共代谢MBR处理甲基硫醇锡废水的试验研究
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摘要
甲基硫醇锡热稳定剂因其稳定性高、互溶性好而成为当前PVC制品的一种最重要的稳定剂，但其生产过程中产生的废水含有大量氨氮、有机锡、有机硫等有毒有害物质，其造成的环境污染也越来越受到人们的关注。目前对甲基硫醇锡废水的处理工艺并不成熟，探索出一条稳定、有效的处理工艺就显得尤为必要。本课题以081基地生产甲基硫醇锡过程中产生的废水为研究对象，由于其为高浓度、有毒、生物难降解污水，不能直接对其采用生化处理，故本实验主要研究经一系列预处理后废水的好氧可生化性。将共代谢与膜生物反应器(MBR)结合来处理预处理后的水，就处理过程中有机污染物去除特性、污泥特性的变化、膜污染过程及机理、膜清洗方法展开了研究。此外，还采用了间歇反应器(FBR)法评价废水的好氧可生化性，在短时间内达到对废水特性的进一步了解，指导实际生化处理。试验结果表明：
将原有FBR法的连续进水改为间歇进水，测定项目由测OUR改为测COD，原有的FBR法是整个实验过程全进废水样，而本研究采用前80min进淀粉溶液，后100min进废水。通过以上的改进以及FBR法对光臭氧，Fenton，脱硫，铁炭内电解以及活性炭吸附等预处理后废水好氧可生化性的评价，以及MBR运行试验对其结果的验证。得出FBR法可以在相同的污泥特性，相同的实验条件下评价比较不同废水的好氧可生化性；而单独地评价一种废水的好氧可生化性，污泥特性的不同对其可生化性结论并无影响。
采用共代谢MBR对吹脱后水进行处理时，外加碳源(麦粉)COD与废水COD之比依次在5／1，2／1，1／1条件下运行，处理效果逐渐变差，生物去除率由最初的60％左右，降到了最后的-84％，主要因为大量难降解有机物积累在膜区，微生物受抑制所致。
MBR反应器在不排泥的情况下运行，运行期间污泥浓度基本维持在8.6～9.2g／L之间，评价污泥活性的指标VSS／SS在0.64～0.72之间。污泥沉降比为100／100，几乎不沉降，主要由于毒性物质积累，污泥特性变差所致。
将污泥浓度由最初的1～3g／L提高到8～9g／L时，膜通量下降的速率变快，膜清洗更为频繁，说明污泥浓度越大，膜污染越迅速越严重。采用终端过滤器对膜面污染阻力进行分析，得出在膜固有阻力和内部污染阻力近似为0的情况下，沉积层阻力是造成膜污染的主要污染阻力，且此阻力主要由上清液中物质沉积造成。
振荡1min只能将膜通量提高60％左右，且在仅仅80min后膜通量就衰减了30％多，而化学清洗不但可以将膜通量恢复到90％以上，还在膜污染相对严重时使运行持续了20天左右。化学清洗时依次采用酸，碱，氧化剂对膜进行清洗，HCL清洗后通量恢复指数为0.86～0.97，NaOH清洗后通量恢复指数为0.98～1.13，NaCLO清洗后通量恢复指数为1.15～1.42，相对于前一种溶液清洗后，后一种溶液的清洗总能使膜通量有进一步的提高，这说明化学清洗时酸洗，碱洗以及氧化剂清洗同时采用比单独采用效果好。其中通量恢复指数大于1，主要由于实验采用的旧膜，之前对其的清洗不彻底造成。
Methyltin mercaptide is one of the most important heat stabilizer for PVC products for its high stability and dissolvability. However, the wastewater generated from methyltin mercaptide's production process consists of large quantities of organic pollutants, ammoniacal nitrogen and toxic substance, such as organotin and organic sulfur, and the pollution caused by the wastewater has drawn more and more attentions. At present, the method for methyltin mercaptide wastewater treatment is immature. It is necessary to explore a stable and effective method to treat the wastewater. The wasterwater got from methyltin mercaptide production process of 081 base can't be treated by biochemical plants directly for its high concentration of organics, toxicity and bad biorefractory. Therefore, this experiment mainly studied pretreated wastewater's aerobic biodegradability. Cometabolism and membrane bioreactor (MBR) are combined to treat the pretreated wastewater by different method. A series of research were carried on based on removal effect of the organic contaminants, changing of sludge characteristic, membrane fouling process and mechanism and membrane washing method. Furthermore, fitful bioreactor (FBR) is used to evaluate aerobic biodegradability of the wastewater in order to know wastewater's characteristic in a relatively short time to instruct biochemical treatment. Experimental results showed:
The biodegradations of effluents from MBR, UV-03, Fenton, internal electrolysis and adsorption were evaluated by the innovative FBR, measuring COD instead of OUR, whose influent is a intermittent mixture of a starch solution in the first 80 minutes and the 081 wastewater in the later 100 minutes. And It was concluded that FBR could be used to evaluate the aerobic biodegradations of different waters of different qualities under the same condition of sludge characteristics and experimental conditions. When it was used to evaluate the aerobic biodegradation of a single water, the sludge characteristics influent little on the result got from the FBR.
When the COD ratio of additional carbon and wastewater varies from 5/1 to 1/1, removal rate of pollutants is not ideal in every single condition and declined gradually from 60% to -84% because the accumalation of toxic substances make the micoorganisms inhibited.
When the MBR is operating normally without sludge discharge, sludge concentration is 8.6～9.2g/L, VSS/SS is in a low level between 0.64 and 0.72, and SV is 100/100 because the accumalation of toxic substances make the sludge characteristic bad.
The membrane fouling became more serious when the slugde concentration gets higher. The accumalation of toxic substances in the reactor worsen the sludge property and contributes a lot to the membrane fouling. Sedmentary deposit resistance is the main pollute resistance in membrance fouling process and mainly caused by these substances which exist in supernatant.
Compared with physical washing, chemical washing can improve membrane's filtration capability thoroughly whose life-span is longer. 1 minute' osillation could increase the flux by 60% but declined 30% after 80 minutes' operation. While the chemical washing could increase the flux by 60%, and had performed normally for 20 days with quite a serious membrane fouling. Chemical washing was carried out in the sequence of acid liquor, lye and oxidizer whose flux recovering indexes were respectively 0.86-0.97, 0.98-1.13, 1.15-1.42. A better washing result can be obtained in the combination of lye, acid liquor and oxidizer than applying only one of them. More than 100% of the flux was recovered because the old membrane was not cleaned thoroughfully.
将原有FBR法的连续进水改为间歇进水，测定项目由测OUR改为测COD，原有的FBR法是整个实验过程全进废水样，而本研究采用前80min进淀粉溶液，后100min进废水。通过以上的改进以及FBR法对光臭氧，Fenton，脱硫，铁炭内电解以及活性炭吸附等预处理后废水好氧可生化性的评价，以及MBR运行试验对其结果的验证。得出FBR法可以在相同的污泥特性，相同的实验条件下评价比较不同废水的好氧可生化性；而单独地评价一种废水的好氧可生化性，污泥特性的不同对其可生化性结论并无影响。
采用共代谢MBR对吹脱后水进行处理时，外加碳源(麦粉)COD与废水COD之比依次在5／1，2／1，1／1条件下运行，处理效果逐渐变差，生物去除率由最初的60％左右，降到了最后的-84％，主要因为大量难降解有机物积累在膜区，微生物受抑制所致。
MBR反应器在不排泥的情况下运行，运行期间污泥浓度基本维持在8.6～9.2g／L之间，评价污泥活性的指标VSS／SS在0.64～0.72之间。污泥沉降比为100／100，几乎不沉降，主要由于毒性物质积累，污泥特性变差所致。
将污泥浓度由最初的1～3g／L提高到8～9g／L时，膜通量下降的速率变快，膜清洗更为频繁，说明污泥浓度越大，膜污染越迅速越严重。采用终端过滤器对膜面污染阻力进行分析，得出在膜固有阻力和内部污染阻力近似为0的情况下，沉积层阻力是造成膜污染的主要污染阻力，且此阻力主要由上清液中物质沉积造成。
振荡1min只能将膜通量提高60％左右，且在仅仅80min后膜通量就衰减了30％多，而化学清洗不但可以将膜通量恢复到90％以上，还在膜污染相对严重时使运行持续了20天左右。化学清洗时依次采用酸，碱，氧化剂对膜进行清洗，HCL清洗后通量恢复指数为0.86～0.97，NaOH清洗后通量恢复指数为0.98～1.13，NaCLO清洗后通量恢复指数为1.15～1.42，相对于前一种溶液清洗后，后一种溶液的清洗总能使膜通量有进一步的提高，这说明化学清洗时酸洗，碱洗以及氧化剂清洗同时采用比单独采用效果好。其中通量恢复指数大于1，主要由于实验采用的旧膜，之前对其的清洗不彻底造成。
Methyltin mercaptide is one of the most important heat stabilizer for PVC products for its high stability and dissolvability. However, the wastewater generated from methyltin mercaptide's production process consists of large quantities of organic pollutants, ammoniacal nitrogen and toxic substance, such as organotin and organic sulfur, and the pollution caused by the wastewater has drawn more and more attentions. At present, the method for methyltin mercaptide wastewater treatment is immature. It is necessary to explore a stable and effective method to treat the wastewater. The wasterwater got from methyltin mercaptide production process of 081 base can't be treated by biochemical plants directly for its high concentration of organics, toxicity and bad biorefractory. Therefore, this experiment mainly studied pretreated wastewater's aerobic biodegradability. Cometabolism and membrane bioreactor (MBR) are combined to treat the pretreated wastewater by different method. A series of research were carried on based on removal effect of the organic contaminants, changing of sludge characteristic, membrane fouling process and mechanism and membrane washing method. Furthermore, fitful bioreactor (FBR) is used to evaluate aerobic biodegradability of the wastewater in order to know wastewater's characteristic in a relatively short time to instruct biochemical treatment. Experimental results showed:
The biodegradations of effluents from MBR, UV-03, Fenton, internal electrolysis and adsorption were evaluated by the innovative FBR, measuring COD instead of OUR, whose influent is a intermittent mixture of a starch solution in the first 80 minutes and the 081 wastewater in the later 100 minutes. And It was concluded that FBR could be used to evaluate the aerobic biodegradations of different waters of different qualities under the same condition of sludge characteristics and experimental conditions. When it was used to evaluate the aerobic biodegradation of a single water, the sludge characteristics influent little on the result got from the FBR.
When the COD ratio of additional carbon and wastewater varies from 5/1 to 1/1, removal rate of pollutants is not ideal in every single condition and declined gradually from 60% to -84% because the accumalation of toxic substances make the micoorganisms inhibited.
When the MBR is operating normally without sludge discharge, sludge concentration is 8.6～9.2g/L, VSS/SS is in a low level between 0.64 and 0.72, and SV is 100/100 because the accumalation of toxic substances make the sludge characteristic bad.
The membrane fouling became more serious when the slugde concentration gets higher. The accumalation of toxic substances in the reactor worsen the sludge property and contributes a lot to the membrane fouling. Sedmentary deposit resistance is the main pollute resistance in membrance fouling process and mainly caused by these substances which exist in supernatant.
Compared with physical washing, chemical washing can improve membrane's filtration capability thoroughly whose life-span is longer. 1 minute' osillation could increase the flux by 60% but declined 30% after 80 minutes' operation. While the chemical washing could increase the flux by 60%, and had performed normally for 20 days with quite a serious membrane fouling. Chemical washing was carried out in the sequence of acid liquor, lye and oxidizer whose flux recovering indexes were respectively 0.86-0.97, 0.98-1.13, 1.15-1.42. A better washing result can be obtained in the combination of lye, acid liquor and oxidizer than applying only one of them. More than 100% of the flux was recovered because the old membrane was not cleaned thoroughfully.
引文
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[2] 高俊敏，胡建英等．水环境中的有机锡污染调查．中国给水排水，2004，20(7)：25～27．
[3] Montigny C B, Lespes G, Gautier M P. Improved routine speciation of organotin compounds in environmental samples by pulsed flame photometric detection [J]. Journal of chromatographA , 2000, 896: 149～158.
[4] Gao J M, Hu J Y, Wan Y, et al. Butyltin compounds distribution in the coastal waters of Bohal Bay in China [J]. Bulletin of Environmental Contamination and Toxicology, 2004, 5: 72～76.
[5] 江桂斌．国内外有机锡污染研究现状[J]．卫生研究，2001，30(1)：1～3．
[6] Chao Y K, Maguire R J, Brown M, et al. Occurrence of organotin compounds in Canadian aquatic environment five years after the regulation of antifouling uses oftributyltin [J]. Water QualResJCanda, 1997, 32 (3): 453～521.
[7] Strmae M. Effects of triphenyltin acetate on survival hatching success, and liver ultrastructure of early life stages of zebrafish [J]. Eeotoxicol Environ Safety, 1999, 44 (1): 25～29.
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