厦门附近海区多相介质中石油烃的组成特征及其生物地球化学指示
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摘要
本论文以港口和养殖功能兼备的厦门港及其临近海区为研究对象，采用现代分析技术，从分子水平研究石油烃进入近岸海洋环境后在各相介质(水-沉积物-生物体)中的生物地球化学，取得以下结果：
1．优化实验条件，建立了不同相样品中痕量石油烃的分析方法，特别是完善了沉积物中痕量组分的分析方法，并采用标准参照物进行了校准；
2．石油烃中各种组分特别是正构烷烃与多环芳烃量化指标具有很好的生物地球化学指示作用。首次发现厦门地区水体、沉积物中nC11含量很高，与煤污染有一定关系。另外厦门海区水体中萘含量与以前相比很高，通过对比判别，认为与厦门地区日益增多的机动车、居民与宾馆大量使用樟脑丸有一定关系。
3．本文首次研究了微表层海水中石油烃各种组分的富集系数，进一步探讨了富集的机理，对了解石油烃在海洋环境中的分布及其生物地球化学行为有重要意义。研究发现，微表层对烷烃的富集，主要受物质来源的控制，在上、下层物质输入基本相同时，正构烷烃在微表层海水的富集：低碳数时富集偶数碳，从nC14-nC20，富集倍数逐渐降低；高碳数富集奇数碳，微表层对烷烃总量的富集系数为6倍左右。微表层海水对多环芳烃各组分的富集顺序，基本呈5环＞4环＞3环＞2环，微表层对多环芳烃的富集倍数随环数的增加以幂级升高，这与不同环数多环芳烃在水中的溶解度、溶沸点、挥发度等变化规律相吻合。微表层对多环芳烃总量的富集在1-5之间，平均富集倍数为3.14倍。
4．研究了石油烃在底层水-间隙水—沉积物界面之间的生物地球化学的变化特征，发现石油烃在间隙水中的分配主要以水溶性较高、溶沸点较低的短链烷烃和低环数的多环芳烃为主；在沉积物中的分配主要以水溶性较低、溶沸点较高的长链烷烃和高环数的多环芳烃组成为主；推测沉积物-间隙水是一物质分配平衡的异相平衡体系。厦门附近海区间隙水中石油烃的浓度基本上小于底层水的浓度，主要是底层水向下的输入，使两者达到动态平衡。
5．结合多种生物标志物判别，推断厦门附近海区表层沉积物，厦门港口内油码头附近的W05站、员当湖出口的W06站、马銮湾养殖区的W07站的表层沉积物受到石油烃污染较为明显，污染来源主要是机动船的含油废水排放、市区生活污水、汽、柴油的燃烧及煤的污染；九龙江口的W01、W02、W03站，石油烃以燃烧源为主。
6．通过对油码头及海！刁岛柱状沉积物的污染历史研究，发现海门岛曾经经历过石
油泄漏或煤的污染，油码头柱状沉积物相对海I］岛沉积物石油烃污染较轻，tl
在八十年代－九十年代早期遭受过轻微污染，自94年油码头改建后，改变了该＊
的沉积环境及沉积速率，石油烃污染也不太明显，但最近两年又有增强的趋势。
7．通过现场采样与实验室相结合的研究方法，研究了石油烃在养殖翡翠贻贝个同
组织中组成与分配规律，发现石油烃在贻贝不同组织中的组成与富集差异和贝
类的摄食途径与代谢有关。
8．通过对养殖鱼排区水、翡翠贻贝体内石油烃组分的分析，发现翡翠贻贝的内肌
团对烷烃的平均富集倍数约为2500倍，对多环芳烃的富集倍数则近1000倍，
翡翠贻贝对烷烃的富集较多环芳烃多，这与烷烃的水溶性较多环芳烃小、亲脂
性强有关。
9．厦门附近海区四个鱼排的翡翠贻贝不同程度遭受到石油烃的污染，特别是马銮
湾鱼排，由于水动力活动较弱，使贝类更易富集石油烃。
10、本文首次采用大型统计软件 SPSS（10刀）对大量的原始数据进行统计分析，以
研究石油烃的来源及迁移、转化规律。
总之，论文的根本点是从分于水平出发，深入、系统研究了近岸海洋环境各相
介质中石油烃的组成特征及其生物地球化学指示，探索性研究了控制石油烃生物地
球化学行为过程的机理，为海洋环境的保护和管理提供科学依据。
Based on the study of the composition and biogeochemical characteristics of petroleum hydrocarbons (PH) in different interfaces (water-sediment-organisms) in Xiamen Harbour and adjacent area using modern analysis techniques, the biogeochemical process of petroleum hydrocarbons in marine environment were discussed. The results show that:
1. Optimized the conditions of experiments and established the analysis methods of trace petroleum hydrocarbons of samples in different phase. Especially optimized the analysis method of trace components of petroleum hydrocarbons in sediments and calibrated the method using SRM (Standard Reference Material).
2. Quantification index of n-akanes and polycyclic aromatic hydrocarbons (PAHs) were proved as the good biomarker for indicating the biogeochemical process of petroleum hydrocarbons; It was the first time to find the high level of nC 11 in Xiamen water and sediments were related to the coal pollution. Additionally, the high level of Naphthalene were considered with the increasing motor -driven vehicles and the use of camphor ball in hotels and in families in Xiamen City.
3. It was the first time to study the accumulation of each component of petroleum hydrocarbons in microlayer detail. The mechanism of accumulation was discussed. Found that the sources of material controlled the accumulation coefficient of PH in microlayer seawater. When the sources of upper layer and down layer were almost same, microlayer water accumulated even carbons in short chain n-alkanes; accumulated odd carbons in long chain n-alkanes. The accumulation coefficients of alkanes were 6. The accumulation order of microlayer water for PAHs was 5 rings >4 ring >3 rings>2 rings and the coefficients increasing with power series, were related with the solubility, boil and melting points and evaporate degree. Microlayer water accumulate ?PAHs was 1 -5 (mean 3.14).
4. Based on the biogeochemical characteristics of PH between bottom water-pore water-sediments interfaces, found that the short chain n-alkanes and low rings PAHs with high solubility and low melting and boiling points distributed in pore water and the long chain n-alkanes and high rings PAHs with lower solubility and high melting and boiling points distributed in sediments. This partition pattern between sediments and pore water indicated the balance system between water and sediments. The
concentrations of PH in pore water was lower than that in bottom water indicated PH in sediments mainly came from the deposition of PH from bottom water.
5. Combined several kinds of biomarkers, we could guessed that the sources of PH in Xiamen Harbour mainly came from oil-containing waste water discharge, urban water discharge and the combustions of fuels and gasoline; the sources of PH near Jioulong River Estuary mainly was combustion of fossil fuel.
6. Based on the analysis of composition of petroleum hydrocarbon in Oil port core sediment and Haimen Island core sediment, Jiulong sediment were polluted by petroleum hydrocarbon in 1994, oil port sediment were contaminated increasing in recent years.
7. Based on the study of petroleum hydrocarbons in seawater and mussels in fish cages, the accumulation coefficients of organisms for PH very high. Mussels could accumulate n-alakanes for 2500 times and PAHs 1000 times.
8. From the combination experiments of in situ and laboratory, the distribution and transportation characteristic of petroleum hydrocarbons in different tissues of mussels were studied. It was found that the composition and accumulation of petroleum hydrocarbon in mussels were related with the pathway of eating and metabolize processes.
9. The mussels in four fish cages were contaminated by PH, especially in Maluan Bay.
10. This paper were first time to use the statistics software SPSS 10.0 to study the sources, transportation and transform regular.
In the all, the thesis researched the composition characteristics and biogeochemical processes of petroleum hydrocarbons deeply and comprehensively f
1．优化实验条件，建立了不同相样品中痕量石油烃的分析方法，特别是完善了沉积物中痕量组分的分析方法，并采用标准参照物进行了校准；
2．石油烃中各种组分特别是正构烷烃与多环芳烃量化指标具有很好的生物地球化学指示作用。首次发现厦门地区水体、沉积物中nC11含量很高，与煤污染有一定关系。另外厦门海区水体中萘含量与以前相比很高，通过对比判别，认为与厦门地区日益增多的机动车、居民与宾馆大量使用樟脑丸有一定关系。
3．本文首次研究了微表层海水中石油烃各种组分的富集系数，进一步探讨了富集的机理，对了解石油烃在海洋环境中的分布及其生物地球化学行为有重要意义。研究发现，微表层对烷烃的富集，主要受物质来源的控制，在上、下层物质输入基本相同时，正构烷烃在微表层海水的富集：低碳数时富集偶数碳，从nC14-nC20，富集倍数逐渐降低；高碳数富集奇数碳，微表层对烷烃总量的富集系数为6倍左右。微表层海水对多环芳烃各组分的富集顺序，基本呈5环＞4环＞3环＞2环，微表层对多环芳烃的富集倍数随环数的增加以幂级升高，这与不同环数多环芳烃在水中的溶解度、溶沸点、挥发度等变化规律相吻合。微表层对多环芳烃总量的富集在1-5之间，平均富集倍数为3.14倍。
4．研究了石油烃在底层水-间隙水—沉积物界面之间的生物地球化学的变化特征，发现石油烃在间隙水中的分配主要以水溶性较高、溶沸点较低的短链烷烃和低环数的多环芳烃为主；在沉积物中的分配主要以水溶性较低、溶沸点较高的长链烷烃和高环数的多环芳烃组成为主；推测沉积物-间隙水是一物质分配平衡的异相平衡体系。厦门附近海区间隙水中石油烃的浓度基本上小于底层水的浓度，主要是底层水向下的输入，使两者达到动态平衡。
5．结合多种生物标志物判别，推断厦门附近海区表层沉积物，厦门港口内油码头附近的W05站、员当湖出口的W06站、马銮湾养殖区的W07站的表层沉积物受到石油烃污染较为明显，污染来源主要是机动船的含油废水排放、市区生活污水、汽、柴油的燃烧及煤的污染；九龙江口的W01、W02、W03站，石油烃以燃烧源为主。
6．通过对油码头及海！刁岛柱状沉积物的污染历史研究，发现海门岛曾经经历过石
油泄漏或煤的污染，油码头柱状沉积物相对海I］岛沉积物石油烃污染较轻，tl
在八十年代－九十年代早期遭受过轻微污染，自94年油码头改建后，改变了该＊
的沉积环境及沉积速率，石油烃污染也不太明显，但最近两年又有增强的趋势。
7．通过现场采样与实验室相结合的研究方法，研究了石油烃在养殖翡翠贻贝个同
组织中组成与分配规律，发现石油烃在贻贝不同组织中的组成与富集差异和贝
类的摄食途径与代谢有关。
8．通过对养殖鱼排区水、翡翠贻贝体内石油烃组分的分析，发现翡翠贻贝的内肌
团对烷烃的平均富集倍数约为2500倍，对多环芳烃的富集倍数则近1000倍，
翡翠贻贝对烷烃的富集较多环芳烃多，这与烷烃的水溶性较多环芳烃小、亲脂
性强有关。
9．厦门附近海区四个鱼排的翡翠贻贝不同程度遭受到石油烃的污染，特别是马銮
湾鱼排，由于水动力活动较弱，使贝类更易富集石油烃。
10、本文首次采用大型统计软件 SPSS（10刀）对大量的原始数据进行统计分析，以
研究石油烃的来源及迁移、转化规律。
总之，论文的根本点是从分于水平出发，深入、系统研究了近岸海洋环境各相
介质中石油烃的组成特征及其生物地球化学指示，探索性研究了控制石油烃生物地
球化学行为过程的机理，为海洋环境的保护和管理提供科学依据。
Based on the study of the composition and biogeochemical characteristics of petroleum hydrocarbons (PH) in different interfaces (water-sediment-organisms) in Xiamen Harbour and adjacent area using modern analysis techniques, the biogeochemical process of petroleum hydrocarbons in marine environment were discussed. The results show that:
1. Optimized the conditions of experiments and established the analysis methods of trace petroleum hydrocarbons of samples in different phase. Especially optimized the analysis method of trace components of petroleum hydrocarbons in sediments and calibrated the method using SRM (Standard Reference Material).
2. Quantification index of n-akanes and polycyclic aromatic hydrocarbons (PAHs) were proved as the good biomarker for indicating the biogeochemical process of petroleum hydrocarbons; It was the first time to find the high level of nC 11 in Xiamen water and sediments were related to the coal pollution. Additionally, the high level of Naphthalene were considered with the increasing motor -driven vehicles and the use of camphor ball in hotels and in families in Xiamen City.
3. It was the first time to study the accumulation of each component of petroleum hydrocarbons in microlayer detail. The mechanism of accumulation was discussed. Found that the sources of material controlled the accumulation coefficient of PH in microlayer seawater. When the sources of upper layer and down layer were almost same, microlayer water accumulated even carbons in short chain n-alkanes; accumulated odd carbons in long chain n-alkanes. The accumulation coefficients of alkanes were 6. The accumulation order of microlayer water for PAHs was 5 rings >4 ring >3 rings>2 rings and the coefficients increasing with power series, were related with the solubility, boil and melting points and evaporate degree. Microlayer water accumulate ?PAHs was 1 -5 (mean 3.14).
4. Based on the biogeochemical characteristics of PH between bottom water-pore water-sediments interfaces, found that the short chain n-alkanes and low rings PAHs with high solubility and low melting and boiling points distributed in pore water and the long chain n-alkanes and high rings PAHs with lower solubility and high melting and boiling points distributed in sediments. This partition pattern between sediments and pore water indicated the balance system between water and sediments. The
concentrations of PH in pore water was lower than that in bottom water indicated PH in sediments mainly came from the deposition of PH from bottom water.
5. Combined several kinds of biomarkers, we could guessed that the sources of PH in Xiamen Harbour mainly came from oil-containing waste water discharge, urban water discharge and the combustions of fuels and gasoline; the sources of PH near Jioulong River Estuary mainly was combustion of fossil fuel.
6. Based on the analysis of composition of petroleum hydrocarbon in Oil port core sediment and Haimen Island core sediment, Jiulong sediment were polluted by petroleum hydrocarbon in 1994, oil port sediment were contaminated increasing in recent years.
7. Based on the study of petroleum hydrocarbons in seawater and mussels in fish cages, the accumulation coefficients of organisms for PH very high. Mussels could accumulate n-alakanes for 2500 times and PAHs 1000 times.
8. From the combination experiments of in situ and laboratory, the distribution and transportation characteristic of petroleum hydrocarbons in different tissues of mussels were studied. It was found that the composition and accumulation of petroleum hydrocarbon in mussels were related with the pathway of eating and metabolize processes.
9. The mussels in four fish cages were contaminated by PH, especially in Maluan Bay.
10. This paper were first time to use the statistics software SPSS 10.0 to study the sources, transportation and transform regular.
In the all, the thesis researched the composition characteristics and biogeochemical processes of petroleum hydrocarbons deeply and comprehensively f
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