胶团强化超滤法处理含铅废水工艺研究
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摘要
工业生产过程中会产生大量的含铅废水,而Pb~(2+)对人体危害极大,必须采取措施从废水中去除Pb~(2+)。胶团强化超滤(MEUF)工艺是一种新兴的从废水中高效去除重金属的方法,但是其存在表面活性剂用量大、渗透出水中表面活性剂含量高等问题,严重制约着其工业化应用进程,基于此,本论文采用复配体系和实现表面活性剂的回用来达到减少十二烷基硫酸钠(SDS)用量并降低出水中SDS浓度的目的。
基于SDS的MEUF工艺研究确定了25℃纯水中SDS的临界胶团浓度(CMC)为9mM。处理含Pb~(2+)浓度为5mg/L模拟废水时,最佳工艺条件为:进料液在搅拌器下搅拌30min并静止3h,进水SDS浓度为9mM,不调节溶液pH,在0.07MPa膜操作压力下采用单级无循环连续错流式操作模式运行超滤膜组件,运行时间为18min,此时MEUF各项指标达到稳定,渗透液中Pb~(2+)达到污水综合排放标准。
为了降低SDS用量,选用两种非离子表面活性剂壬基酚聚氧乙烯醚(NP10)和聚氧乙烯失水山梨醇单油酸酯(Tween80)同SDS复配,发现Tween80/SDS复配体系在表面活性剂用量较少的情况下性能优于NP10/SDS复配体系,所以确定最佳的复配体系为SDS浓度为1mM,Tween80/SDS摩尔复配比为0.05,此时胶团相对稳定,溶液Zeta电位值达到-32.23mV。实验采用化学沉淀法降低渗透液中SDS的含量,确定最佳的CaCl_2/SDS摩尔比为0.9,此时SDS去除率达到了87.62%,SDS浓度为19.18mg/L,达到了污水综合排放标准第二类污染物三级标准;采用化学沉淀再生法实现了浓缩液中SDS的沉淀和再生,在CaCl_2/SDS摩尔比为0.9时,SDS沉淀率达到89.26%,而浓缩液中Tween80和Pb~(2+)浓度基本不变,实现了浓缩液中SDS同Pb~(2+)较好的分离;确定最佳的Na_2CO_3/Ca(C_(12)H_(25)SO_4)_2摩尔比为4,此时溶液中SDS浓度达到1.285mM, Ca(C_(12)H_(25)SO_4)_2的再溶率达到91.26%;全过程SDS的再生率达到81.46%,且再生的SDS性质未变,回用于MEUF工艺的效果良好,Pb~(2+)的截留率达到99.3%。
本论文明确了不同清洗剂的作用,四种清洗剂对Pb~(2+)的清洗能力强弱顺序为NaOH>HNO_3>NaOCl>H_2O,对SDS的清洗能力强弱顺序为NaOCl>HNO_3>H_2O>NaOH,对膜的渗透通量恢复能力强弱顺序为HNO_3>H2O>NaOH>NaOCl;本论文综合四种清洗剂的特点,设计了最佳清洗流程,在基于SDS的MEUF工艺中可以实现对膜污染的完全清洗,渗透通量恢复率达到99.17%,在基于最佳复配体系的MEUF工艺中,最佳清洗流程可以使渗透通量恢复率达到87%。
A large amount of lead-containing waste water is generated in industrial process. Since Pb~(2+) is harmful to human health, it is of great importance to take measures to remove Pb~(2+) from waste water. Micellar-enhanced ultrafiltration (MEUF) is an emerging technology to remove heavy metals from waste water efficiently, but there are still some disadvantages seriously restricting their industrial application process. For instance, a large amount of surfactant is needed in the process, and the concentration of surfactant is still very high. Therefore, mixed surfactants were used to reduce the use of Sodium Dodecyl Sulfate (SDS) and the concentration of SDS in effluent in this paper.
In SDS-based MEUF process, the critical micelle concentration (CMC) of SDS is identified as 9mM in the water at 25℃. In the treatment of lead-containing waste water with the concentration of 5mg/L, the optimum condition was shown that the feed solution was firstly stirred for 30min and kept still for 3h, the concentration of SDS in feed solution set as 9mM, pH value not adjusted, and the feed solution was filtered through ultrafiltration membrane module using single-stage loop-free continuous cross-flow operation mode at 0.07 MPa. After 18min operation, every factors of MEUF process reached stable, and the concentration of Pb~(2+) in permeate solution met the sewage discharge standards.
In order to reduce the use of SDS, two kinds of nonionic surfactants, polyxyethylene nonyl phenyl ether (NP10) and polyoxyethylene sorbitan monooleate (Tween80) were used to mix with SDS. The results shown that the performance of Tween80/SDS mixed micellar system was better than that of NP10/SDS mixed micellar system in the case of using fewer amounts of surfactants. Therefore the optimal mixed micellar system was selected: the concentration of SDS was 1mM and the mole ratio of Tween80 and SDS was 0.05. The Zeta potential was -32.23mV under the optimum mole ratio of Tween80 and SDS condition and the micelles were stable at that moment.
Chemical precipitation method was used to reduce the use of SDS in the permeate solution. The results indicated that the optimal mole ratio of CaCl_2 and SDS was 0.9, then the precipitation efficiency of SDS reached 87.62%, and the concentration of SDS in permeate solution was 19.18mg/L, which met the third grade standard of wastewater discharge standards of the second type of pollutants. Chemical precipitation-regeneration method was used to recover SDS from retentate solution. When the molar ratio of CaCl_2 and SDS was 0.9, the precipitation efficiency of SDS was 89.26%, and the concentration of Tween80 and Pb~(2+) were unchanged essentially. SDS and Pb~(2+) in retentate solution were effectively separated. When the optimal mole ratio of Na2CO_3 and Ca(C_(12)H_(25)SO_4)_2 was selected as 4, the concentration of SDS in permeate solution was 1.285mM, and the redissolution percent of SDS was 91.26%. In the whole process, the recover efficiency of SDS was 81.46%, and the performance of regenerated SDS did not change. The regenerated SDS could be used in MEUF process again, and the retention rate of Pb~(2+) could reach 99.3%.
The function of different cleaning agents was revealed. The order for cleaning Pb~(2+) was NaOH>HNO_3>NaOCl>H_2O, the order for cleaning SDS was NaOCl> HNO_3> H2O> NaOH, and the order for the flux recovery was HNO_3> H_2O> NaOH> NaOCl. The optimal cleaning process was designed based on the characteristics of four cleaning agents. In SDS-based MEUF process, the fouled membrane could be completely regenerated by the cleaning process and the flux could be recovered to 99.17%, while in mixed micellar system, the flux could be recovered to 87%.
基于SDS的MEUF工艺研究确定了25℃纯水中SDS的临界胶团浓度(CMC)为9mM。处理含Pb~(2+)浓度为5mg/L模拟废水时,最佳工艺条件为:进料液在搅拌器下搅拌30min并静止3h,进水SDS浓度为9mM,不调节溶液pH,在0.07MPa膜操作压力下采用单级无循环连续错流式操作模式运行超滤膜组件,运行时间为18min,此时MEUF各项指标达到稳定,渗透液中Pb~(2+)达到污水综合排放标准。
为了降低SDS用量,选用两种非离子表面活性剂壬基酚聚氧乙烯醚(NP10)和聚氧乙烯失水山梨醇单油酸酯(Tween80)同SDS复配,发现Tween80/SDS复配体系在表面活性剂用量较少的情况下性能优于NP10/SDS复配体系,所以确定最佳的复配体系为SDS浓度为1mM,Tween80/SDS摩尔复配比为0.05,此时胶团相对稳定,溶液Zeta电位值达到-32.23mV。实验采用化学沉淀法降低渗透液中SDS的含量,确定最佳的CaCl_2/SDS摩尔比为0.9,此时SDS去除率达到了87.62%,SDS浓度为19.18mg/L,达到了污水综合排放标准第二类污染物三级标准;采用化学沉淀再生法实现了浓缩液中SDS的沉淀和再生,在CaCl_2/SDS摩尔比为0.9时,SDS沉淀率达到89.26%,而浓缩液中Tween80和Pb~(2+)浓度基本不变,实现了浓缩液中SDS同Pb~(2+)较好的分离;确定最佳的Na_2CO_3/Ca(C_(12)H_(25)SO_4)_2摩尔比为4,此时溶液中SDS浓度达到1.285mM, Ca(C_(12)H_(25)SO_4)_2的再溶率达到91.26%;全过程SDS的再生率达到81.46%,且再生的SDS性质未变,回用于MEUF工艺的效果良好,Pb~(2+)的截留率达到99.3%。
本论文明确了不同清洗剂的作用,四种清洗剂对Pb~(2+)的清洗能力强弱顺序为NaOH>HNO_3>NaOCl>H_2O,对SDS的清洗能力强弱顺序为NaOCl>HNO_3>H_2O>NaOH,对膜的渗透通量恢复能力强弱顺序为HNO_3>H2O>NaOH>NaOCl;本论文综合四种清洗剂的特点,设计了最佳清洗流程,在基于SDS的MEUF工艺中可以实现对膜污染的完全清洗,渗透通量恢复率达到99.17%,在基于最佳复配体系的MEUF工艺中,最佳清洗流程可以使渗透通量恢复率达到87%。
A large amount of lead-containing waste water is generated in industrial process. Since Pb~(2+) is harmful to human health, it is of great importance to take measures to remove Pb~(2+) from waste water. Micellar-enhanced ultrafiltration (MEUF) is an emerging technology to remove heavy metals from waste water efficiently, but there are still some disadvantages seriously restricting their industrial application process. For instance, a large amount of surfactant is needed in the process, and the concentration of surfactant is still very high. Therefore, mixed surfactants were used to reduce the use of Sodium Dodecyl Sulfate (SDS) and the concentration of SDS in effluent in this paper.
In SDS-based MEUF process, the critical micelle concentration (CMC) of SDS is identified as 9mM in the water at 25℃. In the treatment of lead-containing waste water with the concentration of 5mg/L, the optimum condition was shown that the feed solution was firstly stirred for 30min and kept still for 3h, the concentration of SDS in feed solution set as 9mM, pH value not adjusted, and the feed solution was filtered through ultrafiltration membrane module using single-stage loop-free continuous cross-flow operation mode at 0.07 MPa. After 18min operation, every factors of MEUF process reached stable, and the concentration of Pb~(2+) in permeate solution met the sewage discharge standards.
In order to reduce the use of SDS, two kinds of nonionic surfactants, polyxyethylene nonyl phenyl ether (NP10) and polyoxyethylene sorbitan monooleate (Tween80) were used to mix with SDS. The results shown that the performance of Tween80/SDS mixed micellar system was better than that of NP10/SDS mixed micellar system in the case of using fewer amounts of surfactants. Therefore the optimal mixed micellar system was selected: the concentration of SDS was 1mM and the mole ratio of Tween80 and SDS was 0.05. The Zeta potential was -32.23mV under the optimum mole ratio of Tween80 and SDS condition and the micelles were stable at that moment.
Chemical precipitation method was used to reduce the use of SDS in the permeate solution. The results indicated that the optimal mole ratio of CaCl_2 and SDS was 0.9, then the precipitation efficiency of SDS reached 87.62%, and the concentration of SDS in permeate solution was 19.18mg/L, which met the third grade standard of wastewater discharge standards of the second type of pollutants. Chemical precipitation-regeneration method was used to recover SDS from retentate solution. When the molar ratio of CaCl_2 and SDS was 0.9, the precipitation efficiency of SDS was 89.26%, and the concentration of Tween80 and Pb~(2+) were unchanged essentially. SDS and Pb~(2+) in retentate solution were effectively separated. When the optimal mole ratio of Na2CO_3 and Ca(C_(12)H_(25)SO_4)_2 was selected as 4, the concentration of SDS in permeate solution was 1.285mM, and the redissolution percent of SDS was 91.26%. In the whole process, the recover efficiency of SDS was 81.46%, and the performance of regenerated SDS did not change. The regenerated SDS could be used in MEUF process again, and the retention rate of Pb~(2+) could reach 99.3%.
The function of different cleaning agents was revealed. The order for cleaning Pb~(2+) was NaOH>HNO_3>NaOCl>H_2O, the order for cleaning SDS was NaOCl> HNO_3> H2O> NaOH, and the order for the flux recovery was HNO_3> H_2O> NaOH> NaOCl. The optimal cleaning process was designed based on the characteristics of four cleaning agents. In SDS-based MEUF process, the fouled membrane could be completely regenerated by the cleaning process and the flux could be recovered to 99.17%, while in mixed micellar system, the flux could be recovered to 87%.
引文
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