膨润土/表面活性剂一体化工艺吸附去除染化废水中的持久性有机污染物
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摘要
持久性有机污染物(POPs)广泛存在于染化废水中,如不得到有效处理,将会造成严重危害,因此,研究并控制染化废水中POPs污染至关重要。本论文采用液液萃取、固相萃取、HPLC及GC/MS等技术,建立了染化废水中POPs的分离、分析方法；以膨润土／表面活性剂一体化工艺替代聚铝絮凝工艺,探讨了一体化工艺的可行性及其对染化废水中典型POPs的去除机制；最后考察了吸附饱和后膨润土热再生的可行性。论文取得了以下有价值的研究结果：
(1)建立了染化废水中POPs的分离、分析方法,探明了废水中的POPs主要有类POPs染料、五氯苯酚、PAHs及PCBs等4大类,其浓度水平分别为50-95mg/L、15-50μg/L、800-1200ng/L和7-20ng/L。POPs染料以分散染料为主(>85%),低分子量PAHs和PCB-11是主要的PAHs和PCBs物种,并且多以吸附态存在。
(2)将膨润土／表面活性剂一体化工艺应用于大规模的染化废水处理工程,与常规絮凝工艺,染化废水中典型POPs去除率显著提高,其中类POPs染料去除率为93.6%、五氯苯酚为98.7%,PAHs为90.4%,PCBs为61.4%；同时出水的生物可生化性(B/C)从0.24提高到0.48,为后续生化处理工艺稳定运行和废水达标排放提供了有效的保障。
(3)探明了膨润土／表面活性剂一体化工艺对染化废水中典型POPs的去除机制。膨润土可以通过离子交换吸附阳离子,同时自组装成有机膨润土,再以化学吸附作用去除阴离子型POPs,以分配作用去除非离子型POPs;表面活性剂与POPs间的相互作用可以提高膨润土对其的吸附；自组装有机膨润土可以高效吸附非极性POPs。
(4)考察了吸附饱和后膨润土的热再生。最佳再生条件是450℃加热1.5h,多次再生后样品对苯胺吸附量是原土的6倍,为解决膨润土二次污染提供参考。
Persistent Organic Pollutants (POPs) widely exist in dyeing wastewater. If not effectively treated, they would cause serious harms to human beings and environments. Therefore, it is essential to study and control the POPs pollution in dyeing wastewater. Here, a method of POPs enrichment and analysis from dyeing wastewater was established by using liquid-liquid extraction, solid phase extraction, HPLC and GC/MS technologies. A bentonite/surfactant one-step process was proposed to replace the traditional PAC flocculation process in order to improve the removal efficiencies of POPs in dyeing wastewater. In this thesis, the removal of representative POPs in the one-step process was evaluated and their removal mechanism was also discussed. Additionally, the adsorbed organobentonite sludge was regenerated by theomo processing. The main valuable findings were as follows:
(1) A method of POPs enrichment and analysis from dyeing wastewater was established, and four categories of POPs species were detected, including six POPs-like dyes (disperse orange30, disperse orange62, disperse red43, vat purple1, reactive blue13and acid yellow72), pentachlorophenol, PAHs and PCBs in the range of50-95mg/L,15-50μg/L,800-1200ng/L and7-20ng/L, respectively. Disperse POPs-like dyes were the main type of dyes, accounting for more than85%. The low molecular weight PAHs and PCB-11were the major PAHs and PCBs species, and mainly adsorbed on particulates or sludges.
(2) Bentonite/surfactant one-step process was applied in the treatment of dyeing wastewater. Comparing with the traditional PAC flocculation process, the removal of representative POPs increased significantly, which were93.6%,98.7%,90.4%and61.4%for POPs-like dyes, pentachlorophenol, PAHs and PCBs, respectively. Meanwhile, biological biodegradability (B/C) increased from0.24to0.48in the effluent, which provide an effective guarantee for the stable operation of the subsequent biological treatment process and the safe discharge of wastewater.
(3) The main removal mechanism of representative POPs in dyeing wastewater by bentonite/surfactant one-step process was investigated in detail. In the bentonite/surfactant one-step process, raw bentonite can adsorb organic cations by ion exchange, and then assemble the organobentonite automatically. In the one-step process, the removal of anionic POPs from wastewater was mainly controlled by chemical adsorption, and the adsorption of nonionic POPs complied with linear sorption model, which was mainly controlled by partition. The interaction between surfactant and POPs could promote the adsorption of POPs onto the self-assembled organobentonite. Meanwhile, polar or weekly polar organic compounds could promote the adsorption of nonpolar POPs. Self-assembled organobentonite can efficiently adsorb the non-polar POPs in dyeing wastewater.
(4) Organobentonite sludge sorbing POPs was regenerated by thermo processing. The best regeneration temperature was450℃and the best time was1.5h. After several times of repeated adsorption and regeneration, the adsorption capacity of the regenerated sample for aniline was nearly six times to raw bentonite. It could be considered as an effective way to solve the secondary pollution of sludges.
(1)建立了染化废水中POPs的分离、分析方法,探明了废水中的POPs主要有类POPs染料、五氯苯酚、PAHs及PCBs等4大类,其浓度水平分别为50-95mg/L、15-50μg/L、800-1200ng/L和7-20ng/L。POPs染料以分散染料为主(>85%),低分子量PAHs和PCB-11是主要的PAHs和PCBs物种,并且多以吸附态存在。
(2)将膨润土／表面活性剂一体化工艺应用于大规模的染化废水处理工程,与常规絮凝工艺,染化废水中典型POPs去除率显著提高,其中类POPs染料去除率为93.6%、五氯苯酚为98.7%,PAHs为90.4%,PCBs为61.4%；同时出水的生物可生化性(B/C)从0.24提高到0.48,为后续生化处理工艺稳定运行和废水达标排放提供了有效的保障。
(3)探明了膨润土／表面活性剂一体化工艺对染化废水中典型POPs的去除机制。膨润土可以通过离子交换吸附阳离子,同时自组装成有机膨润土,再以化学吸附作用去除阴离子型POPs,以分配作用去除非离子型POPs;表面活性剂与POPs间的相互作用可以提高膨润土对其的吸附；自组装有机膨润土可以高效吸附非极性POPs。
(4)考察了吸附饱和后膨润土的热再生。最佳再生条件是450℃加热1.5h,多次再生后样品对苯胺吸附量是原土的6倍,为解决膨润土二次污染提供参考。
Persistent Organic Pollutants (POPs) widely exist in dyeing wastewater. If not effectively treated, they would cause serious harms to human beings and environments. Therefore, it is essential to study and control the POPs pollution in dyeing wastewater. Here, a method of POPs enrichment and analysis from dyeing wastewater was established by using liquid-liquid extraction, solid phase extraction, HPLC and GC/MS technologies. A bentonite/surfactant one-step process was proposed to replace the traditional PAC flocculation process in order to improve the removal efficiencies of POPs in dyeing wastewater. In this thesis, the removal of representative POPs in the one-step process was evaluated and their removal mechanism was also discussed. Additionally, the adsorbed organobentonite sludge was regenerated by theomo processing. The main valuable findings were as follows:
(1) A method of POPs enrichment and analysis from dyeing wastewater was established, and four categories of POPs species were detected, including six POPs-like dyes (disperse orange30, disperse orange62, disperse red43, vat purple1, reactive blue13and acid yellow72), pentachlorophenol, PAHs and PCBs in the range of50-95mg/L,15-50μg/L,800-1200ng/L and7-20ng/L, respectively. Disperse POPs-like dyes were the main type of dyes, accounting for more than85%. The low molecular weight PAHs and PCB-11were the major PAHs and PCBs species, and mainly adsorbed on particulates or sludges.
(2) Bentonite/surfactant one-step process was applied in the treatment of dyeing wastewater. Comparing with the traditional PAC flocculation process, the removal of representative POPs increased significantly, which were93.6%,98.7%,90.4%and61.4%for POPs-like dyes, pentachlorophenol, PAHs and PCBs, respectively. Meanwhile, biological biodegradability (B/C) increased from0.24to0.48in the effluent, which provide an effective guarantee for the stable operation of the subsequent biological treatment process and the safe discharge of wastewater.
(3) The main removal mechanism of representative POPs in dyeing wastewater by bentonite/surfactant one-step process was investigated in detail. In the bentonite/surfactant one-step process, raw bentonite can adsorb organic cations by ion exchange, and then assemble the organobentonite automatically. In the one-step process, the removal of anionic POPs from wastewater was mainly controlled by chemical adsorption, and the adsorption of nonionic POPs complied with linear sorption model, which was mainly controlled by partition. The interaction between surfactant and POPs could promote the adsorption of POPs onto the self-assembled organobentonite. Meanwhile, polar or weekly polar organic compounds could promote the adsorption of nonpolar POPs. Self-assembled organobentonite can efficiently adsorb the non-polar POPs in dyeing wastewater.
(4) Organobentonite sludge sorbing POPs was regenerated by thermo processing. The best regeneration temperature was450℃and the best time was1.5h. After several times of repeated adsorption and regeneration, the adsorption capacity of the regenerated sample for aniline was nearly six times to raw bentonite. It could be considered as an effective way to solve the secondary pollution of sludges.
引文
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