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| Concentrations and isotopic characteristics of atmospheric reactive nitrogen around typical sources in Beijing, China |
| LIU Jieyun1,2,3, ZHANG Ying1, LIU Xuejun1*, TANG Aohan1, QIU Husen3, ZHANG Fusuo1 |
1 Center for Resources, Environment and Food Security, Key Laboratory of Plant-Soil Interactions, Ministry of Education, College of Resources & Environmental Sciences, China Agricultural University, Beijing 100193, China;
2 School of Environment and Surveying Engineering, Suzhou University, Suzhou 234100, China;
3 Changsha Research Station for Agricultural Environment Monitoring & Key Laboratory of Agro-Ecological Processes in Subtropical Region, Institute of Subtropical Agriculture, Chinese Academy of Sciences, Changsha 410125, China |
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Abstract With rapid economic growth in China, anthropogenic reactive nitrogen (Nr) emissions have more than doubled over the last two or three decades. Atmospheric Nr pollution is an environmental concern in China especially in megacities such as Beijing. In order to identify the impact of emission sources on atmospheric Nr pollution, we measured atmospheric Nr concentrations and their isotopic composition (δ15N) dynamics at three typical sites: landfill, pig farm and road traffic sites in Beijing from April 2010 to March 2011. Passive samplers were used for monitoring ammonia (NH3) and nitrogen dioxide (NO2), two major Nr species, while their δ15N values were measured by a diffusion method combined with mass spectrometer approach. The raw water pool of the landfill and fattening house of the pig farm were important NH3 sources with mean NH3 concentrations being 2,829 and 2,369 μg/m3, respectively, while the road traffic site was a minor NH3 source (10.6 μg/m3). NH3 concentrations at sites besides the landfill and roads were high in summer and low in winter due to the annual variation of temperature and the change of emission source intensity. In contrast, the NH3 concentrations inside the pig farm house were high in winter and low in summer, for the barn windows were open in summer and closed in winter. The mean NO2 concentrations were 89.8, 32.9 and 23.0 μg/m3 at the road traffic, the landfill and pig farm sites, respectively. Due to vehicle fuel combustion, NO2 concentration at the road traffic was the highest among the three sources, and the road traffic was a main NO2 emission source. PM10, pNH4+ and pNO3– concentrations in particulate matter were higher in summer than in winter (except PM10 for the pig farm). The δ15NH3 values ranged from –19.14‰ to 7.82‰, with an average of –0.05‰ for the landfill site, and the lowest values were observed in June and July. The δ15NH3 values for the pig farm site ranged from –29.78‰ to –14.05‰ with an average of –24.51‰, and the δ15NH3 values were more negative in summer than in the other seasons. The δ15NO2 values were –9.63‰ to 7.04‰ with an average of –3.72‰ for the road traffic site. The δ15NO2 values were more negative in summer than those in the other seasons. The different δ15N values for the various Nr species in different sources may serve as important indicators for identifying atmospheric Nr sources in megacities. The results may also provide the theoretical basis for research on the atmospheric N deposition and its sources.
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Received: 02 January 2016
Published: 01 December 2016
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| Fund: The work was supported by the National Basic Research Program of China (2014CB954202), the National Natural Science Foundation of China (40425007, 41071151, 31421092) and the Suzhou University Startup Foundation for Doctor (2015jb04). |
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| Ammann M, Siegwolf R, Pichlmayer F, et al. 1999. Estimating the uptake of traffic-derived NO2 from 15N abundance in Norway spruce needles. Oecologia, 118(2): 124–131. Aneja V P, Roelle P A, Murray G C, et al. 2001. Atmospheric nitrogen compounds II: emissions, transport, transformation, deposition and assessment. Atmospheric Environment, 35(11): 1903–1911. Barlaz M A, Milke M W, Ham R K. 1987. Gas production parameters in sanitary landfill simulators. Waste Management & Research, 5(1): 27–39. Blanes-Vidal V, Hansen M N, Pedersen S, et al. 2008. Emissions of ammonia, methane and nitrous oxide from pig houses and slurry: Effects of rooting material, animal activity and ventilation flow. Agriculture, Ecosystems & Environment, 124(3–4): 237–244. Bouwman A F, Van Der Hoek K W. 1997. Scenarios of animal waste production and fertilizer use and associated ammonia emission for the developing countries. Atmospheric Environment, 31(24): 4095–4102. Bragazza L, Limpens J, Gerdol R, et al. 2005. Nitrogen concentration and δ15N signature of ombrotrophic Sphagnum mosses at different N deposition levels in Europe. Global Change Biology, 11(1): 106–114. Brooks P D, Stark J M, McInteer B B, et al. 1989. Diffusion method to prepare soil extracts for automated nitrogen-15 analysis. Soil Science Society of America Journal, 53(6): 1707–1711. Carslaw D C, Carslaw N. 2007. Detecting and characterising small changes in urban nitrogen dioxide concentrations. Atmospheric Environment, 41(22): 4723–4733. Clarisse L, Clerbaux C, Dentener F, et al. 2009. Global ammonia distribution derived from infrared satellite observations. Nature Geoscience, 2(7): 478–483. Dincer F, Odabasi M, Muezzinoglu A. 2006. Chemical characterization of odorous gases at a landfill site by gas chromatography-mass spectrometry. Journal of Chromatography A, 1122(1–2): 222–229. Ding Y, Cai C Y, Hu B, et al. 2012. Characterization and control of odorous gases at a landfill site: A case study in Hangzhou, China. Waste Management, 32(2): 317–326. Elliott E M, Kendall C, Wankel S D, et al. 2007. Nitrogen isotopes as indicators of NOx source contributions to atmospheric nitrate deposition across the Midwestern and Northeastern United States. Environmental Science & Technology, 41(22): 7661–7667. European Topic Centre on Air Pollution and Climate Change Mitigation (ETC). 2011. Report on the European Ambient Air Quality Monitoring and State in 2009. [2011-06-22]. http://acm.eionet.europa.eu/announcements/ann1308731514. Felix J D, Elliott E M, Gish T, et al. 2014. Examining the transport of ammonia emissions across landscapes using nitrogen isotope ratios. Atmospheric Environment, 95: 563–570. Frati L, Caprasecca E, Santoni S, et al. 2006. Effects of NO2 and NH3 from road traffic on epiphytic lichens. Environmental Pollution, 142(1): 58–64. Freyer H D. 1978. Seasonal trends of NH4+ and NO3– nitrogen isotope composition in rain collected at Jülich, Germany. Tellus, 30(1): 83–92. Gruber N, Galloway J N. 2008. An Earth-system perspective of the global nitrogen cycle. Nature, 451(7176): 293–296. Hayes E T, Curran T P, Dodd V A. 2006. Odour and ammonia emissions from intensive pig units in Ireland. Bioresource Technology, 97(7): 940–948. He C E, Liu X J, Fangmeier A, et al. 2007. Quantifying the total airborne nitrogen input into agroecosystems in the North China Plain. Agriculture, Ecosystems & Environment, 121(4): 395–400. He P J, Yang N, Gu H L, et al. 2011. N2O and NH3 emissions from a bioreactor landfill operated under limited aerobic degradation conditions. Journal of Environmental Sciences, 23(6): 1011–1019. Heaton T H E. 1986. Isotopic studies of nitrogen pollution in the hydrosphere and atmosphere: A review. Chemical Geology: Isotope Geoscience Section, 59: 87–102. Heaton T H E. 1987. 15N/14N ratios of nitrate and ammonium in rain at Pretoria, South Africa. Atmospheric Environment (1967), 21(4): 843–852. Heaton T H E. 1990. 15N/14N ratios of NOx from vehicle engines and coal-fired power stations. Tellus B, 42(3): 304–307. Ianniello A, Spataro F, Esposito G, et al. 2010. Occurrence of gas phase ammonia in the area of Beijing (China). Atmospheric Chemistry and Physics, 10(19): 9487–9503. Kang Y N, Liu M X, Song Y, et al. 2016. High-resolution ammonia emissions inventories in China from 1980 to 2012. Atmospheric Chemistry and Physics, 16(4): 2043–2058. Kean A J, Harley R A, Littleton D, et al. 2000. On-road measurement of ammonia and other motor vehicle exhaust emissions. In: Proceedings of the 10th CRC On-road Vehicle Emissions Workshop. San Diego, CA: Hyatt Islandia Hotel, 27–29. Kiga T, Watanabe S, Yoshikawa K, et al. 2000. Evaluation of NOx formation in pulverized coal firing by use of nitrogen isotope ratios. In: ASME 2000 International Joint Power Generation Conference. Miami Beach, FL: American Society of mechanical Engineers, 23–26. Kirchner M, Jakobi G, Feicht E, et al. 2005. Elevated NH3 and NO2 air concentrations and nitrogen deposition rates in the vicinity of a highway in Southern Bavaria. Atmospheric Environment, 39(25): 4531–4542. Lin W, Xu X, Ge B, et al. 2011. Gaseous pollutants in Beijing urban area during the heating period 2007–2008: variability, sources, meteorological, and chemical impacts. Atmospheric Chemistry and Physics, 11(15): 8157–8170. Liu X J, Ju X T, Zhang Y, et al. 2006. Nitrogen deposition in agroecosystems in the Beijing area. Agriculture, Ecosystems & Environment, 113(1–4): 370–377. Liu X J, Duan L, Mo J M, et al. 2011. Nitrogen deposition and its ecological impact in China: An overview. Environmental Pollution, 155(10): 2251–2264. Liu X J, Zhang Y, Han W X, et al. 2013. Enhanced nitrogen deposition over China. Nature, 494(7438): 459–462. Liu X Y, Xiao H Y, Liu C Q, et al. 2008. Stable carbon and nitrogen isotopes of the moss Haplocladium microphyllum in an urban and a background area (SW China): the role of environmental conditions and atmospheric nitrogen deposition. Atmospheric Environment, 42(21): 5413–5423. Marttinen S K, Kettunen R H, Sormunen K M, et al. 2002. Screening of physical-chemical methods for removal of organic material, nitrogen and toxicity from low strength landfill leachates. Chemosphere, 46(6): 851–858. Meng Z Y, Lin W L, Jiang X M, et al. 2011. Characteristics of atmospheric ammonia over Beijing, China. Atmospheric Chemistry and Physics, 11(12): 6139–6151. Moore H. 1977. The isotopic composition of ammonia, nitrogen dioxide and nitrate in the atmosphere. Atmospheric Environment, 11(12): 1239–1243. Pan Y P, Wang Y S, Tang G Q, et al. 2012. Wet and dry deposition of atmospheric nitrogen at ten sites in Northern China. Atmospheric Chemistry and Physics, 12(14): 6515–6535. Perrino C, Catrambone M, Di Menno Di Bucchianico A, et al. 2002. Gaseous ammonia in the urban area of Rome, Italy and its relationship with traffic emissions. Atmospheric Environment, 36(34): 5385–5394. Proemse B C, Mayer B, Fenn M E, et al. 2013. A multi-isotope approach for estimating industrial contributions to atmospheric nitrogen deposition in the Athabasca oil sands region in Alberta, Canada. Environmental Pollution, 182: 80–91. Rebolledo B, Gil A, Pallarés J. 2013. A spatial ammonia emission inventory for pig farming. Atmospheric Environment, 64: 125–131. Reche C, Viana M, Pandolfi M, et al. 2012. Urban NH3 levels and sources in a Mediterranean environment. Atmospheric Environment, 57: 153–164. Shen J L, Tang A H, Liu X J, et al. 2009. High concentrations and dry deposition of reactive nitrogen species at two sites in the North China Plain. Environmental Pollution, 157(11): 3106–3113. Sutton M A, Dragosits U, Tang Y S, et al. 2000. Ammonia emissions from non-agricultural sources in the UK. Atmospheric Environment, 34(6): 855–869. Tang Y S, Cape J N, Sutton M A. 2001. Development and types of passive samplers for monitoring atmospheric NO2 and NH3 concentrations. The Scientific World Journal, 1: 513–529. Van Der Hoek K W. 1998. Estimating ammonia emission factors in Europe: summary of the work of the UNECE ammonia expert panel. Atmospheric Environment, 32(3): 315–316. Vranken E, Claes S, Hendriks J, et al. 2004. Intermittent measurements to determine ammonia emissions from livestock buildings. Biosystems Engineering, 88(3): 351–358. Xiao H Y, Liu C Q. 2002. Sources of nitrogen and sulfur in wet deposition at Guiyang, southwest China. Atmospheric Environment, 36(33): 5121–5130. Xiao H Y, Tang C G, Xiao H W, et al. 2010. Stable sulphur and nitrogen isotopes of the moss Haplocladium microphyllum at urban, rural and forested sites. Atmospheric Environment, 44(34): 4312–4317. Xu W, Zheng K, Liu X J, et al. 2014. Atmospheric NH3 dynamics at a typical pig farm in China and their implications. Atmospheric Pollution Research, 5(3): 455–463. Zhang Y, Liu X J, Fangmeier A, et al. 2008. Nitrogen inputs and isotopes in precipitation in the North China Plain. Atmospheric Environment, 42(7): 1436–1448. |
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