摘要
河流与河口是陆地碳库和海洋碳库的主要链接。陆源有机质是海洋生态系统中重要的物质来源,在生物地球化学过程中扮演了重要的角色。在全球气候变化的背景下,极端的气候事件例如暴雨,台风等发生的频率可能增加,而同时人文活动对自然过程的干扰日益加剧,对河流-河口区域有机质的组成、来源和控制因素的研究有助于人们认识人文活动对生物地球化学过程的影响。由于人文活动特别是流域内筑坝的影响,在很多河流体系,溶解态有机质取代颗粒态有机质,成为陆地向海洋输送的有机碳的主要形式。虽然我国已经有不少的研究对河流颗粒态和溶解态有机质进行了研究,但系统的、分子水平上的定量分析却鲜见报道,特别是对溶解态有机质。本文以长江流域、海南热带小河口以及浙江河流为研究对象,利用有机质的总体性质(碳氮比值(C/N)、稳定同位素(δ13C)等)和生物标志物(木质素),并且结合野外观测和实验室模拟,对以上区域的颗粒态和溶解态有机质的组成、来源进行示踪,并探讨人文活动与自然过程是怎样共同的影响这些区域的有机质的组成、迁移和转化。
长江流域的颗粒态有机质主要来源于土壤有机质、高等植物碎屑和现场生产。利用稳定同位素(613C)和木质素(1ignin)对颗粒态有机质做了定量估算,结果显示土壤有机质为长江流域有机质的主要来源,占50%-70%左右,并且季节变化不大。高等植物碎屑和浮游植物的贡献比例随采样站位和季节的变化而不同,现场生产所占的比例在枯季明显高于洪季,但现场生产不是有机质的主要贡献者。支流的有机质来源相对较丰富,不同的支流主要的贡献者不同,并且支流的洪枯季变化不同,特别需要注意的是洞庭湖和鄱阳湖有机质组成在洪枯季的差异:洪季两湖现场生产的贡献量高达80%,而在枯季则小于20%,与干流洪枯季有机质组成不同。汉江的洪枯季变化不如两湖明显,但在枯季浮游生物对汉江的POC的贡献量也接近50%。长江流域溶解态木质素浓度的变化范围为6.1μg/L-11.6gg/L,而2010年7月-8月洪水时期为10.8μg/L-19.2μg/L。2009年8月-10月,以溶解态木质素Vanillyl(V)系列对有机碳的贡献比例(mg/100mgOC)估算出植物碎屑对溶解态有机质的贡献比例为12%-36%(2009年8月-10月)和24%-32%(2010年7月-8月),并且上游(24.5±8.3%)高于中下游(15.4±2.4%),长江中下游洪水期间高于(27.0±4.0%)高于非洪水期间(15.44±2.4%)。
长江流域季节性的悬浮颗粒物浓度(TSM)的变化、三峡蓄水以及与此相关的长江中下游的冲刷、两湖调节等因素是影响长江入海颗粒态有机质组成和通量主要因素。特别需要注意的是,三峡蓄水后,来自于上游泥沙的减少以及相对不变的水动力过程(除了每年9月中旬-10月中旬,三峡的蓄水时期),使得中下游的两湖和冲刷过程成为枯季长江入海颗粒态有机质组成的主要因素。影响长江流域干流DOC的主要因素为流域地形地势、TSM的变化以及人文活动,而溶解态陆源有机质则主要受到光化学降解过程、有机质来源、季节变化、水体浊度、停留时间、三峡蓄水、絮凝以及颗粒态和溶解态有机质之间的相互作用等因素,并且这些因素相互影响,例如絮凝、水体浊度等受到三峡蓄水的影响;有机质来源则与季节变化有关。
对不同体系有机质的暗降解培养和光降解培养实验表明有机质的来源是影响其生物可利用性和光降解特性的关键因素。海南红树林间隙水由于经历较少的光降解过程,因此其光降解速率(-0.132d-1)远高于已经经历长时间搬运和降解过程的长江三峡库区的溶解态木质素(-0.033d-1)。不同系列的木质素由于其化学结构的不同,降解速率也不同,Syringyl (S)系列的降解速率高于V系列。木质素的酸醛比值((Ad/Al)v)的变化也与初始有机质组成有关,红树林间隙水的溶解态木质素(Ad/Al)v显著上升,但三峡库区的则有一定的波动,并且上升的幅度不大。将长江三峡库区的荧光结果与木质素比对,可以发现木质素的降解速率与UVC类腐殖质峰相近,与他人研究中得到的两者的显著相关相符,进一步表明长江三峡库区的溶解态木质素在进入库区前已经经历了充分的降解过程,可能与长江是大河流体系,水体在流域内有较长的停留时间有关。
对海南文昌河流-河口的悬浮颗粒物的δ13C和木质素对有机碳的贡献比例(人8)等参数不同季节的调查表明在文昌河流及河口,颗粒态有机质主要以现场生产为主,并且海草对河口区有机质没有添加作用;通过对溶解态有机质的V(mg/100mg OC)与植物V(mg/100mg OC)比较,可以粗略估算出维管植物对八门湾内DOC的贡献约为14%-40%,而在近岸约为7%-16%。河流内植物碎屑对DOC的贡献比例比长江蓄水时期高,与长江洪水时期相近。红树林对颗粒态和溶解态有机质的贡献不同,八门湾区域溶解态木质素浓度的升高以及(Ad/A1)v的几乎不变,表明红树林对溶解态有机质的显著添加;于此相对的,在红树林区域观察不到颗粒态有机质的显著添加。一些极端气候事件对河流的影响大于季节变化,例如台风期间河口的TSM的变化高于海南不同季节之间的差异;台风期间大量的陆源有机质从流域内冲刷出,并且可以被输送至近岸。河口区水动力过程、台风过程、光化学降解、季节变化、红树林及虾池对河口区颗粒态和溶解态有机质的组成均有不同程度的影响。
对浙江小河流洪枯季颗粒态和溶解态有机质的调查结果显示浙江河流颗粒态有机质的来源主要以土壤有机质为主,植物碎屑在有机质中所占比例较小;高等植物碎屑对溶解态有机质的贡献比例为10%-50%;与长江等大河流对污水排放的稀释作用不同,由于小河流系统的低流量以及流域内相对较高的人口密度,浙江河流的DOC在很大程度上受到废水排放的影响。通过统计学(SPSS)的差异性分析得出,两个季节(洪季和枯季)的总体性质上没有显著差异,但∑8存在显著性差异,总体上,洪季悬浮颗粒物的陆源有机质含量更高。这也进一步表明相对于总体性质(POC%、δ13C等),木质素等生物标志物对物源变化更加敏感,可以反映出更细致的物源变化。
通过对不同河流以及河口的研究表明人文因素以及自然过程对河流颗粒态和溶解态有机质向海输送的过程中扮演了不同的角色,但这些角色因河流流域大小、流域地形地貌不同。由于受到人文活动的干扰,一些自然过程变得更加重要,例如受到筑坝的影响,光化学降解、淡水絮凝等过程在河流中可能显著,这些都有待更多更深入的研究。
Rivers and estuaries are the major link between land and ocean. Terrestrial organic matter (OM) is a major food source for the marine organism. It plays an important role in the global biogeochemical cycle. Under the background of global climate change, the extreme climate events such as storms, typhoon may increase, in the meantime, the human impact on the natural process increased in the past decades. The study of the sources, composition and fluxes of fluvial organic carbon would help us to understand how the human activities would influence the biogeochemical cycles. Due to the dam constructions in many river systems, dissolved organic matter (DOM) became the dominated. Though there were studies focused on the fluvial OM transportation in China, however, the systematically, quantified and molecular level studies are scarce, especially for DOM. Here we carried out studies that focused on Changijang, small tropical estuary in Hainan Island and Zhejiang small river systems. Bulk properties (carbon to nitrogen molar ratio (C/N), stable carbon isotope (δ13C)) and biomarker (lignin phenols), field observation and lab incubation were used in present studies. Our objectives were1) to trace the sources of both particulate and dissolved organic matter in different river and estuary systems;2) to understand how the human activities and natural process affected the composition and transportation of terrestrial OM.
The particulate organic matter (POM) in Changjiang was mainly composed of soil OM, higher plant tissue and phytoplankton. Stable carbon isotope (δ13C) and lignin phenols were used to quantify the contribution of contribution from different OM sources. The results showed that soil OM is the major OM sources of particulate organic matter in Changjiang, it contribute approximately50%-70%to the total OM. The contribution from soil OM did not show significant seasonal variation can be observed. The contribution from higher plant tissue and phytoplankton was variable temporally and spatially. The contribution from phytoplankton was higher in dry season than in flooding period. The dominant OM sources in tributaries of Changjiang were different and also with seasonal variation. Special notice should be put into Dongting Lake and Poyang Lake. In rainy season, the OM in the two lakes was predominated by in situ production. The contribution from phytoplankton was approximately80%. However, in dry season, phytoplankton only contributed approximately20%to the total OM. The seasonal OM sources variation in Hanjiang was close to that of Changjiang. The dissolved lignin phenols concentrations varied from6.1μg/L to11.6μg/L in2009sampling campaign, and varied from10.8μg/L to19.2μg/L in2010. Utilizing the vanillyl (Ⅴ) end-member value derived from Hernes et al.(2007), it can be calculated that the contribution from higher plant to DOM was approximately12%-36%and24%-32%in August-October2009and July August2010, respectively. Moreover, the contribution from higher plant tissue was higher in upper reach DOM samples (24.5±8.3%) than that in middle and lower reach (15.4±2.4%), higher in the flooding period (27.0±4.0%) than in non-flooding rainy season (15.4±2.4%).
Seasonal TSM variation of Changjiang, TGD impoundment, input from two lakes and channel erosion in middle and lower Changjiang are the major factors that influenced the composition and flux of OM in Changjiang. Specially, after the impoundment of TGD, approximately80%of the sediment from upper reach was trapped within TGR. However, the water discharge from upper Changjiang was almost unaffected (except during the impoundment period, which is mainly during the middle Spetember and middle Octorber), which makes the channel erosion and lakes become more important in determining the Changjiang OM composition and fluxes. The geomorphology, TSM and sewage input was the major factors affecting DOC concentration in the mainstream, while the compositions and fluxes of dissolved terrestrial OM was influenced by its sources, turbidity of the water column, residence time, TGD impoundment, flocculation as well as the interaction between POM and DOM.
The photochemical degradation and dark incubation experiment carried out in different samples indicated that the OM source is the major factor that would influence their bioavailability and photochemical degradation character. The less degraded mangrove pore water from Hainan Wenchang/Wenjiao Estuary had much higher degradation rate than that of dissolved lignin phenols from Three Gorges Reservoir (TGR) which might have experienced longer degradation process. The different compounds of lignin phenols had different degradation rates, syringyl (S) degraded faster than V. The variation of mass ratios of vanillic acid to vanillin ((Ad/Al)v) was also related to the sources of lignin phenols, the increase of (Ad/Al)v of mangrove pore water samples were significant, however, in the TGR samples, it was more variable. The comparison between the fluorescence spectroscopy and lignin phenols in the TGR sample showed that the photochemical degradation rates of lignin phenols were similar to UVC humic-like substance, which is similar to other's study. The similar degradation rates further indicated that lignin phenols in TGR were pre-degraded.
The seasonal observation of813C and A8in Wenchang River/Estuary showed that the major OM source in the Wenchang River was in situ production. Utilizing the V yield of dissolved lignin phenols, it can be calculated that the contribution of higher plant tissues to DOC was approximately14%-40%in Bamen Bay and7%-16%in the coastal region. The contrition of higher plant tissue to DOC in Wenchang River was higher than in Changjiang during "impoundment" period, however, lower than Changjiang during flooding period. The contribution of mangrove forest was different between POM and DOM. The contribution of mangrove to POM was insignificant, however, the higher dissolved lignin phenols concentration in Bamen Bay and the relatively lower (Ad/Al)v revealed the input from mangrove forest to DOM, this is similar to the results in other regions. The impact of extreme events was higher than seasonal variation. During the typhoon "Kammuri", the increase of TSM in Bamen bay was higher than the seasonal variation. Large amount of soil derived terrestrial OM could be transported to the coastal region during the typhoon period. The hydrodynamic process, typhoon, photochemical degradation, seasonal variation, mangrove and aquaculture ponds all had effect on the composition of POM and DOM in the Wenchang/Wenjiao Estuary in different extends.
The observation of POM and DOM in both dry season and rainy season in Zhejiang river showed that soil is the major POM source, the contribution from higher plant tissue is less; the contribution of plant tissues to DOM varied from10%-50%in different river systems. Unlike in Changjiang, DOC in the Zhejiang Rivers was strongly affected by the human activities, which was caused by their small drainage basins and higher population densities. The statistical (SPSS) analysis indicated that the difference of bulk properties between two seasons was insignificant. However, significant difference could be found for lignin phenol concentration (∑8). Higher∑8in the rainy season suggested that POM in rainy season contained higher portion of terrestrial OM, this is similar to the seasonal OM composition variation in Changjiang. The statistical results further suggested that lignin phenols were more sensitive to the OM sources change than bulk properties. Moreover, the human impact was more significant in dry season.
The present study showed that human activities and natural process played different roles during the fluvial transport of POM and DOM. However, their roles were affected by the drainage basin scales as well as the geomorphology of the drainage basin. Due to the human impact, some natural processes become more important, e.g., because of the dam construction, photochemical degradation, freshwater flocculation might be more significant in the river systems. More efforts should be put into those process based studies.
引文
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