膜生物反应器去除水中PPCPs的效果及SRT的影响研究
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摘要
研究膜-生物反应器(MBR)对微量有机物的去除,对保障MBR出水的安全性,发掘其在污水回用领域的应用潜力有着重要作用。本研究选取10种典型药品和个人护肤品(PPCPs)为代表,研究了MBR对典型PPCPs的去除效果和去除途径。同时,考察了污泥龄(SRT)对去除效果的影响并通过间歇试验对其主要去除途径进行了深入分析。
在相似的运行条件下,对比考察了MBR和序批式活性污泥法(SBR)对PPCPs的去除效果。结果表明MBR在出水的安全性和稳定性上存在着一定的优势,对于甲氧苄氨嘧啶(Trimethoprim)和硫氰酸盐(Erythromycin)的去除,两反应器之间并无明显差别;但对于其他目标物质,尤其是咖啡因(Caffeine),酮洛芬(Ketoprofen),避蚊胺(DEET),MBR的去除率明显高于SBR。通过对目标物在两反应器中分布情况的研究,发现膜过滤过程和SBR中的沉淀过程对目标PPCPs浓度的影响都不明显,但膜过滤过程可以截留部分吸附有目标物的胶体,目标物质的在MBR和SBR中的主要去除途径均为生物降解,表观分配系数的研究给出了各目标物质污泥吸附的相对强弱。
利用膜生物反应器中的污泥进行间歇试验,进一步分析了MBR混合液对目标PPCPs的主要去除途径。研究结果表明各物质主要的去除均为生物降解,污泥吸附作用对硫氰酸盐(Erythromycin)和卡马西平(Carbamazepine)的去除无明显影响,对其他物质的去除具有一定的贡献,酮洛芬(Ketoprofen),避蚊胺(DEET)和咖啡因(Caffeine)可被污泥吸附约20%,双氯芬酸(Diclofenac)和氯贝酸(Clofibric acid)可被吸附15%左右。
通过运行4个不同SRT(5d,10d, 20d,40d)下的MBR,考察其对PPCPs去除的影响。目标物质不同,SRT对其去除的影响不同。研究结果表明,舒必利(Sulpiride)和卡马西平(Carbamazepine)在反应器中基本不能被去除,美托洛尔(Metoprolol)和避蚊胺(DEET)的去除效果基本不受SRT的影响,去除率分别为50%和80%左右,咖啡因(Caffeine),酮洛芬(Ketoprofen)和甲氧苄氨嘧啶(Trimethoprim)的去除率随SRT的增加而缓慢增加,变化幅度10%左右,氯贝酸(Clofibric acid)和双氯芬酸(Diclofenac)在SRT为20d时去除效果最佳,对于硫氰酸盐(Erythromycin),其去除率受SRT的影响较大,去除率从低于70%增大到90%以上。
Research on removal of micro-pollutants by membrane bioreactor (MBR) is needed to ensure the safety of MBR effluent and can be helpful in exploring utilization of MBR in the wastewater reclaimation process. 10 pharmaceuticals and personal care products (PPCPs) were selected as representatives of micro-pollutants in this thesis. Removal efficiency and pathway of these PPCPs by MBR were studied. The solids rention time (SRT) of MBR was changed in order to find its influence on PPCPs removal. Furthermore, batch experiments were taken to analysis the removal pathway.
To evaluate the removal of PPCPs by MBR, a MBR and a sequencing batch reactor (SBR) were operated under the same condition.The results showed that MBR was more efficient in the safty and stablity of the effluence. There was no significant difference between the two bioreactors on the removal of Trimethoprim and Erythromycin. However,The MBRs exhibited greater elimination rates for other selected PPCPs, especially Caffeine、Ketoprofen and DEET . Research on transfer pathway of PPCPs revealed that neither membrane in the MBR nor sedimentation process in the SBR can removal the targets obviously. But the membrane can withhold some investigated substances that absorted to the colloid particles. The main removal pathways of the selected substances in MBR and SBR were both biodegradion, the study on sludge-water partition coefficient (Kd) of PPCPs showed the relative intensity of sludge adsorption.
Batch experiments were conducted to analysis the mechanism of the selected PPCPs’s removal.The results showed that the mechanism for their transfer and variation was basinally biodegradation.The sludge adsorption contributed little to the removal of Erythromycin and Carbamazepine while other targets can be adsorbed partially. The proportion of Ketoprofen、DEET and Caffeine that were adsorbed by sludge was about 20% while the proportion of Diclofenac and Clofibric acid was about 15%.
The MBRs were operated at 4 different SRTs (5d, 10d, 20d, 40d) to evaluate the SRT’s impact.The results showed that neither Sulpiride nor Carbamazepine can be eliminated effectively,the removal of Metoprolol and DEET was not relative with SRT,and the removal rates of the two substances were 50% and 80% respectively. The removal rates of Caffeine、Ketoprofen and Trimethoprim increased with longer SRTs slowly,the increasing range is about 10%. Clofibric acid and Diclofenac were best eliminated at SRT=20d. Erythromycin were removed better when the SRT increased obviously, the range is from blow 70% when SRT=5d to above 90% when SRT=40d.
在相似的运行条件下,对比考察了MBR和序批式活性污泥法(SBR)对PPCPs的去除效果。结果表明MBR在出水的安全性和稳定性上存在着一定的优势,对于甲氧苄氨嘧啶(Trimethoprim)和硫氰酸盐(Erythromycin)的去除,两反应器之间并无明显差别;但对于其他目标物质,尤其是咖啡因(Caffeine),酮洛芬(Ketoprofen),避蚊胺(DEET),MBR的去除率明显高于SBR。通过对目标物在两反应器中分布情况的研究,发现膜过滤过程和SBR中的沉淀过程对目标PPCPs浓度的影响都不明显,但膜过滤过程可以截留部分吸附有目标物的胶体,目标物质的在MBR和SBR中的主要去除途径均为生物降解,表观分配系数的研究给出了各目标物质污泥吸附的相对强弱。
利用膜生物反应器中的污泥进行间歇试验,进一步分析了MBR混合液对目标PPCPs的主要去除途径。研究结果表明各物质主要的去除均为生物降解,污泥吸附作用对硫氰酸盐(Erythromycin)和卡马西平(Carbamazepine)的去除无明显影响,对其他物质的去除具有一定的贡献,酮洛芬(Ketoprofen),避蚊胺(DEET)和咖啡因(Caffeine)可被污泥吸附约20%,双氯芬酸(Diclofenac)和氯贝酸(Clofibric acid)可被吸附15%左右。
通过运行4个不同SRT(5d,10d, 20d,40d)下的MBR,考察其对PPCPs去除的影响。目标物质不同,SRT对其去除的影响不同。研究结果表明,舒必利(Sulpiride)和卡马西平(Carbamazepine)在反应器中基本不能被去除,美托洛尔(Metoprolol)和避蚊胺(DEET)的去除效果基本不受SRT的影响,去除率分别为50%和80%左右,咖啡因(Caffeine),酮洛芬(Ketoprofen)和甲氧苄氨嘧啶(Trimethoprim)的去除率随SRT的增加而缓慢增加,变化幅度10%左右,氯贝酸(Clofibric acid)和双氯芬酸(Diclofenac)在SRT为20d时去除效果最佳,对于硫氰酸盐(Erythromycin),其去除率受SRT的影响较大,去除率从低于70%增大到90%以上。
Research on removal of micro-pollutants by membrane bioreactor (MBR) is needed to ensure the safety of MBR effluent and can be helpful in exploring utilization of MBR in the wastewater reclaimation process. 10 pharmaceuticals and personal care products (PPCPs) were selected as representatives of micro-pollutants in this thesis. Removal efficiency and pathway of these PPCPs by MBR were studied. The solids rention time (SRT) of MBR was changed in order to find its influence on PPCPs removal. Furthermore, batch experiments were taken to analysis the removal pathway.
To evaluate the removal of PPCPs by MBR, a MBR and a sequencing batch reactor (SBR) were operated under the same condition.The results showed that MBR was more efficient in the safty and stablity of the effluence. There was no significant difference between the two bioreactors on the removal of Trimethoprim and Erythromycin. However,The MBRs exhibited greater elimination rates for other selected PPCPs, especially Caffeine、Ketoprofen and DEET . Research on transfer pathway of PPCPs revealed that neither membrane in the MBR nor sedimentation process in the SBR can removal the targets obviously. But the membrane can withhold some investigated substances that absorted to the colloid particles. The main removal pathways of the selected substances in MBR and SBR were both biodegradion, the study on sludge-water partition coefficient (Kd) of PPCPs showed the relative intensity of sludge adsorption.
Batch experiments were conducted to analysis the mechanism of the selected PPCPs’s removal.The results showed that the mechanism for their transfer and variation was basinally biodegradation.The sludge adsorption contributed little to the removal of Erythromycin and Carbamazepine while other targets can be adsorbed partially. The proportion of Ketoprofen、DEET and Caffeine that were adsorbed by sludge was about 20% while the proportion of Diclofenac and Clofibric acid was about 15%.
The MBRs were operated at 4 different SRTs (5d, 10d, 20d, 40d) to evaluate the SRT’s impact.The results showed that neither Sulpiride nor Carbamazepine can be eliminated effectively,the removal of Metoprolol and DEET was not relative with SRT,and the removal rates of the two substances were 50% and 80% respectively. The removal rates of Caffeine、Ketoprofen and Trimethoprim increased with longer SRTs slowly,the increasing range is about 10%. Clofibric acid and Diclofenac were best eliminated at SRT=20d. Erythromycin were removed better when the SRT increased obviously, the range is from blow 70% when SRT=5d to above 90% when SRT=40d.
引文
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2.周海东.城市污水中微量有机物的分布与迁移研究.北京:清华大学环境科学与工程,2008.
3. Salgot M, Huertas E, Weber S, et al. Wastewater reuse and risk: Definition of key objectives. Desalination, 2006, 187(1~3): 29~40
4.黄霞,曹斌,文湘华.膜-生物反应器在我国的研究与应用新进展.环境科学学报, 2008, 28(3): 416~432
5. Boyd G R, Palmeri J M, Zhang S. Pharmaceuticals and personal care products (PPCPs) and endocrine disrupting chemicals (EDCs) in stormwater canals and Bayou St. John in New Orleans, Louisiana, USA . Science of The Total Environment, 2004, 333(1-3): 137~148.
6. Swartz C H, Reddy S, Benotti M J. Steroid Estrogens, Nonylphenol Ethoxylate Metabolites, and Other Wastewater Contaminants in Groundwater Affected by a Residential Septic System on Cape Cod, MA . Environ. Sci. Technol., 2006, 40(16): 4894~4902.
7. Chen B, Xuan X, Zhu L. Distributions of polycyclic aromatic hydrocarbons in surface waters, sediments and soils of Hangzhou City, China . Water Research, 2004, 38(16): 3558~3568.
8. Stackelberg P E, Furlong E T, Meyer M T. Persistence of pharmaceutical compounds and other organic wastewater contaminants in a conventional drinking-water-treatment plant . Science of The Total Environment, 2004, 329(1-3): 99~113
9. U. S. EPA. Special report on environmental endocrine disruption: An effects assessment and analysis. Washington, DC, U.S. Environmental Protect Agency, Risk Assessment Forum, 1997. 13
10. Hutchinson T H and Pickford D B. Ecological risk assessment and testing for endocrine disruption in the aquatic environment. Toxicology, 2002, (181-182): 383~387
11. Nakada N, Komori K, Suzuki Y. Occurrence of 70 pharmaceutical and personal care products in Tone River basin in Japan. Water Sci Technol, 2007, 56(12): 133~140
12. Terzic S, Senta I, Ahel M. Occurrence and fate of emerging wastewater contaminants in Western Balkan Region. Sci Total Environ, 2008, 399(1-3): 66~77
13. ELLIS J B. Pharmaceutical and personal care products(PPCPs) in urban receiving waters.Environmental Pollution,2006,144(1):184~189.
14. Pascoe D,Karntanut W,M Ller C T.Do pharmaceuticals affect freshwater invertebrates: A study with the cnidarian hydra vulgaris . Chemosphere, 2003,51(6) :521~528.
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