固废拆解地区农田土壤多氯联苯污染调查与生物修复研究
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摘要
电子电器固体废弃物的粗放拆解导致我国东南部分地区土壤等环境受到重金属、持久性有机物的严重污染。采用生物修复技术对有机污染土壤进行治理是当前研究的热点,但是目前国内外生物修复技术的野外应用研究还很缺乏。本论文选取东南沿海某典型固废拆解地区为研究对象,在土壤污染调查与风险评价基础上,对主要污染物多氯联苯(Polychlorinated biphenyls, PCBs)进行自然消减和生物修复研究,并选取实际PCBs污染农田(4800m2)进行野外中试生物修复实验。取得的主要研究结果与结论如下：
(1)针对典型固废拆解区域农田土壤进行了重金属和有机物污染调查和评价。拆解密集的A、B两镇农田土壤均受到重金属、有机物的严重污染,主要污染物为Cd、Cu、PAHs和PCBs等,其中PCBs浓度分别为27.1-415.1μg/kg和13.3-242.2μg/kg。小型拆解作坊由于采用露天粗放拆解方式,比大型拆解工厂对周边农田土壤污染贡献更大。土壤中重金属Cu、Pb与有机物PAHs、PCBs含量之间相关性显著,表明这些污染物可能具有相似的来源。
(2)筛选典型农田进行详细调查和风险评价,确定了农田土壤修复目标值,建立了土壤污染空间推估方法,为PCBs污染土壤的分区修复提供依据。筛选获得固废拆解地区6处典型农田进行详细重金属和有机物污染调查与评价。对其中重度PCBs污染农田地块(4800m2)进行健康风险评价,结果表明该地块作为农用地具有较高的健康风险,必须采取修复措施。采用健康风险评价方法反推得到该地块PCBs污染修复目标值为90.0pg/kg。建立了以CFBP类神经网络为分析手段的土壤污染空间推估方法,并利用该体系对拟修复农田进行了污染空间模拟,结果优于常用地统计Kriging模拟方法。
(3)野外调查结果表明,当地水田中PCBs残留量显著低于旱地,且水田中高氯代PCBs残留比例较低。不同水分处理土壤中PCBs消减规律研究表明,相对于落干或淹水处理,干湿交替处理条件下土壤中PCBs的去除效果最好,且高氯代PCBs组分可被降解。以上研究结果表明水田土壤厌氧-好氧环境对PCBs自然消减具有促进作用。
(4)针对较高浓度PCBs污染土壤进行了实验室和野外生物堆制修复研究。以实际PCBs污染土壤(2.9-3.1mg/kg)为对象进行17-24天的堆制处理,结果表明不控温自然堆制较控温处理好,添加大豆卵磷脂等可使土壤中PCBs去除率达到20%。以添加PCBs污染土壤(224.4-310.8mg/kg)分别进行自然堆制和强制通风堆制实验,添加大豆卵磷脂、蚯蚓或PCBs降解菌等,堆制97天后土壤中PCBs去除率最高可分别达到57.1%和73.5%,其中低氯代PCBs组分的去除效果较高氯代组分更好。厌氧堆制后土壤中PCBs总浓度未显著降低,但高氯代组分转化为低氯代组分。基于实验室堆制研究,提出厌氧-好氧堆制工艺并设计制造了DANO滚筒堆制修复设备(处理能力15m3/台)。对实际污染农田实施了野外DANO堆制修复,结果表明,初始平均浓度为187μg/kg的污染土壤修复90天后PCBs下降16.1%。
(5)针对中低浓度PCBs污染土壤开展了实验室和野外植物修复研究。温室盆栽实验结果表明,黑麦草结合β-环糊精进行植物修复对受PCBs长期污染的农田土壤是一种有效的修复手段：初始浓度为4.52mg/kg的污染土壤,修复4个月PCBs去除率可达38%。β-环糊精的加入提高了土壤中PCBs的生物可利用性和土壤中微生物活性,从而加速了土壤中PCBs的微生物降解。植物体内的PCBs总量约是总PCBs去除量的0.08%,表明土壤中PCBs的主要去除途径不是植物吸收而是根际微生物降解。对实际污染农田进行了植物修复中试研究,初始浓度为102的污染土壤修复110天后,PCBs下降7.9%。
The crude and unregulated recycling activities of electronic and electric waste have resulted in severe and complex contamination of the surrounding environment by toxic chemicals such as heavy metals as well as persistent organic compounds. Bioremediation is an emerging effective and environmentally friendly mean of remediation for the organic compounds polluted soil. However, most of current bioremediation research works in China were conducted in laboratory. There are few bioremediation cases for the real contaminated soil. Taking a typical e-waste recycling area in Southeast China as an example, we had finished a systematic investigation of heavy metals and organic pollution in agricultural soil. Furthermore, some laboratory studies were carried out to investigate the feasibility of different bioremediation technologies for polychlorinated biphenyls (PCBs). A field study in a PCBs contaminated farmland (4800m2) was also conducted. The main results were summarized as follows.
A systematic investigation of heavy metals and organic pollution in agricultural soil was conducted. The results indicated that the e-waste recycling activity had caused critical soil pollution for Town A and B in e-waste recycling area. Cd, Cu, PAHs and PCBs were the main contaminants. The concentration of PCBs was27.1-415.1μg/kg and13.3-242.2μg/kg in soil of Town A and B, respectively. Comparison among the different sampling areas indicated that the soil was highly contaminated in the agricultural area near e-waste recycling workshops. There was significant correlation among Cu, Pb, PAHs, and PCBs, indicating that these contaminants might have a common source.
Soil investigation and risk assessment was conducted in typical farmlands in e-waste rccyling area. Furthermore, the remediation target concentration was discussed and the spatial distribution estimation method was established. Six typical polluted farmlands were selected for further heavy metals and organic pollution investigation. Through the health risk assessment, the typical PCBs polluted farmland (4800m2) was observed that had a high level of health risk and was suggested to be remediated immediately. The remediation target concentration was suggested to be90μg/kg for agricultural soil. The spatial distribution estimation of soil pollution data was conducted by the back-propagation neural network analysis. The estimated result was more reasonable than the result estimated by the traditional Kriging analysis.
After the investigation and analysis of the field samples in the e-waste recycling area, we found that the residues of PCBs in paddy soil were significantly lower than those from dry land. Then the natural attenuation of PCB congener31or congener mixtures was studied in aged contaminated soil or spiked soil with alternative wet-dry, flooded or dry condition, respectively. It was found that PCBs degradation was more enhanced in the alternative wet-dry treatments as compared to other two treatments. Highly chlorinated PCBs could also be degraded in the alternative wet-dry conditions. The results suggested that the typical anaerobic-aerobic environment in the farmland could enhance the natural attenuation of PCBs.
Several composting studies were investigated for the higher concentration of PCBs. With the addition of auxiliary components such as soybean phosphatide, composting without temperature control could remove approximately20percent of PCBs from the real contaminated soil (2.9-3.1mg/kg) within17-24days. After adding earthworms or microorganisms, the removal efficiency increased to about57.1percent after97days of composting for the spiked PCBs soil (224.4-310.8mg/kg). The removal efficiency was increased to nearly70percent when taking some intensive measures such as forced draft ventilation, the addition of soybean phosphatide, earthworms and microorganisms. However, the removal of highly chlorinated PCBs was limited. The concentration of PCBs in the soil was not significantly affected during the anaerobic composting process while the percentage of highly chlorinated PCBs decreased and lower chlorinated congeners increased. On the basis of laboratory-based composting experiments, an anaerobic-aerobic composting technique was presented and a DANO drum composting equipment was designed. Finally, a field composting study was conducted. Results showed that PCBs was removed by16.1percent during the90days of composting treatment, the initial concentration was187μg/kg.
For the lower concentration of PCBs, a phytoremediation study was conducted both in greenhouse and field. Greenhouse pot experiment results showed that the combination phytoremedaiton using ryegrass and β-cyclodextrin was an effective means for the PCBs-contaminated agricultural soils. After120days of plant growth, the highest PCB removal percentage (about38%) was observed in the ryegrass planted soil, the initial concentration of which was4.52mg/kg. Addition ofβ-cyclodextrin increased the PCBs bioavailability as well as the biological activities, which might lead to the enhanced degradation of PCBs. Plant uptake contributed about0.08percent of PCBs loss, suggesting that plant uptake was not the main pathway for the PCBs removal in the soil. Furthermore, the phytoremediation efficiency of PCBs was studied in field for110days. Results showed that PCBs could be removed by7.9percent.
(1)针对典型固废拆解区域农田土壤进行了重金属和有机物污染调查和评价。拆解密集的A、B两镇农田土壤均受到重金属、有机物的严重污染,主要污染物为Cd、Cu、PAHs和PCBs等,其中PCBs浓度分别为27.1-415.1μg/kg和13.3-242.2μg/kg。小型拆解作坊由于采用露天粗放拆解方式,比大型拆解工厂对周边农田土壤污染贡献更大。土壤中重金属Cu、Pb与有机物PAHs、PCBs含量之间相关性显著,表明这些污染物可能具有相似的来源。
(2)筛选典型农田进行详细调查和风险评价,确定了农田土壤修复目标值,建立了土壤污染空间推估方法,为PCBs污染土壤的分区修复提供依据。筛选获得固废拆解地区6处典型农田进行详细重金属和有机物污染调查与评价。对其中重度PCBs污染农田地块(4800m2)进行健康风险评价,结果表明该地块作为农用地具有较高的健康风险,必须采取修复措施。采用健康风险评价方法反推得到该地块PCBs污染修复目标值为90.0pg/kg。建立了以CFBP类神经网络为分析手段的土壤污染空间推估方法,并利用该体系对拟修复农田进行了污染空间模拟,结果优于常用地统计Kriging模拟方法。
(3)野外调查结果表明,当地水田中PCBs残留量显著低于旱地,且水田中高氯代PCBs残留比例较低。不同水分处理土壤中PCBs消减规律研究表明,相对于落干或淹水处理,干湿交替处理条件下土壤中PCBs的去除效果最好,且高氯代PCBs组分可被降解。以上研究结果表明水田土壤厌氧-好氧环境对PCBs自然消减具有促进作用。
(4)针对较高浓度PCBs污染土壤进行了实验室和野外生物堆制修复研究。以实际PCBs污染土壤(2.9-3.1mg/kg)为对象进行17-24天的堆制处理,结果表明不控温自然堆制较控温处理好,添加大豆卵磷脂等可使土壤中PCBs去除率达到20%。以添加PCBs污染土壤(224.4-310.8mg/kg)分别进行自然堆制和强制通风堆制实验,添加大豆卵磷脂、蚯蚓或PCBs降解菌等,堆制97天后土壤中PCBs去除率最高可分别达到57.1%和73.5%,其中低氯代PCBs组分的去除效果较高氯代组分更好。厌氧堆制后土壤中PCBs总浓度未显著降低,但高氯代组分转化为低氯代组分。基于实验室堆制研究,提出厌氧-好氧堆制工艺并设计制造了DANO滚筒堆制修复设备(处理能力15m3/台)。对实际污染农田实施了野外DANO堆制修复,结果表明,初始平均浓度为187μg/kg的污染土壤修复90天后PCBs下降16.1%。
(5)针对中低浓度PCBs污染土壤开展了实验室和野外植物修复研究。温室盆栽实验结果表明,黑麦草结合β-环糊精进行植物修复对受PCBs长期污染的农田土壤是一种有效的修复手段：初始浓度为4.52mg/kg的污染土壤,修复4个月PCBs去除率可达38%。β-环糊精的加入提高了土壤中PCBs的生物可利用性和土壤中微生物活性,从而加速了土壤中PCBs的微生物降解。植物体内的PCBs总量约是总PCBs去除量的0.08%,表明土壤中PCBs的主要去除途径不是植物吸收而是根际微生物降解。对实际污染农田进行了植物修复中试研究,初始浓度为102的污染土壤修复110天后,PCBs下降7.9%。
The crude and unregulated recycling activities of electronic and electric waste have resulted in severe and complex contamination of the surrounding environment by toxic chemicals such as heavy metals as well as persistent organic compounds. Bioremediation is an emerging effective and environmentally friendly mean of remediation for the organic compounds polluted soil. However, most of current bioremediation research works in China were conducted in laboratory. There are few bioremediation cases for the real contaminated soil. Taking a typical e-waste recycling area in Southeast China as an example, we had finished a systematic investigation of heavy metals and organic pollution in agricultural soil. Furthermore, some laboratory studies were carried out to investigate the feasibility of different bioremediation technologies for polychlorinated biphenyls (PCBs). A field study in a PCBs contaminated farmland (4800m2) was also conducted. The main results were summarized as follows.
A systematic investigation of heavy metals and organic pollution in agricultural soil was conducted. The results indicated that the e-waste recycling activity had caused critical soil pollution for Town A and B in e-waste recycling area. Cd, Cu, PAHs and PCBs were the main contaminants. The concentration of PCBs was27.1-415.1μg/kg and13.3-242.2μg/kg in soil of Town A and B, respectively. Comparison among the different sampling areas indicated that the soil was highly contaminated in the agricultural area near e-waste recycling workshops. There was significant correlation among Cu, Pb, PAHs, and PCBs, indicating that these contaminants might have a common source.
Soil investigation and risk assessment was conducted in typical farmlands in e-waste rccyling area. Furthermore, the remediation target concentration was discussed and the spatial distribution estimation method was established. Six typical polluted farmlands were selected for further heavy metals and organic pollution investigation. Through the health risk assessment, the typical PCBs polluted farmland (4800m2) was observed that had a high level of health risk and was suggested to be remediated immediately. The remediation target concentration was suggested to be90μg/kg for agricultural soil. The spatial distribution estimation of soil pollution data was conducted by the back-propagation neural network analysis. The estimated result was more reasonable than the result estimated by the traditional Kriging analysis.
After the investigation and analysis of the field samples in the e-waste recycling area, we found that the residues of PCBs in paddy soil were significantly lower than those from dry land. Then the natural attenuation of PCB congener31or congener mixtures was studied in aged contaminated soil or spiked soil with alternative wet-dry, flooded or dry condition, respectively. It was found that PCBs degradation was more enhanced in the alternative wet-dry treatments as compared to other two treatments. Highly chlorinated PCBs could also be degraded in the alternative wet-dry conditions. The results suggested that the typical anaerobic-aerobic environment in the farmland could enhance the natural attenuation of PCBs.
Several composting studies were investigated for the higher concentration of PCBs. With the addition of auxiliary components such as soybean phosphatide, composting without temperature control could remove approximately20percent of PCBs from the real contaminated soil (2.9-3.1mg/kg) within17-24days. After adding earthworms or microorganisms, the removal efficiency increased to about57.1percent after97days of composting for the spiked PCBs soil (224.4-310.8mg/kg). The removal efficiency was increased to nearly70percent when taking some intensive measures such as forced draft ventilation, the addition of soybean phosphatide, earthworms and microorganisms. However, the removal of highly chlorinated PCBs was limited. The concentration of PCBs in the soil was not significantly affected during the anaerobic composting process while the percentage of highly chlorinated PCBs decreased and lower chlorinated congeners increased. On the basis of laboratory-based composting experiments, an anaerobic-aerobic composting technique was presented and a DANO drum composting equipment was designed. Finally, a field composting study was conducted. Results showed that PCBs was removed by16.1percent during the90days of composting treatment, the initial concentration was187μg/kg.
For the lower concentration of PCBs, a phytoremediation study was conducted both in greenhouse and field. Greenhouse pot experiment results showed that the combination phytoremedaiton using ryegrass and β-cyclodextrin was an effective means for the PCBs-contaminated agricultural soils. After120days of plant growth, the highest PCB removal percentage (about38%) was observed in the ryegrass planted soil, the initial concentration of which was4.52mg/kg. Addition ofβ-cyclodextrin increased the PCBs bioavailability as well as the biological activities, which might lead to the enhanced degradation of PCBs. Plant uptake contributed about0.08percent of PCBs loss, suggesting that plant uptake was not the main pathway for the PCBs removal in the soil. Furthermore, the phytoremediation efficiency of PCBs was studied in field for110days. Results showed that PCBs could be removed by7.9percent.
引文
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