Nitrogen speciation and stable nitrogen and oxygen isotopic compostions of maritime aerosol in spring over the continental shelf sea in eastern china and the Northwest Pacific Ocean

大气气溶胶是大气化学中多相反应的催化剂，其化学成份极其复杂。人类活动释放到大气中的不同形态的活性氮是大气气溶胶中一个重要的组成部分。在东亚冬季季风的驱使下，含有活性氮的气溶胶可以在大气中长距离传输并沉降到下风向区域的边缘海和开阔大洋。稳定氮同位素可用于追溯海洋源气溶胶中活性氮的主要来源及其在大气中的化学过程。但由于氮同位素在大气传输和化学转化过程中的分馏效应，使得其应用变得复杂。起源于西伯利亚的东亚冬季季风通过人为活性氮排放强烈的中国东北后又覆盖了整个中国东部陆架海和西北太平洋海域，而且在该海域的春季，沙尘和海雾频现。这为研究该海域海洋源气溶胶中人为源活性氮的空间分布以及在大气中长距离传输及其...Aerosols catalyze the atmospheric heterogeneous reactions, and consist of complex chemical compositions. The reactive nitrogen in atmosphere sourced from the anthropogenic emission is an important part of the aerosols. Influenced by the Asian winter monsoon, aerosols mixed with reactive nitrogen can transport far away from the inland to the open-ocean and deposit into the open-ocean by gravity set...学位：理学博士院系专业：海洋与地球学院_海洋化学学号：2232012015344

Source apportionment of water-soluble ions in spring TSP of Pengjia Islet, Taiwan

于2010年春季,在台湾省北部东海海域彭佳屿岛采集了60个总悬浮颗粒(TSP)样品,用离子色谱测定了8种水溶性离子(Na~+、Mg~(2+)、; Ca~(2+)、K~+、NH_4~+、Cl~-、SO_4~(2-)和NO_3~-)浓度.结合HYSPLIT气团后向轨迹模型、离子化学计量学关系、; 离子相关性分析和主成分分析,探讨了彭佳屿岛春季TSP中水溶性离子的主要来源.结果表明:彭佳屿岛春季TSP中水溶性离子质量浓度顺序依次为SO_4~; (2-)(7.704.53)mug/m~3> Cl~-(6.17 3.85)mug/m~3>Na~+(4.59 ; 2.28)mug/m~3>NO_3~-(4.24 3.07)mug/m~3>NH_4~+(1.53 ; 1.20)mug/m~3>Ca~(2+)(0.95 1.47)mug/m~3>Mg~(2+)(0.59 ; 0.30)mug/m~3>K~+(0.310.17)mug/m~3.其中Cl~-、Na~+和Mg~(2+)全部来源于海洋源;K~+来源较多,除了; 海洋源外,煤和生物质燃烧以及陆源矿物等都可能是彭佳屿岛春季TSP中K~+的来源;60%的Ca~(2+)来源于当地的建筑粉尘;77%的SO_4~(; 2-)源于煤和生物质燃烧释放;NO_3~-主要源于汽车尾气、煤和生物质燃烧等释放;NH_4~+主要来源于二次气溶胶和生物质燃烧等.通过整合本研究; 与前人的观测,发现在春季从中国东北至西北太平洋开阔海域,TSP中Cl~-、Na~+和Mg~(2+)的浓度在空间上呈现逐渐升高趋势,而Ca~(2+; )、K~+、NH_4~+、SO_4~(2-)和NO_3~-的浓度在空间上呈现逐渐下降趋势,显示了TSP中不同水溶性离子在海洋大气传输过程中的空间; 变化特征.In spring of 2010, sixty total suspended particulate (TSP) samples we; collected in Pengjia Islet, northern sea of Taiwan, China. The; concentrations of water-soluble ions (Na~+, Mg~(2+), Ca~(2+), K~+,; NH_4~+, Cl~-, SO_4~(2-) and NO_3~-) in the TSP samples were extracted; and then determined using an Ion Chromatography. Using these data, we; investigated the sources of water-soluble ions by a multiple-technique; analysis combining with the HYSPLIT model, ion stoichiometry,; correlation analysis of water-soluble ions and primary component; analysis. According to a decreasing order in the average mass; concentration, these ions ranked as SO_4~(2-)(7.704.53)mug/m~3,; Cl~-(6.173.85)mug/m~3, Na~+(4.592.28)mug/m~3, NO_3~-(4.24 3.07)mug/m~3,; NH_4~+(1.531.20)mug/m~3, Ca~(2+)(0.951.47)mug/m~3,; Mg~(2+)(0.590.30)mug/m~3 and K~+(0.310.17)mug/m~3. The sea water was; identified as the dominant source for Cl~-, Na~+ and Mg~(2+). Besides; the contribution from the sea salt, the K~+ had other sources, such as; coal and biomass burning, and mineral etc. 60% Ca~(2+) came from the; local construction dust, while 77% SO_4~(2-) originated from coal and; biomass burning. The NO_3~- dominantly sourced from the vehicle exhaust,; coal and biomass burning, while NH_4~+ totally originated from the; second inorganic aerosol and biomass burning. By combining our results; with previous findings, in spring, the concentrations of Cl~-, Na~+ and; Mg~(2+) in TSP increased gradually from the Northeast of China to the; Northwest Pacific Ocean; on the contrary, the Ca~(2+), K~+, NH_4~+,; SO_4~(2-) and NO_3~- in TSP decreased gradually. The spatial; characteristics of different water-soluble ions in TSP were associated; with their long-range transport in the marine boundary layer.国家973计划项目; 国家自然科学基金项目台湾海峡联合基金资助项目; 东华理工大学校科技创新团队科研启动基金项目; 江西省教育厅科技项目;; 东华理工大学博士科研启动基金项