光敏化产生单线态氧转化水中磺胺类抗生素

发布时间：2018-03-14 17:00

本文选题：玫瑰红　切入点：光敏化　出处：《大连理工大学》2015年硕士论文　论文类型：学位论文

【摘要】：随着抗生素在医药业、畜牧业和水产养殖业的大量使用,抗生素通过各种途径排放到环境中,近些年被频繁检出。抗生素不仅本身具有一定的健康和生态毒性,而且会诱导产生抗性基因,对生态安全和人体健康存在严重的风险。抗生素污染已经成为重要的环境问题,受到公众和科学界的广泛关注。抗生素不易生物降解,传统的废水处理技术一般对抗生素的去除效率不高。近年来,在抗生素的高效处理技术方面开展了很多研究,其中研究较多的是光化学氧化技术。但是,大部分光化学氧化技术都依赖于紫外光,这会增加能耗和应用成本。水环境中存在一些天然的光敏剂,如溶解性有机质和卟啉等,吸光后可以产生具有较强氧化能力的的单线态氧可以促进污染物的转化。玫瑰红(RB)是一种人工合成的光敏剂,其单线态氧的量子产率高达0.76。前人研究表明RB在太阳光下敏化产生单线态氧能够快速转化苯酚和2-氯酚。很多抗生素与单线态氧的二级反应速率常数大于苯酚和2-氯酚。因此推测单线态氧具有快速转化抗生素的潜力。水的理化性质和溶解性物质可能对单线态氧转化抗生素存在影响。本研究选取用量大、水环境中经常检出的磺胺类抗生素(SAs)为目标化合物,以玫瑰红作为光敏剂,在太阳光和模拟光源下,考察了单线态氧对SAs的转化的能力,同时考察了pH、模拟尿液和表面活性剂对单线态氧转化磺胺类抗生素的影响。结果表明,研究的5种SAs与单线态氧反应的二级反应速率常数为0.33×107M-1s-1。-9.17×107M-1s-1。在自然光及模拟光下,相对于SAs自身的光解,单线态氧均能显著促进SAs的转化,促进程度随SAs的不同而存在差异,其中对磺胺嘧啶(SD)转化的促进高达216倍。SD在不同pH下离子形态分布不同,其与单线态氧反应速率常数受pH影响显著,其中,pH=7时SD与单线态氧反应速率常数最大。不同模拟尿液组成对SD与单线态氧的反应影响不同。模拟新鲜尿液和水解尿液对单线态氧转化SD均表现为显著抑制效应。在考察的三个浓度范围内,单线态氧的均能够促进SAs的转化。表面活性剂能够显著影响单线态氧转化SAs,其中阳离子型表面活性剂十六烷基三甲基溴化铵(CTAB)表现出显著的促进作用。在自然光和模拟光下,CTAB对单线态氧转化5种磺胺类抗生素均具有促进作用,促进程度可高达530倍。
[Abstract]:With the extensive use of antibiotics in medicine, animal husbandry and aquaculture, antibiotics are discharged into the environment through various channels and are frequently detected in recent years. Antibiotics not only have certain health and ecological toxicity, Antibiotic contamination has become an important environmental problem and has attracted widespread attention from the public and the scientific community. Antibiotics are not easily biodegradable. In recent years, many researches have been carried out on the efficient treatment of antibiotics, among which photochemical oxidation is the most important one. Most photochemical oxidation technologies depend on ultraviolet light, which increases energy consumption and application cost. There are some natural Guang Min agents in water environment, such as dissolved organic matter and porphyrin. The absorption of light can produce singlet oxygen with strong oxidation ability, which can promote the transformation of pollutants. The quantum yield of singlet oxygen is as high as 0.76. Previous studies have shown that RB sensitized to produce singlet oxygen can rapidly transform phenol and 2-chlorophenol. The second-order reaction rate constants of many antibiotics with singlet oxygen are larger than those of phenol and phenol. 2-chlorophenol. Therefore, it is speculated that singlet oxygen has the potential of rapid transformation of antibiotics. The physicochemical properties and soluble substances of water may affect the conversion of single-line oxygen to antibiotics. Sulfanilamide antibiotics (Sas), which are often detected in water environment, were used as target compounds and rose red as Guang Min. The conversion ability of singlet oxygen to SAs was investigated under solar light and simulated light source. At the same time, the effects of pH, simulated urine and surfactant on the conversion of sulfonamides from singlet oxygen to sulfanilamides were investigated. The results showed that the second-order reaction rate constants of the five kinds of SAs with singlet oxygen were 0.33 脳 107M-1s-1.-9.17 脳 107M-1s-1s-1.In the natural and simulated light, the second order reaction rate constants were 0.33 脳 107M-1s-1.-9.17 脳 107M-1s-1. Compared with the photolysis of SAs itself, singlet oxygen can significantly promote the transformation of SAs, and the degree of promotion is different with the SAs. Among them, the conversion of sulfadiazine is promoted up to 216 times. SD has different ionic speciation distribution at different pH. The rate constant of its reaction with singlet oxygen is significantly affected by pH. Among them, pH = 7:00 SD has the largest reaction rate constant with singlet oxygen. Different composition of simulated urine has different effects on the reaction between SD and singlet oxygen. Both simulated fresh urine and hydrolyzed urine have significant inhibitory effects on the transformation of singlet oxygen into SD. In the three ranges of concentrations examined, Surfactant can significantly affect the conversion of singlet oxygen. Cetyltrimethylammonium bromide cetyltrimethylammonium bromide (cetyltrimethylammonium bromide) cetyltrimethylammonium bromide (cetyltrimethylammonium bromide) cetyltrimethylammonium bromide (cetyltrimethylammonium bromide), a cetyltrimethylammonium bromide. CTAB and CTAB can promote the conversion of 5 sulfonamides to singlet oxygen. The degree of promotion can be as high as 530 times.
【学位授予单位】：大连理工大学
【学位级别】：硕士
【学位授予年份】：2015
【分类号】：X703

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