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Nitrogen isotope fractionation during gas-to-particle conversion of NOx to NO3- in the atmosphere - implications for isotope-based NOx source apportionment

文献类型：期刊论文

作者Chang, Yunhua; Zhang, Yanlin; Tian, Chongguo; Zhang, Shichun; Ma, Xiaoyan; Cao, Fang; Liu, Xiaoyan; Zhang, Wenqi; Kuhn, Thomas; Lehmann, Moritz F.
刊名ATMOSPHERIC CHEMISTRY AND PHYSICS
出版日期2018-08-16
卷号18期号:16页码:11647-11661
ISSN号1680-7316
关键词PM2.5 CARBONACEOUS AEROSOLS YANGTZE-RIVER DELTA EMISSION INVENTORY HETEROGENEOUS OXIDATION THEORETICAL CALCULATION SATELLITE-OBSERVATIONS RAINWATER NITRATE TROPOSPHERIC NOX AMMONIUM-SULFATE 1ST MEASUREMENTS
DOI10.5194/acp-18-11647-2018
产权排序[Chang, Yunhua ; Zhang, Yanlin ; Cao, Fang ; Liu, Xiaoyan ; Zhang, Wenqi] Nanjing Univ Informat Sci & Technol, Yale NUIST Ctr Atmospher Environm, Int Joint Lab Climate & Environm Change ILCEC, Nanjing 210044, Jiangsu, Peoples R China ; [Chang, Yunhua ; Zhang, Yanlin ; Cao, Fang ; Liu, Xiaoyan ; Zhang, Wenqi] Nanjing Univ Informat Sci & Technol, Key Lab Meteorol Disaster, Minist Educ KLME, CIC FEMD, Nanjing 210044, Jiangsu, Peoples R China ; [Chang, Yunhua ; Zhang, Yanlin ; Cao, Fang ; Liu, Xiaoyan ; Zhang, Wenqi] Nanjing Univ Informat Sci & Technol, Coll Appl Meteorol, Jiangsu Prov Key Lab Agr Meteorol, Nanjing 210044, Jiangsu, Peoples R China ; [Tian, Chongguo] Chinese Acad Sci, Yantai Inst Coastal Zone Res, Key Lab Coastal Environm Proc & Ecol Remediat, Yantai 264003, Peoples R China ; [Zhang, Shichun] Chinese Acad Sci, Northeast Inst Geog & Agroecol, 4888 Shengbei Rd, Changchun 130102, Jilin, Peoples R China ; [Ma, Xiaoyan] Nanjing Univ Informat Sci & Technol, Earth Syst Modeling Ctr, Key Lab Aerosol Cloud Precipitat, China Meteorol Adm, Nanjing 10044, Jiangsu, Peoples R China ; [Kuhn, Thomas ; Lehmann, Moritz F.] Univ Basel, Dept Environm Sci, Aquat & Isotope Biogeochem, CH-4056 Basel, Switzerland
文献子类Article
英文摘要Atmospheric fine-particle (PM2.5) pollution is frequently associated with the formation of particulate nitrate (pNO(3)(-)), the end product of the oxidation of NOx gases (NO+NO2) in the upper troposphere. The application of stable nitrogen (N) (and oxygen) isotope analyses of pNO(3)(-) to constrain NOx source partitioning in the atmosphere requires knowledge of the isotope fractionation during the reactions leading to nitrate formation. Here we determined the delta N-15 values of fresh pNO(3)(-) (delta N-15-pNO(3)(-)) in PM2.5 at a rural site in northern China, where atmospheric pNO(3)(-) can be attributed exclusively to biomass burning. The observed delta N-15-pNO(3)(-) (12.17 +/- 1.55 parts per thousand; n = 8) was much higher than the N isotopic source signature of NOx from biomass burning (1.04 +/- 4.13 parts per thousand). The large difference between delta N-15-pNO(3)(-) and delta N-15-NOx (Delta(delta N-15)) can be reconciled by the net N isotope effect (epsilon(N)) associated with the gasparticle conversion from NOx to NO3-. For the biomass burning site, a mean epsilon(N)(approximate to Delta(delta N-15)) of 10.99 +/- 0.74 parts per thousand was assessed through a newly developed computational quantum chemistry (CQC) module. epsilon(N) depends on the relative importance of the two dominant N isotope exchange reactions involved (NO2 reaction with OH versus hydrolysis of dinitrogen pentoxide (N2O5) with H2O) and varies between regions and on a diurnal basis. A second, slightly higher CQC-based mean value for epsilon(N) (15.33 +/- 4.90 parts per thousand) was estimated for an urban site with intense traffic in eastern China and integrated in a Bayesian isotope mixing model to make isotope-based source apportionment estimates for NOx at this site. Based on the delta N-15 values (10.93 +/- 3.32 parts per thousand; n = 43) of ambient pNO(3)(-) determined for the urban site, and considering the location-specific estimate for epsilon(N), our results reveal that the relative contribution of coal combustion and road traffic to urban NOx is 32%+/- 11% and 68%+/- 11%, respectively. This finding agrees well with a regional bottom-up emission inventory of NOx. Moreover, the variation pattern of OH contribution to ambient pNO(3)(-) formation calculated by the CQC module is consistent with that simulated by the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem), further confirming the robustness of our estimates. Our investigations also show that, without the consideration of the N isotope effect during pNO(3)(-) formation, the observed delta(NpNO3-)-Np-15 at the study site would erroneously imply that NOx is derived almost entirely from coal combustion. Similarly, reanalysis of reported delta(NNO3-)-N-15 data throughout China and its neighboring areas suggests that NOx emissions from coal combustion may be substantively overestimated (by > 30%) when the N isotope fractionation during atmospheric pNO(3)(-) formation is neglected.
WOS关键词PM2.5 CARBONACEOUS AEROSOLS ; YANGTZE-RIVER DELTA ; EMISSION INVENTORY ; HETEROGENEOUS OXIDATION ; THEORETICAL CALCULATION ; SATELLITE-OBSERVATIONS ; RAINWATER NITRATE ; TROPOSPHERIC NOX ; AMMONIUM-SULFATE ; 1ST MEASUREMENTS
WOS研究方向Meteorology & Atmospheric Sciences
语种英语
WOS记录号WOS:000441783700005
资助机构National Key Research and Development Program of China [2017YFC0210101] ; National Natural Science Foundation of China [91644103, 41705100, 41575129] ; Provincial Natural Science Foundation of Jiangsu [BK20170946] ; University Science Research Project of Jiangsu Province [17KJB170011] ; International Joint Laboratory on Climate and Environment Change (ILCEC) ; Collaborative Innovation Center on Forecast and Evaluation of Meteorological Disasters (CIC-FEMD) through NUIST ; Collaborative Innovation Center on Forecast and Evaluation of Meteorological Disasters (CIC-FEMD) through University of Basel research funds
源URL[http://ir.yic.ac.cn/handle/133337/24511]  
专题烟台海岸带研究所_近岸生态与环境实验室
烟台海岸带研究所_中科院海岸带环境过程与生态修复重点实验室
作者单位1.Nanjing Univ Informat Sci & Technol, Yale NUIST Ctr Atmospher Environm, Int Joint Lab Climate & Environm Change ILCEC, Nanjing 210044, Jiangsu, Peoples R China;
2.Nanjing Univ Informat Sci & Technol, Key Lab Meteorol Disaster, Minist Educ KLME, CIC FEMD, Nanjing 210044, Jiangsu, Peoples R China;
3.Nanjing Univ Informat Sci & Technol, Coll Appl Meteorol, Jiangsu Prov Key Lab Agr Meteorol, Nanjing 210044, Jiangsu, Peoples R China;
4.Chinese Acad Sci, Yantai Inst Coastal Zone Res, Key Lab Coastal Environm Proc & Ecol Remediat, Yantai 264003, Peoples R China;
5.Univ Basel, Dept Environm Sci, Aquat & Isotope Biogeochem, CH-4056 Basel, Switzerland
6.Chinese Acad Sci, Northeast Inst Geog & Agroecol, 4888 Shengbei Rd, Changchun 130102, Jilin, Peoples R China;
7.Nanjing Univ Informat Sci & Technol, Earth Syst Modeling Ctr, Key Lab Aerosol Cloud Precipitat, China Meteorol Adm, Nanjing 10044, Jiangsu, Peoples R China;
推荐引用方式
GB/T 7714		 Chang, Yunhua,Zhang, Yanlin,Tian, Chongguo,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.
APA Chang, Yunhua.,Zhang, Yanlin.,Tian, Chongguo.,Zhang, Shichun.,Ma, Xiaoyan.,...&Lehmann, Moritz F..(2018).Nitrogen isotope fractionation during gas-to-particle conversion of NOx to NO3- in the atmosphere - implications for isotope-based NOx source apportionment.ATMOSPHERIC CHEMISTRY AND PHYSICS,18(16),11647-11661.
MLA Chang, Yunhua,et al."Nitrogen isotope fractionation during gas-to-particle conversion of NOx to NO3- in the atmosphere - implications for isotope-based NOx source apportionment".ATMOSPHERIC CHEMISTRY AND PHYSICS 18.16(2018):11647-11661.

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来源：烟台海岸带研究所

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