焦化废水强化处理工艺特性和机理及排水生物毒性研究
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摘要
新的焦化废水排放标准正准备实施，其建议新建企业的COD和氨氮排放限值分别为50mg/L和10mg/L，但目前许多焦化企业的废水处理其COD和氨氮远不能达到现行的100mg/L和15mg/L的排放标准。因此，开展焦化废水强化处理工艺的研究，强化污染物的去除，可为新标准的实施提供技术支持。本研究为适应更严格的焦化废水处理要求，开发一种生物或化学强化处理工艺，以达到新排放标准的排放水质要求。
采用厌氧/缺氧/生物沸石-膜生物反应器（A_1/A_2/ZB-MBR）处理实际焦化废水，考察了运行参数对处理效果的影响。结果表明，在HRT为73h，回流比为2:1，ZB-MBR内溶解氧控制为4-6mg/L时，系统出水氨氮浓度为5.6±4.1mg/L，可稳定达到新排放标准的要求，但出水COD为145±27mg/L，仍不能达到新标准要求。
在ZB-MBR内投加苯酚、吡啶、喹啉、萘和咔唑等污染物的高效降解菌可有效去除焦化废水中以上难降解物质，但其出水COD仅由145mg/L下降至130mg/L左右，仍不能达到新标准。对生物强化出水进行物质分析，发现其有机物组成复杂，且每种有机物的含量均较低，其中相对含量较高的正十八烷浓度仅0.38mg/L。采用化学强化进一步降低出水COD，当混凝剂PAC投加量为120mg/L时，出水COD可降至约110mg/L，接近现有企业的排放限值；采用Fenton和电-Fenton氧化处理，出水COD稳定低于50mg/L，可满足新建企业的排放限值。
采用T-RFLP和高通量测序技术研究生物处理过程的微生物群落结构，结果表明，系统运行前期增加膜过滤促进了氨氧化菌Nitrosospira的生长；而增加沸石后，Nitrosomonas和Nitrobacter的数量明显升高，并成为ZB-MBR内氨氮转化的优势菌群。此外，投加高效菌剂后，生物强化反应器的微生物多样性和主要微生物类群的含量也明显升高。
对上述不同处理工艺的出水进行综合排水毒性测定，结果表明，A_1/A_2/ZB-MBR工艺、生物强化和混凝出水的急性和慢性毒性较低，而增加Fenton和电-Fenton化学处理后，出水的急性和慢性毒性均明显升高，说明化学强化处理会在一定程度上增大出水的生态风险，而以COD为首要控制目标所选择的处理工艺并非完全利于出水的安全排放。
A new coking wastewater discharge standard will be implemented in China, andthe COD and ammonia emission limits were recommended as50mg/L and10mg/L,respectively. However, the coking wastewater treatment in many plants could not evenreach the current COD and ammonia emission limits of100mg/L and15mg/L.Therefore, it could provide a technical support for the implementation of the newstandard to improve the coking wastewater treatment process and enhance the removalof pollutants. The purpose of this study is to explore an biologically/chemicallyenhanced treatment process for coking wastewater in order to meet the new dischargestandard.
A combined anaerobic/anoxic/bio-zeolite–membrane bioreactor (A_1/A_2/ZB-MBR)process was used to treat real coking wastewater, and the influence of operatingparameters on the treatment efficiency was investigated. The results showed that whenHRT was73h, and the reflux ratio was2:1, and the dissolved oxygen in ZB-MBR was4-6mg/L, the effluent ammonia of5.6±4.1mg/L could reach the new emission standardstably, but the effluent COD (145±27mg/L) failed to meet the new emission standard.
The recalcitrant contaminants, such as phenol, pyridine, quinoline, naphthalene,and carbazole, could be effectively removed by adding isolated strains in ZB-MBR.However, the COD removal was limited with the effluent COD of about130mg/L.Moreover, the analysis of bioaugmented effluent showed that the organic matters incoking wastewater were complex, and the concentration of each organic was low. Forexample, the concentration of octadecane was only0.38mg/L, which is proved to berelatively higher than other organics by GC/MS. Chemical treatment was conducted tofurther reduce the effluent COD. PAC coagulation could reduced the CODconcentration to about110mg/L, close to the existing emission limit. The effluent CODof Fenton and electro-Fenton oxidation was below50mg/L, which could meet the newemission limit.
The microbial community structure was investigated by T-RFLP andhigh-throughput sequencing technology. The results showed that the membrane in thesystem promoted the growth of ammonia oxidation bacteria Nitrosospira, and the number of Nitrosomonas and Nitrobacter increased significantly after the addition ofzeolite in the system. They became the dominant microorganisms for ammoniatransformation in ZB-MBR. In addition, both the microbial diversity and the number ofthe main microbial groups increased after the addition of high efficiency strains.
The determination of whole effluent toxicity for effluent of different enhancedprocesses showed that the acute and chronic toxicity of A_1/A_2/ZB-MBR andbioaugmentation effluent were low. However, Fenton and electro-Fenton treatmentincreased the acute and chronic toxicities of the effluent significantly, which indicatedthat chemically enhanced treatment may increase the ecological risk of the effluent to acertain extent. It is not always beneficial for water safety to select COD as the primarycontrol index.
采用厌氧/缺氧/生物沸石-膜生物反应器（A_1/A_2/ZB-MBR）处理实际焦化废水，考察了运行参数对处理效果的影响。结果表明，在HRT为73h，回流比为2:1，ZB-MBR内溶解氧控制为4-6mg/L时，系统出水氨氮浓度为5.6±4.1mg/L，可稳定达到新排放标准的要求，但出水COD为145±27mg/L，仍不能达到新标准要求。
在ZB-MBR内投加苯酚、吡啶、喹啉、萘和咔唑等污染物的高效降解菌可有效去除焦化废水中以上难降解物质，但其出水COD仅由145mg/L下降至130mg/L左右，仍不能达到新标准。对生物强化出水进行物质分析，发现其有机物组成复杂，且每种有机物的含量均较低，其中相对含量较高的正十八烷浓度仅0.38mg/L。采用化学强化进一步降低出水COD，当混凝剂PAC投加量为120mg/L时，出水COD可降至约110mg/L，接近现有企业的排放限值；采用Fenton和电-Fenton氧化处理，出水COD稳定低于50mg/L，可满足新建企业的排放限值。
采用T-RFLP和高通量测序技术研究生物处理过程的微生物群落结构，结果表明，系统运行前期增加膜过滤促进了氨氧化菌Nitrosospira的生长；而增加沸石后，Nitrosomonas和Nitrobacter的数量明显升高，并成为ZB-MBR内氨氮转化的优势菌群。此外，投加高效菌剂后，生物强化反应器的微生物多样性和主要微生物类群的含量也明显升高。
对上述不同处理工艺的出水进行综合排水毒性测定，结果表明，A_1/A_2/ZB-MBR工艺、生物强化和混凝出水的急性和慢性毒性较低，而增加Fenton和电-Fenton化学处理后，出水的急性和慢性毒性均明显升高，说明化学强化处理会在一定程度上增大出水的生态风险，而以COD为首要控制目标所选择的处理工艺并非完全利于出水的安全排放。
A new coking wastewater discharge standard will be implemented in China, andthe COD and ammonia emission limits were recommended as50mg/L and10mg/L,respectively. However, the coking wastewater treatment in many plants could not evenreach the current COD and ammonia emission limits of100mg/L and15mg/L.Therefore, it could provide a technical support for the implementation of the newstandard to improve the coking wastewater treatment process and enhance the removalof pollutants. The purpose of this study is to explore an biologically/chemicallyenhanced treatment process for coking wastewater in order to meet the new dischargestandard.
A combined anaerobic/anoxic/bio-zeolite–membrane bioreactor (A_1/A_2/ZB-MBR)process was used to treat real coking wastewater, and the influence of operatingparameters on the treatment efficiency was investigated. The results showed that whenHRT was73h, and the reflux ratio was2:1, and the dissolved oxygen in ZB-MBR was4-6mg/L, the effluent ammonia of5.6±4.1mg/L could reach the new emission standardstably, but the effluent COD (145±27mg/L) failed to meet the new emission standard.
The recalcitrant contaminants, such as phenol, pyridine, quinoline, naphthalene,and carbazole, could be effectively removed by adding isolated strains in ZB-MBR.However, the COD removal was limited with the effluent COD of about130mg/L.Moreover, the analysis of bioaugmented effluent showed that the organic matters incoking wastewater were complex, and the concentration of each organic was low. Forexample, the concentration of octadecane was only0.38mg/L, which is proved to berelatively higher than other organics by GC/MS. Chemical treatment was conducted tofurther reduce the effluent COD. PAC coagulation could reduced the CODconcentration to about110mg/L, close to the existing emission limit. The effluent CODof Fenton and electro-Fenton oxidation was below50mg/L, which could meet the newemission limit.
The microbial community structure was investigated by T-RFLP andhigh-throughput sequencing technology. The results showed that the membrane in thesystem promoted the growth of ammonia oxidation bacteria Nitrosospira, and the number of Nitrosomonas and Nitrobacter increased significantly after the addition ofzeolite in the system. They became the dominant microorganisms for ammoniatransformation in ZB-MBR. In addition, both the microbial diversity and the number ofthe main microbial groups increased after the addition of high efficiency strains.
The determination of whole effluent toxicity for effluent of different enhancedprocesses showed that the acute and chronic toxicity of A_1/A_2/ZB-MBR andbioaugmentation effluent were low. However, Fenton and electro-Fenton treatmentincreased the acute and chronic toxicities of the effluent significantly, which indicatedthat chemically enhanced treatment may increase the ecological risk of the effluent to acertain extent. It is not always beneficial for water safety to select COD as the primarycontrol index.
引文
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