剩余污泥中重金属污染的蚯蚓活化—花卉植物修复机理研究
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摘要
随着我国经济发展和城市化进程的加快,城市剩余污泥的产量急剧增加,其科学化处置问题已备受国内外环境学者的关注。在对剩余污泥的各类处置方法中,土地利用是最有潜力的污泥处置方式,但是重金属却成为主要限制因子。针对重金属污染问题,植物修复技术因其低成本、绿色环保而迅速发展起来,但该技术的研究目前主要侧重于重金属污染的土壤。
污泥与土壤介质不同,采用植物修复剩余污泥中重金属的机理和效果需要通过实验来进行研究和验证。为此,本论文以四个不同规模和类型的污水处理厂剩余污泥为研究对象,先后进行了剩余污泥中重金属含量形态测试与分析实验、污泥中重金属污染修复的花卉植物筛选实验和蚯蚓对污泥重金属的活化实验,并在此基础上提出了赤子爱胜蚓-吊兰联合修复技术,其研究结果对剩余污泥中重金属污染修复具有重要的理论意义和潜在的应用价值,并为污泥无害化处置提供新途径。主要研究结论如下:
(1)重金属含量分析结果表明,同种重金属在四个不同类型污水处理厂污泥中的含量不同,徐州市荆马河污水处理厂的Cu、Zn、Pb含量最高(其值分别为2013.48mg/kg、4862.18mg/kg、541.79mg/kg),徐州市姚庄污水处理厂的Cd含量最高(其值为25.42 mg/kg),淮北市污水处理厂的Cr含量最高(其值为462.19mg/kg);重金属Cu、Zn、P b、Cd不同程度超过城镇污水处理厂污染物排放标准(GB18918-2002)。
(2)重金属形态分析结果表明,四个污水处理厂污泥中各类重金属主要以稳定态(硫化物结合态、残渣态)形式存在。重金属Zn以碳酸盐态(范围为20.26%～27.11%)和残渣态(范围为45.08%～61.70%55)为主,重金属Cu、Pb、Cr以硫化物结合态(范围分别为51.79%～60.87%、23.12%～31.45%、61.28%～78.36%)和残渣态(范围分别为27.43%～34.62%、.68%～63.50%、21.64%～38.72%)为主,重金属Cd以硫化物结合态(范围为38.45%～51.60%)和铁锰氧化物结合态(范围为15.69%～30.20%)为主。
(3)花卉植物筛选实验结果表明,吊兰生长旺盛,未表现出任何受毒害症状,并对重金属Cu、Zn、Cd、Pb具有一定的积累能力,是适合联合修复污泥中重金属的花卉植物。实验期内,吊兰在全泥处理(3:0、2:0)中对Cu、Zn、Cd、Pb的总积累量均为最大,其值分别为5.70mg plant ~(-1)、14.53mg plant ~(-1)、0.340mg plant ~(-1)和0.580mg plant ~(-1)。
(4)蚯蚓活化实验结果表明,赤子爱胜蚓能够在一定配比浓度的Cu、Zn、Pb、Cd污泥中正常生长,改变污泥的理化性质,并提高污泥中重金属的生物有效性。蚯蚓活动使得Cu配比浓度为150 mg/kg、Zn配比浓度为200 mg/kg和Pb配比浓度为400 mg/kg污泥中重金属的活化率增加值最大,对Cd不同配比浓度污泥中重金属的活化率影响不大。
(5)蚯蚓-花卉联合修复实验结果表明,赤子爱胜蚓能够改变污泥理化性质,促进吊兰生长,增强吊兰吸收污泥中重金属的能力。在Cu不同配比浓度污泥中,吊兰总积累量分别增加了0.99 mg plant ~(-1)、4.69 mg plant ~(-1)、1.62 mg plant ~(-1)和8.03 mg plant ~(-1);在Zn不同配比浓度污泥中,吊兰总积累量分别增加了2.74mg plant ~(-1)、2.29mg plant ~(-1)、3.47mg plant ~(-1)和1.26mg plant ~(-1);在Pb不同配比浓度污泥中,吊兰总积累量分别增加了4.81mg plant ~(-1)、1 .13mg plant ~(-1)、3 .71mg plant ~(-1)和0.45mg plant ~(-1)。接种赤子爱胜蚓后,均不同程度提高了吊兰茎叶部和根部的富集系数和转运系数,其中当Cu配比浓度为50mg/kg和100mg/kg、Pb配比浓度为0mg/kg时,根部的富集系数大于1。
该论文有图73幅,表46个,参考文献215篇。
With the development of economy and urbanization in China, the amount of municipal sludge increased dramatically. How to scientifically deal with the municipal sludge has been concerned widely by environmentalist at home and abroad. Among most of the residual sludge treatment methods, land utilization is one of the most potential methods. But the heavy metal is a main factor limiting its effectiveness. For the heavy metal pollution, the phytoremediation technology has been developed rapidly for its low cost and good environmental effect, but the study about this technology is now focused primarily on the soil contaminated by heavy metal.
For the different characters of sludge compared with those of the soil, the mechanism and effect that plants remedy heavy metal of the residual sludge need to be explored and validated by experiments. This thesis has taken the residual sludge from four different scale and type sewage plants as research objects, conducted the analysis and experiment of heavy metal contents and speciation in the residual sludge, and carried out screening test of the heavy metal pollution remediation by ornamental plants in the residual sludge and the activation of the earthworm in the residual sludge polluted with the heavy metal. Based on the analysis the thesis has put forward the eisenia foelide and Chlorophytum comosum combined remediation technique for the heavy metal in the residual sludge. The research had important theoretical meaning and potential application value for the heavy metal remediation of the residual sludge and would provided a new way for the sludge detoxification. The main conclusions of the thesis include:
(1)The analysis of heavy metal content shows that: the contents of heavy metals in the sludge from four different types of sewage plants are different. The Jingmahe sewage plant in Xuzhou city has the highest contents of Cu, Zn and Pb (the values are 2013.48mg/kg, 4862.18mg/kg and 541.79mg/kg).The Yaozhuang sewage plant in Xuzhou city has the highest content of Cd (the value is 25.42 mg/kg). The Huaibei sewage treatment plant has the highest content of Cr (the value is 462.19 mg/kg). Meanwhile, the contents of Cu, Zn, Pb and Cd in the sludge from all plants exceed prescribed discharge standards of Discharge standard of pollutants for municipal wastewater treatment plant (GB18918-2002).
(2)The analysis of the heavy metal speciation in the residual sludge shows that: all kinds of heavy metal in the sludge from four sewage plants mainly exist in stable states (sulfide-bound state, residual form). The most speciation of Zn are carbonate state(from 20.26% to 27.11%) and residual form (from 45.08% to 61.70%).Cu, Pb, Cr mainly exist with the speciation of sulfide-bound state(the proportions of 51.79%～60.87%, 23.12%～31.45% and 61.28%～78.36% respectively) and residual form(the proportions of 27.43%～34.62%, 55.68%～63.50% and 21.64%～38.72%).Most of the Cd exists in sulfide-bound state(the proportion of 38.45%～51.60%) and Fe-Mn-bound state(the proportion of 15.69%～30.20%).
(3)The screening test of ornamental plants shows that: For its vigorous growth Chlorophytum comosum has the ability to accumulate the heavy metal of Cu, Zn, Cd and Pb to some extent without the symptom of being poisoned, thus it is suitable for the combined remediation of the heavy metal pollution. In the period of experiments, the Chlorophytum comosum has the largest total accumulation amount of the heavy metal of Cu, Zn, Cd and Pb which is 5.70mg plant ~(-1)、14.53mg plant ~(-1) 0.340mg plant ~(-1)和0.580mg plant ~(-1) respectively with the sludge treatment(3:0,2:0).
(4)The activiation experiments of the earthworm show that: The earthworm Eisenia fetida Andrei can grow normally in the sludge added with certain proportion concentraition of Cu, Zn, Pb and Cd. This kind of earthworm can change the physical and chemical character of the sludge and improve the bioavailability of the heavy metal in the sludge. The bioavailability of the heavy metal will be most improved by the acitivity of the earthworm when the proportion concentration of Cu is 150 mg/kg and that of Zn is 200 mg/kg and that of Pb is 400 mg/kg.
(5)The combined remediation experiments by the earthworm and the ornamental plants show that: The earthworm Eisenia fetida Andrei can change the physical and chemical character of sludge, accelerate the growth of the Chlorophytum comosum and enhance the absorption of the heavy metal in the sludge. For the sludge with different Cu proportion concentration, the total accumulation amount by the Chlorophytum comosum has increased 0.99 mg plant ~(-1), 4.69 mg plant ~(-1), 1.62 mg plant ~(-1) and 8.03 mg plant ~(-1) respectively. For the sludge with different Pb proportion concentration, the total accumulation amount by the Chlorophytum comosum has increased 4.81mg plant ~(-1), 1.13mg plant ~(-1), 3.707mg plant ~(-1) and 0.45mg plant ~(-1) respectively. The earthworm Eisenia fetida Andrei has raised the enrichment coefficient and the transfer coefficient of the stem and leaf and the root of the Chlorophytum comosum. The enrichment coefficient of the root of the Chlorophytum comosum is larger than 1 when the proportion concentration of Cu is 50mg/kg or100mg/kg and the proportion concentration of Pb is 0mg/kg.
There are 73 figures, 46 tables and 215 references in the thesis.
污泥与土壤介质不同,采用植物修复剩余污泥中重金属的机理和效果需要通过实验来进行研究和验证。为此,本论文以四个不同规模和类型的污水处理厂剩余污泥为研究对象,先后进行了剩余污泥中重金属含量形态测试与分析实验、污泥中重金属污染修复的花卉植物筛选实验和蚯蚓对污泥重金属的活化实验,并在此基础上提出了赤子爱胜蚓-吊兰联合修复技术,其研究结果对剩余污泥中重金属污染修复具有重要的理论意义和潜在的应用价值,并为污泥无害化处置提供新途径。主要研究结论如下:
(1)重金属含量分析结果表明,同种重金属在四个不同类型污水处理厂污泥中的含量不同,徐州市荆马河污水处理厂的Cu、Zn、Pb含量最高(其值分别为2013.48mg/kg、4862.18mg/kg、541.79mg/kg),徐州市姚庄污水处理厂的Cd含量最高(其值为25.42 mg/kg),淮北市污水处理厂的Cr含量最高(其值为462.19mg/kg);重金属Cu、Zn、P b、Cd不同程度超过城镇污水处理厂污染物排放标准(GB18918-2002)。
(2)重金属形态分析结果表明,四个污水处理厂污泥中各类重金属主要以稳定态(硫化物结合态、残渣态)形式存在。重金属Zn以碳酸盐态(范围为20.26%～27.11%)和残渣态(范围为45.08%～61.70%55)为主,重金属Cu、Pb、Cr以硫化物结合态(范围分别为51.79%～60.87%、23.12%～31.45%、61.28%～78.36%)和残渣态(范围分别为27.43%～34.62%、.68%～63.50%、21.64%～38.72%)为主,重金属Cd以硫化物结合态(范围为38.45%～51.60%)和铁锰氧化物结合态(范围为15.69%～30.20%)为主。
(3)花卉植物筛选实验结果表明,吊兰生长旺盛,未表现出任何受毒害症状,并对重金属Cu、Zn、Cd、Pb具有一定的积累能力,是适合联合修复污泥中重金属的花卉植物。实验期内,吊兰在全泥处理(3:0、2:0)中对Cu、Zn、Cd、Pb的总积累量均为最大,其值分别为5.70mg plant ~(-1)、14.53mg plant ~(-1)、0.340mg plant ~(-1)和0.580mg plant ~(-1)。
(4)蚯蚓活化实验结果表明,赤子爱胜蚓能够在一定配比浓度的Cu、Zn、Pb、Cd污泥中正常生长,改变污泥的理化性质,并提高污泥中重金属的生物有效性。蚯蚓活动使得Cu配比浓度为150 mg/kg、Zn配比浓度为200 mg/kg和Pb配比浓度为400 mg/kg污泥中重金属的活化率增加值最大,对Cd不同配比浓度污泥中重金属的活化率影响不大。
(5)蚯蚓-花卉联合修复实验结果表明,赤子爱胜蚓能够改变污泥理化性质,促进吊兰生长,增强吊兰吸收污泥中重金属的能力。在Cu不同配比浓度污泥中,吊兰总积累量分别增加了0.99 mg plant ~(-1)、4.69 mg plant ~(-1)、1.62 mg plant ~(-1)和8.03 mg plant ~(-1);在Zn不同配比浓度污泥中,吊兰总积累量分别增加了2.74mg plant ~(-1)、2.29mg plant ~(-1)、3.47mg plant ~(-1)和1.26mg plant ~(-1);在Pb不同配比浓度污泥中,吊兰总积累量分别增加了4.81mg plant ~(-1)、1 .13mg plant ~(-1)、3 .71mg plant ~(-1)和0.45mg plant ~(-1)。接种赤子爱胜蚓后,均不同程度提高了吊兰茎叶部和根部的富集系数和转运系数,其中当Cu配比浓度为50mg/kg和100mg/kg、Pb配比浓度为0mg/kg时,根部的富集系数大于1。
该论文有图73幅,表46个,参考文献215篇。
With the development of economy and urbanization in China, the amount of municipal sludge increased dramatically. How to scientifically deal with the municipal sludge has been concerned widely by environmentalist at home and abroad. Among most of the residual sludge treatment methods, land utilization is one of the most potential methods. But the heavy metal is a main factor limiting its effectiveness. For the heavy metal pollution, the phytoremediation technology has been developed rapidly for its low cost and good environmental effect, but the study about this technology is now focused primarily on the soil contaminated by heavy metal.
For the different characters of sludge compared with those of the soil, the mechanism and effect that plants remedy heavy metal of the residual sludge need to be explored and validated by experiments. This thesis has taken the residual sludge from four different scale and type sewage plants as research objects, conducted the analysis and experiment of heavy metal contents and speciation in the residual sludge, and carried out screening test of the heavy metal pollution remediation by ornamental plants in the residual sludge and the activation of the earthworm in the residual sludge polluted with the heavy metal. Based on the analysis the thesis has put forward the eisenia foelide and Chlorophytum comosum combined remediation technique for the heavy metal in the residual sludge. The research had important theoretical meaning and potential application value for the heavy metal remediation of the residual sludge and would provided a new way for the sludge detoxification. The main conclusions of the thesis include:
(1)The analysis of heavy metal content shows that: the contents of heavy metals in the sludge from four different types of sewage plants are different. The Jingmahe sewage plant in Xuzhou city has the highest contents of Cu, Zn and Pb (the values are 2013.48mg/kg, 4862.18mg/kg and 541.79mg/kg).The Yaozhuang sewage plant in Xuzhou city has the highest content of Cd (the value is 25.42 mg/kg). The Huaibei sewage treatment plant has the highest content of Cr (the value is 462.19 mg/kg). Meanwhile, the contents of Cu, Zn, Pb and Cd in the sludge from all plants exceed prescribed discharge standards of Discharge standard of pollutants for municipal wastewater treatment plant (GB18918-2002).
(2)The analysis of the heavy metal speciation in the residual sludge shows that: all kinds of heavy metal in the sludge from four sewage plants mainly exist in stable states (sulfide-bound state, residual form). The most speciation of Zn are carbonate state(from 20.26% to 27.11%) and residual form (from 45.08% to 61.70%).Cu, Pb, Cr mainly exist with the speciation of sulfide-bound state(the proportions of 51.79%～60.87%, 23.12%～31.45% and 61.28%～78.36% respectively) and residual form(the proportions of 27.43%～34.62%, 55.68%～63.50% and 21.64%～38.72%).Most of the Cd exists in sulfide-bound state(the proportion of 38.45%～51.60%) and Fe-Mn-bound state(the proportion of 15.69%～30.20%).
(3)The screening test of ornamental plants shows that: For its vigorous growth Chlorophytum comosum has the ability to accumulate the heavy metal of Cu, Zn, Cd and Pb to some extent without the symptom of being poisoned, thus it is suitable for the combined remediation of the heavy metal pollution. In the period of experiments, the Chlorophytum comosum has the largest total accumulation amount of the heavy metal of Cu, Zn, Cd and Pb which is 5.70mg plant ~(-1)、14.53mg plant ~(-1) 0.340mg plant ~(-1)和0.580mg plant ~(-1) respectively with the sludge treatment(3:0,2:0).
(4)The activiation experiments of the earthworm show that: The earthworm Eisenia fetida Andrei can grow normally in the sludge added with certain proportion concentraition of Cu, Zn, Pb and Cd. This kind of earthworm can change the physical and chemical character of the sludge and improve the bioavailability of the heavy metal in the sludge. The bioavailability of the heavy metal will be most improved by the acitivity of the earthworm when the proportion concentration of Cu is 150 mg/kg and that of Zn is 200 mg/kg and that of Pb is 400 mg/kg.
(5)The combined remediation experiments by the earthworm and the ornamental plants show that: The earthworm Eisenia fetida Andrei can change the physical and chemical character of sludge, accelerate the growth of the Chlorophytum comosum and enhance the absorption of the heavy metal in the sludge. For the sludge with different Cu proportion concentration, the total accumulation amount by the Chlorophytum comosum has increased 0.99 mg plant ~(-1), 4.69 mg plant ~(-1), 1.62 mg plant ~(-1) and 8.03 mg plant ~(-1) respectively. For the sludge with different Pb proportion concentration, the total accumulation amount by the Chlorophytum comosum has increased 4.81mg plant ~(-1), 1.13mg plant ~(-1), 3.707mg plant ~(-1) and 0.45mg plant ~(-1) respectively. The earthworm Eisenia fetida Andrei has raised the enrichment coefficient and the transfer coefficient of the stem and leaf and the root of the Chlorophytum comosum. The enrichment coefficient of the root of the Chlorophytum comosum is larger than 1 when the proportion concentration of Cu is 50mg/kg or100mg/kg and the proportion concentration of Pb is 0mg/kg.
There are 73 figures, 46 tables and 215 references in the thesis.
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