黄河及河口烃类有机物的分布特征及源解析
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摘要
黄河是中国的第二大河，世界上著名的高浊度河流，其陆源碳的入海对渤海乃至整个西北太平洋边缘海的生物地球化学过程会产生重要影响，为了更好的了解黄河及河口地区有机碳来源及其迁移转化规律，本论文采用正构烷烃、多环芳烃和脂肪酸三种烃类化合物作为生物标志物，对黄河不同区段以及黄河口水、悬浮颗粒物、沉积物中三种烃类化合物的分布特征及物源进行了较为系统的研究，同时对黄河口利津站不同粒径悬浮颗粒物中正构烷烃和多环芳烃的分布特征也作了探讨。本文内容主要有五部分：①黄河流域正构烷烃的分布及物源分析；②黄河流域脂肪酸的分布及物源分析；③黄河流域多环芳烃的分布及物源分析；④黄河口悬浮颗粒物中烃类化合物的分布及其对有机碳运移的解释；⑤黄河口沉积物中烃类化合物的分布及其对有机碳运移的解释。主要实验结果和结论如下：
黄河水体正构烷烃浓度为5μg/L-31．57μg/L，脂肪酸总浓度在1．63μg／L-40．09μg/L之间，16种多环芳烃的总浓度为118．27 ng／L-979．15 ng／L。烃类化合物的分布具有明显的地域差异，TSS是水体中烃类化合物分布的主要影响因素，浮游生物及微生物等对烃类化合物的分布也有一定影响。正构烷烃以陆源优势为主，脂肪酸以水生源为主，总体上黄河上游水体有机质陆源优势强于中、下游，下游水生源优势较强。多环芳烃除银川以高环为主外，其余断面均以2-3环为主。各断面多环芳烃主要来源于草木、煤等的燃烧，潼关、银川受到一定程度的石油污染。除贵德和刘家峡外，其余断面溶解态苯并[a]芘均超过生活饮用水卫生标准。
黄河口颗粒态正构烷烃和正脂肪酸浓度有明显的季节差异，4月，正构烷烃含量为7．01μg／g-33．62μg／g，正脂肪酸含量为2．11μg／g-14．59μg／g，随盐度的增加而增加。正构烷烃L／H比值为0．41-0．65，在高盐度区水生源优势最强，在盐度1-13区间，呈现较强的陆源优势；9月，正构烷烃含量为11．83μg／g-74．80μg／g，正脂肪酸含量为8．8 1μg／g-49．23μg／g，整体随离岸距离的增加而降低，9月低盐度区L／H比值与4月相近，高盐度区低于4月，说明9月高盐度区陆源优势强于4月，分析认为沉积物再悬浮是导致这种现象的主要因素。黄河口淡水区多环芳烃含量为393．16 ng／g，主要来源于热解源，混合区PAHs含量为781．35 ng／g，受石油源和热解源共同影响。
论文对黄河口利津站正构烷烃和多环芳烃随悬浮物的粒级分布做了研究，结果表明烃类合物的含量在不同粒级颗粒物中的分布具有很大的差别。与POC随粒级的分配趋势相近，烃类化合物也主要分布在小颗粒粒级中，小于32μm的细颗粒承载了绝大部分的正构烷烃和多环芳烃。调查显示黄河口颗粒态正构烷烃受陆源和水生源的共同影响，其中细颗粒悬浮物中水生源正构烷烃的优势更为明显；多环芳烃主要来源于热解源，32-63μm粒级颗粒物中多环芳烃燃烧源贡献最低。
黄河口表层沉积物正构烷烃含量为0．38μg/g-2．55μg／g，正脂肪酸含量为0．08μg／g-0．26μg／g，多环芳烃含量0．371μg／g-0．650μg／g。烃类化合物分布特征不同，从空间分布趋势看，南线受黄河水影响较强，除正脂肪酸在口门附近较高外，正构烷烃和多环芳烃的含量都随离岸距离的增加而增加。正构烷烃以陆源为主，正脂肪酸主要以水生源为主。综合分析，认为黄河口南线沉积物有机质随离岸距离的增加，受陆源影响减弱，受水生源的影响增强。沉积物中多环芳烃主要来自于热解源，中环多环芳烃呈现较为明显的优势。北线受黄河水影响较弱，整体呈现陆源和水生源共同作用的结果，受胜利油田及陆源污染的影响，在口门附近3种烃类化合物含量都比较高，正构烷烃色谱峰显示存在微弱的不能分辨包状组分，多环芳烃也呈现燃烧源和石油源共同来源。
The Yellow River is the second longest river in China.As one of the highest tubidriver in the world,it has important effect on carbon cycle of North-west Pacific Ocean.To better understand the distributions and sources of organic matter in the YellowRiver and its Adjacent Sea,n-alkanes,fatty acids and polycyclic aromatichydrocarbons (PAHs) were choosed as the biomakers.The distributions and sourcesof the three kinds of hydrocarbons in water,suspended and sedimentary particles fromthe Yellow River and its Adjacent Sea were discussed,and the size distributions ofPAHs and n-alkanes in suspended particles at Lijin Hydrographic Station were studied.The following five sections were discussed in the present thesis:①The distributionand sources of n-alkanes in the Yellow River;②The distribution and sources of fattyacids in the Yellow River;③The distribution and sources of PAHs in the YellowRiver;④Compositional feature of hydrocarbons in suspended particles from theYellow River Estuary and its implication to transport and distribution of organiccarbon。⑤Compositional feature of hydrocarbons in sediment particles from theYellow River Estuary and its implication to transport and distribution of organiccarbon。
The particulate samples from the Yellow River in surface water were collected inautumn,2003 and July,2007 respectively.The results show that the concentrations ofn-alkanes,fatty acids and PAHs are 7.01μg/g-33.62μg/g,2.11μg/g-14.59μg/g and118.27 ng/L-979.15 ng/L respectively.The hydrocarbons in the suspended particulatesamples from the Yellow River show a spatial characteristic.Terrestrial organic mattermakes a major contribution for particulate n-alkanes and aquatic organic matter makesa major contribution for particulate fatty acids.More terrestrial organic matter isfound in the upper reaches than that in lower reaches.The relative proportions of 16 PAHs in all stations are similar,and the 2-3 ring PAHs play a most important role inall the stations except Yinchuan.Source analysis reveals that PAHs mainly originatefrom coal burning.PAHs originating from combustion of petroleum cannot be ignoredin Yinchuan and Tongguan.The concentrations of benzo[a]pyrene are all abovedrinking water standards in most of the stations sampled except Guide and Liujiaxia.
The concentrations of n-alkanes and fatty acids show a marked seasonal differencein the Yellow River Estuary.In April,the content of alkane is 7.01μg/g-33.62μg/g,and the content of fatty acid is 2.11μg/g-14.59μg/g.The contents of both alkane andfatty acid increase with the increasing of the salinity.L/Hs of n-alkane are rangedfrom 0.41 to 0.65.Aquatic organic matter plays an important role in the higher salinityregions,and terrestrial organic matter plays an important role at salinity of 1-13;inSeptember,the content of alkane is 11.83μg/g-74.80μg/g,and the content of fattyacid is 8.81μg/g-49.23μg/g.The contents of both alkane and fatty acid increase withthe decreasing of the distance from the coast.The L/Hs are similar to that in April inlow salinity and L/Hs are lower than that in April in high salinity,which is seem as theresult of sediment resuspension.The content of PAHs in the freshwater is 393.16 ng/g,which is lower than 781.35 ng/g,the content of PAHs in the mixing zone.The PAHsmainly originate from coal burning in the freshwater,and PAH inputs could comefrom petroleum.and coal burning in the mixing zone。
Suspended particle samples from the Yellow River estuary were sorted into fivegrain size fractions to explore the effect of grain size distribution on organic mattercontent and composition.The results show that there are distinct differences in theorganic material associated with individual grain size fractions corresponding todifferences in content and composition.PAHs and n-alkanes are more abundant in thefiner fractions and fine particles (＜32μm) play a significant role in organic matter.This investigation shows that particulate n-alkanes in the Yellow River estuary consistof a mixture of compounds from terrigenous and riverine biogenic n-alkanes and morebiogenic n-alkanes accumulate in finer particles.Particulate PAHs are related tocombustion/pyrolysis processes of coal/wood combustion,and less pyrolytic PAHsare found in the particles with diameter from 32 to 63μm.
Concentrations of n-alkane,fatty acids and PAHs are 0.38μg/g-2.55μg/g,0.08-0.26μg/g and 0.371μg/g-0.650μg/g in the sediments from the Yellow River Estuary,respectively.Significant differences are observed between the north route and thesouth route.With the effect of the water from the Yellow River in the south route,thehydrocarbons increase with the increasing of the distance from the coast.The fartheraway from the river,the less terrestrial organic matter is observed in the estuary.ThePAHs mainly originate from coal burning.The 4-ring PAHs are predominant insediment PAHs.With the effect of the oilfield near the Huanghe delta,the levels ofthree kinds of hydrocarbons show the highest level in the mouth.The UCM ofn-alkane is found and PAHs origin from the mixture of combustion and petroleum inthe sample from the N 1 location.
黄河水体正构烷烃浓度为5μg/L-31．57μg/L，脂肪酸总浓度在1．63μg／L-40．09μg/L之间，16种多环芳烃的总浓度为118．27 ng／L-979．15 ng／L。烃类化合物的分布具有明显的地域差异，TSS是水体中烃类化合物分布的主要影响因素，浮游生物及微生物等对烃类化合物的分布也有一定影响。正构烷烃以陆源优势为主，脂肪酸以水生源为主，总体上黄河上游水体有机质陆源优势强于中、下游，下游水生源优势较强。多环芳烃除银川以高环为主外，其余断面均以2-3环为主。各断面多环芳烃主要来源于草木、煤等的燃烧，潼关、银川受到一定程度的石油污染。除贵德和刘家峡外，其余断面溶解态苯并[a]芘均超过生活饮用水卫生标准。
黄河口颗粒态正构烷烃和正脂肪酸浓度有明显的季节差异，4月，正构烷烃含量为7．01μg／g-33．62μg／g，正脂肪酸含量为2．11μg／g-14．59μg／g，随盐度的增加而增加。正构烷烃L／H比值为0．41-0．65，在高盐度区水生源优势最强，在盐度1-13区间，呈现较强的陆源优势；9月，正构烷烃含量为11．83μg／g-74．80μg／g，正脂肪酸含量为8．8 1μg／g-49．23μg／g，整体随离岸距离的增加而降低，9月低盐度区L／H比值与4月相近，高盐度区低于4月，说明9月高盐度区陆源优势强于4月，分析认为沉积物再悬浮是导致这种现象的主要因素。黄河口淡水区多环芳烃含量为393．16 ng／g，主要来源于热解源，混合区PAHs含量为781．35 ng／g，受石油源和热解源共同影响。
论文对黄河口利津站正构烷烃和多环芳烃随悬浮物的粒级分布做了研究，结果表明烃类合物的含量在不同粒级颗粒物中的分布具有很大的差别。与POC随粒级的分配趋势相近，烃类化合物也主要分布在小颗粒粒级中，小于32μm的细颗粒承载了绝大部分的正构烷烃和多环芳烃。调查显示黄河口颗粒态正构烷烃受陆源和水生源的共同影响，其中细颗粒悬浮物中水生源正构烷烃的优势更为明显；多环芳烃主要来源于热解源，32-63μm粒级颗粒物中多环芳烃燃烧源贡献最低。
黄河口表层沉积物正构烷烃含量为0．38μg/g-2．55μg／g，正脂肪酸含量为0．08μg／g-0．26μg／g，多环芳烃含量0．371μg／g-0．650μg／g。烃类化合物分布特征不同，从空间分布趋势看，南线受黄河水影响较强，除正脂肪酸在口门附近较高外，正构烷烃和多环芳烃的含量都随离岸距离的增加而增加。正构烷烃以陆源为主，正脂肪酸主要以水生源为主。综合分析，认为黄河口南线沉积物有机质随离岸距离的增加，受陆源影响减弱，受水生源的影响增强。沉积物中多环芳烃主要来自于热解源，中环多环芳烃呈现较为明显的优势。北线受黄河水影响较弱，整体呈现陆源和水生源共同作用的结果，受胜利油田及陆源污染的影响，在口门附近3种烃类化合物含量都比较高，正构烷烃色谱峰显示存在微弱的不能分辨包状组分，多环芳烃也呈现燃烧源和石油源共同来源。
The Yellow River is the second longest river in China.As one of the highest tubidriver in the world,it has important effect on carbon cycle of North-west Pacific Ocean.To better understand the distributions and sources of organic matter in the YellowRiver and its Adjacent Sea,n-alkanes,fatty acids and polycyclic aromatichydrocarbons (PAHs) were choosed as the biomakers.The distributions and sourcesof the three kinds of hydrocarbons in water,suspended and sedimentary particles fromthe Yellow River and its Adjacent Sea were discussed,and the size distributions ofPAHs and n-alkanes in suspended particles at Lijin Hydrographic Station were studied.The following five sections were discussed in the present thesis:①The distributionand sources of n-alkanes in the Yellow River;②The distribution and sources of fattyacids in the Yellow River;③The distribution and sources of PAHs in the YellowRiver;④Compositional feature of hydrocarbons in suspended particles from theYellow River Estuary and its implication to transport and distribution of organiccarbon。⑤Compositional feature of hydrocarbons in sediment particles from theYellow River Estuary and its implication to transport and distribution of organiccarbon。
The particulate samples from the Yellow River in surface water were collected inautumn,2003 and July,2007 respectively.The results show that the concentrations ofn-alkanes,fatty acids and PAHs are 7.01μg/g-33.62μg/g,2.11μg/g-14.59μg/g and118.27 ng/L-979.15 ng/L respectively.The hydrocarbons in the suspended particulatesamples from the Yellow River show a spatial characteristic.Terrestrial organic mattermakes a major contribution for particulate n-alkanes and aquatic organic matter makesa major contribution for particulate fatty acids.More terrestrial organic matter isfound in the upper reaches than that in lower reaches.The relative proportions of 16 PAHs in all stations are similar,and the 2-3 ring PAHs play a most important role inall the stations except Yinchuan.Source analysis reveals that PAHs mainly originatefrom coal burning.PAHs originating from combustion of petroleum cannot be ignoredin Yinchuan and Tongguan.The concentrations of benzo[a]pyrene are all abovedrinking water standards in most of the stations sampled except Guide and Liujiaxia.
The concentrations of n-alkanes and fatty acids show a marked seasonal differencein the Yellow River Estuary.In April,the content of alkane is 7.01μg/g-33.62μg/g,and the content of fatty acid is 2.11μg/g-14.59μg/g.The contents of both alkane andfatty acid increase with the increasing of the salinity.L/Hs of n-alkane are rangedfrom 0.41 to 0.65.Aquatic organic matter plays an important role in the higher salinityregions,and terrestrial organic matter plays an important role at salinity of 1-13;inSeptember,the content of alkane is 11.83μg/g-74.80μg/g,and the content of fattyacid is 8.81μg/g-49.23μg/g.The contents of both alkane and fatty acid increase withthe decreasing of the distance from the coast.The L/Hs are similar to that in April inlow salinity and L/Hs are lower than that in April in high salinity,which is seem as theresult of sediment resuspension.The content of PAHs in the freshwater is 393.16 ng/g,which is lower than 781.35 ng/g,the content of PAHs in the mixing zone.The PAHsmainly originate from coal burning in the freshwater,and PAH inputs could comefrom petroleum.and coal burning in the mixing zone。
Suspended particle samples from the Yellow River estuary were sorted into fivegrain size fractions to explore the effect of grain size distribution on organic mattercontent and composition.The results show that there are distinct differences in theorganic material associated with individual grain size fractions corresponding todifferences in content and composition.PAHs and n-alkanes are more abundant in thefiner fractions and fine particles (＜32μm) play a significant role in organic matter.This investigation shows that particulate n-alkanes in the Yellow River estuary consistof a mixture of compounds from terrigenous and riverine biogenic n-alkanes and morebiogenic n-alkanes accumulate in finer particles.Particulate PAHs are related tocombustion/pyrolysis processes of coal/wood combustion,and less pyrolytic PAHsare found in the particles with diameter from 32 to 63μm.
Concentrations of n-alkane,fatty acids and PAHs are 0.38μg/g-2.55μg/g,0.08-0.26μg/g and 0.371μg/g-0.650μg/g in the sediments from the Yellow River Estuary,respectively.Significant differences are observed between the north route and thesouth route.With the effect of the water from the Yellow River in the south route,thehydrocarbons increase with the increasing of the distance from the coast.The fartheraway from the river,the less terrestrial organic matter is observed in the estuary.ThePAHs mainly originate from coal burning.The 4-ring PAHs are predominant insediment PAHs.With the effect of the oilfield near the Huanghe delta,the levels ofthree kinds of hydrocarbons show the highest level in the mouth.The UCM ofn-alkane is found and PAHs origin from the mixture of combustion and petroleum inthe sample from the N 1 location.
引文
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