珠江口及近海沉积物中重金属元素的分布、赋存形态及其潜在生态风险评价
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摘要
本文分析测定了珠江口及近海典型环境下沉积柱中Cr、Co、Ni、Cd、Cu、Pb、Zn、Mn和Fe的总量，对其进行了逐级提取，并分析了不同季节沉积柱中的酸挥发性硫化物(AVS)和同步提取重金属(SEM)的含量。在此基础上，对珠江口及近海沉积物中重金属的时空分布、赋存形态、来源、迁移及其累积规律进行了研究，并采用基于重金属总量、重金属逐级提取和AVS／SEM三个体系的不同方法对研究区的重金属污染水平及潜在生态风险进行了评价，探讨了不同评价体系之间的相互联系和对应关系。
采用珠江口外近海两个受人类活动影响较弱站位的沉积柱样品，对珠江口及近海沉积物背景值进行了研究。各元素的背景值分别为：Fe为20240.4 mg／kg、Mn为306.8 mg／kg、Cr为41 mg／kg、Co为12.3 mg／kg、Ni为23.1 mg／kg、Cu为9.8 mg／kg、Zn为45 mg／kg、Pb为29mg／kg、Cd为0.2mg／kg、P为203mg／kg。
珠江口内重金属含量高于口外近海，尤其是Cu、Zn和Cd，珠江口内均值比口外近海高约3～5倍。珠江口内沉积柱中Cu含量高于Ni和Co，Zn含量明显高于Cr和Pb，而口外近海Cu含量则低于Ni和Co，且Zn含量与Cr和Pb相近，这反映了珠江口内和口外近海沉积物中重金属来源的差异；珠江口内西滩和中滩站位4(靠近深圳湾)重金属含量较高，而中滩另两个站位重金属含量相对较低，这种差异是陆源输入、水动力条件以及沉积环境作用的综合体现。部分站位沉积柱中重金属含量随深度逐渐降低，可能反映了这些站位接受陆源污染物增加，重金属污染有加重的趋势。
应用改进的BCR逐级提取方法对珠江口及近海沉积柱样品中重金属(Cr、Co、Ni、Cu、Pb、Zn、Fe、Mn)赋存形态的研究结果表明，锰主要以酸提取态存在(52.57％)，铬、镍、铁、钴残渣态所占比重均高于60％；重金属总可提取态(酸提取态、可还原态和可氧化态)所占比例与重金属总量呈正相关性，这表明人为输入的重金属主要以可提取态的形式存在，这可能是重金属总量能在一定程度上反映沉积物重金属潜在生态风险的内在原因。
AVS和SEM的空间分布和季节性变化的研究结果表明，珠江口沉积物中AVS含量范围为0～27.47μmol·g~(-1)，且随深度而增加。总体来看，春季和夏季AVS含量高于冬季，底层沉积物AVS含量高于表层。沉积物中硫酸盐还原菌活性和氧化还原状态是其主要影响因素。SEM含量变化范围为0.82～4.66μmol·g~(-1)，随深度加深略有降低。珠江口沉积物中AVS和SEM含量的季节性变化可能导致不同季节重金属的生物有效性的变化。
采用基于三种不同评价体系的(基于重金属总量、基于重金属形态分析和基于AVS／SEM)生态风险评价方法对珠江口沉积物重金属潜在生态风险进行了评价，分析探讨了不同评价方法的优劣，针对其中一些评价方法的不足提出了改进建议，并根据不同的需要为今后重金属潜在生态风险评价设计了几套综合评价方案。本文采用的具体评价方法分别为：中国海洋沉积物质量标准法、沉积物富集系数法、多元生态危害评价法、地质累积指数法、沉积物质量基准法(TEL／PEL，ERL／ERM)、次生相与原生相比值法、次生相富集系数法以及AVS／SEM法。综合不同评价体系对珠江口沉积物重金属的潜在生态风险评价结果表明：西滩站位6和7、中滩站位4潜在生态风险较高，而西滩站位2、中滩站位1和3相对较低。
SEM的含量接近于酸可提取态与还原提取态之和，明显低于重金属总量。由于AVS的存在将形成金属硫化物而降低重金属的生物毒性，基于总量和逐级提取的重金属污染评价方法均没有考虑AVS的影响，其结果往往会过高地估计重金属的生态风险，对于还原性强的沉积物尤为如此。
当SEM-AVS的摩尔差值大于零时，表明有过剩重金属存在，并且有可能产生重金属生物毒性，但目前仍缺少基于过剩重金属的毒性评价标准。以AVS／SEM为基础，结合其它的评价方法，才能较全面地反映沉积物中重金属的潜在生态风险。
The total concentration, speciation of elements (Fe, Mn, Cr, Co, Ni, Cu, Pb, Zn), AVS (acid volatile sulfide) and SEM (simultaneously extracted metals) were determined in sediment cores collected from the Pearl River Estuary (PRE) and adjacent shelf. Based on which, the spatial and temporal distributions, speciation, sources, transport and accumulation were investigated. Several ecological assessment methods, which based on three different assessment systems (total concentration, sequential extraction and AVS/SEM), were applied to assess the heavy metals pollution and potential biotoxicity in sediments from the PRE and adjacent shelf. The interrelationship and correspondence relationship of different evaluation methods were also discussed.
The background values of elements in sediment of the PRE and adjacent shelf were determined with the samples collected from sites E4 and C5, where were slightly influenced by human activities. The result showed that the background values were: Fe 20240.4 mg/kg, Mn 306.8 mg/kg, Cr 41 mg/kg, Co 12.3 mg/kg, Ni 23.1 mg/kg, Cu 9.8 mg/kg, Zn 45 mg/kg, Pb29mg/kg, Cd 0.2mg/kg, P 203 mg/kg.
The total heavy metal concentrations indicated that there was an obvious difference between the heavy metal contents in the PRE and in the adjacent shelf, especially for Cu, Zn, Cd, with the average contents of heavy metals in the PRE being trinary to quintuple of those in the adjacent shelf. Further, differences in the distribution pattern of heavy metals between the PRE and the adjacent shelf were also found: (1) The Cu content is higher than that of Ni and Co in sediment cores from the PRE, but is lower in the adjacent shelf; (2) the content of Zn is significantly higher than that of Cr and Pb in the PRE, but is slightly higher in the adjacent shelf. These observations may reflect the difference in the sources of heavy metals between the PRE and the adjacent shelf, and reflect the characteristics of the sources. The concentrations of heavy metals in the west shoal and at site 4 were higher than the site 1 and 3. This difference was an integrated manifestation of terrestrial inputs, hydrodynamic conditions and sedimentary environment. According to the vertical distribution, the heavy metal contents decrease with the depth in sediment cores at sites 2, 4 and 7, which reflect that these sites received more land source pollutants and the heavy metal pollution became more and more serious in the past years. Obvious vertical variation trend of heavy metal contents was not observed at other sites in the PRE.
The modified BCR-sequential extraction technique was used to determine the speciation (acid-soluble, reducible, oxidisable and residual) of metals (Cr, Co, Ni, Cu, Pb, Zn, Fe, Mn) in sediment samples from the PRE and the adjacent shelf. The results showed that most Cr, Ni, Fe and Co in the residual fraction were more than 60% of their respective content. There was a positive correlation between the recoverable (acid-soluble+reducible+oxidisable) fractions and the total content of heavy metals. This may reflect that heavy metals, which came from human activities, were mainly in the recoverable fractions, not in the residual fraction.
The spatial and seasonal distribution of AVS and SEM in sediment cores from the PRE, showed that the AVS content varies in a large range (0～27.47μmol·g~(-1)) and usually increases with depth. On the whole, the AVS content was higher in spring and summer than in winter, and was higher in bottom sediments than in surface sediments. The activity of sulfate-reducing bacteria and content of dissolved oxygen in sediments were the main influencing factor. The SEM concentration ranges from 0.82 to 4.66μmol·g~(-1) and displays a slightly decreasing trend with depth. The seasonal variations of AVS and SEM may lead to variations in metal bioavailability during the year.
Several methods, which based on total concentration, sequential extraction and AVS/SEM, were applied to assess the pollution level and potential ecological toxicity of heavy metals in sediments from the PRE and adjacent shelf. A comprehensive assessment of the PRE indicated that the potential ecological risk of heavy metal was higher at sites 4, 6 and 7 than at sites 1,2 and 3.
Generally, the SEM is close to the sum of acid soluble and reducible fractions, and is obviously lower than the total contents of heavy metals. Because the risk assessing methods that are based on total metal content and sequential extractions ignore the immobilization of heavy metals by sulfides, these methods would most probably over-estimate the ecological risk of heavy metals, especially in reducing environments. AVS/SEM analysis is proposed to combine with other methods to better assess the ecological risk of heavy metals in sediments.
采用珠江口外近海两个受人类活动影响较弱站位的沉积柱样品，对珠江口及近海沉积物背景值进行了研究。各元素的背景值分别为：Fe为20240.4 mg／kg、Mn为306.8 mg／kg、Cr为41 mg／kg、Co为12.3 mg／kg、Ni为23.1 mg／kg、Cu为9.8 mg／kg、Zn为45 mg／kg、Pb为29mg／kg、Cd为0.2mg／kg、P为203mg／kg。
珠江口内重金属含量高于口外近海，尤其是Cu、Zn和Cd，珠江口内均值比口外近海高约3～5倍。珠江口内沉积柱中Cu含量高于Ni和Co，Zn含量明显高于Cr和Pb，而口外近海Cu含量则低于Ni和Co，且Zn含量与Cr和Pb相近，这反映了珠江口内和口外近海沉积物中重金属来源的差异；珠江口内西滩和中滩站位4(靠近深圳湾)重金属含量较高，而中滩另两个站位重金属含量相对较低，这种差异是陆源输入、水动力条件以及沉积环境作用的综合体现。部分站位沉积柱中重金属含量随深度逐渐降低，可能反映了这些站位接受陆源污染物增加，重金属污染有加重的趋势。
应用改进的BCR逐级提取方法对珠江口及近海沉积柱样品中重金属(Cr、Co、Ni、Cu、Pb、Zn、Fe、Mn)赋存形态的研究结果表明，锰主要以酸提取态存在(52.57％)，铬、镍、铁、钴残渣态所占比重均高于60％；重金属总可提取态(酸提取态、可还原态和可氧化态)所占比例与重金属总量呈正相关性，这表明人为输入的重金属主要以可提取态的形式存在，这可能是重金属总量能在一定程度上反映沉积物重金属潜在生态风险的内在原因。
AVS和SEM的空间分布和季节性变化的研究结果表明，珠江口沉积物中AVS含量范围为0～27.47μmol·g~(-1)，且随深度而增加。总体来看，春季和夏季AVS含量高于冬季，底层沉积物AVS含量高于表层。沉积物中硫酸盐还原菌活性和氧化还原状态是其主要影响因素。SEM含量变化范围为0.82～4.66μmol·g~(-1)，随深度加深略有降低。珠江口沉积物中AVS和SEM含量的季节性变化可能导致不同季节重金属的生物有效性的变化。
采用基于三种不同评价体系的(基于重金属总量、基于重金属形态分析和基于AVS／SEM)生态风险评价方法对珠江口沉积物重金属潜在生态风险进行了评价，分析探讨了不同评价方法的优劣，针对其中一些评价方法的不足提出了改进建议，并根据不同的需要为今后重金属潜在生态风险评价设计了几套综合评价方案。本文采用的具体评价方法分别为：中国海洋沉积物质量标准法、沉积物富集系数法、多元生态危害评价法、地质累积指数法、沉积物质量基准法(TEL／PEL，ERL／ERM)、次生相与原生相比值法、次生相富集系数法以及AVS／SEM法。综合不同评价体系对珠江口沉积物重金属的潜在生态风险评价结果表明：西滩站位6和7、中滩站位4潜在生态风险较高，而西滩站位2、中滩站位1和3相对较低。
SEM的含量接近于酸可提取态与还原提取态之和，明显低于重金属总量。由于AVS的存在将形成金属硫化物而降低重金属的生物毒性，基于总量和逐级提取的重金属污染评价方法均没有考虑AVS的影响，其结果往往会过高地估计重金属的生态风险，对于还原性强的沉积物尤为如此。
当SEM-AVS的摩尔差值大于零时，表明有过剩重金属存在，并且有可能产生重金属生物毒性，但目前仍缺少基于过剩重金属的毒性评价标准。以AVS／SEM为基础，结合其它的评价方法，才能较全面地反映沉积物中重金属的潜在生态风险。
The total concentration, speciation of elements (Fe, Mn, Cr, Co, Ni, Cu, Pb, Zn), AVS (acid volatile sulfide) and SEM (simultaneously extracted metals) were determined in sediment cores collected from the Pearl River Estuary (PRE) and adjacent shelf. Based on which, the spatial and temporal distributions, speciation, sources, transport and accumulation were investigated. Several ecological assessment methods, which based on three different assessment systems (total concentration, sequential extraction and AVS/SEM), were applied to assess the heavy metals pollution and potential biotoxicity in sediments from the PRE and adjacent shelf. The interrelationship and correspondence relationship of different evaluation methods were also discussed.
The background values of elements in sediment of the PRE and adjacent shelf were determined with the samples collected from sites E4 and C5, where were slightly influenced by human activities. The result showed that the background values were: Fe 20240.4 mg/kg, Mn 306.8 mg/kg, Cr 41 mg/kg, Co 12.3 mg/kg, Ni 23.1 mg/kg, Cu 9.8 mg/kg, Zn 45 mg/kg, Pb29mg/kg, Cd 0.2mg/kg, P 203 mg/kg.
The total heavy metal concentrations indicated that there was an obvious difference between the heavy metal contents in the PRE and in the adjacent shelf, especially for Cu, Zn, Cd, with the average contents of heavy metals in the PRE being trinary to quintuple of those in the adjacent shelf. Further, differences in the distribution pattern of heavy metals between the PRE and the adjacent shelf were also found: (1) The Cu content is higher than that of Ni and Co in sediment cores from the PRE, but is lower in the adjacent shelf; (2) the content of Zn is significantly higher than that of Cr and Pb in the PRE, but is slightly higher in the adjacent shelf. These observations may reflect the difference in the sources of heavy metals between the PRE and the adjacent shelf, and reflect the characteristics of the sources. The concentrations of heavy metals in the west shoal and at site 4 were higher than the site 1 and 3. This difference was an integrated manifestation of terrestrial inputs, hydrodynamic conditions and sedimentary environment. According to the vertical distribution, the heavy metal contents decrease with the depth in sediment cores at sites 2, 4 and 7, which reflect that these sites received more land source pollutants and the heavy metal pollution became more and more serious in the past years. Obvious vertical variation trend of heavy metal contents was not observed at other sites in the PRE.
The modified BCR-sequential extraction technique was used to determine the speciation (acid-soluble, reducible, oxidisable and residual) of metals (Cr, Co, Ni, Cu, Pb, Zn, Fe, Mn) in sediment samples from the PRE and the adjacent shelf. The results showed that most Cr, Ni, Fe and Co in the residual fraction were more than 60% of their respective content. There was a positive correlation between the recoverable (acid-soluble+reducible+oxidisable) fractions and the total content of heavy metals. This may reflect that heavy metals, which came from human activities, were mainly in the recoverable fractions, not in the residual fraction.
The spatial and seasonal distribution of AVS and SEM in sediment cores from the PRE, showed that the AVS content varies in a large range (0～27.47μmol·g~(-1)) and usually increases with depth. On the whole, the AVS content was higher in spring and summer than in winter, and was higher in bottom sediments than in surface sediments. The activity of sulfate-reducing bacteria and content of dissolved oxygen in sediments were the main influencing factor. The SEM concentration ranges from 0.82 to 4.66μmol·g~(-1) and displays a slightly decreasing trend with depth. The seasonal variations of AVS and SEM may lead to variations in metal bioavailability during the year.
Several methods, which based on total concentration, sequential extraction and AVS/SEM, were applied to assess the pollution level and potential ecological toxicity of heavy metals in sediments from the PRE and adjacent shelf. A comprehensive assessment of the PRE indicated that the potential ecological risk of heavy metal was higher at sites 4, 6 and 7 than at sites 1,2 and 3.
Generally, the SEM is close to the sum of acid soluble and reducible fractions, and is obviously lower than the total contents of heavy metals. Because the risk assessing methods that are based on total metal content and sequential extractions ignore the immobilization of heavy metals by sulfides, these methods would most probably over-estimate the ecological risk of heavy metals, especially in reducing environments. AVS/SEM analysis is proposed to combine with other methods to better assess the ecological risk of heavy metals in sediments.
引文
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