臭氧活性炭—高级氧化组合技术处理水中有机污染物的研究
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摘要
本论文采用臭氧活性炭—高级氧化组合技术(AC／TiO_2／O_3／UV)，对饮用水中环境激素类的代表性污染物—邻苯二甲酸二(2-乙基己)酯和消毒副产物类的有机氯化物—三氯乙醛进行了降解实验，详细研究了降解的效果、影响因素、降解动力学及机理，主要获得如下成果与认识：
(1)臭氧活性炭—高级氧化组合技术对三氯乙醛与邻苯二甲酸二(2-乙基己)酯(DEHP)具有非常好的降解效果，其反应速率快，降解效率高，能达到完全矿化，氧化降解反应符合准一级动力学规律。
(2)影响臭氧活性炭—高级氧化组合技术降解反应的动力学因素主要包括：降解物初始浓度、起始pH值、光催化剂负载量、外加氧化剂的浓度、光照方式及溶液中的HCO_3~(2-)、NO_3~-、Cl~-等阴离子。
(3)TOC、pH值与目标化合物浓度分析检测表明，臭氧活性炭—光催化非均相高级氧化体系(AC／TiO_2／O_3／UV)降解有机污染物的过程中，有机物不是直接被矿化，而是通过形成一系列的中间产物后再被彻底矿化。
(4)三氯乙醛降解过程中主要的中间产物是二氯乙酸、甲酸、二氯甲烷、甲醛、二氯氧；邻苯二甲酸二(2-乙基己)酯降解过程中主要的中间产物是邻苯二甲酸单(2-乙基己)酯、邻苯二甲酸二丁酯、苯甲酸甲酯、邻苯二甲酸、苯甲酸、邻羟基苯甲酸以及甲酸、乙酸、乙二酸、2-丁烯二酸等开环产物。
本研究将传统的臭氧活性炭与光催化技术结合起来形成臭氧活性炭-光催化高级氧化组合技术体系，不仅丰富了高级氧化技术理论，而且为该组合技术在饮用水深度处理中的应用提供了理论基础。
In this study, di(2-ethylhexy)phthalate, a representational environmental hormone pollutant, and chloral, a typical disinfection by-products of drinking water, were degraded using a combination technique of ozone-activated carbon and advanced oxidation ( AC/O_3/TiO_2/UV ) . Their degradation effects, influencing factors, degradation kinetics and degradation mechanisms were investigated. The following main results have been achieved.
(1) It was found that the combination technique of ozone- activated carbon and advanced oxidation can efficiently degrade the two organic pollutants, with high reaction rate constants and complete mineralization. The oxidation degradation reactions follow the pseudo first order kinetics.
(2) It was found that a few of factors, such as the initial concentration of degraded pollutants, the pH value of the solution, the quantity of T1O2 loaded in the activated carbon, the concentration of added oxidant, the duration of illumination and some anion ions of HCO_3~-, NO_3~- and Cl~- in the solution had a significant effect on the degradation.
(3) The measurements of TOC, pH values and targeted pollutants show that the degradation of TOC was obviously slower than that of their parent compounds, and that the variation of pH value in the system indicated the formation of some organic acids during degradation. This implicates that the organic pollutants were not mineralized to CO_2 and H_2O directly, but were converted to some intermediates firstly, and then mineralized completely.
(4) The identified intermediates formed during chloral degradation mainly include acetic acid dichloride, formic acid, dichloromethane, dichloride oxide and formaldehyde, and the intermediates of di(2-ethylhexyl)phthalate are 1,2-benzenedicarboxylic acid, mono(2-ethylhexyl)ester, benzoic acid methyl ester, 2-hydroxy benzoic acid, 1,2-benzonodicarboxylicacid, di(butyl)phthalate, benzoic acid, formic acid, acetic acid, fumaric acid and oxalic acid.
This result presents a new combination technique of ozone-activated carbon and advanced oxidation system. It has not only developed the theory of heterogeneous advanced oxidation process in some extent, but also will provide a foundation for the application of this combination technique to water deep treatment.
(1)臭氧活性炭—高级氧化组合技术对三氯乙醛与邻苯二甲酸二(2-乙基己)酯(DEHP)具有非常好的降解效果，其反应速率快，降解效率高，能达到完全矿化，氧化降解反应符合准一级动力学规律。
(2)影响臭氧活性炭—高级氧化组合技术降解反应的动力学因素主要包括：降解物初始浓度、起始pH值、光催化剂负载量、外加氧化剂的浓度、光照方式及溶液中的HCO_3~(2-)、NO_3~-、Cl~-等阴离子。
(3)TOC、pH值与目标化合物浓度分析检测表明，臭氧活性炭—光催化非均相高级氧化体系(AC／TiO_2／O_3／UV)降解有机污染物的过程中，有机物不是直接被矿化，而是通过形成一系列的中间产物后再被彻底矿化。
(4)三氯乙醛降解过程中主要的中间产物是二氯乙酸、甲酸、二氯甲烷、甲醛、二氯氧；邻苯二甲酸二(2-乙基己)酯降解过程中主要的中间产物是邻苯二甲酸单(2-乙基己)酯、邻苯二甲酸二丁酯、苯甲酸甲酯、邻苯二甲酸、苯甲酸、邻羟基苯甲酸以及甲酸、乙酸、乙二酸、2-丁烯二酸等开环产物。
本研究将传统的臭氧活性炭与光催化技术结合起来形成臭氧活性炭-光催化高级氧化组合技术体系，不仅丰富了高级氧化技术理论，而且为该组合技术在饮用水深度处理中的应用提供了理论基础。
In this study, di(2-ethylhexy)phthalate, a representational environmental hormone pollutant, and chloral, a typical disinfection by-products of drinking water, were degraded using a combination technique of ozone-activated carbon and advanced oxidation ( AC/O_3/TiO_2/UV ) . Their degradation effects, influencing factors, degradation kinetics and degradation mechanisms were investigated. The following main results have been achieved.
(1) It was found that the combination technique of ozone- activated carbon and advanced oxidation can efficiently degrade the two organic pollutants, with high reaction rate constants and complete mineralization. The oxidation degradation reactions follow the pseudo first order kinetics.
(2) It was found that a few of factors, such as the initial concentration of degraded pollutants, the pH value of the solution, the quantity of T1O2 loaded in the activated carbon, the concentration of added oxidant, the duration of illumination and some anion ions of HCO_3~-, NO_3~- and Cl~- in the solution had a significant effect on the degradation.
(3) The measurements of TOC, pH values and targeted pollutants show that the degradation of TOC was obviously slower than that of their parent compounds, and that the variation of pH value in the system indicated the formation of some organic acids during degradation. This implicates that the organic pollutants were not mineralized to CO_2 and H_2O directly, but were converted to some intermediates firstly, and then mineralized completely.
(4) The identified intermediates formed during chloral degradation mainly include acetic acid dichloride, formic acid, dichloromethane, dichloride oxide and formaldehyde, and the intermediates of di(2-ethylhexyl)phthalate are 1,2-benzenedicarboxylic acid, mono(2-ethylhexyl)ester, benzoic acid methyl ester, 2-hydroxy benzoic acid, 1,2-benzonodicarboxylicacid, di(butyl)phthalate, benzoic acid, formic acid, acetic acid, fumaric acid and oxalic acid.
This result presents a new combination technique of ozone-activated carbon and advanced oxidation system. It has not only developed the theory of heterogeneous advanced oxidation process in some extent, but also will provide a foundation for the application of this combination technique to water deep treatment.
引文
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