聚环氧琥珀酸对污泥中重金属的萃取过程及机理研究
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摘要
污泥中重金属的污染是影响其资源化利用的关键问题，如何应用绿色化学的理论解决土壤及污泥中的重金属污染问题是环境科学研究的热点之一。本文在国家自然科学基金项目(No．50478103)的支持下，根据国际上绿色化学的发展趋势，针对城市工业废水污泥中重金属含量较高的特征，以上海市桃浦污水厂污泥为对象，重点研究了易生物降解的聚环氧琥珀酸(Poly-epoxy-succinic Acid，简称PESA)对污泥中重金属的分离过程，并从溶液配位化学的角度研究了聚环氧琥珀酸与典型重金属离子的相互作用机理，提出了用环境友好的聚环氧琥珀酸治理城市污泥重金属污染的修复技术。并针对矿区附近土壤普遍受重金属污染的环境现状，以福建省三明地区实际受重金属污染土壤为对象，研究了污染土壤中重金属的迁移转化规律。论文可以为受重金属污染的污泥或土壤的治理及修复提供理论指导和实际技术支持。
论文主要分为四部分：(Ⅰ)PESA(聚环氧琥珀酸)与典型重金属离子相互作用机理的研究；(Ⅱ)PESA对污泥中重金属的分离过程研究；(Ⅲ)EDDS(S，S-ethylenediaminedisuccinic Acid，乙二胺二琥珀酸)、EDTA(Ethylene DiamineTetraacetic Acid，乙二胺四乙酸)与PESA对重金属分离作用的比较研究；(Ⅳ)污染土壤中重金属迁移转化规律的研究。
第一部分：聚环氧琥珀酸与典型重金属离子相互作用机理的研究
利用pH电位滴定和先进的BEST数据处理程序，研究了PESA与典型重金属离子Zn~(2+)、pb~(2+)、Cd~(2+)、Ni~(2+)、Cr~(3+)、Cu~(2+)之间的配位化学作用，得到了PESA的酸离解常数、相应配合物的稳定常数及不同pH下各种配合物的形态分布图。研究结果表明：(1)将PESA简化为具有五个结构单元的二级电离模型的误差o较小，且模拟滴定曲线与实验滴定曲线的符合程度较好，所得的pK_a1=4．68、pK_a2=4．92，说明实验所设计的配位化学模型比较合理，结果准确。表明通过合理配位化学模型的建立来处理PESA的酸离解及其与重金属离子间的配位化学作用是可行的。(2)从溶液配位化学角度讲，PESA与重金属离子有较强的结合能力。按形成的主要配合物种ML来看，Zn~(2+)、pb~(2+)、Cd~(2+)、Ni~(2+)、Cr~(3+)、Cu~(2+)与PESA配位能力大小的顺序为Cu~(2+)>Cr~(3+)>Cd~(2+)>Zn~(2+)>Ni~(2+)>pb~(2+)。
第二部分：聚环氧琥珀酸对污泥中重金属的分离过程研究
以上海市桃浦污水厂污泥为研究对象，研究了聚环氧琥珀酸对污泥中重金属的萃取作用，重点考察了萃取体系pH值、萃取剂用量、萃取时间、萃取温度、重金属的存在形态、添加H_2O_2、添加H_3PO_4等条件对重金属萃取的影响。研究发现：(1)PESA对污泥中的重金属具有较好的萃取效果，当PESA与污泥中重金属总量的摩尔比为2：1且pH=4的条件下，PESA对污泥中目标重金属的综合萃取效果最好，此时PESA对污泥中各重金属的萃取效率由大到小的顺序为：Cd>Zn>Pb>Ni>Cu>Cr，对应的萃取率分别为78％、73％、72％、60％、54％、36％。(2)重金属与PESA配合物的稳定性、PESA用量、萃取体系pH值、萃取时间、萃取温度、重金属的存在形态等是影响污泥中重金属萃取的重要因素。BCR(European Community Bureau of Reference，简称BCR)连续提取法表明，PESA萃取污泥中的重金属主要是从水溶态、酸溶态、可还原态三种形态中提取，可氧化态可实现部分萃取。(3)H_2O_2对污泥中的Ni、Cu、Zn有较好的分离作用，H_2O_2和PESA复合体系对污泥中Cu的分离有明显的促进作用。(4)低浓度的H_3PO_4对污泥中的重金属Zn、Cd、Ni具有很好的分离作用，H_3PO_4与PESA复合体系对Pb的分离有明显的促进作用。
第三部分：EDDS、EDTA与PESA对重金属分离作用的比较研究
以上海市桃浦污水厂污泥为实验材料，在萃取剂与重金属总量的摩尔比为1：1和10：1以及调节萃取体系pH值的条件下，比较研究了EDDS、EDTA与PESA对重金属的分离作用。实验结果表明：(1)EDTA在实验pH值范围内对多数目标重金属如Cd、Zn、Pb、Cu、Ni具有较好的萃取作用；当EDTA与重金属总量的摩尔比为10：1时，EDTA对污泥中重金属萃取效率由大到小的顺序为Cd>Zn>Pb>Cu>Ni>Cr。(2)EDDS适合在中性偏碱性条件下使用，对Cu、Cd、Zn、Pb、Ni具有较好的萃取作用；当EDDS与重金属总量的摩尔比为10：1时，EDDS对污泥中重金属萃取效率由大到小的顺序为Cu>Cd>Zn>Pb>Ni>Cr。(3)PESA在偏酸性条件下对Cd、zn、Pb、Ni、Cu、Cr具有良好的萃取作用；当PESA与重金属总量的摩尔比为10：1时，PESA对污泥中重金属萃取效率由大到小的顺序为Cd>Zn>Pb>Ni>Cu>Cr。在pH=4且PESA与污泥中重金属总量的摩尔比为10：1时，PESA对Cd、Zn和Pb萃取效率可与EDTA和EDDS相当，对Cr的萃取效率高于EDTA和：EDDS。(4)对Cr的萃取，PESA优于EDTA和EDDS；对Cu的萃取，EDTA和EDDS优于PESA；对Pb的萃取，EDTA优于：EDDS和PESA。(5)相对于EDTA的难生物降解、EDDS含氮有引起水体富营养化的潜在威胁且价格较昂贵，PESA由于具有环境友好、易生物降解、对重金属螯合性能好的优点，是一种很有发展前途的环境友好替代萃取剂。
第四部分：污染土壤中重金属迁移转化规律的研究
以福建三明地区实际受重金属污染的土壤样品为研究对象，通过模拟酸雨淋溶土柱的试验方法，研究了酸雨作用下污染土壤中重金属元素的溶出及迁移转化规律。研究结果表明：(1)随着酸雨pH值的降低，污染土壤淋滤液的电导呈递增变化，而滤液pH值相应降低；随着淋溶量的增加，淋滤液的电导逐渐下降。(2)模拟酸雨作用于该受重金属污染土壤时，污染土壤中不同重金属呈现不同的溶出规律。淋滤液中锌、镍、铜、铬和铅的含量均随模拟酸雨pH值的降低而增加，但锌、镍和铜的释放过程可分为快速释放和准稳定两个阶段，铬和铅的释放过程则分为快速释放和慢速释放两个阶段。(3)相同酸雨强度下，该污染土壤中重金属累积释放量由大到小的顺序为Zn>Cu>Cr>Ni>Pb。(4)不同重金属在酸雨作用下向下层土壤迁移的规律不同。在pH=3．6的酸雨作用下，污染土壤中的Zn、Pb、Cu、Cf、Ni都具有一定的向下层土壤迁移性，Zn、Ni的迁移性较强，而Cu、Pb、Cr的迁移性相对较弱。相同酸雨强度下，污染土壤中各重金属下层土壤的迁移能力由大到小的顺序为Zn>Ni>Cu>Pb>Cr。随着土壤深度的增加，各层土壤中迁移重金属的浓度逐渐降低。同一层土壤中迁移重金属的浓度由大到小的顺序为：Zn>Pb>Cu>Cr>Ni。
The retained heavy metals in sewage sludge will pose the risk of human health and phytotoxicity from land application, which restricts significantly the reuse of sewage sludge. Therefore, how to remove the heavy metals from soil and sewage sludge with the green chemical theory has attracted more attention in recent years. Focussing on the recent development trend of green chemistry and the characteristic for sewage sludge containing higher concentration heavy metal, the extraction efficiencies for poly-epoxy-succinic acid (PESA) as a novel biodegradable chelant to remove heavy metals from sewage aludge based on chemical extraction technology were studied in this paper. The complexation mechanism between PESA and several heavy metal cations were studied by means of acid-base potentionmetric titration. The migration of heavy metals in the actual polluted soil sampled nearby Pb-Zn ore washing plant was investigated based on the condition of soil near ore plant contaminated widely by heavy metals. Under the support of the Natural Science Foundation of China, the purpose of this research is to provide academic suggestion and technical guidance for the development of green remediation technology of soils and sewage sludge contaminated with heavy metals.
This paper consists of four parts: ( I ) Study on the complexation mechanism between PESA and heavy metal cations. (II) Study on the separation of heavy meatls from sewage sludge with PESA. (III) Study on the comparison of extraction efficiency for heavy metals from sewage sludge with EDDS, EDTA and PESA. (IV) Study on the migration of heavy metals in the actual polluted soil.
(I) Study on the complexation mechanism between PESA and heavy metal cations. Based on the acid-base potentionmetric titration and the advanced BEST computer program developed by A. E Martell et al, the deprotonnation constant of PESA and the complex formation constants of PESA with six heavy metal cations (Zn~(2+), Pb~(2+), Cd~(2+), Ni~(2+), Cr~(3+), Cu~(2+)) were determined. The distribution curves of the species in aqueous solution at different pH were also given out. It was demonstrated that the H_2L model with five structure unit to describe the coordination chemistry of PESA, which was set up according to the experimental data, is reasonable and the contants are also accurate. The experimental results confirmed that the models were feasible to match the deprotonation of PESA and the conplexation between PESA and heavy metal cations. The chelation abilities of PESA with heavy metal cations are good. Considering the main complex ML, the order of complexation tendency between heavy metal cations and PESA is Cu~(2+)>Cr~(3+)>Cd~(2+)>Zn~(2+)>Ni~(2+)>Pb~(2+).
(II) Study on the separation of heavy meatls from sewage sludge with PESA. Based on chemical extraction technology, PESA was used to remove the heavy metals from the sewage sludge. For the sewage sludge from Shanghai Taopu Municipal Wastewater Plant, the influence factors including system pH, concentration of PESA, extraction time, extraction temperature, heavy metal species distribution, H_2O_2 and H_3PO_4 addition on the extraction efficiency were investigated. It was found that PESA could extract target heavy metals from sludge effectively. The total extraction efficiency for all of the target heavy metals is good when the molar ratio of PESA to total heavy metals was 2:1 and system pH was 4. The order for heavy metals extracted with PESA is Cd>Zn>Pb>Ni>Cu>Cr, and the extraction efficiency is 78%, 73 %, 12%, 60%, 54% and 36% respectively. The results showed that the complex formation constants of PESA with heavy metal cations, concentration of PESA, system pH, extraction time, extraction temperature, heavy metal species distribution, H_2O_2 and H_3PO_4 addition have a significant effect on the extraction efficiencies. The BCR (European Community Bureau of Reference) analysis of species distribution showed that the extracted heavy metals mainly came from the following species, water soluble, acid soluble, reducible and oxidizable fractions. H_2O_2 addition could remove Ni, Cu and Zn from sludge effectively, and the H_2O_2-PESA associated system could promote the separation of Cu obviously. H_3PO_4 addition could remove Zn, Cd and Ni from sludge effectively, and the H_3PO_4-PESA associated system could promote the separation of Pb apparently.
(III) Study on the comparison of extraction efficiency for heavy metals from sewage sludge with EDDS, EDTA and PESA. Under conditions of molar ratio of chelat and the sum of heavy metals was 1:1 or 10:1 with system pH adjusted, the extraction efficiencies for heavy metal extracted with EDDS, EDTA and PESA were compared. The result revealed that EDTA had higher extraction efficiency for Cd, Zn, Pb, Cu and Ni within experiment pH range, and the order for heavy meatals extracted with EDTA is Cd>Zn>Pb>Cu>Ni>Cr when molar ratio of EDTA and sum of heavy metals was 10:1. EDDS had higher extraction efficiency for Cu, Cd, Zn, Pb and Ni under neutral or alkali condition, and the order for heavy meatals extracted with EDDS is Cu>Cd>Zn>Pb>Ni>Cr when molar ratio of EDDS and sum of heavy metals was 10:1. PESA had higher extraction efficiency for Cd, Zn, Pb, Ni, Cu and Cr under acidic condition, and the order for heavy meatals extracted with PESA is Cd>Zn>Pb>Ni>Cu>Cr when molar ratio of PESA and sum of heavy metals was 10:1. Under conditions of pH=4 and ratio 10:1, PESA gave comparable better extraction efficiency than EDDS and EDTA in extracting Cd, Zn or Pb. PESA gave better performance than EDDS and EDTA for Cr extraction, EDTA and EDDS better than PESA for Cu, and EDTA better than EDDS and PESA for Pb. In comparison with EDTA or EDDS, PESA gave potential alternative performance in extracting heavy metals such as Cd, Zn, Pb or Cr, in addition to the other advantages, such as ready biodegradability and nitrogen- and phophorus-free components.
(IV) Study on the migration of heavy metals in the actual polluted soil. The soil column leaching model was used to study the leaching process and migration of heavy metals with the washing of simulated acid rain. The pH of the simulated acid rain was controlled in three levels of 2.5, 3.6 and 5.6. The investigation revealed that, with the pH decrement of the acid rain, the conductivity of the soil leachate increased gradually while the pH of the leachate decreased under the same conditions. With the pH increment of the acid rain, the total content of all the five heavy metals in the leachate showed the rising tendence. However, the results also showed that different kind of heavy metals had their own leaching characteristics. The release of zinc, nickel and copper from the polluted soil increased rapidly in the first stage and then maintained a relative stable state. For the release process of chromium or lead, it can be divided into two stages of fast leaching and slow leaching. The order of the total released amount of five heavy metals was Zn>Cu> Cr>Ni>Pb under the same condition. The results revealed that Zn, Pb, Cu, Cr or Ni in the polluted soil might migrate to deeper soil when pH of the simulated acid rain was 3.6, and the translation ability for Zn or Ni was greater than Cu, Pb or Cr. Under the same acid rain intensity, the heavy metals migration in soil followed the sequence of Zn>Ni>Cu>Pb>Cr, and the heavy metals content in the same soil depths was in the order of Zn>Pb>Cu>Cr>Ni.
论文主要分为四部分：(Ⅰ)PESA(聚环氧琥珀酸)与典型重金属离子相互作用机理的研究；(Ⅱ)PESA对污泥中重金属的分离过程研究；(Ⅲ)EDDS(S，S-ethylenediaminedisuccinic Acid，乙二胺二琥珀酸)、EDTA(Ethylene DiamineTetraacetic Acid，乙二胺四乙酸)与PESA对重金属分离作用的比较研究；(Ⅳ)污染土壤中重金属迁移转化规律的研究。
第一部分：聚环氧琥珀酸与典型重金属离子相互作用机理的研究
利用pH电位滴定和先进的BEST数据处理程序，研究了PESA与典型重金属离子Zn~(2+)、pb~(2+)、Cd~(2+)、Ni~(2+)、Cr~(3+)、Cu~(2+)之间的配位化学作用，得到了PESA的酸离解常数、相应配合物的稳定常数及不同pH下各种配合物的形态分布图。研究结果表明：(1)将PESA简化为具有五个结构单元的二级电离模型的误差o较小，且模拟滴定曲线与实验滴定曲线的符合程度较好，所得的pK_a1=4．68、pK_a2=4．92，说明实验所设计的配位化学模型比较合理，结果准确。表明通过合理配位化学模型的建立来处理PESA的酸离解及其与重金属离子间的配位化学作用是可行的。(2)从溶液配位化学角度讲，PESA与重金属离子有较强的结合能力。按形成的主要配合物种ML来看，Zn~(2+)、pb~(2+)、Cd~(2+)、Ni~(2+)、Cr~(3+)、Cu~(2+)与PESA配位能力大小的顺序为Cu~(2+)>Cr~(3+)>Cd~(2+)>Zn~(2+)>Ni~(2+)>pb~(2+)。
第二部分：聚环氧琥珀酸对污泥中重金属的分离过程研究
以上海市桃浦污水厂污泥为研究对象，研究了聚环氧琥珀酸对污泥中重金属的萃取作用，重点考察了萃取体系pH值、萃取剂用量、萃取时间、萃取温度、重金属的存在形态、添加H_2O_2、添加H_3PO_4等条件对重金属萃取的影响。研究发现：(1)PESA对污泥中的重金属具有较好的萃取效果，当PESA与污泥中重金属总量的摩尔比为2：1且pH=4的条件下，PESA对污泥中目标重金属的综合萃取效果最好，此时PESA对污泥中各重金属的萃取效率由大到小的顺序为：Cd>Zn>Pb>Ni>Cu>Cr，对应的萃取率分别为78％、73％、72％、60％、54％、36％。(2)重金属与PESA配合物的稳定性、PESA用量、萃取体系pH值、萃取时间、萃取温度、重金属的存在形态等是影响污泥中重金属萃取的重要因素。BCR(European Community Bureau of Reference，简称BCR)连续提取法表明，PESA萃取污泥中的重金属主要是从水溶态、酸溶态、可还原态三种形态中提取，可氧化态可实现部分萃取。(3)H_2O_2对污泥中的Ni、Cu、Zn有较好的分离作用，H_2O_2和PESA复合体系对污泥中Cu的分离有明显的促进作用。(4)低浓度的H_3PO_4对污泥中的重金属Zn、Cd、Ni具有很好的分离作用，H_3PO_4与PESA复合体系对Pb的分离有明显的促进作用。
第三部分：EDDS、EDTA与PESA对重金属分离作用的比较研究
以上海市桃浦污水厂污泥为实验材料，在萃取剂与重金属总量的摩尔比为1：1和10：1以及调节萃取体系pH值的条件下，比较研究了EDDS、EDTA与PESA对重金属的分离作用。实验结果表明：(1)EDTA在实验pH值范围内对多数目标重金属如Cd、Zn、Pb、Cu、Ni具有较好的萃取作用；当EDTA与重金属总量的摩尔比为10：1时，EDTA对污泥中重金属萃取效率由大到小的顺序为Cd>Zn>Pb>Cu>Ni>Cr。(2)EDDS适合在中性偏碱性条件下使用，对Cu、Cd、Zn、Pb、Ni具有较好的萃取作用；当EDDS与重金属总量的摩尔比为10：1时，EDDS对污泥中重金属萃取效率由大到小的顺序为Cu>Cd>Zn>Pb>Ni>Cr。(3)PESA在偏酸性条件下对Cd、zn、Pb、Ni、Cu、Cr具有良好的萃取作用；当PESA与重金属总量的摩尔比为10：1时，PESA对污泥中重金属萃取效率由大到小的顺序为Cd>Zn>Pb>Ni>Cu>Cr。在pH=4且PESA与污泥中重金属总量的摩尔比为10：1时，PESA对Cd、Zn和Pb萃取效率可与EDTA和EDDS相当，对Cr的萃取效率高于EDTA和：EDDS。(4)对Cr的萃取，PESA优于EDTA和EDDS；对Cu的萃取，EDTA和EDDS优于PESA；对Pb的萃取，EDTA优于：EDDS和PESA。(5)相对于EDTA的难生物降解、EDDS含氮有引起水体富营养化的潜在威胁且价格较昂贵，PESA由于具有环境友好、易生物降解、对重金属螯合性能好的优点，是一种很有发展前途的环境友好替代萃取剂。
第四部分：污染土壤中重金属迁移转化规律的研究
以福建三明地区实际受重金属污染的土壤样品为研究对象，通过模拟酸雨淋溶土柱的试验方法，研究了酸雨作用下污染土壤中重金属元素的溶出及迁移转化规律。研究结果表明：(1)随着酸雨pH值的降低，污染土壤淋滤液的电导呈递增变化，而滤液pH值相应降低；随着淋溶量的增加，淋滤液的电导逐渐下降。(2)模拟酸雨作用于该受重金属污染土壤时，污染土壤中不同重金属呈现不同的溶出规律。淋滤液中锌、镍、铜、铬和铅的含量均随模拟酸雨pH值的降低而增加，但锌、镍和铜的释放过程可分为快速释放和准稳定两个阶段，铬和铅的释放过程则分为快速释放和慢速释放两个阶段。(3)相同酸雨强度下，该污染土壤中重金属累积释放量由大到小的顺序为Zn>Cu>Cr>Ni>Pb。(4)不同重金属在酸雨作用下向下层土壤迁移的规律不同。在pH=3．6的酸雨作用下，污染土壤中的Zn、Pb、Cu、Cf、Ni都具有一定的向下层土壤迁移性，Zn、Ni的迁移性较强，而Cu、Pb、Cr的迁移性相对较弱。相同酸雨强度下，污染土壤中各重金属下层土壤的迁移能力由大到小的顺序为Zn>Ni>Cu>Pb>Cr。随着土壤深度的增加，各层土壤中迁移重金属的浓度逐渐降低。同一层土壤中迁移重金属的浓度由大到小的顺序为：Zn>Pb>Cu>Cr>Ni。
The retained heavy metals in sewage sludge will pose the risk of human health and phytotoxicity from land application, which restricts significantly the reuse of sewage sludge. Therefore, how to remove the heavy metals from soil and sewage sludge with the green chemical theory has attracted more attention in recent years. Focussing on the recent development trend of green chemistry and the characteristic for sewage sludge containing higher concentration heavy metal, the extraction efficiencies for poly-epoxy-succinic acid (PESA) as a novel biodegradable chelant to remove heavy metals from sewage aludge based on chemical extraction technology were studied in this paper. The complexation mechanism between PESA and several heavy metal cations were studied by means of acid-base potentionmetric titration. The migration of heavy metals in the actual polluted soil sampled nearby Pb-Zn ore washing plant was investigated based on the condition of soil near ore plant contaminated widely by heavy metals. Under the support of the Natural Science Foundation of China, the purpose of this research is to provide academic suggestion and technical guidance for the development of green remediation technology of soils and sewage sludge contaminated with heavy metals.
This paper consists of four parts: ( I ) Study on the complexation mechanism between PESA and heavy metal cations. (II) Study on the separation of heavy meatls from sewage sludge with PESA. (III) Study on the comparison of extraction efficiency for heavy metals from sewage sludge with EDDS, EDTA and PESA. (IV) Study on the migration of heavy metals in the actual polluted soil.
(I) Study on the complexation mechanism between PESA and heavy metal cations. Based on the acid-base potentionmetric titration and the advanced BEST computer program developed by A. E Martell et al, the deprotonnation constant of PESA and the complex formation constants of PESA with six heavy metal cations (Zn~(2+), Pb~(2+), Cd~(2+), Ni~(2+), Cr~(3+), Cu~(2+)) were determined. The distribution curves of the species in aqueous solution at different pH were also given out. It was demonstrated that the H_2L model with five structure unit to describe the coordination chemistry of PESA, which was set up according to the experimental data, is reasonable and the contants are also accurate. The experimental results confirmed that the models were feasible to match the deprotonation of PESA and the conplexation between PESA and heavy metal cations. The chelation abilities of PESA with heavy metal cations are good. Considering the main complex ML, the order of complexation tendency between heavy metal cations and PESA is Cu~(2+)>Cr~(3+)>Cd~(2+)>Zn~(2+)>Ni~(2+)>Pb~(2+).
(II) Study on the separation of heavy meatls from sewage sludge with PESA. Based on chemical extraction technology, PESA was used to remove the heavy metals from the sewage sludge. For the sewage sludge from Shanghai Taopu Municipal Wastewater Plant, the influence factors including system pH, concentration of PESA, extraction time, extraction temperature, heavy metal species distribution, H_2O_2 and H_3PO_4 addition on the extraction efficiency were investigated. It was found that PESA could extract target heavy metals from sludge effectively. The total extraction efficiency for all of the target heavy metals is good when the molar ratio of PESA to total heavy metals was 2:1 and system pH was 4. The order for heavy metals extracted with PESA is Cd>Zn>Pb>Ni>Cu>Cr, and the extraction efficiency is 78%, 73 %, 12%, 60%, 54% and 36% respectively. The results showed that the complex formation constants of PESA with heavy metal cations, concentration of PESA, system pH, extraction time, extraction temperature, heavy metal species distribution, H_2O_2 and H_3PO_4 addition have a significant effect on the extraction efficiencies. The BCR (European Community Bureau of Reference) analysis of species distribution showed that the extracted heavy metals mainly came from the following species, water soluble, acid soluble, reducible and oxidizable fractions. H_2O_2 addition could remove Ni, Cu and Zn from sludge effectively, and the H_2O_2-PESA associated system could promote the separation of Cu obviously. H_3PO_4 addition could remove Zn, Cd and Ni from sludge effectively, and the H_3PO_4-PESA associated system could promote the separation of Pb apparently.
(III) Study on the comparison of extraction efficiency for heavy metals from sewage sludge with EDDS, EDTA and PESA. Under conditions of molar ratio of chelat and the sum of heavy metals was 1:1 or 10:1 with system pH adjusted, the extraction efficiencies for heavy metal extracted with EDDS, EDTA and PESA were compared. The result revealed that EDTA had higher extraction efficiency for Cd, Zn, Pb, Cu and Ni within experiment pH range, and the order for heavy meatals extracted with EDTA is Cd>Zn>Pb>Cu>Ni>Cr when molar ratio of EDTA and sum of heavy metals was 10:1. EDDS had higher extraction efficiency for Cu, Cd, Zn, Pb and Ni under neutral or alkali condition, and the order for heavy meatals extracted with EDDS is Cu>Cd>Zn>Pb>Ni>Cr when molar ratio of EDDS and sum of heavy metals was 10:1. PESA had higher extraction efficiency for Cd, Zn, Pb, Ni, Cu and Cr under acidic condition, and the order for heavy meatals extracted with PESA is Cd>Zn>Pb>Ni>Cu>Cr when molar ratio of PESA and sum of heavy metals was 10:1. Under conditions of pH=4 and ratio 10:1, PESA gave comparable better extraction efficiency than EDDS and EDTA in extracting Cd, Zn or Pb. PESA gave better performance than EDDS and EDTA for Cr extraction, EDTA and EDDS better than PESA for Cu, and EDTA better than EDDS and PESA for Pb. In comparison with EDTA or EDDS, PESA gave potential alternative performance in extracting heavy metals such as Cd, Zn, Pb or Cr, in addition to the other advantages, such as ready biodegradability and nitrogen- and phophorus-free components.
(IV) Study on the migration of heavy metals in the actual polluted soil. The soil column leaching model was used to study the leaching process and migration of heavy metals with the washing of simulated acid rain. The pH of the simulated acid rain was controlled in three levels of 2.5, 3.6 and 5.6. The investigation revealed that, with the pH decrement of the acid rain, the conductivity of the soil leachate increased gradually while the pH of the leachate decreased under the same conditions. With the pH increment of the acid rain, the total content of all the five heavy metals in the leachate showed the rising tendence. However, the results also showed that different kind of heavy metals had their own leaching characteristics. The release of zinc, nickel and copper from the polluted soil increased rapidly in the first stage and then maintained a relative stable state. For the release process of chromium or lead, it can be divided into two stages of fast leaching and slow leaching. The order of the total released amount of five heavy metals was Zn>Cu> Cr>Ni>Pb under the same condition. The results revealed that Zn, Pb, Cu, Cr or Ni in the polluted soil might migrate to deeper soil when pH of the simulated acid rain was 3.6, and the translation ability for Zn or Ni was greater than Cu, Pb or Cr. Under the same acid rain intensity, the heavy metals migration in soil followed the sequence of Zn>Ni>Cu>Pb>Cr, and the heavy metals content in the same soil depths was in the order of Zn>Pb>Cu>Cr>Ni.
引文
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