电离辐照联合BAF处理水中药物及抗菌剂的研究
发布时间：2018-11-05 09:47
【摘要】：自然水体中的药物及个人护理品(PPCPs)对人体和环境具有潜在的危害,传统的废水处理技术难以对其有效去除,如何将其有效去除成为研究焦点。电离辐照技术作为一种高级氧化技术,在水处理领域日益得到重视,具有潜在的应用前景。论文选取甲氧苄氨嘧啶、卡马西平和三氯生为代表性PPCPs,研究了三种PPCPs辐照降解的影响因素,探讨了其辐照降解动力学特性,提出了降解路径,考察了辐照技术与其他氧化技术联合对PPCPs降解的作用,并比较了PPCPs辐照前后的可生化性变化。主要结论如下:(1)研究了影响PPCPs辐照降解的主要因素,包括PPCPs的初始浓度,其他氧化剂的投加量和溶液初始pH值。结果表明,较低的浓度有利于PPCPs降解与矿化。过硫酸钾的加入对PPCPs辐照降解具有显著的促进作用。当K2S2O8投加量为1.5 mM时,在1000 Gy的吸收剂量下各PPCPs的矿化率由16%-34%提升至32%-94.1%。K2FeO4的加入在辐照降解初期对PPCPs的去除有抑制作用,随后却在一定程度上提高了矿化率。在偏酸性条件下(pH=6.5)有利于各PPCPs的辐照降解。(2)分析了不同辐照体系下PPCPs的辐照降解动力学。结果表明三种PPCPs的在不同辐照体系中的降解符合准一级动力学反应规律。(3)探讨了各PPCPs在不同辐照体系下的降解途径和机理。结果表明甲氧苄氨嘧啶主要通过羟基化、去甲基化、裂解以及脱氢作用实现降解和矿化;卡马西平的降解主要通过羟基化和裂解作用实现;而三氯生的降解则通过羟基化、脱氯及裂解作用实现。在各过程中HO·起主要作用,SO4-·通过电子传递促进HO·降解PPCPs的反应进程,而Fe(VI)则直接氧化PPCPs实现对其的降解。(4)通过比较活性污泥呼吸耗氧量,考察了辐照前后PPCPs的可生化性。结果表明:各PPCPs在辐照前难以被生物利用甚至具有生物毒性,辐照处理后其可生化性提高。辐照处理含1 mg/L甲氧苄氨嘧啶/三氯生的二级出水经过曝气生物滤池处理后发现COD、TOC和NH4+-N的去除率均显著提高。这为辐照技术与曝气生物滤池工艺联合应用于二级出水深度处理提供了理论依据和技术支持。研究对辐照技术处理含PPCPs的废水具有重要的理论和实际应用价值。
[Abstract]:Drugs and personal care products (PPCPs) in natural water have potential harm to human body and environment. It is difficult for traditional wastewater treatment technology to remove them effectively. How to remove them effectively has become the focus of research. As a kind of advanced oxidation technology, ionizing irradiation technology has been paid more and more attention in the field of water treatment and has a potential application prospect. In this paper, trimethoprim, carbamazepine and triclosan were selected as representative PPCPs, to study the influencing factors of three kinds of PPCPs irradiation degradation. The effects of irradiation and other oxidation technologies on the degradation of PPCPs were investigated, and the biodegradability of PPCPs before and after irradiation was compared. The main conclusions are as follows: (1) the main factors affecting the degradation of PPCPs irradiated were studied, including the initial concentration of PPCPs, the dosage of other oxidants and the initial pH value of the solution. The results showed that low concentration was beneficial to PPCPs degradation and mineralization. The addition of potassium persulfate can significantly promote the degradation of PPCPs by irradiation. When the dosage of K2S2O8 was 1.5 mM, at the absorbed dose of 1000 Gy, the mineralization rate of each PPCPs increased from 16% to 34%, and the addition of 32%-94.1%.K2FeO4 inhibited the removal of PPCPs at the early stage of irradiation degradation. Subsequently, the mineralization rate was increased to a certain extent. Under the condition of partial acidity (pH=6.5), the irradiation degradation of PPCPs was facilitated. (2) the kinetics of irradiation degradation of PPCPs in different irradiation systems was analyzed. The results show that the degradation of three kinds of PPCPs in different irradiation systems accords with the quasi-first-order kinetic reaction law. (3) the degradation pathway and mechanism of PPCPs in different irradiation systems are discussed. The results showed that the degradation and mineralization of trimethoprim were mainly achieved by hydroxylation demethylation cracking and dehydrogenation while the degradation of carbamazepine was mainly achieved by hydroxylation and cleavage. The degradation of triclosan was achieved by hydroxylation, dechlorination and pyrolysis. HO plays a major role in each process. SO4- promotes the degradation of PPCPs by HO through electron transfer, while Fe (VI) directly oxidizes PPCPs to achieve its degradation. (4) oxygen consumption in respiration of activated sludge is compared. The biodegradability of PPCPs before and after irradiation was investigated. The results showed that each PPCPs was difficult to be bioutilized or even biotoxic before irradiation, and its biodegradability was improved after irradiation. The removal rates of COD,TOC and NH4-N in the secondary effluent containing 1 mg/L trimethoprim / trichlorogenate were significantly increased after biological aerated filter treatment. This provides a theoretical basis and technical support for the combined application of irradiation technology and biological aerated filter in advanced treatment of secondary effluent. The study has important theoretical and practical application value for the treatment of wastewater containing PPCPs by irradiation technology.
【学位授予单位】：中国地质大学(北京)
【学位级别】：博士
【学位授予年份】：2017
【分类号】：X703
本文编号：2311685
[Abstract]:Drugs and personal care products (PPCPs) in natural water have potential harm to human body and environment. It is difficult for traditional wastewater treatment technology to remove them effectively. How to remove them effectively has become the focus of research. As a kind of advanced oxidation technology, ionizing irradiation technology has been paid more and more attention in the field of water treatment and has a potential application prospect. In this paper, trimethoprim, carbamazepine and triclosan were selected as representative PPCPs, to study the influencing factors of three kinds of PPCPs irradiation degradation. The effects of irradiation and other oxidation technologies on the degradation of PPCPs were investigated, and the biodegradability of PPCPs before and after irradiation was compared. The main conclusions are as follows: (1) the main factors affecting the degradation of PPCPs irradiated were studied, including the initial concentration of PPCPs, the dosage of other oxidants and the initial pH value of the solution. The results showed that low concentration was beneficial to PPCPs degradation and mineralization. The addition of potassium persulfate can significantly promote the degradation of PPCPs by irradiation. When the dosage of K2S2O8 was 1.5 mM, at the absorbed dose of 1000 Gy, the mineralization rate of each PPCPs increased from 16% to 34%, and the addition of 32%-94.1%.K2FeO4 inhibited the removal of PPCPs at the early stage of irradiation degradation. Subsequently, the mineralization rate was increased to a certain extent. Under the condition of partial acidity (pH=6.5), the irradiation degradation of PPCPs was facilitated. (2) the kinetics of irradiation degradation of PPCPs in different irradiation systems was analyzed. The results show that the degradation of three kinds of PPCPs in different irradiation systems accords with the quasi-first-order kinetic reaction law. (3) the degradation pathway and mechanism of PPCPs in different irradiation systems are discussed. The results showed that the degradation and mineralization of trimethoprim were mainly achieved by hydroxylation demethylation cracking and dehydrogenation while the degradation of carbamazepine was mainly achieved by hydroxylation and cleavage. The degradation of triclosan was achieved by hydroxylation, dechlorination and pyrolysis. HO plays a major role in each process. SO4- promotes the degradation of PPCPs by HO through electron transfer, while Fe (VI) directly oxidizes PPCPs to achieve its degradation. (4) oxygen consumption in respiration of activated sludge is compared. The biodegradability of PPCPs before and after irradiation was investigated. The results showed that each PPCPs was difficult to be bioutilized or even biotoxic before irradiation, and its biodegradability was improved after irradiation. The removal rates of COD,TOC and NH4-N in the secondary effluent containing 1 mg/L trimethoprim / trichlorogenate were significantly increased after biological aerated filter treatment. This provides a theoretical basis and technical support for the combined application of irradiation technology and biological aerated filter in advanced treatment of secondary effluent. The study has important theoretical and practical application value for the treatment of wastewater containing PPCPs by irradiation technology.
【学位授予单位】：中国地质大学(北京)
【学位级别】：博士
【学位授予年份】：2017
【分类号】：X703
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