石家庄市大气PM_1、PM_(2.5)和PM_(10)中重金属元素分布特征及来源的对比研究
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摘要
为了解元素(尤其是重金属元素)在不同粒径大气颗粒物中的分布规律、污染特征及来源,于2016年在石家庄市采集PM_1、PM_(2.5)和PM_(10)样品。利用等离子体质谱仪(ICP-MS)测定了Al、Ti、V、Cr、Mn、Fe、Cu、Zn、As、Sb、Hg、Pb和Cd共13种元素的质量浓度,采用富集因子(EF)法分析各种元素在PM_1、PM_(2.5)和PM_(10)中的分布特征,并通过主成分分析法讨论了这些元素的主要来源。富集因子分析显示出Al、Fe、Ti、Mn受人为因素影响较少(EF<10),其他元素则出现显著至极强的人为影响,尤其是Cd元素(EF>103),并发现颗粒物粒径较小时,富集因子较大,即人为因素影响更重。主成分分析表明:PM_1中元素有工业冶炼及燃煤活动、机动车燃油排放、生活燃煤3个来源,PM_(2.5)中元素有地壳源、电厂及居民生活燃煤、金属冶炼等工业活动、机动车尾气4个来源,PM_(10)中元素有化石燃料燃烧和地壳源、与机动车相关的道路扬尘及工业尘、垃圾焚烧及机动车排放与磨损、燃煤活动4个来源。
In order to investigate the pollution characteristics and sources of chemicals(especially heavy metals)in atmospheric particles of different sizes,we collected PM_1,PM_(2.5) and PM_(10) samples from Shijiazhuang City in 2016.We determined the mass concentrations of 13 elements including Al,Ti,V,Cr,Mn,Fe,Cu,Zn,As,Sb,Hg,Pb and Cd by ICP-MS.We analyzed the distribution characteristics of these elements in PM_1,PM_(2.5) and PM_(10) by the enrichment factor(EF)method,and discussed the main sources of these elements based on principal component analysis(PCA).The enrichment factor analysis showed that Al,Fe,Ti,and Mn were less influenced by human factors(EF<10),while other elements had significant to extremely strong human influences,especially Cd(EF>103).In addition,smaller particle size correlates with larger enrichment factor,indicating greater influence of human factors in small particles.Principal component analysis showed that there are three sources for the elements in PM_1 and four for PM_(2.5) or PM_(10).The sources are mainly related to industrial activities,fossil fuel combustion,motor vehicle exhaust and wear,and garbage burning.
In order to investigate the pollution characteristics and sources of chemicals(especially heavy metals)in atmospheric particles of different sizes,we collected PM_1,PM_(2.5) and PM_(10) samples from Shijiazhuang City in 2016.We determined the mass concentrations of 13 elements including Al,Ti,V,Cr,Mn,Fe,Cu,Zn,As,Sb,Hg,Pb and Cd by ICP-MS.We analyzed the distribution characteristics of these elements in PM_1,PM_(2.5) and PM_(10) by the enrichment factor(EF)method,and discussed the main sources of these elements based on principal component analysis(PCA).The enrichment factor analysis showed that Al,Fe,Ti,and Mn were less influenced by human factors(EF<10),while other elements had significant to extremely strong human influences,especially Cd(EF>103).In addition,smaller particle size correlates with larger enrichment factor,indicating greater influence of human factors in small particles.Principal component analysis showed that there are three sources for the elements in PM_1 and four for PM_(2.5) or PM_(10).The sources are mainly related to industrial activities,fossil fuel combustion,motor vehicle exhaust and wear,and garbage burning.
引文
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[22]张鉴达,周美玲,杨小雨,等.石家庄市冬季大气颗粒物中水溶性离子与重金属成分研究[J].河北工业科技,2017,34(6):202-207.
[23]张霖琳,高愈霄,刀谞,等.京津冀典型城市采暖季颗粒物浓度与元素分布特征[J].中国环境监测,2014,30(6):53-61.
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[27]姬亚芹,朱坦,冯银厂,等.用富集因子法评价我国城市土壤风沙尘元素的污染[J].南开大学学报(自然科学版),2006,39(2):94-99.
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[29]迟清华,鄢明才.应用地球化学:元素丰度数据手册[M].北京:地质出版社,2007:82.
[30]戴树桂.环境化学[M].2版.北京:高等教育出版社,2006:140.
[31]RIZZIO E,GIAVERI G,ARGINELLI D,et al.Trace elements total content and particle sizes distribution in the air particulate matter of a rural residential area in North Italy investigated by neutron activation analysis[J].Science of the Total Environment,1999,226:47-56.
[32]MOHANRAL R,AZEEZ PA,PRISCILLA T,et al.Heavy metals in airborne particulate matter of urban Coimbatore[J].Environmental Contamination and Toxicology,2004,47B:162-167.
[33]宋少洁,吴烨,蒋靖坤,等.北京市典型道路交通环境细颗粒物元素组成及分布特征[J].环境科学学报,2012,32(1):66-73.
[34]NIKOLAOS S.THOMAIDIS E,PANAYOTIS A S.Characterization of lead,cadmium,arsenic and nickel in PM2.5particles in the Athens atmosphere[J].Greece Chemosphere,2003,52(1):959-966.
[35]周雪明,郑乃嘉,李英红,等.2011-2012北京大气PM2.5中重金属的污染特征与来源分析[J].环境科学,2017,38(10):4054-4060.
[36]谭吉华,段菁春.中国大气颗粒物重金属污染、来源及控制建议[J].中国科学院研究生院学报,2013,30(2):145-155.
[37]TIAN H,CHENG K,WANG Y,et al.Temporal and spatial variation characteristics of atmospheric emissions of Cd,Cr,and Pb from coal in China[J].Atmospheric Environment,2012,50:157-163.
[38]杨怀金,杨德容,叶芝祥,等.成都西南郊区春季PM2.5中元素特征及重金属潜在生态风险评价[J].环境科学,2016,37(12):4490-4503.
[39]HUANG S,TU J,LIU H,et al.Multivariate analysis of trace element concentrations in atmospheric deposition in the Yangtze River Delta,East China[J].Atmospheric Environment,2009,43(36):5781-5790.
[40]占长林,张家泉,郑敬茹,等.鄂东典型工业城市大气PM10中元素浓度特征和来源分析[J].环境科学,2017,38(11):4464-4468.
[41]RISTOVSKI Z D,MORAWSKA L,BOFINGER N D,et al.Submicrometer and supermicrometer particulate emission from sparkignition vehicles[J].Environmental Science and Technology,1998,32(24):3845-3852.
[42]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.
[43]VU T V,DELGADO-SABORIT J M,HARRISON R M.Review:particle number size distributions from seven major sources and implications for source apportionment studies[J].Atmospheric Environment,2015,122:114-132.
[44]SEAMES W S.An initial study of the fine fragmentation fly ash particle mode generated during pulverized coal combustion[J].Fuel Processing Technology,2003,812:109-125.
[45]HJORTENKRANS DS T,BERGBACK B G,HAGGERUDA V.Metal emissions from brake linings and tires:case studies of Stockholm,Sweden 1995/1998and 2005[J].Environmental Science and Technology,2007,41(15):5224-5230.
[46]郝玉,徐宏勇,柏舸,等.垃圾焚烧飞灰中Cd、Pb、Zn的螯合稳定与水泥固化处理[J].环境工程学报,2018,12(8):2357-2362.
[47]李建陶,曾鸣.生活垃圾焚烧飞灰矿物学特性及重金属分布[J].环境科学,2018,39(10):1-10.
[2]SATO K,TAMURA T,FURUTA N.Partitioning between soluble and insoluble fractions of major and trace elements in size-classified airborne particulate matter collected in Tokyo[J].Journal of Environmental Monitoring,2008,10(2):211-218.
[3]杨复沫,贺克斌,马永亮,等.北京大气PM2.5中微量元素的浓度变化特征与来源[J].环境科学,2003,24(6):33-37.
[4]戴塔根,罗莹华,梁凯.重金属在不同粒径PM10中的含量与形态[J].地球科学与环境学报,200,28(4):87-91.
[5]谢华林,张萍,贺惠,等.大气颗粒物中重金属元素在不同粒径上的形态分布[J].环境工程,2002,20(6):55-57.
[6]方凤满.中国大气颗粒物中金属元素环境地球化学行为研究[J].生态环境学报,2010,19(4):979-984.
[7]CHOI J,FUENTES M,REICH B J.Spatial-temporal association between fine particulate matter and daily mortality[J].Computational Statistics and Data Analysis,2009,53(8):2989-3000.
[8]洪也,周德平,马雁军,等.沈阳市夏秋季节大气细颗粒物元素浓度及分布特征[J].中国环境科学,2010,30(7):972-979.
[9]伊丽米热·阿布达力木,迪丽努尔·塔力甫,阿布力孜·依米提.乌鲁木齐市大气颗粒物中的重金属浓度的分布特征[J].环境科学与技术,2012,35(8):107-111.
[10]王红斌,陈杰,刘鹤,等.西安市夏季空气颗粒物污染特征及来源分析[J].气候与环境研究,2000,5(1):51-57.
[11]刘齐,熊莎莎,刘文军.柳州市空气可吸入颗粒物中重金属污染特征分析[J].环境科学导刊,2012,31(1):76-79.
[12]李德禄,张元勋,李爱国,等.冬季上海吴淞地区大气颗粒物PM10的元素主成分分析[J].核技术,2005,2:109-112.
[13]杨勇杰,王跃思,温天雪,等.采暖期开始前后北京大气颗粒物中化学元素特征及来源[J].环境科学,2008,29(11):3275-3279.
[14]郭璇华,高瑞英,黄瑞毅,等.大气颗粒物中无机元素特性的研究[J].环境科学与技术,2006,29(6):49-51.
[15]李凤英,彭琴,杨孟,等.南京市北郊冬季大气颗粒物中重金属污染研究[J].环境科学与技术,2017,40(7):173-179.
[16]张恒,周自强,赵海燕,等.青奥会前后南京PM2.5重金属污染水平与健康风险评估[J].环境科学,2016,37(1):28-34.
[17]CYRYS J,STOLZEL M,HEINRICH J,et al.Elemental composition and sources of fine and ultrafine ambient particles in Erurt,Germany[J].Science of the Total Environment,2003,305(1/2/3):143-156.
[18]HSU S C,LIU S C,JENG W L,et al.Variations of Cd/Pb and Zn/Pb ratios in Taipei aerosols reflecting long-range transport or local pollution emissions[J].Science of the Total Environment,2005,347:111-121.
[19]张志刚.鞍山市环境空气颗粒物中重金属元素分布特征[J].中国环境监测,2009,25(5):103-106.
[20]环境保护部.环境空气PM10和PM2.5的测定重量法(HJ 618-2011)[S].北京:中国标准出版社,2011.
[21]段二红,张微微,李璇,等.石家庄市采暖期大气细颗粒物中PAHs污染特征[J].环境科学研究,2017,30(2):193-201.
[22]张鉴达,周美玲,杨小雨,等.石家庄市冬季大气颗粒物中水溶性离子与重金属成分研究[J].河北工业科技,2017,34(6):202-207.
[23]张霖琳,高愈霄,刀谞,等.京津冀典型城市采暖季颗粒物浓度与元素分布特征[J].中国环境监测,2014,30(6):53-61.
[24]环境保护部,国家质量检验检疫总局.环境空气质量标准(GB 3095-2012)[S].北京:中国环境科学出版社,2012.
[25]BILO C,COLOMBO J C,SKORUPKA C N,et al.Sources distribution and variability of airborne trace metals in La Plata City area,Argentina[J].Environmental Pollution,2001,111(1):149-158.
[26]WAKED A,FAVE O,ALLEMAN L Y,et al.Source apportionment of PM10in a north-western Europe regional urban background site(Lens,France)using positive matrix factorization and including primary biogenic emissions[J].Atmospheric Chemistry and Physics,2014,14(7):3325-3346.
[27]姬亚芹,朱坦,冯银厂,等.用富集因子法评价我国城市土壤风沙尘元素的污染[J].南开大学学报(自然科学版),2006,39(2):94-99.
[28]中国环境监测总站.中国土壤元素背景值[M].北京:中国环境科学出版社,1990:1-501.
[29]迟清华,鄢明才.应用地球化学:元素丰度数据手册[M].北京:地质出版社,2007:82.
[30]戴树桂.环境化学[M].2版.北京:高等教育出版社,2006:140.
[31]RIZZIO E,GIAVERI G,ARGINELLI D,et al.Trace elements total content and particle sizes distribution in the air particulate matter of a rural residential area in North Italy investigated by neutron activation analysis[J].Science of the Total Environment,1999,226:47-56.
[32]MOHANRAL R,AZEEZ PA,PRISCILLA T,et al.Heavy metals in airborne particulate matter of urban Coimbatore[J].Environmental Contamination and Toxicology,2004,47B:162-167.
[33]宋少洁,吴烨,蒋靖坤,等.北京市典型道路交通环境细颗粒物元素组成及分布特征[J].环境科学学报,2012,32(1):66-73.
[34]NIKOLAOS S.THOMAIDIS E,PANAYOTIS A S.Characterization of lead,cadmium,arsenic and nickel in PM2.5particles in the Athens atmosphere[J].Greece Chemosphere,2003,52(1):959-966.
[35]周雪明,郑乃嘉,李英红,等.2011-2012北京大气PM2.5中重金属的污染特征与来源分析[J].环境科学,2017,38(10):4054-4060.
[36]谭吉华,段菁春.中国大气颗粒物重金属污染、来源及控制建议[J].中国科学院研究生院学报,2013,30(2):145-155.
[37]TIAN H,CHENG K,WANG Y,et al.Temporal and spatial variation characteristics of atmospheric emissions of Cd,Cr,and Pb from coal in China[J].Atmospheric Environment,2012,50:157-163.
[38]杨怀金,杨德容,叶芝祥,等.成都西南郊区春季PM2.5中元素特征及重金属潜在生态风险评价[J].环境科学,2016,37(12):4490-4503.
[39]HUANG S,TU J,LIU H,et al.Multivariate analysis of trace element concentrations in atmospheric deposition in the Yangtze River Delta,East China[J].Atmospheric Environment,2009,43(36):5781-5790.
[40]占长林,张家泉,郑敬茹,等.鄂东典型工业城市大气PM10中元素浓度特征和来源分析[J].环境科学,2017,38(11):4464-4468.
[41]RISTOVSKI Z D,MORAWSKA L,BOFINGER N D,et al.Submicrometer and supermicrometer particulate emission from sparkignition vehicles[J].Environmental Science and Technology,1998,32(24):3845-3852.
[42]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.
[43]VU T V,DELGADO-SABORIT J M,HARRISON R M.Review:particle number size distributions from seven major sources and implications for source apportionment studies[J].Atmospheric Environment,2015,122:114-132.
[44]SEAMES W S.An initial study of the fine fragmentation fly ash particle mode generated during pulverized coal combustion[J].Fuel Processing Technology,2003,812:109-125.
[45]HJORTENKRANS DS T,BERGBACK B G,HAGGERUDA V.Metal emissions from brake linings and tires:case studies of Stockholm,Sweden 1995/1998and 2005[J].Environmental Science and Technology,2007,41(15):5224-5230.
[46]郝玉,徐宏勇,柏舸,等.垃圾焚烧飞灰中Cd、Pb、Zn的螯合稳定与水泥固化处理[J].环境工程学报,2018,12(8):2357-2362.
[47]李建陶,曾鸣.生活垃圾焚烧飞灰矿物学特性及重金属分布[J].环境科学,2018,39(10):1-10.
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