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湖泊沉积物中有机磷的地球化学特征及其富营养化效应——以太湖、红枫湖、百花湖和洱海为例
其他题名Geochemical Characteristics of Organic Phosphorus in the Lake Sediments and its Effects on Lake Eutrophication: A Case Study of Lake Taihu, Lake Hongfeng, Lake Baihua and Lake Erhai in China
张润宇
2007-10-24
学位授予单位中国科学院地球化学研究所
学位授予地点地球化学研究所
学位名称博士
关键词湖泊富营养化 沉积物 有机磷 形态 组成 有机质 液体磷核磁共振波谱法 长江中下游地区 云贵高原地区
摘要磷是水生生态系统初级生产力的主要限制因子,也是造成湖泊富营养化的关键营养元素。湖泊富营养化现已成为世界性的环境问题,它不但制约了湖泊资源的可利用性,而且直接影响着人类的健康生存与社会经济的可持续发展。沉积物内源磷的释放是决定湖泊水体营养水平、影响湖泊富营养化治理成效的重要因素。因此,研究沉积物中磷的组成形态、含量分布及迁移转化等对于全面了解湖泊生态系统中磷的生物地球化学循环,有效控制和管理湖泊富营养化具有重要的意义。然而目前对沉积物中的无机磷(Pi)及其生物可利用性进行了大量的研究,有机磷(Po)作为沉积物中的重要化学成分,它的地球化学特征及其对湖泊富营养化的作用却了解甚少。 长江中下游地区和云贵高原地区是我国淡水湖泊的主要分布区,也是我国湖泊富营养化最为严重的地区。本论文工作选取两地区具不同流域特征、水文状况、生态结构、污染程度的代表性湖泊(太湖梅梁湾、鼋头渚、贡湖、东太湖, 红枫湖, 百花湖和洱海)为研究对象,结合传统的化学连续提取手段和最新的液体磷核磁共振(31P NMR)波谱分析,研究了这些湖泊沉积物中Po的形态、组成以及剖面分布特征,揭示了Po对湖泊富营养化的重要作用;并运用高效体积排阻色谱法、分子荧光光谱法探讨了它们与沉积物中有机质的关系。主要研究结果如下: 1. 采用改进的土壤Po分级体系研究湖泊沉积物中Po的赋存形态,沉积物中Po的回收率可达94.3-101.1%,平均为98.5±2.2%,说明了该方法基本上包括了沉积物中全部Po。这是因为本方法对活性Po和腐殖质磷萃取的时间更长,提取更为完全;对富里酸磷和胡敏酸磷的区分更加明确;还特别增加了残渣态有机磷(Residual Po)的测定,使得Po的形态分析更为周密和准确。沉积物中Residual Po的含量占总Po的29.9-57.2%,进一步表明了此方法的可取性,这将为以后开展湖泊沉积物中Po的形态研究奠定了基础。 2. 湖泊沉积物中磷形态的不同分布特征可能与两地区不同的湖泊类型、有机质降解过程的差异以及各种磷形态之间的相互转化有关。Po形态在不同污染程度沉积物中的含量与分布也充分说明了沉积物是水体富营养化的主要内源,Po对湖泊富养化的作用不容忽视。 3.太湖梅梁湾、鼋头渚和贡湖沉积物不同提取液中有机质的分子量分布特征可能表明了其中有机质和Po组成的差异,而沉积物中有机C/N和C/P比值分析和三维荧光光谱特征的相似形可能反映了太湖(浅水湖泊)沉积物中有机质与磷的地球化学特性及其相互关系。 4. 31P NMR的测定结果显示,湖泊沉积物中磷主要由正磷酸盐(Ortho-P)、磷酸单酯(Monoester-P)与二酯(Diester-P)组成,焦磷酸盐(Pyro-P)和膦酸盐(Phosphonate)的含量非常低。Ortho-P在重富营养化和浅水湖泊沉积物中的相对含量高于富营养化、中富营养化和深水湖泊沉积物,Monoester-P的分布特征正好相反,表明了这些磷化合物在不同湖泊生态系统磷的循环中的差异。此外,Monoester-P中肌糖磷酸的大量存在,也同时证实了前面Po化学连续提取中高含量的Residual Po。 5. 梅梁湾和洱海沉积物中总磷(TP)、Pi、Ortho-P、Monoester-P、总有机碳(TOC)和总氮(TN)表现出不同的剖面分布特征,说明了有机质和磷在不同湖泊环境中的分解转化规律,可能解释了内源磷的释放对两湖富营养化的影响。此外,Diester-P中DNA-P的剖面变化和前人报道的沉积物中DNA的分布特征正好吻合,表明了DNA-P主要来源于沉积物中细菌和微生物的DNA。
其他摘要Phosphorus is a main limiting agent for the primary production in the aquatic ecosystems, and is also an essential nutrient for lake eutrophication. Nowadays, lake eutrophication is a universal environmental problem which has imposed as a threat to water resource, human health and social sustainable development. Internal phosphorus loading by sediment release plays a big role in the trophic status of the lake water, and affects the lake restoration. Therefore, it is necessary to investigate the composition, form distribution and transformation of phosphorus in the sediments for a comprehensive understanding of phosphorus biogeochemical cycles and for effective control and management of lake eutrophication. However, most of those previous studies mainly focused on inorganic phosphorus (Pi) fractions and their bioavailbility. Little information is available on the geochemical characteristics of organic phosphorus (Po) and its role for lake eutrophication, despite constituting a large proportion of lake sediments. The middle and lower reaches of Yangtze and Southwestern China Plateau are the major two areas not only of freshwater lakes, but also of eutrophication lakes in China. The objectives of this study are to investigate the forms, composition and vertical distributions of Po in the sediments of Meiliang Lake, Yuantouzhu Lake, Gonghu Lake, East Taihu Lake, Hongfeng Lake, Baihua Lake and Erhai Lake (those lakes representing different features, such as, drainage area, hydrodynamic condition, entironment, pollution degree) by applying conventional chemical sequential fractionation and solution 31P nuclear magnetic resonance (NMR) spectroscopy, the role of Po for lake eutrophication was also elucidated. Meanwhile, the relationship between phosphorus and organic matter was discussed using molecular fluorescence spectroscopy and high performance size exclusion chromatography. The conclusions have been reached as follows: 1. The recovery of Po ranged from 94.3% to 101.1%, with the average of 98.5±2.2% by using an improved soil Po fractionation scheme. This suggests that total Po in sediments was satisfactorily extracted with this procedure, due to the longer shaking time for labile Po and Po associated with humic substances and an additional step for residual Po determination, thus the results were relatively accurate for Po concentrations in lake sediments. The proportion of residual Po to total Po reached 29.9–57.2% in these sediments, which indicated that the procedure was feasible to fractionate the sediment Po, and laid a foundation for further investigation of Po forms in lake sediments. 2. Different distribution patterns of P fractions observed in those two different regions may be related to different lake types, different decomposition processes of organic matter and the transformation between Pi and Po fractions in different lake environments. The concentrations of Po fractions in the heavily polluted sediments were higher than those in moderately and no polluted sediments. It is suggested that Po should be paid more attention beside Pi for lake eutrophication. 3. The difference in the molecular weight distributions of organic matter in the various extracts from the sediments of Meiliang Lake, Yuantouzhu Lake and Gonghu Lake may suggest the composition of organic matter and Po differed. However, the similarity of the values of organic C/N and C/P and their three-dimensional fluorescence spectroscopy in these three sediments may elucidate their characteristics and relationships in Taihu Lake (shallow lake). 4. The results showed that the sediment extracts were dominated by orthophosphate (Ortho-P) and orthophosphate monoesters (Monoester-P), with smaller amounts of orthophosphate diesters (Diester-P), pyrophosphate (Pyro-P) and phosphonates by solution 31P NMR spectroscopy analysis. The relative distribution of Ortho-P for hypertrophic and shallow lake sediments was higher than that for eutrophic and mesotrophic and deep lake sediments, while the relative distribution of Monoester-P was the opposite indicated that various P compounds were involved in the P recycling in those lakes to different extents. In addition, the abundance of inositol phosphate in Monoester-P supported the high concentration of residual Po in sediment Po fractionation studies mentioned in earlier chapter. 5. The different profiles of TP、Pi、Ortho-P、Monoester-P、TOC and TN in Meiliang Lake and Erhai Lake sediments suggested that the mechanisms of decomposition and transformation of organic matter and phosphorus varied in different lake environments. This may explain the role of internal loading for lake eutrophication in these two lakes. Furthermore, the occurrence of DNA-P detected in the surface sediments is consistent with the distribution of DNA reported previously. It is suggested that DNA-P in sediments mostly originated from DNA of bacteria and microorganisms.
页数114
语种中文
文献类型学位论文
条目标识符http://ir.gyig.ac.cn/handle/352002/3268
专题研究生_研究生_学位论文
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张润宇. 湖泊沉积物中有机磷的地球化学特征及其富营养化效应——以太湖、红枫湖、百花湖和洱海为例[D]. 地球化学研究所. 中国科学院地球化学研究所,2007.
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