生物扰动对河口沉积物中多环芳烃环境行为的影响
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摘要
多环芳烃(polycyclic aromatic hydrocarbons,PAHs)是环境中常见污染物,因其在环境中难降解、持久性和具有较强的“三致”效应,其生物地球化学行为倍受关注。作为一类典型的憎水性有机污染物,PAHs特别易于被颗粒物吸附,因此进入水环境中的PAHs最终富集于沉积物中。河口作为海陆的交错地区,汇集海、陆两个来源的污染物。与此同时,河口拥有大量的底栖动物,它们的摄食、爬行、避敌、掘穴和建造栖所等活动会改变沉积物结构,这一过程称为生物扰动。生物扰动显著改变沉积物的物理、化学和生物性质,从而改变沉积物中污染物的生物地球化学行为。本论文采用野外调查与室内微宇宙模拟实验相结合的方法系统研究了生物扰动对河口沉积物中PAHs环境行为的影响,并对有关机理进行了探讨。
利用微宇宙示踪技术,定量研究了天津北塘河口优势底栖动物,天津厚蟹(Helice tientsinensis)、沙蚕(Nereis diversicolor)、青蛤(Cyclina sinensis)和泥螺(Bullacta exarata)对沉积物的扰动作用。结果表明,不同底栖动物的扰动作用不同,对表层沉积物的扰动强度(扩散系数,10-3cm2/d)大小依次为沙蚕(2.95)>天津厚蟹(1.00)>青蛤(0.78)>泥螺(0.35)>对照(0.05)；对深层沉积物则是天津厚蟹(3.10)>沙蚕(2.33)>青蛤(0.28)>泥螺(0.15)>对照(0.05)。可见,在北塘河口,对沉积物扰动强度最大的是天津厚蟹。
在天津北塘河口附近采集代表不同扰动程度的不同类型的沉积物,包括来自没有厚蟹活动的对照区和有厚蟹活动的扰动区(又分蟹洞内和蟹洞外),研究生物扰动对河口沉积物中PAHs分布的影响。结果表明,3种类型的沉积物中总PAHs含量为蟹洞外(2722 ng/g)>蟹洞内(1239 ng/g)>对照区(1173 ng/g),单个PAHs(InP和BgP除外)也呈现同样的变化趋势。根据质量平衡计算了扰动区蟹洞内和蟹洞外沉积物PAHs含量的差异,结果表明,生物扰动造成了蟹洞内50%总PAHs的消失,除了Fla、InP和BgP之外,各PAHs也有不同程度的消失。生物扰动一方面增强沉积物中PAHs向间隙水释放,由此造成沉积物中PAHs向海洋输送；另一方面,生物扰动促进微生物降解PAHs.此外,厚蟹还富集部分PAHs.因此,生物扰动显著影响沉积物中PAHs的分布。
为了验证野外研究发现的生物扰动促进PAHs从沉积物相向水相释放的结论,利用室内微宇宙研究生物扰动对河口沉积物PAHs释放的影响。结果表明,生物扰动促进沉积物再悬浮,在此过程中向水相释放PAHs;与此同时,生物活动提高上覆水中的溶解性有机质含量,促进PAHs从悬浮物及表层沉积物发生解吸,从而显著提高上覆水中溶解态PAHs含量.由此证明了野外研究的结论,生物扰动促进沉积物中PAHs向水体释放。
由于溶解态PAHs能被生物所利用,因此这些被释放出来的溶解态PAHs具有潜在的生态风险。在室内微宇宙,利用半透膜被动采样技术(Semi-permeable membrane device,SPMD)评价了生物扰动对沉积物中PAHs生物有效性的影响。结果发现,在生物扰动的沉积物中,SPMD富集的总PAHs量显著高于没有生物扰动的,各单个PAHs具有同样的规律。SPMD-沉积物累积因子(SSAF)结果表明,低、中环PAHs的SSAF值在生物扰动处理中高于无生物扰动的；而高环PAHs的则在生物扰动处理中低于无生物扰动的。由此可见,生物扰动增加了低、中环PAHs的生物有效性,而对高环PAHs,影响不显著,这是因为溶解性有机质结合态的PAHs不具有生物有效性。
在室内微宇宙中研究生物扰动对沉积物中PAHs生物降解的影响,发现厚蟹通过排泄、降低沉积物粒度等方式增加沉积物中的有机质含量。由于有机质含量的增加,促进微生物繁殖,显著提高微生物的数量,进而提高微生物对沉积物中PAHs的降解能力。与无生物扰动相比,生物扰动提高降解率高达3.3-4倍,但生物降解主要发生在低、中环(尤其是3环)PAHs.此外,生物扰动也加强了共代谢作用的发生,进而也促进了部分高环PAHs发生生物降解。由此验证了野外研究的结论,生物扰动促进沉积物中PAHs生物降解。与此同时,也发现生物扰动对沉积物中PAHs环境行为影响最大的是促进其向水相释放。
本研究提供了生物扰动对河口沉积物中PAHs环境行为的基本信息,为客观地评价生物扰动对沉积物中PAHs在环境中的迁移转化过程中的环境风险的影响提供了科学依据。
Polycyclic aromatic hydrocarbons (PAHs) comprise a large class of widespread environmental contaminants. These compounds are widely distributed in the environment, notably in sediments of estuaries and coastal marine areas throughout the world. Due to their carcinogenic potential, there is great interest in their fate in the environment in recent years.
Due to the range of hydrodynamic and chemical conditions, estuaries have high biodiversity and intense biological activity. The feeding, burrowing, and reworking of benthic invertebrates, collectively termed bioturbation, are expected to modify the physical, chemical, and biological properties of the sediment. As a result, the fate of the contaminants in sediment should be modified. The purpose of the present study was to determine whether PAH fate would be influenced by bioturbation in the sediment through both field investigation and laboratory microcosm experiments.
Firstly, the bioturbation of Helice tientsinensis, Nereis diversicolor, Bullacta exarata, and Cyclina sinensis on sediment from the Beitang Estuary (Tianjin, China) was studied quantitatively by the microcosm tracer technique. The results showed that the distribution of sediment was significantly affected by bioturbation. The bioturbation capacity of different macrofauna varied a lot, with diffusion coefficient (10-3 cm2/d) in an order of N. diversicolor (2.95)> H. tientsinensis (1.00)> C. sinensis (0.78)> B. exarata. (0.35)> control (0.05) in surface sediment, while in deep sediment, the order was H. tientsinensis (3.10)> N. diversicolor (2.33)> C. sinensis (0.28)> B. exarata. (0.15)> control (0.05). These differences were mainly caused by that the macrofauna belonged to different functional groups. Correlation analysis revealed that the biovolume was significant correlated to the diffusion coefficient in surface sediment (p< 0.05), indicating that the biovolume of macrofauna could be used to predict their bioturbation intensity in sediment.
Bioturbation by the burrowing crab H. tiensinensis was investigated to determine its impact on PAH-contaminated estuarine sediments in a field investigation at Beitang Estuary. The concentrations of 16 USEPA priority PAHs in sediment and porewater from a crab bed (including surface and burrow samples) and a control area, as well as in crabs were measured. The total concentration of the 16 USEPA priority PAHs in surface sediment of the crab bed (average 2772 ng/g dry weight) was significantly higher than in the control area (1173 ng/g dry weight). In the crab bed, the total concentration of PAHs in burrow sediment (1239 ng/g dry weight) was lower than in surface sediment, and similar trend was found for most of individual PAHs except for InP and BgP. In order to further clarify the fate of PAHs in burrow, the mass of PAHs in the burrow as compared to that in the surface sediment was examined. The results shown that the mass difference was calculated to be< 0 to 73% for individual PAHs and 50% for the total PAHs. The enhanced PAH desorption in the burrow, which could be attributed to the increase in dissolved organic matter in porewater as well as the mechanic mixing by the crab, is expected to increase PAH flux to sea. Furthermore, the stimulated microbial degradation was proposed as an ignorable factor for the lower the PAH concentration in burrow sediment because crab bioturbation could increase the abundance and activity of microorganisms by several ways. In addition, H. tientsinensis incorporated a total PAHs concentration of 8816 ng/g lipid in their body, this may be another reason for the lower PAH concentration in burrow sediment. This field investigation indicated that crab bioturbation influences PAH fate in estuarine sediments.
In order to verify the conclusion of the field study, the effects of crab bioturbation on PAHs release from the sediment were studied in laboratory microcosms. The results shown that sediment resuspension was enhanced by the bioturbation. Due to sediment resuspension, both particulate and dissolved PAHs increased into the water column. Moreover, dissolved organic carbon (DOC) in overlying water was elevated by the bioturbation of crab. The DOC has been confirmed to enhance the distribution of PAHs from sediment to water. As a consequence, obvious desorption of PAHs from suspended particles and sediment to water occurred. This supports the conclusion of the field study.
Once the PAHs is released from sediment to overlying water, they will be uptaken by aquatic organisms, then pose potential risks to fish and to humans and wildlife that consume aquatic organisms. The impact on PAHs bioavailability in the water column of bioturbation was studied by semipermeable membrane device (SPMD) through laboratory experiments. During 119 d test, all the individual PAHs in SPMD in the microcosm with crab showed higher concentration than that without crab. However, the availability of the individual PAHs was different between small-intermediate and large ringed PAHs based on the SPMD-sediment accumulation factor. For the small-intermediate ringed PAHs, the SSAF value was higher in treatment with crab than without crab, while there was an inverse relationship for the large ringed PAHs. It indicates that the bioavailability was enhanced for small-intermediate ringed PAHs by crab bioturbation, and the large ringed PAHs were not significantly affected. This is because large ringed PAHs associated to DOC was not available.
The effects of crab bioturbation on PAH biodegradation from sediment were studied in microcosm. The results showed that the crab bioturbation enhanced the organic matter and fine particles in the sediment by the egesta, stimulating microbial activity. Thus, PAH biodegradation was enhanced with biodegradation rate of some PAhs increasing by 3.3-4 times by the crab bioturbation. Biodegradation enhancement occurred mainly for small-intermediate ringed PAHs. Additionally, some of large ringed PAHs were degraded by comebolism. The experiment in microcosm verified the conclusion of the field that biotubance enhanced biodegradation. Furthermore, the result showed the the most important impact of crab bioturbation on the environmental behavior of the PAHs in sediment is the PAHs were enhaned release fome sediment to water.
This dissertation could provide some useful information on bioturbation influences on the PAH fate in estuarine surface sediments. It is very important to the evaluation the ecological risk of the PAHs transfer by the bioturbation.
利用微宇宙示踪技术,定量研究了天津北塘河口优势底栖动物,天津厚蟹(Helice tientsinensis)、沙蚕(Nereis diversicolor)、青蛤(Cyclina sinensis)和泥螺(Bullacta exarata)对沉积物的扰动作用。结果表明,不同底栖动物的扰动作用不同,对表层沉积物的扰动强度(扩散系数,10-3cm2/d)大小依次为沙蚕(2.95)>天津厚蟹(1.00)>青蛤(0.78)>泥螺(0.35)>对照(0.05)；对深层沉积物则是天津厚蟹(3.10)>沙蚕(2.33)>青蛤(0.28)>泥螺(0.15)>对照(0.05)。可见,在北塘河口,对沉积物扰动强度最大的是天津厚蟹。
在天津北塘河口附近采集代表不同扰动程度的不同类型的沉积物,包括来自没有厚蟹活动的对照区和有厚蟹活动的扰动区(又分蟹洞内和蟹洞外),研究生物扰动对河口沉积物中PAHs分布的影响。结果表明,3种类型的沉积物中总PAHs含量为蟹洞外(2722 ng/g)>蟹洞内(1239 ng/g)>对照区(1173 ng/g),单个PAHs(InP和BgP除外)也呈现同样的变化趋势。根据质量平衡计算了扰动区蟹洞内和蟹洞外沉积物PAHs含量的差异,结果表明,生物扰动造成了蟹洞内50%总PAHs的消失,除了Fla、InP和BgP之外,各PAHs也有不同程度的消失。生物扰动一方面增强沉积物中PAHs向间隙水释放,由此造成沉积物中PAHs向海洋输送；另一方面,生物扰动促进微生物降解PAHs.此外,厚蟹还富集部分PAHs.因此,生物扰动显著影响沉积物中PAHs的分布。
为了验证野外研究发现的生物扰动促进PAHs从沉积物相向水相释放的结论,利用室内微宇宙研究生物扰动对河口沉积物PAHs释放的影响。结果表明,生物扰动促进沉积物再悬浮,在此过程中向水相释放PAHs;与此同时,生物活动提高上覆水中的溶解性有机质含量,促进PAHs从悬浮物及表层沉积物发生解吸,从而显著提高上覆水中溶解态PAHs含量.由此证明了野外研究的结论,生物扰动促进沉积物中PAHs向水体释放。
由于溶解态PAHs能被生物所利用,因此这些被释放出来的溶解态PAHs具有潜在的生态风险。在室内微宇宙,利用半透膜被动采样技术(Semi-permeable membrane device,SPMD)评价了生物扰动对沉积物中PAHs生物有效性的影响。结果发现,在生物扰动的沉积物中,SPMD富集的总PAHs量显著高于没有生物扰动的,各单个PAHs具有同样的规律。SPMD-沉积物累积因子(SSAF)结果表明,低、中环PAHs的SSAF值在生物扰动处理中高于无生物扰动的；而高环PAHs的则在生物扰动处理中低于无生物扰动的。由此可见,生物扰动增加了低、中环PAHs的生物有效性,而对高环PAHs,影响不显著,这是因为溶解性有机质结合态的PAHs不具有生物有效性。
在室内微宇宙中研究生物扰动对沉积物中PAHs生物降解的影响,发现厚蟹通过排泄、降低沉积物粒度等方式增加沉积物中的有机质含量。由于有机质含量的增加,促进微生物繁殖,显著提高微生物的数量,进而提高微生物对沉积物中PAHs的降解能力。与无生物扰动相比,生物扰动提高降解率高达3.3-4倍,但生物降解主要发生在低、中环(尤其是3环)PAHs.此外,生物扰动也加强了共代谢作用的发生,进而也促进了部分高环PAHs发生生物降解。由此验证了野外研究的结论,生物扰动促进沉积物中PAHs生物降解。与此同时,也发现生物扰动对沉积物中PAHs环境行为影响最大的是促进其向水相释放。
本研究提供了生物扰动对河口沉积物中PAHs环境行为的基本信息,为客观地评价生物扰动对沉积物中PAHs在环境中的迁移转化过程中的环境风险的影响提供了科学依据。
Polycyclic aromatic hydrocarbons (PAHs) comprise a large class of widespread environmental contaminants. These compounds are widely distributed in the environment, notably in sediments of estuaries and coastal marine areas throughout the world. Due to their carcinogenic potential, there is great interest in their fate in the environment in recent years.
Due to the range of hydrodynamic and chemical conditions, estuaries have high biodiversity and intense biological activity. The feeding, burrowing, and reworking of benthic invertebrates, collectively termed bioturbation, are expected to modify the physical, chemical, and biological properties of the sediment. As a result, the fate of the contaminants in sediment should be modified. The purpose of the present study was to determine whether PAH fate would be influenced by bioturbation in the sediment through both field investigation and laboratory microcosm experiments.
Firstly, the bioturbation of Helice tientsinensis, Nereis diversicolor, Bullacta exarata, and Cyclina sinensis on sediment from the Beitang Estuary (Tianjin, China) was studied quantitatively by the microcosm tracer technique. The results showed that the distribution of sediment was significantly affected by bioturbation. The bioturbation capacity of different macrofauna varied a lot, with diffusion coefficient (10-3 cm2/d) in an order of N. diversicolor (2.95)> H. tientsinensis (1.00)> C. sinensis (0.78)> B. exarata. (0.35)> control (0.05) in surface sediment, while in deep sediment, the order was H. tientsinensis (3.10)> N. diversicolor (2.33)> C. sinensis (0.28)> B. exarata. (0.15)> control (0.05). These differences were mainly caused by that the macrofauna belonged to different functional groups. Correlation analysis revealed that the biovolume was significant correlated to the diffusion coefficient in surface sediment (p< 0.05), indicating that the biovolume of macrofauna could be used to predict their bioturbation intensity in sediment.
Bioturbation by the burrowing crab H. tiensinensis was investigated to determine its impact on PAH-contaminated estuarine sediments in a field investigation at Beitang Estuary. The concentrations of 16 USEPA priority PAHs in sediment and porewater from a crab bed (including surface and burrow samples) and a control area, as well as in crabs were measured. The total concentration of the 16 USEPA priority PAHs in surface sediment of the crab bed (average 2772 ng/g dry weight) was significantly higher than in the control area (1173 ng/g dry weight). In the crab bed, the total concentration of PAHs in burrow sediment (1239 ng/g dry weight) was lower than in surface sediment, and similar trend was found for most of individual PAHs except for InP and BgP. In order to further clarify the fate of PAHs in burrow, the mass of PAHs in the burrow as compared to that in the surface sediment was examined. The results shown that the mass difference was calculated to be< 0 to 73% for individual PAHs and 50% for the total PAHs. The enhanced PAH desorption in the burrow, which could be attributed to the increase in dissolved organic matter in porewater as well as the mechanic mixing by the crab, is expected to increase PAH flux to sea. Furthermore, the stimulated microbial degradation was proposed as an ignorable factor for the lower the PAH concentration in burrow sediment because crab bioturbation could increase the abundance and activity of microorganisms by several ways. In addition, H. tientsinensis incorporated a total PAHs concentration of 8816 ng/g lipid in their body, this may be another reason for the lower PAH concentration in burrow sediment. This field investigation indicated that crab bioturbation influences PAH fate in estuarine sediments.
In order to verify the conclusion of the field study, the effects of crab bioturbation on PAHs release from the sediment were studied in laboratory microcosms. The results shown that sediment resuspension was enhanced by the bioturbation. Due to sediment resuspension, both particulate and dissolved PAHs increased into the water column. Moreover, dissolved organic carbon (DOC) in overlying water was elevated by the bioturbation of crab. The DOC has been confirmed to enhance the distribution of PAHs from sediment to water. As a consequence, obvious desorption of PAHs from suspended particles and sediment to water occurred. This supports the conclusion of the field study.
Once the PAHs is released from sediment to overlying water, they will be uptaken by aquatic organisms, then pose potential risks to fish and to humans and wildlife that consume aquatic organisms. The impact on PAHs bioavailability in the water column of bioturbation was studied by semipermeable membrane device (SPMD) through laboratory experiments. During 119 d test, all the individual PAHs in SPMD in the microcosm with crab showed higher concentration than that without crab. However, the availability of the individual PAHs was different between small-intermediate and large ringed PAHs based on the SPMD-sediment accumulation factor. For the small-intermediate ringed PAHs, the SSAF value was higher in treatment with crab than without crab, while there was an inverse relationship for the large ringed PAHs. It indicates that the bioavailability was enhanced for small-intermediate ringed PAHs by crab bioturbation, and the large ringed PAHs were not significantly affected. This is because large ringed PAHs associated to DOC was not available.
The effects of crab bioturbation on PAH biodegradation from sediment were studied in microcosm. The results showed that the crab bioturbation enhanced the organic matter and fine particles in the sediment by the egesta, stimulating microbial activity. Thus, PAH biodegradation was enhanced with biodegradation rate of some PAhs increasing by 3.3-4 times by the crab bioturbation. Biodegradation enhancement occurred mainly for small-intermediate ringed PAHs. Additionally, some of large ringed PAHs were degraded by comebolism. The experiment in microcosm verified the conclusion of the field that biotubance enhanced biodegradation. Furthermore, the result showed the the most important impact of crab bioturbation on the environmental behavior of the PAHs in sediment is the PAHs were enhaned release fome sediment to water.
This dissertation could provide some useful information on bioturbation influences on the PAH fate in estuarine surface sediments. It is very important to the evaluation the ecological risk of the PAHs transfer by the bioturbation.
引文
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