杭州市2017年冬季一次重灰霾过程中PM_(2.5)水溶性离子特征、来源及成因分析
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摘要
利用在线监测仪测量了杭州市一次重灰霾过程(2017年12月29日至2018年1月3日)中PM_(2.5)主要水溶性离子(Cl~-、 SO_4~(2-)、 NO_3~-、 NH_4~+、 Na~+、 Ga~(2+)、 Mg~(2+))及主要气态污染物(SO_2、 NO_2、 O_3、 NO、 CO、HCl、NH_3、HNO_2、HNO_3)的小时浓度。结合混合受体模型和国控监测分析,研究了2017年12月30-31日重灰霾事件的污染特征、来源和成因。研究结果表明:PM_(2.5)浓度高达318μg·m~(-3); NO_3~-/SO_4~(2-)最大值为2.68,说明移动源污染是杭州市PM_(2.5)形成的重要来源; PM_(2.5)/CO最高达到0.19,说明二次细颗粒物对PM_(2.5)贡献很大;NO_3~-、SO_4~(2-)、NH_4~+的浓度总和占PM_(2.5)平均浓度的64.3%,说明二次无机细颗粒物是杭州重灰霾形成的重要原因,且NO_3~-的贡献最大,占33.5%。混合受体模型分析显示,杭州市重灰霾污染的潜在源区主要位于安徽、江苏、河南、山东四省交界处,以及安徽省中东部、蚌埠、芜湖等工业污染较为严重的城市。夹杂着大量污染物的北方干冷空气远距离传输叠加部分局地源是杭州此次重雾霾形成的根本原因。因此,为了改善杭州市空气质量,不仅需控制当地的污染物排放,而且还需对整个长三角地区甚至跨区域采取大气联防联控策略。
The hourly concentrations of water soluble ions(Cl~-、SO_4~(2-)、NO_3~-、NH_4~+、Na~+、Ga~(2+)、Mg~(2+)) of PM_(2.5) and the major gaseous pollutants(SO_2、NO_2、NO、CO、HCl、NH_3、HNO_2、HNO_3) floating in the atmosphere in Hangzhou during the period of December 29, 2017 to January 3, 2018 were measured by online monitoring instruments. With the hybrid receptor model and observations data at the national monitoring stations, we analyzed the characteristics, sources and origins of this heavy haze episode in Hangzhou based on the data recorded during December30 to 31, 2017. It showed that during the heavy haze episode, the maximum values of PM_(2.5) and NO_3~-/SO_4~(2-)were318 μg·m-3 and 2.68, respectively, indicating that the mobile source was one of the major contributors to the formation of PM_(2.5), and the maximum value of PM_(2.5)/CO was 0.19, indicating the significant contribution of secondary PM. The fact that the total concentrations of NO_3~-, NH_4~+ and SO_4~(2-) account for 64.3% of PM_(2.5) concentrations with the 33.5%biggest contribution from NO_3~- indicated that the formation of haze was mainly caused by the secondary inorganic aerosols in Hangzhou. The results of the hybrid receptor model analyses reveal that potential source areas for the haze in Hangzhou are mainly located in the border areas of the four provinces(Anhui, Jiangsu, Henan and Shandong), centralsouthern Anhui province, and cities with highly polluted industries such as Bengbu and Wuhu. In addition to the local sources, long-distance transport of a large amount of air pollutants brought by the cold dry air flow from the north is a fundamental cause of this heavy haze episode in Hangzhou. Therefore, to improve the air quality in Hangzhou, it is necessary to control local pollution emissions, and also call for a joint control strategy for air pollution emissions in the Yangtze River Delta, and even bigger regions.
The hourly concentrations of water soluble ions(Cl~-、SO_4~(2-)、NO_3~-、NH_4~+、Na~+、Ga~(2+)、Mg~(2+)) of PM_(2.5) and the major gaseous pollutants(SO_2、NO_2、NO、CO、HCl、NH_3、HNO_2、HNO_3) floating in the atmosphere in Hangzhou during the period of December 29, 2017 to January 3, 2018 were measured by online monitoring instruments. With the hybrid receptor model and observations data at the national monitoring stations, we analyzed the characteristics, sources and origins of this heavy haze episode in Hangzhou based on the data recorded during December30 to 31, 2017. It showed that during the heavy haze episode, the maximum values of PM_(2.5) and NO_3~-/SO_4~(2-)were318 μg·m-3 and 2.68, respectively, indicating that the mobile source was one of the major contributors to the formation of PM_(2.5), and the maximum value of PM_(2.5)/CO was 0.19, indicating the significant contribution of secondary PM. The fact that the total concentrations of NO_3~-, NH_4~+ and SO_4~(2-) account for 64.3% of PM_(2.5) concentrations with the 33.5%biggest contribution from NO_3~- indicated that the formation of haze was mainly caused by the secondary inorganic aerosols in Hangzhou. The results of the hybrid receptor model analyses reveal that potential source areas for the haze in Hangzhou are mainly located in the border areas of the four provinces(Anhui, Jiangsu, Henan and Shandong), centralsouthern Anhui province, and cities with highly polluted industries such as Bengbu and Wuhu. In addition to the local sources, long-distance transport of a large amount of air pollutants brought by the cold dry air flow from the north is a fundamental cause of this heavy haze episode in Hangzhou. Therefore, to improve the air quality in Hangzhou, it is necessary to control local pollution emissions, and also call for a joint control strategy for air pollution emissions in the Yangtze River Delta, and even bigger regions.
引文
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[22]YE B,JI X L,YANG H Z,et al.Concentration and chemical composition of PM2.5in Shanghai for a 1-year period[J].Atmospheric Environment,2003,37(4):499-510.DOI:10.1046/j.1365-3113.2000.00127.x
[2]GUO S,HU M,ZAMORA M L,et al.Elucidating severe urban haze formation in China[J].Proceedings of the National Academy of Sciences,2014,111(49):17373-17378.DOI:10.1073/pnas.1419604111
[3]朱彤,尚静,赵德峰.大气复合污染及灰霾形成中非均相化学过程的作用[J].中国科学(化学),2010,40(12):1731-1740.ZHU T,SHANG J,ZHAO D F.The roles of heterogeneous chemical processes in the formation of an air pollution complex and gray haze[J].Scientia Sinica Chimica,2010,40(12):1731-1740.
[4]SCHWATZ J,DOEKERY D W,NEAS L S.Is daily mortality associated specifically with fine particles[J].Journal of the Air Waste Management Association,1996,46(10):927-939.DOI:10.1080/10473289.1996.10467528
[5]SCHWARTZ J.Harvesting and long term exposure effects in the relation between air pollution and mortality[J].American Journal of Epidemiology,2000,151(5):440-448.DOI:10.1046/j.1439-0523.1999.00435.x
[6]COHEN A J,ERSON H R,OSTRA B,et al.The global burden of disease due to outdoor air pollution[J].Journal of Toxicology and Environmental Health,2005,68(13/14):1301-1307.DOI:10.1080/15287390590936166
[7]徐港,王斯,李鹏飞,等.温州市灰霾污染特征与成因分析[J].环境污染与防治,2017,39(10):1101-1107.DOI:10.15985/j.cnki.1001-3865.2017.10.012XU G,WANG S,LI P F,et al.Characteristics and origins of haze pollution in Wenzhou[J].Environmental Pollution and Control,2017,39(10):1101-1107.DOI:10.15985/j.cnki.1001-3865.2017.10.012
[8]HU M,HE L Y,ZHANG Y H,et al.Seasonal variation of ionic species in fine particles at Qingdao,China[J].Atmospheric Environment,2002,36(38):5853-5859.DOI:10.1016/S1352-2310(02)00581-2
[9]包贞,冯银厂,焦荔,等.杭州市大气PM2.5和PM10污染特征及来源解析[J].中国环境监测,2010,26(2):44-48.BAO Z,FENG Y C,JIAO L,et al.Characterization and source apportionment of PM2.5and PM10in Hangzhou[J].Environmental Monitoring in China,2010,26(2):44-48.
[10]王晓浩,赵倩彪,崔虎雄.基于在线监测的上海郊区冬季PM2.5来源解析[J].南京大学学报(自然科学版),2015(3):517-523.DOI:10.13232/j.cnki.jnju.2015.03.008WANG X H,ZHAO Q B,CUI H X.PM2.5source apportionment at suburb of Shanghai in winter based on real time monitoring[J].Journal of Nanjing University(Natural Sciences),2015(3):517-523.DOI:10.13232/j.cnki.jnju.2015.03.008
[11]操文祥,陈楠,田一平,等.武汉地区秋冬季清洁与重污染过程的水溶性离子特征研究[J].环境科学学报,2017,37(1):82-88.DOI:10.13671/j.hjkxxb.2016.0177CAO W X,CHEN N,TIAN Y P,et al.Characteristic analysis of water-soluble ions during clean and heavy pollution processes in autumn and winter in Wuhan[J].Acta Scientiae Circumstantiae,2017,37(1):82-88.DOI:10.13671/j.hjkxxb.2016.0177
[12]ZHANG Q Y,YAN R C,FAN J W,et al.A heavy haze episode in Shanghai in December of 2013:Characteristics,origins and implications[J].Aerosol and Air Quality Research,2015,15(5):1881-1893.
[13]YU S C,ZHANG Q Y,YAN R C,et al.Origin of air pollution during a weekly heavy haze episode in Hangzhou,China[J].Environmental Chemistry Letters,2014,12(4):543-550.DOI:10.1007/s10311-014-0483-1
[14]ZHANG Y L,CAO F.Fine particulate matter(PM2.5)in China at a city level[J].Scientific Reports,2015(5):1-12.DOI:10.1038/srep14884
[15]GOUW J A D,WELSHBON D,WARNEKE C,et al.Emission and chemistry of organic carbon in the gas and aerosol phase at a sub-urban site near Mexico city in March 2006 during the MILAGRO study[J].Atmospheric Chemistry&Physics Discussions,2009,8(6):3425-3442.DOI:10.5194/acpd-8-21265-2008
[16]ARIMOTO R,DUCE R A,SAVOIE D L,et al.Relationships among aerosol constituents from Asia and the North Pacific during Pem-West A[J].Journal of Geophysical Research,1996,101(D1):2011-2023.DOI:10.1029/95JD01071
[17]周敏,陈长虹,王红丽,等.上海市秋季典型大气高污染过程中颗粒物的化学组成变化特征[J].环境科学学报,2012,32(1):81-92.DOI:10.13671/j.hjkxxb.2012.01.019ZHOU M,CHEN C H,WANG H L,et al.Chemical characteristics of particulate matters during air pollution episodes in autumn of Shanghai,China[J].Acta Scientiae Circumstantiae,2012,32(1):81-92.DOI:10.13671/j.hjkxxb.2012.01.019
[18]YAO X H,FANG M,HE K B,et al.The water-soluble ionic composition of PM2.5in Shanghai and Beijing,China[J].Atmospheric Environment,2002,36(26):4223-4234.DOI:10.1016/S1352-2310(02)00342-4
[19]葛顺,汤莉莉,秦玮,等.南京地区秋季灰霾天气特征及其水溶性离子分析[J].环境科学与技术,2015,38(2):99-104.DOI:10.3969/j.issn.1003-6504.2015.02.019GE S,TANG L L,QIN W,et al.Characteristics analysis of haze and water-soluble ion in Nanjing in Autumn[J].Environmental Science&Technology,2015,38(2):99-104.DOI:10.3969/j.issn.1003-6504.2015.02.019
[20]WANG Y,ZHUANG G S,TANG A H,et al.The ion chemistry and the source of PM2.5aerosol in Beijing[J].Atmospheric Environment,2005,39(21):3771-3784.DOI:10.1016/j.atmosenv.2005.03.013
[21]沈振兴,李丽珍,杜娜,等.西安市春季大气细粒子的质量浓度及其水溶性组分的特征[J].生态环境,2007,16(4):1193-1198.DOI:10.3969/j.issn.1674-5906.2007.04.025SHEN Z X,LI L Z,DU N,et al.Mass concentration and water-soluble ions in spring aerosol(PM2.5)at Xi'an[J].Ecology and Environment,2007,16(4):1193-1198.DOI:10.3969/j.issn.1674-5906.2007.04.025
[22]YE B,JI X L,YANG H Z,et al.Concentration and chemical composition of PM2.5in Shanghai for a 1-year period[J].Atmospheric Environment,2003,37(4):499-510.DOI:10.1046/j.1365-3113.2000.00127.x