生物滴滤器净化甲苯废气工艺及机理研究
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摘要
生物滴滤法净化挥发性有机物(VOCs)是有机废气治理领域的新兴技术,而反应器生物膜中微生物的特性与反应器的操作运行参数对生物系统的稳定运行与有机物的高效净化有着重要的影响。本论文以甲苯气体作为唯一碳源,在筛选出高效降解甲苯菌种的基础上,系统地研究了生物滴滤器净化甲苯过程中中间产物的形成与积累机制及气流配置方式对系统净化性能、运行稳定性与种群结构的影响,并深入探讨了微生物对甲苯及中间代谢产物的趋化性反应与滴滤器净化过程的内在关系,取得了以下的主要结果:
以焦化废水活性污泥为菌源,甲苯为唯一碳源进行递进式诱导驯化,筛选得到3株甲苯高效降解菌株:Pseudomonas putida,Gordonia sp.和Ochrobactrum sp.。
通过对菌株Pseudomonas putida降解甲苯的序批式实验和生物滴滤器净化甲苯废气试验的研究表明:生物降解甲苯过程中有邻苯二酚等中间产物积累,在试验条件下,邻苯二酚最大累积量可达0.045 mg·L~(-1)。但当停止向生物反应体系供给甲苯气体时,体系中积累的邻苯二酚在5~10 h内可以完全矿化。
基于生物降解甲苯过程与降解甲苯代谢中间产物过程的分离,并从中间产物的积累对酶的抑制作用出发,建立了甲苯消耗动力学和细胞生长动力学模型。
采用双向流交替进气(FDS)方式,对生物滴滤器内的微生物种群进行选择,构建净化有机废气的高效生物滴滤新工艺。通过生物滴滤系统进气方式改变的平行对比试验研究表明:与单向进气(UF)运行方式相比,FDS运行方式可以显著提高滴滤器最大去除能力与停运恢复能力。FDS系统对甲苯的最大去除能力为480 g·m~(-3)·h~(-1),且停运48 h后,经3~4 h系统就可以恢复稳定;而UF系统对甲苯的最大去除能力为410 g·m~(-3)·h~(-1),停运48 h后,需要9~10 h才能恢复稳定。
通过对FDS生物滴滤器中微生物群落的代谢特征研究表明: FDS运行模式下,可通过生物选择作用显著提高生物膜群落代谢活性、功能多样性和分布均匀程度,从而提高系统去除能力与稳定性。FDS系统出气段最高AWCD(每孔溶液平均吸光度)值、Mdntonch指数分别比UF系统高出46.8%和31.5%。
考察了菌株Gordonia sp.和Ochrobactrum sp.对甲苯和邻苯二酚的趋化现象,结果表明:细菌对疏水性底物和中间产物的趋化作用可推动生物膜的形成,增强相间传质推动力和生物降解效果。建立了“固液相主动吸附-生物降解”生物膜理论与稳态条件下生物滴滤器净化苯系有机气体的动力学模型,利用该模型成功预测了不同进口浓度,床层体积与运行温度下的净化性能,模型计算值与实验测试值具有较好的一致性。
该论文有图75幅,表21个,参考文献174篇。
Biotrickling filter treatment is an attractive approach for treating volatile organic compounds (VOCs) in waste-gas treatment fields. The characteristics of microbial populations in biomembrane and running conditions of bioreactors both play crucial roles in biological waste-gas treatments by significantly influencing the stability and treatment efficiency of systems. In this dissertation, based on the screening of the obligate toluene-degrading bacteria and toluene chosed as the sole carbon source, the production of metabolic intermediates by microorganisms degrading toluene and its accilimation mechanism in biotricking filters were investigated. The effect of waste-gas flow configuration pattern on biotrckling filter performance, stability and microbial community, and the roles of microbial chemotaxis to toluene and intermediates in the purification process of biotrickling filters were also researched. The main contributions to the current understanding of this topic were described below.
The consortium source in this research was derived from the activated sludge of a coking plant, and the toluene was used as the only carbon source and inducer with concentration increasing by degrees to acclimate the toluene-degrading consortium. Three strains with high toluene-degrading activity were gained, and were identified as P.putida,Gordonia sp. and Ochrobactrum sp.
Toluene biodegradation by Pseudomonas putida in batch cultues and purification in a laboratary-scale biotrickling filter were investigated. The results showed that intermediates including catechol accumulated during the degradation of toluene. Under the condition of our experimentation, the catechol which accumulated to the maximal concentration of 0.045 mg·L-1 during biodegradation could be totally mineralized within 5~10 h during shutdown periods.
By incorporating the inhibition effects of metabolic intermediates, the toluene biodegradation and cell growth kinetics is proposed to simulate toluene degradation profiles, which is based on the production and later consumption of metabolic intermediates.
A novel flow-directional-switching biotrickling filter was designed by improving the structure and running condition to select effective microbial populations. Two identical sized laboratory-scale biotrickling filters with flow configuration of flow-directional–switching (FDS) and conventional undirectional flow (UF) respectively, were used to study the purification of toluene waste-gas streams. The results show that FDS operation can improve the maximum elimination capacity of the biotrickling filter and quickly recover its nominal performance after system shutdowns. The maximum elimination capacities of 480 and 410 g·m-3·h-1 were obtained, respectively. When the systems were operated with continuous feed, then shut down for 48 hours, the elimination efficiency of FDS and UF systems were resumed to normal level with continuous feed after 3~4 h and 9~10 h, respectively.
The metabolic characteristics of the microbial communities in FDS and UF biotrickling filters were accessed. The diversity indexes and principle component analysis demonstrate that FDS operation can improve the microbial reaction capacity and community functional diversity,produce a more uniform distribution of biomass along the length of packed bed. The maximum values of AWCD (Average Well Color Development) and Mdntonch index near the oulet packed bed of FDS system were 46.8% and 31.5% higher than that of UF system.
Two strains of bacteria, identified as Gordonia sp.and Ochrobactrum sp., were tested for their chemotactic responses to toluene and catechol. The results show that bacteria chemotaxis can significantly accelerate the biofilm formation, interphase mass transfer process and biodegradation process of biotrickling filters. Then, a new theory called "Solid and Liquid phase Active Adsorption" is put forward and a related kinetic model is also established in this research. It is shown that the model agrees well with the experimental data, predicting the variations of purification performance with different inlet concentration, packed bed volumes and running temperture.
以焦化废水活性污泥为菌源,甲苯为唯一碳源进行递进式诱导驯化,筛选得到3株甲苯高效降解菌株:Pseudomonas putida,Gordonia sp.和Ochrobactrum sp.。
通过对菌株Pseudomonas putida降解甲苯的序批式实验和生物滴滤器净化甲苯废气试验的研究表明:生物降解甲苯过程中有邻苯二酚等中间产物积累,在试验条件下,邻苯二酚最大累积量可达0.045 mg·L~(-1)。但当停止向生物反应体系供给甲苯气体时,体系中积累的邻苯二酚在5~10 h内可以完全矿化。
基于生物降解甲苯过程与降解甲苯代谢中间产物过程的分离,并从中间产物的积累对酶的抑制作用出发,建立了甲苯消耗动力学和细胞生长动力学模型。
采用双向流交替进气(FDS)方式,对生物滴滤器内的微生物种群进行选择,构建净化有机废气的高效生物滴滤新工艺。通过生物滴滤系统进气方式改变的平行对比试验研究表明:与单向进气(UF)运行方式相比,FDS运行方式可以显著提高滴滤器最大去除能力与停运恢复能力。FDS系统对甲苯的最大去除能力为480 g·m~(-3)·h~(-1),且停运48 h后,经3~4 h系统就可以恢复稳定;而UF系统对甲苯的最大去除能力为410 g·m~(-3)·h~(-1),停运48 h后,需要9~10 h才能恢复稳定。
通过对FDS生物滴滤器中微生物群落的代谢特征研究表明: FDS运行模式下,可通过生物选择作用显著提高生物膜群落代谢活性、功能多样性和分布均匀程度,从而提高系统去除能力与稳定性。FDS系统出气段最高AWCD(每孔溶液平均吸光度)值、Mdntonch指数分别比UF系统高出46.8%和31.5%。
考察了菌株Gordonia sp.和Ochrobactrum sp.对甲苯和邻苯二酚的趋化现象,结果表明:细菌对疏水性底物和中间产物的趋化作用可推动生物膜的形成,增强相间传质推动力和生物降解效果。建立了“固液相主动吸附-生物降解”生物膜理论与稳态条件下生物滴滤器净化苯系有机气体的动力学模型,利用该模型成功预测了不同进口浓度,床层体积与运行温度下的净化性能,模型计算值与实验测试值具有较好的一致性。
该论文有图75幅,表21个,参考文献174篇。
Biotrickling filter treatment is an attractive approach for treating volatile organic compounds (VOCs) in waste-gas treatment fields. The characteristics of microbial populations in biomembrane and running conditions of bioreactors both play crucial roles in biological waste-gas treatments by significantly influencing the stability and treatment efficiency of systems. In this dissertation, based on the screening of the obligate toluene-degrading bacteria and toluene chosed as the sole carbon source, the production of metabolic intermediates by microorganisms degrading toluene and its accilimation mechanism in biotricking filters were investigated. The effect of waste-gas flow configuration pattern on biotrckling filter performance, stability and microbial community, and the roles of microbial chemotaxis to toluene and intermediates in the purification process of biotrickling filters were also researched. The main contributions to the current understanding of this topic were described below.
The consortium source in this research was derived from the activated sludge of a coking plant, and the toluene was used as the only carbon source and inducer with concentration increasing by degrees to acclimate the toluene-degrading consortium. Three strains with high toluene-degrading activity were gained, and were identified as P.putida,Gordonia sp. and Ochrobactrum sp.
Toluene biodegradation by Pseudomonas putida in batch cultues and purification in a laboratary-scale biotrickling filter were investigated. The results showed that intermediates including catechol accumulated during the degradation of toluene. Under the condition of our experimentation, the catechol which accumulated to the maximal concentration of 0.045 mg·L-1 during biodegradation could be totally mineralized within 5~10 h during shutdown periods.
By incorporating the inhibition effects of metabolic intermediates, the toluene biodegradation and cell growth kinetics is proposed to simulate toluene degradation profiles, which is based on the production and later consumption of metabolic intermediates.
A novel flow-directional-switching biotrickling filter was designed by improving the structure and running condition to select effective microbial populations. Two identical sized laboratory-scale biotrickling filters with flow configuration of flow-directional–switching (FDS) and conventional undirectional flow (UF) respectively, were used to study the purification of toluene waste-gas streams. The results show that FDS operation can improve the maximum elimination capacity of the biotrickling filter and quickly recover its nominal performance after system shutdowns. The maximum elimination capacities of 480 and 410 g·m-3·h-1 were obtained, respectively. When the systems were operated with continuous feed, then shut down for 48 hours, the elimination efficiency of FDS and UF systems were resumed to normal level with continuous feed after 3~4 h and 9~10 h, respectively.
The metabolic characteristics of the microbial communities in FDS and UF biotrickling filters were accessed. The diversity indexes and principle component analysis demonstrate that FDS operation can improve the microbial reaction capacity and community functional diversity,produce a more uniform distribution of biomass along the length of packed bed. The maximum values of AWCD (Average Well Color Development) and Mdntonch index near the oulet packed bed of FDS system were 46.8% and 31.5% higher than that of UF system.
Two strains of bacteria, identified as Gordonia sp.and Ochrobactrum sp., were tested for their chemotactic responses to toluene and catechol. The results show that bacteria chemotaxis can significantly accelerate the biofilm formation, interphase mass transfer process and biodegradation process of biotrickling filters. Then, a new theory called "Solid and Liquid phase Active Adsorption" is put forward and a related kinetic model is also established in this research. It is shown that the model agrees well with the experimental data, predicting the variations of purification performance with different inlet concentration, packed bed volumes and running temperture.
引文
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