电镀废（液）水综合治理与资源化利用新工艺开发研究
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摘要
本文研究了以改性剩余活性污泥对电镀废水处理的可能性,主要内容包括三部分：第一部分研究了改性剩余活性污泥对真实废水中重金属离子的吸附热力学,得到了在复杂水体中,重金属离子在活性污泥表面的吸附模型：第二部分主要研究了改性污泥对重金属废水的处理过程,探讨了污泥浓度、反应时间、系统pH值以及S2-和反应温度对重金属离子脱除率的影响；第三部分主要研究了以H2SO4对污泥中金属离子进行浸取的过程,探讨了系统pH值、液固比、反应时间对金属离子浸出率的影响,同时我们还考察了循环逆流浸取的可能性。
以经饱和石灰水改性处理后的改性剩余活性污泥为原料研究了其对真实废水中Cu2+、Ni2+、Zn2+和Cr3+的吸附性能。在给定的实验条件下,改性剩余活性污泥对Cu2+、Ni2+、Zn2+口Cr3+的饱和吸附量可达8.9、10.3、9.8和2.0mg/g；Cu2+和Zn2+的吸附等温线模型与Freundlich型符合的较好,Ni2+则更为符合Langmuir模型,而Cr3+却与Henry型符合较好。在实验条件下,高浓度金属离子对低浓度金属离子的吸附具有一定抑制作用。
以经消石灰改性的剩余活性污泥为原料,研究了其对电镀废水(液)处理的可能性。对于中高浓度电镀废水(液),污泥浓度、反应时间和系统pH值对去除效果有较大影响；而反应温度和S2-对去除率影响则较小。在给定的条件下,Cu2+、Ni2+、Zn2+和CrT(T代表总铬)的去除率最高可达89.0、94.08、95.98和-100%。对于中低浓度电镀废水,污泥浓度、S2-和反应时间均对去除效果有较为显著的影响；Cu2+、Ni2+、Zn2+和CrT的去除率最高可达88.58、97.13、99.31和99.88%,出水中上述四种金属离子浓度可降至5.1、2.0、0.06和0.15mg/L,出水pH值为8-9。我们同时考察了污泥的沉降性能,并讨论改性剩余污泥去除重金属离子可能的机理。
以吸附实验中产生的污泥为实验材料,研究了H2SO4对污泥中金属离子的浸出。结果发现,浸取液pH值和液固比对浸出率有较大影响,而反应时间对浸出率的影响则较小。在给定的条件下,Cu2+、Ni2+、Zn2+和CrT的浸出率最高可达98.07、99.08、98.80和95.63%。当采用循环逆流浸取工艺时,反应池不应超过三级,同时应保证其中至少两个反应池中反应液的pH值不高于2。
最后,基于实验中所获得的数据,我们开发了改性剩余活性污泥对电镀废水处理并资源化利用的新工艺。
In this paper, we investigated the possibility of electroplating wastewater treatment by modified activated sludge. There are three main contents as following: the first section is adsorption thermodynamics of modified activated sludge to heavy metal ions in real wastewater, and the models of heavy metal ions adsorption on modified activated sludge in complex wastewater system were obtained. In the second section, we considered the process of heavy metal wastewater by modified activated sludge. And sludge concentration, contact time, the pH value of system, reaction temperature and addition of S2- on the treatment effect were investigated. In the third section, we studied the leaching process of heavy metal ions containing in sludge by sulfuric acid. The pH value of system, liquid to solid ratio and reaction time on the leaching effect were discussed. Meanwhile, we researched the possibility of countercurrent leaching process.
The adsorption of Cu2+, Ni2+, Zn2+ and Cr3+ on activated sludge pretreated by saturated lime solution was investigated. Under the given condition, the saturated adsorption capacity of Cu2+, Ni2+, Zn2+ and Cr3+ on activated sludge are up to 8.9, 10.3,9.8 and 2.0mg/g. The adsorption isotherm of Cu2+ and Zn2+ are in keeping with Freundlich model, and Langmuir model is better coincidence of Ni2+ while Cr3+ agrees with Henry model. Under the experimental condition, the inhibition effect of high concentration metal ions to low was observed.
We studied the possibility of heavy metal wastewater(liquid) treatment by activated sludge pretreated by lime. For high concentration electroplating wastewater(liquid), sludge concentration, contact time and the pH value of system have notable influence on the treatment effect, while the influence of reaction temperature and addition of S2" are weaker. Under the certain factor, the highest removal rate of Cu2+, Ni2+, Zn2+ and Cr are up to 89.0,94.08,95.98 and-100%. For the low concentration electroplating wastewater, the highest removal rate of Cu2+ Ni2+, Zn2+ and Cr are 88.58,97.13,99.31 and 99.88%. The concentration of the above mentioned ions in the effluent have been reduced to 5.1,2.0,0.06 and 0.15mg/L, and the pH value is 8～9. We also investigated sludge settling characteristics, and the possible mechanism of heavy metal ions removal by modified activated sludge was discussed, too.
We considered the leaching process of metal ions containing in sludge by sulfuric acid. It is observed that the pH value of leaching solution and liquid to solid ration have notable influence on leaching rate while the reaction time get weaker influence. Under the fixed condition, the leaching rate of Cu2+, Ni2+, Zn2+ and Cr are up to 98.07,99.08,98.80 and 95.63%. When the countercurrent leaching was applied, the reactor should not be more than three, and it is necessary that at least two of the three reactor should hold the pH value of their reaction solution under two.
At last, we developed the novel technology of electroplating wastewater (liquid) treatment and utilization based on the obtained data in experiments.
以经饱和石灰水改性处理后的改性剩余活性污泥为原料研究了其对真实废水中Cu2+、Ni2+、Zn2+和Cr3+的吸附性能。在给定的实验条件下,改性剩余活性污泥对Cu2+、Ni2+、Zn2+口Cr3+的饱和吸附量可达8.9、10.3、9.8和2.0mg/g；Cu2+和Zn2+的吸附等温线模型与Freundlich型符合的较好,Ni2+则更为符合Langmuir模型,而Cr3+却与Henry型符合较好。在实验条件下,高浓度金属离子对低浓度金属离子的吸附具有一定抑制作用。
以经消石灰改性的剩余活性污泥为原料,研究了其对电镀废水(液)处理的可能性。对于中高浓度电镀废水(液),污泥浓度、反应时间和系统pH值对去除效果有较大影响；而反应温度和S2-对去除率影响则较小。在给定的条件下,Cu2+、Ni2+、Zn2+和CrT(T代表总铬)的去除率最高可达89.0、94.08、95.98和-100%。对于中低浓度电镀废水,污泥浓度、S2-和反应时间均对去除效果有较为显著的影响；Cu2+、Ni2+、Zn2+和CrT的去除率最高可达88.58、97.13、99.31和99.88%,出水中上述四种金属离子浓度可降至5.1、2.0、0.06和0.15mg/L,出水pH值为8-9。我们同时考察了污泥的沉降性能,并讨论改性剩余污泥去除重金属离子可能的机理。
以吸附实验中产生的污泥为实验材料,研究了H2SO4对污泥中金属离子的浸出。结果发现,浸取液pH值和液固比对浸出率有较大影响,而反应时间对浸出率的影响则较小。在给定的条件下,Cu2+、Ni2+、Zn2+和CrT的浸出率最高可达98.07、99.08、98.80和95.63%。当采用循环逆流浸取工艺时,反应池不应超过三级,同时应保证其中至少两个反应池中反应液的pH值不高于2。
最后,基于实验中所获得的数据,我们开发了改性剩余活性污泥对电镀废水处理并资源化利用的新工艺。
In this paper, we investigated the possibility of electroplating wastewater treatment by modified activated sludge. There are three main contents as following: the first section is adsorption thermodynamics of modified activated sludge to heavy metal ions in real wastewater, and the models of heavy metal ions adsorption on modified activated sludge in complex wastewater system were obtained. In the second section, we considered the process of heavy metal wastewater by modified activated sludge. And sludge concentration, contact time, the pH value of system, reaction temperature and addition of S2- on the treatment effect were investigated. In the third section, we studied the leaching process of heavy metal ions containing in sludge by sulfuric acid. The pH value of system, liquid to solid ratio and reaction time on the leaching effect were discussed. Meanwhile, we researched the possibility of countercurrent leaching process.
The adsorption of Cu2+, Ni2+, Zn2+ and Cr3+ on activated sludge pretreated by saturated lime solution was investigated. Under the given condition, the saturated adsorption capacity of Cu2+, Ni2+, Zn2+ and Cr3+ on activated sludge are up to 8.9, 10.3,9.8 and 2.0mg/g. The adsorption isotherm of Cu2+ and Zn2+ are in keeping with Freundlich model, and Langmuir model is better coincidence of Ni2+ while Cr3+ agrees with Henry model. Under the experimental condition, the inhibition effect of high concentration metal ions to low was observed.
We studied the possibility of heavy metal wastewater(liquid) treatment by activated sludge pretreated by lime. For high concentration electroplating wastewater(liquid), sludge concentration, contact time and the pH value of system have notable influence on the treatment effect, while the influence of reaction temperature and addition of S2" are weaker. Under the certain factor, the highest removal rate of Cu2+, Ni2+, Zn2+ and Cr are up to 89.0,94.08,95.98 and-100%. For the low concentration electroplating wastewater, the highest removal rate of Cu2+ Ni2+, Zn2+ and Cr are 88.58,97.13,99.31 and 99.88%. The concentration of the above mentioned ions in the effluent have been reduced to 5.1,2.0,0.06 and 0.15mg/L, and the pH value is 8～9. We also investigated sludge settling characteristics, and the possible mechanism of heavy metal ions removal by modified activated sludge was discussed, too.
We considered the leaching process of metal ions containing in sludge by sulfuric acid. It is observed that the pH value of leaching solution and liquid to solid ration have notable influence on leaching rate while the reaction time get weaker influence. Under the fixed condition, the leaching rate of Cu2+, Ni2+, Zn2+ and Cr are up to 98.07,99.08,98.80 and 95.63%. When the countercurrent leaching was applied, the reactor should not be more than three, and it is necessary that at least two of the three reactor should hold the pH value of their reaction solution under two.
At last, we developed the novel technology of electroplating wastewater (liquid) treatment and utilization based on the obtained data in experiments.
引文
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[11]KilIc, M.; Keskin, M. E.; Mazlum, S.; Mazlum, N., Hg(Ⅱ) and Pb(Ⅱ) adsorption on activated sludge biomass:Effective biosorption mechanism. International Journal of Mineral Processing 2008,87(1-2),1-8
[12]Comte, S.; Guibaud, G.; Baudu, M., Relations between extraction protocols for activated sludge extracellular polymeric substances (EPS) and complexation properties of Pb and Cd with EPS:Part Ⅱ. Consequences of EPS extraction methods on Pb2+ and Cd2+ complexation. Enzyme and Microbial Technology 2006,38 (1-2),246-252
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[1]陈纯.污泥对重金属离子吸附的研究及其对高盐度废水的处理[D].[硕士学位论文].郑州：郑州大学,2005
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[3]Wang, X.; Chen, L.; Xia, S.; Zhao, J.; Chovelon, J.-M.; Renault, N. J., Biosorption of Cu(Ⅱ) and Pb(Ⅱ) from aqueous solutions by dried activated sludge. Minerals Engineering 2006,19 (9), 968-971.
[4]Comte, S.; Guibaud, G.; Baudu, M., Biosorption properties of extracellular polymeric substances (EPS) towards Cd, Cu and Pb for different pH values. Journal of Hazardous Materials 2008,151(1),185-193.
[5]Pagnanelli, F.; Mainelli, S.; Bornoroni, L.; Dionisi, D.; Toro, L., Mechanisms of heavy-metal removal by activated sludge. Chemosphere 2009,75 (8),1028-1034.
[6]Hammaini, A.; Gonzalez, F.; Ballester, A.; Blazquez, M. L.; Munoz, J. A., Biosorption of heavy metals by activated sludge and their desorption characteristics. Journal of Environmental Management 2007,84 (4),419-426.
[7]Al-Qodah, Z., Biosorption of heavy metal ions from aqueous solutions by activated sludge. Desalination 2006,196(1-3),164-176.
[8]环境保护部.GB21900-2008电镀污染物排放标准[S].北京：中国标准出版社,2008
[9]You, S.-J.; Tsai, Y.-P.; Huang, R.-Y., Effect of heavy metals on nitrification performance in different activated sludge processes. Journal of Hazardous Materials 2009,165 (1-3),987-994.
[10]段晓飞.配合态重金属离子对活性污泥生长影响的研究[D].[硕士学位论文].郑州：郑州大学,2011
[1]Luo, S.-1.; Yuan, L.; Chai, L.-y.; Min, X.-b.; Wang, Y.-y.; Fang, Y.; Wang, P., Biosorption behaviors of Cu2+, Zn2+, Cd2+ and mixture by waste activated sludge. Transactions of Nonferrous Metals Society of China 2006,16 (6),1431-1435.
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[1]陈诵英主编.吸附与催化[M].郑州：河南科学技术出版社,2001.1-25
[2]Luo, S.-1.; Yuan, L.; Chai, L.-y.; Min, X.-b.; Wang, Y.-y.; Fang, Y.; Wang, P., Biosorption behaviors of Cu2+, Zn2+, Cd2+ and mixture by waste activated sludge. Transactions of Nonferrous Metals Society of China 2006,16 (6),1431-1435.
[3]Wang, X.; Chen, L.; Xia, S.; Zhao, J.; Chovelon, J.-M.; Renault, N. J., Biosorption of Cu(Ⅱ) and Pb(Ⅱ) from aqueous solutions by dried activated sludge. Minerals Engineering 2006,19 (9), 968-971.
[4]Al-Qodah, Z., Biosorption of heavy metal ions from aqueous solutions by activated sludge. Desalination 2006,196 (1-3),164-176.
[5]Hammaini, A.; Gonzalez, F.; Ballester, A.; Blazquez, M. L.; Munoz, J. A., Biosorption of heavy metals by activated sludge and their desorption characteristics. Journal of Environmental Management 2007,84 (4),419-426.
[6]Aksu, Z.; AcIkel, U.; Kabasakal, E.; Tezer, S., Equilibrium modelling of individual and simultaneous biosorption of chromium(Ⅵ) and nickel(Ⅱ) onto dried activated sludge. Water Research 2002,36 (12),3063-3073.
[7]陈纯.污泥对重金属离子吸附的研究及其对高盐度废水的处理[D].[硕士学位论文].郑州：郑州大学,2005
[8]张哲.活性污泥对水体中有机污染物吸附性能的研究[D].[硕士学位论文].郑州：郑州大学,2002
[9]Comte, S.; Guibaud, G.; Baudu, M., Biosorption properties of extracellular polymeric substances (EPS) towards Cd, Cu and Pb for different pH values. Journal of Hazardous Materials 2008,151(1),185-193
[10]Guibaud, G.; Bordas, F.; Saaid, A.; D'Abzac, P.; Van Hullebusch, E., Effect of pH on cadmium and lead binding by extracellular polymeric substances (EPS) extracted from environmental bacterial strains. Colloids and Surfaces B:Biointerfaces 2008,63 (1),48-54
[11]KilIc, M.; Keskin, M. E.; Mazlum, S.; Mazlum, N., Hg(Ⅱ) and Pb(Ⅱ) adsorption on activated sludge biomass:Effective biosorption mechanism. International Journal of Mineral Processing 2008,87(1-2),1-8
[12]Comte, S.; Guibaud, G.; Baudu, M., Relations between extraction protocols for activated sludge extracellular polymeric substances (EPS) and complexation properties of Pb and Cd with EPS:Part Ⅱ. Consequences of EPS extraction methods on Pb2+ and Cd2+ complexation. Enzyme and Microbial Technology 2006,38 (1-2),246-252
[13]Loaec, M.; Olier, R.; Guezennec, J., Uptake of lead, cadmium and zinc by a novel bacterial exopolysaccharide. Water Research 1997,31 (5),1171-1179.
[14]Bhaskar, P. V.; Bhosle, N. B., Bacterial extracellular polymeric substance (EPS):A carrier of heavy metals in the marine food-chain. Environment International 2006,32 (2),191-198
[15]Pagnanelli, F.; Mainelli, S.; Bornoroni, L.; Dionisi, D.; Toro, L., Mechanisms of heavy-metal removal by activated sludge. Chemosphere 2009,75 (8),1028-1034.
[1]陈纯.污泥对重金属离子吸附的研究及其对高盐度废水的处理[D].[硕士学位论文].郑州：郑州大学,2005
[2]Luo, S.-1.; Yuan, L.; Chai, L.-y.; Min, X.-b.; Wang, Y.-y.; Fang, Y.; Wang, P., Biosorption behaviors of Cu2+, Zn2+, Cd2+ and mixture by waste activated sludge. Transactions of Nonferrous Metals Society of China 2006,16 (6),1431-1435.
[3]Wang, X.; Chen, L.; Xia, S.; Zhao, J.; Chovelon, J.-M.; Renault, N. J., Biosorption of Cu(Ⅱ) and Pb(Ⅱ) from aqueous solutions by dried activated sludge. Minerals Engineering 2006,19 (9), 968-971.
[4]Comte, S.; Guibaud, G.; Baudu, M., Biosorption properties of extracellular polymeric substances (EPS) towards Cd, Cu and Pb for different pH values. Journal of Hazardous Materials 2008,151(1),185-193.
[5]Pagnanelli, F.; Mainelli, S.; Bornoroni, L.; Dionisi, D.; Toro, L., Mechanisms of heavy-metal removal by activated sludge. Chemosphere 2009,75 (8),1028-1034.
[6]Hammaini, A.; Gonzalez, F.; Ballester, A.; Blazquez, M. L.; Munoz, J. A., Biosorption of heavy metals by activated sludge and their desorption characteristics. Journal of Environmental Management 2007,84 (4),419-426.
[7]Al-Qodah, Z., Biosorption of heavy metal ions from aqueous solutions by activated sludge. Desalination 2006,196(1-3),164-176.
[8]环境保护部.GB21900-2008电镀污染物排放标准[S].北京：中国标准出版社,2008
[9]You, S.-J.; Tsai, Y.-P.; Huang, R.-Y., Effect of heavy metals on nitrification performance in different activated sludge processes. Journal of Hazardous Materials 2009,165 (1-3),987-994.
[10]段晓飞.配合态重金属离子对活性污泥生长影响的研究[D].[硕士学位论文].郑州：郑州大学,2011
[1]Luo, S.-1.; Yuan, L.; Chai, L.-y.; Min, X.-b.; Wang, Y.-y.; Fang, Y.; Wang, P., Biosorption behaviors of Cu2+, Zn2+, Cd2+ and mixture by waste activated sludge. Transactions of Nonferrous Metals Society of China 2006,16 (6),1431-1435.
[2]Bhaskar, P. V.; Bhosle, N. B., Bacterial extracellular polymeric substance (EPS):A carrier of heavy metals in the marine food-chain. Environment International 2006,32 (2),191-198
[3]Pagnanelli, F.; Mainelli, S.; Bornoroni, L.; Dionisi, D.; Toro, L., Mechanisms of heavy-metal removal by activated sludge. Chemosphere 2009,75 (8),1028-1034.