临安夏季霾和清洁天气PM_(2.5)化学组成特征比较
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摘要
本研究对长江三角洲背景地区临安大气本底站夏季PM_(2.5)进行连续采集,并对其分别进行OC/EC和水溶性离子测试分析.研究结果发现,临安夏季PM_(2.5)中OC和EC平均质量浓度分别为(14.3±3.95)μg·m-3和(3.33±1.47)μg·m-3.与城市地区相比,本研究临安背景地区夏季气溶胶中OC和EC相关性较弱(R2=0.31,P<0.01).二次无机离子,即SO_4~(2-)、NO_3~-、NH_4~+(SNA),明显高于其它水溶性无机离子,平均浓度分别为(8.70±5.66)、(2.04±1.07)和(3.25±2.29)μg·m-3.基于对临安夏季PM_(2.5)连续加密观测、气团后向轨迹以及火点图研究分析,发现静稳天气条件和区域传输都可以影响临安地区PM_(2.5)的化学组成特征.此外,通过对临安本底站霾天和清洁天PM_(2.5)化学组成特征比较发现,与清洁天相比,霾污染天气POC和EC占PM_(2.5)的质量分数没有明显变化,而SOC占PM_(2.5)的质量分数却呈现了明显的下降趋势.与SOC不同,SO_4~(2-)和NH_4~+占PM_(2.5)的质量分数在霾污染天气均呈现了上升的趋势,说明二次无机离子有另一种明显增强的化学生成路径,即非均相化学反应.
PM_(2.5) samples were collected at a background site of the Yangtze River Delta in China,during summertime,of which the carbonaceous components,i. e.,OC and EC,and water-soluble inorganic ions,including sulfate,nitrate,and ammonium,were quantified. The average concentrations of OC and EC in PM_(2.5) during summer at Lin'an were( 14. 3 ± 3. 95) μg·m-3 and( 3. 33 ±1. 47) μg·m-3,respectively. Compared to an urban site,the correlation between OC and EC during summertime in Lin'an,which was a rural site,was relatively weak( R2= 0. 31,P < 0. 01). The concentrations of secondary inorganic aerosols( sulfate as SO_4~(2-),nitrate as NO-3,and ammonium as NH+4) were much higher than those of other water-soluble inorganic ions,with average values of( 8. 70 ±5. 66),( 2. 04 ± 1. 07),and( 3. 25 ± 2. 29) μg·m-3,respectively. Based on long-term intensive observations,combined with the analysis of back trajectory and fire spots observations,it was revealed that regional transport and stable synoptic conditions both play important roles in controlling the variations in aerosol chemical components. During the transition from clean to hazy days,the EC and POC fractions showed no obvious variation; in contrast,the SOC fraction decreased obviously. Unlike for SOAs,relative contributions of sulfate and ammonia to PM_(2.5) increased during hazy days,suggesting enhanced chemical production via other pathways for these two secondary inorganic ions,probably through heterogeneous reactions.
PM_(2.5) samples were collected at a background site of the Yangtze River Delta in China,during summertime,of which the carbonaceous components,i. e.,OC and EC,and water-soluble inorganic ions,including sulfate,nitrate,and ammonium,were quantified. The average concentrations of OC and EC in PM_(2.5) during summer at Lin'an were( 14. 3 ± 3. 95) μg·m-3 and( 3. 33 ±1. 47) μg·m-3,respectively. Compared to an urban site,the correlation between OC and EC during summertime in Lin'an,which was a rural site,was relatively weak( R2= 0. 31,P < 0. 01). The concentrations of secondary inorganic aerosols( sulfate as SO_4~(2-),nitrate as NO-3,and ammonium as NH+4) were much higher than those of other water-soluble inorganic ions,with average values of( 8. 70 ±5. 66),( 2. 04 ± 1. 07),and( 3. 25 ± 2. 29) μg·m-3,respectively. Based on long-term intensive observations,combined with the analysis of back trajectory and fire spots observations,it was revealed that regional transport and stable synoptic conditions both play important roles in controlling the variations in aerosol chemical components. During the transition from clean to hazy days,the EC and POC fractions showed no obvious variation; in contrast,the SOC fraction decreased obviously. Unlike for SOAs,relative contributions of sulfate and ammonia to PM_(2.5) increased during hazy days,suggesting enhanced chemical production via other pathways for these two secondary inorganic ions,probably through heterogeneous reactions.
引文
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[2]牛彧文,顾骏强,浦静姣,等.浙江城市区域灰霾天气的长期变化[J].热带气象学报,2010,26(6):807-812.Niu Y W,Gu J Q,Pu J J,et al.The long-term variation of haze weather in urban areas of Zhejiang[J].Journal of Tropical Meteorology,2010,26(6):807-812.
[3]穆泉,张世秋.2013年1月中国大面积雾霾事件直接社会经济损失评估[J].中国环境科学,2013,33(11):2087-2094.Mu Q,Zhang S Q.An evaluation of the economic loss due to the heavy haze during January 2013 in China[J].China Environmental Science,2013,33(11):2087-2094.
[4]Lelieveld J,Evans J S,Fnais M,et al.The contribution of outdoor air pollution sources to premature mortality on a global scale[J].Nature,2015,525(7569):367-371.
[5]刘丹,解强,张鑫,等.北京冬季雾霾频发期VOCs源解析及健康风险评价[J].环境科学,2016,37(10):3693-3701.Liu D,Xie Q,Zhang X,et al.Source apportionment and health risk assessment of VOCs during the haze period in the winter in Beijing[J].Environmental Science,2016,37(10):3693-3701.
[6]谢元博,陈娟,李巍.雾霾重污染期间北京居民对高浓度PM2.5持续暴露的健康风险及其损害价值评估[J].环境科学,2014,35(1):1-8.Xie Y B,Chen J,Li W.An assessment of PM2.5related health risks and impaired values of Beijing residents in a consecutive high-level exposure during heavy haze days[J].Environmental Science,2014,35(1):1-8.
[7]薛国强,朱彬,王红磊.南京市大气颗粒物中水溶性离子的粒径分布和来源解析[J].环境科学,2014,35(5):1633-1643.Xue G Q,Zhu B,Wang H L.Size distributions and source apportionment of soluble ions in aerosol in Nanjing[J].Environmental Science,2014,35(5):1633-1643.
[8]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.
[9]Tan J H,Duan J C,He K B,et al.Chemical characteristics of PM2.5during a typical haze episode in Guangzhou[J].Journal of Environmental Sciences,2009,21(6):774-781.
[10]Huang K,Zhuang G,Lin Y,et al.Typical types and formation mechanisms of haze in an Eastern Asia megacity,Shanghai[J].Atmospheric Chemistry and Physics,2012,12(1):105-124.
[11]Sun Y L,Zhuang G S,Tang A H,et al.Chemical characteristics of PM2.5and PM10in haze-fog episodes in Beijing[J].Environmental Science&Technology,2006,40(10):3148-3155.
[12]Fang S X,Zhou L X,Tans P P,et al.In situ measurement of atmospheric CO2at the four WMO/GAW stations in China[J].Atmospheric Chemistry and Physics,2014,14(5):2541-2554.
[13]Tang J,Wang M L,Cheng H B,et al.Variation characteristics of ambient NMHCs at Shangdianzi and Lin'an regional GAW sites[J].Acta Meteorologica Sinica,2007,21(3):334-341.
[14]Xu X B,Lin W L,Wang T,et al.Long-term trend of surface ozone at a regional background station in eastern China 1991-2006:enhanced variability[J].Atmospheric Chemistry and Physics,2008,8(10):2595-2607.
[15]Zhang L,Sun J Y,Shen X J,et al.Observations of relative humidity effects on aerosol light scattering in the Yangtze River Delta of China[J].Atmospheric Chemistry and Physics,2015,15(14):8439-8454.
[16]Feng J L,Hu J C,Xu B H,et al.Characteristics and seasonal variation of organic matter in PM2.5at a regional background site of the Yangtze River Delta region,China[J].Atmospheric Environment,2015,123:288-297.
[17]颜鹏,张养梅,杨东贞,等.2003年夏季临安地区大气气溶胶离子成分的尺度分布特征[J].气象学报,2005,63(6):980-987.Yan P,Zhang Y M,Yang D Z,et al.The characteristics of aerosol ionic size distributions at Lin'an in summer of 2003[J].Acta Meteorologica Sinica,2005,63(6):980-987.
[18]徐宏辉,刘洁,王跃思,等.临安本底站大气气溶胶水溶性离子浓度变化特征[J].环境化学,2012,31(6):796-802.Xu H H,Liu J,Wang Y S,et al.Variation pattern of watersoluble ions in atmospheric at Lin'an regional background station[J].Environmental Chemistry,2012,31(6):796-802.
[19]沈利娟,王红磊,李莉,等.嘉兴市春季一次持续雾霾过程中气象条件与污染物变化特征分析[J].环境科学,2016,37(8):2871-2880.Shen L J,Wang H L,Li L,et al.Observation analysis on the characteristics of meteorological elements and pollutants during a continuous fog and haze episode in spring in Jiaxing city[J].Environmental Science,2016,37(8):2871-2880.
[20]张养梅,颜鹏,杨东贞,等.临安大气气溶胶理化特性季节变化[J].应用气象学报,2007,18(5):635-644.Zhang Y M,Yan P,Yang D Z,et al.Seasonal physical and chemical features variation of ambient aerosol in Lin'an[J].Journal of Applied Meteorological Science,2007,18(5):635-644.
[21]Duan F K,He K B,Ma Y L,et al.Characteristics of carbonaceous aerosols in Beijing,China[J].Chemosphere,2005,60(3):355-364.
[22]Wang F W,Guo Z G,Lin T,et al.Seasonal variation of carbonaceous pollutants in PM2.5at an urban‘supersite’in Shanghai,China[J].Chemosphere,2016,146:238-244.
[23]Zhao M F,Qiao T,Huang Z S,et al.Comparison of ionic and carbonaceous compositions of PM2.5in 2009 and 2012 in Shanghai,China[J].Science of the Total Environment,2015,536:695-703.
[24]王杨君,董亚萍,冯加良,等.上海市PM2.5中含碳物质的特征和影响因素分析[J].环境科学,2010,31(8):1755-1761.Wang Y J,Dong Y P,Feng J L,et al.Characteristics and influencing factors of carbonaceous aerosols in PM2.5in Shanghai,China[J].Environmental Science,2010,31(8):1755-1761.
[25]Feng J L,Chan C K,Fang M,et al.Characteristics of organic matter in PM2.5in Shanghai[J].Chemosphere,2006,64(8):1393-1400.
[26]张懿华,王东方,赵倩彪,等.上海城区PM2.5中有机碳和元素碳变化特征及来源分析[J].环境科学,2014,35(9):3263-3270.Zhang Y H,Wang D F,Zhao Q B,et al.Characteristics and sources of organic carbon and elemental carbon in PM2.5in Shanghai urban area[J].Environmental Science,2014,35(9):3263-3270.
[27]Yang F M,Huang L,Duan F K,et al.Carbonaceous species in PM2.5at a pair of rural/urban sites in Beijing,2005-2008[J].Atmospheric Chemistry and Physics,2011,11(15):7893-7903.
[28]Lim H J,Turpin B J.Origins of primary and secondary organic aerosol in Atlanta:results of time-resolved measurements during the Atlanta supersite experiment[J].Environmental Science&Technology,2002,36(21):4489-4496.
[29]Lin N H,Tsay S C,Maring H B,et al.An overview of regional experiments on biomass burning aerosols and related pollutants in Southeast Asia:from BASE-ASIA and the Dongsha experiment to7-SEAS[J].Atmospheric Environment,2013,78:1-19.
[30]Hertwig D,Burgin L,Gan C,et al.Development and demonstration of a Lagrangian dispersion modeling system for realtime prediction of smoke haze pollution from biomass burning in Southeast Asia[J].Journal of Geophysical Research:Atmospheres,2015,120(24):12605-12630.
[31]Chuang M T,Lee C T,Chou C C K,et al.Aerosol transport from Chiang Mai,Thailand to Mt.Lulin,Taiwan-implication of aerosol aging during long-range transport[J].Atmospheric Environment,2016,137:101-112.
[32]Peltier R E,Hecobian A H,Weber R J,et al.Investigating the sources and atmospheric processing of fine particles from Asia and the Northwestern United States measured during INTEX B[J].Atmospheric Chemistry and Physics,2008,8(6):1835-1853.
[33]Chow J C,Watson J G,Lu Z Q,et al.Descriptive analysis of PM2.5and PM10at regionally representative locations during SJVAQS/AUSPEX[J].Atmospheric Environment,1996,30(12):2079-2112.
[34]Zhang Y H,Hu M,Zhong L J,et al.Regional integrated experiments on air quality over Pearl River Delta 2004(PRIDEPRD2004):overview[J].Atmospheric Environment,2008,42(25):6157-6173.
[35]邹嘉南,安俊琳,王红磊,等.亚青会期间南京污染气体与气溶胶中水溶性离子的分布特征[J].环境科学,2014,35(11):4044-4051.Zou J N,An J L,Wang H L,et al.Distribution characteristics of pollution gases and water soluble Ion in aerosol during the Asian Youth Games of Nanjing,China[J].Environmental Science,2014,35(11):4044-4051.
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