环丙沙星在水溶液中的光化学降解研究
摘要
环丙沙星作为喹诺酮类抗生素的一种,被广泛用于医疗、畜牧业、农业和水产养殖业等行业,可以通过很多渠道进入到环境水体中。环丙沙星可以对人体产生中枢系统毒性、肝肾毒性、血液系统毒性以及光毒性,也可以使环境中的细菌对其产生抗性,所以它在环境中的存在会对生态系统和人类健康构成潜在的危害,环丙沙星在环境中的迁移转化越来越引起人们的关注。在表层水体中,有机物最主要的降解方式是光降解,因此本文模拟自然水体中的各种主要因素,研究其对环丙沙星光降解的影响。
在利用高效液相色谱仪确立了水体中环丙沙星的监测分析方法后,首先研究了环丙沙星在光、暗条件下的降解反应。在没有光源照射的条件下,环丙沙星几乎没有降解,而对500W氙灯的照射下进行的光降解反应所得数据进行拟合,发现符合一级反应动力学规律。通过对不同初始浓度的环丙沙星进行光降解研究发现光降解速率常数随浓度的增大而减小,由此可知环丙沙星的光降解符合表观的一级反应动力学。
通过在实验中通入氧气和氮气来研究溶解氧对环丙沙星的光降解产生的影响,发现通氧气抑制了光降解,而通氮气则促进了光降解。这是由于环丙沙星的光降解可以分为直接光降解和自敏化光降解,溶解氧能促进自敏化光降解而抑制直接光降解,由于自敏化增加的反应速率小于直接降解减小的反应速率,造成环丙沙星光降解速率减慢。
然后研究了水中无机氮随着环境pE值改变而发生形态(NO_3~-,NO_2~-和NH_4~+)变化时,对环丙沙星光降解的影响。结果表明,NO_3~-受到光照能够产生活性基团,促进光降解;NO_~-能够猝灭环丙沙星自敏化反应中产生的活性基团,从而抑制光降解;而由于NH_4~+的光稳定性很强,因此没有对光降解产生影响。在研究不同pE值对环丙沙星光降解时,发现光降解速率随着pE的增长先增大后减小,当亚硝酸根和铵根离子共存时,两者相互不起作用;当亚硝酸根和硝酸根共存时,通过对比实际抑制率和理论抑制率可以发现,亚硝酸根能够与硝酸根光敏化产生的羟基自由基反应,生成不活泼物质,抑制了硝酸根光敏化降解环丙沙星。
同时还研究了pH以及环境水体中不同的共存物质对环丙沙星光降解的影响,发现pH在5-8范围内时,光降解速率随pH的增大而增大;Zn~(2+)和Cl-在高浓度的时候能够对环丙沙星的光降解产生一定的影响,Zn~(2+)抑制光降解,而Cl-促进光降解,但影响都很小;Cu~(2+)和腐殖酸都能够非常明显的抑制环丙沙星光降解的进行,抑制率随浓度的增加而增大;阴离子表面SDBS活性剂能够对环丙沙星的光降解产生非常明显的促进作用,在低浓度的时候随浓度的增加而增大,而达到一定浓度之后随浓度的增加而有所减小;Fe~(3+)在低浓度的时候能够对环丙沙星的光降解起到明显的促进作用,促进率随浓度的增大而增加,而达到一定浓度之后,促进率随浓度的增大而减小,进一步加大浓度会出现抑制作用。
As a fluoroquinolone antibiotic, ciprofloxacin which is widely applied in medical, animal husbandry, agriculture and aquaculture can enter the aquatic environment through variety of ways. Ciprofloxacin which exit in the environment would damage the health of human body and ecological ,because it not only can be toxic to the central nervous system, liver , kidney, and hematologic system of human body, but also have bacterial resistance. So its environmental behavior already arouse people’s more and more attention. In surface waters, photochemical degradation is the main factor in determining the fate of organic matter. This present study the effect of photodegradation of ciprofloxacin when add the different compounds which simulate the environment.
After established the analysis method of ciprofloxacin in water, we studied the infection in the dark or under 500W Xenon light. The research results show that: no photodegradation occurred in the dark and the photolysis of ciprofloxacin followed first-order kinetics under the light. With increase of initial concentration of ciprofloxacin, the photo-degradation rate of ciprofloxacin decreased gradually.
We also studied the different influences on photo-degradation of ciprofloxacin in different dissolved oxygen levels, the different concentrations of nitrate, nitrite, ammonium ions, and different pE values when these three forms of N elements coexisted. The result showed that nitrate promoted the degradation of ciprofloxacin, nitrite inhibited it and ammonium had little effect. the influence of the dissolved oxygen levels to the photo-degradation of ciprofloxacin is the same with that of nitrate. The photodegradation rate of ciprofloxacin decreased and then increased follow with the increase of pE value. When nitrate coexisted with ammonium, they wouldn’t affect each other. When nitrite coexisted with nitrate, the degradation rate was less than theoretical value. It indicated that nitrite inhibited the photo-degradation of ciprofloxacin by nitrate.
At the same time, we study the affect of photodegradation by the factor which we simulated the nature water , such as pH, humic acid, Cl~- and so on. The result showed that with increase of pH among the 5-8, the photodegradation rate of ciprofloxacin decreased gradually. Cl- promoted the degradation of ciprofloxacin, Zn~(2+), Cu~(2+) and HA inhibited it and both CTAB and Tween-80 had little effect. Fe~(3+) and SDBS promoted the degradation in low concentrations, and in high concentrations inhibited it.
在利用高效液相色谱仪确立了水体中环丙沙星的监测分析方法后,首先研究了环丙沙星在光、暗条件下的降解反应。在没有光源照射的条件下,环丙沙星几乎没有降解,而对500W氙灯的照射下进行的光降解反应所得数据进行拟合,发现符合一级反应动力学规律。通过对不同初始浓度的环丙沙星进行光降解研究发现光降解速率常数随浓度的增大而减小,由此可知环丙沙星的光降解符合表观的一级反应动力学。
通过在实验中通入氧气和氮气来研究溶解氧对环丙沙星的光降解产生的影响,发现通氧气抑制了光降解,而通氮气则促进了光降解。这是由于环丙沙星的光降解可以分为直接光降解和自敏化光降解,溶解氧能促进自敏化光降解而抑制直接光降解,由于自敏化增加的反应速率小于直接降解减小的反应速率,造成环丙沙星光降解速率减慢。
然后研究了水中无机氮随着环境pE值改变而发生形态(NO_3~-,NO_2~-和NH_4~+)变化时,对环丙沙星光降解的影响。结果表明,NO_3~-受到光照能够产生活性基团,促进光降解;NO_~-能够猝灭环丙沙星自敏化反应中产生的活性基团,从而抑制光降解;而由于NH_4~+的光稳定性很强,因此没有对光降解产生影响。在研究不同pE值对环丙沙星光降解时,发现光降解速率随着pE的增长先增大后减小,当亚硝酸根和铵根离子共存时,两者相互不起作用;当亚硝酸根和硝酸根共存时,通过对比实际抑制率和理论抑制率可以发现,亚硝酸根能够与硝酸根光敏化产生的羟基自由基反应,生成不活泼物质,抑制了硝酸根光敏化降解环丙沙星。
同时还研究了pH以及环境水体中不同的共存物质对环丙沙星光降解的影响,发现pH在5-8范围内时,光降解速率随pH的增大而增大;Zn~(2+)和Cl-在高浓度的时候能够对环丙沙星的光降解产生一定的影响,Zn~(2+)抑制光降解,而Cl-促进光降解,但影响都很小;Cu~(2+)和腐殖酸都能够非常明显的抑制环丙沙星光降解的进行,抑制率随浓度的增加而增大;阴离子表面SDBS活性剂能够对环丙沙星的光降解产生非常明显的促进作用,在低浓度的时候随浓度的增加而增大,而达到一定浓度之后随浓度的增加而有所减小;Fe~(3+)在低浓度的时候能够对环丙沙星的光降解起到明显的促进作用,促进率随浓度的增大而增加,而达到一定浓度之后,促进率随浓度的增大而减小,进一步加大浓度会出现抑制作用。
As a fluoroquinolone antibiotic, ciprofloxacin which is widely applied in medical, animal husbandry, agriculture and aquaculture can enter the aquatic environment through variety of ways. Ciprofloxacin which exit in the environment would damage the health of human body and ecological ,because it not only can be toxic to the central nervous system, liver , kidney, and hematologic system of human body, but also have bacterial resistance. So its environmental behavior already arouse people’s more and more attention. In surface waters, photochemical degradation is the main factor in determining the fate of organic matter. This present study the effect of photodegradation of ciprofloxacin when add the different compounds which simulate the environment.
After established the analysis method of ciprofloxacin in water, we studied the infection in the dark or under 500W Xenon light. The research results show that: no photodegradation occurred in the dark and the photolysis of ciprofloxacin followed first-order kinetics under the light. With increase of initial concentration of ciprofloxacin, the photo-degradation rate of ciprofloxacin decreased gradually.
We also studied the different influences on photo-degradation of ciprofloxacin in different dissolved oxygen levels, the different concentrations of nitrate, nitrite, ammonium ions, and different pE values when these three forms of N elements coexisted. The result showed that nitrate promoted the degradation of ciprofloxacin, nitrite inhibited it and ammonium had little effect. the influence of the dissolved oxygen levels to the photo-degradation of ciprofloxacin is the same with that of nitrate. The photodegradation rate of ciprofloxacin decreased and then increased follow with the increase of pE value. When nitrate coexisted with ammonium, they wouldn’t affect each other. When nitrite coexisted with nitrate, the degradation rate was less than theoretical value. It indicated that nitrite inhibited the photo-degradation of ciprofloxacin by nitrate.
At the same time, we study the affect of photodegradation by the factor which we simulated the nature water , such as pH, humic acid, Cl~- and so on. The result showed that with increase of pH among the 5-8, the photodegradation rate of ciprofloxacin decreased gradually. Cl- promoted the degradation of ciprofloxacin, Zn~(2+), Cu~(2+) and HA inhibited it and both CTAB and Tween-80 had little effect. Fe~(3+) and SDBS promoted the degradation in low concentrations, and in high concentrations inhibited it.
引文
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