三氯乙烯的好氧共代谢与挥发模型研究
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摘要
大量的氯代烃因不合理的使用、处理和处置进入环境中造成了严重的地下水环境污染,引起了环境工作者的广泛关注,其中三氯乙烯(TCE)是地下水中常见的一种氯代烃有机污染物。对于地下水中TCE的修复,由于生物法具有成本低、操作方便、易行、能够充分发挥微生物的降解能力,针对性地去除某种或某类有机物等特点,成为国内外专家和学者的研究热点。生物法修复TCE尤以好氧共代谢降解TCE最为有效。
论文选取了甲苯、苯、氯苯、苯酚、苯甲酸、苯胺等六种芳香族化合物作为TCE的共代谢基质,通过对微生物的驯化、富集培养,以瓦呼仪作为测试手段,分析了六种共代谢基质在其驯化后活性污泥中的可生物降解性,及六种共代谢基质驯化后的混合微生物共代谢降解TCE的可能性。
研究了六种共代谢基质和TCE共代谢降解的动力学性质。为了比较TCE好氧共代谢降解速率,实验同时对TCE为唯一碳源的降解动力学进行了研究。研究表明,TCE的降解动力学均符合一级反应动力学方程。TCE的降解速率常数的关系为:Ksa苯酚> Ksa甲苯> Ksa苯甲酸> Ksa苯胺> Ksa苯> KsaTCE唯一碳源> Ksa氯苯,速率常数依次为0.3078, 0.1698, 0.1254, 0.0443, 0.0286, 0.0268, 0.0147 L / g?h。本实验分别对单一代谢基质的降解(不加TCE)和共代谢条件下基质的降解动力学进行了研究,结果表明在两种情况下代谢基质的降解均符合一级动力学方程。通过对TCE和共代谢基质速率常数的比较,得出如下结论:苯酚是最有效的共代谢基质,其次是甲苯、苯;氯苯不宜作为TCE的共代谢降解的基质。经研究化合物的分子结构和生物降解性的关系得出,共代谢基质的空间参数是影响共代谢降解的主要因素。
在实验室条件下研究了TCE在灭菌污泥和活性污泥中的挥发模型。由于生物降解的作用,活性污泥中TCE的挥发速率常数明显低于灭菌污泥中对应的数值;25℃时两体系中TCE的挥发速率常数均与该温度下TCE在水溶相中的挥发速率常数在一个数量级上,这说明在含有污泥的溶液体系中挥发模型同样适用。
Chlorinated hydrocarbons have a widespread use in industry and agriculture,because of their accidental spills, leakages and improper use, which caused greatconcern by environmental staff. Trichloroethylene (TCE) is one of the most extensivecontaminants in groundwater. Because of convenient operation, lower expense andusing selected microbes to remove organic compounds, biological treatment forTCE-contaminated waters becomes a hot topic. TCE is efficiently biodegraded byaerobic cometabolism
In the Ph. D. dissertation, six aromatic compounds, including toluene, benzene,chlorobenzene, phenol, benzoic acid and aniline, were used TCE cometabolicsubstrates to acclimate the activated sludge. The biodegradability of the sixacclimated substrates and that of TCE through cometabolism are conducted bymeasuring oxygen consumption with Warburg respirometer.
The biodegradation kinetics of the six cometabolic substrates and that of TCE bycometabolic degradation were studied. In order to compare with TCE cometabolicdegradation kinetic rates, the degradation kinetics of TCE using TCE as the solecarbon source was conducted. The results were shown that a first-order linear rate lawapplied to TCE biodegradation under the conditions mentioned aboved. The first orderrate constant relationship of TCE was as follows: Ksa phenol > Ksa toluene > Ksabenzoic acid > Ksa aniline > Ksa benzene > Ksa TCE > Ksa chlorobenzene,and therate constant was 0.3078, 0.1698, 0.1254, 0.0443, 0.0286, 0.0268, 0.0147 L/g?h,respectively. The biodegradation kinetics experiments of the metabolic substrateswithout TCE and under cometabolic conditions were conducted. The results wereshown that the six metabolic substrates confirmed to the first order equation underboth conditions. Compared to TCE cometabolic rate constant, conclusions weredrawn that phenol was the most suitable cometabolic substrate, toluene second, andbenzene third;chlorobenzene was not suitable substrate. Space descriptor ofcometabolic substrate was the effective factor in cometabolic biodegradation processby Quantitative structure biodegradability relationships(QSBR)study.
The volatile model of TCE was discussed in autoclaved sludge and activatedsludge systems in the laboratory. Results suggested that the volatile rate constant ofTCE in activated sludge was apparently lower than that of TCE in autoclaved sludge,due to the biodegradation.The volatile rate constant of TCE in both systems at 25℃
was within the range of the estimate value in aquatic phase, which expressed thevolatile model was also applied in sludge system.
论文选取了甲苯、苯、氯苯、苯酚、苯甲酸、苯胺等六种芳香族化合物作为TCE的共代谢基质,通过对微生物的驯化、富集培养,以瓦呼仪作为测试手段,分析了六种共代谢基质在其驯化后活性污泥中的可生物降解性,及六种共代谢基质驯化后的混合微生物共代谢降解TCE的可能性。
研究了六种共代谢基质和TCE共代谢降解的动力学性质。为了比较TCE好氧共代谢降解速率,实验同时对TCE为唯一碳源的降解动力学进行了研究。研究表明,TCE的降解动力学均符合一级反应动力学方程。TCE的降解速率常数的关系为:Ksa苯酚> Ksa甲苯> Ksa苯甲酸> Ksa苯胺> Ksa苯> KsaTCE唯一碳源> Ksa氯苯,速率常数依次为0.3078, 0.1698, 0.1254, 0.0443, 0.0286, 0.0268, 0.0147 L / g?h。本实验分别对单一代谢基质的降解(不加TCE)和共代谢条件下基质的降解动力学进行了研究,结果表明在两种情况下代谢基质的降解均符合一级动力学方程。通过对TCE和共代谢基质速率常数的比较,得出如下结论:苯酚是最有效的共代谢基质,其次是甲苯、苯;氯苯不宜作为TCE的共代谢降解的基质。经研究化合物的分子结构和生物降解性的关系得出,共代谢基质的空间参数是影响共代谢降解的主要因素。
在实验室条件下研究了TCE在灭菌污泥和活性污泥中的挥发模型。由于生物降解的作用,活性污泥中TCE的挥发速率常数明显低于灭菌污泥中对应的数值;25℃时两体系中TCE的挥发速率常数均与该温度下TCE在水溶相中的挥发速率常数在一个数量级上,这说明在含有污泥的溶液体系中挥发模型同样适用。
Chlorinated hydrocarbons have a widespread use in industry and agriculture,because of their accidental spills, leakages and improper use, which caused greatconcern by environmental staff. Trichloroethylene (TCE) is one of the most extensivecontaminants in groundwater. Because of convenient operation, lower expense andusing selected microbes to remove organic compounds, biological treatment forTCE-contaminated waters becomes a hot topic. TCE is efficiently biodegraded byaerobic cometabolism
In the Ph. D. dissertation, six aromatic compounds, including toluene, benzene,chlorobenzene, phenol, benzoic acid and aniline, were used TCE cometabolicsubstrates to acclimate the activated sludge. The biodegradability of the sixacclimated substrates and that of TCE through cometabolism are conducted bymeasuring oxygen consumption with Warburg respirometer.
The biodegradation kinetics of the six cometabolic substrates and that of TCE bycometabolic degradation were studied. In order to compare with TCE cometabolicdegradation kinetic rates, the degradation kinetics of TCE using TCE as the solecarbon source was conducted. The results were shown that a first-order linear rate lawapplied to TCE biodegradation under the conditions mentioned aboved. The first orderrate constant relationship of TCE was as follows: Ksa phenol > Ksa toluene > Ksabenzoic acid > Ksa aniline > Ksa benzene > Ksa TCE > Ksa chlorobenzene,and therate constant was 0.3078, 0.1698, 0.1254, 0.0443, 0.0286, 0.0268, 0.0147 L/g?h,respectively. The biodegradation kinetics experiments of the metabolic substrateswithout TCE and under cometabolic conditions were conducted. The results wereshown that the six metabolic substrates confirmed to the first order equation underboth conditions. Compared to TCE cometabolic rate constant, conclusions weredrawn that phenol was the most suitable cometabolic substrate, toluene second, andbenzene third;chlorobenzene was not suitable substrate. Space descriptor ofcometabolic substrate was the effective factor in cometabolic biodegradation processby Quantitative structure biodegradability relationships(QSBR)study.
The volatile model of TCE was discussed in autoclaved sludge and activatedsludge systems in the laboratory. Results suggested that the volatile rate constant ofTCE in activated sludge was apparently lower than that of TCE in autoclaved sludge,due to the biodegradation.The volatile rate constant of TCE in both systems at 25℃
was within the range of the estimate value in aquatic phase, which expressed thevolatile model was also applied in sludge system.
引文
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