微污染水源水处理过程中消毒副产物及病毒类微生物变化特性研究
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摘要
研究中采用铜绿微囊藻、铜绿微囊藻EPS、牛白蛋白、腐殖酸、DNA、鱼油和淀粉代表和模拟生物源有机前体物藻、藻EPS、蛋白质、腐殖酸、DNA、脂肪和多糖,通过调节臭氧浓度及溴碘离子浓度考察其消毒副产物生成特性。试验发现不同的生物源模拟化合物在消毒过程中表现出不同的DBPs生成特性。针对THMs而言,随着臭氧投加浓度的升高,铜绿微囊藻EPS和淀粉的TTHMs生成浓度变化不明显；DNA的TTHMs生成浓度随之升高；铜绿微囊藻、牛白蛋白、腐殖酸和鱼油的TTHMs生成浓度随之降低。针对HAAs而言,随着臭氧投加浓度的升高,铜绿微囊藻EPS、鱼油和牛白蛋白的THAAs生成浓度变化不明显；DNA、腐殖酸和铜绿微囊藻的THAAs生成浓度随之升高；淀粉的THAAs生成浓度随之降低。而溴碘离子的投加能够极大地增大各类生物源有机前体物的THMs生成反应活性,溴碘离子投加后生成的TTHMs浓度显著高于未投加时。溴碘离子的投加对生成的HAAs种类和浓度变化无明显影响。在溴离子对NDMA生成的影响试验中发现,溴离子可反应消耗掉一定剂量的臭氧,导致各类生物源有机物的NDMA生成浓度随溴离子投加浓度升高而降低。比较各种生物源前体物模拟化合物的DBPs生成特性表明,铜绿微囊藻及其EPS和腐殖酸普遍具有较其它生物源模拟化合物更高的DBPs前体物浓度,在经消毒反应以及溴碘离子投加后能够产生较其它生物源模拟化合物相对更高的DBPs浓度。
不同微污染原水处理过程中DBPs生成特性变化试验通过在三种微污染原水处理过程中取样进行臭氧/氯化反应后测定消毒副产物。研究表明,不同微污染原水中均检测到了诸如多糖、腐殖酸、DNA等的生物源物质成分,以及在部分原水中检出了叶绿素a,表明不同微污染原水中微生物及藻类物质的存在,通过与上一章生物源物质的DBPs生成特性比较可知,不同微污染原水中检出的DBPs生成势种类与各种生物源物质的DBPs生成特性相符。臭氧/氯化消毒的THMs生成势浓度显著低于相对应的直接氯化消毒的THMs生成势浓度,因此认为臭氧反应能够有效氧化去除水体中的THMs前体物,降低水体中的THMs生成势浓度。而与此相反的是,臭氧/氯化消毒的HAAs生成势浓度高于相对应的直接氯化消毒的HAAs生成势浓度,表明臭氧对水体中污染物质氧化后的产物,较氧化之前能更为行之有效地与氯反应生成HAAs,臭氧的投加提高了水体中HAAs生成势浓度。混凝沉淀较其它工艺而言能够相对更有效地去除水体中的蛋白质、多糖、腐殖酸和DNA等各类生物源有机前体物,从而达到有效降低THMs和HAAs生成势的目的。但是生物工艺的应用导致了THMs和HAAs生成势浓度的升高,分析发现经过生物工艺处理后水体中蛋白质、多糖、腐殖酸和DNA等生物源有机物浓度增大,究其原因认为可能源于生物处理工艺中细菌等微生物分泌及胞内物质外泄所导致的SMP和EPS。因此可推断生物处理工艺单元中细菌等微生物的存在可能导致水体中SMP和EPS含量的升高,而这些生物源有机物成分是THMs和HAAs重要的前体物,因此生物工艺中微生物分泌及胞内物质外泄所导致的SMP和EPS将可能影响后续消毒过程中DBPs的生成特性,也因此在生物单元的出水中呈现出更高的THMs和HAAs生成势浓度。
连续流中试试验通过建立一套中试工艺系统进行。尽管采用生物预处理后联接PACS混凝沉淀工艺的流程B中表现出对DBPs前体物替代参数较好的去除性能,但是对于含有高有机物浓度的微污染原水而言,该工艺还是稍显落后,尚不能使出水达到国家饮用水标准。而流程A采用的生物预处理、预臭氧、主臭氧以及活性炭工艺显著提高了系统对微污染源水中有机物的去除性能。研究表明适当的预臭氧浓度能够强化后续的混凝过程对有机物的去除,适当的主臭氧浓度能够促进后续的活性炭滤池对有机物的吸附去除。当流程A中预臭氧浓度为0.5mg/L,主臭氧浓度为2.5mg/L,混凝剂PACS投加剂量为8.9mg/L(以A1203计)时,流程A对微污染原水中COD的去除量能够始终维持在5.0mg/L左右,性能显著高于流程B。因此可推断原水-生物预处理-预臭氧-混凝沉淀-砂滤-主臭氧-活性炭滤池-消毒-出水的工艺流程可有效去除微污染原水中以有机物为表征的DBPs前体物成分,有助于系统对DBPs的控制性能。研究还发现溴碘离子的存在不利于臭氧对病毒微生物的灭活性能,原因在于溴碘离子能与臭氧发生反应,消耗一定剂量的臭氧,相对降低参与病毒灭活的臭氧剂量,从而降低臭氧对病毒微生物的灭活性能。然而溴碘离子的存在可提高氯对病毒的灭活性能,原因在于其可以同氯反应产生较HC10而言更强的卤化剂,增强了对病毒微生物的灭活性能。在连续流中试系统中,当臭氧和氯的投加浓度分别为0.5mg/L和1.0mg/L时,即可高效地去除天然水体中的细菌及病毒类微生物,可较好地保证饮用水的微生物安全性。
在中国南方某市的三个生产性水厂中调查研究了不同的水厂工艺过程中DBPs和病毒类微生物的变化特性。研究发现在采用常规混凝沉淀工艺、深度两级生物处理工艺以及深度臭氧活性炭工艺的三个水厂的工艺过程中均未能检测到NDMA。CHCl3广泛地存在于A、B两厂的原水中,C厂的原水中未检出任何THMs的存在,在C厂原水中检出的MS2和Phix174噬菌体效价也低于A、B两厂原水,表明C厂的原水所受污染程度较A、B两厂的原水而言更轻。C厂过程中检出TTHMs浓度范围0-7.22pμL；B厂过程中检出TTHMs浓度范围0-24.53μg/L；A厂过程中检出TTHMs浓度范围20.54-48.04μg/L。三个水厂的处理过程中THAAs浓度水平差别不大。三个水厂所采用的不同工艺对包括溴碘代DBPs在内的各类DBPs的控制均不够理想。混凝沉淀工艺对作为DBPs前体物替代参数的UV254和TOC,蛋白质、腐殖酸、DNA和多糖等生物源物质的去除效果相对不够理想,但在MS2和Phix174噬菌体的去除中却表现出了良好的性能。A厂混凝沉淀段对UV254和TOC的去除率分别为22.05%和64.57%,对蛋白质、腐殖酸、DNA和多糖的去除率分别为41.01%、0%、10.45%和98.80%,对MS2和Phix174噬菌体的去除率分别为99.91%和99.86%；B厂混凝沉淀段对UV254和TOC的去除率分别为17.64%和11.89%,对蛋白质、腐殖酸、DNA和多糖的去除率分别为0%、56.31%、13.07%和0%,对MS2和Phix174噬菌体的去除率分别为99.95%和99.94%；C厂混凝沉淀段对UV254和TOC的去除率分别为59.79%和21.32%,对蛋白质、腐殖酸、DNA和多糖的去除率分别为0%、48.08%、2.19%和4.91%,对MS2和Phix174噬菌体的去除率分别为99.33%和99.57%。值得注意的是,在采用了两级生物处理工艺的B水厂中,在生物预处理出水的红外图谱中发现在2956cm-1的位置上出现了一个新的有机物官能团吸收峰,分析认为可能源于生物预处理中细菌等微生物分泌及胞内物质外泄所导致的SMP和EPS。而在之前章节的研究中已经表明水体中存在的各种生物源有机物成分是重要的DBPs前体物,因此生物处理中细菌、藻类等微生物分泌及胞内物质外泄所导致的生物源物质成分对DBPs生成的影响值得重视。
The investigation of the species and concentration of DBPs and their formation potential were conducted with microcystis aeruginosa cell, EPS of microcystis aeruginosa cell, fish oil, DNA, humic acids, starch and bovine serum albumin. There were NDMA precursors in microcystis aeruginosa cell, EPS of microcystis aeruginosa cell, DNA, humic acids and bovine serum albumin, and no NDMA precursors existed in fish oil and starch. With the increase of ozone dose, the variation of THMs which was produced by EPS and starch was insignificant, the concentration of THMs which was produced by DNA increased, the concentration of THMs which was produced by microcystis aeruginosa, fish oil, humic acids and bovine serum albumin decrased, the variation of HAAs which was produced by EPS of microcystis aeruginosa cell, fish oil and bovine serum albumin was insignificant, the concentration of HAAs which was produced by DNA, humic acids and microcystis aeruginosa increased, the concentration of HAAs which was produced by starch decrased. Bromide and iodide increased the reaction activity of biological source material in disinfection process. After bromide and iodide were added, the concentration of TTHMs increased, the variation of HAAs was insignificant.
The investigation of the species and concentration of DBPs formation potential were conducted with three micropolluted raw water. No NDMA and its formation potential were detected at raw water and the processes of these three drinking water plants. The THMs formation potential which was produced by the combination of ozonation and chlorination was lower than the formation potential which was produced by single chlorination. The results clearly indicated that the THMs precursors were decreased by ozonation efficiently. The HAAs formation potential which was produced by the combination of ozonation and chlorination was higher than the formation potential which was produced by single chlorination. The results clearly indicated that the HAAs precursors were increased by ozonation. The formation potential of THMs and HAAs was removed by coagulation/sedimentation efficiently. However, soluble microbial products (SMP) and extracellular polymeric substances (EPS), the important precursors of THMs and HAAs, were produced by biological technology in water treatment process.
Optimization of coagulation and ozonation processes for removal of organic matters in micropolluted raw water was conducted by a continuous flow pilot scale test. The water source was mainly influenced by agriculture pollution and inland waterway transportation. Coagulation/sedimentation was not enough to treat the micropolluted raw water with highly concentrated organic matter, and the extra ozonation and granular activated carbon (GAC) filtration were necessary. Proper poly-aluminum-chloride-sulfates (PACS), pre-ozone and post-ozone dosages were required for improving the removal performance of organic matters. Considering the treatment performances and economic costs, we found that the optimum PACS, pre-ozone and post-ozone dosages should be8.9mg/L Al2O3,0.5mg/L and2.5mg/L respectively. At the optimum PACS dose, removal efficiencies of93.28%turbidity,27.76%UV254and38.55%COD were achieved at Train B (the control). At the optimum pre-ozone dose, removal efficiencies of95.65%turbidity,54.81%UV254and58.14%COD were achieved at Train A. At the optimum post-ozone dose, removal efficiencies of97.09%turbidity,71.83%UV254and66.11%COD were achieved at Train A.
The removal and inactivation of viruses in portable water was conducted in a continuous flow pilot scale system. Bacteriophage MS2was used as model organism for human enteric viruses. The effect of disinfection technologies (single or combination of ozonation and chlorination) and interfering substances (bromide and iodide) on inactivation of viruses, and the removal and inactivation performance of viruses in natural water by the continuous flow pilot scale system were investigated. The results indicated that ozone was more effective in inactivation of viruses than chlorine. The optimum dose of ozone and chlorine was0.5mg/L and1.0mg/L respectively in the combined process of ozonation and chlorination. Bromide and iodide ions in raw water were detrimental to inactivation of viruses by ozone they could consume a certain amount of ozone. However, they enhanced the inactivation of viruses by chlorine, due to the formation of stronger halogenating agent. The continuous flow pilot scale water treatment system was effective in removal of viruses in natural water at optimum conditions, which the dose of ozone and chlorine was0.5mg/L and1.0mg/L respectively.
The removal of disinfection by-products (DBPs) and viruses at three drinking water plants (A, B and C) in a city of southern China was investigated. Coliphages MS2and Phixl74were used as indicators of viruses. The results clearly indicated that no NDMA were detected at raw water and the processes of these three drinking water plants. CHCl3exsited in the raw water of Plant A and B widely, however, no THMs was detected in the raw water of Plant C. The titer of MS2and Phix174in the raw water of Plant C was lower than Plant A and B. It can be concluded that the pollution of raw water of Plant C was slight, and the pollution of raw water of Plant A and B was serious. The removal efficiency of MS2and Phix174was over99%by conventional coagulation/sedimentation at Plant A, B and C. MS2and Phix174were not detected in the effluent of these three plants. However, the removal efficiency of UV254and TOC by coagulation/sedimentation was only22.05%and64.57%at Plant A,17.64%and11.89%at Plant B,59.79%and21.32%at Plant C respectively. Acorrding to the previous study in this paper SMP and EPS were the important precursors of THMs and HAAs. It is worthwhile to note that a new peak at2956cm-1had emerged in the infrared spectrogram of biological pretreatment effluent of Plant B. This result is presumably due to the SMP and EPS which are related to bacteria metabolism and cell lysis produced in biological filter.
不同微污染原水处理过程中DBPs生成特性变化试验通过在三种微污染原水处理过程中取样进行臭氧/氯化反应后测定消毒副产物。研究表明,不同微污染原水中均检测到了诸如多糖、腐殖酸、DNA等的生物源物质成分,以及在部分原水中检出了叶绿素a,表明不同微污染原水中微生物及藻类物质的存在,通过与上一章生物源物质的DBPs生成特性比较可知,不同微污染原水中检出的DBPs生成势种类与各种生物源物质的DBPs生成特性相符。臭氧/氯化消毒的THMs生成势浓度显著低于相对应的直接氯化消毒的THMs生成势浓度,因此认为臭氧反应能够有效氧化去除水体中的THMs前体物,降低水体中的THMs生成势浓度。而与此相反的是,臭氧/氯化消毒的HAAs生成势浓度高于相对应的直接氯化消毒的HAAs生成势浓度,表明臭氧对水体中污染物质氧化后的产物,较氧化之前能更为行之有效地与氯反应生成HAAs,臭氧的投加提高了水体中HAAs生成势浓度。混凝沉淀较其它工艺而言能够相对更有效地去除水体中的蛋白质、多糖、腐殖酸和DNA等各类生物源有机前体物,从而达到有效降低THMs和HAAs生成势的目的。但是生物工艺的应用导致了THMs和HAAs生成势浓度的升高,分析发现经过生物工艺处理后水体中蛋白质、多糖、腐殖酸和DNA等生物源有机物浓度增大,究其原因认为可能源于生物处理工艺中细菌等微生物分泌及胞内物质外泄所导致的SMP和EPS。因此可推断生物处理工艺单元中细菌等微生物的存在可能导致水体中SMP和EPS含量的升高,而这些生物源有机物成分是THMs和HAAs重要的前体物,因此生物工艺中微生物分泌及胞内物质外泄所导致的SMP和EPS将可能影响后续消毒过程中DBPs的生成特性,也因此在生物单元的出水中呈现出更高的THMs和HAAs生成势浓度。
连续流中试试验通过建立一套中试工艺系统进行。尽管采用生物预处理后联接PACS混凝沉淀工艺的流程B中表现出对DBPs前体物替代参数较好的去除性能,但是对于含有高有机物浓度的微污染原水而言,该工艺还是稍显落后,尚不能使出水达到国家饮用水标准。而流程A采用的生物预处理、预臭氧、主臭氧以及活性炭工艺显著提高了系统对微污染源水中有机物的去除性能。研究表明适当的预臭氧浓度能够强化后续的混凝过程对有机物的去除,适当的主臭氧浓度能够促进后续的活性炭滤池对有机物的吸附去除。当流程A中预臭氧浓度为0.5mg/L,主臭氧浓度为2.5mg/L,混凝剂PACS投加剂量为8.9mg/L(以A1203计)时,流程A对微污染原水中COD的去除量能够始终维持在5.0mg/L左右,性能显著高于流程B。因此可推断原水-生物预处理-预臭氧-混凝沉淀-砂滤-主臭氧-活性炭滤池-消毒-出水的工艺流程可有效去除微污染原水中以有机物为表征的DBPs前体物成分,有助于系统对DBPs的控制性能。研究还发现溴碘离子的存在不利于臭氧对病毒微生物的灭活性能,原因在于溴碘离子能与臭氧发生反应,消耗一定剂量的臭氧,相对降低参与病毒灭活的臭氧剂量,从而降低臭氧对病毒微生物的灭活性能。然而溴碘离子的存在可提高氯对病毒的灭活性能,原因在于其可以同氯反应产生较HC10而言更强的卤化剂,增强了对病毒微生物的灭活性能。在连续流中试系统中,当臭氧和氯的投加浓度分别为0.5mg/L和1.0mg/L时,即可高效地去除天然水体中的细菌及病毒类微生物,可较好地保证饮用水的微生物安全性。
在中国南方某市的三个生产性水厂中调查研究了不同的水厂工艺过程中DBPs和病毒类微生物的变化特性。研究发现在采用常规混凝沉淀工艺、深度两级生物处理工艺以及深度臭氧活性炭工艺的三个水厂的工艺过程中均未能检测到NDMA。CHCl3广泛地存在于A、B两厂的原水中,C厂的原水中未检出任何THMs的存在,在C厂原水中检出的MS2和Phix174噬菌体效价也低于A、B两厂原水,表明C厂的原水所受污染程度较A、B两厂的原水而言更轻。C厂过程中检出TTHMs浓度范围0-7.22pμL；B厂过程中检出TTHMs浓度范围0-24.53μg/L；A厂过程中检出TTHMs浓度范围20.54-48.04μg/L。三个水厂的处理过程中THAAs浓度水平差别不大。三个水厂所采用的不同工艺对包括溴碘代DBPs在内的各类DBPs的控制均不够理想。混凝沉淀工艺对作为DBPs前体物替代参数的UV254和TOC,蛋白质、腐殖酸、DNA和多糖等生物源物质的去除效果相对不够理想,但在MS2和Phix174噬菌体的去除中却表现出了良好的性能。A厂混凝沉淀段对UV254和TOC的去除率分别为22.05%和64.57%,对蛋白质、腐殖酸、DNA和多糖的去除率分别为41.01%、0%、10.45%和98.80%,对MS2和Phix174噬菌体的去除率分别为99.91%和99.86%；B厂混凝沉淀段对UV254和TOC的去除率分别为17.64%和11.89%,对蛋白质、腐殖酸、DNA和多糖的去除率分别为0%、56.31%、13.07%和0%,对MS2和Phix174噬菌体的去除率分别为99.95%和99.94%；C厂混凝沉淀段对UV254和TOC的去除率分别为59.79%和21.32%,对蛋白质、腐殖酸、DNA和多糖的去除率分别为0%、48.08%、2.19%和4.91%,对MS2和Phix174噬菌体的去除率分别为99.33%和99.57%。值得注意的是,在采用了两级生物处理工艺的B水厂中,在生物预处理出水的红外图谱中发现在2956cm-1的位置上出现了一个新的有机物官能团吸收峰,分析认为可能源于生物预处理中细菌等微生物分泌及胞内物质外泄所导致的SMP和EPS。而在之前章节的研究中已经表明水体中存在的各种生物源有机物成分是重要的DBPs前体物,因此生物处理中细菌、藻类等微生物分泌及胞内物质外泄所导致的生物源物质成分对DBPs生成的影响值得重视。
The investigation of the species and concentration of DBPs and their formation potential were conducted with microcystis aeruginosa cell, EPS of microcystis aeruginosa cell, fish oil, DNA, humic acids, starch and bovine serum albumin. There were NDMA precursors in microcystis aeruginosa cell, EPS of microcystis aeruginosa cell, DNA, humic acids and bovine serum albumin, and no NDMA precursors existed in fish oil and starch. With the increase of ozone dose, the variation of THMs which was produced by EPS and starch was insignificant, the concentration of THMs which was produced by DNA increased, the concentration of THMs which was produced by microcystis aeruginosa, fish oil, humic acids and bovine serum albumin decrased, the variation of HAAs which was produced by EPS of microcystis aeruginosa cell, fish oil and bovine serum albumin was insignificant, the concentration of HAAs which was produced by DNA, humic acids and microcystis aeruginosa increased, the concentration of HAAs which was produced by starch decrased. Bromide and iodide increased the reaction activity of biological source material in disinfection process. After bromide and iodide were added, the concentration of TTHMs increased, the variation of HAAs was insignificant.
The investigation of the species and concentration of DBPs formation potential were conducted with three micropolluted raw water. No NDMA and its formation potential were detected at raw water and the processes of these three drinking water plants. The THMs formation potential which was produced by the combination of ozonation and chlorination was lower than the formation potential which was produced by single chlorination. The results clearly indicated that the THMs precursors were decreased by ozonation efficiently. The HAAs formation potential which was produced by the combination of ozonation and chlorination was higher than the formation potential which was produced by single chlorination. The results clearly indicated that the HAAs precursors were increased by ozonation. The formation potential of THMs and HAAs was removed by coagulation/sedimentation efficiently. However, soluble microbial products (SMP) and extracellular polymeric substances (EPS), the important precursors of THMs and HAAs, were produced by biological technology in water treatment process.
Optimization of coagulation and ozonation processes for removal of organic matters in micropolluted raw water was conducted by a continuous flow pilot scale test. The water source was mainly influenced by agriculture pollution and inland waterway transportation. Coagulation/sedimentation was not enough to treat the micropolluted raw water with highly concentrated organic matter, and the extra ozonation and granular activated carbon (GAC) filtration were necessary. Proper poly-aluminum-chloride-sulfates (PACS), pre-ozone and post-ozone dosages were required for improving the removal performance of organic matters. Considering the treatment performances and economic costs, we found that the optimum PACS, pre-ozone and post-ozone dosages should be8.9mg/L Al2O3,0.5mg/L and2.5mg/L respectively. At the optimum PACS dose, removal efficiencies of93.28%turbidity,27.76%UV254and38.55%COD were achieved at Train B (the control). At the optimum pre-ozone dose, removal efficiencies of95.65%turbidity,54.81%UV254and58.14%COD were achieved at Train A. At the optimum post-ozone dose, removal efficiencies of97.09%turbidity,71.83%UV254and66.11%COD were achieved at Train A.
The removal and inactivation of viruses in portable water was conducted in a continuous flow pilot scale system. Bacteriophage MS2was used as model organism for human enteric viruses. The effect of disinfection technologies (single or combination of ozonation and chlorination) and interfering substances (bromide and iodide) on inactivation of viruses, and the removal and inactivation performance of viruses in natural water by the continuous flow pilot scale system were investigated. The results indicated that ozone was more effective in inactivation of viruses than chlorine. The optimum dose of ozone and chlorine was0.5mg/L and1.0mg/L respectively in the combined process of ozonation and chlorination. Bromide and iodide ions in raw water were detrimental to inactivation of viruses by ozone they could consume a certain amount of ozone. However, they enhanced the inactivation of viruses by chlorine, due to the formation of stronger halogenating agent. The continuous flow pilot scale water treatment system was effective in removal of viruses in natural water at optimum conditions, which the dose of ozone and chlorine was0.5mg/L and1.0mg/L respectively.
The removal of disinfection by-products (DBPs) and viruses at three drinking water plants (A, B and C) in a city of southern China was investigated. Coliphages MS2and Phixl74were used as indicators of viruses. The results clearly indicated that no NDMA were detected at raw water and the processes of these three drinking water plants. CHCl3exsited in the raw water of Plant A and B widely, however, no THMs was detected in the raw water of Plant C. The titer of MS2and Phix174in the raw water of Plant C was lower than Plant A and B. It can be concluded that the pollution of raw water of Plant C was slight, and the pollution of raw water of Plant A and B was serious. The removal efficiency of MS2and Phix174was over99%by conventional coagulation/sedimentation at Plant A, B and C. MS2and Phix174were not detected in the effluent of these three plants. However, the removal efficiency of UV254and TOC by coagulation/sedimentation was only22.05%and64.57%at Plant A,17.64%and11.89%at Plant B,59.79%and21.32%at Plant C respectively. Acorrding to the previous study in this paper SMP and EPS were the important precursors of THMs and HAAs. It is worthwhile to note that a new peak at2956cm-1had emerged in the infrared spectrogram of biological pretreatment effluent of Plant B. This result is presumably due to the SMP and EPS which are related to bacteria metabolism and cell lysis produced in biological filter.
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