青岛冬季霾-沙尘重污染过程PM1理化特征及来源分析

彭倩倩; 刘晓环; 杜金花; 刘子杨; 韩枝燏; 王征; 薛莲; 刘翔; 孙英杰; 张宜升

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中国环境科学 ›› 2020, Vol. 40 ›› Issue (9) : 3731-3740.

大气污染与控制

青岛冬季霾-沙尘重污染过程PM₁理化特征及来源分析

彭倩倩¹, 刘晓环², 杜金花¹, 刘子杨¹, 韩枝燏¹, 王征³, 薛莲³, 刘翔⁴, 孙英杰¹, 张宜升¹

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Physicochemical characteristics and source analysis of PM₁ during winter haze-dust pollution event in Qingdao

PENG Qian-qian¹, LIU Xiao-huan², DU Jin-hua¹, LIU Zi-yang¹, HAN Zhi-yu¹, WANG Zheng³, XUE Lian³, LIU Xiang⁴, SUN Ying-jie¹, ZHANG Yi-sheng¹

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文章历史 +

摘要

对2018年11月21日~12月2日期间青岛市大气PM₁的质量浓度、化学组分和数浓度进行连续观测，结合国控站点监测数据和气象条件，分析青岛市秋末冬初一次典型霾-沙尘重污染过程的特征及污染物来源.结果表明：本次污染过程可分为霾前（11月21~23日）、霾期（11月24~25日）、霾-沙尘叠加期（11月26日）、沙尘期（11月27~29日）、沙尘后（11月30日~12月2日）5个发展阶段，观测期间PM₁质量浓度为（40±20）μg/m³，霾期PM₁为沙尘期的2.03倍.冷锋锋前以人为污染物气团为主，锋后以冷干沙尘气团为主，并在长距离传输中保持干燥，受沙尘传输过程中经过区域的影响较小，导致沙尘阶段PM_2.5和PM₁₀错峰12h出现.霾期PM₁中SO₄^2-、NO₃^-质量浓度比霾前分别升高73%、111%，SOR、NOR分别升高28%、67%，表明霾期NO₃^-的二次转化明显升高.PM₁中NH₄⁺主要以（NH₄）₂SO₄和NH₄NO₃形式存在，为富氨条件.本次沙尘事件气团传输过程中途经山西、河北、山东西北部等污染物高强度排放区域，前锋到达青岛时，携带的人为污染物占主导，导致沙尘期PM₁中OC、EC占比为霾期的1.73、1.53倍.霾期SOC/OC值为0.43，略低于沙尘期，表明霾期SOC生成受到抑制.

Abstract

During an episode of winter haze-dust pollution event in Qingdao from November 21 to December 2 in 2018, we continuously measured the mass concentration, chemical composition and number concentration of PM₁, in combination with the routine monitoring data from a national ambient air quality station, to study pollutant characteristics, source attribution for this typical winter air pollution event. The results showed that the whole event could be divided into five stages: pre-haze (November 21 to 23), haze period (November 24 to 25), haze-dust mixing period (November 26), dust period (November 27 to 29), and post-dust period (November 30 to December 2). During the pollution, the mean mass concentration of PM₁ was (40±20)μg/m³, and PM₁ in the haze period was 2.03 times higher than that of the dust period. In the post-front, the dust air kept the air dry and was mainly dominated by cold dry dust particles, which were less affected by accumulated anthropogenic pollutants from the areas it passed through during the long distance transmission. During the pre-front, the air was mainly dominated by polluted air masses from regions with intense anthropogenic emissions, resulting in more than 12 hours delays between the peaks of PM_2.5 and PM₁₀ in the dust period. The mass concentrations of SO₄^2- and NO₃^- in PM₁during the haze period increased by 73% and 111% than those of the pre-haze, respectively. SOR and NOR during the haze period increased by 28% and 67% than those of the pre-haze, indicating that the secondary formation of NO₃^- increased significantly during the haze period. NH₄⁺ in PM₁ mainly existed in the form of (NH₄)₂SO₄ and NH₄NO₃, when inorganic ions were sufficiently neutralized by ammonium. Before reaching Qingdao, air masses passed over of the regions with intense anthropogenic emissions, such as Shanxi, Hebei and northwest of Shandong. Thus, when the pre-front arrived, these anthropogenic pollutants leaded to 1.73 and 1.53 times increase of OC and EC masses in PM₁ during the dust period than in the haze period. The mass proportion of SOC in total OC in the haze period was 0.43 lower than that that in the dust period (0.48). This indicated that the SOC formation during the haze period had been suppressed.

导出引用

彭倩倩, 刘晓环, 杜金花, 刘子杨, 韩枝燏, 王征, 薛莲, 刘翔, 孙英杰, 张宜升. 青岛冬季霾-沙尘重污染过程PM₁理化特征及来源分析[J]. 中国环境科学. 2020, 40(9): 3731-3740

PENG Qian-qian, LIU Xiao-huan, DU Jin-hua, LIU Zi-yang, HAN Zhi-yu, WANG Zheng, XUE Lian, LIU Xiang, SUN Ying-jie, ZHANG Yi-sheng. Physicochemical characteristics and source analysis of PM₁ during winter haze-dust pollution event in Qingdao[J]. China Environmental Science. 2020, 40(9): 3731-3740

中图分类号： X513

参考文献

[1] 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]. PANS, 2019,116(18):8657-8666.
[2] Hu W W, Hu M, Hu W, et al. Chemical composition, sources, and aging process of submicron aerosols in Beijing:Contrast between summer and winter[J]. Journal of Geophysical Research, 2016,121(4):1955-1977.
[3] 宿文康,鲍晓磊,倪爽英,等.2018年石家庄市秋冬季典型霾污染特征[J]. 环境科学, 2019,40(11):4755-4763. Su W K, Bao X L, Ni S Y, et al. Characteristics of Haze Pollution Episodes During Autumn and Winter in 2018 in Shijiazhuang[J]. Environmental Science, 2019,40(11):4755-4763.
[4] Zhang D Z, Iwasaka Y, Shi G Y, et al. Separated status of the natural dust plume and polluted air masses in an Asian dust storm event at coastal areas of China[J]. Journal of Geophysical Research, 2005,110(6):1-9.
[5] 张凯,高会旺,张仁建,等.我国沙尘的来源、移动路径及对东部海域的影响[J]. 地球科学进展, 2005,20(6):627-636. Zhang K, Gao H W, Zhang R J, et al. Source sand movement routes of sand-dust aerosols and their impact probabilities on China seas in 2000-2002[J]. Advances in Earth Science, 2005,20(6):627-636.
[6] Fu H B, Chen J M. Formation, features and controlling strategies of severe haze-fog pollutions in China[J]. Science of the Total Environment, 2017,578(1):121-138.
[7] 熊亚军,唐宜西,寇星霞,等.北京春季一次霾和沙尘混合污染天气过程分析[J]. 干旱气象, 2017,35(1):100-107. Xiong Y J, Tang Y X, Kou X X, et al. Analysis of the weather conditions for a case of heavy pollution in Beijing[J]. Meteorological Monthly, 2017,35(1):100-107.
[8] 王耀庭,李青春,郑祚芳,等.北京春季一次霾-沙天气污染特性与成因分析[J]. 环境科学, 2019,40(6):2582-2594. Wang Y T, Li Q C, Zheng Z F, et al. Research on the pollution characteristics and causality of haze-sand air pollution in Beijing in spring[J]. Environmental Science, 2019,40(6):2582-2594.
[9] 殷丽娜,褚旸晰,段菁春,等."2+26"城市一次多因素叠加重污染过程的特征分析[J]. 环境科学研究, 2019,32(12):2022-2030. Yin L N, Chu Y X, Duan J C, et al. Characteristics of a multi-factor superimposing haze episode in ‘2+26’ cities[J]. Research of Environmental Sciences, 2019,32(12):2022-2030.
[10] 朱媛媛,高愈霄,柴文轩,等.京津冀及周边区域PM_2.5叠加沙尘重污染过程特征及预报效果分析[J]. 环境科学, 2019,41(2):574-586. Zhu Y Y, Gao Y X, Chai W X, et al. Characteristics of heavy pollution and assessment of model predicted results of PM_2.5in Beijing-Tianjin-Hebei region and its surrounding areas during November 23to December 4, 2018[J]. Environmental Science, 2019,41(2):574-586.
[11] Chong X X, Wang Y, Liu R H, et al. Pollution characteristics and source difference of gaseous elemental mercury between haze and non-haze days in winter[J]. Science of The total Environment, 2019, 678:671-680.
[12] 张周祥,张养梅,张小曳,等.秋冬季节华北背景地区PM₁污染特征及来源[J]. 环境科学, 2017,38(7):2647-2655. Zhang Z X, Zhang Y M, Zhang X Y, et al. Sources and characteristics of regional background PM1in North China During the Autumn and Winter polluted period[J]. Environmental Science, 2017,38(7):2647-2655.
[13] 张婷,曹军骥,刘随心.宝鸡市PM_2.5中水溶性离子组分污染特征及来源分析[J]. 地球环境学报, 2017,8(1):46-54. Zhang T, Cao J J, Liu S X. Pollution characteristics and sources of water-soluble ions in PM_2.5 in Baoji[J]. Journal of Earth Environment, 2017,8(1):46-54.
[14] 王心培,王格慧,谢郁宁,等.长三角背景点夏季大气PM_2.5中水溶性无机离子污染特征及来源解析[J]. 环境科学研究, 2020,33(6):1399-1375. Wang X P, Wang G H, Xie Y N, et al. Chemical characterization and source apportionment of water-soluble inorganic ions of summertime atmospheric PM_2.5 in the background of Yangtze River Delta Region, China[J]. Research of Environmental Sciences, 2020,33(6):1366-1375.
[15] Zhai L, Li S, Zou B, et al. An improved geographically weighted regression model for PM_2.5 concentration estimation in large areas[J]. Atmospheric Environment, 2018,181:145-154.
[16] 罗玉,马振峰,赵鹏国,等.近36a来四川盆地持续霾事件特征及环流分析[J]. 中国环境科学, 2019,39(9):3604-3615. Luo Y, Ma Z F, Zhao P G, et al. Characteristics of persistent haze events and circulation analysis in Sichuan Basin in recent 36years[J]. China Environmental Science, 2019,39(9):3604-3615.
[17] 刘安康,王红磊,陈魁,等.南京市一次霾污染过程中水溶性离子分布特征[J]. 中国环境科学, 2019,39(5):1793-1803. Liu A K, Wang H L, Chen K, et al. Distribution characteristics of water-soluble ions during a haze pollution process in Nanjing[J]. China Environmental Science, 2019,39(5):1793-1803.
[18] 徐文帅,李云婷,孙瑞雯,等.典型沙尘回流天气过程对北京市空气质量影响的特征分析[J]. 环境科学学报, 2014,34(2):297-302. Xu W S, Li Y T, Sun R W, et al. Impact characteristics of a typical dust backflow weather on the air quality in Beijing[J]. Acta Scientiae Circumstantiae, 2014,34(2):297-302.
[19] Wu F, Zhang D Z, Cao J J, et al. Limited production of sulfate and nitrate on front-associated dust storm particles moving from desert to distant populated areas in northwestern China[J]. Atmospheric Chemistry and Physics, 2017,17(23):14473-14484.
[20] 周旭,张镭,郭琪,等.强沙尘暴的数值模拟及PM₁₀浓度的时空变化分析[J]. 中国环境科学, 2017,37(1):1-12. Zhou X, Zhang L, Guo Q, et al. Numerical simulation of a strong dust storm and the spatial-temporal distribution of PM₁₀concentration[J]. China Environmental Science, 2017,37(1):1-12.
[21] 李瑞芃,石金辉,张代洲,等.天气条件及气团来源对青岛春季大气颗粒物数浓度谱分布的影响[J]. 中国环境科学, 2012,32(8):1392-1399. Li R P, Shi J H, Zhang D Z, et al. Size distribution of atmospheric particles in number concentration in relation to meteorological conditions and air mass origins in Qingdao in spring[J]. China Environmental Science, 2012,32(8):1392-1399.
[22] 刘立忠,么远,韩婧,等.西安市大气颗粒物数浓度分布及典型天气条件特征变化[J]. 中国环境科学, 2015,35(12):3588-3594. Liu L Z, Yao Y, Han J, et al. Distribution of atmospheric particle number concentration in Xi'an and variations in typical weather conditions[J]. China Environmental Science, 2015,35(12):3588-3594.
[23] 沈利娟,施双双,郭振东,等.长三角沙尘中气溶胶粒径分布及化学组分特征[J]. 中国环境科学, 2019,39(6):2241-2248. Shen L J, Shi S S, Guo Z D, et al. Characteristics of aerosol size distribution and chemical components during a dust pollution episode in the Yangtze River Delta[J]. China Environmental Science, 2019, 39(6):2241-2248.
[24] Wang X M, Cheng J M, Cheng T T, et al. Particle number concentration, size distribution and chemical composition during haze and photochemical smog episodes in Shanghai[J]. Journal of Environmental Sciences, 2014,26(9):1894-1902.
[25] Shao P Y, Tian H Z, Sun Y J, et al. Characterizing remarkable changes of severe haze events and chemical compositions in multi-size airborne particles (PM₁, PM_2.5 and PM₁₀) from January 2013 to 2016~2017 winter in Beijing, China[J]. Atmospheric Environment, 2018,189:133-144.
[26] Cheng H R, Gong W, Wang Z W, et al. Ionic composition of submicron particles (PM_1.0) during the long-lasting haze period in January 2013 in Wuhan, central China[J]. Journal of Environmental Sciences, 2014,26(4):810-817.
[27] Liu J, Wu D, Fan S J, et al. A one-year, on-line, multi-site observational study on water-soluble inorganic ions in PM_2.5 over the Pearl River Delta region, China[J]. Science of the Total Environment, 2017,601:1720-1732.
[28] Luo L, Zhang Y Y, Xiao H Y, et al. Spatial distributions and sources of inorganic chlorine in PM_2.5 across China in Winter[J]. Atmosphere, 2019,40(9):505.
[29] 梁晓宇,单春艳,孟瑶,等.唐山一次冬季重污染过程污染特征及成因分析[J]. 中国环境科学, 2019,39(5):1804-1812. Liang X Y, Shan C Y, Meng Y, et al. Characteristics and formation mechanism of a heavy winter air pollution event in Tangshan[J]. China Environmental Science, 2019,39(5):1804-1812.
[30] Liu P F, Zhang C L, Mu Y J, et al. The possible contribution of the periodic emissions from farmers' activities in the North China Plain to atmospheric water-soluble ions in Beijing[J]. Atmospheric Chemistry and Physics, 2016,16(15):10097-10109.
[31] 徐虹,肖致美,孔君,等.天津市冬季典型大气重污染过程特征[J]. 中国环境科学, 2017,37(4):1239-1246. Xu H, Xiao Z M, Kong J, et al. Characteristic of atmospheric heavy pollution episodes in winter of Tianjin[J]. China Environmental Science, 2017,37(4):1239-1246.
[32] Tian M, Wang H B, Chen Y, et al. Characteristics of aerosol pollution during heavy haze events in Suzhou, China[J]. Atmospheric Chemistry and Physics, 2016,16(11):7357-7371.
[33] Teng X L, Hu Q J, Zhang L M, et al. Identification of major sources of atmospheric NH₃ in an urban environment in northern China during wintertime[J]. Environmental Science & Technology, 2017,51(12):6839-6848.
[34] Li Q, Jiang J K, Cai S Y, et al. Gaseous ammonia emissions from coal and biomass combustion in household stoves with different combustion efficiencies[J]. Environmental Science & Technology, 2016,3(3):98-103.
[35] Xu X M, Zhang H F, Chen J M, et al. Six sources mainly contributing to the haze episodes and health risk assessment of PM_2.5 at Beijing suburb in winter 2016[J]. Ecotoxicology and Environmental Safety, 2018,166:146-156.
[36] Cao J J, Lee S C, Ho K F, et al. Spatial and seasonal variations of atmospheric organic carbon and elemental carbon in Pearl River Delta Region, China[J]. Atmospheric Environment, 2004,38(27):4447-4456.
[37] Zhang Y, Huang W, Ji T Q, et al. Concentrations and chemical compositions of fine particles (PM_2.5) during haze and non-haze days in Beijing[J]. Atmospheric Research, 2016,174:62-69.
[38] Chow J C, Watson J G, Lu Z, et al. Descriptive analysis of PM_2.5and PM₁₀at regionally representative locations during SJVAQAS/AUSPEX[J]. Atmospheric Environment, 1996,30(12):2079-2112.
[39] Ji D S, Li L, Wang Y S, et al. The heaviest particulate air-pollution episodes occurred in northern China in January, 2013:Insights gained from observation[J]. Atmospheric Environment, 2014,92:546-556.
[40] Zhao M F, Qiao T, Huang Z S, et al. Comparison of ionic and carbonaceous compositions of PM_2.5 in 2009 and 2012 in Shanghai, China[J]. Science of The Total Environment, 2015,536:695-703.
[41] 李兴华.生物质燃烧大气污染物排放特征研究[D]. 北京:清华大学, 2007. Li X H. Characterization of air pollutants emitted from biomass burning in China[D]. Beijing:Tsinghua University, 2007.
[42] Zhang R J, Tao J, Ho K F, et al. Characterization of atmospheric organic and elemental carbon of PM_2.5 in a typical semi-Arid Area of northeastern China[J]. Aerosol and Air Quality Research, 2012,12(5):792-802.
[43] Ram K, Sarin M M. Day-night variability of EC, OC, WSOC and inorganic ions in urban environment of Indo-Gangetic Plain:Implications to secondary aerosol formation[J]. Atmospheric Environment, 2011,45(2):460-468.
[44] Qiao B T, Chen Y, Tian M, et al. Characterization of water soluble inorganic ions and their evolution processes during PM_2.5 pollution episodes in a small city in southwest China[J]. Science of the total Environment, 2019,650:2605-2613.
[45] 张养梅,孙俊英,张小曳,等.北京亚微米气溶胶化学组分及粒径分布季节变化特征[J]. 中国科学:地球科学, 2013,43(4):606-617. Zhang Y M, Sun J Y, Zhang X Y, et al. Seasonal characterization of components and size distributions for submicron aerosols in Beijing[J]. Science China:Earth Sciences, 2013,56:890-900.
[46] Zhao L, Wang L T, Tan J H, et al. Changes of chemical composition and source apportionment of PM_2.5 during 2013~2017 in urban Handan, China[J]. Atmospheric Environment, 2019,206:119-131.
[47] 张宜升.农村典型燃烧源含碳物质排放及其环境风险研究[M]. 北京:科学出版社, 2017:99-101. Zhang Y S. Research on primary carbonaceous gases and aerosol emissions form rural typical combustion sources and its environmental risks[M]. Beijing:Science Press, 2017:99-101.
[48] 樊啸辰,郎建垒,程水源,等.北京市大气环境PM_2.5和PM₁及其碳质组分季节变化特征及来源分析[J]. 环境科学, 2018,39(10):4430-4438. Fan X C, Lang J L, Cheng S Y et al. Seasonal variation and source analysis for PM_2.5, PM₁ and their carbonaceous components in Beijing[J]. Environmental Science, 2018,39(10):4430-4438.
[49] 李璇,赵晓楠,俞磊,等.石家庄市采暖前后大气颗粒物及其碳组分特征[J]. 环境科学研究, 2018,31(4):679-687. Li X, Zhao X N, Yu L et al. Characteristics of carbon components in atmospheric particles before and during the heating period in Shijiazhuang city[J]. Research of Environmental Sciences, 2018,31(4):679-687.
[50] Zhang Y Y, Lang J L, Cheng S Y, et al. Chemical composition and sources of PM₁ and PM_2.5 in Beijing in autumn[J]. Science of The Total Environment, 2018,630:72-82.
[51] Chow J C, Watson J G, Kuhns H, et al. Source profiles for industrial, mobile, and area sources in the big bend regional aerosol visibility and observational study[J]. Chemosphere, 2004,54(2):185-208.
[52] Cao J J, Wu F, Chow J C, et al. Characterization and source apportionment of atmospheric organic and elemental carbon during fall and winter of 2003 in Xi' an, China[J]. Atmospheric Chemistry and Physics, 2005,5(11):3127-3137.
[53] Xu H M, Cao J J, Chow J C et al. Inter-annual variability of wintertime PM_2.5 chemical composition in Xi'an, China:Evidences of changing source emissions[J]. Science of the Total Environment, 2016,545:546-555.