京津冀郊区站点秋冬季大气PM_(2.5)来源解析
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摘要
为了增进对京津冀地区大气PM_(2.5)来源情况的认识,于2014～2015年秋冬季在京津冀地区4个郊区站点进行了PM_(2.5)的采样,并用化学质量平衡模型(chemical mass balance model,CMB)进行了PM_(2.5)源解析工作.结果表明:二次颗粒物(36%～58%)、交通(8%～26%)、民用燃煤(8%～16%)和生物质燃烧(5%～16%)是京津冀郊区站点秋冬季PM_(2.5)的主要贡献源.其中,二次硝酸盐是大部分站点秋冬季PM_(2.5)的首要贡献源(11%～27%).不同污染程度的源解析显示,冬季各站点各污染源在重污染天的贡献变化趋势的同步性不如秋季明显,且秋季二次源在重污染天的贡献增加值(47. 2～115. 7μg·m~(-3))明显高于一次源(29. 5～43. 4μg·m~(-3)),但此现象在冬季不显著.对比北京市城区源解析结果,发现郊区燃煤总贡献率较为相似,但郊区燃煤源中多以民用燃煤为主,这说明对于京津冀城郊地区,控制民用燃煤源对PM_(2.5)污染控制有重要意义.
To identify the main sources of PM_(2.5) in Beijing-Tianjin-Hebei( BTH) region,PM_(2.5) samples were collected at four suburban sites in BTH region during autumn and winter in 2014-2015. Source apportionment of PM_(2.5) was conducted using the chemical mass balance model( CMB). It shows that the main sources of PM_(2.5) in autumn and winter were secondary aerosols( 36%-58%),traffic( 8%-26%),residential coal combustion( 8%-16%),and biomass burning( 5%-16%). Secondary nitrate was the most important source of PM_(2.5) at most sites during autumn and winter( 11%-27%). The source apportionment at different pollution levels indicates that the coherence of the increasing trend of different sources among the four sites were much more obvious in autumn than in winter. Also,the increasing contribution of secondary sources( 47. 2-115. 7 μg·m~(-3)) was much higher than that of primary sources( 29. 5-43. 4 μg·m~(-3)) in autumn,but such trend was not significant in winter. The total contribution of coal combustion at suburban sites was quite similar to that in urban sites,but in suburban areas residential coal combustion dominates the contribution from coal combustion. Thus,it is very necessary for suburban areas of the BTH region to control emissions from residential coal combustion.
To identify the main sources of PM_(2.5) in Beijing-Tianjin-Hebei( BTH) region,PM_(2.5) samples were collected at four suburban sites in BTH region during autumn and winter in 2014-2015. Source apportionment of PM_(2.5) was conducted using the chemical mass balance model( CMB). It shows that the main sources of PM_(2.5) in autumn and winter were secondary aerosols( 36%-58%),traffic( 8%-26%),residential coal combustion( 8%-16%),and biomass burning( 5%-16%). Secondary nitrate was the most important source of PM_(2.5) at most sites during autumn and winter( 11%-27%). The source apportionment at different pollution levels indicates that the coherence of the increasing trend of different sources among the four sites were much more obvious in autumn than in winter. Also,the increasing contribution of secondary sources( 47. 2-115. 7 μg·m~(-3)) was much higher than that of primary sources( 29. 5-43. 4 μg·m~(-3)) in autumn,but such trend was not significant in winter. The total contribution of coal combustion at suburban sites was quite similar to that in urban sites,but in suburban areas residential coal combustion dominates the contribution from coal combustion. Thus,it is very necessary for suburban areas of the BTH region to control emissions from residential coal combustion.
引文
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[29]李松,郎建垒,程水源,等.典型固定燃烧源颗粒物成分谱特征研究[J].安全与环境学报,2016,16(5):312-319.Li S,Lang J L,Cheng S Y,et al.Analysis of the profiles'characteristic features of the particulate matters in regard to the stationary coal combustion sources[J].Journal of Safety and Environment,2016,16(5):312-319.
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[32]Zhu W H,Xu X D,Zheng J,et al.The characteristics of abnormal wintertime pollution events in the Jing-Jin-Ji region and its relationships with meteorological factors[J].Science of the Total Environment,2018,626:887-898.
[33]Cai S Y,Li Q,Wang S X,et al.Pollutant emissions from residential combustion and reduction strategies estimated via a village-based emission inventory in Beijing[J].Environmental Pollution,2018,238:230-237.
[34]National Aeronautics and Space Administration.Fire information for resource management system[DB/OL].https://firms.modaps.eosdis.nasa.gov/map,2018-09-03.
[35]王琴,刘保献,张大伟,等.北京市大气VOCs的时空分布特征及化学反应活性[J].中国环境科学,2017,37(10):3636-3646.Wang Q,Liu B X,Zhang D W,et al.Temporal and spatial distribution of VOCs and their role in chemical reactivity in Beijing[J].China Environmental Science,2017,37(10):3636-3646.
[36]Chang X,Wang S X,Zhao B,et al.Assessment of inter-city transport of particulate matter in the Beijing-Tianjin-Hebei region[J].Atmospheric Chemistry and Physics,2018,18(7):4843-4858.
[2]天津市环境保护局.2015天津市环境状况公报[R].天津:天津市环境保护局,2016.1-31.
[3]河北省环保厅.2015年河北省环境状况公报[R].河北:河北省环保厅,2016.1-33.
[4]高愈霄,霍晓芹,闫慧,等.京津冀区域大气重污染过程特征初步分析[J].中国环境监测,2016,32(6):26-35.Gao Y X,Huo X Q,Yan H,et al.Preliminary analysis on the characteristics of heavy air pollution events in Beijing-TianjinHebei region[J].Environmental Monitoring in China,2016,32(6):26-35.
[5]Zheng M,Salmon L G,Schauer J J,et al.Seasonal trends in PM2.5source contributions in Beijing,China[J].Atmospheric Environment,2005,39(22):3967-3976.
[6]Wang H L,Zhuang Y H,Wang Y,et al.Long-term monitoring and source apportionment of PM2.5/PM10in Beijing,China[J].Journal of Environmental Sciences,2008,20(11):1323-1327.
[7]Liu Z R,Hu B,Liu Q,et al.Source apportionment of urban fine particle number concentration during summertime in Beijing[J].Atmospheric Environment,2014,96:359-369.
[8]Yang H N,Chen J,Wen J J,et al.Composition and sources of PM2.5around the heating periods of 2013 and 2014 in Beijing:implications for efficient mitigation measures[J].Atmospheric Environment,2016,124:378-386.
[9]Wang J,Zhou M,Liu B S,et al.Characterization and source apportionment of size-segregated atmospheric particulate matter collected at ground level and from the urban canopy in Tianjin[J].Environmental Pollution,2016,219:982-992.
[10]杨妍妍,李金香,梁云平,等.应用受体模型(CMB)对北京市大气PM2.5来源的解析研究[J].环境科学学报,2015,35(9):2693-2700.Yang Y Y,Li J X,Liang Y P,et al.Source apportionment of PM2.5in Beijing by the chemical mass balance[J].Acta Scientiae Circumstantiae,2015,35(9):2693-2700.
[11]唐邈.天津市环境空气PM2.5来源解析[D].天津:南开大学,2014.1-80.
[12]Huang R J,Zhang Y L,Bozzetti C,et al.High secondary aerosol contribution to particulate pollution during haze events in China[J].Nature,2014,514(7521):218-222.
[13]王琴,张大伟,刘保献,等.基于PMF模型的北京市PM2.5来源的时空分布特征[J].中国环境科学,2015,35(10):2917-2924.Wang Q,Zhang D W,Liu B X,et al.Spatial and temporal variations of ambient PM2.5source contributions using positive matrix factorization[J].China Environmental Science,2015,35(10):2917-2924.
[14]Wang H L,Zhou Y M,Zhuang Y H,et al.Characterization of PM2.5/PM2.5-10and source tracking in the juncture belt between urban and rural areas of Beijing[J].Chinese Science Bulletin,2009,54(14):2506-2515.
[15]Watson J G,Chow J C,Lu Z Q,et al.Chemical mass balance source apportionment of PM10during the southern California air quality study[J].Aerosol Science and Technology,1994,21(1):1-36.
[16]Cai S Y,Wang Y J,Zhao B,et al.The impact of the“Air Pollution Prevention and Control Action Plan”on PM2.5concentrations in Jing-Jin-Ji region during 2012-2020[J].Science of the Total Environment,2017,580:197-209.
[17]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.
[18]马召辉,梁云平,张健,等.北京市典型排放源PM2.5成分谱研究[J].环境科学学报,2015,35(12):4043-4052.Ma Z H,Liang Y P,Zhang J,et al.PM2.5profiles of typical sources in Beijing[J].Acta Scientiae Circumstantiae,2015,35(12):4043-4052.
[19]郝吉明,段雷,易红宏,等.燃烧源可吸入颗粒物的物理化学特征[M].北京:科学出版社,2008.116-129.
[20]赵浩宁.黑色金属冶炼(钢铁)行业细颗粒物PM2.5排放特性及减排策略研究[D].北京:华北电力大学,2014.1-48.
[21]马京华.钢铁企业典型生产工艺颗粒物排放特征研究[D].重庆:西南大学,2009.1-47.
[22]孔少飞.大气污染源排放颗粒物组成、有害组分风险评价及清单构建研究[D].天津:南开大学,2012.1-346.
[23]Li X H,Wang S X,Duan L,et al.Particulate and trace gas emissions from open burning of wheat straw and corn Stover in China[J].Environmental Science&Technology,2007,41(17):6052-6058.
[24]US EPA.Speciate version 4.4[DB/OL].https://cfpub.epa.gov/speciate/,2014-03-20.
[25]王刚,郎建垒,程水源,等.重型柴油车PM2.5和碳氢化合物的排放特征[J].中国环境科学,2015,35(12):3581-3587.Wang G,Lang J L,Cheng S Y,et al.Characteristics of PM2.5and hydrocarbon emitted from heavy-duty diesel vehicle[J].China Environmental Science,2015,35(12):3581-3587.
[26]Wu B B,Shen X B,Cao X Y,et al.Characterization of the chemical composition of PM2.5emitted from on-road China III and China IV diesel trucks in Beijing,China[J].Science of the Total Environment,2016,551-552:579-589.
[27]Zhang Y Z,Yao Z L,Shen X B,et al.Chemical characterization of PM2.5emitted from on-road heavy-duty diesel trucks in China[J].Atmospheric Environment,2015,122:885-891.
[28]Chiang H L,Lai Y M,Chang S Y.Pollutant constituents of exhaust emitted from light-duty diesel vehicles[J].Atmospheric Environment,2012,47:399-406.
[29]李松,郎建垒,程水源,等.典型固定燃烧源颗粒物成分谱特征研究[J].安全与环境学报,2016,16(5):312-319.Li S,Lang J L,Cheng S Y,et al.Analysis of the profiles'characteristic features of the particulate matters in regard to the stationary coal combustion sources[J].Journal of Safety and Environment,2016,16(5):312-319.
[30]李海萍,赵颖,傅毅明.京津冀国家干线公路污染空间特征分析[J].环境科学学报,2016,36(10):3515-3526.Li H P,Zhao Y,Fu Y M.Spatial distribution of air pollutant emissions from national trunk highway in Beijing-Tianjin-Hebei(BTH)[J].Acta Scientiae Circumstantiae,2016,36(10):3515-3526.
[31]Watson J G,Chow J C,Chen L W A,et al.Particulate emission factors for mobile fossil fuel and biomass combustion sources[J].Science of the Total Environment,2011,409(12):2384-2396.
[32]Zhu W H,Xu X D,Zheng J,et al.The characteristics of abnormal wintertime pollution events in the Jing-Jin-Ji region and its relationships with meteorological factors[J].Science of the Total Environment,2018,626:887-898.
[33]Cai S Y,Li Q,Wang S X,et al.Pollutant emissions from residential combustion and reduction strategies estimated via a village-based emission inventory in Beijing[J].Environmental Pollution,2018,238:230-237.
[34]National Aeronautics and Space Administration.Fire information for resource management system[DB/OL].https://firms.modaps.eosdis.nasa.gov/map,2018-09-03.
[35]王琴,刘保献,张大伟,等.北京市大气VOCs的时空分布特征及化学反应活性[J].中国环境科学,2017,37(10):3636-3646.Wang Q,Liu B X,Zhang D W,et al.Temporal and spatial distribution of VOCs and their role in chemical reactivity in Beijing[J].China Environmental Science,2017,37(10):3636-3646.
[36]Chang X,Wang S X,Zhao B,et al.Assessment of inter-city transport of particulate matter in the Beijing-Tianjin-Hebei region[J].Atmospheric Chemistry and Physics,2018,18(7):4843-4858.