长江口盐度梯度下不同形态碳的分布、来源与混合行为
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摘要
河口碳的生物地球化学过程是全球碳循环的重要组成。通过测定溶解无机碳(DIC)及其稳定同位素丰度(δ~(13)C_(DIC)),溶解有机碳(DOC),有色溶解有机物(CDOM),颗粒有机碳(POC)及其稳定同位素丰度(δ~(13)C_(POC))与元素比值(N/C)及相关指标,研究了2014年7月长江口盐度梯度下不同形态碳的分布、来源和混合行为。结果表明,DIC浓度、DOC浓度、POC含量分别为1 583.2～1 739.6μmol/L,128.4～369.4μmol/L和51.2～530.8μmol/L,这些不同形态碳及CDOM的荧光组分的分布模式相似,均是从口内到口外,整体呈现先增大后减小的趋势,并与盐度呈现非保守混合行为。添加作用主要发生在在口门处最大浑浊带附近。与含量相反,从口内到口外,δ~(13)C_(DIC)和δ~(13)C_(POC)均呈现逐渐减小再增大的趋势,在口门附近达到最低值,分别为-9.7‰和-26.7‰。在口门附近不同形态碳含量上升及δ~(13)C_(DIC)、δ~(13)C_(POC)的降低可能主要与沉积物再悬浮及微生物作用有关。基于蒙特卡洛模拟的三端元混合模型的结果显示,河口内外POC来源变化明显,口内POC以陆源有机碳贡献为主,平均为62.3%,口外海源贡献逐渐增加。CDOM相关参数结果表明长江口CDOM主要来自陆源输入,海源及人类活动等也对其产生影响。
The biogeochemical processes of carbon in estuaries are an important part of global carbon cycle. Dissolved inorganic carbon(DIC), stable carbon isotopic abundance of(δ~(13)C_(DIC)), dissolved organic carbon(DOC), chromophoric dissolved organic matter(CDOM), particle organic carbon(POC), stable carbon isotopic abundance of POC(δ~(13)C_(POC)), atomic element ratios(N/C) and other related parameters were analyzed in order to study the distribution, sources and mixing behavior of different carbon species along a salinity gradient in the Changjiang Estuary in July 2014. The concentrations of DIC, DOC and POC range from 1 583.2 to 1 739.6 μmol/L, 128.4 to 369.4 μmol/L, 51.2 to 530.8 μmol/L, respectively. Similar with CDOM, these carbon species increase first and then decrease from the inner estuary to outer estuary, showing non-conservative mixing behaviors with salinity. The addition behavior of these carbon species mostly occurs in the turbidity maximum zone. In contrast, the values of δ~(13)C_(DIC) and δ~(13)C_(POC) first decrease and then increase from the inner estuary to outer estuary, with the minimum values are found in the river mouth(-9.7‰ and-26.7‰, respectively). The increasing of carbon concentrations and decreasing of δ~(13)C_(DIC), δ~(13)C_(POC) values near the river mouth could be attributed to sediment re-suspension and/or microbial processes. The results of a three end-member mixing model based on Monte-Carlo Simulation indicate that the sources of POC vary greatly from the inner estuary to outer estuary. Terrestrial organic carbon is the main source of POC in the inner estuary, with the average value of 62.3%, whereas contribution of marine organic carbon gradually increase in the outer estuary. The results of CDOM related parameters show that the CDOM is mainly derived from terrestrial input, however, marine sources and human activities may also have impacts in the Changjiang Estuary.
The biogeochemical processes of carbon in estuaries are an important part of global carbon cycle. Dissolved inorganic carbon(DIC), stable carbon isotopic abundance of(δ~(13)C_(DIC)), dissolved organic carbon(DOC), chromophoric dissolved organic matter(CDOM), particle organic carbon(POC), stable carbon isotopic abundance of POC(δ~(13)C_(POC)), atomic element ratios(N/C) and other related parameters were analyzed in order to study the distribution, sources and mixing behavior of different carbon species along a salinity gradient in the Changjiang Estuary in July 2014. The concentrations of DIC, DOC and POC range from 1 583.2 to 1 739.6 μmol/L, 128.4 to 369.4 μmol/L, 51.2 to 530.8 μmol/L, respectively. Similar with CDOM, these carbon species increase first and then decrease from the inner estuary to outer estuary, showing non-conservative mixing behaviors with salinity. The addition behavior of these carbon species mostly occurs in the turbidity maximum zone. In contrast, the values of δ~(13)C_(DIC) and δ~(13)C_(POC) first decrease and then increase from the inner estuary to outer estuary, with the minimum values are found in the river mouth(-9.7‰ and-26.7‰, respectively). The increasing of carbon concentrations and decreasing of δ~(13)C_(DIC), δ~(13)C_(POC) values near the river mouth could be attributed to sediment re-suspension and/or microbial processes. The results of a three end-member mixing model based on Monte-Carlo Simulation indicate that the sources of POC vary greatly from the inner estuary to outer estuary. Terrestrial organic carbon is the main source of POC in the inner estuary, with the average value of 62.3%, whereas contribution of marine organic carbon gradually increase in the outer estuary. The results of CDOM related parameters show that the CDOM is mainly derived from terrestrial input, however, marine sources and human activities may also have impacts in the Changjiang Estuary.
引文
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[11] 徐亚宏, 姚鹏, 苏荣国, 等. 长江口盐度梯度下有色溶解有机物的分布、来源与季节变化[J]. 海洋学报, 2017, 39(6): 21-32. Xu Yahong, Yao Peng, Su Rongguo, et al. Distribution, sources, and seasonal variation of colored dissolved organic matter along salinity gradients in the Changjiang Estuary[J]. Haiyang Xuebao, 2017, 39(6): 21-32.
[12] Zhu Wenzhuo, Zhang Honghai, Zhang Jing, et al. Seasonal variation in chromophoric dissolved organic matter and relationships among fluorescent components, absorption coefficients and dissolved organic carbon in the Bohai Sea, the Yellow Sea and the East China Sea[J]. Journal of Marine Systems, 2018, 180: 9-23.
[13] Liu Qiong, Pan Delu, Bai Yan, et al. The satellite reversion of dissolved organic carbon (DOC) based on the analysis of the mixing behavior of DOC and colored dissolved organic matter: the East China Sea as an example[J]. Acta Oceanologica Sinica, 2013, 32(2): 1-11.
[14] 孙欣, 宋贵生, Xie Huixiang. 长江口溶解有机物光漂白和光矿化表观量子产率[J]. 海洋学报, 2016, 38(4): 120-129. Sun Xin, Song Guisheng, Xie Huixiang. The apparent quantum yields of dissolved organic matter photobleaching and photomineralization in the Changjiang River Estuary[J]. Haiyang Xuebao, 2016, 38(4): 120-129.
[15] Wang Xuchen, Luo Chunle, Ge Tiantian, et al. Controls on the sources and cycling of dissolved inorganic carbon in the Changjiang and Huanghe River Estuaries, China: 14C and 13C studies[J]. Limnology and Oceanography, 2016, 61(4): 1358-1374.
[16] Zhai Weidong, Yan Xiuli, Qi Di. Biogeochemical generation of dissolved inorganic carbon and nitrogen in the North Branch of inner Changjiang Estuary in a dry season[J]. Estuarine, Coastal and Shelf Science, 2017, 197: 136-149.
[17] Patra P, 刘丛强, 李思亮, 等. 长江口溶解无机碳循环的地球化学研究[J]. 地球与环境, 2010, 38(4): 409-413. Patra S, Liu Congqiang, Li Siliang, et al. A geochemical study on carbon cycling in the Changjiang estuary[J]. Earth and Environment, 2010, 38(4): 409-413.
[18] Grasshoff K, Kremling K, Ehrhardt M. Methods of Seawater Analysis[M]. 3rd ed. Weinheim: Wiley-VCH, 2007: 407-420.
[19] Xue Yuejun, Ge Tiantian, Wang Xuchen. An effective method of UV-oxidation of dissolved organic carbon in natural waters for radiocarbon analysis by accelerator mass spectrometry[J]. Journal of Ocean University of China, 2015, 14(6): 989-993.
[20] Guo Weidong, Stedmon C A, Han Yuchao, et al. The conservative and non-conservative behavior of chromophoric dissolved organic matter in Chinese estuarine waters[J]. Marine Chemistry, 2007, 107(3): 357-366.
[21] Stedmon C A, Markager S, Kaas H. Optical properties and signatures of chromophoric dissolved organic matter (CDOM) in Danish coastal waters[J]. Estuarine, Coastal and Shelf Science, 2000, 51(2): 267-278.
[22] Gjessing E T, K?llqvist T. Algicidal and chemical effect of u.v.-radiation of water containing humic substances[J]. Water Research, 1991, 25(4): 491-494.
[23] Bai Ying, Su Rongguo, Shi Xiaoyong. Assessing the dynamics of chromophoric dissolved organic matter in the Southern Yellow Sea by excitation–emission matrix fluorescence and parallel factor analysis (EEM-PARAFAC)[J]. Continental Shelf Research, 2014, 88: 103-116.
[24] Huguet A, Vacher L, Relexans S, et al. Properties of fluorescent dissolved organic matter in the Gironde Estuary[J]. Organic Geochemistry, 2009, 40(6): 706-719.
[25] Cai Weijun, Dai Minhan, Wang Yongchen, et al. The biogeochemistry of inorganic carbon and nutrients in the Pearl River Estuary and the adjacent Northern South China Sea[J]. Continental Shelf Research, 2004, 24(12): 1301-1319.
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[27] Andersson A. A systematic examination of a random sampling strategy for source apportionment calculations[J]. Science of the Total Environment, 2011, 412-413: 232-238.
[28] Zhang Jing, Wu Ying, Jennerjahn T C, et al. Distribution of organic matter in the Changjiang (Yangtze River) Estuary and their stable carbon and nitrogen isotopic ratios: implications for source discrimination and sedimentary dynamics[J]. Marine Chemistry, 2007, 106(1/2): 111-126.
[29] Coble P G. Characterization of marine and terrestrial DOM in seawater using excitation-emission matrix spectroscopy[J]. Marine Chemistry, 1996, 51(4): 325-346.
[30] Samanta S, Dalai T K, Pattanaik J K, et al. Dissolved inorganic carbon (DIC) and its δ13C in the Ganga (Hooghly) River Estuary, India: evidence of DIC generation via organic carbon degradation and carbonate dissolution[J]. Geochimica et Cosmochimica Acta, 2015, 165: 226-248.
[31] Guo Xianghui, Wong G T F. Carbonate chemistry in the northern South China Sea shelf-sea in June 2010[J]. Deep Sea Research Part II: Topical Studies in Oceanography, 2015, 117: 119-130.
[32] Zhang Longjun, Xue Ming, Wang Min, et al. The spatiotemporal distribution of dissolved inorganic and organic carbon in the main stem of the Changjiang (Yangtze) River and the effect of the Three Gorges Reservoir[J]. Journal of Geophysical Research, 2014, 119(5): 741-757.
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