渤海水体中溶解态黑碳的时空分布与来源通量

	渤海水体中溶解态黑碳的时空分布与来源通量
其他题名	The Spatial-temporal Vairations of Dissolved Black Carbon in the the Bohai Sea Water, China and the River Fluxes
	黄国培
学位类型	博士
导师	陈颖军 ; 田崇国
	2016-05-22
学位授予单位	中国科学院大学
学位授予地点	北京
学位专业	环境科学
关键词	溶解态黑碳渤海时空变化河流入海通量渤海储量
其他摘要	溶解态黑碳广泛存在于各类天然水体中，是溶解有机碳的重要成分。它的分子结构中含有浓缩稠环芳香核，芳香核的外周带有亲水性官能团，H/C和O/C的比值明显不同于溶解有机碳中常见的生物源成分和腐殖质类物质，具有富碳贫氢的特征。浓缩稠环结构是有机质经受高温（通常情况下为燃烧）后产生的特征性结构，其产物即通常所称的“黑碳”。黑碳是疏水性富碳颗粒物。溶解有机碳中含有黑碳标志性结构的一类物质被称为“溶解态黑碳”。研究已证实溶解态黑碳的前身是黑碳。因此，溶解态黑碳指一类含有亲水性官能团可溶于水且来源于高温（燃烧）过程的浓缩稠环有机化合物。溶解态黑碳涉及到黑碳和碳循环、污染物的迁移和生物可利用性、水生生态系统的初级生产力以及水体水质等诸多气候、环境和生态问题，成为当前的研究热点。溶解态黑碳是黑碳的降解中间产物，水体是黑碳两个主要储库——陆地土壤和海洋沉积物的联接体，因此水体是黑碳的重要中间储库。我国华北地区是黑碳排放的高强度区，而渤海是华北地区各类染污物（包括黑碳）的重要汇集地。为了调查渤海地区河流-海洋系统水体中溶解态黑碳的浓度时空分布、源-汇过程及控制因素，2010年到2014年，分季节分层位采集渤海和黄海水样1155个，同时分季节采集环渤海45条主要河流水样119个，在建立和优化溶解态黑碳分析方法——苯多羧酸分子标记物法的基础上分析水样中溶解态黑碳的浓度，并同时分析溶解有机碳、颗粒态黑碳、颗粒有机碳和悬浮颗粒物的浓度。结合温盐数据、流场、河流水文、降雨等信息，讨论了渤海地区河流-海洋系统中溶解态黑碳的迁移过程，估算了河流溶解态黑碳的入海通量和渤海水体中溶解态黑碳的储量。环渤海入海河流水体中溶解态黑碳的浓度范围为79.5 - 1328.0 µg L^-1，平均值为341.6 ± 209.3 µg L^-1，中值为303.3 µg L^-1（n = 115），居于全世界河流溶解态黑碳的浓度范围内。渤海水体中溶解态黑碳的浓度范围为36.5 - 208.3 μg L^-1，平均值为85.5 ± 27.1 μg L^-1，中值为82.9 μg L^-1（n = 846），高于黄海水体中溶解态黑碳的浓度，与美国海岸带水体中溶解态黑碳的浓度相当，显著高于开放大洋水体中溶解态黑碳的浓度。河流和海洋水体中溶解态黑碳的浓度均具有显著的时空三维变化特征，呈现河流-近岸-近海-远海明显递减的趋势。河流水体溶解态黑碳的浓度具有显著的流域空间差异，表现为渤海湾和莱州湾入海河流溶解态黑碳的浓度明显高于辽东湾和北黄海北岸入海河流溶解态黑碳的浓度，其平均值分别为488.0 ± 219.1、385.7 ± 192.1、218.3 ± 87.0和124.7 ± 25.5 µg L^-1。与之相对应，渤海湾和莱州湾水体中溶解态黑碳的浓度也高于辽东湾水体中溶解态黑碳的浓度，其平均值分别为105.1 ± 24.7、117.6 ± 33.2、和90.9 ± 14.3 μg L^-1。渤海海湾水体中溶解态黑碳的浓度高于渤海中部和黄海水体中溶解态黑碳的浓度，它们的平均值分别为75.1 ± 19.5和56.4 ± 14.3 μg L^-1。在垂直空间上，由于渤海水深较浅，水体上下容易混合，从而使渤海水体中溶解态黑碳的浓度在垂向上变化很小。在时间变化角度上，环渤海河流水体中溶解态黑碳的浓度表现为平水期最高、丰水期次之、枯水期最低；由于受到河流入海通量的年际变化影响，2013年夏-秋季渤海湾和莱州湾水体中溶解态黑碳的浓度（平均值分别为136.2 ± 34.3和131.2 ± 30.7 μg L^-1）高于2014年夏-秋季渤海湾和莱州湾水体中溶解态黑碳的浓度（平均值分别为107.4 ± 28.0和95.5 ± 12.1 μg L^-1）；由于在冬季强劲的偏北季风影响下，渤海沿岸流显著增强，进而使渤海海湾与渤海中部的水交换速率明显加大，从而呈现出渤海中部水体中溶解态黑碳的浓度在冬季明显高于其他三个季节，2010 - 2011年冬、春、夏和秋季4个航次的平均浓度分别为87.0 ± 22.1、73.9 ± 17.3、73.7 ± 19.2和79.8 ± 21.9 μg L^-1。 2014年环渤海河流溶解态黑碳的入海量为7.43 ± 1.51 Gg，其中黄河的贡献率达到25.9%。环渤海河流以约占全世界河流0.84‰的入海水量输送了约占全世界河流携带至海洋的溶解态黑碳通量的0.28‰。渤海水体中溶解态黑碳的储量为113.81 Gg。 ; Dissolved black carbon (DBC) is an important component of dissolved organic carbon and ubiquitous in natural waters. Its molecular structure is consisted of a condensed aromatic core usually contains four to seven aromatic rings and peripherally substituted by hydrophilic function groups. Dissolved black carbon is carbon-rich and hydrogen-deficient substances and its ratios of H/C and O/C are distinctly different from the common components derived from biomass and humic substances. The condensed aromatic structures are the characteristical molecular structures derived from heating-processes (commonly combustion), whose by-production is well known as “black carbon”. Black carbon is hydrophobic and carbon-rich particles. A series of compounds containing the characteristic structures of black carbon in dissolved organic carbon is given the name of “dissolved black carbon”. It has been proven that the precursor of dissolve black carbon is black carbon. Therefore, dissolved black carbon is a term to describe a series of condensed aromatic compounds which are derived from heating-processes (combustion) and are able to dissolve in water because of containing hydrophilic function groups. Dissolved black carbon has potential impacts on black carbon and carbon cycle, the translocation and biological availability of pollutants, the primary production of aquatic biological system, the quality of natural water and something-like these issues on the climate change, environment, biology and ecology. Dissolved black carbon has been a hot spot nowadays. Dissolved black carbon is the intermediate production of black carbon decomposition and water is the connector of the two major pools of black carbon, terrestrial soil and marine sediment, thus hydrosphere should be an important intermediate pool of black carbon. The North China Plane has high density emission of black carbon and the Bohai Sea is the major pool of pollutions including black carbon emitted from the North China Plane. To investigate the concentrations, distributions, spatial-temporal variations, source-sink and its control factors of dissolve black carbon in the river-sea water system of the Bohai sea, 1155 seawater samples were taken in different seasons and water depth in the Bohai Sea and the Yellow Sea from 2010 to 2014, meanwhile 119 river water samples were taken in 45 rivers entering the Bohai Sea and the North Yellow Sea during the high flow, low flow and normal flow seasons. The concentrations of dissolved black carbon were measured by the benzene polycarboxylic acid method, a molecular marker method after establishment and optimization in our laboratory. The concentrations of organic carbon, particulate black carbon, particulate organic carbon and suspended particulate matter were also measured. The geochemistry dynamics of dissolved black carbon was discussed according the seawater temperature and salinity, water currents, river hydrodynamics, precipitation and something like these physical parameters. The river fluxes and the Bohai Sea inventory of dissolved black carbon were also estimated. The concentrations of dissolved black carbon in the rivers were ranged from 79.5 to 1328.0 µg L^-1, with mean value of 341 ± 209.3 µg L^-1 and median value of 303.3 µg L^-1（n = 115）, within the concentrations ranges of dissolved black carbon among the world rivers. And the concentrations of dissolved black carbon in the Bohai sea were ranged from 36.5 to 28.3 µg L^-1, with mean value of 85.5 ± 27.1 µg L^-1 and median value of 82.9 µg L^-1（n = 846），higher than that in the Yellow Sea water, comparable to the coastal zone area seawater of America, but much higher than that in the open ocean seawater. The concentrations of dissolved black carbon in the rivers and the sea both had three-dimensional spatial-temporal variations, decreasing from river to coastal zone, offshore and to outer sea. The concentrations of dissolved black carbon in different river catchments had distinct spatial variations. It was obvious that the concentrations of dissolved black carbon in the rivers entering the Bohai Bay and the Laizhou Bay were much higher than those rivers entering the Liaodong Bay and North Yellow Sea along the Liaonig Province coastal line. And the average concentrations of dissolved black carbon in the rivers entering the Bohai Bay, Laizhou Bay, Liaodong Bay and the North Yellow Sea along the Liaonig Province coastal line were 488.0 ± 219.1, 385.7 ± 192.1, 218.3 ± 87.0 and 124.7 ± 25.5 µg L^-1 respectively. The concentrations of dissolved black carbon in the Bohai Bay and Laizhou Bay seawater were higher than that in the Liaodong Bay seawater, consistent with the concentrations difference of dissolved black carbon among the rivers. The average concentrations of dissolved black carbon were 105.1 ± 24.7、117.6 ± 33.2 and 90.9 ± 14.3 μg L^-1 in the Bohai Bay, Laizhou Bay and Liaodong Bay respectively. What’s more, the concentrations of dissolved black carbon were higher in the Bays than the Central Bohai Sea and the Yellow Sea whose average concentrations of dissolved black carbon were 75.1 ± 19.5 and 56.4 ± 14.3 μg L^-1 respectively. On contrast, the concentractions of dissolved black carbon had no significant difference in the vertical water column and the main reason was that the Bohai Sea is a shallow sea where the water can be easily vertically mixed well by wave and tide. On the temporal view, the concentractions of dissolved black carbon in the rivers were the highest in the normal flow season, second higher in the high flow season and the lowest in the low flow season. In late summer and early autumn season, the concentractions of dissolved black carbon in the Bohai Bay and the Laizhou Bay were higher in 2013 ( average concentractions were 136.2 ± 34.3 and 131.2 ± 30.7 μg L^-1 respectively ) than 2014 ( average concentractions were 107.4 ± 28.0 and 95.5 ± 12.1 μg L^-1 respectively ) mainly because that the river fluex of dissolved black carbon had interannual variation. The concentractions of dissolved black carbon in the Central Bohai Sea were significant higher in winter than the other three seasons. The average concentractions of dissolved black carbon in winter, spring, summer, and autumn were 87.0 ± 22.1, 73.9 ± 17.3, 73.7 ± 19.2 and 79.8 ± 21.9 μg L^-1 respectively from the year of 2010 to 2011 in the Central Bohai Sea. These was the results of the enhancement of the prevailing northward wind of monsoon in winter which strengthened the coastal currents and speeded up the water exchange rate between the Bays and the Central Bohai Sea. The river fluxes of dissolved black carbon was estimated to 7.43 ± 1.51 Gg in the year of 2014, while the Yellow River contributed to 25.9%. The total water fluxes of the rivers entering the Boahai Sea and the North Yellow Sea was account for ca 0.84‰ of the whole world river water fluxes, carriling ca 0.28‰ of dissolved black carbon to the ocean transported by the whole rivers. The volume of dissolved black carbon in the Bohai Sea was estimated to 113.81 Gg.
语种	中文
文献类型	学位论文
条目标识符	http://ir.yic.ac.cn/handle/133337/13828
专题	中国科学院烟台海岸带研究所知识产出_学位论文
作者单位	中国科学院烟台海岸带研究所
第一作者单位	中国科学院烟台海岸带研究所
推荐引用方式 GB/T 7714	黄国培. 渤海水体中溶解态黑碳的时空分布与来源通量[D]. 北京. 中国科学院大学,2016.

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