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Multi-scale evolutions of atmospheric NR-PM1 characteristics and its influencing mechanisms |
TIAN Jian, HAN Li-hui, LAN Tong, QI Chao-nan, XIAO Qian, WANG Hai-yan |
Key Laboratory of Beijing on Regional Air Pollution Control, College of Environmental Sciences and Technology, Beijing University of Technology, Beijing 100124, China |
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Abstract An Aerodyne Aerosol Chemical Speciation Monitor (ACSM) was deployed to in situ measure the concentrations ofnon-refractory submicron particulate NR-PM1 and its species as organics Org, sulfate SO42-, nitrate NO3-, ammonium NH4+ andchloride Cl- at the southeast urban area in Beijing from December 2021 to November 2022, and further investigate the changecharacteristics of NR-PM1 and its species at different time scales, especially during the different pollution periods, and the importantfactors affecting the formation of secondary sulfate and nitrate. Meanwhile, the positive matrix factorization PMF and backwardtrajectory clustering analysis were used to study the change characteristics of organic aerosol OA components in the different periods,and the influence mechanism of air mass long-distance transport on NR-PM1 and its species in the different periods, respectively. Theresults showed that the annual average mass concentration of NR-PM1 during the study period was (7.60±10.35) μg/m3, being lowerthan the corresponding annual average since 2016, and showed a decline trend year by year. The average concentrations of NR-PM1 in different seasons showed an obvious seasonal variation characterized by autumn > spring > winter > summer, and the diurnalvariations in different seasons followed the order of night > day. The average annual mass concentration of NR-PM1 species showedan order of Org> NO3-> NH4+~ SO42-> Cl-, among which Org contributed the largest fraction of NR-PM1 with about 41.16%,followed by nitrate 33.05%, ammonium 12.47%, sulfate 11.99%, and chloride contributing the lowest fraction with 1.33%. Thediurnal variations of NR-PM1 concentrations in different seasons were all smaller, and the average concentrations of NR-PM1 and itsspecies in haze days were higher than those in ozone pollution days and clean days. The presence of alkaline NH3 in the atmosphereand the meteorological conditions during the haze days were more favorable for the secondary transformation of gaseous precursors.The OA components were different in different seasons. SOA in winter, spring and autumn is the main component of OA,while POA in summer is the main component of OA. OA in haze and ozone-polluted days was mainly affected by secondary organicmatter. The transport pathways of air mass were different in different seasons. It is noted that the haze pollution days were mainlyaffected by the short-distance transports of air mass from the southeast direction and the south direction, and NO3- showed a greatercontribution to NR-PM1. O3-polluted days were mainly affected by short-distance transports of air mass from the south direction,while clean days were mainly affected by long-distance transports of air mass from the northwest direction.
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Received: 29 February 2024
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[1] Zheng G J, Duan F K, Su H, et al. Exploring the severe winter haze in Beijing: the impact of synoptic weather, regional transport and heterogeneous reactions [J]. Atmospheric Chemistry and Physics. 2015,15(6):2969-2983. [2] Zhou Y, Xing X F, Lang J L, et al. A comprehensive biomass burning emission inventory with high spatial and temporal resolution in China [J]. Atmospheric Chemistry and Physics, 2017,17(4):2839-2864. [3] Han L H, Yan H T, Xiang X, et al. Characteristics, evolution, and potential source regions of submicron aerosol in Beijing, China [J]. Atmospheric Environment, 2021,246:118061. [4] Han L H, Xiang X, Zhang H L, et al. Insights into submicron particulate evolution, sources and influences on haze pollution in Beijing, China [J]. Atmospheric Environment, 2019,201:360-368. [5] Vecchi R, Marcazzan G, Valli G, et al. The role of atmospheric dispersion in the seasonal variation of PM1 and PM2.5 concentration and composition in the urban area of Milan (Italy) [J]. Atmospheric Environment, 2004,38(27):4437-4446. [6] Valotto G, Squizzato S, Masiol M, et al. Elemental characterization, sources and wind dependence of PM1 near Venice, Italy [J]. Atmospheric Research. 2014,143:371-379. [7] Corsini E, Vecchi R, Marabini L, et al. The chemical composition of ultrafine particles and associated biological effects at an alpine town impacted by wood burning [J]. Science of the Total Environment, 2017,587:223-231. [8] Qi M, Zhu X, Du W, et al. Exposure and health impact evaluation based on simultaneous measurement of indoor and ambient PM2.5 in Haidian, Beijing [J]. Environmental Pollution, 2017,220:704-712. [9] Hua Y, Wang S X, Jiang J K, et al. Characteristics and sources of aerosol pollution at a polluted rural site southwest in Beijing, China [J]. Science of the Total Environment, 2018,626:519-527. [10] 韩力慧,时瑞芳,崔建硕,等.北京市典型区域大气亚微米颗粒物理化特性及其来源[J]. 中国环境科学, 2022,42(8):3522-3535. Han L H, Shi R F, Cui J S, et al. Physicochemical characteristics and sources of atmospheric submicro particulate matter at a typical area in Beijing [J]. China Environmental Science, 2022,42(8):3522-3535. [11] Xu W, Zhou W, Li Z, et al. Changes in primary and secondary aerosols during a controlled Chinese New Year [J]. Environmental Pollution, 2022,315:120408. [12] Ng N L, Herndon S C, Trimborn A, et al. An aerosol chemical speciation monitor (ACSM) for routine monitoring of the composition and mass concentrations of ambient aerosol [J]. Aerosol Science and Technology, 2011,45(7):780-794. [13] Ulbrich I M, Canagaratna M R, Zhang Q, et al. Interpretation of organic components from Positive Matrix Factorization of aerosol mass spectrometric data [J]. Atmospheric Chemistry and Physics, 2009,9(9):28. [14] Zhang Q, Jimenez J L, Canagaratna M R, et al. Understanding atmospheric organic aerosols via factor analysis of aerosol mass spectrometry: a review [J]. Analytical and Bioanalytical Chemistry, 2011,401(10):23. [15] 王晓琦,周颖,程水源,等.典型城市冬季PM2.5水溶性离子污染特征与传输规律研究[J]. 中国环境科学, 2016,36(8):2289-2296. Wang X Q, Zhou Y, Cheng S Y, et al. Characterization and regional transmission impact of water-soluble ions in PM2.5during winter in typical cities [J]. China Environmental Science, 2016,36(8):2289-2296. [16] Zhang Y, Huang W, Cai T, et al. Concentrations and chemical compositions of fine particles (PM2.5) during haze and non-haze days in Beijing [J]. Atmospheric Research, 2016,174-175:62-69. [17] Li J, Gao W, Cao L, et al. Effects of different stagnant meteorological conditions on aerosol chemistry and regional transport changes in Beijing, China [J]. Atmospheric Environment, 2021,258:10. [18] 沈嵩,刘蕾,温维,等.北京及周边地区夏季PM2.5中含碳组分污染特征与来源解析[J]. 环境工程, 2022,40(2):71-80. Shen S, Liu L, Wen W, et al. Pollution characterization and source analysis of carbon components of PM2.5 in Beijing and surrounding areas in summer [J]. Environmental Engineering, 2022,40(2):71-80. [19] Wang J Q, Gao J, Che F, et al. Decade-long trends in chemical component properties of PM2.5 in Beijing, China (2011~2020) [J]. Science of the Total Environment, 2022,832:154664. [20] Xu S, Ren L, Lang Y, et al. Molecular markers of biomass burning and primary biological aerosols in urban Beijing : size distribution and seasonal variation [J]. Atmospheric Chemistry and Physics, 2020, 20(6):3623-3644. [21] 韩力慧,王红梅,向欣,等.北京市典型区域降水特性及其对细颗粒物影响[J]. 中国环境科学, 2019,39(9):3635-3646. Han L H, Wang H M, Xiang X, et al. The characteristics of precipitation and its impact on fine particles at a representative region in Beijing [J]. China Environmental Science, 2019,39(9):3635-3646. [22] Han L, Yan H, Xiang X, et al. Characteristics, evolution, and potential source regions of submicron aerosol in Beijing, China [J]. Atmospheric Environment, 2021,246:118061. [23] Zhang H, Cheng S, Wang X, et al. Continuous monitoring, compositions analysis and the implication of regional transport for submicron and fine aerosols in Beijing, China [J]. Atmospheric Environment, 2018,195:30-45. [24] Kim Y J, Spak S N, Carmichael G R, et al. Modeled aerosol nitrate formation pathways during wintertime in the Great Lakes region of North America [J]. Journal of Geophysical Research-Atmospheres, 2014,119(21):12420-12445. [25] Hennigan C J, Bergin M H, Dibb J E, et al. Enhanced secondary organic aerosol formation due to water uptake by fine particles [J]. Geophysical Research Letters, 2008,35(18). [26] Ranjan M, Presto A A, May A A, et al. Temperature dependence of gas-particle partitioning of primary organic aerosol emissions from a small diesel engine [J]. Aerosol Science and Technology, 2012,46(1):13-21. [27] Chen Z Y, Chen D L, Wen W, et al. Evaluating the "2+26" regional strategy for air quality improvement during two air pollution alerts in Beijing: variations in PM2.5 concentrations, source apportionment, and the relative contribution of local emission and regional transport [J]. Atmospheric Chemistry and Physics, 2019,19(10):6879-6891. [28] Yao X H, Chan C K, Fang M, et al. The water-soluble ionic composition of PM2.5 in Shanghai and Beijing, China [J]. Atmospheric Environment, 2002,36(26):4223-4234. [29] Sun Y L, Wang Z F, Fu P Q, et al. Aerosol composition, sources and processes during wintertime in Beijing, China [J]. Atmospheric Chemistry and Physics, 2013,13(9):4577-4592. [30] Zhang J K, Wang Y S, Huang X J, et al. Characterization of organic aerosols in Beijing using an aerodyne high-resolution aerosol mass spectrometer [J]. Advances in Atmospheric Sciences, 2015,32(6):877-888. [31] Xu P, Zhang J, Ji D, et al. Characterization of submicron particles during autumn in Beijing, China [J]. Journal of Environmental Sciences, 2018,63:16-27. [32] Chen X R, Wang H C, Lu K D, et al. Field determination of nitrate formation pathway in winter Beijing [J]. Environmental Science & Technology, 2020,54(15):9243-9253. [33] Sun Y L, Wang Z F, Dong H B, et al. Characterization of summer organic and inorganic aerosols in Beijing, China with an Aerosol Chemical Speciation Monitor [J]. Atmospheric Environment, 2012,51:250-259. [34] An Z S, Huang R J, Zhang R Y, et al. Severe haze in northern China: A synergy of anthropogenic emissions and atmospheric processes [J]. Proceedings of the National Academy of Sciences of the United States of America, 2019,116(18):8657-8666. [35] Kong L W, Feng M, Liu Y F, et al. Elucidating the pollution characteristics of nitrate, sulfate and ammonium in PM2.5 in Chengdu, southwest China, based on 3-year measurements [J]. Atmospheric Chemistry and Physics, 2020,20(19):11181-11199. [36] Cheng Y F, Zheng G J, Wei C, et al. Reactive nitrogen chemistry in aerosol water as a source of sulfate during haze events in China [J]. Science Advances. 2016,2(12):e1601530. [37] Cheng Y, Engling G, He K B, et al. The characteristics of Beijing aerosol during two distinct episodes: Impacts of biomass burning and fireworks [J]. Environmental Pollution, 2014,185:149-157. [38] Zhang Q, Zheng Y X, Tong D, et al. Drivers of improved PM2.5 air quality in China from 2013 to 2017[J]. Proceedings of the National Academy of Sciences of the United States of America, 2019,116(49):24463-24469. [39] 王瑛,黄汝锦,钟昊斌,等.北京春季亚微米气溶胶的化学组分、特性及有机气溶胶来源解析[J]. 地球环境学报, 2019,10(6):556-566. Wang Y, Huang R J, Zhong H B, et al. Chemical composition, characteristics and sources of PM1 in Beijing spring [J]. Journal of Earth Environment, 2019,10(6):556-566. [40] Ng N L, Canagaratna M R, Zhang Q, et al. Organic aerosol components observed in Northern Hemispheric datasets from Aerosol Mass Spectrometry [J]. Atmospheric Chemistry and Physics, 2010, 10(10):4625-4641. [41] Zhong J, Zhang X, Zhang Y, et al. Drivers of the rapid rise and daily-based accumulation in PM1[J]. Science of the Total Environment, 2021,760:143394. [42] Qu Q, Wang S, Zhao B, et al. Response of organic aerosol in Beijing to emission reductions during the XXIV Olympic Winter Games [J]. Science of the Total Environment, 2024,914:170033. [43] Sun Y, Wang Z, Dong H, et al. Characterization of summer organic and inorganic aerosols in Beijing, China with an Aerosol Chemical Speciation Monitor [J]. Atmospheric Environment, 2012,51:250-259. [44] 高韩钰.北京南郊区与市区PM2.5中水溶性无机离子季节变化特征研究[D]. 保定:河北农业大学, 2018. Gao H Y. Seasonal Variation of Water-Soluble Inorganic Ions in PM2.5in the Southern Suburbs and Urban Areas of Beijing [D]. Baoding: Hebei Agricultural University, 2018. |
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