水中卤乙酸生成和去除特性的研究
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摘要
目前我国还主要使用氯消毒工艺,氯消毒剂会与饮用水源中的消毒副产物前体物反应,生成氯化消毒副产物,而卤乙酸(HAAs)的浓度是控制消毒副产物的总致癌风险的首要指标参数。因此,针对黄浦江微污染原水,本论文重点进行卤乙酸生成和去除特性的研究。
本论文以黄浦江微污染水源经常规工艺的各处理单元出水为对象,调查研究黄浦江原水经预氯化和滤后水二次加氯消毒过程中卤乙酸的生成特性及其季节性的变化规律。同时,结合国家863项目的中试工艺流程,试验研究了卤乙酸生成潜能(HAAFP)在O_3/BAC深度处理工艺流程中的去除效果,对比液氯、氯胺、二氧化氯及其组合工艺的消毒效果,研究卤乙酸生成的影响因素,筛选出适合的、安全的消毒剂。并进而对卤乙酸的去除进行了研究,通过小试,分别以活性炭吸附、O_3氧化、H_2O_2氧化、UV氧化及其联合工艺等处理单元考察不同消毒技术对已生成的卤乙酸的控制效果。
研究结果表明,水厂常规处理工艺的卤乙酸生成量夏季比冬季更大,沉淀水、砂滤水、出厂水中消毒副产物浓度大小顺序基本为沉淀水>出厂水>砂滤水。黄浦江水质测定HAAFP最佳投氯量为13.52mg/L,最大反应时间为6d。O_3/BAC深度处理工艺对HAAFP的去除效果能达到60%左右,较低的臭氧投量(2.0mg/L)就能保证对水中HAAFP有较好的去除效果,并且随着臭氧投加量的增加其去除率不断提高。采用氯胺和二氧化氯作为消毒剂,可以明显降低卤乙酸的生成量。二氧化氯和氯胺联合消毒效果明显优于二者单独使用。
颗粒活性炭(GAC)对三氯乙酸(TCAA)和二氯乙酸(DCAA)吸附研究表明,在单底质条件下,活性炭对卤乙酸的吸附等温线最符合修正的Freundlich方程,浓度小于200μg/L时,活性炭对卤乙酸基本表现为单层吸附。活性炭投加量为1600mg/L时,GAC对TCAA和DCAA的去除率分别达到98.49%和98.01%。活性炭对TCAA的吸附能力高于DCAA,当平衡浓度为0.3μmol/L时,其对二者的摩尔吸附容量比为1.17:1。酸性条件下有利于活性炭吸附卤乙酸。多底质共存条件下,两种卤乙酸之间存在竞争吸附,与单底质条件下相比,活性炭对TCAA的吸附受影响程度低于DCAA。同时进行了吸附速率比较表明活性炭对DCAA的吸附速率较快。
At present, chlorine was used as the primary disinfectant in our country, and could be reacted with organic matter(NOM) to generate disinfection by-products (DBPs). Haloacetic acids as an indicator of the total carcinogentic risk of disinfection by-products(DBPs).For the micro-contaminated source water of the HuangPu river, the thesis focus on studying characteristics of formation and removal of haloacetic acids(HAAs) in water.In the thesis, aimed at the raw water of the Huangpu river and effluent of different conventional treatment units, and investigated the rule of formation and variation with seasons of HAAs after prechlorination and secondary dosing chlorine into filtered water for disinfection. Simultanous, combine with the treatment process of pilot-scale experiment of the national 863 program, the removal effect of HAAFP by ozonation-biological activated carbon(O_3/BAC) process was investigated. Comparing with the disinfection effects of chlorine,chloramine, chlorine dioxide and their combination processes, the influence factor of HAAs formation was studied in order to select safe and appropriate disinfectant. Furthermore, the removing methods of HAAs were researched through the bench-scale experiments, such as granular activated carbon(GAC) adsorption, UV, O_3, H_2O_2, UV/H_2O_2 and UV/H_2O_2/O_3,etc, to control the HAAs formed in different water treatment units..The results indicated that: the HAAs quantity formed after conventional water treatment processes in summer is larger than in winter. The sequence of HAAs concemtration is that settleing water > finished water > filtered water. When measuring the haloacetic acids formation potential(HAAFP) of Huangpu raw water, the adoptable dosage of chlorine is 13.52mg/L, and the largest react time is 6 days. The removal efficiency of HAAFP by O_3/ BAC advanced treatment process is about 60%. The low dosage of ozone(2.0mg/L) can make sure the removal effect of HAAFP in water, and the removal efficiency will be improved as increasing of the dosage of ozone. Using the chloramine and chlorine dioxide as disinfectant can decrease the formation quantity of HAAs. The disinfect effect of combination technique of chloramine and chlorine
dioxide is better than using them alone.GAC were adopted to study and contrast the adsorption characteristics of two kinds of HAAs in drinking water. It has to mentioned that the adsoption isotherm of HAAs is best according with the amendatory Freundlich equation under single component system . At the concentration below 200ug/L. When the quantity of GAC is 1600mg/L,the removal efficiency for trichloroacetic acid (TCAA) and dichloroacetic acid (DCAA) can arrive at 98.49% and 98.01% respectively. The adsorption capacity for trichloroacetic acid (TCAA) is larger than dichloroacetic acid (DCAA), the mol adsorption capacity for TCAA is 1.17 times as much as for DCAA at the mol equation concentration of 0.3umol/L.It's better for GAC adsorption of HAAs in the acidic condition.Under multicomponent system, there were competition for adsorption between different kinds of HAAs, compared with the case under monocomponent system the influence on adsorption capacity for TCAA is slighter than DCAA, the above results consist with structure character of different organic compounds.At the same time, the adsorption rate were contrasted to show that the adsorption rate for DCAA is rather high.HAAs is difficult to be oxidated after reacting 2 hours, the removal efficiency of HAAs are both blow 15% by using O3 or H2O2 alone, and the removal efficiency of DCAA and TCAA by UV advanced oxidation technique were increased appreciably. The removal efficiency of DCAA and TCAA are preferable by UV/H2O2 or UV/H2O2/O3. Even more, the affect factors of removing DCAA and TCAA were discussed.
本论文以黄浦江微污染水源经常规工艺的各处理单元出水为对象,调查研究黄浦江原水经预氯化和滤后水二次加氯消毒过程中卤乙酸的生成特性及其季节性的变化规律。同时,结合国家863项目的中试工艺流程,试验研究了卤乙酸生成潜能(HAAFP)在O_3/BAC深度处理工艺流程中的去除效果,对比液氯、氯胺、二氧化氯及其组合工艺的消毒效果,研究卤乙酸生成的影响因素,筛选出适合的、安全的消毒剂。并进而对卤乙酸的去除进行了研究,通过小试,分别以活性炭吸附、O_3氧化、H_2O_2氧化、UV氧化及其联合工艺等处理单元考察不同消毒技术对已生成的卤乙酸的控制效果。
研究结果表明,水厂常规处理工艺的卤乙酸生成量夏季比冬季更大,沉淀水、砂滤水、出厂水中消毒副产物浓度大小顺序基本为沉淀水>出厂水>砂滤水。黄浦江水质测定HAAFP最佳投氯量为13.52mg/L,最大反应时间为6d。O_3/BAC深度处理工艺对HAAFP的去除效果能达到60%左右,较低的臭氧投量(2.0mg/L)就能保证对水中HAAFP有较好的去除效果,并且随着臭氧投加量的增加其去除率不断提高。采用氯胺和二氧化氯作为消毒剂,可以明显降低卤乙酸的生成量。二氧化氯和氯胺联合消毒效果明显优于二者单独使用。
颗粒活性炭(GAC)对三氯乙酸(TCAA)和二氯乙酸(DCAA)吸附研究表明,在单底质条件下,活性炭对卤乙酸的吸附等温线最符合修正的Freundlich方程,浓度小于200μg/L时,活性炭对卤乙酸基本表现为单层吸附。活性炭投加量为1600mg/L时,GAC对TCAA和DCAA的去除率分别达到98.49%和98.01%。活性炭对TCAA的吸附能力高于DCAA,当平衡浓度为0.3μmol/L时,其对二者的摩尔吸附容量比为1.17:1。酸性条件下有利于活性炭吸附卤乙酸。多底质共存条件下,两种卤乙酸之间存在竞争吸附,与单底质条件下相比,活性炭对TCAA的吸附受影响程度低于DCAA。同时进行了吸附速率比较表明活性炭对DCAA的吸附速率较快。
At present, chlorine was used as the primary disinfectant in our country, and could be reacted with organic matter(NOM) to generate disinfection by-products (DBPs). Haloacetic acids as an indicator of the total carcinogentic risk of disinfection by-products(DBPs).For the micro-contaminated source water of the HuangPu river, the thesis focus on studying characteristics of formation and removal of haloacetic acids(HAAs) in water.In the thesis, aimed at the raw water of the Huangpu river and effluent of different conventional treatment units, and investigated the rule of formation and variation with seasons of HAAs after prechlorination and secondary dosing chlorine into filtered water for disinfection. Simultanous, combine with the treatment process of pilot-scale experiment of the national 863 program, the removal effect of HAAFP by ozonation-biological activated carbon(O_3/BAC) process was investigated. Comparing with the disinfection effects of chlorine,chloramine, chlorine dioxide and their combination processes, the influence factor of HAAs formation was studied in order to select safe and appropriate disinfectant. Furthermore, the removing methods of HAAs were researched through the bench-scale experiments, such as granular activated carbon(GAC) adsorption, UV, O_3, H_2O_2, UV/H_2O_2 and UV/H_2O_2/O_3,etc, to control the HAAs formed in different water treatment units..The results indicated that: the HAAs quantity formed after conventional water treatment processes in summer is larger than in winter. The sequence of HAAs concemtration is that settleing water > finished water > filtered water. When measuring the haloacetic acids formation potential(HAAFP) of Huangpu raw water, the adoptable dosage of chlorine is 13.52mg/L, and the largest react time is 6 days. The removal efficiency of HAAFP by O_3/ BAC advanced treatment process is about 60%. The low dosage of ozone(2.0mg/L) can make sure the removal effect of HAAFP in water, and the removal efficiency will be improved as increasing of the dosage of ozone. Using the chloramine and chlorine dioxide as disinfectant can decrease the formation quantity of HAAs. The disinfect effect of combination technique of chloramine and chlorine
dioxide is better than using them alone.GAC were adopted to study and contrast the adsorption characteristics of two kinds of HAAs in drinking water. It has to mentioned that the adsoption isotherm of HAAs is best according with the amendatory Freundlich equation under single component system . At the concentration below 200ug/L. When the quantity of GAC is 1600mg/L,the removal efficiency for trichloroacetic acid (TCAA) and dichloroacetic acid (DCAA) can arrive at 98.49% and 98.01% respectively. The adsorption capacity for trichloroacetic acid (TCAA) is larger than dichloroacetic acid (DCAA), the mol adsorption capacity for TCAA is 1.17 times as much as for DCAA at the mol equation concentration of 0.3umol/L.It's better for GAC adsorption of HAAs in the acidic condition.Under multicomponent system, there were competition for adsorption between different kinds of HAAs, compared with the case under monocomponent system the influence on adsorption capacity for TCAA is slighter than DCAA, the above results consist with structure character of different organic compounds.At the same time, the adsorption rate were contrasted to show that the adsorption rate for DCAA is rather high.HAAs is difficult to be oxidated after reacting 2 hours, the removal efficiency of HAAs are both blow 15% by using O3 or H2O2 alone, and the removal efficiency of DCAA and TCAA by UV advanced oxidation technique were increased appreciably. The removal efficiency of DCAA and TCAA are preferable by UV/H2O2 or UV/H2O2/O3. Even more, the affect factors of removing DCAA and TCAA were discussed.
引文
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