查干湖低温期内源磷的释放及其对富营养化的影响
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摘要
富营养化已经成为全球性的生态危机，它不仅严重破坏水环境生态平衡，而且还严重威胁到人类的生存与发展。随着各国对富营养化的重视及相关治理，在外部污染源逐步受到控制和消除的情况下，浅水湖泊沉积物中的磷代替外源磷素污染物，成为引起富营养化的内源污染源。沉积物中磷的不仅在常温期或高温期释放，而且在低温期也会持续释放，这成为北方湖泊富营养化发生的重要诱因。然而，对于低温期北方湖泊的内源磷在沉积物-水界面间迁移转化规律以及影响各形态磷相互转变的地球化学作用，尤其是化学环境与微生物的作用，目前仍缺乏研究。本文以吉林省西部典型的北方浅水湖泊——查干湖为研究对象，以低温期水化学特征和氮、磷营养盐分布规律为基础，采用欧盟推荐的SMT分析方法，调查与分析了查干湖沉积物中不同形态磷的时空变化特征。在实验室内采用实验模拟的方式，深入分析了沉积物-水两相间磷的迁移转化机制以及生物、物理、化学等因素在该过程中所起到的作用。结合叶绿素a和藻类在查干湖水体中的分布规律，探讨了低温期沉积物中磷的释放对我国北方浅水湖泊富营养化的影响，并利用解析动力学模型对释放过程进行描述。同时基于查干湖水质指标，采用综合营养指数法（TLI）对查干湖低温期富营养化程度进行了评价。本文的研究成果可为控制北方同类型湖泊内源磷元素的释放以及低温期富营养化治理提供理论支持。
调查并测定分析了查干湖低温期水化学特征以及不同形态的氮、磷在水体中的时空分布规律。低温时期查干湖pH介于9.35～9.40之间，属于偏碱性湖泊，其水质具有高浊度、高硬度以及高矿化度的特点。水中阴离子以HCO_3~-为主，阳离子以Na~+为主，主要阴、阳离子的含量浓度为：Na~+>Mg~(2+)>Ca~(2+)>K~+，HCO_3~-> Cl~->CO_3~(2-)>SO_4~(2-)，其水化学类型为重碳酸盐钠组I型。低温期查干湖中各种离子浓度均高于常温期，并且在补给水、地质条件等因素影响下，呈现出东南高、西北低分布规律。低温期查干湖周边农业活动停止，在无外源氮、磷输入的情况下，查干湖水中各形态的氮、磷仍具有较高的浓度，说明沉积物已经成为查干湖污染的内源。氨氮（NH_4~+-N）是氮的主要存在形态，呈现出南部高北部低，湖中部高岸边低的分布特征；溶解性总磷（TDP）是磷的主要存在形态，呈现出南部低北部高的分布特征。虽然低温期查干湖的总氮（TN）和总磷（TP）平均浓度已超过富营养化发生的临界浓度，但是低温抑制藻类增殖、高浊度减弱光照强度以及能够被藻类直接利用的正磷酸盐浓度较低等因素共同影响，查干湖并没有出现藻类异常增殖的情况。从时间上来看， NH_4~+-N和亚硝态氮（NO2--N）高浓度区域面积在逐年缩小；TP和TDP浓度整体呈现降低的趋势。
在总结和分析抓斗式和重力柱式沉积物采样器优缺点的基础上，结合采样过程中所遇到的实际问题，研发了一款具有自主知识产权的便携式沉积物采样器，并获得国家发明专利。在实际使用过程中，该采集器能够采集不同质地的沉积物样品，提高了采样效率。在减少研究人员工作量和工作强度的同时，还能最大程度的保持沉积物原始氧化还原状态，并能够避免沉积物样品在向存储容器转移时受到污染或破坏，提高了沉积样品采集的精度与科学性。
明确了查干湖沉积物中各形态磷的空间分布情况。采用SMT分级方法对查干湖不同深度的沉积物中各形态磷进行了分析与研究，结果发现沉积物中磷以无机磷（IP）为主；而钙结合磷（Ca-P）是IP中的主要形态。沉积物中的Ca-P主要来自查干湖周边高钙土。高钙土中磷酸盐在环境条件改变情况下，逐渐转化成水溶性磷酸钙，随地表径流进入查干湖后沉淀，最终在沉积物中形成Ca-P，其含量与TP的含量呈现极显著相关。从水平方向来看，查干湖沉积物中各形态磷浓度具有西南高的分布特点；从垂向来看，呈现从上向下增加的趋势，即各形态磷的含量随深度增加而增加，这说明近年来外源磷污染的输入量在逐渐减少。
分析了查干湖低温期藻类分布情况以及影响藻种组成的因素。低温期查干湖主要藻种为蓝藻门、绿藻门、硅藻门和裸藻门。由于蓝藻具有偏好中碱性水体、较高的细胞贮磷能力等特点，使蓝藻代替硅藻和绿藻成为低温期的优势藻种并且成为查干湖富营养化的潜在威胁。较低水温、光照条件、水生植物之间的竞争以及水生动物对其捕食等原因，抑制蓝藻等藻类过度繁殖，成为富营养化的限制条件，遏制了富营养化发生的风险。通过对藻类与氮素和磷素的相关关系进行分析，结果表明低温期查干湖藻类分布和浓度与氮素无关而与磷素有显著相关性，这说明查干湖是磷控制性湖泊。
揭示了低温条件下查干湖内源磷迁移过程以及影响因素。在有无光照、有无溶解氧的情况下，低温期沉积物中的磷均仍能够持续释放，使上覆水中磷素的含量持续增加。由于Ca-P在沉积物中含量最多，因此解析出来的磷主要是Ca-P且释放出的数量最多。在厌氧有光照的条件下，沉积物中各形态磷的释放速率和释放量最大，是易引发富营养化的环境条件。在光照条件下，上覆水中的叶绿素a与磷素浓度具有明显的相关性。藻类的大量增殖会减少水体中磷的含量，进而加快沉积物磷的释放；沉积物磷的释放又为藻类增殖提供了物质基础，两者之间相互促进。不同形态的磷的释放量与释放速率受到pH、光照、藻类、溶解氧等因素的影响而不同。控制沉积物中磷的释放是抑制查干湖富营养化的关键。
初步探讨了低温环境下沉积物磷的解析动力学以及查干湖富营养化程度。利用水静态模拟的方法，在一定解析时间和水土比条件下，研究沉积物中磷解析的
过程。根据实验数据，得出解析动力学模型P_d=0.017P_0t~(0.375)W~(1.493)，该模型可以用以描述低温期查干湖沉积物中磷的解析过程。采用综合营养指数法（TLI）对查干湖富营养的程度进行综合评价，结果表明查干湖的营养级别从2009年的贫营养（TLI=28.56）转变成2010年（TLI=38.25）和2011年（TLI=30.19）的中等营养，说明查干湖存在发生富营养化的风险。
Eutrophication has developed into global ecological crisis, it is harmful for theecological balance of aquatic and a serious threat to human survival and development.The external sources of pollution were controlled and eliminated gradually.Phosphorus in the shallow lake sediments become internal pollution sources foreutrophication, instead of external sources of pollution. Phosphorus in sedimentreleases not only at nomal temperature and high temperature period, but also at lowtemperature period. It has became an important factor for eutrophication in the lakesof north of China. However, the geochemical processes of internal phosphorusmigration and transformation at the sediment-water interface are still lack, especiallythe knowledge of role of chemical environment and the microorganisms on theprocess at low temperature period. A typical northern shallow lake–Chagan Lake inthe west of Jilin Province was chosen as the study object. Based on the hydrochemicalcharacteristics of Chagan Lake and the distribution characteristics of N and P at lowtemperatures period, the temporal and spatial variation in forms of P fractions in thesediment were investigated and analysed, with SMT analytical methods recommendedby the EU. The mechanisms of P migration and transformation and process at thesediment-water interface was analysed using the aquatic microcosms system, alsothe impact of the biological effects, physical and chemical effects. Effects of P releasein sediment in notrhtern shallow lakes to the eutrophication were studied, based on thechlorophyll-a and algae in the distribution of Chagan Lake at the low temperature.The process of P released from sediment can be described by a desorption-kineticsmodel. It built a trophic level index (TLI) to evaluate the level of Chagan Lakeeutrophication. The results of this study provided theoretical and technical support forthe sediment nutrient control and eutrophication control in northern lakes.
The hydrochemical characteristics of Chagan Lake as well as the temporal andspatial distribution of different forms of N and P were investigated in low-temperature.The pH ranged from9.35to9.40and the Chagan Lake’s characteristics was highturbidity, high hardness and high salinity. HCO_3~-and Na~+were main anion and cation，ion content characteristic was Na~+>Mg~(2+)>Ca~(2+)>K~+，HCO_3~-> Cl~-> CO_3~(2-)>SO_4~(2-). Thehydrochemicaln of Chagan Lake is Bicarbonate-Na-I type. The concentration ofvarious ions at low temperature was higher than the nomal temperature. The distribution of ions concentration was northwest lower than southeast in lake becauseof the supply of water, geological conditions and other factors. In the case ofagricultural activities stopped surrounding Chagan Lake at low temperature, noexternal phosphorus input Chagan lake. The forms of N and P had a highconcentration in water, because of internal pollution in sediments of Chagan Lake.NH_4~+-N was the primary form of nitrogen and TDP was the primary form ofphosphorus. TN and TP has more than average levels of eutrophication in the criticalconcentration, but thanks to the low temperature, the high turbidity and the lowconcentration of PO43-, which were not conducive to the propagation of algae, andChagan Lake hasn’t appear the bloom of algae. The area of high concentrations ofNH_4~+-N and NO2-N were shrinking year by year. The concentration of TP and TDPalso showed a decreasing trend.
On the basis of the advantages and disadvantages of the existingsediment-collecting distributors, and the practical problems encountered in thesampling process, a portable sediment sampler with independent intellectual propertywas invented. The collector can facilitate the collection of sediment samples ofdifferent textures, greatly improves the sampling efficiency. Significantly reduce theworkload and intensity of work of researchers at the same time, improve the accuracyof the sample collection and keep the sediment sampling original state. It is able toavoid sample polluted and broken when them are transfered to a storage container.
The distribution of various forms of P in the sediment surface and bottom ofChagan Lake was investigated by SMT method. The result showed that the IP was themain form of P in sediment and the Ca-P was the main form of IP. The phosphate inthe surrounding high calcium soil of Chagan Lake gradually transformed into awater-soluble calcium phosphate as the environmental conditions changed, withsurface runoff into Chagan Lake and re-settlement. The re-settlement Ca-P insediment was highly significant correlation of TP. The high concentration area of P inthe sediment was in southwest. The various forms of P content increased withincreasing depth in sediment in vertical direction. It showed that the external input ofP pollution gradually reduced in recent years.
The distribution of algae in Chagan Lake in low temperature and the factors thataffect algal species composition were studied. The Chagan Lake algae species wereCyanophyta, Chlorophyta, Bacillariophyta and Euglenophyta in low temperature.Blue-green algae prefer alkaline water and high cell storage ability of phosphorus, which are conducive to blue-green algae instead of diatoms and green algae becomethe dominant at low temperature period. It became a potential threat to eutrophicationin Chagan Lake. But the lower water temperature, lighting conditions, aquatic plantsand aquatic animals preying and other reasons inhibited excessive propagation ofalgae such as cyanobacteria and restrictions risk of eutrophication. By correlationanalysis of algae with N, P, low temperature of Chagan Lake algae distribution andconcentration, the result showed algea had no ralitionship with N, but significantcorrelation P. Chagan Lake is phosphorus controlling lake.
The mechanisms and the influencing factors of P migration and transformation inChagan Lake sediment at low temperature were studied. The P in sediment was stillable to sustained releasing in the presence or absence of illumination and DO, and itmade the content of the overlying water TP sustained increase. Because of Ca-Pcontent in the sediments was most, desorbed phosphorus was most from Ca-P. It wasanaerobic and non-illumination conditions that easily lead to eutrophication, becauseof the release rate of various forms of P in the sediments greatly under thisenvironmental conditions. The chlorophyll-a and P had a significant correlation withillumination. The proliferation of algae reduce the P content in water, and thus speedup the release of P in sediment, meanwhile P release is material basis for algaeproliferation. The raito and the quantity of P release was effected by DO, pH,illumination. The control of sediment phosphorus release is key condition to inhibiteeutrophication in Chagan Lake.
P desorption kinetics of Chagan Lake sediment and eutrophication were analysed.Using water static simulation method in the laboratory to study the desorption kineticswith the content of phosphorus, desorption time (t) and water/soil ratios (W) at lowtemperature. A simple desorption kinetics model could be created, as=0.01700.3751.493, which be used to describe the process of phosphorusdesorption in Chagan Lake sediment at low temperature. It built a trophic levelindex(TLI) model to assess the eutrophication, the results showed that: from2009（TLI=28.56）to2011（TLI=30.19）, the nutritional level of Chagan Lake isoligotrophic into moderate eutrophication. The risks of eutrophication in Chagan Lakeexist.
调查并测定分析了查干湖低温期水化学特征以及不同形态的氮、磷在水体中的时空分布规律。低温时期查干湖pH介于9.35～9.40之间，属于偏碱性湖泊，其水质具有高浊度、高硬度以及高矿化度的特点。水中阴离子以HCO_3~-为主，阳离子以Na~+为主，主要阴、阳离子的含量浓度为：Na~+>Mg~(2+)>Ca~(2+)>K~+，HCO_3~-> Cl~->CO_3~(2-)>SO_4~(2-)，其水化学类型为重碳酸盐钠组I型。低温期查干湖中各种离子浓度均高于常温期，并且在补给水、地质条件等因素影响下，呈现出东南高、西北低分布规律。低温期查干湖周边农业活动停止，在无外源氮、磷输入的情况下，查干湖水中各形态的氮、磷仍具有较高的浓度，说明沉积物已经成为查干湖污染的内源。氨氮（NH_4~+-N）是氮的主要存在形态，呈现出南部高北部低，湖中部高岸边低的分布特征；溶解性总磷（TDP）是磷的主要存在形态，呈现出南部低北部高的分布特征。虽然低温期查干湖的总氮（TN）和总磷（TP）平均浓度已超过富营养化发生的临界浓度，但是低温抑制藻类增殖、高浊度减弱光照强度以及能够被藻类直接利用的正磷酸盐浓度较低等因素共同影响，查干湖并没有出现藻类异常增殖的情况。从时间上来看， NH_4~+-N和亚硝态氮（NO2--N）高浓度区域面积在逐年缩小；TP和TDP浓度整体呈现降低的趋势。
在总结和分析抓斗式和重力柱式沉积物采样器优缺点的基础上，结合采样过程中所遇到的实际问题，研发了一款具有自主知识产权的便携式沉积物采样器，并获得国家发明专利。在实际使用过程中，该采集器能够采集不同质地的沉积物样品，提高了采样效率。在减少研究人员工作量和工作强度的同时，还能最大程度的保持沉积物原始氧化还原状态，并能够避免沉积物样品在向存储容器转移时受到污染或破坏，提高了沉积样品采集的精度与科学性。
明确了查干湖沉积物中各形态磷的空间分布情况。采用SMT分级方法对查干湖不同深度的沉积物中各形态磷进行了分析与研究，结果发现沉积物中磷以无机磷（IP）为主；而钙结合磷（Ca-P）是IP中的主要形态。沉积物中的Ca-P主要来自查干湖周边高钙土。高钙土中磷酸盐在环境条件改变情况下，逐渐转化成水溶性磷酸钙，随地表径流进入查干湖后沉淀，最终在沉积物中形成Ca-P，其含量与TP的含量呈现极显著相关。从水平方向来看，查干湖沉积物中各形态磷浓度具有西南高的分布特点；从垂向来看，呈现从上向下增加的趋势，即各形态磷的含量随深度增加而增加，这说明近年来外源磷污染的输入量在逐渐减少。
分析了查干湖低温期藻类分布情况以及影响藻种组成的因素。低温期查干湖主要藻种为蓝藻门、绿藻门、硅藻门和裸藻门。由于蓝藻具有偏好中碱性水体、较高的细胞贮磷能力等特点，使蓝藻代替硅藻和绿藻成为低温期的优势藻种并且成为查干湖富营养化的潜在威胁。较低水温、光照条件、水生植物之间的竞争以及水生动物对其捕食等原因，抑制蓝藻等藻类过度繁殖，成为富营养化的限制条件，遏制了富营养化发生的风险。通过对藻类与氮素和磷素的相关关系进行分析，结果表明低温期查干湖藻类分布和浓度与氮素无关而与磷素有显著相关性，这说明查干湖是磷控制性湖泊。
揭示了低温条件下查干湖内源磷迁移过程以及影响因素。在有无光照、有无溶解氧的情况下，低温期沉积物中的磷均仍能够持续释放，使上覆水中磷素的含量持续增加。由于Ca-P在沉积物中含量最多，因此解析出来的磷主要是Ca-P且释放出的数量最多。在厌氧有光照的条件下，沉积物中各形态磷的释放速率和释放量最大，是易引发富营养化的环境条件。在光照条件下，上覆水中的叶绿素a与磷素浓度具有明显的相关性。藻类的大量增殖会减少水体中磷的含量，进而加快沉积物磷的释放；沉积物磷的释放又为藻类增殖提供了物质基础，两者之间相互促进。不同形态的磷的释放量与释放速率受到pH、光照、藻类、溶解氧等因素的影响而不同。控制沉积物中磷的释放是抑制查干湖富营养化的关键。
初步探讨了低温环境下沉积物磷的解析动力学以及查干湖富营养化程度。利用水静态模拟的方法，在一定解析时间和水土比条件下，研究沉积物中磷解析的
过程。根据实验数据，得出解析动力学模型P_d=0.017P_0t~(0.375)W~(1.493)，该模型可以用以描述低温期查干湖沉积物中磷的解析过程。采用综合营养指数法（TLI）对查干湖富营养的程度进行综合评价，结果表明查干湖的营养级别从2009年的贫营养（TLI=28.56）转变成2010年（TLI=38.25）和2011年（TLI=30.19）的中等营养，说明查干湖存在发生富营养化的风险。
Eutrophication has developed into global ecological crisis, it is harmful for theecological balance of aquatic and a serious threat to human survival and development.The external sources of pollution were controlled and eliminated gradually.Phosphorus in the shallow lake sediments become internal pollution sources foreutrophication, instead of external sources of pollution. Phosphorus in sedimentreleases not only at nomal temperature and high temperature period, but also at lowtemperature period. It has became an important factor for eutrophication in the lakesof north of China. However, the geochemical processes of internal phosphorusmigration and transformation at the sediment-water interface are still lack, especiallythe knowledge of role of chemical environment and the microorganisms on theprocess at low temperature period. A typical northern shallow lake–Chagan Lake inthe west of Jilin Province was chosen as the study object. Based on the hydrochemicalcharacteristics of Chagan Lake and the distribution characteristics of N and P at lowtemperatures period, the temporal and spatial variation in forms of P fractions in thesediment were investigated and analysed, with SMT analytical methods recommendedby the EU. The mechanisms of P migration and transformation and process at thesediment-water interface was analysed using the aquatic microcosms system, alsothe impact of the biological effects, physical and chemical effects. Effects of P releasein sediment in notrhtern shallow lakes to the eutrophication were studied, based on thechlorophyll-a and algae in the distribution of Chagan Lake at the low temperature.The process of P released from sediment can be described by a desorption-kineticsmodel. It built a trophic level index (TLI) to evaluate the level of Chagan Lakeeutrophication. The results of this study provided theoretical and technical support forthe sediment nutrient control and eutrophication control in northern lakes.
The hydrochemical characteristics of Chagan Lake as well as the temporal andspatial distribution of different forms of N and P were investigated in low-temperature.The pH ranged from9.35to9.40and the Chagan Lake’s characteristics was highturbidity, high hardness and high salinity. HCO_3~-and Na~+were main anion and cation，ion content characteristic was Na~+>Mg~(2+)>Ca~(2+)>K~+，HCO_3~-> Cl~-> CO_3~(2-)>SO_4~(2-). Thehydrochemicaln of Chagan Lake is Bicarbonate-Na-I type. The concentration ofvarious ions at low temperature was higher than the nomal temperature. The distribution of ions concentration was northwest lower than southeast in lake becauseof the supply of water, geological conditions and other factors. In the case ofagricultural activities stopped surrounding Chagan Lake at low temperature, noexternal phosphorus input Chagan lake. The forms of N and P had a highconcentration in water, because of internal pollution in sediments of Chagan Lake.NH_4~+-N was the primary form of nitrogen and TDP was the primary form ofphosphorus. TN and TP has more than average levels of eutrophication in the criticalconcentration, but thanks to the low temperature, the high turbidity and the lowconcentration of PO43-, which were not conducive to the propagation of algae, andChagan Lake hasn’t appear the bloom of algae. The area of high concentrations ofNH_4~+-N and NO2-N were shrinking year by year. The concentration of TP and TDPalso showed a decreasing trend.
On the basis of the advantages and disadvantages of the existingsediment-collecting distributors, and the practical problems encountered in thesampling process, a portable sediment sampler with independent intellectual propertywas invented. The collector can facilitate the collection of sediment samples ofdifferent textures, greatly improves the sampling efficiency. Significantly reduce theworkload and intensity of work of researchers at the same time, improve the accuracyof the sample collection and keep the sediment sampling original state. It is able toavoid sample polluted and broken when them are transfered to a storage container.
The distribution of various forms of P in the sediment surface and bottom ofChagan Lake was investigated by SMT method. The result showed that the IP was themain form of P in sediment and the Ca-P was the main form of IP. The phosphate inthe surrounding high calcium soil of Chagan Lake gradually transformed into awater-soluble calcium phosphate as the environmental conditions changed, withsurface runoff into Chagan Lake and re-settlement. The re-settlement Ca-P insediment was highly significant correlation of TP. The high concentration area of P inthe sediment was in southwest. The various forms of P content increased withincreasing depth in sediment in vertical direction. It showed that the external input ofP pollution gradually reduced in recent years.
The distribution of algae in Chagan Lake in low temperature and the factors thataffect algal species composition were studied. The Chagan Lake algae species wereCyanophyta, Chlorophyta, Bacillariophyta and Euglenophyta in low temperature.Blue-green algae prefer alkaline water and high cell storage ability of phosphorus, which are conducive to blue-green algae instead of diatoms and green algae becomethe dominant at low temperature period. It became a potential threat to eutrophicationin Chagan Lake. But the lower water temperature, lighting conditions, aquatic plantsand aquatic animals preying and other reasons inhibited excessive propagation ofalgae such as cyanobacteria and restrictions risk of eutrophication. By correlationanalysis of algae with N, P, low temperature of Chagan Lake algae distribution andconcentration, the result showed algea had no ralitionship with N, but significantcorrelation P. Chagan Lake is phosphorus controlling lake.
The mechanisms and the influencing factors of P migration and transformation inChagan Lake sediment at low temperature were studied. The P in sediment was stillable to sustained releasing in the presence or absence of illumination and DO, and itmade the content of the overlying water TP sustained increase. Because of Ca-Pcontent in the sediments was most, desorbed phosphorus was most from Ca-P. It wasanaerobic and non-illumination conditions that easily lead to eutrophication, becauseof the release rate of various forms of P in the sediments greatly under thisenvironmental conditions. The chlorophyll-a and P had a significant correlation withillumination. The proliferation of algae reduce the P content in water, and thus speedup the release of P in sediment, meanwhile P release is material basis for algaeproliferation. The raito and the quantity of P release was effected by DO, pH,illumination. The control of sediment phosphorus release is key condition to inhibiteeutrophication in Chagan Lake.
P desorption kinetics of Chagan Lake sediment and eutrophication were analysed.Using water static simulation method in the laboratory to study the desorption kineticswith the content of phosphorus, desorption time (t) and water/soil ratios (W) at lowtemperature. A simple desorption kinetics model could be created, as=0.01700.3751.493, which be used to describe the process of phosphorusdesorption in Chagan Lake sediment at low temperature. It built a trophic levelindex(TLI) model to assess the eutrophication, the results showed that: from2009（TLI=28.56）to2011（TLI=30.19）, the nutritional level of Chagan Lake isoligotrophic into moderate eutrophication. The risks of eutrophication in Chagan Lakeexist.
引文
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