, 1233–1242, 2002.

Cao, J. J., Zhang, T., Chow, J. C., Watson, J. G., Wu, F., and Li, H.: Characterization of Atmospheric Ammonia over Xi'an, China, Aerosol and Air Quality Research, 9, 277–289, 2009.

Carmichael, G. R., Ferm, M., Thongboonchoo, N., Woo, J., Chan, L. Y., Murano, K., Viet, P. H., and Mossberg, C., Bala, R., Boonjawat, J., Upatum, P., Mohan, M., Adhikary, S. P., Shrestha, A. B., Pienaar, J. J., Brunke, E. B., Chen, T., Jie, T., Guoan, D., Peng, L. C., Dhiharto, S., Harjanto, H., Jose, A. M., Kimani, W., Kirouane, A., Lacaux, J. P., Richard, S., Barturen, O., Cerda, J. C., Athayde, A., Tavares, T., Cotrina, J. S., and Bilici, E.: Measurements of sulfur dioxide, ozone and ammonia concentrations in Asia, Africa, and South America using passive samplers, Atmos. Environ., 37, 1293–1308, 2003.

Clarisse, L., Clerbaux, C., Dentener, F., Hurtmans, D., and Coheur, P. F.: Global ammonia distribution derived from infrared satellite observations, Nature Geosci., 2, 478–483, http://dx.doi.org/10.1038/NGEO551doi:10.1038/NGEO551, 2009.

Chou, M. S. and Wang, C. H.: Treatment of Ammonia in Air Stream by Biotrickling Filter, Aerosol Air Qual. Res., 7, 17–32, 2007.

Dentener, F. J. and Crutzen, P. J.: A three-dimensional model of the global ammonia cycle, J. Atmos. Chem., 19, 331–369, 1994.

Ellis, R. A., Murphy, J. G., Pattey, E., van Haarlem, R., O'Brien, J. M., and Herndon, S. C.: Characterizing a Quantum Cascade Tunable Infrared Laser Differential Absorption Spectrometer (QC-TILDAS) for measurements of atmospheric ammonia, Atmos. Meas. Tech., 3, 397–406, http://dx.doi.org/10.5194/amt-3-397-2010doi:10.5194/amt-3-397-2010, 2010.

Ellis, R. A., Murphy, J. G., Markovic, M. Z., VandenBoer, T. C., Makar, P. A., Brook, J., and Mihele, C.: The influence of gas-particle partitioning and surface-atmosphere exchange on ammonia during BAQS-Met, Atmos. Chem. Phys., 11, 133–145, http://dx.doi.org/10.5194/acp-11-133-2011doi:10.5194/acp-11-133-2011, 2011.

Galloway, J. N., Zhao, D. W., Xiong, J., and Likens, G. E.: Acid Rain: China, US and a Remote Area, Science, 230, 1559–1562, 1987.

Galloway, J. N., Aber, J. D., Erisman, J. W., Seitzinger, S. P., Howarth, R. W., Cowling, E. B., and Cosby, B. J.: The nitrogen cascade, BioScience, 53, 341–353, 2003.

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.

Hao, J., Wang, L., Li, L., Hu, J. N., and Yu, X. C.: Air pollutants contribution and control strategies of energy-use related sources in Beijing, Sci. China Ser. D, 48, (Suppl. II), 138–146, 2005.

Heeb, N. V., Saxer, C. J., Forss, A.-M., and Brühlmann, S.: Trends of NO-, NO$_2^-$, and NH3-emissions from gasoline-fueled Euro-3- to Euro-4-passenger cars, Atmos. Environ., 42, 2543–2554, 2008.

Horvath, H.: Effects on visibility, weather and climate, in: Atmospheric acidity: sources, consequences and abatement, edited by: Radojevic, M. and Harrison, R. M., chapter 13, London: Elsevier Applied Science, 1992.

Huai, T., Durbin, T. D., Younglove, T., Scora, G., and Norbeck, J. M.: Vehicle specific power approach to estimating on-road NH3 emissions from light duty vehicles, Environ. Sci. Technol., 39, 9595–9600, 2005.

Ianniello, A., Spataro, F., Esposito, G., Allegrini, I., Rantica, E., Ancora, M. P., Hu, M., and Zhu, T.: Occurrence of gas phase ammonia in the area of Beijing (China), Atmos. Chem. Phys., 10, 9487–9503, http://dx.doi.org/10.5194/acp-10-9487-2010doi:10.5194/acp-10-9487-2010, 2010.

Ju, X., Liu, X., Zhang, F., and Roelche, M.: Nitrogen fertilization, soil nitrate accumulation, and policy recommendations in several agricultural regions of China, Ambio, 33, 300–305, 2004.

Kean, A. J., Harley, R. A., Littlejohn, D., and Kendall, G. R.: On road measurement of ammonia and other motor vehicle exhaust emissions, Environ. Sci. Technol., 34, 3535–3539, 2000.

Khemani, L. T., Momin, G. A., Naik, M. S., Rao, P. S. P., Safai, P. D., and Murty, A. S. R.: Influence of Alkaline Particulates on pH of Cloud and Rain Water in India, Atmos. Environ., 21, 1137–1145, 1987.

Klimont, Z.: Current and Future emissions of Ammonia in China, 10th International Emission Inventory Conference: One Atmosphere, One Inventory, Many Challenges, US EPA, 1–3 May, Denver, USA, available at: http://www.epa.gov/ttn/chief/conference/ei10/ammonia/klimont.pdf, 2001.

Kobara, H., Takeuchi, K., and Ibusuki, T.: Effect of Relative Humidity on Aerosol Generation through Experiments at Low Concentrations of Gaseous Nitric Acid and Ammonia, Aerosol Air Qual. Res., 7, 193–204, 2007.

Kulshrestha, U. C., Sarkar, A. K., Srivastava, S. S., and Parashar, D. C.: Investigation into Atmospheric Deposition through Precipitation Studies at New Delhi (India), Atmos. Environ., 30, 4149–4154, 1996.

Lenhard, V. and Gravenhorst, G.: Evaluation of Ammonia of Fluxes into the Free Atmosphere over Western Germany, Tellus, 328, 48–55, 1980.

Likens, G. E., Keene, W. C., Miller, J. M., and Galloway, J. N.: Chemistry of Precipitation from a Remote, Terrestrial Site in Australia, J. Geophys. Res., 92, 13299–13314, 1987.

Lin, W., Xu, X., Zhang, X., and Tang, J.: Contributions of pollutants from North China Plain to surface ozone at the Shangdianzi GAW Station, Atmos. Chem. Phys., 8, 5889–5898, http://dx.doi.org/10.5194/acp-8-5889-2008doi:10.5194/acp-8-5889-2008, 2008.

Lin, W., Xu, X., Ge, B., and Liu, X.: Gaseous pollutants in Beijing urban area during the heating period 2007–2008: variability, sources, meteorological and chemical impacts, Atmos. Chem. Phys. Discuss., 11, 6919–6956, http://dx.doi.org/10.5194/acpd-11-6919-2011doi:10.5194/acpd-11-6919-2011, 2011.

Matthews, E.: Nitrogenous fertilizers: Global distribution of consumption and associated emissions of nitrous oxide and ammonia, Glob. Biogeochem., 8, 411–439, 1994.

Meng, Z. Y., Jiang, X. M., Yan, P., Lin, W. L., Zhang, H. D., and Wang, Y.: Characteristics and sources of PM$_2.5$ and carbonaceous species during winter in Taiyuan, China, Atmos. Environ., 41, 6901–6908, 2007.

Meng, Z. Y., Xu, X. B., Yan, P., Ding, G. A., Tang, J., Lin, W. L., Xu, X. D., and Wang, S. F.: Characteristics of trace gaseous pollutants at a regional background station in Northern China, Atmos. Chem. Phys., 9, 927–936, http://dx.doi.org/10.5194/acp-9-927-2009doi:10.5194/acp-9-927-2009, 2009.

Meng, Z. Y., Xu, X. B., Wang, T., Zhang, X. Y., Yu, X. L., Wang, S. F., Lin, W. L., Chen, Y. Z., Jiang, Y. A., and An, X. Q.: Ambient sulfur dioxide, nitrogen dioxide, and ammonia at ten background and rural sites in China during 2007–2008, Atmos. Environ., 44, 2625–2631, 2010.

Nemitz, E., Milford, C., and Sutton, M. A.: A Two-Layer Canopy Compensation Point Model for Describing Bi-directional Biosphere–Atmosphere Exchange of Ammonia, Q. J. Roy. Meteorol. Soc., 127, 815–833, 2001.

Perrino, C., Catrambone, M., Di Menno Di Bucchianico, A., and Allegrini, I.: Gaseous ammonia in the urban area of Rome, Italy, and its relationship with traffic emissions, Atmos. Environ., 36, 5385–5394, 2002.

Possanzini, M., Buttini, P., and Dipalo, V.: Characterization of a Rural Area in Terms of Dry and Wet Deposition, Sci. Total. Environ., 74, 111–120, 1988.

Robarge, W. P., Walker, J. T., McCulloch, R. B., and Murray, G.: Atmospheric concentrations of ammonia and ammonium at an agricultural site in the southeast United States, Atmos. Environ., 36, 1661–1674, 2002.

Saylor, R. D., Edgerton, E. S., Hartsell, B. E., Baumann, K., and Hansen, D. A.: Continuous gaseous and total ammonia measurements from the southeastern aerosol research and characterization (SEARCH) study, Atmos. Environ., 44, 4994–5004, 2010.

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.-Atmos., 108(D21), 8809, http://dx.doi.org/10.1029/2002JD003093doi:10.1029/2002JD003093, 2003.

Suh, H. H,. Allen, G. A., Koutrakis, P., and Burton, R. M.: Spatial variation in acidic sulphate and ammonia concentrations within metropolitan Philadelphia, J. Air Waste Manage. Assoc., 45, 442–452, 1995.

Sutton, M. A., Asman, W. A. H., and Schjørring, J. K.: Dry deposition of reduced nitrogen, Tellus, 46B, 255–273, 1994.

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

Tanner, P.: Vehicle-related ammonia emissions in Hong Kong, Environ. Chem. Lett., 7, 37–40, 2009.

Tuncel, S. G. and Ungor, S.: Rain Water Chemistry in Ankara, Turkey, Atmos. Environ., 30, 2721–2727, 1996.

Walker, J. T., Whitall, D., Robarge, W. P., and Paerl, H.: Ambient ammonia and ammonium aerosol across a region of variable ammonia emission density, Atmos. Environ., 38, 1235–1246, 2004.

Wang, B., Shao, M., Lu, S. H., Yuan, B., Zhao, Y., Wang, M., Zhang, S. Q., and Wu, D.: Variation of ambient non-methane hydrocarbons in Beijing city in summer 2008, Atmos. Chem. Phys., 10, 5911–5923, http://dx.doi.org/10.5194/acp-10-5911-2010doi:10.5194/acp-10-5911-2010, 2010.

Whitehead, J. D., Longley, I. D., and Gallagher, M. W.: Seasonal and diurnal variation in atmospheric ammonia in an urban environment measured using a quantum cascade laser absorption spectrometer, Water Air Soil Poll., 183, 317–329, 2007.

Wu, Z. J., Hu, M., Shao, K. S., and Slanina, J.: Acidic gases, NH3 and secondary inorganic ions in PM$_10$ during summertime in Beijing, China and their relation to air mass history, Chemoshere, 76, 1028–1035, 2009.

Yao, X. H., Lau, A. P. S., Fang, M., Chan, C. K., and Hu, M.: Size distributions and formation of ionic species in atmospheric particulate pollutants in Beijing, China: 1-inorganic ions, Atmos. Environ., 37, 2991–3000, 2003.

Yao, X. H., Ling, T. Y., Fang, M., and Chan, C. K.: Comparison of Thermodynamic Predictions for in Situ pH in PM$_2.5$, Atmos. Environ., 40, 2835–2844, 2006.

Zhang, Y., Dore, A. J., Ma, L., Liu, X. J., Ma, W. Q., Cape, J. N., and Zhang, F. S.: Agricultural ammonia emissions inventory and spatial distribution in the North China Plain, Environ. Pollut., 158, 490–501, 2010.