地下水中BTEX的迁移规律及其原位生物修复技术研究
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摘要
苯系物(苯、甲苯、乙苯和二甲苯,BTEX),作为单环芳烃类物质,主要存在于原油和石油产品(如天然气)中,并作为工业溶剂广泛应用于化工行业。BTEX具有“致癌、致畸和致突变”效应,其在生产、储存和运输过程中极易进入地下环境,并严重威胁地下水的公共安全,因此研究地下水环境中BTEX的迁移规律及其原位修复技术具有重要的理论价值和应用前景。本文首先建立污染物在土壤—地下水环境中迁移转化基本控制方程,并对BTEX在多孔介质中的迁移传递规律进行了研究;同时针对构建的固定化生物格栅系统,从微生物驯化、降解菌群落结构分析以及生物固定化技术等方面对地下水中BTEX的原位生物修复过程进行了系统研究。
由等温吸附平衡确定了BTEX在夹砂粉质粘土中的吸附行为表现为线性规律,通过土柱弥散实验计算得到BTEX在夹砂粉质粘土中的弥散系数和阻滞系数。对于阻滞系数Rd来说,其由小到大依次为苯<甲苯<二甲苯<乙苯,说明土壤对BTEX混合物各组分的截留和净化能力不同,其中对苯的作用最弱,而对甲苯、乙苯和二甲苯的截留和净化作用相对较强。
对富集驯化所得到的BTEX混合降解菌,确定了其好氧降解的最适条件为:温度30℃、pH值7.5、接种量为2.61 mg/L。底物降解动力学研究结果表明:其一级降解速率常数由大到小依次为二甲苯>乙苯>甲苯>苯,而BTEX共存时由于存在竞争抑制作用导致各组分的一级降解速率常数降低。综合考虑BTEX基质利用和混合菌的生长,采用Monod动力学模型拟合得到混合菌以苯、甲苯、乙苯和二甲苯作为共同基质的最大比增长速率分别为0.3395、0.5199、0.6298和0.2701 h-1,而基质半饱和常数为160.6、124.6、168.3、227.8 mg/L。
针对苯、甲苯、乙苯、二甲苯和BTEX混合基质五种驯化方式下的混合菌,研究了其菌种群结构特点并初步探讨了BTEX好氧代谢途径。结果表明:不同驯化方式的混合菌,其种群具有一定相似性和基因多样性,因此其生物降解性能不同。BTEX混合基质驯化降解菌的总DNA中含有儿茶酚-1,2-双氧酶,说明代谢过程首先是将苯系物转化为含烷基的儿茶酚,然后通过正位裂解转化为含烷基的顺式粘康酸,最终进入三羧酸循环转化为CO2和H2O。
以固定化微生物作为反应格栅填充介质为目的,制备并比较了海藻酸钠-活性炭纤维型(SA-MB)和聚乙烯醇-活性炭纤维型(PVA-MB)固定化填充介质的微观结构、降解性能和可重复利用性,从而确定海藻酸钠作为包埋载体更具优势,而活性炭纤维是一种较好的改进载体,起到了支撑稳定结构和强化生物降解作用。
SA-MB填充介质具有良好的渗透性能,满足作为生物格栅填充介质的要求。采用土柱实验研究了BTEX混合组分在固定化生物格栅中的去除过程。结果表明:所构建的生物格栅系统能够很好地去除污染地下水中的BTEX,研究结果可对现场修复提供一定的依据和参考。
Benzene, toluene, ethylene and xylenes (BTEX, in brief), as important aromatic compounds, exist in oil and petroleum products and were widely used as solvents in industry. BTEX were improved to be carcinogenic, teratogenetic and mutagenic to endanger human-beings’health by contaminating underground water with leakage and delivery. To study the migration and removal of BTEX-contaminated groundwater is of theoretical and application importance. In this study, the transport and transformation formulation was established for BTEX in soil and groundwater system. Then the immobilized biological barrier has been presented for describing the remediation of BTEX-contaminated groundwater, which was included the domestic influence and community analysis of mixed culture, preparation of immobilized bio-beads and in situ removal process of BTEX.
The detailed works of this thesis are as follows:
The results of batch experiment indicated that linear equilibrium adsorption equation can well describe the adsorption behavior of BTEX in clayed soil. A soil column experiment was performed to calculate the dispersive coefficient and retardation factor of the test medium. As for Rd, the retardation factors were followed by benzene, toluene, ethyl benzene and xylenes, which meant the aquifer medium had hardly the abilities to retard and attenuate benzene and could partly retard toluene,ethyl benzene and xylenes.
Based on the enrichment and purposed acclimation of the aerobic microbes, degradation performance of BTEX was studied and optimal temperature was 30℃, pH value was 7.5 and inoculums was 2.61 mg/L. The one-order kinetics constants of substrates’degradation were followed as: benzene < toluene < ethyl benzene < xylenes. As for BTEX mixture, the dynamics parameters were apparently decreased because of competitive effect. Through Monod kinetics simulation, the maximum-specific-growth rates of mixed culture were separately 0.3395, 0.5199, 0.6298 and 0.2701 h-1, while the half-saturation concentrations were 160.6, 124.6, 168.3 and 227.8 mg/L.
Different domestic conditions have been taken to study the changes of microbial community structure. The results of PCR-DGGE showed that different domestic indeed influenced the mixture’s DNA diversity and biodegradation. The microbes, acclimated by BTEX mixture, had the key metabolism enzyme as catechol-1, 2-dioxygenese, which indicated the microbes could firstly biodegrade BTEX into catechol with alkyl, then degrade into cis,cis-muconic acid with alkyl by ortho-cleavage, at last transform into carbon dioxide and water in tricarboxylic acid cycle.
Bench experiments of degradation were carried out to assess the performance of two kinds of new-typed immobilized bio-beads, which were produced with sodium alginate (SA), polyvinyl alcohol (PVA) and activated carbon fiber (ACF). As a result, SA-MB was considered better in the microstructure, degradation and reusability, and ACF was a well-performing encapsulation carrier, which could enhance biodegradation of BTEX by changing the microstructure and stabilities of MB.
Permeability of SA-MB as medium of biobarrier was measured as1.32×10-10 m2, which was proved to be suitable for permeable reactive system. Furthermore, the removal of BTEX was studied in the biobarrier which was simulated by laboratory column. It showed that the presented biobarrier with immobilized biobeads could do well in remedying BTEX-contaminated groundwater and provide dependable basis for in situ remediation practice.
由等温吸附平衡确定了BTEX在夹砂粉质粘土中的吸附行为表现为线性规律,通过土柱弥散实验计算得到BTEX在夹砂粉质粘土中的弥散系数和阻滞系数。对于阻滞系数Rd来说,其由小到大依次为苯<甲苯<二甲苯<乙苯,说明土壤对BTEX混合物各组分的截留和净化能力不同,其中对苯的作用最弱,而对甲苯、乙苯和二甲苯的截留和净化作用相对较强。
对富集驯化所得到的BTEX混合降解菌,确定了其好氧降解的最适条件为:温度30℃、pH值7.5、接种量为2.61 mg/L。底物降解动力学研究结果表明:其一级降解速率常数由大到小依次为二甲苯>乙苯>甲苯>苯,而BTEX共存时由于存在竞争抑制作用导致各组分的一级降解速率常数降低。综合考虑BTEX基质利用和混合菌的生长,采用Monod动力学模型拟合得到混合菌以苯、甲苯、乙苯和二甲苯作为共同基质的最大比增长速率分别为0.3395、0.5199、0.6298和0.2701 h-1,而基质半饱和常数为160.6、124.6、168.3、227.8 mg/L。
针对苯、甲苯、乙苯、二甲苯和BTEX混合基质五种驯化方式下的混合菌,研究了其菌种群结构特点并初步探讨了BTEX好氧代谢途径。结果表明:不同驯化方式的混合菌,其种群具有一定相似性和基因多样性,因此其生物降解性能不同。BTEX混合基质驯化降解菌的总DNA中含有儿茶酚-1,2-双氧酶,说明代谢过程首先是将苯系物转化为含烷基的儿茶酚,然后通过正位裂解转化为含烷基的顺式粘康酸,最终进入三羧酸循环转化为CO2和H2O。
以固定化微生物作为反应格栅填充介质为目的,制备并比较了海藻酸钠-活性炭纤维型(SA-MB)和聚乙烯醇-活性炭纤维型(PVA-MB)固定化填充介质的微观结构、降解性能和可重复利用性,从而确定海藻酸钠作为包埋载体更具优势,而活性炭纤维是一种较好的改进载体,起到了支撑稳定结构和强化生物降解作用。
SA-MB填充介质具有良好的渗透性能,满足作为生物格栅填充介质的要求。采用土柱实验研究了BTEX混合组分在固定化生物格栅中的去除过程。结果表明:所构建的生物格栅系统能够很好地去除污染地下水中的BTEX,研究结果可对现场修复提供一定的依据和参考。
Benzene, toluene, ethylene and xylenes (BTEX, in brief), as important aromatic compounds, exist in oil and petroleum products and were widely used as solvents in industry. BTEX were improved to be carcinogenic, teratogenetic and mutagenic to endanger human-beings’health by contaminating underground water with leakage and delivery. To study the migration and removal of BTEX-contaminated groundwater is of theoretical and application importance. In this study, the transport and transformation formulation was established for BTEX in soil and groundwater system. Then the immobilized biological barrier has been presented for describing the remediation of BTEX-contaminated groundwater, which was included the domestic influence and community analysis of mixed culture, preparation of immobilized bio-beads and in situ removal process of BTEX.
The detailed works of this thesis are as follows:
The results of batch experiment indicated that linear equilibrium adsorption equation can well describe the adsorption behavior of BTEX in clayed soil. A soil column experiment was performed to calculate the dispersive coefficient and retardation factor of the test medium. As for Rd, the retardation factors were followed by benzene, toluene, ethyl benzene and xylenes, which meant the aquifer medium had hardly the abilities to retard and attenuate benzene and could partly retard toluene,ethyl benzene and xylenes.
Based on the enrichment and purposed acclimation of the aerobic microbes, degradation performance of BTEX was studied and optimal temperature was 30℃, pH value was 7.5 and inoculums was 2.61 mg/L. The one-order kinetics constants of substrates’degradation were followed as: benzene < toluene < ethyl benzene < xylenes. As for BTEX mixture, the dynamics parameters were apparently decreased because of competitive effect. Through Monod kinetics simulation, the maximum-specific-growth rates of mixed culture were separately 0.3395, 0.5199, 0.6298 and 0.2701 h-1, while the half-saturation concentrations were 160.6, 124.6, 168.3 and 227.8 mg/L.
Different domestic conditions have been taken to study the changes of microbial community structure. The results of PCR-DGGE showed that different domestic indeed influenced the mixture’s DNA diversity and biodegradation. The microbes, acclimated by BTEX mixture, had the key metabolism enzyme as catechol-1, 2-dioxygenese, which indicated the microbes could firstly biodegrade BTEX into catechol with alkyl, then degrade into cis,cis-muconic acid with alkyl by ortho-cleavage, at last transform into carbon dioxide and water in tricarboxylic acid cycle.
Bench experiments of degradation were carried out to assess the performance of two kinds of new-typed immobilized bio-beads, which were produced with sodium alginate (SA), polyvinyl alcohol (PVA) and activated carbon fiber (ACF). As a result, SA-MB was considered better in the microstructure, degradation and reusability, and ACF was a well-performing encapsulation carrier, which could enhance biodegradation of BTEX by changing the microstructure and stabilities of MB.
Permeability of SA-MB as medium of biobarrier was measured as1.32×10-10 m2, which was proved to be suitable for permeable reactive system. Furthermore, the removal of BTEX was studied in the biobarrier which was simulated by laboratory column. It showed that the presented biobarrier with immobilized biobeads could do well in remedying BTEX-contaminated groundwater and provide dependable basis for in situ remediation practice.
引文
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[2] Farhadian M, Vachelard C, Duchez D, et al. In situ bioremediation of monoaromatic pollutants in Ground Water: A review. Bioresource Technology, 2008, 99: 5296~5308
[3] Hutchins S R, Downs W C, Wilson J T. Effect of nitrate addition on biorestoration of fuel-contaminated aquifer: field demonstration. Ground Water, 1991, 29(4): 571~580.
[4] Robert C B, Carios A G, Mark T B. Geochemical indicators of intrinsic bioremediation. Ground Water, 1995, 33(2): 180~189
[5] Brian C, Kirtland C, Marjorie A. Petroleum mass removal from low permeability sediment using air sparging /soil vapor extraction: impact of continuous or pulsed operation. Journal of Contaminant Hydrology, 2000, 41, 367~383
[6] Menendez-Vega D, Pelaez A I, Cordoba G F, et al. Engineered in situ bioremediation of soil and groundwater polluted with weathered hydrocarbons. European Journal of Soil Biology, 2007, 43 (5-6): 310~321
[7] Juhler R K, Felding G. Monitoring methyl tertiary butyl-ether (BTEX) and other organic micropollutants in groundwater: results from the Danish national monitoring program. Water, Air, and Soil Pollution, 2003, 149: 145~161.
[8] Lee J Y, Lee K K. Viability of natural attenuation in a petroleum contaminated shallow sandy aquifer. Environmental Pollution, 2003, 126(2): 201~212
[9] Katrin A, Matthias M, Adolf E, et al. Microcosms experiments to acess the potential for natural attenuation of contaminated groundwater. Water Research, 2001, 35(3): 720~728
[10]郭永海,沈照理,钟佐燊，等，河北平原地下水有机氯污染及其防污性能的关系,水文地质工程地质,1996,23(1):40~42
[11]郭华明,王焰新.地下水有机污染治理技术现状及发展前景,地质科技情报, 1999,18(2):69~72
[12]徐绍辉,朱学愚.地下水石油污染的水力截获技术及数值模拟,水利学报, 1999, 1(1):71~76
[13]史箴,李抗美.用毛细管柱测定水和废水中的苯系物,甘肃环境研究与监测, 1999,12(3):123~125
[14] Mackay D M, Cherry J A, Groundwater contamination: pump-and-treatremediation. Journal of Environmental Science and Technology, 1989, 23(6): 630~636
[15] Faisal I K, Tahir H, Ramzi H. An overview and analysis of site remediation technologies. Journal of Environmental Management, 2004, 71: 95~122
[16] Daifullah A M, Girgis B S. Impact of surface characteristics of activated carbon on adsorption of BTEX. Colloids Surfaces A: Phys. Engineering Aspects, 2003, 214(1-3), 181~193
[17] Ranck, J M, Bowman R S, Weeber J L, et al. BTEX removal from produced water using surfactant-modified zeolite. Journal of Environmental Engineering, 2005, 131(3): 434~442
[18]任子平,杨赞中,矿物的环保功能及其应用研究进展,矿产保护与利用, 2001,3:44~48
[19] Robin S, Krishna R R. Mechanisms controlling toluene removal from saturated soils during in situ air sparging. Journal of Hazardous Materials, 1998, 57: 209~230
[20]纪录,张晖,原位化学氧化法在土壤和地下水修复中的研究进展,环境污染治理技术与设备,2003,4(6),37~42
[21] Tiburtius E R, Peralta-Zamora P, Emmel A. Treatment of gasoline-contaminated waters by advanced oxidation processes. Journal of Hazardous Materials, 2005, 126, 86~90
[22] Mascolo G, Ciannarella R, Balest L, et al. Effectiveness of UV-based advanced oxidation processes for the remediation of hydrocarbon pollution in the groundwater: A laboratory investigation. Journal of Hazardous Materials, 2007, 152(3): 1138~1145
[23]陈士夫,空心玻璃微球附载TiO2清除水面漂浮的油层,中国环境科学,1999, l(1):47~50
[24] Gabriel J, Baldrian P, Verma P, et al. Degradation of BTEX and PAHs by Co(Ⅱ)and Cu(Ⅱ)-based radical-generating systems. Applied catalysis B: Environmental, 2004, 51: 159 ~164
[25]于勇,谢天强,蔺延项等,受石油污染地下水的臭氧处理技术研究,工业用水与废水,2001,32(2):14~15
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