强化膜生物反应器除磷性能及磷回收试验研究
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摘要
污水中的磷未经有效处理是造成水体富营养化的主要原因,同时使磷这种不可再生资源流失。膜生物反应器具有良好的除污染性能和优良的出水水质而被认为是现有城市污水处理工艺的替代工艺,然而,它却存在着除磷效率低的问题。因此,开展强化膜生物反应器除磷和磷回收试验研究具有重要的意义。
试验首先考察了复合式膜生物反应器(HMBR工艺)处理生活污水的净化效能。该工艺稳定运行时对COD、氨氮、SS的去除率都在90%以上,对总氮也有40%左右的去除率,但对磷的去除效果不理想。采用化学混凝预处理可以使MBR工艺出水TP低于1mg/L,相对于协同投药,前置投药能够取得更好的除磷效果。除磷混凝药剂的筛选试验结果表明,以硫酸铝作为混凝剂,同时投加不超过20mg/L的氢氧化钙为最佳的投药方式,并且处理后水pH值波动不大。
试验重点考察了污泥外循环—复合式膜生物反应器(ERP-HMBR工艺)的除污染性能。在稳定运行的情况下,ERP-HMBR工艺对COD和氨氮的去除率都在90%以上,对总氮的去除率在70%左右。外循环污泥的释磷程度决定了工艺对总磷的去除效果,当外循环污泥释磷充分时,工艺对磷的去除率稳定在80%以上;当外循环污泥释磷受到抑制时,工艺对磷的去除率下降至60%左右。污泥厌氧释磷的最佳时间为1.5~2.0h;以乙酸钠作为释磷碳源时,污泥每释放1mmol的磷大约需要消耗1.048mmol的乙酸钠。
根据ERP-HMBR工艺在污泥外循环过程中会产生少量富含磷的污水这一特征,设计烧杯试验考察了人工配制的富磷污水磷回收过程中的影响因素。在以鸟粪石沉淀为主要产物的磷回收过程中,最佳pH值随着初始磷浓度的增加而逐渐降低,并最终稳定在8.5左右,当pH值在不超过9时,磷酸镁沉淀副产物对鸟粪石沉淀过程的干扰可以忽略;当初始磷浓度低于35mg/L时不建议采用以鸟粪石形态对磷进行回收;当[Mg~(2+)]:[NH_3-N]:[P]由1:1:1逐渐增加至为2:2:1时,磷的回收率由33.2%增加至86.8%;且[NH_3-N]:[P]变化要比[Mg~(2+)]:[P]变化对磷回收率的影响严重;对于钙离子含量高的富磷污水,建议以磷酸钙盐的形式回收其中的磷。在以磷酸钙盐沉淀为主要形态的磷回收试验过程中,磷回收的最佳pH值随着初始磷浓度的增加而逐渐降低;在最佳反应pH值条件下,磷的回收率随钙磷比的增加而增加并逐渐趋于稳定,初始钙磷比在2:1以上时均能取得85%以上的磷回收率。
对磷回收产物组分分析结果表明,采用模拟废水回收的鸟粪石中各主要元素的质量百分比与理论值较为接近,采用实际废水回收的鸟粪石中钙离子的干扰使得磷、镁和氨氮的质量百分比均低于理论值;在磷酸钙盐沉淀过程中,模拟废水与实际污水的回收产物中钙磷质量百分比比较接近,且均低于理论值,磷酸钙盐沉淀中可能含有结晶水是造成钙磷质量百分比低于理论值的原因。
Much phosphorus in the treated urban wastewater causes water eutrophication and phosphorus loss. Membrane Bioreactor (MBR) is gradually used in wastewater treatment for its good performance and excellent effluent except limited phosphorus removal. So, it is significant to study enhanced MBR phosphorus removal and phosphorus reclamation simultaneously.
Firstly the effect of single Hybrid Membrane Bioreactor (HMBR) on treating domestic wastewater was studied. The removal efficiency of COD, NH4-N and SS were above 90% and TN was about 40% when the process was operated steadily.But the removal efficiency of P was bad. The chemical-coagulation pretreatment could make the TP in effluent under 1 mg/L. Pre-dosage was better than synergic dosage on phosphorus removal. The results of screening coagulant for phosphorus removal indicated that, the optimum addition method was selecting Al2(SO4)3 as coagulant and Ca(OH)2 at dosage no higher than 20mg/L, and the pH value of effluent was little fluctuating.
Secondly the effect of External Recycle of Activated Sludge Processes- Hybrid Membrane Bioreactor(ERP-HMBR) on treating domestic wastewater was studied. In the steady state, the removal efficiency of COD and NH4-N were above 90% respectively, the removal efficiency of TN was about 70%. The removal efficiency of TP was determined by the amount of phosphorus release from external recycle sludge. The removal efficiency of P was steadly above 80% when the phosphorus releas from external recycle sludge is sufficient and less of 60% when the phosphorus releas was bad. The results of effecting factor analysise indicated that, suitable anaerobic phosphorus release time was 1.5~2.0h; when acetateas was used as phosphorus release carbon resource organic substrate, 1mmol phosphorus release need about 1.048mmol acetate.
According to the characteristic that the ERP-HMBR process would produce less wastewater with higher phosphorus concentration, the impacting factors in the process of phosphorus reclamation were studied by batch tests used simulated high-phosphorus wastewater. During the reclamation process in which the main product was struvite, the best pH would gradually decrease with the increase of initial phosphorus concentration and eventually stabilized at about 8.5. If pH value was no more than 9, the disturbance of magnesium phosphorus to the struvite deposition could be neglected. If the initial phosphorus concentration was less than 35mg/L, it was not suggested toreclamation phosphorus in the form of struvite. When the ratio of [Mg~(2+)]:[NH_3-N]:[P] increase gradually from 1:1:1 to 2:2:1, the phosphorus reclamation percentage would increase from 33.2% to 86.8%. Moreover the ratio of [NH_3-N]:[P] can affect the reclamation percentage more than the ratio of [Mg~(2+)]:[P]. Phosphorus reclamation in the form of calcium phosphate was better than the form of struvite when there was much calcium ion in the wastewater. During the reclamation process in which the main product was calcium phosphate, the results of tests indicated that the best pH value for phosphorus reclamation would gradually diminish with the increase of initial concentration of phosphorus. Under the condition of best pH, the phosphorus reclamation percentage would gradually become stable with the increase of the ratio of calcium to phosphorus , it could come to 85% or more when the ratio of calcium to phosphorus was 2:1.
The composition analysis of the phosphorus reclamation product indicated that, the mass percentage of main elements in struvite deposited from the reclamation process of simulated wastewater is approximately equal to the theoretic ratio, the mass percentage of phosphorus, magnesium and NH3-N was lower than the theoretic value because of the calcium disturbance. During the calcium phosphorus deposition process, the mass percentage of calcium and phosphorus in simulated wastewater approached to that in real wastewater, both of which were lower than the theoretic value, which indicated that the probable existence of crystal water in calcium phosphorus deposit may be the reason why the mass percentage of calcium and phosphorus was lower than the theoretic value.
试验首先考察了复合式膜生物反应器(HMBR工艺)处理生活污水的净化效能。该工艺稳定运行时对COD、氨氮、SS的去除率都在90%以上,对总氮也有40%左右的去除率,但对磷的去除效果不理想。采用化学混凝预处理可以使MBR工艺出水TP低于1mg/L,相对于协同投药,前置投药能够取得更好的除磷效果。除磷混凝药剂的筛选试验结果表明,以硫酸铝作为混凝剂,同时投加不超过20mg/L的氢氧化钙为最佳的投药方式,并且处理后水pH值波动不大。
试验重点考察了污泥外循环—复合式膜生物反应器(ERP-HMBR工艺)的除污染性能。在稳定运行的情况下,ERP-HMBR工艺对COD和氨氮的去除率都在90%以上,对总氮的去除率在70%左右。外循环污泥的释磷程度决定了工艺对总磷的去除效果,当外循环污泥释磷充分时,工艺对磷的去除率稳定在80%以上;当外循环污泥释磷受到抑制时,工艺对磷的去除率下降至60%左右。污泥厌氧释磷的最佳时间为1.5~2.0h;以乙酸钠作为释磷碳源时,污泥每释放1mmol的磷大约需要消耗1.048mmol的乙酸钠。
根据ERP-HMBR工艺在污泥外循环过程中会产生少量富含磷的污水这一特征,设计烧杯试验考察了人工配制的富磷污水磷回收过程中的影响因素。在以鸟粪石沉淀为主要产物的磷回收过程中,最佳pH值随着初始磷浓度的增加而逐渐降低,并最终稳定在8.5左右,当pH值在不超过9时,磷酸镁沉淀副产物对鸟粪石沉淀过程的干扰可以忽略;当初始磷浓度低于35mg/L时不建议采用以鸟粪石形态对磷进行回收;当[Mg~(2+)]:[NH_3-N]:[P]由1:1:1逐渐增加至为2:2:1时,磷的回收率由33.2%增加至86.8%;且[NH_3-N]:[P]变化要比[Mg~(2+)]:[P]变化对磷回收率的影响严重;对于钙离子含量高的富磷污水,建议以磷酸钙盐的形式回收其中的磷。在以磷酸钙盐沉淀为主要形态的磷回收试验过程中,磷回收的最佳pH值随着初始磷浓度的增加而逐渐降低;在最佳反应pH值条件下,磷的回收率随钙磷比的增加而增加并逐渐趋于稳定,初始钙磷比在2:1以上时均能取得85%以上的磷回收率。
对磷回收产物组分分析结果表明,采用模拟废水回收的鸟粪石中各主要元素的质量百分比与理论值较为接近,采用实际废水回收的鸟粪石中钙离子的干扰使得磷、镁和氨氮的质量百分比均低于理论值;在磷酸钙盐沉淀过程中,模拟废水与实际污水的回收产物中钙磷质量百分比比较接近,且均低于理论值,磷酸钙盐沉淀中可能含有结晶水是造成钙磷质量百分比低于理论值的原因。
Much phosphorus in the treated urban wastewater causes water eutrophication and phosphorus loss. Membrane Bioreactor (MBR) is gradually used in wastewater treatment for its good performance and excellent effluent except limited phosphorus removal. So, it is significant to study enhanced MBR phosphorus removal and phosphorus reclamation simultaneously.
Firstly the effect of single Hybrid Membrane Bioreactor (HMBR) on treating domestic wastewater was studied. The removal efficiency of COD, NH4-N and SS were above 90% and TN was about 40% when the process was operated steadily.But the removal efficiency of P was bad. The chemical-coagulation pretreatment could make the TP in effluent under 1 mg/L. Pre-dosage was better than synergic dosage on phosphorus removal. The results of screening coagulant for phosphorus removal indicated that, the optimum addition method was selecting Al2(SO4)3 as coagulant and Ca(OH)2 at dosage no higher than 20mg/L, and the pH value of effluent was little fluctuating.
Secondly the effect of External Recycle of Activated Sludge Processes- Hybrid Membrane Bioreactor(ERP-HMBR) on treating domestic wastewater was studied. In the steady state, the removal efficiency of COD and NH4-N were above 90% respectively, the removal efficiency of TN was about 70%. The removal efficiency of TP was determined by the amount of phosphorus release from external recycle sludge. The removal efficiency of P was steadly above 80% when the phosphorus releas from external recycle sludge is sufficient and less of 60% when the phosphorus releas was bad. The results of effecting factor analysise indicated that, suitable anaerobic phosphorus release time was 1.5~2.0h; when acetateas was used as phosphorus release carbon resource organic substrate, 1mmol phosphorus release need about 1.048mmol acetate.
According to the characteristic that the ERP-HMBR process would produce less wastewater with higher phosphorus concentration, the impacting factors in the process of phosphorus reclamation were studied by batch tests used simulated high-phosphorus wastewater. During the reclamation process in which the main product was struvite, the best pH would gradually decrease with the increase of initial phosphorus concentration and eventually stabilized at about 8.5. If pH value was no more than 9, the disturbance of magnesium phosphorus to the struvite deposition could be neglected. If the initial phosphorus concentration was less than 35mg/L, it was not suggested toreclamation phosphorus in the form of struvite. When the ratio of [Mg~(2+)]:[NH_3-N]:[P] increase gradually from 1:1:1 to 2:2:1, the phosphorus reclamation percentage would increase from 33.2% to 86.8%. Moreover the ratio of [NH_3-N]:[P] can affect the reclamation percentage more than the ratio of [Mg~(2+)]:[P]. Phosphorus reclamation in the form of calcium phosphate was better than the form of struvite when there was much calcium ion in the wastewater. During the reclamation process in which the main product was calcium phosphate, the results of tests indicated that the best pH value for phosphorus reclamation would gradually diminish with the increase of initial concentration of phosphorus. Under the condition of best pH, the phosphorus reclamation percentage would gradually become stable with the increase of the ratio of calcium to phosphorus , it could come to 85% or more when the ratio of calcium to phosphorus was 2:1.
The composition analysis of the phosphorus reclamation product indicated that, the mass percentage of main elements in struvite deposited from the reclamation process of simulated wastewater is approximately equal to the theoretic ratio, the mass percentage of phosphorus, magnesium and NH3-N was lower than the theoretic value because of the calcium disturbance. During the calcium phosphorus deposition process, the mass percentage of calcium and phosphorus in simulated wastewater approached to that in real wastewater, both of which were lower than the theoretic value, which indicated that the probable existence of crystal water in calcium phosphorus deposit may be the reason why the mass percentage of calcium and phosphorus was lower than the theoretic value.
引文
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62王绍贵,张兵,汪慧贞.以鸟粪石的形式在污水处理厂回收磷的研究.环境工程. 2005, 23(3):78~80
63 Cote P., Thompson D. Wastewater treatment using membrane: The North American experience. Wat. Sci. Tech. 2000, 41(10-11):209~215
64张立秋,封莉,邹联沛等.一体式与复合式MBR运行特性对比研究.给水排水. 2002, 28(12):17~19
65顾国维,何义亮.膜生物反应器-在污水处理中的研究和应用.化学工业出版社, 2002.
66 Yamamoto K., Hiasa M., Mahmood T. Direct solid-liquid separation using hollow fiber membrane in an activated sludge aeration tank. Wat. Sci. Tech. 1989, 20(4-5):43~54
67邢传宏, Tardieu Eric,钱易.无机膜-生物反应器处理生活污水试验研究.环境科学. 1997, 18(3):1~4
68李红兵,顾国维,谢维民.中空纤维膜生物反应器处理生活污水的特性.环境科学. 1999, 20(2):53~56
69 Bussion.H., Cote P., Paderie M. The use of immersed membranes for upgrading wastewater treatment plants. Wat. Sci. Tech. 1998, 37(9):89~95
70 Xia Huang, Rui Liu, Yi Qian. Behaviour of soluble microbial products in a membrane bioreactor. Process Biochemistry. 2000, 36:401~406
71刘锐,黄霞,钱易.一体式膜生物反应器长期运行中的膜污染控制.环境科学. 2000, 21(2):58-61
72郑祥,樊耀波.膜生物反应器运行条件的优化及膜污染的控制.给水排水. 2001, 27(4):41-45
73 Liao B.Q., Bagley D.M., Kraemer G., et al. A review of biofouling and its control in membrane separation bioreactors. Water Environ. Res. 2004, 76(5):425~436
74 Gaoka H, Kono S, Yamanishi S, et al. Influence of organic loading on membrane fouling in membrane sepa ration activated sludge process. Wat. Sci. Tech. 2000, 41(10-11):355~362
75 Nagoaka H., Yamanishi S., Miya A. Modeling of biofouling by extracellular polymers in a membrane separation activated sludge. Wat. Sci. Tech. 1998, 38 (4-5): 497~504
76 Boris Lesjean, Regina Gnirss, Christian Adam. Process configurations adapted to membrane bioreactors for enhanced biological phosphorous and nitrogenremoval. Desalination. 2002, 149: 217~224
77 Yeom Ick-Tae, Nah Yoo-Mi, Ahn Kyu-Hong. Treatment of household wastewater with an intermittently aerated membrane bioreactor. Desalination. 1999, 124: 193~204
78刘江峰,王志伟,吴志超等.一体式膜生物反应器同步硝化反硝化中试试验.环境工程. 2007, 25(1):13~15
79邹联沛,王宝贞,范延臻等. SRT对膜生物反应器出水水质的影响研究.中国给水排水. 2000, 7:17~19
80 Ghyoot W., Vandaele S., Verstraete W. Nitrogen removal from sludge reject water with a membrane assisted bioreactor. Wat. Res. 1999, 33:23~32
81李春杰,耿琰,顾国维.焦化废水的-体式膜-序批式生物反应器处理研究.上海环境科学. 2001, 20(1): 24~27
82 Tatsuli U., Kenji H. Domestic wasterwater treatment by a submerged membrane bioreactor with gravitational filtration. Wat. Res. 1999, 33(12):2888~2892
83邹联沛,薛罡,王宝贞.膜生物反应器中化学除磷的研究.中国给水排水. 2002, 11:20~22
84迟军,王宝贞,吕斯濠.一体化复合式膜生物反应器除磷研究.水处理技术. 2003, 29(1):47~49
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87 Pedro A.Castillo, Simon Gonzalez-Martinez, I?aki Tejero. Biological phosphorus removal using a biofilm membrane reactor: operation at high organic loading rates. Wat. Sci. Tech. 1999, 40(4-5): 321~329
88 Kyu-Hong Ahn, Kyung-Guen Song, Eulsaeng Cho et al. Enhanced biological phosphorus and nitrogen removal using a sequencing anoxic/anaerobic membrane bioreactor (SAM) process. Desalination. 2003, 157:345~352
89刘硕,王宝贞,王正等.复合式膜生物反应器强化脱氮除磷的实验研究.现代化工. 2006, 26(5):40~44
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91 Chiemchaisri, Yamamoto, Vigneswarons. Household membrane bioreactor fordomestic wastewater treatment. Wat. Sci. Tech. 1992, 27(1):171~178
92 Davies W J, Le M S, Heat C R. Intensified activated sludg process with submerged membrane microfiltration. Wat. Sci. Tech. 1998, 38(4-5):421~428
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94邱立平.曝气生物滤池处理生活污水的运行特性及生态学研究.哈尔滨工业大学博士毕业论文. 2003:38~40
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60陈瑶,李小明,曾光明等.以磷酸钙盐的形式从污水处理厂回收磷的研究.环境科学与管理. 2006, 31(4):110~112
61 Battistoni P., Fava G.., Pavan P., et al. Phosphate removal in anaerobic liquors by struvite crystallization without addition of chemicals: preliminary results. Wat. Res. 1997, 31:2925~2929
62王绍贵,张兵,汪慧贞.以鸟粪石的形式在污水处理厂回收磷的研究.环境工程. 2005, 23(3):78~80
63 Cote P., Thompson D. Wastewater treatment using membrane: The North American experience. Wat. Sci. Tech. 2000, 41(10-11):209~215
64张立秋,封莉,邹联沛等.一体式与复合式MBR运行特性对比研究.给水排水. 2002, 28(12):17~19
65顾国维,何义亮.膜生物反应器-在污水处理中的研究和应用.化学工业出版社, 2002.
66 Yamamoto K., Hiasa M., Mahmood T. Direct solid-liquid separation using hollow fiber membrane in an activated sludge aeration tank. Wat. Sci. Tech. 1989, 20(4-5):43~54
67邢传宏, Tardieu Eric,钱易.无机膜-生物反应器处理生活污水试验研究.环境科学. 1997, 18(3):1~4
68李红兵,顾国维,谢维民.中空纤维膜生物反应器处理生活污水的特性.环境科学. 1999, 20(2):53~56
69 Bussion.H., Cote P., Paderie M. The use of immersed membranes for upgrading wastewater treatment plants. Wat. Sci. Tech. 1998, 37(9):89~95
70 Xia Huang, Rui Liu, Yi Qian. Behaviour of soluble microbial products in a membrane bioreactor. Process Biochemistry. 2000, 36:401~406
71刘锐,黄霞,钱易.一体式膜生物反应器长期运行中的膜污染控制.环境科学. 2000, 21(2):58-61
72郑祥,樊耀波.膜生物反应器运行条件的优化及膜污染的控制.给水排水. 2001, 27(4):41-45
73 Liao B.Q., Bagley D.M., Kraemer G., et al. A review of biofouling and its control in membrane separation bioreactors. Water Environ. Res. 2004, 76(5):425~436
74 Gaoka H, Kono S, Yamanishi S, et al. Influence of organic loading on membrane fouling in membrane sepa ration activated sludge process. Wat. Sci. Tech. 2000, 41(10-11):355~362
75 Nagoaka H., Yamanishi S., Miya A. Modeling of biofouling by extracellular polymers in a membrane separation activated sludge. Wat. Sci. Tech. 1998, 38 (4-5): 497~504
76 Boris Lesjean, Regina Gnirss, Christian Adam. Process configurations adapted to membrane bioreactors for enhanced biological phosphorous and nitrogenremoval. Desalination. 2002, 149: 217~224
77 Yeom Ick-Tae, Nah Yoo-Mi, Ahn Kyu-Hong. Treatment of household wastewater with an intermittently aerated membrane bioreactor. Desalination. 1999, 124: 193~204
78刘江峰,王志伟,吴志超等.一体式膜生物反应器同步硝化反硝化中试试验.环境工程. 2007, 25(1):13~15
79邹联沛,王宝贞,范延臻等. SRT对膜生物反应器出水水质的影响研究.中国给水排水. 2000, 7:17~19
80 Ghyoot W., Vandaele S., Verstraete W. Nitrogen removal from sludge reject water with a membrane assisted bioreactor. Wat. Res. 1999, 33:23~32
81李春杰,耿琰,顾国维.焦化废水的-体式膜-序批式生物反应器处理研究.上海环境科学. 2001, 20(1): 24~27
82 Tatsuli U., Kenji H. Domestic wasterwater treatment by a submerged membrane bioreactor with gravitational filtration. Wat. Res. 1999, 33(12):2888~2892
83邹联沛,薛罡,王宝贞.膜生物反应器中化学除磷的研究.中国给水排水. 2002, 11:20~22
84迟军,王宝贞,吕斯濠.一体化复合式膜生物反应器除磷研究.水处理技术. 2003, 29(1):47~49
85成英俊,张捍民,张兴文等.生物膜-膜生物反应器脱氮除磷性能.中国环境科学. 2004, 24(1):72~75
86张捍民,肖景霓,成英俊等.强化膜生物反应器脱氮除磷性能对比试验研究.环境科学学报. 2005, 25(2):242~248
87 Pedro A.Castillo, Simon Gonzalez-Martinez, I?aki Tejero. Biological phosphorus removal using a biofilm membrane reactor: operation at high organic loading rates. Wat. Sci. Tech. 1999, 40(4-5): 321~329
88 Kyu-Hong Ahn, Kyung-Guen Song, Eulsaeng Cho et al. Enhanced biological phosphorus and nitrogen removal using a sequencing anoxic/anaerobic membrane bioreactor (SAM) process. Desalination. 2003, 157:345~352
89刘硕,王宝贞,王正等.复合式膜生物反应器强化脱氮除磷的实验研究.现代化工. 2006, 26(5):40~44
90国家环保局《水和废水监测分析方法》编委会.水和废水监测分析方法,第四版.北京:中国环境科学出版社, 2002.
91 Chiemchaisri, Yamamoto, Vigneswarons. Household membrane bioreactor fordomestic wastewater treatment. Wat. Sci. Tech. 1992, 27(1):171~178
92 Davies W J, Le M S, Heat C R. Intensified activated sludg process with submerged membrane microfiltration. Wat. Sci. Tech. 1998, 38(4-5):421~428
93王景峰,王暄,季民等.好氧颗粒污泥膜生物反应器脱氮特性.环境科学. 2007, 28(3):528~533
94邱立平.曝气生物滤池处理生活污水的运行特性及生态学研究.哈尔滨工业大学博士毕业论文. 2003:38~40
95郑兴灿,李亚新.污水除磷脱氮技术.中国建筑工业出版社, 1998
96邢伟,黄文敏,李顿海等.铁盐除磷技术机理及铁盐混凝剂的研究进展.给水排水. 2006, 32(2):88~91
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