四种三氯乙烯去除工艺的基础研究与比较
摘要
随着工农业的迅速发展,以三氯乙烯(trichloroethylene, TCE)为代表的大量有机氯代烃因不合理的使用、处理和处置进入环境造成严重的水环境污染。颗粒活性炭(granular activated carbon, GAC)吸附工艺作为一套成熟可靠的工艺被广泛用于难降解有机污染物的去除,可以达到深度净化的目的(如<10μg/L)；生物活性炭(biological activated carbon, BAC)工艺可以通过生物再生的方式克服活性炭吸附容量的限制,延长活性炭的使用周期；厌氧膨胀颗粒污泥床(expanded granular sludge bed, EGSB)反应器对高浓度有毒污染物有独特的处理优势；生物滴滤器(biotrickling filter, BTF)对于气体抽提后的难降解有机气体有良好的去除效果。本文探讨了上述这四种工艺用于去除TCE的可行性,考察不同工艺操作条件对TCE去除效果的影响,分析它们各自的适用场合和应用前景,从而为特定TCE污染情况的处理提供切实可行的方法。
为评价活性炭对TCE的吸附性能,以10种不同原料制备的活性炭样品进行了TCE的平衡容量实验和连续流微型快速穿透(MCRB)实验。各种活性炭对TCE的吸附容量的排列与其苯酚值排列相同,TCE初始浓度和少量甲醇的加入不会影响活性炭的吸附容量。相比其他炭型,含有丰富中孔的煤质炭对TCE吸附容量较低,但吸附容量利用率较高,适合用于实际工艺中去除TCE；由毛竹制备而成的竹质炭,对TCE的去除量和吸附容量利用率均颇为可观,是一种值得开发的新型环保炭型。水体中的共存有机物会降低活性炭对TCE的吸附容量,其竞争吸附的程度跟水体中有机物的分子量大小分布有关。两个串联的活性炭炭床是高效低耗吸附处理工艺的关键单元,因为前置炭床的利用率能得到大幅度提升,后置炭床能保障出水达标。
好氧条件下TCE只能通过共代谢方式降解。苯酚是一种高效的共代谢基质,以活性污泥培养驯化的苯酚混合菌为TCE降解菌源,通过批式降解实验评估其对TCE的降解性能。苯酚能诱导产生氧化酶和TCE共代谢需要的能量,是TCE共降解过程中必不可少的共代谢基质；TCE的大幅度降解要在苯酚基本利用后才会发生。通过接种驯化好的TCE降解菌,可以迅速启动BAC系统；在170天的连续运行期间,BAC对TCE的去除率维持在20-40%。使用对TCE具有高吸附量的活性炭能确保BAC工艺在运行初期和有冲击负荷情况下的高度处理效果。生长基质苯酚的进水浓度是TCE去除效率的关键因素,苯酚浓度过高会加重TCE共代谢的竞争性抑制,过低不足以维持其高效降解。苯酚浓度在2-4mg/L,苯酚/TCE进水负荷比率在15左右时,BAC对TCE的去除率最高达到40%左右。根据TCE-苯酚的共代谢降解规律,使用苯酚、TCE单独循环进水的工艺操作模式,有效避免了竞争性抑制,较好地维持了微生物的生长和降解活性,强化了TCE去除效率；在每天2h苯酚进水、22h TCE的进水情况下,TCE去除率最高为72%(进水浓度200μg/L),平均去除率达到65%,最大去除能力为0.39g/m3/h。
厌氧条件下TCE能通过还原脱氯依次转化为二氯乙烯、一氯乙烯和乙烯。利用生物强化的方法将商业脱氯菌SDC-9投入到接种颗粒污泥的厌氧EGSB反应器中,达成快速启动；进水浓度在2-10mg/L,水力停留时间在6h时,TCE的去除率为85%左右,其最大去除能力超过1.5g/m3/h。将EGSB转为序批式操作模式,延长反应时间有助于乙烯的生成。厌氧颗粒污泥是一种优良的生物载体,可以很好地负载特定降解菌并有效防止微生物脱落,从而使EGSB反应器工艺达到长期稳定降解TCE的功能。
通过接种SDC-9快速启动厌氧BTF；空床停留时间为12min时,稳定运行下的气态TCE去除率在99%以上(进气浓度为700mg/m3),终产物乙烯占到50%左右。厌氧BTF对TCE的最大去除能力达到9.0g/m3/h,显示出优越的处理性能,而且150多天的稳定运行证实了BTF不会因床层堵塞等问题造成处理性能的下降。在运行过程中,降解TCE的床层区域会逐渐转移到反应器前半部分。不同高度床层的处理性能与脱氯菌种和基因的种类、数量和活性之间存在关联性。停运60天后厌氧BTF内的微生物只剩2%的TCE降解活性,同时微生物总量减少了50%,但BTF重启后可以快速恢复TCE去除性能；停运28天和60天的厌氧BTF分别在1天和8天后基本恢复原先的TCE去除能力,但全面恢复之前的降解性能(乙烯转化率)则需要更长时间。
本课题研究了四种各具特色并有各自适用场合的TCE去除工艺。GAC工艺主要用于去除TCE轻度污染水体,达到深度净化的目的；BAC工艺持续稳定、抗冲击负荷强,能长期稳定的处理低浓度TCE(<500μg/L)水体；厌氧EGSB反应器工艺具有较高的TCE去除能力,适用于TCE严重污染水体(<10mg/L)的处理；对于需要使用气提去除水体里TCE的场合,厌氧BTF工艺可以高效去除进气中的TCE,潜在的应用前景广阔。本文的特色在于：在GAC工艺研究阶段,提出使用苯酚值可以预测活性炭对于TCE的吸附性能,丹宁酸值能表征吸附容量利用率,竞争吸附对活性炭吸附容量的影响程度跟水体中有机物的分子量大小分布有关,同时验证了MCRB测试可以准确模拟传统穿透实验,并提出一套高效低耗的GAC吸附工艺；在BAC工艺中,通过研究TCE-苯酚的共代谢降解规律,研发了新型的苯酚、TCE循环进水的BAC运行模式,有效提高了BAC工艺对TCE的降解效率；在厌氧BTF中,研究了相关菌种和特定基因在BTF不同床层高度的分布变化及随时间的迁移转换,揭示了脱氯菌群和功能基因的种类、数量和活性与BTF处理性能之间的内在关联性；同时,还对厌氧BTF在停运闲置期间微生物的TCE脱氯性能、活性和数量的变化进行了分析,并评估了反应器在长期停运后的恢复运行效果。
Along with the rapid industrial and agricultural development of the modern society, trichloroethylene (TCE) and other chlorinated hydrocarbons have entered environment due to improper disposal practices and accidental leaks resulting in serious contamination of groundwater in many parts of the world. Granular activated carbon (GAC) adsorption has often been employed for removing persistent organic pollutants (POPs) to produce a clean effluent meeting a very low discharge limit (<10μg/L); taking advantage of the concurrent biodegradation of the adsorbed POPs in many GAC adsorbers, biological activated carbon (BAC) process can be used to extend the GAC service life; expanded granular sludge bed (EGSB) process has been employed for treating influents containing high concentrations of toxic pllutants; biotrickling filter (BTF) process is capable of removing POPs from the exhaust stream of the stripping operation. This research has been conducted to determine the feasibility of the four treatment processes for removing TCE, to identify the potential applications, and to produce results useful for remediation of TCE contaminated groundwater.
Ten GAC samples of different raw materials and preparation were employed in the batch adsorption isotherm runs for measuring their TCE capacities and the continuous flow breakthrough runs for simulating the TCE removal in actual treatment applications. The GACs'adsorptive capacities for TCE were in the same order as their phenol numbers; they were not affected by the starting TCE concentration and/or the presence of small amount of methanol. The higher utilization rate found for the meso pore rich coal based GAC makes it competitive despite its relatively low TCE capacity. The GAC made from toxicant free, low cost and renewable bamboo is attractive because of its relatively high TCE capacity and availability. GACs'capacities for TCE in pure water were reduced by competitive adsorption of other organic constituents of the water samples; small organic compounds in tap water were more competitive than the NOM in the higher TOC well water sample. The MCRB data confirmed the GACs'available TCE capacities and that the serial bed treatment is desirable because most of the first absorber's capacity can be utilized for removing the pollutants.
Under the aerobic condition, TCE can be biodegraded only in the presence of a co-substrate such as phenol. Phenol can induce the production of oxidase and the energy necessary for TCE cometablism; high degree of TCE degradation would take place after most of the phenol has been biodegraded. Acclimated mixed phenol degraders originated from activated sludge were employed for the batch experiments to assess their TCE degrading capability. Inoculation of highly acclimated TCE degraders quickly established the BAC system which removed 20-40% TCE of the feed during the 170d treatment run. Using a GAC with a high TCE capacity ensured the treatment performance during the start-up stage and/or under the shock loading conditions. The TCE removal rate was dependent on the phenol concentration of the feed; a higher than the optimum concentration of phenol would cause competitive inhibition while too low a concentration would result in reduced rate of TCE degradation; up to 40% TCE removal was obtained in treating a feed of 2-4mg/L of phenol and a phenol/TCE loading ratio of 15. Based on the mechanism of cometabolism in the TCE-phenol system, sequential feeding of phenol (2h) and TCE (22h), which avoided competitive inhibition in the BAC and thus would enhanced the growth rate and activity of the TCE degraders, was employed to acheive a better treatment performance of 65% TCE removal (influent concentration=200ug/L) with a substantially higher max removal of 72% (0.39g/m3/h).
TCE can be anaerobically dechlorinated to dichloroethylene, vinyl chloride and ethylene. In treating an influent with 2-10mg/L of TCE under a hydraulic retention time of 6h, the addition of the commercial SDC-9 bacteria to the anaerobic granular sludge in an EGSB bioreactor enhanced its performance with a faster start-up and a stable higher TCE removal of about 85%(max removal capability=1.5g/m3/h). More ethylene was produced in a longer treatment time when the EGSB treatment was conducted in the sequential mode. The results also have demonstrated that anerobic granular sludge was a good medium for retaining and growing the supplemented active bacteria which enabled the outstanding long term stable TCE removal of the EGSB process.
Inoculation of SDC-9 accomplished rapid start-up of the BTF process; operating at an empty bed residence time of 12min, more than 99% of TCE was removed from the nitrogen influent (feed concentration=700mg/m3) with an outstanding TCE removal capability of up to 9.0g/m3/h; the bed plugging and other operating problems which would adversely affect the excellent treatment performance were not observed during the 150d+ test period. TCE removal capability of BTF sections was dependent on the type, density and activity of the residing TCE degraders; more TCE was degraded in the front part as the treatment progressed. The TCE removal capability of an ineffective BTF (2% of the former activity associated with the 50% remaining microorganisms 60d after the treatment ended) was mostly restored 8 days after the system was restarted. For the BTF which was suspended for 28d, its TCE removal capability was basically recovered 1d after the treatment was resumed; however, a longer time was required to achieve the same degree of ethylene yield.
Overall, the results have confirmed the feasibility of the four researched processes for cost effective TCE removal from contaminated water bodies. The highly effective GAC process is the one to choose for achieving total TCE removal; the long lasting aerobic BAC process may be beneficially employed for treating a low concentration (<500μg/L) influent; the stable anaerobic EGSB process is preferred for treating a higher concentration (up to 10mg/L) influent; the high loading anaerobic BTF is the best for removing gaseous phase TCE after nitrogen stripping of TCE contaminated water body.
The features and applications of the effective GAC process and the three innovative biological TCE removal processes are presented. The adsorption study results have demonstrated that the GACs'adsorptive capacities for TCE is in the same order as their phenol number, that the capacities for TCE in pure water are reduced more by the small molecule organic consistutents of tap water relative to the larger constituents of the well water, that the efficient MCRB method can be use to conclude the essential breakthrough in about 1% of the time required by the conventional method, and that the two-adsorber-in-series mode of treatment is the key to the cost effective application of the GAC process. The BAC study results have shown the aerobic TCE degradation was achieved by cometabolism and that the sequential addition of the co-substrate (phenol) and TCE produced better TCE removal due to avoid competitive inhibition. The TCE removal capabilities of the SDC-9 enhanced anaerobic EGSB and BTF processes have been defined and that advanced molecular biology techniques can be employed to identify the type, the dechlorination genes, the population dynamics and the distribution of the TCE degraders in the treatment systems.
为评价活性炭对TCE的吸附性能,以10种不同原料制备的活性炭样品进行了TCE的平衡容量实验和连续流微型快速穿透(MCRB)实验。各种活性炭对TCE的吸附容量的排列与其苯酚值排列相同,TCE初始浓度和少量甲醇的加入不会影响活性炭的吸附容量。相比其他炭型,含有丰富中孔的煤质炭对TCE吸附容量较低,但吸附容量利用率较高,适合用于实际工艺中去除TCE；由毛竹制备而成的竹质炭,对TCE的去除量和吸附容量利用率均颇为可观,是一种值得开发的新型环保炭型。水体中的共存有机物会降低活性炭对TCE的吸附容量,其竞争吸附的程度跟水体中有机物的分子量大小分布有关。两个串联的活性炭炭床是高效低耗吸附处理工艺的关键单元,因为前置炭床的利用率能得到大幅度提升,后置炭床能保障出水达标。
好氧条件下TCE只能通过共代谢方式降解。苯酚是一种高效的共代谢基质,以活性污泥培养驯化的苯酚混合菌为TCE降解菌源,通过批式降解实验评估其对TCE的降解性能。苯酚能诱导产生氧化酶和TCE共代谢需要的能量,是TCE共降解过程中必不可少的共代谢基质；TCE的大幅度降解要在苯酚基本利用后才会发生。通过接种驯化好的TCE降解菌,可以迅速启动BAC系统；在170天的连续运行期间,BAC对TCE的去除率维持在20-40%。使用对TCE具有高吸附量的活性炭能确保BAC工艺在运行初期和有冲击负荷情况下的高度处理效果。生长基质苯酚的进水浓度是TCE去除效率的关键因素,苯酚浓度过高会加重TCE共代谢的竞争性抑制,过低不足以维持其高效降解。苯酚浓度在2-4mg/L,苯酚/TCE进水负荷比率在15左右时,BAC对TCE的去除率最高达到40%左右。根据TCE-苯酚的共代谢降解规律,使用苯酚、TCE单独循环进水的工艺操作模式,有效避免了竞争性抑制,较好地维持了微生物的生长和降解活性,强化了TCE去除效率；在每天2h苯酚进水、22h TCE的进水情况下,TCE去除率最高为72%(进水浓度200μg/L),平均去除率达到65%,最大去除能力为0.39g/m3/h。
厌氧条件下TCE能通过还原脱氯依次转化为二氯乙烯、一氯乙烯和乙烯。利用生物强化的方法将商业脱氯菌SDC-9投入到接种颗粒污泥的厌氧EGSB反应器中,达成快速启动；进水浓度在2-10mg/L,水力停留时间在6h时,TCE的去除率为85%左右,其最大去除能力超过1.5g/m3/h。将EGSB转为序批式操作模式,延长反应时间有助于乙烯的生成。厌氧颗粒污泥是一种优良的生物载体,可以很好地负载特定降解菌并有效防止微生物脱落,从而使EGSB反应器工艺达到长期稳定降解TCE的功能。
通过接种SDC-9快速启动厌氧BTF；空床停留时间为12min时,稳定运行下的气态TCE去除率在99%以上(进气浓度为700mg/m3),终产物乙烯占到50%左右。厌氧BTF对TCE的最大去除能力达到9.0g/m3/h,显示出优越的处理性能,而且150多天的稳定运行证实了BTF不会因床层堵塞等问题造成处理性能的下降。在运行过程中,降解TCE的床层区域会逐渐转移到反应器前半部分。不同高度床层的处理性能与脱氯菌种和基因的种类、数量和活性之间存在关联性。停运60天后厌氧BTF内的微生物只剩2%的TCE降解活性,同时微生物总量减少了50%,但BTF重启后可以快速恢复TCE去除性能；停运28天和60天的厌氧BTF分别在1天和8天后基本恢复原先的TCE去除能力,但全面恢复之前的降解性能(乙烯转化率)则需要更长时间。
本课题研究了四种各具特色并有各自适用场合的TCE去除工艺。GAC工艺主要用于去除TCE轻度污染水体,达到深度净化的目的；BAC工艺持续稳定、抗冲击负荷强,能长期稳定的处理低浓度TCE(<500μg/L)水体；厌氧EGSB反应器工艺具有较高的TCE去除能力,适用于TCE严重污染水体(<10mg/L)的处理；对于需要使用气提去除水体里TCE的场合,厌氧BTF工艺可以高效去除进气中的TCE,潜在的应用前景广阔。本文的特色在于：在GAC工艺研究阶段,提出使用苯酚值可以预测活性炭对于TCE的吸附性能,丹宁酸值能表征吸附容量利用率,竞争吸附对活性炭吸附容量的影响程度跟水体中有机物的分子量大小分布有关,同时验证了MCRB测试可以准确模拟传统穿透实验,并提出一套高效低耗的GAC吸附工艺；在BAC工艺中,通过研究TCE-苯酚的共代谢降解规律,研发了新型的苯酚、TCE循环进水的BAC运行模式,有效提高了BAC工艺对TCE的降解效率；在厌氧BTF中,研究了相关菌种和特定基因在BTF不同床层高度的分布变化及随时间的迁移转换,揭示了脱氯菌群和功能基因的种类、数量和活性与BTF处理性能之间的内在关联性；同时,还对厌氧BTF在停运闲置期间微生物的TCE脱氯性能、活性和数量的变化进行了分析,并评估了反应器在长期停运后的恢复运行效果。
Along with the rapid industrial and agricultural development of the modern society, trichloroethylene (TCE) and other chlorinated hydrocarbons have entered environment due to improper disposal practices and accidental leaks resulting in serious contamination of groundwater in many parts of the world. Granular activated carbon (GAC) adsorption has often been employed for removing persistent organic pollutants (POPs) to produce a clean effluent meeting a very low discharge limit (<10μg/L); taking advantage of the concurrent biodegradation of the adsorbed POPs in many GAC adsorbers, biological activated carbon (BAC) process can be used to extend the GAC service life; expanded granular sludge bed (EGSB) process has been employed for treating influents containing high concentrations of toxic pllutants; biotrickling filter (BTF) process is capable of removing POPs from the exhaust stream of the stripping operation. This research has been conducted to determine the feasibility of the four treatment processes for removing TCE, to identify the potential applications, and to produce results useful for remediation of TCE contaminated groundwater.
Ten GAC samples of different raw materials and preparation were employed in the batch adsorption isotherm runs for measuring their TCE capacities and the continuous flow breakthrough runs for simulating the TCE removal in actual treatment applications. The GACs'adsorptive capacities for TCE were in the same order as their phenol numbers; they were not affected by the starting TCE concentration and/or the presence of small amount of methanol. The higher utilization rate found for the meso pore rich coal based GAC makes it competitive despite its relatively low TCE capacity. The GAC made from toxicant free, low cost and renewable bamboo is attractive because of its relatively high TCE capacity and availability. GACs'capacities for TCE in pure water were reduced by competitive adsorption of other organic constituents of the water samples; small organic compounds in tap water were more competitive than the NOM in the higher TOC well water sample. The MCRB data confirmed the GACs'available TCE capacities and that the serial bed treatment is desirable because most of the first absorber's capacity can be utilized for removing the pollutants.
Under the aerobic condition, TCE can be biodegraded only in the presence of a co-substrate such as phenol. Phenol can induce the production of oxidase and the energy necessary for TCE cometablism; high degree of TCE degradation would take place after most of the phenol has been biodegraded. Acclimated mixed phenol degraders originated from activated sludge were employed for the batch experiments to assess their TCE degrading capability. Inoculation of highly acclimated TCE degraders quickly established the BAC system which removed 20-40% TCE of the feed during the 170d treatment run. Using a GAC with a high TCE capacity ensured the treatment performance during the start-up stage and/or under the shock loading conditions. The TCE removal rate was dependent on the phenol concentration of the feed; a higher than the optimum concentration of phenol would cause competitive inhibition while too low a concentration would result in reduced rate of TCE degradation; up to 40% TCE removal was obtained in treating a feed of 2-4mg/L of phenol and a phenol/TCE loading ratio of 15. Based on the mechanism of cometabolism in the TCE-phenol system, sequential feeding of phenol (2h) and TCE (22h), which avoided competitive inhibition in the BAC and thus would enhanced the growth rate and activity of the TCE degraders, was employed to acheive a better treatment performance of 65% TCE removal (influent concentration=200ug/L) with a substantially higher max removal of 72% (0.39g/m3/h).
TCE can be anaerobically dechlorinated to dichloroethylene, vinyl chloride and ethylene. In treating an influent with 2-10mg/L of TCE under a hydraulic retention time of 6h, the addition of the commercial SDC-9 bacteria to the anaerobic granular sludge in an EGSB bioreactor enhanced its performance with a faster start-up and a stable higher TCE removal of about 85%(max removal capability=1.5g/m3/h). More ethylene was produced in a longer treatment time when the EGSB treatment was conducted in the sequential mode. The results also have demonstrated that anerobic granular sludge was a good medium for retaining and growing the supplemented active bacteria which enabled the outstanding long term stable TCE removal of the EGSB process.
Inoculation of SDC-9 accomplished rapid start-up of the BTF process; operating at an empty bed residence time of 12min, more than 99% of TCE was removed from the nitrogen influent (feed concentration=700mg/m3) with an outstanding TCE removal capability of up to 9.0g/m3/h; the bed plugging and other operating problems which would adversely affect the excellent treatment performance were not observed during the 150d+ test period. TCE removal capability of BTF sections was dependent on the type, density and activity of the residing TCE degraders; more TCE was degraded in the front part as the treatment progressed. The TCE removal capability of an ineffective BTF (2% of the former activity associated with the 50% remaining microorganisms 60d after the treatment ended) was mostly restored 8 days after the system was restarted. For the BTF which was suspended for 28d, its TCE removal capability was basically recovered 1d after the treatment was resumed; however, a longer time was required to achieve the same degree of ethylene yield.
Overall, the results have confirmed the feasibility of the four researched processes for cost effective TCE removal from contaminated water bodies. The highly effective GAC process is the one to choose for achieving total TCE removal; the long lasting aerobic BAC process may be beneficially employed for treating a low concentration (<500μg/L) influent; the stable anaerobic EGSB process is preferred for treating a higher concentration (up to 10mg/L) influent; the high loading anaerobic BTF is the best for removing gaseous phase TCE after nitrogen stripping of TCE contaminated water body.
The features and applications of the effective GAC process and the three innovative biological TCE removal processes are presented. The adsorption study results have demonstrated that the GACs'adsorptive capacities for TCE is in the same order as their phenol number, that the capacities for TCE in pure water are reduced more by the small molecule organic consistutents of tap water relative to the larger constituents of the well water, that the efficient MCRB method can be use to conclude the essential breakthrough in about 1% of the time required by the conventional method, and that the two-adsorber-in-series mode of treatment is the key to the cost effective application of the GAC process. The BAC study results have shown the aerobic TCE degradation was achieved by cometabolism and that the sequential addition of the co-substrate (phenol) and TCE produced better TCE removal due to avoid competitive inhibition. The TCE removal capabilities of the SDC-9 enhanced anaerobic EGSB and BTF processes have been defined and that advanced molecular biology techniques can be employed to identify the type, the dechlorination genes, the population dynamics and the distribution of the TCE degraders in the treatment systems.
引文
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