Tracking the source and contribution of NO3- in precipitation in Nanchang in autumn and winter by dual isotope
AI Wen-qiang1,2, XIAO Hong-wei1,2, SUN Qi-bin3, ZHANG Yong-yun3, ZHANG Zei-yu2, LI Jing-wen2
1. Jiangxi Province Key Laboratory of the Causes and Control of Atmospheric Pollution, Nanchang 330013, China; 2. School of Water Resources and Environmental Engineering, East China University of Technology, Nanchang 330013, China; 3. School of Atmospheric Sciences, Sun Yat-sen University, Zhuhai 519082, China
Abstract：Rainwater was collected from September 1, 2016 to February 28, 2017 in Nanchang, as well as stable isotope of nitrate (δ15N) and chemical compositions of rainwater were analyzed. The results showed that the concentration of NO3- ranged from 7.3 to 99.5μmol/L, and the mean is 36.1μmol/L; the δ15N of NO3- ranged from -6.0‰ to +8.3‰, and the mean is -0.8‰. Combined with chemical composition and isotope analysis, it is shown that NO3- was mainly affected by the region and mainly comes from biomass burning, traffic, coal combustion while biological soil is the secondary source in the sampling period. Bayesian mixing model (MixSIA) which took account of the isotope fractionation wes used to make precise estimations of the contribution of different sources. The results showed that the contribution of biomass burning emissions, traffic and coal combustion was more than 86%. However, in this case, the contribution of biomass burning emissions and traffic was more than 63%, and the coal combustion was only 23.1%, which indicated that a necessity to control NOx from traffic and biomass burning strictly to reduce air pollution.
艾文强, 肖红伟, 孙启斌, 张永运, 张泽雨, 李静雯. 氮氧同位素示踪南昌秋冬季降水中NO3-来源及其贡献[J]. 中国环境科学, 2021, 41(9): 4043-4050.
AI Wen-qiang, XIAO Hong-wei, SUN Qi-bin, ZHANG Yong-yun, ZHANG Zei-yu, LI Jing-wen. Tracking the source and contribution of NO3- in precipitation in Nanchang in autumn and winter by dual isotope. CHINA ENVIRONMENTAL SCIENCECE, 2021, 41(9): 4043-4050.
Fang Y T, Koba K, Wang X M, et al. Anthropogenic imprints on nitrogen and oxygen isotopic composition of precipitation nitrate in a nitrogen-polluted city in southern China[J]. Atmos. Chem. Phys., 2011,11(3):1313-1325.
Chen F, Lao Q, Jia G, et al. Seasonal variations of nitrate dual isotopes in wet deposition in a tropical city in China[J]. Atmospheric Environment, 2019,196:1-9.
Jin Z, Wang Y, Qian L, et al. Combining chemical components with stable isotopes to determine nitrate sources of precipitation in Hangzhou and Huzhou, SE China[J]. Atmospheric Pollution Research, 2019,10(2):386-394.
Zhao Z-Y, Cao F, Fan M-Y, et al. Coal and biomass burning as major emissions of NOx in Northeast China:Implication from dual isotopes analysis of fine nitrate aerosols[J]. Atmospheric Environment, 2020.
Zong Z, Tan Y, Wang X, et al. Dual-modelling-based source apportionment of NOx in five Chinese megacities:Providing the isotopic footprint from 2013 to 2014[J]. Environ Int, 2020,137:105592.
Zhang W, Zhang Y. Oxygen isotope anomaly (Δ < sup> 17</sup> O) in atmospheric nitrate:A review[J]. Chinese Science Bulletin, 2019,64(7):649-662.
Walters W W, Simonini D S, Michalski G. Nitrogen isotope exchange between NO and NO2 and its implications for δ15N variations in tropospheric NOx and atmospheric nitrate[J]. 2016,43(1):440-448.
Zong Z, Wang X, Tian C, et al. First Assessment of NOx Sources at a regional background site in North China using isotopic analysis linked with modeling[J]. Environmental Science & Technology, 2017,51(11):5923-5931.
Li Z, Walters W W, Hastings M G, et al. Nitrate isotopic composition in precipitation at a Chinese megacity:Seasonal variations, atmospheric processes, and implications for sources[J]. Earth and Space Science, 2019,6(11):2200-2213.
Itahashi S, Yumimoto K, Uno I, et al. A 15-year record (2001~2015) of the ratio of nitrate to non-sea-salt sulfate in precipitation over East Asia[J]. Atmospheric Chemistry and Physics, 2018,18(4):2835-2852.
中华人民共和国生态环境部.中国生态环境状况公报[M]. 2013:23-24.Ministry of Ecology and Environment of the People's Repulic of China. Report on the State of the Ecology and Environment in China[M]. 2013:23-24.
中华人民共和国生态环境部.中国生态环境状况公报[R]. 2014:27-28.Ministry of Ecology and Environment of the People's Repulic of China. Report on the state of the ecology and environment in China[R]. 2014:27-28.
中华人民共和国生态环境部.中国生态环境状况公报[R]. 2015:14-15.Ministry of Ecology and Environment of the People's Repulic of China. Report on the state of the ecology and environment in China[M]. 2015:14-15.
中华人民共和国生态环境部.中国生态环境状况公报[R]. 2016:15-16.Ministry of Ecology and Environment of the People's Repulic of China. Report on the state of the ecology and environment in China[R]. 2016:15-16.
中华人民共和国生态环境部.中国生态环境状况公报[R]. 2017:15-16.Ministry of Ecology and Environment of the People's Repulic of China. Report on the state of the ecology and environment in China[R]. 2017:15-16.
Wang Y, Gao W, Wang S, et al. Contrasting trends of PM2.5 and surface-ozone concentrations in China from 2013 to 2017[J]. National Science Review, 2020.
Felix J D, Elliott E M, Avery G B, et al. Isotopic composition of nitrate in sequential Hurricane Irene precipitation samples:Implications for changing NOx sources[J]. Atmospheric Environment, 2015,106:191-195.
Felix J D, Elliott E M, Shaw S L. Nitrogen isotopic composition of coal-fired power plant NOx:influence of emission controls and implications for global emission inventories[J]. Environ. Sci. Technol., 2012,46(6):3528-35.
Walters W W, Tharp B D, Fang H, et al. Nitrogen isotope composition of thermally produced NOx from various fossil-fuel combustion sources[J]. Environ. Sci. Technol., 2015,49(19):11363-71.
Felix J D, Elliott E M. Isotopic composition of passively collected nitrogen dioxide emissions:Vehicle, soil and livestock source signatures[J]. Atmospheric Environment, 2014,92:359-366.
Heaton T H, Spiro B, Robertson S M. Potential canopy influences on the isotopic composition of nitrogen and sulphur in atmospheric deposition[J]. Oecologia, 1997,109(4):600-607.
Walters W W, Goodwin S R, Michalski G. Nitrogen stable isotope composition (δ15N) of vehicle-emitted NOx[J]. Environmental Science & Technology, 2015,49(4):2278-2285.
Felix J D, Elliott E M. The agricultural history of human-nitrogen interactions as recorded in ice core δ15N-NO3-[J]. Geophysical Research Letters, 2013,40(8):1642-1646.
Fibiger D L, Hastings M G. First Measurements of the nitrogen isotopic composition of NOx from biomass burning[J]. Environ Sci Technol, 2016,50(21):11569-11574.
Hastings M G, Jarvis J C, Steig E J. Anthropogenic impacts on nitrogen isotopes of ice-core nitrate[J]. Science, 2009,324(5932):1288.
Li D, Wang X. Nitrogen isotopic signature of soil-released nitric oxide (NO) after fertilizer application[J]. Atmospheric Environment, 2008, 42(19):4747-4754.
Liu X-Y, Yin Y-M, Song W. Nitrogen isotope differences between major atmospheric NOy species:Implications for transformation and deposition processes[J]. Environmental Science & Technology Letters, 2020,7(4):227-233.
Xiao H W, Zhu R G, Pan Y Y, et al. Differentiation between nitrate aerosol formation pathways in a Southeast Chinese city by dual isotope and modeling studies[J]. Journal of Geophysical Research:Atmospheres, 2020,125(13).
Liu X Y, Xiao H W, Xiao H Y, et al. Stable isotope analyses of precipitation nitrogen sources in Guiyang, southwestern China[J]. Environ Pollut, 2017,230:486-494.
Luo L, Kao S J, Bao H, et al. Sources of reactive nitrogen in marine aerosol over the Northwest Pacific Ocean in spring[J]. Atmos. Chem. Phys., 2018,18(9):6207-6222.
Altieri K E, Hastings M G, Gobel A R, et al. Isotopic composition of rainwater nitrate at Bermuda:The influence of air mass source and chemistry in the marine boundary layer[J]. Journal of Geophysical Research:Atmospheres, 2013,118(19):11,304-11,316.
Hastings M G, Sigman D M, Lipschultz F. Isotopic evidence for source changes of nitrate in rain at Bermuda[J]. Journal of Geophysical Research:Atmospheres, 2003,108(D24):n/a-n/a.
Buffam I, Mcglathery K. Effect of ultraviolet light on dissolved nitrogen transformations in coastal lagoon water[J]. Limnology and Oceanography, 2003,48:723-734.
Gobel A R, Altieri K E, Peters A J, et al. Insights into anthropogenic nitrogen deposition to the North Atlantic investigated using the isotopic composition of aerosol and rainwater nitrate[J]. Geophysical Research Letters, 2013,40(22):5977-5982.
Luo L, Wu Y, Xiao H, et al. Origins of aerosol nitrate in Beijing during late winter through spring[J]. Science of The Total Environment, 2019, 653:776-782.
Parnell A C, Phillips D L, Bearhop S, et al. Bayesian stable isotope mixing models[J]. Environmetrics, 2013:n/a-n/a.
Walters W W, Michalski G. Theoretical calculation of nitrogen isotope equilibrium exchange fractionation factors for various NOy molecules[J]. Geochimica et Cosmochimica Acta, 2015,164:284-297.
Walters W W, Michalski G. Theoretical calculation of oxygen equilibrium isotope fractionation factors involving various NOy molecules, OH, and H2O and its implications for isotope variations in atmospheric nitrate[J]. Geochimica et Cosmochimica Acta, 2016,191:89-101.
肖红伟,肖化云,龙爱民,等.贵阳地区大气降水中δ15N-NO3组成及来源分析[J]. 环境科学学报, 2012,32(4):940-945.Xiao H W, Xiao H Y, Long A M, et al. Nitrogen isotopic composition and source of nitrate in precipitation at Guiyang[J]. Acta Scientiae Circumstantiae, 2012,32(4):940-945.
Jia G, Chen F. Monthly variations in nitrogen isotopes of ammonium and nitrate in wet deposition at Guangzhou, south China[J]. Atmospheric Environment, 2010,44(19):2309-2315.
Zhao X, Yan X, Xiong Z, et al. Spatial and temporal variation of inorganic nitrogen wet deposition to the Yangtze River Delta Region, China[J]. Water, Air, and Soil Pollution, 2009,203(1-4):277-289.
肖致美,李鹏,陈魁,等.天津市大气降水化学组成特征及来源分析[J]. 环境科学研究, 2015,28(7):1025-1030.Xiao Z M, Li P, Chen K, et al. Characteristics and sources of chemical composition of atmospheric precipitation in Tianjin[J]. Research of Environmental Sciences, 2015,28(7):1025-1030.
Xu Z, Han G. Chemical and strontium isotope characterization of rainwater in Beijing, China[J]. Atmospheric Environment, 2009, 43(12):1954-1961.
肖红伟,肖化云,张忠义,等.西沙永兴岛大气降水化学特征及来源分析[J]. 2016,36(11):3237-3244.Xiao H W, Xiao H Y, Zhang Z Y, et al. Chemical characteristics and source apportionment of atmospheric precipitation in Yongxing Island[J]. China Environmental Science, 2016,36(11):3237-3244.
Zhang D D, Peart M, Jim C Y, et al. Precipitation chemistry of Lhasa and other remote towns, Tibet[J]. Atmospheric Environment, 2003, 37(2):231-240.
Chen W, Yan L, Zhao H. Seasonal Variations of Atmospheric Pollution and Air Quality in Beijing[J]. Atmosphere, 2015,6(11):1753-1770.
Xing M, Liu W. Variations in the concentration and isotopic composition of nitrate nitrogen in wet deposition and their relation with meteorological conditions in Xi'an city, Northwest China[J]. Applied Geochemistry, 2012,27(4):831-840.
Li C, Li S L, Yue F J, et al. Nitrate sources and formation of rainwater constrained by dual isotopes in Southeast Asia:Example from Singapore[J]. Chemosphere, 2020,241:125024.
Zhang Y, Liu X J, Fangmeier A, et al. Nitrogen inputs and isotopes in precipitation in the North China Plain[J]. Atmospheric Environment, 2008,42(7):1436-1448.
Xiao H-W, Wu J-F, Luo L, et al. Enhanced biomass burning as a source of aerosol ammonium over cities in central China in autumn[J]. Environmental Pollution, 2020,266:115278.
江西省生态环境厅.江西省环境统计年报[M]. 2016:21-32.Department of Ecology and Environment of JiangXi Province. Environmental statistics annual report of JiangXi Province[M]. 2016:21-32.
江西省统计局.江西统计年鉴[M]. 中国统计出版社, 2017.Jiangxi Provincial Bureau of Statistics. Jiangxi statistical yearbook[M]. 2017
江西省统计局.江西统计年鉴[M]. 中国统计出版社, 2018.Jiangxi Provincial Bureau of Statistics. Jiangxi statistical yearbook[M]. 2018.
Chang Y, Zhang Y, Tian C, et al. Nitrogen isotope fractionation during gas-to-particle conversion of NOx to NO3- in the atmosphere-implications for isotope-based NOx source apportionment[J]. Atmospheric Chemistry and Physics, 2018,18(16):11647-11661.
Shen J, Zhao Q, Cheng Z, et al. Insights into source origins and formation mechanisms of nitrate during winter haze episodes in the Yangtze River Delta[J]. Sci. Total Environ., 2020,741:140187.