中国东海、黄海DMS和DMSP的生物地球化学研究
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摘要
二甲基硫(DMS)是海洋中最重要的挥发性生源硫化物,其在大气中的氧化产物对全球气候变化和酸雨的形成产生重要的影响。近岸、陆架海区虽然只占全球海洋的一小部分,但对全球DMS释放的贡献较大。因此对典型的近海海洋环境中DMS及其前体物质-二甲巯基丙酸内盐(DMSP)的生物地球化学进行研究,有助于深入了解DMS、DMSP和生物圈、大气环境之间复杂的相互作用,对在区域和全球尺度上准确估算DMS的海-气通量及其对环境气候的影响具有重要的意义。
本论文以受人类活动影响较大的中国东海和黄海为研究目标,从海水和大气两方面入手,对海水中DMS和DMSP的浓度分布、时空变化、海-气通量、影响因素以及与海区内生物特征、生态环境的关系进行了较为系统的研究,同时对近海污染大气中DMS浓度水平及其氧化产物对气溶胶中非海盐硫酸盐(nss-SO_4~(2-))的贡献情况进行了考察。主要研究结果如下:
(1)参考国内外文献,在实验室原有海水DMS分析测试系统的基础上,整合建立了一套海水DMS/DMSP、大气DMS及气溶胶中MSA、nss-SO_4~(2-)等一系列含硫化合物的分析检测方法,方法的精密度和准确度与国内外同类方法相当,为中国东、黄海海水及大气中各种硫化物的分析测定工作打下了坚实的基础。
(2)于2006年6-7月、2007年1-2月和11月对东海、南黄海海域DMS、DMSP的浓度分布和DMS海-气通量的时空变化进行了研究。夏季东海、南黄海表层海水中DMS、DMSPd和DMSPp浓度分别为5.64(1.70-12.24)、8.59(2.37-14.77)和18.97(9.44-36.15)nmol L-1;冬季浓度分别为1.78(1.02-3.51)、3.92(2.12-6.25)和7.09(3.80-13.34)nmol L-1;秋季浓度分别为3.38(1.83-7.26)、5.40(2.26-10.51)和9.35(3.25-26.64)nmol L-1。由此看出,东海、南黄海DMS和DMSP浓度呈现明显的季节变化,夏季最高,冬季最低,与监测到的Chl-a浓度的季节变化规律相一致。东海、南黄海DMS和DMSP的空间分布明显受到长江冲淡水和贫营养的黑潮水系及其分支的影响。各季节DMS和DMSP的水平分布特征大致相似,即从近岸向外海呈逐渐降低的趋势,但各季节又呈现出各自一定的特点。另外,各季节DMS和DMSP周日变化的总体趋势是白天高夜晚低,表明DMS/DMSP的生物生产过程与日光辐射有关。
尽管东海、南黄海水文条件比较复杂,导致DMS、DMSP和Chl-a浓度变化范围较大,但各季节DMS、DMSPp和Chl-a之间存在较好的相关性,说明浮游植物生物量在控制东海、南黄海DMS/DMSP的生产与分布方面发挥重要的作用。东海、南黄海DMS/Chl-a与DMSPp/Chl-a比值表现出明显的季节变化,其中夏季浓度比值是秋冬季比值的2倍,这与不同季节浮游植物的种群组成及生物量存在差异有关。同航次浮游植物鉴定结果表明,与夏季相比,秋季和冬季浮游植物组成中甲藻和金藻(DMSP高产种)的种类和数量明显减少,可能是导致DMS/Chl-a和DMSPp/Chl-a比值存在季节差异的主要原因。根据现场风速和表层海水DMS浓度,利用Liss & Merlivat公式(LM86)和Wanninkhof公式(W92)分别计算了DMS海-气交换通量。东海、南黄海DMS海-气通量具有明显的季节差异,夏季较高的DMS浓度和秋季较大的风速都贡献出较大的DMS通量。根据夏、冬、秋三季DMS的年平均通量和东海、南黄海海域面积,初步估算出东海、南黄海DMS年释放量为8.47×10~(-2) -19.11×10~(-2) Tg S a~(-1)。虽然东海、南黄海面积只占全球海洋的0.27%,而其向大气释放的DMS却占到全球海洋年释放量的0.58%,表明陆架海区虽然只占全球海洋的一小部分,但对全球海洋释放DMS的贡献较大。
(3)于2006年7月-2007年10月期间对北黄海海水DMS、DMSP,大气DMS及其氧化产物MSA、nss-SO_4~(2-)的时空分布及季节变化特征进行了研究。研究结果表明:北黄海表层海水中DMS和DMSP浓度的季节变化非常明显,夏季最高、春秋季次之、冬季最低,其中夏季DMS、DMSPd和DMSPp浓度分别是冬季浓度的3.2、2.5和2.9倍。北黄海四个季节DMS、DMSPd和DMSPp的年平均浓度分别为4.05±1.78、6.94±2.75和11.82±5.46 nmol L~(-1)。尽管不同季节DMS和DMSP的浓度变化范围较大,但它们的水平分布特征基本相同,即从辽东半岛、山东半岛近岸向外海海域逐渐降低的趋势,显示出近岸人为活动对浮游植物DMS生产的影响。从单一季节来看,北黄海表层海水中DMS、DMSPp与Chl-a浓度存在显著的相关性;但从四个季节整体综合考虑,DMS、DMSPp与Chl-a之间并不存在相关关系,这与不同季节浮游植物的组成及生物量存在差异有关,因为不同种类的浮游植物生产Chl-a和DMSP的能力存在较大差异。
北黄海DMS海-气通量的季节差异较大,利用LM86和W92方法计算得到的DMS年平均通量分别为4.92±2.10和10.97±4.58μmol m~(-2) d~(-1)。结合北黄海海域面积,初步估算出北黄海DMS年释放量为0.41×10~(-2) - 0.91×10~(-2) Tg S a~(-1)。北黄海只占到全球海洋的0.017%,而其向大气释放的DMS量占全球海洋DMS年释放量的0.029%,此结果也表明近海海域是全球DMS排放通量的重要来源。与DMS海-气通量的季节变化相对应,北黄海大气中DMS浓度夏季最高,冬季最低。然而线性回归结果表明,各季节大气中DMS浓度与DMS海-气通量的相关性很弱或没有相关性,说明海-气扩散并不是影响大气DMS浓度的唯一因素。北黄海大气气溶胶中MSA和nss-SO_4~(2-)浓度同样存在明显的季节差异,然而由于人为释放SO_2对nss-SO_4~(2-)的贡献导致二者的季节变化规律并不一致。利用nss-SO_4~(2-)bio/MSA比值估算了北黄海生源硫释放对nss-SO_4~(2-)的贡献比例,其中春、夏、秋、冬四季的贡献率分别为11.0%、10.4%、2.0%和2.8%。这些研究结果表明,人为输入是北黄海大气气溶胶中nss-SO_4~(2-)的主要来源,但是在春夏季节来源于海洋DMS释放的贡献也是不容忽视的。
(4)于2006年4月对黄海微表层与次表层中DMS的生物生产、浓度分布、迁移转化等生物地球化学过程进行了研究。次表层海水中DMS、DMSPd和DMSPp浓度分别为5.42(1.78-12.75)、9.22(2.85-19.73)和17.50(4.33-36.09) nmol L~(-1);微表层中的浓度分别为4.92(1.69-10.66)、17.08(3.13-38.82)和22.54 (4.85-47.24)nmol L~(-1)。对微表层的富集行为研究表明,DMS未得到富集,而DMSPd和DMSPp得到不同程度的富集,富集因子分别为1.98和1.39。DMS、DMSP和Chl-a在微表层中的浓度分别与其在次表层中的浓度显著相关,表明微表层与次表层水体间存在着强烈的交换作用。微表层与次表层中DMS、DMSPp浓度分别与Chl-a浓度存在明显的相关性。DMS/Chl-a和DMSPp/Chl-a比值在微表层与次表层中分别为4.57(1.11-9.36)、21.11(8.02-57.98)mmol g~(-1)和5.92(1.70-12.90)、18.54(6.84-41.39)mmol g~(-1)。较低的DMS/Chl-a和DMSPp/Chl-a比值反映出春季黄海海域浮游植物群落结构中硅藻的优势地位,与同航次网采浮游植物的鉴定结果相一致。
微表层与次表层中DMS的生物生产速率分别为7.31(2.41-10.35)和5.39(2.96-13.53)nmol L~(-1)d~(-1),微生物消费速率分别为5.56(2.59-9.67)和4.09(1.89-7.13)nmol L~(-1)d~(-1)。DMS生物生产速率大于其微生物消耗速率,导致DMS的净生物生产作用。微表层DMS的生物生产与消费速率均大于次表层,这与微表层具有独特的化学、生物环境有关。微表层与次表层中DMS的生物周转时间τbio分别为1.12(0.73-2.39)d和1.93(1.06-3.44)d,而DMS海-气周转时间τsea-air分别为3.53(0.10-26.28)min和3.32(0.08-24.45)d。由此可以看出,本体海水中微生物消耗相对于海-气扩散在DMS迁移转化中的作用更加明显,而在微表层中海-气扩散是DMS最主要的去除途径。
Dimethylsulfide (DMS) is the dominant volatile biogenic sulfur compound emanating from the ocean, which plays an important role in the global climate change and acid precipitation due to its oxidation products in the atmosphere. Although coastal and shelf regions only occupy a small part of the world ocean, they appear to be responsible for a large part of the oceanic DMS emission. Therefore studies on the biogeochemistry of DMS and its precursor DMSP in representative coastal waters offer a unique opportunity to link atmospheric chemistry and climate to the ecology and evolution of marine community, which will be helpful to accurately estimate the sea-to-air fluxes of DMS on a local and global scale and to predict the influence of oceanic emissions to the environmental and climate changes.
In the present dissertation, we choose the East China Sea (ECS) and the Yellow Sea (YS) as the study areas that are affected seriously by human activities. The spatial and temporal variations of distributions of DMS and DMSP, sea-to-air fluxes of DMS and factors influencing them are systematically studied. Another objective of this study is to examine the seasonal variations of atmospheric DMS concentrations and their contributions to non-sea-salt sulfate (nss-SO_4~(2-)) in aerosols. The main conclusions are drawn as follows:
(1) On the ground of gas-stripping chromatographic systems of seawater DMS in our lab, we integrate and develop a series of sampling and analysis methods of sulfur containing compounds including seawater DMS and DMSP, atmospheric DMS and methanesulfonic acid (MSA), non-sea-salt sulfate (nss-SO_4~(2-)) in aerosol with strict quality assurance and quality control, which lay a solid foundation for the following research work.
(2) The distributions of DMS and DMSP and sea-to-air fluxes of DMS are determined in the East China Sea (ECS) and the South Yellow Sea (SYS) during Jun-Jul, 2006, Jan-Feb and Nov, 2007. The surface water concentrations of DMS, DMSPd and DMSPp in summer are 5.64 (1.70-12.24), 8.59 (2.37-14.77) and 18.97 (9.44-36.15) nmol L~(-1), respectively. Winter concentrations are 1.78 (1.02-3.51), 3.92 (2.12-6.25) and 7.09 (3.80-13.34) nmol L~(-1), and autumn concentrations are 3.38 (1.83-7.26), 5.40 (2.26-10.51) and 9.35 (3.25-26.64) nmol L~(-1), respectively. DMS and DMSP concentrations show a notable seasonal variation with highest values in summer and lowest ones in winter, which corresponds well with the seasonal change of Chl-a observed in the study area. The spatial distributions of DMS and DMSP in the ECS and the SYS are obviously influenced by the Yangtze River effluent and the oligotrophic Kuroshio waters. When the distribution patterns are compared with each other in different seasons, they are nearly synoptic and decreased from inshore to offshore sites, without being strongly biased by temporal change. In addition, DMS and DMSP exhibit a consistent diurnal variation in different seasons, with higher levels in day and lower ones at night, indicating that the production processes of DMS and DMSP may be related to the sunshine radiation.
Despite the highly variable physical environment of the ECS and the SYS and resultant large ranges in algal biomass, we observe two consistent correlations between DMS, DMSPp and Chl-a concentrations in different seasons, respectively. These results indicate that phytoplankton biomass might play an important role in controlling the distributions of biogenic sulfurs in the study area. The ratios of DMS/Chl-a and DMSPp/Chl-a exhibit obvious seasonal variations, with summer values being 2-fold higher than winter and autumn values, which could be attributed to the seasonal change in phytoplankton community structure. Data observed in the same cruises show that the species and biomass of dinoflagellates (high-DMSP-producers) decrease sharply from summer to autumn and winter, which consolidate the dominant status of diatoms in the phytoplankton community. The lost proportion of dinoflagellates may be responsible for the lower ratios of DMS/Chl-a and DMSPp/Chl-a in winter and autumn. Liss and Merlivat relationship (LM86) and Wanninkhof relationship (W92) are employed to calculate the sea-to-air fluxes of DMS based on the in-situ wind speeds and the measured DMS concentrations in the surface waters. As a result, the higher DMS concentrations in summer and large wind speeds in autumn contribute to the large fluxes of DMS in summer and autumn, respectively. Based on the average fluxes of DMS and the area of the ECS and the SYS, the annual DMS emission is estimated to be 8.47×10~(-2) -19.11×10~(-2) Tg S a~(-1). Although the ECS and the SYS only occupies 0.27% of the total ocean in area, the contribution of ECS and the SYS to the global sea-to-air fluxes of DMS is estimated to be 0.58%, which means that shelf regions contribute significant amount to the total oceanic DMS flux compared to the open sea.
(3) Seasonal variations of seawater, atmospheric DMS and aerosol compounds, potentially linked with DMS oxidation, such as MSA and nss-SO_4~(2-) are examined in the North Yellow Sea (NYS) from Jul, 2006 to Oct, 2007. The concentrations of DMS and DMSP exhibit pronounced seasonal variations, with the highest values in summer and the lowest in winter. As a mean, the surface waters concentrations of DMS, DMSPd and DMSPp in summer are 3.2, 2.5 and 2.9 times higher than those in winter, respectively. The annual averages of DMS, DMSPd and DMSPp in the NYS are 4.05±1.78, 6.94±2.75 and 11.82±5.46 nmol L~(-1), respectively. Both DMS and DMSP display a similar distribution pattern in different seasons, decreasing gradually from the shore waters of Liaodong Peninsula and Shandong Peninsula to the open sea. These results reveal the influence of anthropogenic activities on the coastal environment, for example, enhancing the nutrient levels and consequently resulting in high primary production. Two significant correlations are found between DMS, DMSPp and Chl-a concentrations in the surface waters in one separate season, respectively. However, no correlation is found between integrated DMS or DMSPp and Chl-a concentrations at all stations in four seasons, which could be attributed to the different phytoplankton species as well as biomass in different seasons. Not only do different phytoplankton species produce different amounts of Chl-a, they also differ in their ability to form DMSP.
The sea-to-air fluxes of DMS in the NYS vary widely in different seasons, and the mean annual fluxes obtained by the arithmetic of LM86 and W92 are 4.92±2.10μmol m~(-2) d~(-1) and 10.97±4.58μmol m~(-2) d~(-1), respectively. In connection with the area of the NYS, the preliminary DMS emission from the NYS is estimated to be 8.47×10~(-2) -19.11×10~(-2) Tg S a~(-1). Although the NYS only occupies 0.017% of the global ocean in area, the contribution of the NYS to the total sea-to-air fluxes of DMS is estimated to be 0.029%, which also indicates that the coastal waters is an very important source of atmospheric DMS. Similar to the case of seawater DMS, atmospheric DMS concentrations also show an obvious seasonal variation, with the highest values in summer and the lowest ones in winter. However, no significant correlation appeared between atmospheric DMS concentrations and sea-to-air fluxes of DMS. The concentrations of MSA and nss-SO_4~(2-) in aerosols also show pronounced seasonal changes, however, their seasonal trends are different, due to the contribution of anthropogenic SO_2 to the nss-SO_4~(2-). According to the observed MSA and nss-SO_4~(2-) concentrations as well as their ratios, the relative biogenic sulfur contribution to the total nss-SO_4~(2-) are estimated to be 11.0%, 10.4%, 2.0% and 2.8% in spring, summer, autumn and winter, respectively, implying that anthropogenic source is the major contribution to sulfur budget in the study area.
(4) The distribution and cycling of DMS and DMSP are studied in the surface microlayer and corresponding subsurface waters of the YS in April, 2006. The average concentrations of DMS, DMSPd and DMSPp are 5.42 (1.78-12.75), 9.22 (2.85-19.73) and 17.50 (4.33-36.09) nmol L~(-1) in the subsurface water, and those in the microlayer are 4.92 (1.69-10.66), 17.08 (3.13-38.82) and 22.54 (4.85-47.24) nmol L~(-1), respectively. As a whole, no microlayer DMS enrichment is found due to the loss from the thin film during sampling. In contrast, DMSPd and DMSPp appear to be enriched in the microlayer with average enrichment factors of 1.39 and 1.98, respectively. The concentrations of DMS, DMSP and Chl-a in the microlayer are closely correlated with those in the subsurface water, suggesting that the materials in the microlayer could be related to and transported from the underlying water. The ratios of DMS/Chl-a and DMSPp/Chl-a are 4.57 (1.11-9.36), 21.11 (8.02-57.98) mmol g-1 in the microlayer, and 5.92 (1.70-12.90), 18.54 (6.84-41.39) mmol g~(-1) in the subsurface water. These relative low ratios reflect the fact that diatoms dominate the phytoplankton array in the YS, which is in good agreement with the phytoplankton data obtained in the same cruise.
The biological production rates of DMS in the microlayer and subsurface water are 7.31 (2.41-10.35) and 5.39 (2.96-13.53) nmol L~(-1)d~(-1). By contrast, the microbial consumption rates of DMS are 5.56 (2.59-9.67) and 4.09 (1.89-7.13) nmol L~(-1)d~(-1), respectively. Overall, the production and consumption rates of DMS in the microlayer are mostly higher than those in the subsurface water, demonstrating that the microlayer is biologically active relative to the underlying water. The biological turnover times of DMS in the microlayer and subsurface water are 1.12 (0.73-2.39) d and 1.93 (1.06-3.44) d, respectively, and the sea-to-air turnover time of DMS are 3.53 (0.10-26.28) min and 3.32 (0.08-24.45) d。Thus the above observations lead to a clear conclusion that the major sink of DMS in the microlayer is escape into the atmosphere, which greatly exceeds its bacterial consumption.
本论文以受人类活动影响较大的中国东海和黄海为研究目标,从海水和大气两方面入手,对海水中DMS和DMSP的浓度分布、时空变化、海-气通量、影响因素以及与海区内生物特征、生态环境的关系进行了较为系统的研究,同时对近海污染大气中DMS浓度水平及其氧化产物对气溶胶中非海盐硫酸盐(nss-SO_4~(2-))的贡献情况进行了考察。主要研究结果如下:
(1)参考国内外文献,在实验室原有海水DMS分析测试系统的基础上,整合建立了一套海水DMS/DMSP、大气DMS及气溶胶中MSA、nss-SO_4~(2-)等一系列含硫化合物的分析检测方法,方法的精密度和准确度与国内外同类方法相当,为中国东、黄海海水及大气中各种硫化物的分析测定工作打下了坚实的基础。
(2)于2006年6-7月、2007年1-2月和11月对东海、南黄海海域DMS、DMSP的浓度分布和DMS海-气通量的时空变化进行了研究。夏季东海、南黄海表层海水中DMS、DMSPd和DMSPp浓度分别为5.64(1.70-12.24)、8.59(2.37-14.77)和18.97(9.44-36.15)nmol L-1;冬季浓度分别为1.78(1.02-3.51)、3.92(2.12-6.25)和7.09(3.80-13.34)nmol L-1;秋季浓度分别为3.38(1.83-7.26)、5.40(2.26-10.51)和9.35(3.25-26.64)nmol L-1。由此看出,东海、南黄海DMS和DMSP浓度呈现明显的季节变化,夏季最高,冬季最低,与监测到的Chl-a浓度的季节变化规律相一致。东海、南黄海DMS和DMSP的空间分布明显受到长江冲淡水和贫营养的黑潮水系及其分支的影响。各季节DMS和DMSP的水平分布特征大致相似,即从近岸向外海呈逐渐降低的趋势,但各季节又呈现出各自一定的特点。另外,各季节DMS和DMSP周日变化的总体趋势是白天高夜晚低,表明DMS/DMSP的生物生产过程与日光辐射有关。
尽管东海、南黄海水文条件比较复杂,导致DMS、DMSP和Chl-a浓度变化范围较大,但各季节DMS、DMSPp和Chl-a之间存在较好的相关性,说明浮游植物生物量在控制东海、南黄海DMS/DMSP的生产与分布方面发挥重要的作用。东海、南黄海DMS/Chl-a与DMSPp/Chl-a比值表现出明显的季节变化,其中夏季浓度比值是秋冬季比值的2倍,这与不同季节浮游植物的种群组成及生物量存在差异有关。同航次浮游植物鉴定结果表明,与夏季相比,秋季和冬季浮游植物组成中甲藻和金藻(DMSP高产种)的种类和数量明显减少,可能是导致DMS/Chl-a和DMSPp/Chl-a比值存在季节差异的主要原因。根据现场风速和表层海水DMS浓度,利用Liss & Merlivat公式(LM86)和Wanninkhof公式(W92)分别计算了DMS海-气交换通量。东海、南黄海DMS海-气通量具有明显的季节差异,夏季较高的DMS浓度和秋季较大的风速都贡献出较大的DMS通量。根据夏、冬、秋三季DMS的年平均通量和东海、南黄海海域面积,初步估算出东海、南黄海DMS年释放量为8.47×10~(-2) -19.11×10~(-2) Tg S a~(-1)。虽然东海、南黄海面积只占全球海洋的0.27%,而其向大气释放的DMS却占到全球海洋年释放量的0.58%,表明陆架海区虽然只占全球海洋的一小部分,但对全球海洋释放DMS的贡献较大。
(3)于2006年7月-2007年10月期间对北黄海海水DMS、DMSP,大气DMS及其氧化产物MSA、nss-SO_4~(2-)的时空分布及季节变化特征进行了研究。研究结果表明:北黄海表层海水中DMS和DMSP浓度的季节变化非常明显,夏季最高、春秋季次之、冬季最低,其中夏季DMS、DMSPd和DMSPp浓度分别是冬季浓度的3.2、2.5和2.9倍。北黄海四个季节DMS、DMSPd和DMSPp的年平均浓度分别为4.05±1.78、6.94±2.75和11.82±5.46 nmol L~(-1)。尽管不同季节DMS和DMSP的浓度变化范围较大,但它们的水平分布特征基本相同,即从辽东半岛、山东半岛近岸向外海海域逐渐降低的趋势,显示出近岸人为活动对浮游植物DMS生产的影响。从单一季节来看,北黄海表层海水中DMS、DMSPp与Chl-a浓度存在显著的相关性;但从四个季节整体综合考虑,DMS、DMSPp与Chl-a之间并不存在相关关系,这与不同季节浮游植物的组成及生物量存在差异有关,因为不同种类的浮游植物生产Chl-a和DMSP的能力存在较大差异。
北黄海DMS海-气通量的季节差异较大,利用LM86和W92方法计算得到的DMS年平均通量分别为4.92±2.10和10.97±4.58μmol m~(-2) d~(-1)。结合北黄海海域面积,初步估算出北黄海DMS年释放量为0.41×10~(-2) - 0.91×10~(-2) Tg S a~(-1)。北黄海只占到全球海洋的0.017%,而其向大气释放的DMS量占全球海洋DMS年释放量的0.029%,此结果也表明近海海域是全球DMS排放通量的重要来源。与DMS海-气通量的季节变化相对应,北黄海大气中DMS浓度夏季最高,冬季最低。然而线性回归结果表明,各季节大气中DMS浓度与DMS海-气通量的相关性很弱或没有相关性,说明海-气扩散并不是影响大气DMS浓度的唯一因素。北黄海大气气溶胶中MSA和nss-SO_4~(2-)浓度同样存在明显的季节差异,然而由于人为释放SO_2对nss-SO_4~(2-)的贡献导致二者的季节变化规律并不一致。利用nss-SO_4~(2-)bio/MSA比值估算了北黄海生源硫释放对nss-SO_4~(2-)的贡献比例,其中春、夏、秋、冬四季的贡献率分别为11.0%、10.4%、2.0%和2.8%。这些研究结果表明,人为输入是北黄海大气气溶胶中nss-SO_4~(2-)的主要来源,但是在春夏季节来源于海洋DMS释放的贡献也是不容忽视的。
(4)于2006年4月对黄海微表层与次表层中DMS的生物生产、浓度分布、迁移转化等生物地球化学过程进行了研究。次表层海水中DMS、DMSPd和DMSPp浓度分别为5.42(1.78-12.75)、9.22(2.85-19.73)和17.50(4.33-36.09) nmol L~(-1);微表层中的浓度分别为4.92(1.69-10.66)、17.08(3.13-38.82)和22.54 (4.85-47.24)nmol L~(-1)。对微表层的富集行为研究表明,DMS未得到富集,而DMSPd和DMSPp得到不同程度的富集,富集因子分别为1.98和1.39。DMS、DMSP和Chl-a在微表层中的浓度分别与其在次表层中的浓度显著相关,表明微表层与次表层水体间存在着强烈的交换作用。微表层与次表层中DMS、DMSPp浓度分别与Chl-a浓度存在明显的相关性。DMS/Chl-a和DMSPp/Chl-a比值在微表层与次表层中分别为4.57(1.11-9.36)、21.11(8.02-57.98)mmol g~(-1)和5.92(1.70-12.90)、18.54(6.84-41.39)mmol g~(-1)。较低的DMS/Chl-a和DMSPp/Chl-a比值反映出春季黄海海域浮游植物群落结构中硅藻的优势地位,与同航次网采浮游植物的鉴定结果相一致。
微表层与次表层中DMS的生物生产速率分别为7.31(2.41-10.35)和5.39(2.96-13.53)nmol L~(-1)d~(-1),微生物消费速率分别为5.56(2.59-9.67)和4.09(1.89-7.13)nmol L~(-1)d~(-1)。DMS生物生产速率大于其微生物消耗速率,导致DMS的净生物生产作用。微表层DMS的生物生产与消费速率均大于次表层,这与微表层具有独特的化学、生物环境有关。微表层与次表层中DMS的生物周转时间τbio分别为1.12(0.73-2.39)d和1.93(1.06-3.44)d,而DMS海-气周转时间τsea-air分别为3.53(0.10-26.28)min和3.32(0.08-24.45)d。由此可以看出,本体海水中微生物消耗相对于海-气扩散在DMS迁移转化中的作用更加明显,而在微表层中海-气扩散是DMS最主要的去除途径。
Dimethylsulfide (DMS) is the dominant volatile biogenic sulfur compound emanating from the ocean, which plays an important role in the global climate change and acid precipitation due to its oxidation products in the atmosphere. Although coastal and shelf regions only occupy a small part of the world ocean, they appear to be responsible for a large part of the oceanic DMS emission. Therefore studies on the biogeochemistry of DMS and its precursor DMSP in representative coastal waters offer a unique opportunity to link atmospheric chemistry and climate to the ecology and evolution of marine community, which will be helpful to accurately estimate the sea-to-air fluxes of DMS on a local and global scale and to predict the influence of oceanic emissions to the environmental and climate changes.
In the present dissertation, we choose the East China Sea (ECS) and the Yellow Sea (YS) as the study areas that are affected seriously by human activities. The spatial and temporal variations of distributions of DMS and DMSP, sea-to-air fluxes of DMS and factors influencing them are systematically studied. Another objective of this study is to examine the seasonal variations of atmospheric DMS concentrations and their contributions to non-sea-salt sulfate (nss-SO_4~(2-)) in aerosols. The main conclusions are drawn as follows:
(1) On the ground of gas-stripping chromatographic systems of seawater DMS in our lab, we integrate and develop a series of sampling and analysis methods of sulfur containing compounds including seawater DMS and DMSP, atmospheric DMS and methanesulfonic acid (MSA), non-sea-salt sulfate (nss-SO_4~(2-)) in aerosol with strict quality assurance and quality control, which lay a solid foundation for the following research work.
(2) The distributions of DMS and DMSP and sea-to-air fluxes of DMS are determined in the East China Sea (ECS) and the South Yellow Sea (SYS) during Jun-Jul, 2006, Jan-Feb and Nov, 2007. The surface water concentrations of DMS, DMSPd and DMSPp in summer are 5.64 (1.70-12.24), 8.59 (2.37-14.77) and 18.97 (9.44-36.15) nmol L~(-1), respectively. Winter concentrations are 1.78 (1.02-3.51), 3.92 (2.12-6.25) and 7.09 (3.80-13.34) nmol L~(-1), and autumn concentrations are 3.38 (1.83-7.26), 5.40 (2.26-10.51) and 9.35 (3.25-26.64) nmol L~(-1), respectively. DMS and DMSP concentrations show a notable seasonal variation with highest values in summer and lowest ones in winter, which corresponds well with the seasonal change of Chl-a observed in the study area. The spatial distributions of DMS and DMSP in the ECS and the SYS are obviously influenced by the Yangtze River effluent and the oligotrophic Kuroshio waters. When the distribution patterns are compared with each other in different seasons, they are nearly synoptic and decreased from inshore to offshore sites, without being strongly biased by temporal change. In addition, DMS and DMSP exhibit a consistent diurnal variation in different seasons, with higher levels in day and lower ones at night, indicating that the production processes of DMS and DMSP may be related to the sunshine radiation.
Despite the highly variable physical environment of the ECS and the SYS and resultant large ranges in algal biomass, we observe two consistent correlations between DMS, DMSPp and Chl-a concentrations in different seasons, respectively. These results indicate that phytoplankton biomass might play an important role in controlling the distributions of biogenic sulfurs in the study area. The ratios of DMS/Chl-a and DMSPp/Chl-a exhibit obvious seasonal variations, with summer values being 2-fold higher than winter and autumn values, which could be attributed to the seasonal change in phytoplankton community structure. Data observed in the same cruises show that the species and biomass of dinoflagellates (high-DMSP-producers) decrease sharply from summer to autumn and winter, which consolidate the dominant status of diatoms in the phytoplankton community. The lost proportion of dinoflagellates may be responsible for the lower ratios of DMS/Chl-a and DMSPp/Chl-a in winter and autumn. Liss and Merlivat relationship (LM86) and Wanninkhof relationship (W92) are employed to calculate the sea-to-air fluxes of DMS based on the in-situ wind speeds and the measured DMS concentrations in the surface waters. As a result, the higher DMS concentrations in summer and large wind speeds in autumn contribute to the large fluxes of DMS in summer and autumn, respectively. Based on the average fluxes of DMS and the area of the ECS and the SYS, the annual DMS emission is estimated to be 8.47×10~(-2) -19.11×10~(-2) Tg S a~(-1). Although the ECS and the SYS only occupies 0.27% of the total ocean in area, the contribution of ECS and the SYS to the global sea-to-air fluxes of DMS is estimated to be 0.58%, which means that shelf regions contribute significant amount to the total oceanic DMS flux compared to the open sea.
(3) Seasonal variations of seawater, atmospheric DMS and aerosol compounds, potentially linked with DMS oxidation, such as MSA and nss-SO_4~(2-) are examined in the North Yellow Sea (NYS) from Jul, 2006 to Oct, 2007. The concentrations of DMS and DMSP exhibit pronounced seasonal variations, with the highest values in summer and the lowest in winter. As a mean, the surface waters concentrations of DMS, DMSPd and DMSPp in summer are 3.2, 2.5 and 2.9 times higher than those in winter, respectively. The annual averages of DMS, DMSPd and DMSPp in the NYS are 4.05±1.78, 6.94±2.75 and 11.82±5.46 nmol L~(-1), respectively. Both DMS and DMSP display a similar distribution pattern in different seasons, decreasing gradually from the shore waters of Liaodong Peninsula and Shandong Peninsula to the open sea. These results reveal the influence of anthropogenic activities on the coastal environment, for example, enhancing the nutrient levels and consequently resulting in high primary production. Two significant correlations are found between DMS, DMSPp and Chl-a concentrations in the surface waters in one separate season, respectively. However, no correlation is found between integrated DMS or DMSPp and Chl-a concentrations at all stations in four seasons, which could be attributed to the different phytoplankton species as well as biomass in different seasons. Not only do different phytoplankton species produce different amounts of Chl-a, they also differ in their ability to form DMSP.
The sea-to-air fluxes of DMS in the NYS vary widely in different seasons, and the mean annual fluxes obtained by the arithmetic of LM86 and W92 are 4.92±2.10μmol m~(-2) d~(-1) and 10.97±4.58μmol m~(-2) d~(-1), respectively. In connection with the area of the NYS, the preliminary DMS emission from the NYS is estimated to be 8.47×10~(-2) -19.11×10~(-2) Tg S a~(-1). Although the NYS only occupies 0.017% of the global ocean in area, the contribution of the NYS to the total sea-to-air fluxes of DMS is estimated to be 0.029%, which also indicates that the coastal waters is an very important source of atmospheric DMS. Similar to the case of seawater DMS, atmospheric DMS concentrations also show an obvious seasonal variation, with the highest values in summer and the lowest ones in winter. However, no significant correlation appeared between atmospheric DMS concentrations and sea-to-air fluxes of DMS. The concentrations of MSA and nss-SO_4~(2-) in aerosols also show pronounced seasonal changes, however, their seasonal trends are different, due to the contribution of anthropogenic SO_2 to the nss-SO_4~(2-). According to the observed MSA and nss-SO_4~(2-) concentrations as well as their ratios, the relative biogenic sulfur contribution to the total nss-SO_4~(2-) are estimated to be 11.0%, 10.4%, 2.0% and 2.8% in spring, summer, autumn and winter, respectively, implying that anthropogenic source is the major contribution to sulfur budget in the study area.
(4) The distribution and cycling of DMS and DMSP are studied in the surface microlayer and corresponding subsurface waters of the YS in April, 2006. The average concentrations of DMS, DMSPd and DMSPp are 5.42 (1.78-12.75), 9.22 (2.85-19.73) and 17.50 (4.33-36.09) nmol L~(-1) in the subsurface water, and those in the microlayer are 4.92 (1.69-10.66), 17.08 (3.13-38.82) and 22.54 (4.85-47.24) nmol L~(-1), respectively. As a whole, no microlayer DMS enrichment is found due to the loss from the thin film during sampling. In contrast, DMSPd and DMSPp appear to be enriched in the microlayer with average enrichment factors of 1.39 and 1.98, respectively. The concentrations of DMS, DMSP and Chl-a in the microlayer are closely correlated with those in the subsurface water, suggesting that the materials in the microlayer could be related to and transported from the underlying water. The ratios of DMS/Chl-a and DMSPp/Chl-a are 4.57 (1.11-9.36), 21.11 (8.02-57.98) mmol g-1 in the microlayer, and 5.92 (1.70-12.90), 18.54 (6.84-41.39) mmol g~(-1) in the subsurface water. These relative low ratios reflect the fact that diatoms dominate the phytoplankton array in the YS, which is in good agreement with the phytoplankton data obtained in the same cruise.
The biological production rates of DMS in the microlayer and subsurface water are 7.31 (2.41-10.35) and 5.39 (2.96-13.53) nmol L~(-1)d~(-1). By contrast, the microbial consumption rates of DMS are 5.56 (2.59-9.67) and 4.09 (1.89-7.13) nmol L~(-1)d~(-1), respectively. Overall, the production and consumption rates of DMS in the microlayer are mostly higher than those in the subsurface water, demonstrating that the microlayer is biologically active relative to the underlying water. The biological turnover times of DMS in the microlayer and subsurface water are 1.12 (0.73-2.39) d and 1.93 (1.06-3.44) d, respectively, and the sea-to-air turnover time of DMS are 3.53 (0.10-26.28) min and 3.32 (0.08-24.45) d。Thus the above observations lead to a clear conclusion that the major sink of DMS in the microlayer is escape into the atmosphere, which greatly exceeds its bacterial consumption.
引文
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