溶解性有机质对土/气界面汞释放的影响
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摘要
环境汞污染问题自20世纪50年代日本发生水俣病(Minamata Disease)事件以来,一直是环境科学领域的研究热点问题之一。最近十几年来,人们发现汞可以通过大气环流发生长距离传输污染,因而大气汞的库存量及其输入与输出通量受到特别关注。据估计,全球每年输入到大气中汞的总量约为6000-7500 t,其中自然释汞约占1/3。在自然释汞源中,土壤是最主要的汞源之一。散发到大气中的汞经过一定时间和距离的传输后,超过90%的部分最终会回落到陆地生态系统,并通过陆生食物链威胁人类健康。施用有机物料是农业生产中广泛应用的农艺措施,有研究发现,有机物料进入土壤后会产生大量溶解性有机质(DOM),DOM化学性质非常活跃,对重金属Hg吸附解吸、迁移转化及生物毒性有显著的影响。因此,本试验以重庆市典型土壤--紫色潮土、黄壤和紫色土为调查研究对象,采用模拟试验研究DOM在各种条件下对土/气界面汞释放量的影响,同时对模拟前的紫色土中的汞形态进行分析,研究DOM在各种条件下对紫色土中汞形态变化的影响,最后考察在DOM影响下紫色土中汞各形态变化与土/气界面汞释放量之间是否有相关性。研究结果如下:
在模拟试验中对土/气界面汞释放量的监测结果中可以得知:在三种土壤中加入DOM后,会降低土/气界面的汞释放量;不同的DOM对汞释放量的影响程度不同,其中以堆肥DOM对汞释放量的抑制作用最强;DOM对土/气界面汞释放量的影响与其添加量即最后土壤中的DOM浓度有关,随着土壤DOM浓度的增加,其对土/气界面汞释放量的抑制作用也越强;
在本试验中的两种外源汞浓度下,添加三种DOM都基本上对三种土壤的土/气界面汞释放量有不同程度的抑制作用,并且这种抑制作用会随外源汞浓度的增大而变得更加明显;
DOM对土/气界面汞释放量的影响和其与土壤汞的作用时间,即陈化时间有关,随着陈化时间的增长,无论是否添加DOM,土/气界面的汞释放量都呈下降趋势。未添加DOM的土样,其土/气界面汞释放量下降程度要比添加了DOM的更大;
由于土壤的理化性质各异,如pH、机械组成等的不同,使得三种土壤在同种条件下土/气界面汞释放量的大小不同,其顺序基本为紫色潮土＞紫色土＞黄壤。
在模拟试验中对模拟前紫色土中汞形态的分析结果中可以得知:添加DOM后会使紫色土中各形态含量发生变化。与未添加DOM的土样比较,腐殖土DOM使水溶态酸溶态含量下降,碱溶态、有机态和残留态含量上升;堆肥DOM会使水溶态、酸溶态和有机态含量下降,而使碱溶态和残留态含量上升;稻草DOM会使水溶态、酸溶态含量下降,而使碱溶态、有机态和残留态含量上升;
随着三种DOM添加量的增加,水溶态和酸溶态汞含量都有下降的趋势,其中以稻草DOM最为明显,并且残留态汞含量随稻草DOM添加量的增加有明显的上升趋势;
未添加DOM和添加堆肥DOM的土样受陈化时间长短的影响不大,添加腐殖土DOM和稻草DOM使紫色土中酸溶态汞含量随时间推移明显下降,而残留态汞明显上升;在添加了稻草DOM的紫色土中,酸溶态的下降趋势很明显,从1d到3d,下降了0.0276mg/kg,从3d到5d下降了0.0097mg/kg,总共变化0.0373mg/kg。
和未添加外源汞的土样相比,添加外源汞使得汞形态分布发生变化;外源汞浓度不同,汞形态分布也有所差异,并且汞浓度越大,DOM的添加使得汞形态含量分布对照未添加DOM时的变化也越大。
对整个试验过程中紫色土土/气界面汞释放量和相对应的土壤汞形态含量进行相关性分析,发现紫色土土/气界面的汞释放量与水溶态汞和碱溶态汞含量的变化有相关关系,其中水溶态是正相关关系,相关系数为0.479~(**),碱溶态为负相关关系,相关系数为-0.524~(**),两者都达到了极显著水平。
Since the Minamata disease happened in Japan in the 1950s', environmental mercury pollution has been one of the hot issues study in the field of the environmental science. In the recent 10 years, it was discovered that long-distance transmission of mercury could lead to contamination through the circulation of the atmosphere and the stock of the mercury in the atmosphere and the flux of its input and output were paid special attention. It is estimated that the total amount of mercury that entered the atmosphere every year in the world is about 6000-75001, of which the natural released mercury is about 1/3. Soil is the main source of the natural released mercury. After the mercury is transmited for a certain period of time and distance in the atmosphere, over 90 percent of it would eventually come down to terrestrial ecosystems, and threat human health through terrestrial food chain. Application of organic fertilizer is a widely adopted agronomic method in the agricultural activity. It is found that there would be a large amount of dissolved organic matter (DOM) when the organic fertlizer enter into the soil. The chemical properties of DOM is very active, and it has great impact on the adsorption and desorption, migration and conversion even biological toxicity on the heavy metal Hg. Accordingly, this trial choose Chongqing's typical soil-purple tide soil, yellow soil and purple soil as the object of investigation, test the impact that DOM has on the exchange of mercury in the soil/air interface under a variety of conditions by the simulation test, analyse the forms of mercury in purple soil before the simulation, research the impact that DOM has on the change of mercury's forms in the purple soil under a variety of condition, and finally inspect whether there is relationship between the changes of mercury's form in the purple soil and the release amount of mercury from the soil/air interface under the effect of DOM. The results are as follows:
From the monitoring results of the mercury amount from the soil/air interface, it is found that: adding DOM to the three kinds of soils would reduce the mercury release amount from the soil/air interface; different DOMs have different impact on the mercury release amount from the soil/air interface, and the compost DOM have the strongest inhibit effect on the amount of mercury release. The DOM's impact on the mercury release amount from the soil/air interface is related to the adding amount(that is the last concentration adding to the soil). With the increasing concentration of the DOM in the soil, the inhibit effect on the mercury release amount from the soil/air interface would be stronger.
Under the two kinds of the exotic mercury's concentration, the three sorts of DOM mainly have different degrees of restraining effect to the mercury release amount from the soil/air interface of the three kinds of soil, and this restraining effect becomes more obvious as the concentration of the exotic mercury becomes stronger.
DOM's impact on the mercury release amount from the soil/air interface is related to the reaction time(that is the aged time) between DOM and soil mercury. As the aged time's growing, whether the DOM is added or not, the trend of the mercury release amount from the soil/air interface drops. The dropping degrees of the mercury release amount from the soil/air interface of soil samples with no DOM is greater than the one with DOM.
As the physical and chemical properties of different soils are different, such as their differrent pH, mechanical components ,that make the mercury release amount from the soil/air interface of three kind of soils is diffenrent under the same condition. Basically ,the sequence is purple tide soil> purple soil> yellow soil.
From the result of analysing the forms of mercury in purple soil before the simulation we know that: the content of the chemicals in the purple soil would change after adding DOM. Compared with the soil samples in which DOM is not added, DOM from humic soil would make the content of water-soluble and acid-soluble form decline, but make the content of alkali-soluble form、organic matter form and residual form increase; DOM from compost would make the content of water-soluble form、acid-soluble form and organic matter form decline, but make the content of alkali-soluble form and residual form increase; DOM from straw would make the content of water-soluble form and acid-soluble form decline, but make the content of alkali-soluble form、organic matter form and residual form increase;
As the increasing of the adding amount of the three kinds of DOM, there is a declining tendency of the content of water-soluble form and acid-soluble form, the tendency of straw is particularly obvious, and there's an obvious rising tendency in the content of residual form when the straw DOM's adding amount is increased.
The soil samples with no DOM and compost DOM added are rarely effected by the aged time. The contents of mercury of acid-soluble form in purple soils with straw DOM and compost DOM added drop obviously as the time grows, while the residual form rises; the contents of acid-soluble form mercury in purple soils with straw DOM added drops obviously, the amount of declining is 0.0276mg/kg from 1d to 3d, 0.0097mg/kg from 3d to 5d, the amount varied 0.0373 mg/kg in total.
Compared with the soil sample with no exotic mercury added into, the one that add the exotic mercury made the allocation of the mercury's form change; Differrent concentration of the exotic mercury makes varied allocation of the mercury's form, and with DOM added into the soil, contradistinguishing with that with no DOM added into, the more concentrated the mercury, the greater change the allocation of the content of the mercury' form would have.
The relation between the mercury release amount from the soil/air interface and the corresponding content of soil mercury form is analyzed. It's found that there's relationship between mercury release amount from the soil/air interface and content of water-soluble form mercury and alkali-soluble form mercury. There's a significant positive corresponding with content of water-soluble form mercury, the correlation coefficient is 0.479**, and a significant negative corresponding with alkali-soluble form mercury, the correlation coefficient is -0.524**.
在模拟试验中对土/气界面汞释放量的监测结果中可以得知:在三种土壤中加入DOM后,会降低土/气界面的汞释放量;不同的DOM对汞释放量的影响程度不同,其中以堆肥DOM对汞释放量的抑制作用最强;DOM对土/气界面汞释放量的影响与其添加量即最后土壤中的DOM浓度有关,随着土壤DOM浓度的增加,其对土/气界面汞释放量的抑制作用也越强;
在本试验中的两种外源汞浓度下,添加三种DOM都基本上对三种土壤的土/气界面汞释放量有不同程度的抑制作用,并且这种抑制作用会随外源汞浓度的增大而变得更加明显;
DOM对土/气界面汞释放量的影响和其与土壤汞的作用时间,即陈化时间有关,随着陈化时间的增长,无论是否添加DOM,土/气界面的汞释放量都呈下降趋势。未添加DOM的土样,其土/气界面汞释放量下降程度要比添加了DOM的更大;
由于土壤的理化性质各异,如pH、机械组成等的不同,使得三种土壤在同种条件下土/气界面汞释放量的大小不同,其顺序基本为紫色潮土＞紫色土＞黄壤。
在模拟试验中对模拟前紫色土中汞形态的分析结果中可以得知:添加DOM后会使紫色土中各形态含量发生变化。与未添加DOM的土样比较,腐殖土DOM使水溶态酸溶态含量下降,碱溶态、有机态和残留态含量上升;堆肥DOM会使水溶态、酸溶态和有机态含量下降,而使碱溶态和残留态含量上升;稻草DOM会使水溶态、酸溶态含量下降,而使碱溶态、有机态和残留态含量上升;
随着三种DOM添加量的增加,水溶态和酸溶态汞含量都有下降的趋势,其中以稻草DOM最为明显,并且残留态汞含量随稻草DOM添加量的增加有明显的上升趋势;
未添加DOM和添加堆肥DOM的土样受陈化时间长短的影响不大,添加腐殖土DOM和稻草DOM使紫色土中酸溶态汞含量随时间推移明显下降,而残留态汞明显上升;在添加了稻草DOM的紫色土中,酸溶态的下降趋势很明显,从1d到3d,下降了0.0276mg/kg,从3d到5d下降了0.0097mg/kg,总共变化0.0373mg/kg。
和未添加外源汞的土样相比,添加外源汞使得汞形态分布发生变化;外源汞浓度不同,汞形态分布也有所差异,并且汞浓度越大,DOM的添加使得汞形态含量分布对照未添加DOM时的变化也越大。
对整个试验过程中紫色土土/气界面汞释放量和相对应的土壤汞形态含量进行相关性分析,发现紫色土土/气界面的汞释放量与水溶态汞和碱溶态汞含量的变化有相关关系,其中水溶态是正相关关系,相关系数为0.479~(**),碱溶态为负相关关系,相关系数为-0.524~(**),两者都达到了极显著水平。
Since the Minamata disease happened in Japan in the 1950s', environmental mercury pollution has been one of the hot issues study in the field of the environmental science. In the recent 10 years, it was discovered that long-distance transmission of mercury could lead to contamination through the circulation of the atmosphere and the stock of the mercury in the atmosphere and the flux of its input and output were paid special attention. It is estimated that the total amount of mercury that entered the atmosphere every year in the world is about 6000-75001, of which the natural released mercury is about 1/3. Soil is the main source of the natural released mercury. After the mercury is transmited for a certain period of time and distance in the atmosphere, over 90 percent of it would eventually come down to terrestrial ecosystems, and threat human health through terrestrial food chain. Application of organic fertilizer is a widely adopted agronomic method in the agricultural activity. It is found that there would be a large amount of dissolved organic matter (DOM) when the organic fertlizer enter into the soil. The chemical properties of DOM is very active, and it has great impact on the adsorption and desorption, migration and conversion even biological toxicity on the heavy metal Hg. Accordingly, this trial choose Chongqing's typical soil-purple tide soil, yellow soil and purple soil as the object of investigation, test the impact that DOM has on the exchange of mercury in the soil/air interface under a variety of conditions by the simulation test, analyse the forms of mercury in purple soil before the simulation, research the impact that DOM has on the change of mercury's forms in the purple soil under a variety of condition, and finally inspect whether there is relationship between the changes of mercury's form in the purple soil and the release amount of mercury from the soil/air interface under the effect of DOM. The results are as follows:
From the monitoring results of the mercury amount from the soil/air interface, it is found that: adding DOM to the three kinds of soils would reduce the mercury release amount from the soil/air interface; different DOMs have different impact on the mercury release amount from the soil/air interface, and the compost DOM have the strongest inhibit effect on the amount of mercury release. The DOM's impact on the mercury release amount from the soil/air interface is related to the adding amount(that is the last concentration adding to the soil). With the increasing concentration of the DOM in the soil, the inhibit effect on the mercury release amount from the soil/air interface would be stronger.
Under the two kinds of the exotic mercury's concentration, the three sorts of DOM mainly have different degrees of restraining effect to the mercury release amount from the soil/air interface of the three kinds of soil, and this restraining effect becomes more obvious as the concentration of the exotic mercury becomes stronger.
DOM's impact on the mercury release amount from the soil/air interface is related to the reaction time(that is the aged time) between DOM and soil mercury. As the aged time's growing, whether the DOM is added or not, the trend of the mercury release amount from the soil/air interface drops. The dropping degrees of the mercury release amount from the soil/air interface of soil samples with no DOM is greater than the one with DOM.
As the physical and chemical properties of different soils are different, such as their differrent pH, mechanical components ,that make the mercury release amount from the soil/air interface of three kind of soils is diffenrent under the same condition. Basically ,the sequence is purple tide soil> purple soil> yellow soil.
From the result of analysing the forms of mercury in purple soil before the simulation we know that: the content of the chemicals in the purple soil would change after adding DOM. Compared with the soil samples in which DOM is not added, DOM from humic soil would make the content of water-soluble and acid-soluble form decline, but make the content of alkali-soluble form、organic matter form and residual form increase; DOM from compost would make the content of water-soluble form、acid-soluble form and organic matter form decline, but make the content of alkali-soluble form and residual form increase; DOM from straw would make the content of water-soluble form and acid-soluble form decline, but make the content of alkali-soluble form、organic matter form and residual form increase;
As the increasing of the adding amount of the three kinds of DOM, there is a declining tendency of the content of water-soluble form and acid-soluble form, the tendency of straw is particularly obvious, and there's an obvious rising tendency in the content of residual form when the straw DOM's adding amount is increased.
The soil samples with no DOM and compost DOM added are rarely effected by the aged time. The contents of mercury of acid-soluble form in purple soils with straw DOM and compost DOM added drop obviously as the time grows, while the residual form rises; the contents of acid-soluble form mercury in purple soils with straw DOM added drops obviously, the amount of declining is 0.0276mg/kg from 1d to 3d, 0.0097mg/kg from 3d to 5d, the amount varied 0.0373 mg/kg in total.
Compared with the soil sample with no exotic mercury added into, the one that add the exotic mercury made the allocation of the mercury's form change; Differrent concentration of the exotic mercury makes varied allocation of the mercury's form, and with DOM added into the soil, contradistinguishing with that with no DOM added into, the more concentrated the mercury, the greater change the allocation of the content of the mercury' form would have.
The relation between the mercury release amount from the soil/air interface and the corresponding content of soil mercury form is analyzed. It's found that there's relationship between mercury release amount from the soil/air interface and content of water-soluble form mercury and alkali-soluble form mercury. There's a significant positive corresponding with content of water-soluble form mercury, the correlation coefficient is 0.479**, and a significant negative corresponding with alkali-soluble form mercury, the correlation coefficient is -0.524**.
引文
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