地下水中挥发性有机污染物的原位气相生物修复新型技术研究
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摘要
地下水中的挥发性有机物(Volatile Organic Compounds, VOCs)已经成为地下水污染的主要污染物之一。地下水中挥发性有机物的修复可分为异位修复和原位修复,由于异位修复需要将地下水或土壤移至地表,原位修复成为了主流的修复技术。污染土壤气提法(Soil Vapor Extraction, SVE)和两相提取(Dual-Phase Extraction, DPE)成为了最新的研究方向。主要原理就是将挥发性有机物以气态的形式转移至地表进行处理。气态挥发性有机物在地面的去除技术可以是生物法、活性炭吸附法、热力燃烧法、催化氧化法等。生物法在运营成本、无二次污染等方面有着独特的优点,但其占地面积大,不够专一高效,对特定难降解污染物处理的传统工艺存在技术瓶颈等缺点制约着生物法的应用和发展。
论文以探索研究新型高效的分别处理易溶于水和难溶于水的有机物的生物反应器和研发特定难降解污染物的新技术为核心,以丙酮、正己烷、甲苯、三氯乙烯为处理对象,研究了两种新型生物反应器的各项工艺参数,同时又研究了生物滴滤器对三氯乙烯气体的厌氧脱氯过程。
同国内外其他学者的相关研究相比,论文在以下几点工作具有创新和特色：
(1)本研究采用了凝胶颗粒固定化活性污泥反应器处理丙酮气体。丙酮为易溶于水的物质代表。本研究不仅测试了处理效果,还建立了以颗粒内扩散-降解为基础的反应器模型,引入了颗粒调整系数的概念,讨论了颗粒内污染物的扩散特征和反应动力学特征。该反应器对丙酮的最大去除能力达到了476.8 g/m3/h,为传统生物滴滤器的去除能力的2倍。
(2)本研究讨论了中空纤维膜生物反应器处理甲苯—正己烷二元复合气体的处理特征和物质间的相互影响。甲苯和正己烷是难溶于水的物质的代表,该两种物质在地下水污染中有时同时存在。研究发现甲苯入口浓度较低时,其降解效率不受正己烷的影响；当入口浓度较高时,正己烷对甲苯的降解有抑制作用,同时发现甲苯对正己烷的降解影响不大。该反应器以膜内腔体积计算,对甲苯的最大去除能力达到了700 g/m3/h以上,为传统生物滴滤器的去除能力的数倍。
(3)本研究采用厌氧生物滴滤器对三氯乙烯进行了厌氧脱氯的研究,并测试了不同氧化还原电位,不同氧气浓度,不同电子供体和甲烷抑制剂对三氯乙烯脱氯性能以及各个脱氯基因数量和活性的影响。反应器对三氯乙烯的最大去除能力达到了12.0 g/m3/h以上。氧化还原电位的研究发现由于加入氧化剂后系统脱氯性能变差,而tceA基因的活性没有太大的抑制,因此vcrA基因在脱氯过程中起到了主要的作用。电子供体的研究发现vcrA基因对于维生素B12比tceA更加敏感。
(4)本研究测定了三氯乙烯厌氧脱氯的动力学参数,以及不同氧化还原电位,不同氧气浓度对动力学最大降解速率的影响的活性系数。发现三氯乙烯的最大降解速率在三个氯代乙烯中是最大。顺式二氯乙烯的半饱和常数最大,说明它的酶亲和性是最差的。
VOCs (Volatile Organic Compounds) is a group of contaminants in the groundwater pollution. The remediation of VOCs in the groundwater includes ex-situ and in-situ remediation, as in the ex-situ remdediation the contaminanted soil or groundwater should be transferred to the surface, in-situ remediation turned to more popular. SVE (Soil Vapor Extraction) and DPE (Dual-Phase Extraction) became the latest research directions. The main principle is to extract the gaseous VOCs to the surface prior to degrade them. The techniques for gaseous VOCs removal from groundwater include biofiltration, adsorption by activated carbon, thermal incineration and catalyzed oxidation. Because of low cost and no secondary contaminants, biofiltration is a good choice, but the big reactor volume, lower elimination capacity compared to other methods and very hard to degrade refractory VOCs limit the application and development of biofiltration.
This research focused on the development of novel bioreactors for soluble VOCs and insoluble VOCs, and development of novel technology for degradation of refractory VOCs. Acetone, toluene, n-hexane and TCE(trichloroethylene) were selected as the targeted contaminants, the research of technical parameters of novel bioreactor and TCE dechlorination in the anaerobic biotrickling filter was conducted as well.
Compared to other research, this research contains four creative ideas:
(1) In this research, the study of immobilized activated sludge reactor to treat gaseous acetone was conducted. Acetone is a typical soluble VOC. The reactor model based on the diffusion and degradation in one bead was developed, beads adjusting coefficient was applied in the model. The diffusion and kinetics characteristics of acetone in the bead were discussed. The maximum elimination capacity is 476.8 g/m3/h, which is 2 fold of the elimination capacity of conventional biotrickling filter.
(2) In this research, the removal performance and impact relationship of toluene and n-hexane in the binary gas system was studied and discussed. Toluene and n-hexane are typical insoluble VOCs, and these compounds are sometimes coexisting in the groundwater. Firstly when the inlet concentration of toluene was low, the removal performance of toluene was not impacted by n-hexane, but when the inlet concentration was high, toluene degradation was inhibited by n-hexane. Secondly, no obvious inhibition on n-hexane caused by toluene was observed. The maximum elimination capacity of toluene is above 700 g/m3/h based on the lumen volume of the hollow fiber, which is several fold of elimination capacity of conventional biotrickling filter.
(3) TCE dechlorination in anaerobic biotrickling filter was conducted, dechlorination performance, number and activity of genes under ORP(Oxidation Reduction Potential) variation, oxygen content variation, different electron donor and methane inhibitor were investigated as well. The elimination capacity of this reactor is above 12.0 g/m3/h. Results of ORP variation showed that after the addition of oxidants, the dechlorination performance turned to be bad but the activity of tce A gene was not inhibted too much, so the vcrA gene played the more important role in the dechlorination. Also vcrA gene was more sensitive with vitamin B12 than tceA gene.
(4) In this research, kinetic parameters of TCE dechlorination were determined, the activated coefficients of ORP and oxygen variation were obtained as well. The maximum degradation rate of TCE is the biggest one among TCE, cis-DCE(cis-dichloroethylene) and VC(Vinyl Chloride). The half-saturation constant of cis-DCE is the biggest one among TCE, cis-DCE and VC which shows the affinity of enzyme of cis-DCE is the worst.
论文以探索研究新型高效的分别处理易溶于水和难溶于水的有机物的生物反应器和研发特定难降解污染物的新技术为核心,以丙酮、正己烷、甲苯、三氯乙烯为处理对象,研究了两种新型生物反应器的各项工艺参数,同时又研究了生物滴滤器对三氯乙烯气体的厌氧脱氯过程。
同国内外其他学者的相关研究相比,论文在以下几点工作具有创新和特色：
(1)本研究采用了凝胶颗粒固定化活性污泥反应器处理丙酮气体。丙酮为易溶于水的物质代表。本研究不仅测试了处理效果,还建立了以颗粒内扩散-降解为基础的反应器模型,引入了颗粒调整系数的概念,讨论了颗粒内污染物的扩散特征和反应动力学特征。该反应器对丙酮的最大去除能力达到了476.8 g/m3/h,为传统生物滴滤器的去除能力的2倍。
(2)本研究讨论了中空纤维膜生物反应器处理甲苯—正己烷二元复合气体的处理特征和物质间的相互影响。甲苯和正己烷是难溶于水的物质的代表,该两种物质在地下水污染中有时同时存在。研究发现甲苯入口浓度较低时,其降解效率不受正己烷的影响；当入口浓度较高时,正己烷对甲苯的降解有抑制作用,同时发现甲苯对正己烷的降解影响不大。该反应器以膜内腔体积计算,对甲苯的最大去除能力达到了700 g/m3/h以上,为传统生物滴滤器的去除能力的数倍。
(3)本研究采用厌氧生物滴滤器对三氯乙烯进行了厌氧脱氯的研究,并测试了不同氧化还原电位,不同氧气浓度,不同电子供体和甲烷抑制剂对三氯乙烯脱氯性能以及各个脱氯基因数量和活性的影响。反应器对三氯乙烯的最大去除能力达到了12.0 g/m3/h以上。氧化还原电位的研究发现由于加入氧化剂后系统脱氯性能变差,而tceA基因的活性没有太大的抑制,因此vcrA基因在脱氯过程中起到了主要的作用。电子供体的研究发现vcrA基因对于维生素B12比tceA更加敏感。
(4)本研究测定了三氯乙烯厌氧脱氯的动力学参数,以及不同氧化还原电位,不同氧气浓度对动力学最大降解速率的影响的活性系数。发现三氯乙烯的最大降解速率在三个氯代乙烯中是最大。顺式二氯乙烯的半饱和常数最大,说明它的酶亲和性是最差的。
VOCs (Volatile Organic Compounds) is a group of contaminants in the groundwater pollution. The remediation of VOCs in the groundwater includes ex-situ and in-situ remediation, as in the ex-situ remdediation the contaminanted soil or groundwater should be transferred to the surface, in-situ remediation turned to more popular. SVE (Soil Vapor Extraction) and DPE (Dual-Phase Extraction) became the latest research directions. The main principle is to extract the gaseous VOCs to the surface prior to degrade them. The techniques for gaseous VOCs removal from groundwater include biofiltration, adsorption by activated carbon, thermal incineration and catalyzed oxidation. Because of low cost and no secondary contaminants, biofiltration is a good choice, but the big reactor volume, lower elimination capacity compared to other methods and very hard to degrade refractory VOCs limit the application and development of biofiltration.
This research focused on the development of novel bioreactors for soluble VOCs and insoluble VOCs, and development of novel technology for degradation of refractory VOCs. Acetone, toluene, n-hexane and TCE(trichloroethylene) were selected as the targeted contaminants, the research of technical parameters of novel bioreactor and TCE dechlorination in the anaerobic biotrickling filter was conducted as well.
Compared to other research, this research contains four creative ideas:
(1) In this research, the study of immobilized activated sludge reactor to treat gaseous acetone was conducted. Acetone is a typical soluble VOC. The reactor model based on the diffusion and degradation in one bead was developed, beads adjusting coefficient was applied in the model. The diffusion and kinetics characteristics of acetone in the bead were discussed. The maximum elimination capacity is 476.8 g/m3/h, which is 2 fold of the elimination capacity of conventional biotrickling filter.
(2) In this research, the removal performance and impact relationship of toluene and n-hexane in the binary gas system was studied and discussed. Toluene and n-hexane are typical insoluble VOCs, and these compounds are sometimes coexisting in the groundwater. Firstly when the inlet concentration of toluene was low, the removal performance of toluene was not impacted by n-hexane, but when the inlet concentration was high, toluene degradation was inhibited by n-hexane. Secondly, no obvious inhibition on n-hexane caused by toluene was observed. The maximum elimination capacity of toluene is above 700 g/m3/h based on the lumen volume of the hollow fiber, which is several fold of elimination capacity of conventional biotrickling filter.
(3) TCE dechlorination in anaerobic biotrickling filter was conducted, dechlorination performance, number and activity of genes under ORP(Oxidation Reduction Potential) variation, oxygen content variation, different electron donor and methane inhibitor were investigated as well. The elimination capacity of this reactor is above 12.0 g/m3/h. Results of ORP variation showed that after the addition of oxidants, the dechlorination performance turned to be bad but the activity of tce A gene was not inhibted too much, so the vcrA gene played the more important role in the dechlorination. Also vcrA gene was more sensitive with vitamin B12 than tceA gene.
(4) In this research, kinetic parameters of TCE dechlorination were determined, the activated coefficients of ORP and oxygen variation were obtained as well. The maximum degradation rate of TCE is the biggest one among TCE, cis-DCE(cis-dichloroethylene) and VC(Vinyl Chloride). The half-saturation constant of cis-DCE is the biggest one among TCE, cis-DCE and VC which shows the affinity of enzyme of cis-DCE is the worst.
引文
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