三峡库区土壤磷素界面迁移特征及其控制研究
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摘要
我国的湖泊富营养化问题日益加重,太湖、巢湖和滇池等严重富营养化湖泊已被列为国家水污染控制的重点。大量研究表明,农业非点源磷污染对水环境的恶化具有十分显著的贡献,富营养化现象的发生与土壤磷素的流失密切相关,如在云南滇池入湖的总磷中,农业非点源磷占28%,而在山东南四湖这一比例高达68%。
三峡工程是集发电、航运和防洪于一体的特大型水利工程,库区水环境安全关系到全国经济社会发展的全局。工程淹没土地632 km~2,其库周形成高程为30 m,面积约为60万亩的消落带。消落区土壤淹没后将成为水体N、P等营养物质的重要集纳地和释放源；消落区周期性淹水,土地干湿交替,N、P、重金属等污染物的释放迁移加剧。此外,重庆地貌类型以低山丘陵为主,60%以上的土地为坡耕地,70%以上的土壤为抗蚀性较差的紫色土。土壤平均侵蚀模数4555吨／km2.a,侵蚀总量2.87亿吨／年,入江泥沙量1.45亿吨／年,占长江上游入江泥沙量26%。农业面源污染由于不容易控制,势必成为库区水体营养物质的重要来源。因此,消落区土壤对磷的固定与释放对库区水环境安全就显得十分重要,而影响土壤磷吸持解吸性能最大的因素是土壤胶体。许多研究证实,土壤胶体携带磷而造成磷流失是引起水体富营养化的一个重要原因。从文献调研来看,有关土壤及其胶体性质对磷的吸附解吸影响的同步比较研究报道较少,而磷素随土壤胶体的淋失是坡地土壤磷迁移进入水体的重要方式,不同来源的土壤／胶体与环境条件对于磷的迁移、转化具有深刻的影响,因而系统地研究土壤及其胶体与环境条件对磷的迁移转化影响具有重要的理论意义,特别是以坡耕地为主的三峡库区,在这些方面的研究几乎处于空白。
三峡库区消落区土壤磷吸附解吸研究尽管有一些报道,但与消落区土壤胶体结合研究磷的吸附解吸还未见报道。以往干湿交替和有机酸存在条件下土壤磷释放机制研究,主要是围绕土壤磷形态的转化、作物对磷的吸收和土壤磷的生物有效性而开展的,但针对三峡水库周期性淹水-出露的特殊库水调度方式,从保护水环境角度研究淹水土壤和干湿交替下的磷释放机制及其环境效应尚显不足。同时,由于三峡库区特殊的地形地貌、土壤特性和降雨条件,农业土壤磷素的径流迁移是水体面源污染的主要来源,如何采用简单易行、经济高效的方法控制土壤磷素淋失是需要解决的关键技术问题。聚丙烯酰胺(PAM)可改善土壤物理性质和水分入渗性能,在控制径流养分迁移方面具有应用潜力,但在三峡库区农业生态环境条件F,对PAM的作用效果和优化施用条件,还缺乏系统的研究报道。因此,系统地开展三峡库区消落区典型土壤在不同外部作用条件下(包括pH、低分子量有机酸、周期性淹水模式)对磷的吸持解吸机制,对于在理论上系统阐释消落区土壤磷的迁移转化机制和外部影响条件具有重要的意义；开展库区紫色土坡耕地特定的区域生态环境条件下(坡度、雨强等)PAM对土壤磷流失控制效应及机制,可为坡耕地养分流失控制技术的研发提供基础依据。因此,本文研究对于减轻库区水体富营养化、有效地指导库区水污染防治、保障库区水质安全具有重要的理论与现实意义。
本文以三峡库区消落区典型土壤和重庆坡耕地紫色土为研究对象,研究了消落区土壤及其胶体对磷的吸附与解吸特征,上覆水淹水、干湿交替和有机酸存在下消落区土壤磷的迁移特征,探讨了模拟江水淹水条件下土壤磷素迁移的影响因素和机制；通过等温吸附试验、土柱淋溶试验和人工模拟降雨试验,研究了PAM对紫色土坡耕地土壤磷迁移的影响及其效应。主要研究结果如下：
1.三峡库区消落区潮土、紫色土、黄壤等3种土壤及其胶体对磷的等温吸附解吸试验表明,吸附过程均能很好地用Langmuir方程描述。黄壤的最大吸附量为1666.67 mg／kg,约是潮土的3.7倍,紫色土的2.8倍。土壤磷最大吸附量与土壤中FeOx.AlOx含量一致,而与有机质和粘粒关系不明显；磷解吸率顺序为潮土>紫色土>黄壤。3种土壤胶体对磷的吸附远强于其母体土壤,黄壤胶体、潮土胶体和紫色土胶体对磷的最大吸附量分别为4039.3.3155.9和3117.5 mg／kg,分别为相应土壤磷最大吸附量的2.4、6.9和5.3倍。土壤胶体吸附磷的反应速率比相应母体土壤高。土壤胶体对磷的吸附反应以化学吸附为主,而土壤则以物理吸附为主。
三种土壤胶体动态等温吸附／解吸磷的动力学过程均符合抛物扩散定律。在225 min时,土壤胶体动态等温磷累积吸附量顺序为：黄壤胶体>紫色土胶体>潮土胶体；紫色土胶体、潮土胶体动态等温解吸率相接近(约22.7%),均高于黄壤胶体的解吸率(14.11%)。
2.模拟江水初次淹水期,土壤磷释放能力和速率为潮土>紫色土>黄壤,三种土壤释放到上覆水中的磷量均随土壤添加磷量的提高和淹水时间的延长而增加。土壤磷释放量与淹水时间(4-30d)的关系均可用直线方程Q=a+bt描述。潮土、紫色土、黄壤淹水落干后再淹水的土壤磷释放量、释放速率均明显低于初次淹水期。
土壤对上覆水中磷的动态吸附试验表明,上覆水磷浓度均随淹水时间增加而逐渐降低,初期(≤14 d)土壤吸附速度快,而后期(≥15 d)吸附速度减缓。3种土壤对上覆水磷吸附量与淹水时间关系可用方程Q=a-b|n(t+c)描述。3种土壤对上覆水磷吸附量顺序为：黄壤>紫色土>潮土。
上覆水pH对土壤磷的释放有显著影响,释放量与上覆水初始pH的关系可用非线性方程Q_DP=a·x~b描述。在酸性或碱性强的水体中,土壤磷的释放潜力大,中性水体中释放潜力最低。淹水时间越长,上覆水初始pH对土壤磷释放影响的差异越不明显。
3.相同有机酸作用下,在添加与未添加磷时潮土中磷的释放具有相同的变化趋势,但磷的释放量是前者明显高于后者。有机酸作用下,土壤磷释放能力顺序为紫色潮土>灰棕潮土>黄壤。相同淹水时间,3种有机酸促进同种土壤磷释放能力的顺序为草酸>柠檬酸>酒石酸。有机酸还可促进土壤中铁、锰离子的释放,有机酸浓度越高则释放量越大,对铁离子为柠檬酸>草酸>酒石酸,对锰离子为柠檬酸>酒石酸>草酸。上覆水中土壤磷释放量与铁、锰离子浓度呈极显著正相关。
4.添加PAM土壤磷的等温吸附解吸试验表明,土壤磷吸附量(Q)与PAM(聚丙烯酰胺)使用量(x)的关系可以用指数方程Q=95.5179x~(-03295)描述。在添加PAM后土壤磷吸附量有不同程度降低。土壤对磷的最大缓冲容量(MBC)随PAM用量的增加而增大,最大吸附量(Xm)则降低,但土壤对磷的吸附速率增大和白发性增强。当PAM施入浓度为0.1%～0.2%时,PAM对磷的解吸影响不显著,而在较高浓度(0.4%)时对磷的解吸影响才显著。
土柱淋溶试验表明,施入土壤的PAM显著抑制了磷素在土柱中的垂直迁移,且施用量越大控制效果越明显。
模拟降雨条件下,PAM对坡地试验土槽的表面径流产生总体上表现为滞后效应,有助于壤中流的产生。PAM对较大坡度坡地径流的控制明显强于缓坡。在坡度为15。的坡地,当PAM的施用量为32 mg/kg时,两次降雨过程中总磷(TP)的流失总量为24.48 mg,仅为对照的11.8%；颗粒态磷(PP)的流失总量为3.49 mg,仅为对照的2.4%。当FAM的施用量为32 mg/kg时,15°、20°坡度处理时获得的表面径流总量分别为37.35 L和38.59 L,比8。处理分别减少11.0%和8.1%。PAM对中雨强(34 mm·h-1)下磷素地表径流流失的控制效果较好,而对大雨强下坡地壤中流中磷素的控制效果好于低、中雨强。土壤地表径流总磷的累积流失量与径流历时的关系可用指数方程Q=ath描述。Ⅲ
The Eutrophication occurred in water bodies of China is becoming more aggravated, and several lakes such as Taihu, Caohu and Dianchi have been emphasized as the hot point of water control pollution. Recently many research results showed that water quality pollution caused by phosphorous pollution inlet, mainly account for agricultural non-point (ANP) pollution. Meanwhile, eutrophication has a significant relationship with phosphorous (P) losses from soils, for instance, water pollution caused by phosphorous losses from agricultural non-point highly accounted for 28%and 68%in Dianchi in Yunnan province and Nansihu in Shandong province respectively.
The Three Gorges reservoir is an oversize reservoir with multifunction such as electricity generation, shipping and flood regulations. The environmental water security of the reservoir is so important that affects the country's entire society-economy development. The reservoir project inundated 632 km~2 of land, as the water level fluctuation zones (WLFZ) created due to flooding, which cover an area with 30m vertical height and more than 400 km2 in the reservoir. After flooding or inundation occur, the water level fluctuation zones will be an important pool and source of nitrogen and phosphorous, which accompanied with periodic flooding and alternation of wet and dry conditions, furthermore exacerbated the releases of pollutants including nitrogen (N), P and heavy metals. In addition, in Chongqing, the most of geomorphic type belongs to lands and hills with low slope, which more than 60%of areas are slope land, and excess 70%of soil type is purple soil susceptible to erosion. The sediment load is1.45 x 10~2 million ton/year, which account for 26%of total load from upstream of Yangtze River. Due to the difficulty of control and preventment for ANP, the water fluctuation zones are inevitable to become the most serious source of nutrients, which would cause eutrophication in Three Gorge reservoir.
From the preceding mentions, hence we know the releases and immobilizations of phosphorous from soils of WLFZS are so important for guarantee of water quality safety. However the most significant factor that impacts the adsorption and desorption of phosphorous in soils is soil colloids. Some reports had confirmed the P losses due to soil colloids bound P runoff was the one of the important mechanisms to induce eutrophication in corresponding water bodies. Despite of this broad consensus, it appears that a few researches about the effect of soil and corresponding colloids on adsorption/desorption of P, based on synchronous comparison. Additionally, P losses coupled with soil colloids losses is a vital way for slope soil P transferred into water, and the significant effect of soil/soil colloids in various conditions on P transformation and transfer also is crucial to understand the entire system, thus, it's theoretical significant to research the effect mentioned above. Especially in Three Gorges reservoir, where mainly is a slope lands areas, currently there is lack of systemic reports about the effect of typical soils/soil colloids from these areas (mainly originated from WLFZS) on the mechanism of P sorption, transformation and transfer.
Although there are a few reports about P adsorption of typical soil in WLFZS, the simultaneously researches on P adsorption of soils and related soil colloids are still scarce. Meanwhile the effect of organic acids on P transfer occurred on the water-soil interface is rare to investigated. In previous studies on the mechanism of P adsorption in the conditions of alternation of wet and dry or the existence of organic acids, which mainly focused on the transformation of P speciation, the P uptake by crops and the P availability without giving enough attention on these mechanisms based on water source protection and environmental effect. In addition, there also exist some studies about the polyacrylamide (PAM) application in various farming regions and soil types. However in Three Gorge reservoir, due to the unique environmental conditions, we still don't understand the detailed results of the coordination between PAM and environment and the comprehensive application premises, which need more systemic and entire investigations. Thus, it's so significant to relocate our research attentions on the effect of different external conditions (including pH, low molecule organic acid, periodic flooding model) on P adsorption/desorption, which is helpful to understand the mechanism of P transfer and transformation, meanwhile more better explain the effect of external conditions and interactions with entire environmental system. Additionally, investigations on mechanism and effect of PAM on P losses in the conditions such as slope and rainfall intensity etc, will supply the necessary and comprehensive basic knowledge to figure out an effective and economical way to control of nutrients losses from steep slope lands. In this dissertation, lots of works had been finished for the investigation and discussion of the mitigation mechanism and control methods of P pollution in water. Its significance is building the systemic and extensive technology bases, which have the important practical and theoretic values for mitigation eutrophication, effectively direction and guidance of water pollution treatment and prevention works in reservoir areas, and secure the water quality safety.
We conducted experiments to use typical soils in WLFZS of Three Gorges reservoir and purple soil from steep slope lands, as the research objectives for investigation of the characteristics of P adsorption in soil/soil colloid of WLFZS and the mechanism of P transfer in these areas under conditions of overlying water flooding, alternation of dry and wet and existence of organic acid. Meanwhile, this dissertation discussed the factors and mechanism, which impacted P transfer through simulated flooding experiment by adding artificial Yangtze River water. In addition, isothermal sorption, soil column and simulated rainfall experiments all were performed in attempt to identify the effect of PAM on P losses from purple soils in steep slope lands, and related factors also discussed in the following section below. In this way, the main results in our study went as follows.
Through isothermal sorption experiment of alluvial soil, purple soil and yellowish soil and related soil colloids, it demonstrated the Langmiur equation was the best fitting tool to express the sorption process. For the maximum P adsorption, yellowish soil showed the highest value 1666.67 mg/kg, which was approximately 3.7 and 2.8 times than Alluvial soil and purple soil, respectively. The max P adsorption amount was consistent with FeOx and AlOx in soils, but had a no significant relationship with organic matter and clay. Thus the order of P desorption was alluvial soil> purple soil> yellowish soil. In addition, the P adsorption of the above three soil colloids all were far higher than the soils originated from the same sources, the maximum P adsorption amount were 4039.3,3155.9 and 3117.5 mg/kg, respectively, which approximately equaled 2.4,6.9 and 5.3 times of corresponding soils. More generally, the P adsorption reaction rates of soil colloids were higher than corresponding soils, which indicated the major reaction was chemical sorption, and second physical sorption in the process of P adsorption of soils colloids, in comparison with corresponding soils, which showed the contrary trend.
The dynamic isothermal adsorption/desorption process of three soil colloids all were fitteds by. At 225 min, the rank of P cumulative adsorption amount was:yellowish soil colloid> purple soil colloid> alluvial soil colloid, in which the dynamic isothermal desorption rates of purple soil colloid and Alluvial soil colloid both were the same (about 22.7%), and higher than the desorption rate of yellowish soil (14.11%).
In initial stage of simulated flooding, the rank of P release capacity and rate was alluvial soil> purple soil> yellowish soil. P releases from the above soils to overlying water increased with increasing external P addition rates and time duration. During the experimental flooding time (4-30 d), the relationship between P concentrations in overlying water of three soils and simulated flooding time, could be described by linear equation as Q= a+bt.
In addition, after alternation of dry, water re-flooded in experiment to simulate the second flooding. Hence, both of the P releases amounts and rates were significantly lower than the situation in the first flooding.
Among the various P concentration levels in overlying water, the P concentrations gradually decreased with the time duration. Initially (< 14 d), the P sorption rate of soil was high, in contrast to a lower sorption rate in later period (≥15 d). For indication of the relationship between P sorption amount of overlying water from three soils and flooding time duration, the equation Q= a-bin(t+c) could used to fit and express.
The effect of pH in underlying water on soil P releases is evidentials, and the relationship between initial pH values in overlying water and P releases from soils could use non-linear equation Q_Dp= a·x~b to express. In greater acid or alkaline condition, the potential of P releases was higher. However the ability was the lowest in neural pH of water body. With the increasing time duration, the effect of initial pH on P releases is less significant.
In the condition of three organic acids with various concentrations levels in overlying water, the relationship between P releases amount and flooding time duration was given by equation Q_DP= a x t~b. Due to the impact of organic acid, the P release capacity of three soils followed as alluvial soil> grey alluvial soil> yellowish soil. At the same flooding time duration, the rank of three organic acids increasing P releases was oxalic acid> citric acid> tartaric acid. Meanwhile, our experiment suggested that the organic acids promoted the Fe and Mn ions releases, with more concentrations of organic acids, more release amounts. The both of order of organic acids increasing Fe and Mn ions releases from soils were: citric acid> oxalic acid> tarteric acid, and citric acid> tartaric acid> oxalic acid, respectively. Additionally, the P releases in overlying water had a significant relationship with Fe and Mn ions concentrations.
The isothermal adsorption/desorption curve of soils treated by PAM indicated the relationship between P adsorption amount (Q), PAM application rate (x) could be fitted and expressed as Q= 95.5179X~(-0.3295). The P adsorption decreased by different extents when PAM added into. However the maximum buffer capacity (MBC) was promoted with PAM application rates increasing, in contrast to decreasing maximum adsorption amount (Xm), meanwhile the both of increasing P adsorption rate and reaction spontaneity were observed in our experiment. When PAM application rates were low (among 0.1%-0.2%, by weight/weight), no significant effect on P desorption was observed, conversely, the effect was so significant under greater PAM application rate (0.4%PAM, by w/w).
The soil column experiment demonstrated the PAM applied in soil significantly inhibited the P losses in vertical directions in soil column, and the effect of application was much greater with increasing PAM application rate.
In simulated rainfall condition, the total effect of PAM on runoff load produced in purple slope soil was hysteretic, which helped the generation of interflows. Meanwhile, the effect of PAM application on runoff from steeper slope lands, rather than gentle slope lands, is more significant. Building on this insight and experimental data, in the process of control of P losses from purple soil, the optimal application rate was 32 mg/kg when slope is 15°. In the two process of simulated rainfall, the total P losses and particle P from treatments were 24.48 mg and 3.49 mg, which only accounted for 11.8%and 2.4%of control group, respectively. Furthermore, the total runoff from 15°and 20°were 37.35 L和38.59 L, decreased by 11.0% and 8.1%in comparison with treatment of 8°, respectively, with the PAM application rate was 32 mg/kg. For the rainfall intensity (RI), the effect of PAM on control of P losses from runoff was greater under medium RI. However, the control of interflows by PAM is more significant under high RI, compared with medium and low RI. Moreover, the equation Q= a·t~bcould be used to fit the relationship between total P cumulative losses from runoff and runoff time duration. IX
三峡工程是集发电、航运和防洪于一体的特大型水利工程,库区水环境安全关系到全国经济社会发展的全局。工程淹没土地632 km~2,其库周形成高程为30 m,面积约为60万亩的消落带。消落区土壤淹没后将成为水体N、P等营养物质的重要集纳地和释放源；消落区周期性淹水,土地干湿交替,N、P、重金属等污染物的释放迁移加剧。此外,重庆地貌类型以低山丘陵为主,60%以上的土地为坡耕地,70%以上的土壤为抗蚀性较差的紫色土。土壤平均侵蚀模数4555吨／km2.a,侵蚀总量2.87亿吨／年,入江泥沙量1.45亿吨／年,占长江上游入江泥沙量26%。农业面源污染由于不容易控制,势必成为库区水体营养物质的重要来源。因此,消落区土壤对磷的固定与释放对库区水环境安全就显得十分重要,而影响土壤磷吸持解吸性能最大的因素是土壤胶体。许多研究证实,土壤胶体携带磷而造成磷流失是引起水体富营养化的一个重要原因。从文献调研来看,有关土壤及其胶体性质对磷的吸附解吸影响的同步比较研究报道较少,而磷素随土壤胶体的淋失是坡地土壤磷迁移进入水体的重要方式,不同来源的土壤／胶体与环境条件对于磷的迁移、转化具有深刻的影响,因而系统地研究土壤及其胶体与环境条件对磷的迁移转化影响具有重要的理论意义,特别是以坡耕地为主的三峡库区,在这些方面的研究几乎处于空白。
三峡库区消落区土壤磷吸附解吸研究尽管有一些报道,但与消落区土壤胶体结合研究磷的吸附解吸还未见报道。以往干湿交替和有机酸存在条件下土壤磷释放机制研究,主要是围绕土壤磷形态的转化、作物对磷的吸收和土壤磷的生物有效性而开展的,但针对三峡水库周期性淹水-出露的特殊库水调度方式,从保护水环境角度研究淹水土壤和干湿交替下的磷释放机制及其环境效应尚显不足。同时,由于三峡库区特殊的地形地貌、土壤特性和降雨条件,农业土壤磷素的径流迁移是水体面源污染的主要来源,如何采用简单易行、经济高效的方法控制土壤磷素淋失是需要解决的关键技术问题。聚丙烯酰胺(PAM)可改善土壤物理性质和水分入渗性能,在控制径流养分迁移方面具有应用潜力,但在三峡库区农业生态环境条件F,对PAM的作用效果和优化施用条件,还缺乏系统的研究报道。因此,系统地开展三峡库区消落区典型土壤在不同外部作用条件下(包括pH、低分子量有机酸、周期性淹水模式)对磷的吸持解吸机制,对于在理论上系统阐释消落区土壤磷的迁移转化机制和外部影响条件具有重要的意义；开展库区紫色土坡耕地特定的区域生态环境条件下(坡度、雨强等)PAM对土壤磷流失控制效应及机制,可为坡耕地养分流失控制技术的研发提供基础依据。因此,本文研究对于减轻库区水体富营养化、有效地指导库区水污染防治、保障库区水质安全具有重要的理论与现实意义。
本文以三峡库区消落区典型土壤和重庆坡耕地紫色土为研究对象,研究了消落区土壤及其胶体对磷的吸附与解吸特征,上覆水淹水、干湿交替和有机酸存在下消落区土壤磷的迁移特征,探讨了模拟江水淹水条件下土壤磷素迁移的影响因素和机制；通过等温吸附试验、土柱淋溶试验和人工模拟降雨试验,研究了PAM对紫色土坡耕地土壤磷迁移的影响及其效应。主要研究结果如下：
1.三峡库区消落区潮土、紫色土、黄壤等3种土壤及其胶体对磷的等温吸附解吸试验表明,吸附过程均能很好地用Langmuir方程描述。黄壤的最大吸附量为1666.67 mg／kg,约是潮土的3.7倍,紫色土的2.8倍。土壤磷最大吸附量与土壤中FeOx.AlOx含量一致,而与有机质和粘粒关系不明显；磷解吸率顺序为潮土>紫色土>黄壤。3种土壤胶体对磷的吸附远强于其母体土壤,黄壤胶体、潮土胶体和紫色土胶体对磷的最大吸附量分别为4039.3.3155.9和3117.5 mg／kg,分别为相应土壤磷最大吸附量的2.4、6.9和5.3倍。土壤胶体吸附磷的反应速率比相应母体土壤高。土壤胶体对磷的吸附反应以化学吸附为主,而土壤则以物理吸附为主。
三种土壤胶体动态等温吸附／解吸磷的动力学过程均符合抛物扩散定律。在225 min时,土壤胶体动态等温磷累积吸附量顺序为：黄壤胶体>紫色土胶体>潮土胶体；紫色土胶体、潮土胶体动态等温解吸率相接近(约22.7%),均高于黄壤胶体的解吸率(14.11%)。
2.模拟江水初次淹水期,土壤磷释放能力和速率为潮土>紫色土>黄壤,三种土壤释放到上覆水中的磷量均随土壤添加磷量的提高和淹水时间的延长而增加。土壤磷释放量与淹水时间(4-30d)的关系均可用直线方程Q=a+bt描述。潮土、紫色土、黄壤淹水落干后再淹水的土壤磷释放量、释放速率均明显低于初次淹水期。
土壤对上覆水中磷的动态吸附试验表明,上覆水磷浓度均随淹水时间增加而逐渐降低,初期(≤14 d)土壤吸附速度快,而后期(≥15 d)吸附速度减缓。3种土壤对上覆水磷吸附量与淹水时间关系可用方程Q=a-b|n(t+c)描述。3种土壤对上覆水磷吸附量顺序为：黄壤>紫色土>潮土。
上覆水pH对土壤磷的释放有显著影响,释放量与上覆水初始pH的关系可用非线性方程Q_DP=a·x~b描述。在酸性或碱性强的水体中,土壤磷的释放潜力大,中性水体中释放潜力最低。淹水时间越长,上覆水初始pH对土壤磷释放影响的差异越不明显。
3.相同有机酸作用下,在添加与未添加磷时潮土中磷的释放具有相同的变化趋势,但磷的释放量是前者明显高于后者。有机酸作用下,土壤磷释放能力顺序为紫色潮土>灰棕潮土>黄壤。相同淹水时间,3种有机酸促进同种土壤磷释放能力的顺序为草酸>柠檬酸>酒石酸。有机酸还可促进土壤中铁、锰离子的释放,有机酸浓度越高则释放量越大,对铁离子为柠檬酸>草酸>酒石酸,对锰离子为柠檬酸>酒石酸>草酸。上覆水中土壤磷释放量与铁、锰离子浓度呈极显著正相关。
4.添加PAM土壤磷的等温吸附解吸试验表明,土壤磷吸附量(Q)与PAM(聚丙烯酰胺)使用量(x)的关系可以用指数方程Q=95.5179x~(-03295)描述。在添加PAM后土壤磷吸附量有不同程度降低。土壤对磷的最大缓冲容量(MBC)随PAM用量的增加而增大,最大吸附量(Xm)则降低,但土壤对磷的吸附速率增大和白发性增强。当PAM施入浓度为0.1%～0.2%时,PAM对磷的解吸影响不显著,而在较高浓度(0.4%)时对磷的解吸影响才显著。
土柱淋溶试验表明,施入土壤的PAM显著抑制了磷素在土柱中的垂直迁移,且施用量越大控制效果越明显。
模拟降雨条件下,PAM对坡地试验土槽的表面径流产生总体上表现为滞后效应,有助于壤中流的产生。PAM对较大坡度坡地径流的控制明显强于缓坡。在坡度为15。的坡地,当PAM的施用量为32 mg/kg时,两次降雨过程中总磷(TP)的流失总量为24.48 mg,仅为对照的11.8%；颗粒态磷(PP)的流失总量为3.49 mg,仅为对照的2.4%。当FAM的施用量为32 mg/kg时,15°、20°坡度处理时获得的表面径流总量分别为37.35 L和38.59 L,比8。处理分别减少11.0%和8.1%。PAM对中雨强(34 mm·h-1)下磷素地表径流流失的控制效果较好,而对大雨强下坡地壤中流中磷素的控制效果好于低、中雨强。土壤地表径流总磷的累积流失量与径流历时的关系可用指数方程Q=ath描述。Ⅲ
The Eutrophication occurred in water bodies of China is becoming more aggravated, and several lakes such as Taihu, Caohu and Dianchi have been emphasized as the hot point of water control pollution. Recently many research results showed that water quality pollution caused by phosphorous pollution inlet, mainly account for agricultural non-point (ANP) pollution. Meanwhile, eutrophication has a significant relationship with phosphorous (P) losses from soils, for instance, water pollution caused by phosphorous losses from agricultural non-point highly accounted for 28%and 68%in Dianchi in Yunnan province and Nansihu in Shandong province respectively.
The Three Gorges reservoir is an oversize reservoir with multifunction such as electricity generation, shipping and flood regulations. The environmental water security of the reservoir is so important that affects the country's entire society-economy development. The reservoir project inundated 632 km~2 of land, as the water level fluctuation zones (WLFZ) created due to flooding, which cover an area with 30m vertical height and more than 400 km2 in the reservoir. After flooding or inundation occur, the water level fluctuation zones will be an important pool and source of nitrogen and phosphorous, which accompanied with periodic flooding and alternation of wet and dry conditions, furthermore exacerbated the releases of pollutants including nitrogen (N), P and heavy metals. In addition, in Chongqing, the most of geomorphic type belongs to lands and hills with low slope, which more than 60%of areas are slope land, and excess 70%of soil type is purple soil susceptible to erosion. The sediment load is1.45 x 10~2 million ton/year, which account for 26%of total load from upstream of Yangtze River. Due to the difficulty of control and preventment for ANP, the water fluctuation zones are inevitable to become the most serious source of nutrients, which would cause eutrophication in Three Gorge reservoir.
From the preceding mentions, hence we know the releases and immobilizations of phosphorous from soils of WLFZS are so important for guarantee of water quality safety. However the most significant factor that impacts the adsorption and desorption of phosphorous in soils is soil colloids. Some reports had confirmed the P losses due to soil colloids bound P runoff was the one of the important mechanisms to induce eutrophication in corresponding water bodies. Despite of this broad consensus, it appears that a few researches about the effect of soil and corresponding colloids on adsorption/desorption of P, based on synchronous comparison. Additionally, P losses coupled with soil colloids losses is a vital way for slope soil P transferred into water, and the significant effect of soil/soil colloids in various conditions on P transformation and transfer also is crucial to understand the entire system, thus, it's theoretical significant to research the effect mentioned above. Especially in Three Gorges reservoir, where mainly is a slope lands areas, currently there is lack of systemic reports about the effect of typical soils/soil colloids from these areas (mainly originated from WLFZS) on the mechanism of P sorption, transformation and transfer.
Although there are a few reports about P adsorption of typical soil in WLFZS, the simultaneously researches on P adsorption of soils and related soil colloids are still scarce. Meanwhile the effect of organic acids on P transfer occurred on the water-soil interface is rare to investigated. In previous studies on the mechanism of P adsorption in the conditions of alternation of wet and dry or the existence of organic acids, which mainly focused on the transformation of P speciation, the P uptake by crops and the P availability without giving enough attention on these mechanisms based on water source protection and environmental effect. In addition, there also exist some studies about the polyacrylamide (PAM) application in various farming regions and soil types. However in Three Gorge reservoir, due to the unique environmental conditions, we still don't understand the detailed results of the coordination between PAM and environment and the comprehensive application premises, which need more systemic and entire investigations. Thus, it's so significant to relocate our research attentions on the effect of different external conditions (including pH, low molecule organic acid, periodic flooding model) on P adsorption/desorption, which is helpful to understand the mechanism of P transfer and transformation, meanwhile more better explain the effect of external conditions and interactions with entire environmental system. Additionally, investigations on mechanism and effect of PAM on P losses in the conditions such as slope and rainfall intensity etc, will supply the necessary and comprehensive basic knowledge to figure out an effective and economical way to control of nutrients losses from steep slope lands. In this dissertation, lots of works had been finished for the investigation and discussion of the mitigation mechanism and control methods of P pollution in water. Its significance is building the systemic and extensive technology bases, which have the important practical and theoretic values for mitigation eutrophication, effectively direction and guidance of water pollution treatment and prevention works in reservoir areas, and secure the water quality safety.
We conducted experiments to use typical soils in WLFZS of Three Gorges reservoir and purple soil from steep slope lands, as the research objectives for investigation of the characteristics of P adsorption in soil/soil colloid of WLFZS and the mechanism of P transfer in these areas under conditions of overlying water flooding, alternation of dry and wet and existence of organic acid. Meanwhile, this dissertation discussed the factors and mechanism, which impacted P transfer through simulated flooding experiment by adding artificial Yangtze River water. In addition, isothermal sorption, soil column and simulated rainfall experiments all were performed in attempt to identify the effect of PAM on P losses from purple soils in steep slope lands, and related factors also discussed in the following section below. In this way, the main results in our study went as follows.
Through isothermal sorption experiment of alluvial soil, purple soil and yellowish soil and related soil colloids, it demonstrated the Langmiur equation was the best fitting tool to express the sorption process. For the maximum P adsorption, yellowish soil showed the highest value 1666.67 mg/kg, which was approximately 3.7 and 2.8 times than Alluvial soil and purple soil, respectively. The max P adsorption amount was consistent with FeOx and AlOx in soils, but had a no significant relationship with organic matter and clay. Thus the order of P desorption was alluvial soil> purple soil> yellowish soil. In addition, the P adsorption of the above three soil colloids all were far higher than the soils originated from the same sources, the maximum P adsorption amount were 4039.3,3155.9 and 3117.5 mg/kg, respectively, which approximately equaled 2.4,6.9 and 5.3 times of corresponding soils. More generally, the P adsorption reaction rates of soil colloids were higher than corresponding soils, which indicated the major reaction was chemical sorption, and second physical sorption in the process of P adsorption of soils colloids, in comparison with corresponding soils, which showed the contrary trend.
The dynamic isothermal adsorption/desorption process of three soil colloids all were fitteds by. At 225 min, the rank of P cumulative adsorption amount was:yellowish soil colloid> purple soil colloid> alluvial soil colloid, in which the dynamic isothermal desorption rates of purple soil colloid and Alluvial soil colloid both were the same (about 22.7%), and higher than the desorption rate of yellowish soil (14.11%).
In initial stage of simulated flooding, the rank of P release capacity and rate was alluvial soil> purple soil> yellowish soil. P releases from the above soils to overlying water increased with increasing external P addition rates and time duration. During the experimental flooding time (4-30 d), the relationship between P concentrations in overlying water of three soils and simulated flooding time, could be described by linear equation as Q= a+bt.
In addition, after alternation of dry, water re-flooded in experiment to simulate the second flooding. Hence, both of the P releases amounts and rates were significantly lower than the situation in the first flooding.
Among the various P concentration levels in overlying water, the P concentrations gradually decreased with the time duration. Initially (< 14 d), the P sorption rate of soil was high, in contrast to a lower sorption rate in later period (≥15 d). For indication of the relationship between P sorption amount of overlying water from three soils and flooding time duration, the equation Q= a-bin(t+c) could used to fit and express.
The effect of pH in underlying water on soil P releases is evidentials, and the relationship between initial pH values in overlying water and P releases from soils could use non-linear equation Q_Dp= a·x~b to express. In greater acid or alkaline condition, the potential of P releases was higher. However the ability was the lowest in neural pH of water body. With the increasing time duration, the effect of initial pH on P releases is less significant.
In the condition of three organic acids with various concentrations levels in overlying water, the relationship between P releases amount and flooding time duration was given by equation Q_DP= a x t~b. Due to the impact of organic acid, the P release capacity of three soils followed as alluvial soil> grey alluvial soil> yellowish soil. At the same flooding time duration, the rank of three organic acids increasing P releases was oxalic acid> citric acid> tartaric acid. Meanwhile, our experiment suggested that the organic acids promoted the Fe and Mn ions releases, with more concentrations of organic acids, more release amounts. The both of order of organic acids increasing Fe and Mn ions releases from soils were: citric acid> oxalic acid> tarteric acid, and citric acid> tartaric acid> oxalic acid, respectively. Additionally, the P releases in overlying water had a significant relationship with Fe and Mn ions concentrations.
The isothermal adsorption/desorption curve of soils treated by PAM indicated the relationship between P adsorption amount (Q), PAM application rate (x) could be fitted and expressed as Q= 95.5179X~(-0.3295). The P adsorption decreased by different extents when PAM added into. However the maximum buffer capacity (MBC) was promoted with PAM application rates increasing, in contrast to decreasing maximum adsorption amount (Xm), meanwhile the both of increasing P adsorption rate and reaction spontaneity were observed in our experiment. When PAM application rates were low (among 0.1%-0.2%, by weight/weight), no significant effect on P desorption was observed, conversely, the effect was so significant under greater PAM application rate (0.4%PAM, by w/w).
The soil column experiment demonstrated the PAM applied in soil significantly inhibited the P losses in vertical directions in soil column, and the effect of application was much greater with increasing PAM application rate.
In simulated rainfall condition, the total effect of PAM on runoff load produced in purple slope soil was hysteretic, which helped the generation of interflows. Meanwhile, the effect of PAM application on runoff from steeper slope lands, rather than gentle slope lands, is more significant. Building on this insight and experimental data, in the process of control of P losses from purple soil, the optimal application rate was 32 mg/kg when slope is 15°. In the two process of simulated rainfall, the total P losses and particle P from treatments were 24.48 mg and 3.49 mg, which only accounted for 11.8%and 2.4%of control group, respectively. Furthermore, the total runoff from 15°and 20°were 37.35 L和38.59 L, decreased by 11.0% and 8.1%in comparison with treatment of 8°, respectively, with the PAM application rate was 32 mg/kg. For the rainfall intensity (RI), the effect of PAM on control of P losses from runoff was greater under medium RI. However, the control of interflows by PAM is more significant under high RI, compared with medium and low RI. Moreover, the equation Q= a·t~bcould be used to fit the relationship between total P cumulative losses from runoff and runoff time duration. IX
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