层状硅酸盐矿物用于污染土壤中汞的固定稳定化的研究
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摘要
汞作为重要的工业原料,在各个领域均有广泛的应用,但汞和汞的化合物都是有毒且毒性持续时间长,又能够被生物所富集的化学物质,存在极大的危害性。进入土壤中的汞除一部分能被土壤迅速吸收或固定,还有一部分汞可通过各种形式发生迁移,造成二次污染,土壤汞污染是一项亟待解决的问题。
土壤对汞的固定能力主要来自土壤中的矿物质和有机质,起到固定能力的主要反应是离子交换吸附、表面配合和表面吸附。层状硅酸盐矿物的结构特点对三种吸附反应均有良好的效果,因此选择三种典型层状硅酸盐矿物:蛭石、蒙脱石、高岭土作为污染土壤中汞的固定稳定化剂开展研究。
本实验中发现土壤本身对汞有着很好的固定稳定化能力,在含汞30—135mg/Kg时浸出液浓度低于《危险废物鉴别标准浸出毒性鉴别(GB5085.3-2007)》要求的0.1mg/L;1200mg/Kg以下时,固定稳定化率高于90%;在900mg/Kg时土壤的固定稳定化能力达到饱和;随着汞浓度的升高,土壤对硝酸汞的固定稳定化能力大于氯化汞。
三种矿物对汞的吸附迅速,在150min时达到平衡,其吸附对准二级动力学模型拟合良好,吸附过程由多种反应综合控制。三种矿物对汞都有较好的吸附能力,吸附量随着平衡浓度的增加而增加,最大吸附量分别为,蛭石8.7184mg/g,蒙脱石6.9686mg/g,高岭土6.3205mg/g。投加矿物后土壤浸出液的浓度迅速下降,降低了60%左右,随着投加量的增加,浸出液浓度不断降低。
三种矿物经过酸改性后,最大吸附量有了明显的提高,酸改性对蒙脱石的影响最大;随着酸浓度的增大,最大吸附量均随之提高;在酸浓度1.100mol/L时最大吸附量出现回落;而蒙脱石和高岭土的回落比蛭石要明显偏大。
三种矿物经过热改性,其最大吸附量都有了明显的增加,其中蒙脱石最大吸附量的增加最大,蛭石次之,高岭土的提高最小。蛭石和蒙脱石的最大吸附量都在300-350℃时上升,随后下降,在600℃时下降加速,高岭土的吸附量从300℃时开始稳定下降,下降幅度不大。
Mercury is used as raw material in various kinds of industry. Because the Mercury and Mercury compounds are long-term poisonous and also can be accumulate by biology, these materials are deleterious. Part of the Mercury in the soil can be adsorbed or fixed by the soil, and the other part can transport in different ways. These kinds of transportation lead to secondary pollution. So the treatment of Hg-pollution in soil is urgent needed.
The mineral matter and the organic matter in the soil play a leading role for the immobilization, and the main reactions are ion exchange adsorption, surface complexation, and surface adsorption. The structural characteristics of the Phyllosilicates are favorable for all the three reactions. So three kind of typical Phyllosilicates are chose as the annexing agent to fix the Mercury in the soil.
The experiments showed that this soil has high level of ability to fix Mercury. When the contents of Mercury are 30—135mg/Kg in the soil, the contents of Mercury in the leaching solutions of the soil are lower than 0.1mg/L which is the standard in‘the Standards of Dangerous Waste Identification-leaching toxicity (GB5085.3-2007)’. When the contents of Mercury in the soil are lower than 1200mg/Kg, the efficiency for stabilization of mercury in the soil are higher than 90%. When the content of Mercury in the soil is higher than 900mg/Kg, the Mercury is saturated. With the increasing of contents , the soil’s ability to fix Mercuric nitrate is higher than it to fix Mercuric chloride.
For the three kind of Phyllosilicates, the adsorptions react quickly. At 150 minutes, the adsorptions reached the balance. Second-order equations can describe the adsorptions of Mercury well. The adsorptions are controlled by several reactions. All the three kind of Phyllosilicates have high ability to adsorb Mercury, and the adsorption quantities are increased as the increasing of equilibrium concentration. For vermiculite, the saturation adsorption quantity is 8.7184mg/g; and for smectite, it is 6.9686mg/g; and for kaolin, it is 6.3205mg/g. After adding the Phyllosilicates to the Hg-pollution soil, the contents of Mercury in the leaching solutions of the soil decreased sharply, were decreased by 60%. And the contents are decreasing with the increasing of the addition of the Phyllosilicates.
For the three kind of Phyllosilicates, after modified by acid, the saturation adsorption quantities are increased sharply, and the smectite has the largest increase. For all the three kind of Phyllosilicates, the saturation adsorption quantities are increased as the increasing of acid contents. When the acid content is 1.100mol/L, the saturation adsorption quantities decreased, and decreases of the smectite and kaolin are larger than that of vermiculite.
For the three kind of Phyllosilicates, after modified by heat, the saturation adsorption quantities are increased sharply, and the smectite had the largest increase, and the vermiculite had a lesser one, and the kaolin had the least one. For the vermiculite and smectite, at 300-350℃, both of them increased with the increasing of temperature, and then decreased, at 600℃the saturation adsorption quantities decreased sharply. The kaolin’s saturation adsorption quantity decrease with the increasing of temperature from 300℃to 600℃steadily, but the decrease was not too large.
土壤对汞的固定能力主要来自土壤中的矿物质和有机质,起到固定能力的主要反应是离子交换吸附、表面配合和表面吸附。层状硅酸盐矿物的结构特点对三种吸附反应均有良好的效果,因此选择三种典型层状硅酸盐矿物:蛭石、蒙脱石、高岭土作为污染土壤中汞的固定稳定化剂开展研究。
本实验中发现土壤本身对汞有着很好的固定稳定化能力,在含汞30—135mg/Kg时浸出液浓度低于《危险废物鉴别标准浸出毒性鉴别(GB5085.3-2007)》要求的0.1mg/L;1200mg/Kg以下时,固定稳定化率高于90%;在900mg/Kg时土壤的固定稳定化能力达到饱和;随着汞浓度的升高,土壤对硝酸汞的固定稳定化能力大于氯化汞。
三种矿物对汞的吸附迅速,在150min时达到平衡,其吸附对准二级动力学模型拟合良好,吸附过程由多种反应综合控制。三种矿物对汞都有较好的吸附能力,吸附量随着平衡浓度的增加而增加,最大吸附量分别为,蛭石8.7184mg/g,蒙脱石6.9686mg/g,高岭土6.3205mg/g。投加矿物后土壤浸出液的浓度迅速下降,降低了60%左右,随着投加量的增加,浸出液浓度不断降低。
三种矿物经过酸改性后,最大吸附量有了明显的提高,酸改性对蒙脱石的影响最大;随着酸浓度的增大,最大吸附量均随之提高;在酸浓度1.100mol/L时最大吸附量出现回落;而蒙脱石和高岭土的回落比蛭石要明显偏大。
三种矿物经过热改性,其最大吸附量都有了明显的增加,其中蒙脱石最大吸附量的增加最大,蛭石次之,高岭土的提高最小。蛭石和蒙脱石的最大吸附量都在300-350℃时上升,随后下降,在600℃时下降加速,高岭土的吸附量从300℃时开始稳定下降,下降幅度不大。
Mercury is used as raw material in various kinds of industry. Because the Mercury and Mercury compounds are long-term poisonous and also can be accumulate by biology, these materials are deleterious. Part of the Mercury in the soil can be adsorbed or fixed by the soil, and the other part can transport in different ways. These kinds of transportation lead to secondary pollution. So the treatment of Hg-pollution in soil is urgent needed.
The mineral matter and the organic matter in the soil play a leading role for the immobilization, and the main reactions are ion exchange adsorption, surface complexation, and surface adsorption. The structural characteristics of the Phyllosilicates are favorable for all the three reactions. So three kind of typical Phyllosilicates are chose as the annexing agent to fix the Mercury in the soil.
The experiments showed that this soil has high level of ability to fix Mercury. When the contents of Mercury are 30—135mg/Kg in the soil, the contents of Mercury in the leaching solutions of the soil are lower than 0.1mg/L which is the standard in‘the Standards of Dangerous Waste Identification-leaching toxicity (GB5085.3-2007)’. When the contents of Mercury in the soil are lower than 1200mg/Kg, the efficiency for stabilization of mercury in the soil are higher than 90%. When the content of Mercury in the soil is higher than 900mg/Kg, the Mercury is saturated. With the increasing of contents , the soil’s ability to fix Mercuric nitrate is higher than it to fix Mercuric chloride.
For the three kind of Phyllosilicates, the adsorptions react quickly. At 150 minutes, the adsorptions reached the balance. Second-order equations can describe the adsorptions of Mercury well. The adsorptions are controlled by several reactions. All the three kind of Phyllosilicates have high ability to adsorb Mercury, and the adsorption quantities are increased as the increasing of equilibrium concentration. For vermiculite, the saturation adsorption quantity is 8.7184mg/g; and for smectite, it is 6.9686mg/g; and for kaolin, it is 6.3205mg/g. After adding the Phyllosilicates to the Hg-pollution soil, the contents of Mercury in the leaching solutions of the soil decreased sharply, were decreased by 60%. And the contents are decreasing with the increasing of the addition of the Phyllosilicates.
For the three kind of Phyllosilicates, after modified by acid, the saturation adsorption quantities are increased sharply, and the smectite has the largest increase. For all the three kind of Phyllosilicates, the saturation adsorption quantities are increased as the increasing of acid contents. When the acid content is 1.100mol/L, the saturation adsorption quantities decreased, and decreases of the smectite and kaolin are larger than that of vermiculite.
For the three kind of Phyllosilicates, after modified by heat, the saturation adsorption quantities are increased sharply, and the smectite had the largest increase, and the vermiculite had a lesser one, and the kaolin had the least one. For the vermiculite and smectite, at 300-350℃, both of them increased with the increasing of temperature, and then decreased, at 600℃the saturation adsorption quantities decreased sharply. The kaolin’s saturation adsorption quantity decrease with the increasing of temperature from 300℃to 600℃steadily, but the decrease was not too large.
引文
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Gilberto Abate,Jaim Lichtiq,Masini Jorqe C. Construction and evaluation of a flow -through cell adapted to a commercial staticmercury drop electrode(SMDE)to study the adsorption of Cd(Ⅱ)and Pb(Ⅱ)on vermiculite.Talanta,2002,Vol.58,No.3:433～443.
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