嘉陵江重庆段多环芳烃及溶解性有机质的污染特征及源解析
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摘要
多环芳烃（PAHs）是一类典型的持久性有机污染物，对生物有致癌、和致基因突变作用，其在环境中的分布和污染趋势近年来成为环境领域研究的热点。溶解性有机质(DOM)能与水体中的金属离子、化学农药和多环芳烃等相结合，进而影响到它们在水体的分布，降解及对水生生物的毒性，对水体生态系统和生物化学过程产生重要的影响。论文以嘉陵江重庆段为研究对象，主要针对嘉陵江重庆段PAHs和DOM的浓度分布、时空分布及来源解析等进行研究，这将有利于嘉陵江重庆段的水环境保护，并为嘉陵江重庆段乃至三峡库区的相关水环境保护政策的制定提供支持。
对嘉陵江重庆段PAHs的研究：采集13个月（2009年7月~2010年7月）嘉陵江重庆段13个取样点的样品，包括：169个表层水样，13个悬浮颗粒样，169个表层沉积物样品。对水样采用固相萃取-柱净化及气相色谱-质谱（GC-MS）的方法来测定PAHs含量；对悬浮颗粒和沉积物样品采用：索氏提取-柱净化及气相色谱-质谱（GC-MS）的方法来测定PAHs含量。运用比值法及主成分析-多元线性回归（PCA-MLR）对PAHs进行来源解析，并对嘉陵江重庆段PAHs的生态风险进行评价，结果表明：
①表层水体13个取样点ΣPAHs的浓度范围为245.46ng/L~1074.4ng/L，PAHs组成以中低环PAHs(2~4)环为主，高环的PAHs(5~6)含量浓度很低；悬浮颗粒相ΣPAHs的浓度范围为495.14ng/g~1274.38ng/g，PAHs组成以中高环PAHs(4~5)环为主，高环(6环)及低环(2环)的PAHs含量浓度很低；表层沉积物ΣPAHs的浓度范围为764.8ng/g~2353.5ng/g， PAHs的组成为4环含量最高，其次是3环和5环，2环及6环的PAHs含量浓度较低。
②表层水体及沉积物中ΣPAHs的浓度在时间分布上呈现出相似的规律，均是枯水期的ΣPAHs浓度＞丰水期的ΣPAHs浓度，季节差异比较明显。表层水体、悬浮颗粒及沉积物中的PAHs浓度在沿江的空间分布上都呈现出“升高-降低-升高-降低”的趋势。
③枯水期时，水体中DOC含量与ΣPAHs含量呈现明显的线性正相关(R=0.83)；丰水期时，水体中DOC含量与ΣPAHs含量无明显的线性相关。丰水期时，悬浮颗粒中TOC含量与ΣPAHs含量呈现明显的线性正相关(R=0.86)。枯水期和丰水期时，沉积物中TOC含量与ΣPAHs含量均呈现明显的线性正相关，相关系数分别为(R枯水期=0.82、R丰水期=0.90)。
④嘉陵江重庆段水体16种PAHs生态风险处于较低水平，没有对生物造成较大的风险。通过暴露模型可知嘉陵江重庆段水体中PAHs污染可能引起人体健康风险，其风险度在可接受范围内。
⑤结合(Ant)/(Ant+Phen)、(Flu)/(Flu+Pyr)和(BaA)/(BaA+Chr)3种比值及主成分析-多元线性回归可知：汽油和柴油的发动机燃烧的交通源是嘉陵江重庆段PAHs的主要污染源，其他的污染源如石油源、煤和木材燃烧及外来源的污染也会对PAHs有一定的贡献率。
对于嘉陵江重庆段DOM的研究：采集13个月（2009年7月~2010年7月）嘉陵江重庆段13个取样点的169个表层水样，采用紫外-可见光吸收光谱、荧光发射光谱和三维荧光光谱等分析方法，结合平行因子分析及聚类分析等统计方法对嘉陵江重庆段表层水体DOM的光谱学特性进行了研究，结果表明：
①嘉陵江重庆段表层水体DOM的污染在空间上的分布呈现“升高-降低-升高-降低”的趋势，荧光强度的分布趋势同嘉陵江沿岸的工业分布及外界的有机质输入密切相关，枯水期DOM的污染浓度高于丰水期。
②嘉陵江重庆段表层水体DOM的组成以陆源输入类腐殖类物质为主，內源产生的类蛋白物质为辅，而陆源输入类腐殖类物质又以富里酸为主，腐殖酸为辅。
③嘉陵江重庆段表层水体的DOM的三维荧光光谱由2类5个组分组成分别是：腐殖类组分C1(250,320nm/400nm)、C2(260,360nm/450nm)和C4(230nm/340,450nm)；类蛋白质组分C3(260nm/380nm)和C5(280nm/330nm)。
Polycyclic aromatic hydrocarbons (PAHs) are typical persistent organic pollutantswidely exist in environment, which known for their teratogenic, carcinogenetic andmutagenic effects. The distribution and pollution trend of PAHs in the environment havebecome the focus research in recent years. Dissolved organic matter (DOM) can interactwith the pollutants in the water environment such as metal ions, chemical pesticides andPAHs, therefore affecting their distribution, degradation and toxicity to aquaticorganisms. So DOM has significant impact on the ecosystems and biochemicalprocesses of the water body. Jialing River of Chongqing section was taken as researchtarget to study the concentration, spatial and temporal distribution and sources analysisof PAHs and DOM in the water samples. This study can not only understand the waterenvironmental protection in Jialing River of Chongqing section, but also providesupport for the decision making of water environment protection policy in the ThreeGorges Reservoir.
For the PAHs in the Jialing River of Chongqing section: samples of13months(from2007-07to2010-07) were collected from13sampling sites, including:169surface water samples,13suspended particles samples and169surface sedimentsamples. Solid phase extraction, column purification and gas chromatography-massspectrometry (GC-MS) were used to the determination the PAHs in surface watersamples; Soxhlet extraction, column purification and gas chromatography-massspectrometry (GC-MS) were used to the determination the PAHs in suspended particlesand sediment samples. Isotope ratio combing with principal componentanalysis-multiple linear regression were applied for source apportionment andecological risk evaluation of the PAHs in the Jialing River in Chongqing section, theresults showed that:
①The ΣPAHs concentration in surface water ranged from245.46ng/L to1074.4ng/L; The predominant PAHs were2-4ring PAHs, the5-6ring PAHs had lowproportion of the total PAHs. The ΣPAHs concentration in suspended particles rangedfrom495.14ng/g to1274.38ng/g; the predominant PAHs were4-5ring PAHs, the6ring and2ring PAHs accounted for low proportion of the total PAHs. The ΣPAHsconcentration in sediments ranged from764.8ng/g to2353.5ng/g with the predominant4ring PAHs, other contribution rate were followed by3ring,5ring,2ring and6ring PAHs.
②The PAHs concentration in the surface water and sediment showed similar rulein temporal distribution；PAHs concentration in the dry season was higher than thePAHs in the wet period; the spatial distribution of PAHs concentration in the surfacewater, suspended particles and sediment showed the same trend of” up-down-up-down”alone the river.
③DOC and ΣPAHs concentration showed significant positive linear correlation (R=0.83) in the surface water in dry season and no linear correlation in wet season; TOCand ΣPAHs concentration showed significant positive linear correlation (R=0.86) inthe suspended particles in dry season; TOC and ΣPAHs concentration also showedsignificant positive linear correlation in the sediments both in dry and wet season, thecorrelation coefficient were Rdry=0.82, Rwet=0.90respectively.
④The ecological risk of16PAHs in Jialing River of Chongqing section was atlow level and showed no great risk to biology in water body. From the exposure model,we knew that PAHs pollution may cause human health risk, but the degree of risk waswithin an acceptable range.
⑤The ratios of specific PAHs (Ant/Ant+Phe, Flu/Flu+Pyr and BaA/BaA+Chr) and principal component analysis-multiple linear regression marked that gasolineand diesel engine combustion source is the main PAHs pollution sources of the JialingRiver in Chongqing section, other sources such as petroleum, coal and woodcombustion and external sources were also contributed to the PAHs pollution.
For the DOM in the Jialing River of Chongqing section:169surface water samplesof13months (from2007-07to2010-07) were collected from13sampling sites.UV-visible absorption spectroscopy, fluorescence emission spectra andthree-dimensional fluorescence spectra combing with the parallel factor analysis wereused to characterize spectrum characteristics of DOM in the surface water sample ofJialing River in Chongqing section, results showed that:
①The DOM fluorescence intensity in the surface sample showed the trend of“up-down-up-down-up-down” in spatial distribution, and the distribution fluorescenceintensity showed closely relationship with the industrial distribution along the JialingRiver and the outside organic matter input; The DOM fluorescence intensity in thesurface sample showed the trend of up-down in temporal distribution, and DOMconcentration in dry season was higher than that of the wet period.
②The DOM in the Jialing River of Chongqing section showed predominantly terrestrial origin (including a mayor fulic-like component and humic-like component),protein from Endogenous metabolism contributed little to the water DOM.
③Five separate fluorescent components in two categories were identified by thePARAFAC model, including three humic material components C1(250,320nm/400nm),C2(260,360nm/450nm) and C4(230nm/340,450nm)； and two protein-likecomponents C3(260nm/380nm) and C5(280nm/330nm).
对嘉陵江重庆段PAHs的研究：采集13个月（2009年7月~2010年7月）嘉陵江重庆段13个取样点的样品，包括：169个表层水样，13个悬浮颗粒样，169个表层沉积物样品。对水样采用固相萃取-柱净化及气相色谱-质谱（GC-MS）的方法来测定PAHs含量；对悬浮颗粒和沉积物样品采用：索氏提取-柱净化及气相色谱-质谱（GC-MS）的方法来测定PAHs含量。运用比值法及主成分析-多元线性回归（PCA-MLR）对PAHs进行来源解析，并对嘉陵江重庆段PAHs的生态风险进行评价，结果表明：
①表层水体13个取样点ΣPAHs的浓度范围为245.46ng/L~1074.4ng/L，PAHs组成以中低环PAHs(2~4)环为主，高环的PAHs(5~6)含量浓度很低；悬浮颗粒相ΣPAHs的浓度范围为495.14ng/g~1274.38ng/g，PAHs组成以中高环PAHs(4~5)环为主，高环(6环)及低环(2环)的PAHs含量浓度很低；表层沉积物ΣPAHs的浓度范围为764.8ng/g~2353.5ng/g， PAHs的组成为4环含量最高，其次是3环和5环，2环及6环的PAHs含量浓度较低。
②表层水体及沉积物中ΣPAHs的浓度在时间分布上呈现出相似的规律，均是枯水期的ΣPAHs浓度＞丰水期的ΣPAHs浓度，季节差异比较明显。表层水体、悬浮颗粒及沉积物中的PAHs浓度在沿江的空间分布上都呈现出“升高-降低-升高-降低”的趋势。
③枯水期时，水体中DOC含量与ΣPAHs含量呈现明显的线性正相关(R=0.83)；丰水期时，水体中DOC含量与ΣPAHs含量无明显的线性相关。丰水期时，悬浮颗粒中TOC含量与ΣPAHs含量呈现明显的线性正相关(R=0.86)。枯水期和丰水期时，沉积物中TOC含量与ΣPAHs含量均呈现明显的线性正相关，相关系数分别为(R枯水期=0.82、R丰水期=0.90)。
④嘉陵江重庆段水体16种PAHs生态风险处于较低水平，没有对生物造成较大的风险。通过暴露模型可知嘉陵江重庆段水体中PAHs污染可能引起人体健康风险，其风险度在可接受范围内。
⑤结合(Ant)/(Ant+Phen)、(Flu)/(Flu+Pyr)和(BaA)/(BaA+Chr)3种比值及主成分析-多元线性回归可知：汽油和柴油的发动机燃烧的交通源是嘉陵江重庆段PAHs的主要污染源，其他的污染源如石油源、煤和木材燃烧及外来源的污染也会对PAHs有一定的贡献率。
对于嘉陵江重庆段DOM的研究：采集13个月（2009年7月~2010年7月）嘉陵江重庆段13个取样点的169个表层水样，采用紫外-可见光吸收光谱、荧光发射光谱和三维荧光光谱等分析方法，结合平行因子分析及聚类分析等统计方法对嘉陵江重庆段表层水体DOM的光谱学特性进行了研究，结果表明：
①嘉陵江重庆段表层水体DOM的污染在空间上的分布呈现“升高-降低-升高-降低”的趋势，荧光强度的分布趋势同嘉陵江沿岸的工业分布及外界的有机质输入密切相关，枯水期DOM的污染浓度高于丰水期。
②嘉陵江重庆段表层水体DOM的组成以陆源输入类腐殖类物质为主，內源产生的类蛋白物质为辅，而陆源输入类腐殖类物质又以富里酸为主，腐殖酸为辅。
③嘉陵江重庆段表层水体的DOM的三维荧光光谱由2类5个组分组成分别是：腐殖类组分C1(250,320nm/400nm)、C2(260,360nm/450nm)和C4(230nm/340,450nm)；类蛋白质组分C3(260nm/380nm)和C5(280nm/330nm)。
Polycyclic aromatic hydrocarbons (PAHs) are typical persistent organic pollutantswidely exist in environment, which known for their teratogenic, carcinogenetic andmutagenic effects. The distribution and pollution trend of PAHs in the environment havebecome the focus research in recent years. Dissolved organic matter (DOM) can interactwith the pollutants in the water environment such as metal ions, chemical pesticides andPAHs, therefore affecting their distribution, degradation and toxicity to aquaticorganisms. So DOM has significant impact on the ecosystems and biochemicalprocesses of the water body. Jialing River of Chongqing section was taken as researchtarget to study the concentration, spatial and temporal distribution and sources analysisof PAHs and DOM in the water samples. This study can not only understand the waterenvironmental protection in Jialing River of Chongqing section, but also providesupport for the decision making of water environment protection policy in the ThreeGorges Reservoir.
For the PAHs in the Jialing River of Chongqing section: samples of13months(from2007-07to2010-07) were collected from13sampling sites, including:169surface water samples,13suspended particles samples and169surface sedimentsamples. Solid phase extraction, column purification and gas chromatography-massspectrometry (GC-MS) were used to the determination the PAHs in surface watersamples; Soxhlet extraction, column purification and gas chromatography-massspectrometry (GC-MS) were used to the determination the PAHs in suspended particlesand sediment samples. Isotope ratio combing with principal componentanalysis-multiple linear regression were applied for source apportionment andecological risk evaluation of the PAHs in the Jialing River in Chongqing section, theresults showed that:
①The ΣPAHs concentration in surface water ranged from245.46ng/L to1074.4ng/L; The predominant PAHs were2-4ring PAHs, the5-6ring PAHs had lowproportion of the total PAHs. The ΣPAHs concentration in suspended particles rangedfrom495.14ng/g to1274.38ng/g; the predominant PAHs were4-5ring PAHs, the6ring and2ring PAHs accounted for low proportion of the total PAHs. The ΣPAHsconcentration in sediments ranged from764.8ng/g to2353.5ng/g with the predominant4ring PAHs, other contribution rate were followed by3ring,5ring,2ring and6ring PAHs.
②The PAHs concentration in the surface water and sediment showed similar rulein temporal distribution；PAHs concentration in the dry season was higher than thePAHs in the wet period; the spatial distribution of PAHs concentration in the surfacewater, suspended particles and sediment showed the same trend of” up-down-up-down”alone the river.
③DOC and ΣPAHs concentration showed significant positive linear correlation (R=0.83) in the surface water in dry season and no linear correlation in wet season; TOCand ΣPAHs concentration showed significant positive linear correlation (R=0.86) inthe suspended particles in dry season; TOC and ΣPAHs concentration also showedsignificant positive linear correlation in the sediments both in dry and wet season, thecorrelation coefficient were Rdry=0.82, Rwet=0.90respectively.
④The ecological risk of16PAHs in Jialing River of Chongqing section was atlow level and showed no great risk to biology in water body. From the exposure model,we knew that PAHs pollution may cause human health risk, but the degree of risk waswithin an acceptable range.
⑤The ratios of specific PAHs (Ant/Ant+Phe, Flu/Flu+Pyr and BaA/BaA+Chr) and principal component analysis-multiple linear regression marked that gasolineand diesel engine combustion source is the main PAHs pollution sources of the JialingRiver in Chongqing section, other sources such as petroleum, coal and woodcombustion and external sources were also contributed to the PAHs pollution.
For the DOM in the Jialing River of Chongqing section:169surface water samplesof13months (from2007-07to2010-07) were collected from13sampling sites.UV-visible absorption spectroscopy, fluorescence emission spectra andthree-dimensional fluorescence spectra combing with the parallel factor analysis wereused to characterize spectrum characteristics of DOM in the surface water sample ofJialing River in Chongqing section, results showed that:
①The DOM fluorescence intensity in the surface sample showed the trend of“up-down-up-down-up-down” in spatial distribution, and the distribution fluorescenceintensity showed closely relationship with the industrial distribution along the JialingRiver and the outside organic matter input; The DOM fluorescence intensity in thesurface sample showed the trend of up-down in temporal distribution, and DOMconcentration in dry season was higher than that of the wet period.
②The DOM in the Jialing River of Chongqing section showed predominantly terrestrial origin (including a mayor fulic-like component and humic-like component),protein from Endogenous metabolism contributed little to the water DOM.
③Five separate fluorescent components in two categories were identified by thePARAFAC model, including three humic material components C1(250,320nm/400nm),C2(260,360nm/450nm) and C4(230nm/340,450nm)； and two protein-likecomponents C3(260nm/380nm) and C5(280nm/330nm).
引文
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