珠海市郊区大气PM_(2.5)中元素特征及重金属健康风险评价
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摘要
为探讨珠海市郊区大气环境PM_(2.5)中主要元素尤其是重金属的污染特征及其健康风险,于2014～2015年选取春、夏、秋、冬季4个典型月采集了PM_(2.5)样品.利用X射线荧光光谱法分析得到15种元素的含量,进一步利用富集因子和主成分分析方法分析其来源,并采用US EPA环境健康风险评价模型评估痕量重金属的健康风险.结果表明:大气PM_(2.5)中地壳元素(Al、Si、Ca、Fe、Ti)总质量浓度在春、夏、秋、冬季典型月分别为(708±213)、(645±269)、(1 155±503)和(1 466±492)ng·m~(-3),痕量重金属元素(Ba、Co、Cr、Cu、Mn、Ni、Pb、Sb、V、Zn)总质量浓度在春、夏、秋、冬典型月分别为(271±124)、(163±87. 6)、(424±192)和(546±183) ng·m~(-3).富集因子分析显示Sb、Zn、Pb、Cu、Ni、Ba、Ca、Co等元素富集显著,其富集因子均值范围为172～2 426.主成分分析显示,区域性输送污染源、船舶源、燃煤和电子工业是PM_(2.5)中重金属的主要来源,其贡献率分别为53. 4%、13. 0%、7. 6%和6. 8%.健康风险评价结果表明,Mn元素对儿童存在一定的非致癌风险,Cr、Pb和Co存在一定的致癌风险.
To investigate the characteristics,sources,and health risks of trace heavy metals in fine particles,PM_(2.5) samples were collected at a suburban site of Zhuhai in the Pearl River Delta Region. Fifteen elements in the PM_(2.5) were analyzed by an X-ray fluorescence method. The results showed that the total mass concentrations of crustal elements( Al,Si,Ca,Fe,and Ti) in a typical month during spring,summer,autumn,and winter were( 708 ± 213),( 645 ± 269),( 1 155 ± 503),and( 1 466 ± 492) ng·m~(-3),respectively,while the total mass concentrations of the rest of the trace elements( Ba,Co,Cr,Cu,Mn,Ni,Pb,Sb,V,and Zn)were( 271 ± 124),( 163 ± 87. 6),( 424 ± 192),and( 546 ± 183) ng·m~(-3),respectively. The element concentrations decreased in the following order: Si > Al > Fe > Zn > Ca > Pb > Ba > Mn > Sb > Cu > Ti > V > Ni > Cr > Co. Enrichment factors( EFs) analysis showed that Sb,Zn,Pb,Cu,Ni,Ba,Ca,and Co were heavily enriched,with EFs values ranging from 172 to 2426. Principal component analysis further showed that regional transport,ship emissions,coal combustion,and the electronics industry were the major sources of heavy metals,contributing 53. 4%,13%,7. 6%,and 6. 8% of the total,respectively. Health risk assessment results indicated that Mn may pose a non-carcinogenic risk to children,and Cr,Pb,and Co may pose cancer risks to humans.
To investigate the characteristics,sources,and health risks of trace heavy metals in fine particles,PM_(2.5) samples were collected at a suburban site of Zhuhai in the Pearl River Delta Region. Fifteen elements in the PM_(2.5) were analyzed by an X-ray fluorescence method. The results showed that the total mass concentrations of crustal elements( Al,Si,Ca,Fe,and Ti) in a typical month during spring,summer,autumn,and winter were( 708 ± 213),( 645 ± 269),( 1 155 ± 503),and( 1 466 ± 492) ng·m~(-3),respectively,while the total mass concentrations of the rest of the trace elements( Ba,Co,Cr,Cu,Mn,Ni,Pb,Sb,V,and Zn)were( 271 ± 124),( 163 ± 87. 6),( 424 ± 192),and( 546 ± 183) ng·m~(-3),respectively. The element concentrations decreased in the following order: Si > Al > Fe > Zn > Ca > Pb > Ba > Mn > Sb > Cu > Ti > V > Ni > Cr > Co. Enrichment factors( EFs) analysis showed that Sb,Zn,Pb,Cu,Ni,Ba,Ca,and Co were heavily enriched,with EFs values ranging from 172 to 2426. Principal component analysis further showed that regional transport,ship emissions,coal combustion,and the electronics industry were the major sources of heavy metals,contributing 53. 4%,13%,7. 6%,and 6. 8% of the total,respectively. Health risk assessment results indicated that Mn may pose a non-carcinogenic risk to children,and Cr,Pb,and Co may pose cancer risks to humans.
引文
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[29]郑元铸,葛琳琳,郑旭军,等.温州市区PM2. 5无机元素污染特征及来源分析[J].环境化学,2017,36(1):84-91.Zheng Y Z,Ge L L,Zheng X J,et al. Characteristics and source apportionment of inorganic elements in PM2. 5in Wenzhou,Zhejiang[J]. Environmental Chemistry,2017,36(1):84-91.
[30] Duce R A,Hoffman G L,Zoller W H. Atmospheric trace metals at remote northern and southern hemisphere sites:pollution or natural?[J]. Science,1975,187(4171):59-61.
[31] Tian H Z,Zhu C Y,Gao J J,et al. Quantitative assessment of atmospheric emissions of toxic heavy metals from anthropogenic sources in China:historical trend, spatial distribution,uncertainties,and control policies[J]. Atmospheric Chemistry and Physics,2015,15(17):10127-10147.
[32] Liang F,Zhang G L,Tan M G,et al. Lead in children's blood is mainly caused by coal-fired ash after phasing out of leaded gasoline in Shanghai[J]. Environmental Science&Technology,2010,44(12):4760-4765.
[33] Agrawal H, Welch W A, Miller J W, et al. Emission measurements from a crude oil tanker at sea[J]. Environmental Science&Technology,2008,42(19):7098-7103.
[34] Agrawal H,Eden R,Zhang X Q,et al. Primary particulate matter from ocean-going engines in the Southern California Air Basin[J]. Environmental Science&Technology,2009,43(14):5398-5402.
[35] Tian H Z,Zhao D,Cheng K,et al. Anthropogenic atmospheric emissions of antimony and its spatial distribution characteristics in China[J]. Environmental Science&Technology,2012,46(7):3973-3980.
[36] Cheng H G,Zhou T,Li Q,et al. Anthropogenic chromium emissions in china from 1990 to 2009[J]. PLo S One,2014,9(2):e87753.
[37] Zheng N,Liu J S,Wang Q C,et al. Heavy metals exposure of children from stairway and sidewalk dust in the smelting district,northeast of China[J]. Atmospheric Environment,2010,44(27):3239-3245.
[2] United States Environmental Protection Agency. The clean air act amendments of 1990 list of hazardous air pollutants[EB/OL].https://www3. epa. gov/airtoxics/orig189. html,2016-02-24.
[3] ATSDR(Agency for Toxic Substances and Disease Registry).Toxicological profiles information sheet[EB/OL]. https://www.atsdr. cdc. gov/toxprofiledocs/index. html,2018-10-11.
[4]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.Tan J H,Duan J C. Heavy metals in aerosol in China:pollution,sources, and control strategies[J]. Journal of Graduate University of Chinese Academy of Sciences,2013,30(2):145-155.
[5] Tao J,Zhang L M,Cao J J,et al. Source apportionment of PM2. 5at urban and suburban areas of the Pearl River Delta region,south China-With emphasis on ship emissions[J].Science of the Total Environment,2017,574:1559-1570.
[6] Chen P F,Bi X H,Zhang J Q,et al. Assessment of heavy metal pollution characteristics and human health risk of exposure to ambient PM2. 5in Tianjin,China[J]. Particuology,2015,20:104-109.
[7]景慧敏.北京可吸入颗粒物中元素地球化学特征与健康风险评价[D].北京:中国地质大学(北京),2015.
[8] Hu X,Zhang Y,Ding Z H,et al. Bioaccessibility and health risk of arsenic and heavy metals(Cd,Co,Cr,Cu,Ni,Pb,Zn and Mn)in TSP and PM2. 5in Nanjing,China[J]. Atmospheric Environment,2012,57:146-152.
[9]胡子梅,王军,陶征楷,等.上海市PM2. 5重金属污染水平与健康风险评价[J].环境科学学报,2013,33(12):3399-3406.Hu Z M,Wang J,Tao Z K,et al. Pollution level and health risk assessment of heavy metals in PM2. 5, Shanghai[J]. Acta Scientiae Circumstantiae,2013,33(12):3399-3406.
[10]李友平,刘慧芳,周洪,等.成都市PM2. 5中有毒重金属污染特征及健康风险评价[J].中国环境科学,2015,35(7):2225-2232.Li Y P,Liu H F,Zhou H,et al. Contamination characteristics and health risk assessment of toxic heavy metals in PM2. 5in Chengdu[J]. China Environmental Science,2015,35(7):2225-2232.
[11]赵金平,谭吉华,毕新慧,等.广州市灰霾期间大气颗粒物中无机元素的质量浓度[J].环境化学,2008,27(3):322-326.Zhao J P,Tan J H,Bi X H,et al. The mass concentrations of inorganic elements in atmospheric particles during haze period in Guangzhou[J]. Environmental Chemistry,2008,27(3):322-326.
[12]张洛红,范芳,蒋炜炜,等.珠三角地区大气PM2. 5中重金属污染水平及健康风险评价[J].环境科学学报,2017,37(1):370-380.Zhang L H,Fang F,Jiang W W,et al. Concentrations and health risk assessment of heavy metals in atmospheric PM2. 5in the Pearl River Delta Region[J]. Acta Scientiae Circumstantiae,2017,37(1):370-380.
[13]杜金花,张宜升,何凌燕,等.深圳某地区大气PM2. 5中重金属的污染特征及健康风险评价[J].环境与健康杂志,2012,29(9):838-840.
[14] Tan J H,Duan J C,Ma Y L,et al. Source of atmospheric heavy metals in winter in Foshan,China[J]. Science of the Total Environment,2014,493:262-270.
[15] Xu H M,Cao J J,Ho K F,et al. Lead concentrations in fine particulate matter after the phasing out of leaded gasoline in Xi'an,China[J]. Atmospheric Environment,2012,46:217-224.
[16] Tasdemir Y,Kural C,Cindoruk S S,et al. Assessment of trace element concentrations and their estimated dry deposition fluxes in an urban atmosphere[J]. Atmospheric Research,2006,81(1):17-35.
[17]虎彩娇,成海容,李锦伦,等.黄石市大气PM10和PM2. 5中元素特征及重金属生态风险评价[J].环境化学,2018,37(1):138-145.Hu C J,Cheng H R,Li M L,et al. Characteristics of elements and ecological risk assessment of heavy metals in PM10 and PM2. 5in Huangshi[J]. Environmental Chemistry,2018,37(1):138-145.
[18]国家环境保护局,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. 101-336.
[19] Veysseyre A,Moutard K,Ferrari C,et al. Heavy metals in fresh snow collected at different altitudes in the Chamonix and Maurienne valleys,French Alps:initial results[J]. Atmospheric Environment,2001,35(2):415-425.
[20] United States Environmental Protection Agency. Risk assessment guidance for Superfund. Volume I:Human health evaluation manual(part A)[R]. Washington DC:Office of Emergency and Remedial Response,U. S. Environmental Protection Agency,1989. 636-640.
[21]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,2006,28(4):87-91.Dai T G,Luo Y H,Liang K. Contents and form of heavy metal in PM10of different diameters[J]. Journal of Earth Sciences and Environment,2006,28(4):87-91.
[22] Krzyzanowski M. WHO air quality guidelines for Europe[J].Journal of Toxicology and Environmental Health,Part A:Current Issues,2008,71(1):47-50.
[23] Zhao M J,Zhang Y,Ma W C,et al. Characteristics and ship traffic source identification of air pollutants in China's largest port[J]. Atmospheric Environment,2013,64:277-286.
[24] Zhao P S,Dong F,He D,et al. Characteristics of concentrations and chemical compositions for PM2. 5in the region of Beijing,Tianjin,and Hebei,China[J]. Atmospheric Chemistry and Physics,2013,13(9):4631-4644.
[25] Wang J, Hu Z M, Chen Y Y, et al. Contamination characteristics and possible sources of PM10and PM2. 5in different functional areas of Shanghai,China[J]. Atmospheric Environment,2013,68:221-229.
[26] Zhang F,Wang Z W,Cheng H R,et al. Seasonal variations and chemical characteristics of PM2. 5in Wuhan,central China[J].Science of the Total Environment,2015,518-519:97-105.
[27]王珍.贵阳市大气颗粒物PM10、PM2. 5的来源解析研究[D].贵阳:贵州师范大学,2015. 12-27.
[28]陈刚,刘佳媛,皇甫延琦,等.合肥城区PM10及PM2. 5季节污染特征及来源解析[J].中国环境科学,2016,36(7):1938-1946.Chen G,Liu J Y,Huangfu Y Q,et al. Seasonal variations and source apportionment of ambient PM10and PM2. 5at urban area of Hefei,China[J]. China Environmental Science,2016,36(7):1938-1946.
[29]郑元铸,葛琳琳,郑旭军,等.温州市区PM2. 5无机元素污染特征及来源分析[J].环境化学,2017,36(1):84-91.Zheng Y Z,Ge L L,Zheng X J,et al. Characteristics and source apportionment of inorganic elements in PM2. 5in Wenzhou,Zhejiang[J]. Environmental Chemistry,2017,36(1):84-91.
[30] Duce R A,Hoffman G L,Zoller W H. Atmospheric trace metals at remote northern and southern hemisphere sites:pollution or natural?[J]. Science,1975,187(4171):59-61.
[31] Tian H Z,Zhu C Y,Gao J J,et al. Quantitative assessment of atmospheric emissions of toxic heavy metals from anthropogenic sources in China:historical trend, spatial distribution,uncertainties,and control policies[J]. Atmospheric Chemistry and Physics,2015,15(17):10127-10147.
[32] Liang F,Zhang G L,Tan M G,et al. Lead in children's blood is mainly caused by coal-fired ash after phasing out of leaded gasoline in Shanghai[J]. Environmental Science&Technology,2010,44(12):4760-4765.
[33] Agrawal H, Welch W A, Miller J W, et al. Emission measurements from a crude oil tanker at sea[J]. Environmental Science&Technology,2008,42(19):7098-7103.
[34] Agrawal H,Eden R,Zhang X Q,et al. Primary particulate matter from ocean-going engines in the Southern California Air Basin[J]. Environmental Science&Technology,2009,43(14):5398-5402.
[35] Tian H Z,Zhao D,Cheng K,et al. Anthropogenic atmospheric emissions of antimony and its spatial distribution characteristics in China[J]. Environmental Science&Technology,2012,46(7):3973-3980.
[36] Cheng H G,Zhou T,Li Q,et al. Anthropogenic chromium emissions in china from 1990 to 2009[J]. PLo S One,2014,9(2):e87753.
[37] Zheng N,Liu J S,Wang Q C,et al. Heavy metals exposure of children from stairway and sidewalk dust in the smelting district,northeast of China[J]. Atmospheric Environment,2010,44(27):3239-3245.
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