基于PMF和Pb同位素的农田土壤中重金属分布及来源解析
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摘要
为阐明九龙江中下游沿岸农田土壤中重金属分布特征、污染现状及来源,测定了该区域土壤中Cr、Ni、Cu、Zn、As、Cd、Pb的含量及Pb同位素比值。结果显示研究区域过去20年土壤中重金属含量呈现上升趋势,其中Cd增长幅度最大;空间上,除Cd外,不同功能区组间重金属差异显著,反映出研究区域受到了人为活动的显著影响,高Cd浓度现象可能是农业污染造成的一种普遍的共有现象;潜在危害指数评价法显示该区域大部分站点属于中等生态风险区域,主要贡献因子为Cd;主成分分析法(PCA)和正定矩阵因子分析法(PMF)分析结果均显示土壤重金属主要来自5种污染源,PMF法得出这些污染源的贡献率大小依次为工业源(26.3%)>交通源(23.2%)>自然源(22.0%)>农业源(16.2%)>其他混合源(12.0%);三端源混合模型结合Pb同位素示踪法得到交通源、燃煤和工业源对九龙江土壤中重金属Pb的贡献率分别为57%、34%和9%。三种源解析方法所得结果吻合,三者均能较好地解析土壤中重金属,可以构成互补的多元源解析体系。
To identify the distribution characteristics, pollution status, and pollution sources of heavy metals in farmland soils of the Jiulong River Watershed, the concentrations of Cr, Ni, Cu, Zn, As, Cd, and Pb, along with the lead isotope ratios in the soils, were measured. The results showed that the concentrations of heavy metals in the soils have increased significantly in the studied region over the past two decades. Among all the heavy metals, the rate of increase in concentration was largest for Cd. Pronounced spatial gradients were observed in the concentrations of soil heavy metals at different functional areas, thereby indicating that human activities have important effects on soils in the Jiulong River Watershed. High concentrations of soil Cd associated with agricultural pollution were observed at all stations. The results of the potential hazard index assessment indicated that most studied areas were moderate ecological risk zones, with Cd being the major contributing factor. Principal component analysis(PCA)and positive matrix factorization(PMF)revealed five primary factors(pollution sources)with the following contribution rates:industrial emissions(26.3%), vehicle emissions(23.2%), natural sources(22.0%), agricultural activities(16.2%), and other mixed sources(12.0%). The results of the Pb isotopic mixing model demonstrated that Pb mainly originated from vehicle exhaust(57%), coal combustion(34%), and industrial emissions(9%). The results of the three methods used for source apportionment were in good agreement. Thus, these methods can be used complimentarily to effectively constrain heavy metals pollution sources.
To identify the distribution characteristics, pollution status, and pollution sources of heavy metals in farmland soils of the Jiulong River Watershed, the concentrations of Cr, Ni, Cu, Zn, As, Cd, and Pb, along with the lead isotope ratios in the soils, were measured. The results showed that the concentrations of heavy metals in the soils have increased significantly in the studied region over the past two decades. Among all the heavy metals, the rate of increase in concentration was largest for Cd. Pronounced spatial gradients were observed in the concentrations of soil heavy metals at different functional areas, thereby indicating that human activities have important effects on soils in the Jiulong River Watershed. High concentrations of soil Cd associated with agricultural pollution were observed at all stations. The results of the potential hazard index assessment indicated that most studied areas were moderate ecological risk zones, with Cd being the major contributing factor. Principal component analysis(PCA)and positive matrix factorization(PMF)revealed five primary factors(pollution sources)with the following contribution rates:industrial emissions(26.3%), vehicle emissions(23.2%), natural sources(22.0%), agricultural activities(16.2%), and other mixed sources(12.0%). The results of the Pb isotopic mixing model demonstrated that Pb mainly originated from vehicle exhaust(57%), coal combustion(34%), and industrial emissions(9%). The results of the three methods used for source apportionment were in good agreement. Thus, these methods can be used complimentarily to effectively constrain heavy metals pollution sources.
引文
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[23]贾丽敏,陈秀玲,吕敏.漳州市不同绿地功能区土壤重金属污染特征及评价[J].城市环境与城市生态,2013,26(3):7-11.JIA Li-min,CHEN Xiu-ling,LüMin.Heavy metal contamination of soils and its evaluation in different greenbelt regions of Zhangzhou City[J].Urban Environment&Urban Ecology,2013,26(3):7-11.
[24]Lv J S,Liu Y,Zhang Z L,et al.Assessing heavy metals contamination in soils undergoing recent 10 years rapid urbanization:A case of Dongang,Eastern China[J].Environmental Science and Pollution Research,2015,22(14):10539-10550.
[25]Chen J M,Tan M G,Li Y L,et al.A lead isotope record of Shanghai atmospheric lead emissions in total suspended particles during the period of phasing out of leaded gasoline[J].Atmospheric Environment,2005,39:1245-1253.
[26]董辰寅,张卫国,王冠,等.上海宝山区城市土壤铅污染来源的同位素判别[J].环境科学,2012,33(3):754-758.DONG Chen-yin,ZHANG Wei-guo,WANG Guan,et al.Lead isotope signatures and source identification in urban soil of Baoshan District,Shanghai[J].China Environmental Science,2012,33(3):754-758.
[27]于瑞莲,胡恭任,林燕萍,等.泉州市不同功能区土壤铅同位素组成及其来源分析[J].环境科学学报,2013,33(7):1996-2003.YU Rui-lian,HU Gong-ren,LIN Yan-ping,et al.Lead isotope signatures and source identification in urban soils from different functional areas of Quanzhou City[J].Acta Scientiae Circumstantiae,2013,33(7):1996-2003.
[28]漳州市人民政府.2013漳州规模工业总产值及增加值增速居全省第二[EB/OL].[2014-02-23].http://www.fujian.gov.cn/zwgk/zfgzdt/sxdt/zz/201402/t20140223_700372.htm.Zhangzhou Municipal People's government.Zhangzhou scale industrial gross output value and added value growth rate ranks second in Fujian Province in 2013.[EB/OL].[2014-02-23].http://www.fujian.gov.cn/zwgk/zfgzdt/sxdt/zz/201402/t20140223_700372.htm.
[29]Walraven N,van Os B J H,Klaver G T,et al.The lead(Pb)isotope signature,behaviour and fate of traffic-related lead pollution in roadside soils in The Netherlands[J].Science of the Total Environment,2014,472:888-900.
[30]Cheng H F,Hu Y N.Lead(Pb)isotopic fingerprinting and its applications in lead pollution studies in China:A review[J].Environmental Pollution,2010,158:1134-1146.
[31]Zhu L M,Tang J W,Lee B.Lead concentrations and isotopes in aerosols from Xiamen,China[J].Marine Pollution Bulletin,2010,60(11):1946-1955.
[32]陶志红.漳州市机动车尾气污染状况与防治[J].漳州职业技术学院学报,2010,12(1):22-24.TAO Zhi-hong.Vehicle exhaust pollution and control in the Zhangzhou City[J].Journal of Zhangzhou Institute of Technology,2010,12(1):22-24.1035
[2]Wuana R A,Okieimen F E.Heavy metals in contaminated soils:A review of sources,chemistry,risks and best available strategies for reme-385diation[J].ISRN Ecology,2011:1-21.doi:10.5402/2011/402647
[3]Nicholson F A,Smith S R,Alloway B J,et al.An inventory of heavy metal input to agricultural soil in England and Wales[J].Science of the Total Environment,2003,311(1/2/3):205-219.
[4]Wei B G,Yang L S.A review of heavy metal contaminations in urban soils,urban road dusts and agricultural soils from China[J].Microchemical Journal,2010,94(2):99-107.
[5]Teng Y G,Wu J,Lu S J,et al.Soil and soil environmental quality monitoring in China:A review[J].Environment International,2014,69:177-199.
[6]Khillare P S,Hasan A,Sarkar S.Accumulation and risks of polycyclic aromatic hydrocarbons and trace metals in tropical urban soils[J].Environmental Monitoring and Assessment,2014,186(5):2907-2923.
[7]Hamel S C,Ellickson K M,Lioy P J.The estimation of the bioaccessibility of heavy metals in soils using artificial biofluids by two novel methods:Mass-balance and soil recapture[J].Science of the Total Environment,1999,s243-244(3):273-283.
[8]Liang J,Zeng G,Gao X,et al.Spatial distribution and source identification of heavy metals in surface soils in a typical coal mine city,Lianyuan,China[J].Environmental Pollution,2017,225:681-690.
[9]Kumar M,Furumai H,Kurisu F,et al.Tracing source and distribution of heavy metals in road dust,soil and soakaway sediment through speciation and isotopic fingerprinting[J].Geoderma,2013,s211-212(6):8-17.
[10]Ofelia M B,María T R,Elizabeth H A.Lead isotopes as tracers of anthropogenic pollution in urban topsoils of Mexico City[J].Chemie der Erde,2011,71:189-195.
[11]Liu X,Wu J,Xu J.Characterizing the risk assessment of heavy metals and sampling uncertainty analysis in paddy field by geostatistics and GIS[J].Environmental Pollution,2006,141(2):257-264.
[12]宋志廷,赵玉杰,周其文,等.基于地质统计及随机模拟技术的天津武清区土壤重金属源解析[J].环境科学,2016,37(7):2756-2762.SONG Zhi-ting,ZHAO Yu-jie,ZHOU Qi-wen,et al.Applications of geostatistical analyses and stochastic model to identify sources of soil heavy metals in Wuqing District,Tianjin,China[J].Environmental Science,2016,37(7):2756-2762.
[13]董騄睿,胡文友,黄标.基于正定矩阵因子分析模型的城郊农田土壤重金属源解析[J].中国环境科学,2015,35(7):2103-2111.DONG Lu-rui,HU Wen-you,HUANG Biao,et al.Source appointment of heavy metals in suburban farmland soils based on positive matrix factorization[J].China Environmental Science,2015,35(7):2103-2111.
[14]黄金良,李青生,洪华生,等.九龙江流域土地利用/景观格局-水质的初步关联分析[J].环境科学,2011,32(1):64-71.HUANG Jin-liang,LI Qing-sheng,HONG Hua-sheng,et al.Preliminary study on linking use&landscape pattern and water quality in the Jiulong River watershed[J].Environmental Science,2011,32(1):64-71.
[15]陈锦芳,郑金玲,叶龙翔,等.ICP-MS测定PM2.5中痕量重金属及铅同位素[J].分析试验室,2014,33(4):399-403.20195PMFPb CHEN Jin-fang,ZHENG Jin-ling,YE Long-xiang,et al.Determination of trace heavy metals and lead isotopes in PM2.5 by inductively coupled plasma mass spectrometry[J].Analytical Laboratory,2014,33(4):399-403.
[16]Yuan G L,Sun T H,Han P,et al.Source identification and ecological risk assessment of heavy metals in topsoil using environmental geochemical mapping:Typical urban renewal area in Beijing,China[J].Journal of Geochemical Exploration,2014,136:40-47.
[17]张直,曹英兰,蔡超,等.基于GIS的菜园土壤重金属空间分布及其风险评价[J].安全与环境学报,2013,13(1):129-133.ZHANG Zhi,CAO Ying-lan,CAI Chao,et al.Spatial distribution and potential ecological risk evaluation of heavy metals in vegetable-growing soil based on GIS[J].Journal of Safety and Environment,2013,13(1):129-133.
[18]陈振金,陈春秀,刘用清,等.福建省土壤环境背景值研究[J].环境科学,1991,13(4):70-75.CHEN Zhen-jin,CHEN Chun-xiu,LIU Yong-qing,et al.Study on soil environmental background values in Fujian Province[J].China Environmental Science,1991,13(4):70-75.
[19]Hakanson L.An ecological risk index for aquatic pollution control:Asedimentological approach[J].Water Research,1980,14:975-1001.
[20]连玉武,卢昌义,曾文彬,等.九龙江流域土壤-蔬菜系统中重金属的迁移、分布、积累[J].厦门大学学报,1996,35(6):959-964.LIAN Yu-wu,LU Chang-yi,ZENG Wen-bin,et al.The distribution,translocation and accumulation of heavy metals from vegetable-soil system in the Jiulong-river Valley[J].Journal of Xiamen University(Natural Science),1996,35(6):959-964.
[21]乔胜英,李望成,何方,等.漳州市城市土壤重金属含量特征及控制因素[J].地球化学,2005,34(6):635-640.QIAO Sheng-ying,LI Wang-cheng,HE Fang,et al.Characteristics and controlling factors of heavy metal contents in urban soils in Zhangzhou City,Fujian Province[J].Geochimica,2005,34(6):635-640.
[22]Williams C H,David D J.The effect of superphosphate on the cadmium content of soils and plants[J].Australian Journal of Soil Research,1973,11:43-56.
[23]贾丽敏,陈秀玲,吕敏.漳州市不同绿地功能区土壤重金属污染特征及评价[J].城市环境与城市生态,2013,26(3):7-11.JIA Li-min,CHEN Xiu-ling,LüMin.Heavy metal contamination of soils and its evaluation in different greenbelt regions of Zhangzhou City[J].Urban Environment&Urban Ecology,2013,26(3):7-11.
[24]Lv J S,Liu Y,Zhang Z L,et al.Assessing heavy metals contamination in soils undergoing recent 10 years rapid urbanization:A case of Dongang,Eastern China[J].Environmental Science and Pollution Research,2015,22(14):10539-10550.
[25]Chen J M,Tan M G,Li Y L,et al.A lead isotope record of Shanghai atmospheric lead emissions in total suspended particles during the period of phasing out of leaded gasoline[J].Atmospheric Environment,2005,39:1245-1253.
[26]董辰寅,张卫国,王冠,等.上海宝山区城市土壤铅污染来源的同位素判别[J].环境科学,2012,33(3):754-758.DONG Chen-yin,ZHANG Wei-guo,WANG Guan,et al.Lead isotope signatures and source identification in urban soil of Baoshan District,Shanghai[J].China Environmental Science,2012,33(3):754-758.
[27]于瑞莲,胡恭任,林燕萍,等.泉州市不同功能区土壤铅同位素组成及其来源分析[J].环境科学学报,2013,33(7):1996-2003.YU Rui-lian,HU Gong-ren,LIN Yan-ping,et al.Lead isotope signatures and source identification in urban soils from different functional areas of Quanzhou City[J].Acta Scientiae Circumstantiae,2013,33(7):1996-2003.
[28]漳州市人民政府.2013漳州规模工业总产值及增加值增速居全省第二[EB/OL].[2014-02-23].http://www.fujian.gov.cn/zwgk/zfgzdt/sxdt/zz/201402/t20140223_700372.htm.Zhangzhou Municipal People's government.Zhangzhou scale industrial gross output value and added value growth rate ranks second in Fujian Province in 2013.[EB/OL].[2014-02-23].http://www.fujian.gov.cn/zwgk/zfgzdt/sxdt/zz/201402/t20140223_700372.htm.
[29]Walraven N,van Os B J H,Klaver G T,et al.The lead(Pb)isotope signature,behaviour and fate of traffic-related lead pollution in roadside soils in The Netherlands[J].Science of the Total Environment,2014,472:888-900.
[30]Cheng H F,Hu Y N.Lead(Pb)isotopic fingerprinting and its applications in lead pollution studies in China:A review[J].Environmental Pollution,2010,158:1134-1146.
[31]Zhu L M,Tang J W,Lee B.Lead concentrations and isotopes in aerosols from Xiamen,China[J].Marine Pollution Bulletin,2010,60(11):1946-1955.
[32]陶志红.漳州市机动车尾气污染状况与防治[J].漳州职业技术学院学报,2010,12(1):22-24.TAO Zhi-hong.Vehicle exhaust pollution and control in the Zhangzhou City[J].Journal of Zhangzhou Institute of Technology,2010,12(1):22-24.1035