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红枫湖、百花湖水中溶解有机物分子量分布特征及环境地球化学意义
其他题名Molecular weight distribution of dissolved organic matter in natural water collected in Hongfeng Lake and Baihua Lake
岳兰秀
2004
学位授予单位中国科学院地球化学研究所
学位授予地点中国科学院地球化学研究所
学位名称博士
学位专业环境地球化学
关键词红枫湖 百花蝴 溶解有机物 溶解有机碳 平均分子量 分子量分布 高效体积排阻色谱 有机物降解
摘要溶解有机物(dissolved organio matter, DOM)通常是指能够通过0.45μm滤膜的有机物质。0.45μm的定义是根据传统的过滤滤膜直径来划分的,不是一个绝对的定义。DOM在水环境中起着重要的作用,它是水环境中重要的配位体和吸附载体。DOM在水化学和生态环境中的重要作用,主要表现在它不仅可以和基本的金属离子和有机化合物结合,还可以与毒性金属离子和除草剂、杀虫剂结合(wershow ond Goldberg,1972)。湖泊水中DoM的浓度及物理化学性质能够影响水生态环境的结构及初级生产力。溶解有机物按元素组成来分,主要含有C、O、H、N、P、S以及灰分。按重量计算,其中C占总有机物的50%,其次是O(科O%)、H(一5%)、N(0.5~6.5%)、P(<1.0%)、S(<1.0%)和灰分(1.2-5.0%)(Thurman,1985)。DOM一般由多种有机化合物组成,其中腐殖物质是溶解有机质的主要组成部分,一般占有机质总量的50-80%。目前通常可人为地将腐殖物质划分为胡敏素、胡敏酸和富里酸(Aiken et oL,1 985)。其余的非腐殖类物质主要包括碳水化合物、氨基酸、叶绿素、藻类分泌物、酚酮类化合物、脂肪酸和亲水性有机酸等(Thurman,1985)a在水环境中一些金属离子和微量元素通常和DOM相结合,而这些元素的作用和在水中的迁移都受DoM的分子量分布的影响(chiou etal.,1986)。 DOM的分子量及其分布是指示水质量的一个重要参数,同时在水处理过程中对于研究DOM的去处效率有重要作用(vuorio et oL,1998)。具有不同分子量分布的DOM与金属的络合能力也不同,则它们对金属的生物有效性的作用就不同(wuetal.,2002)。分子量变化的程度可以进一步理解DOM的自然形成过程,也可以在弓!用水处理过程中优化腐殖质的去除过程。红枫湖和百花湖是贵州地区两个人工水库,通过对两湖水文条件的测量,探讨了影响DOM分子量及分布变化的环境因素,包括溶解氧的含量、水体温度、pH值、叶绿素。的含量、光照强度、藻类生长情况、生物活动等,以及溶解有机物的来源,人为污染情况等。本文采样高效体积排阻色谱法(High PerformanceSizeExclusion cbromatograP场,HPsEC)测量了红枫湖、百花湖水中的DOM的含量及分子量分布,得出了以下几点认识:1、选择HPsEC实验的最佳条件:0.03M NaCl和0.002的磷酸盐缓冲液作为流动相,pH为6.8,离子强度为0.034mol几,紫外检测波长为254nm。2、红枫湖、百花湖水中DOM主要以分子量小于3500Da的组分为主,占总溶解有机物的90%以上。根据洗脱曲线的峰面积,可以把DOM分为3个不同 分子量的组分,其中大分子量组分(MW>2000Da)的含量占总DOM的35%一68%;中等分子量组分(Z000Da>MW>1000Da)的含量为27%-57%;小分子量组分(MW<1000Da)占总DOM的3%一31%。 3、红枫湖、百花湖水中Doc含量受气候条件的影响。丰水期,水体上部DOC含量较大,下部较小‘平水期和枯水期,上下水体中DOC含量一致。各组分DOc含量变化与总DOC含量变化相似。DOC含量也表现出明显的季节性变化特征。丰水期DOC含量较高,而在平水期和枯水期含量较低。红枫湖和百花湖二者之间DOC含量没有明显的差别。4、红枫湖、百花湖水中DOM平均分子量也受气候条件的影响。丰水期,随深度的增大,DoM平均分子量增大;平水期和枯水期,上下水体DOM平均分子量一致。DO入左的季节性变化与DOC相反,丰水期,DOM平均分子量偏低;而在平水期和枯水期,DOM平均分子量偏高。5、重均分子量和数均分子量虽然变化趋势相似,但是它们的变化幅度不同,所以多分散系数也会发生变化。总的来说,在水体上部多分散系数偏大,水体下部偏小。丰水期多分散系数较大,平水期和枯水期多分散系数较小。6、随着气候条件的变化,各分子量组分的DOM含量及DOC浓度也在发生变化。大分子量组分随深度而增大,而中等和小分子量组分随深度而减小。丰水期,中等和小分子量组分含量较多,而大分子量组分较少;平水期和枯水期,大分子量组分含量较多,中等和小分子量组分含量较少。
其他摘要Dissolved organic matter (DOM) is operationally defined as the fraction of organic carbon that passes through a 0.45μm filter. The 0.45μm definition is an arbitrary cut-off, which is based on the historical availability of this filter pore size. DOM plays a central role in aquatic environment. It is an important ligand and sorbent. The importance in aquatic chemistry and aquatic ecosystems is expressed by altering the bioavailability of metals, organic contaminants such as ployaromatic hydrocarbons (Driscoll et al. 1990; Oris et al., 1990), as well as increasing the attenuation of visible and ultraviolet radiation and contributing to the natural acidity of waters (Wetzel, 1983; Driscoll et al., 1989). Both the concentration as well as the chemical and physical nature of DOM in lakes can also greatly influence the productivity and structure of aquatic ecosystems. DOC is approximately 50% carbon by weight; the remaining elemental composition comprises oxygen (40%), hydrogen (5%), nitrogen (0.5% to 6.5%), phosphorous (<1.0%), sulfur (<1.0%) and ash (1.2-5.0%) (Thurmanl985). DOM is a complex organic compound. The humic substance occupied 50-80 percent of DOM, which was divided into three parts, including humic acid, futvic acid and humin. The nonhumic substances contain hydrocarbons, amino acid, chlorophyll, algae, phenolic, etal. (Thurman, 1985). Some metal ion and minim element always combine with DOM. The effect of these elements in water is influenced by their molecular weight. The molecular weight of DOM within lakes provides valuable insight into the potential of a particular system to reduce the level of contaminant toxicity. By elucidating the relationship between the structural character or molecular size of DOC and the role it plays in the environment, we can begin to understand, and further, to model the response of freshwater lakes and streams to anthropogenic stresses and circumstances that may arise from climate change. Lake Hongfeng and Baihua arc the two large manual reservoirs, which situated on the Guizhou Plateau. The two reservoirs are the main sources of drinking water in Guiyang. The source of water comes from some streams in drainage area. By determinate the hydrological environment, we discussed the factors that affected the variation of molecular weight distribution of dissolved organic matter, including the abundance of dissolved oxygen, temperature of water, pH value, chlorophyll a, illumination, and bloom of plankton, the origin of dissolved organic matter, the contaminate by human. This research has determined the molecular weight distribution of DOM in Lake Hongfeng and Baihua by HPSEC. Some conclusions were obtained. The optimal experimental condition was collected, including the mobile phase of 0.O3M NaCl and 0.002 phosphate buffer, the pH value of 6.8, the ion strength of 0.034 mol/L, the wavelength of 254 nm. 2 The DOM molecule with molecular weight higher 3000Da occupied the largest part of DOM, account for higher 90 percent. By the peak area of each fraction, we divided the DOM into three fractions with different molecular weight. The large fraction with molecular weight higher than 2000 Da occupied 35% to 68% of total DOM. The medium fraction with 2000Da>MW>1000Da consisted of 27 to 57 percent of total DOM. And small fraction with molecular weight smaller than lOOODa only occupied 3 to 31 percent of total DOM. 3 The content of DOC was influenced by weather. The content of DOC in upper water is higher than that in deeper water in rain season. The carbon content remains relative constant in water column in dry season. The change of carbon content of each fraction is similar with that of the total DOC. The content of DOC also changes with season. It is higher in rain season than that in dry season. But the difference between the two lakes is not remarkable. 4 The averaged molecular weight is also influenced by climate. It becomes higher with depth of water column in rain season. And it remains relative constant in dry season. The variable with season is opposite with that of DOC. It is smaller in dry season than that in rain season. 5 The variable of weight averaged molecular weight and number averaged molecular weight is similar. But the extent of variable is not same. So the polydisperse coefficient changes with depth. It is higher in upper water than that in deeper water. It also higher in rain season, and lower in dry season. The content of fraction DOM and concentration also change with climate. The large fraction becomes higher with depth, and the medium and small fraction lower. 6 The content of medium and small fraction is higher in rain season, and lower in dry season. The content of large is higher in dry season, and lower in rain season.
页数120
语种中文
文献类型学位论文
条目标识符http://ir.gyig.ac.cn/handle/352002/3680
专题研究生_研究生_学位论文
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岳兰秀. 红枫湖、百花湖水中溶解有机物分子量分布特征及环境地球化学意义[D]. 中国科学院地球化学研究所. 中国科学院地球化学研究所,2004.
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