长江口潮滩环境下厌氧氨氧化（Anammox）过程及形成机制研究
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摘要
氮素是地球上生命物质的重要生源要素,长期以来人类一直从生物圈生态发展和满足人类食物需要的角度加以研究和利用。而随着农业、工业和生活N使用量的不断增加,来自工农业生产和生活污水的排放已成为河口及近岸水域富营养化、导致有害赤潮频繁发生的重要原因之一,其生物地球化学循环与影响机制的研究对于深刻认识河口生态系统富营养化演变过程和防止富营养化发生具有极其重要的意义。
目前,厌氧氨氧化过程作为公认的脱氮途径存在于自然界中。自Graaf等人(1990)在污泥处理过程中首次证实了厌氧氨氧化过程的存在后,在海洋生态系统,河口地区和淡水湖泊等环境中陆续发现了该过程的存在。厌氧氨氧化过程的发现,是对氮的生物地球化学循环过程的一种重要补充,为氮元素在水圈中传统的循环模式与机制提出了新的认识和思考,它在氮循环过程中的地位和作用及其产生机制成为目前研究的热点。
长江口滨岸潮滩受潮汐、径流双重影响,是一个典型的海陆交互地带,其特有的河口过程及其特殊的地理位置在国际河口与海岸与海岸研究中占有重要地位。本文选择高强度作用下的城市化河口-—长江河口滨岸潮滩为研究对象,选取浒浦(XP)、吴淞口(WSK)、白龙港(BLG)、浏河口(LHK)、芦潮港(LC)、大新港(DXG)、寅阳(YY)和崇明(CM)八个典型采样断面,利用同位素示踪技术,研究沉积物中厌氧氨氧化速率的时空分布规律,并结合长江口沉积物理化性质特征,探究影响厌氧氨氧化过程的主要控制因子,并估算了该过程在长江口潮滩湿地特殊生境下脱氮过程的影响。主要研究结论如下：
(1)长江口滨岸潮滩表层沉积物中厌氧氨氧化速率变化存在明显的时空分布差异,春、夏、秋、冬四季厌氧氨氧化速率变化范围分别为18.82-52.04μmolN-29*kg-1*d-1,24.92-153.73μmol N-29*kg-1*d-1,34.52-133.41μmol N-29*kg-1*d-1, 7.09-24.33μmol N-29*kg-1*d-1,变异系数分别为0.37,0.52,0.46,0.47。厌氧氨氧化速率季节变化,夏秋强于冬春,空间变化,淡水区域强于咸水区域,并且BLG,WSK两点受附近人为排污影响,速率表现更强。
(2)崇明东滩枯洪两季表层沉积物Anammox速率的时空分布,从空间分布来看,其中洪枯两季的最高值均出现在高潮滩,分别为54.98μmo1 N-29*kg-1*d-1和8.31μmol N-29*kg-1*d-1,最低值出现在低潮滩,分别为23.46μmol N-29*kg-1*d-1和3.41μmol N-29*kg-1*d-1,而对于干湿交替较为强烈的中潮滩来说,则介于两者之间,即从高潮滩向低潮滩递减的趋势。从时间分布可以看出,枯季的均值为8.31μmol N-29*kg-1*d-1,洪季的均值为64.67μmol N-29*kg-1*d-1,即在崇明东滩Anammox速率表现为洪季强于枯季。柱状沉积物中厌氧氨氧化速率变化范围为9.2-52.34μmol N-29*kg-1*d-1,4-6cm时达到最大值,基本上是一个“先升高-再降低”的过程。
(3)长江口潮滩表层沉积物中厌氧氨氧化速率变化主要是受控于盐度和沉积物温度,硫化氢,有机质含量和C/N都对沉积物厌氧氨氧化速率分布存在明显的影响作用；而Fe,Mn等土壤中活跃的金属离子则非厌氧氨氧化速率的主控因子。发现在沉积物中硫化氢,有机质含量和C/N都对沉积物厌氧氨氧化速率的垂向分布存在明显的影响作用。
(4)通过对长江口潮滩沉积物中厌氧氨氧化速率在整个脱氮过程所占比例的研究,发现总脱氮率是101.29-787.31μmol N-30*kg-1*d-1,厌氧氨氧化的脱氮率是7.09-153.73μmol N-29*kg-1*d-1；厌氧氨氧化脱氮量占到总脱氮量的5-23%,表明厌氧氨氧化过程是长江口滨岸带湿地N去除的重要途径。
Nitrogen is one of essential elements for biological growth on earth. It has always been studied and utilized by human being for ecological development and food supply. In recent decades, due to the effects of intense human activities, substantial reactive nitrogen has been transported into estuarine and coastal seas, as a result leading to serious eutrophication and frequent occurrence of harmful algae blooms. Therefore, it is of significant to study the biogeochemical cycle of nitrogen for understanding the occurrence of eutrophication in estuarine ecosystems.
At present, anaerobic ammonium oxidation (anammox) has been identified as a significant pathway of nitrogen removal in natural ecosystems. In the early 1990's the first direct evidence of the anaerobic oxidation of NH4+ came from a waste water treatment facility in Delft, the Netherlands. A few years after the initial discovery of anammox, the anaerobic oxidation of ammonium coupled to nitrite reduction with N2 as the end product, is a newly discovered microbial transformation pathway in the marine ecosystems, estuaries and freshwater lakes. The ubiquitous presence of anammox in marine ecosystems has changed our knowledge of the global nitrogen cycle.
The estuarine and coastal tidal flat, as a typical transitional zone between land and ocean, is a multifunctional and complex ecosystem with special ecological values and potential resources. The study area is situated on the Yangtze Estuary and adjacent coastal tidal flat areas. In the present study, the eight sampling sites were selected along the Yangtze estuarine and coastal lines, including Xupu (XP), Liuhekou (LHK), Wusongkou (WSK), Bailonggong (BLG), Luchaogang (LC), Daxinang (DXG), Yinyang (YY) and Chongming (CM). Based on the technique of nitrogen-isotopic trace, the temporal and spatial changes of the anammox process occurring were investigated in the intertidal sediments of the Yangtze Estuary. The mainly findings are as follows:
1. There were obviously temporal and spatial changes of the anammox rates in the tidal sediments of the Yangtze Estuary. The anammox rates ranges from 18.82 to 52.04μmol N-29*kg-1*d-1,24.92 to 153.73μmol N-29*kg-1*d-1,34.52 to 133.41μmol N-29*kg-1*d-1 and 7.09 to 24.33μmol N-29*kg-1*d-1 in spring, autumn, fall and winter, respectively. In general, the anammox rates in spring and winter were lower than in summer and autumn. Also, the anammox rates in fresh water areas were higher than in brackish areas.
2. Significantly temporal and spatial variations of the anammox rates were observed in the Chongming eastern tidal flat. Generally, the anammox rates in dry season were lower than in flood season. Also, the maximum rates of anammox appeared in the high tidal flat, followed by the middle and low tidal flats.
3. Under the periodical changes of exposure-immersion, the spatial and temporal distributions of the anammox rates were controlled probably by salinity and sediment temperature. H2S, OC and C/N rate can also affect the anammox rate in intertidal surface sediments of the Yangtze Estuary. However, the anammox rate had no correlation with Fe and Mn contents.
4. The results showed that the total rates of nitrogen removal were from 101.29 to 787.31μmol N-30*kg-1*d-1. In contrast, the anammox rates ranged from 7.09-153.73μmol N-29*kg-1*d-1 at the study area. This comparison shows that about 5 to 23% of N2 production in sediments of the Yangtze Estuary may be attributed to the activities of anammox bacteria. Therefore, the anammox process plays a significant role in reactive nitrogen removal at the study area.
目前,厌氧氨氧化过程作为公认的脱氮途径存在于自然界中。自Graaf等人(1990)在污泥处理过程中首次证实了厌氧氨氧化过程的存在后,在海洋生态系统,河口地区和淡水湖泊等环境中陆续发现了该过程的存在。厌氧氨氧化过程的发现,是对氮的生物地球化学循环过程的一种重要补充,为氮元素在水圈中传统的循环模式与机制提出了新的认识和思考,它在氮循环过程中的地位和作用及其产生机制成为目前研究的热点。
长江口滨岸潮滩受潮汐、径流双重影响,是一个典型的海陆交互地带,其特有的河口过程及其特殊的地理位置在国际河口与海岸与海岸研究中占有重要地位。本文选择高强度作用下的城市化河口-—长江河口滨岸潮滩为研究对象,选取浒浦(XP)、吴淞口(WSK)、白龙港(BLG)、浏河口(LHK)、芦潮港(LC)、大新港(DXG)、寅阳(YY)和崇明(CM)八个典型采样断面,利用同位素示踪技术,研究沉积物中厌氧氨氧化速率的时空分布规律,并结合长江口沉积物理化性质特征,探究影响厌氧氨氧化过程的主要控制因子,并估算了该过程在长江口潮滩湿地特殊生境下脱氮过程的影响。主要研究结论如下：
(1)长江口滨岸潮滩表层沉积物中厌氧氨氧化速率变化存在明显的时空分布差异,春、夏、秋、冬四季厌氧氨氧化速率变化范围分别为18.82-52.04μmolN-29*kg-1*d-1,24.92-153.73μmol N-29*kg-1*d-1,34.52-133.41μmol N-29*kg-1*d-1, 7.09-24.33μmol N-29*kg-1*d-1,变异系数分别为0.37,0.52,0.46,0.47。厌氧氨氧化速率季节变化,夏秋强于冬春,空间变化,淡水区域强于咸水区域,并且BLG,WSK两点受附近人为排污影响,速率表现更强。
(2)崇明东滩枯洪两季表层沉积物Anammox速率的时空分布,从空间分布来看,其中洪枯两季的最高值均出现在高潮滩,分别为54.98μmo1 N-29*kg-1*d-1和8.31μmol N-29*kg-1*d-1,最低值出现在低潮滩,分别为23.46μmol N-29*kg-1*d-1和3.41μmol N-29*kg-1*d-1,而对于干湿交替较为强烈的中潮滩来说,则介于两者之间,即从高潮滩向低潮滩递减的趋势。从时间分布可以看出,枯季的均值为8.31μmol N-29*kg-1*d-1,洪季的均值为64.67μmol N-29*kg-1*d-1,即在崇明东滩Anammox速率表现为洪季强于枯季。柱状沉积物中厌氧氨氧化速率变化范围为9.2-52.34μmol N-29*kg-1*d-1,4-6cm时达到最大值,基本上是一个“先升高-再降低”的过程。
(3)长江口潮滩表层沉积物中厌氧氨氧化速率变化主要是受控于盐度和沉积物温度,硫化氢,有机质含量和C/N都对沉积物厌氧氨氧化速率分布存在明显的影响作用；而Fe,Mn等土壤中活跃的金属离子则非厌氧氨氧化速率的主控因子。发现在沉积物中硫化氢,有机质含量和C/N都对沉积物厌氧氨氧化速率的垂向分布存在明显的影响作用。
(4)通过对长江口潮滩沉积物中厌氧氨氧化速率在整个脱氮过程所占比例的研究,发现总脱氮率是101.29-787.31μmol N-30*kg-1*d-1,厌氧氨氧化的脱氮率是7.09-153.73μmol N-29*kg-1*d-1；厌氧氨氧化脱氮量占到总脱氮量的5-23%,表明厌氧氨氧化过程是长江口滨岸带湿地N去除的重要途径。
Nitrogen is one of essential elements for biological growth on earth. It has always been studied and utilized by human being for ecological development and food supply. In recent decades, due to the effects of intense human activities, substantial reactive nitrogen has been transported into estuarine and coastal seas, as a result leading to serious eutrophication and frequent occurrence of harmful algae blooms. Therefore, it is of significant to study the biogeochemical cycle of nitrogen for understanding the occurrence of eutrophication in estuarine ecosystems.
At present, anaerobic ammonium oxidation (anammox) has been identified as a significant pathway of nitrogen removal in natural ecosystems. In the early 1990's the first direct evidence of the anaerobic oxidation of NH4+ came from a waste water treatment facility in Delft, the Netherlands. A few years after the initial discovery of anammox, the anaerobic oxidation of ammonium coupled to nitrite reduction with N2 as the end product, is a newly discovered microbial transformation pathway in the marine ecosystems, estuaries and freshwater lakes. The ubiquitous presence of anammox in marine ecosystems has changed our knowledge of the global nitrogen cycle.
The estuarine and coastal tidal flat, as a typical transitional zone between land and ocean, is a multifunctional and complex ecosystem with special ecological values and potential resources. The study area is situated on the Yangtze Estuary and adjacent coastal tidal flat areas. In the present study, the eight sampling sites were selected along the Yangtze estuarine and coastal lines, including Xupu (XP), Liuhekou (LHK), Wusongkou (WSK), Bailonggong (BLG), Luchaogang (LC), Daxinang (DXG), Yinyang (YY) and Chongming (CM). Based on the technique of nitrogen-isotopic trace, the temporal and spatial changes of the anammox process occurring were investigated in the intertidal sediments of the Yangtze Estuary. The mainly findings are as follows:
1. There were obviously temporal and spatial changes of the anammox rates in the tidal sediments of the Yangtze Estuary. The anammox rates ranges from 18.82 to 52.04μmol N-29*kg-1*d-1,24.92 to 153.73μmol N-29*kg-1*d-1,34.52 to 133.41μmol N-29*kg-1*d-1 and 7.09 to 24.33μmol N-29*kg-1*d-1 in spring, autumn, fall and winter, respectively. In general, the anammox rates in spring and winter were lower than in summer and autumn. Also, the anammox rates in fresh water areas were higher than in brackish areas.
2. Significantly temporal and spatial variations of the anammox rates were observed in the Chongming eastern tidal flat. Generally, the anammox rates in dry season were lower than in flood season. Also, the maximum rates of anammox appeared in the high tidal flat, followed by the middle and low tidal flats.
3. Under the periodical changes of exposure-immersion, the spatial and temporal distributions of the anammox rates were controlled probably by salinity and sediment temperature. H2S, OC and C/N rate can also affect the anammox rate in intertidal surface sediments of the Yangtze Estuary. However, the anammox rate had no correlation with Fe and Mn contents.
4. The results showed that the total rates of nitrogen removal were from 101.29 to 787.31μmol N-30*kg-1*d-1. In contrast, the anammox rates ranged from 7.09-153.73μmol N-29*kg-1*d-1 at the study area. This comparison shows that about 5 to 23% of N2 production in sediments of the Yangtze Estuary may be attributed to the activities of anammox bacteria. Therefore, the anammox process plays a significant role in reactive nitrogen removal at the study area.
引文
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