四环素类抗生素在土壤中的环境行为及生态毒性研究
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摘要
本课题以四环素类抗生素为研究对象,结合2种典型土壤即褐土和红壤,分别通过振荡平衡法和室内模拟方法研究了此类抗生素在土壤中吸附、解吸和降解行为,且在不同介质(水和土壤)中研究了此类抗生素对土壤植物-小麦的生态毒性,研究结果表明:四环素类抗生素在土壤环境中的吸附动力学:在不同条件下,土壤对四环素的吸附均能在24h时达到稳定平衡。随着液土比的降低和土壤有机质的去除,四环素在2种土壤上的吸附速度加快。Elovich方程和双常数方程对四环素在土壤中的吸附动力学具有良好的拟合效果。
四环素类抗生素在土壤环境中的吸附和解吸行为:四环素和土霉素均能被土壤强烈的吸附,结果表明,在本研究所有的测定条件下,土壤吸附了>80.00%的添加在溶液中的四环素类类抗生素,且2种土壤对四环素的吸附强于土霉素。Freundlich方程对此类抗生素在土壤中的吸附等温线具有良好的非线性拟合效果。随着土壤有机质和氧化物的去除,土壤对此类抗生素的吸附容量下降;Ca2+、K+、Na+ 3种离子介质条件下,由于Ca2+与此类抗生素能够形成稳定的络合物,因此以Ca2+介质中抗生素在土壤上的吸附最弱;随着液土比的增加,土壤对抗生素的吸附容量和吸附强度均呈下降趋势;当pH值>5.5,随着实际土壤平衡溶液中的pH的增加,土壤对四环素的吸附下降。此类抗生素在褐土中的解吸滞后系数高于红壤,且土霉素的解吸滞后性强于四环素。去除土壤有机质基本上能够增加此类抗生素在土壤中的滞后性;不同离子条件下,以四环素在Ca2+介质中的解吸滞后系数最大,土霉素在K+介质中的解吸滞后系数最大。温度对此类抗生素吸附解吸的影响并不明显。四环素类抗生素在土壤中的吸附以物理吸附为主。
四环素类抗生素在土壤环境中的降解行为:四环素和土霉素在土壤中的降解随着时间的延长而变缓。根据半衰期数值显示,四环素在土壤中具较易降解性,而土霉素具中等降解性;四环素在褐土中的降解快于红壤,而土霉素在红壤中的降解快于褐土。去除土壤有机质能够延缓四环素和土霉素的降解,且土壤有机质对四环素降解的影响比土霉素强烈。土著微生物并不影响此类抗生素在土壤中的降解。
四环素类抗生素对小麦的生态毒性:根伸长抑制率是此类抗生素最好的生态毒性指示指标。土壤对抗生素污染有重要的缓冲作用,其中对土霉素的缓冲强度高于四环素。在不同介质中,小麦的根伸长抑制率(或芽伸长抑制率)与此类抗生素的浓度之间均存在明显的剂量-效应关系。四环素和土霉素在水溶液中的生态毒性指标IC10分别为25.88,24.22mg/L,而在土壤中分别增加至377.8,717.6mg/kg,介质类型严重影响着污染物的IC10值。
Batch sorption methods and indoor simulation methods were employed to reveal adsorption, desorption and degradation process of antibiotic tetracyclines in two tested soils (cinnamon soil and red soil). The effects of antibiotic tetracyclines on the eco-toxicity of wheat in two medium (water and soil) was also investigated. The results were as follows:
Adsorption dynamic of tetracycline in two soils. Under different condition, the absorption of tetracycline in soil can reach stable equilibrium after 24h. With the decreasing of soil-to-solution ratio and the removal of soil organic matter, absorption rate of tetracycline in two kinds of soil was speeded up. Elovich equation and Exponent equation can better simulate the relationship tetracycline adsorption in the soil and time.
Adsorption and desorption of antibiotic tetracyclines in two soils. Tetracycline and oxytetracycline were both strongly absorbed in soils. In this study, more than 80.00% antibiotic tetracyclines added in the solution were absorbed by soils under all condition. And the absorption of soils on tetracycline was stronger than oxytetracycline. Freundlich equation was better non-linear fitting to the antibiotics adsorption isotherm in soils. As the removal of soil organic matter and soil oxides, the absorption capacity of Soil on such antibiotics declined. Under Ca2+、K+、Na + medium, the adsorption of antibiotics in the soil was the weakest in Ca2+ medium. With the increasing of the soil-to-solution ratio, soil absorption capacity and absorption intensity of antibiotics decreased. When pH is above 5.5, soil absorption of tetracycline decreased with the increasing of pH in the final soil solution.
Hysteresis index (HI) of desorption of anyibiotic in cinnamon soil was higher than in red soil, and HI of oxytetracycline was higher than tetracycline in same soil. Removal of soil organic matter is basically able to increase HI of desorption of such antibiotics in the soil. Under Ca2+、K+、Na + medium, HI of tetracycline in Ca2+ medium and oxytetracycline in K+ medium were higher than other condition. There was obvious effect of temperature on the absorption of antibiotics in soil. The adsorption of antibiotic tetracyclines in the soils mainly was physical adsorption.
The degradation of antibiotic tetracyclines in two soils. The degradation of tetracycline and oxytetracycline in soils gradually slowed with the increasing of time. According to the half-life of antibiotic, tetracycline was easier to degrade and oxytetracycline was middle-easier to degrade. The degradation of tetracycline in cinnamon soil was faster than in red soil, and oxytetracycline was on the contrary. Removal of soil organic matter can decreased the degradation of tetracycline and oxytetracycline in soils. The effect of soil organic matter on tetracycline degradation was stronger than oxytetracycline. Indigenous soil microorganisms can not affect the antibiotics degradation in soil.
The eco-toxicity of tetracycline antibiotics to wheat. The inhibition rate of root elongation was the most appropriate eco-toxicity index in following three parameters including seed germinating, root elongation and shoot elongation. Soil on tetracycline antibiotics pollution has an important buffer. Soil buffer on oxytetracycline was stronger than on tetracycline. In different medium, there was a significant logarithmic relationship between the concentration of antibiotics and the inhibition rates of root elongation (or inhibition rates of shoot elongation) of wheat. IC10 of tetracycline and oxytetracycline in water was 25.88mg/kg and 24.22mg/kg, respectively, however, their IC10 values were increased largely in soil with 377.8mg/kg and 717.6mg/kg, respectively. Aboved results showed that medium can strongly affect IC10 values.
四环素类抗生素在土壤环境中的吸附和解吸行为:四环素和土霉素均能被土壤强烈的吸附,结果表明,在本研究所有的测定条件下,土壤吸附了>80.00%的添加在溶液中的四环素类类抗生素,且2种土壤对四环素的吸附强于土霉素。Freundlich方程对此类抗生素在土壤中的吸附等温线具有良好的非线性拟合效果。随着土壤有机质和氧化物的去除,土壤对此类抗生素的吸附容量下降;Ca2+、K+、Na+ 3种离子介质条件下,由于Ca2+与此类抗生素能够形成稳定的络合物,因此以Ca2+介质中抗生素在土壤上的吸附最弱;随着液土比的增加,土壤对抗生素的吸附容量和吸附强度均呈下降趋势;当pH值>5.5,随着实际土壤平衡溶液中的pH的增加,土壤对四环素的吸附下降。此类抗生素在褐土中的解吸滞后系数高于红壤,且土霉素的解吸滞后性强于四环素。去除土壤有机质基本上能够增加此类抗生素在土壤中的滞后性;不同离子条件下,以四环素在Ca2+介质中的解吸滞后系数最大,土霉素在K+介质中的解吸滞后系数最大。温度对此类抗生素吸附解吸的影响并不明显。四环素类抗生素在土壤中的吸附以物理吸附为主。
四环素类抗生素在土壤环境中的降解行为:四环素和土霉素在土壤中的降解随着时间的延长而变缓。根据半衰期数值显示,四环素在土壤中具较易降解性,而土霉素具中等降解性;四环素在褐土中的降解快于红壤,而土霉素在红壤中的降解快于褐土。去除土壤有机质能够延缓四环素和土霉素的降解,且土壤有机质对四环素降解的影响比土霉素强烈。土著微生物并不影响此类抗生素在土壤中的降解。
四环素类抗生素对小麦的生态毒性:根伸长抑制率是此类抗生素最好的生态毒性指示指标。土壤对抗生素污染有重要的缓冲作用,其中对土霉素的缓冲强度高于四环素。在不同介质中,小麦的根伸长抑制率(或芽伸长抑制率)与此类抗生素的浓度之间均存在明显的剂量-效应关系。四环素和土霉素在水溶液中的生态毒性指标IC10分别为25.88,24.22mg/L,而在土壤中分别增加至377.8,717.6mg/kg,介质类型严重影响着污染物的IC10值。
Batch sorption methods and indoor simulation methods were employed to reveal adsorption, desorption and degradation process of antibiotic tetracyclines in two tested soils (cinnamon soil and red soil). The effects of antibiotic tetracyclines on the eco-toxicity of wheat in two medium (water and soil) was also investigated. The results were as follows:
Adsorption dynamic of tetracycline in two soils. Under different condition, the absorption of tetracycline in soil can reach stable equilibrium after 24h. With the decreasing of soil-to-solution ratio and the removal of soil organic matter, absorption rate of tetracycline in two kinds of soil was speeded up. Elovich equation and Exponent equation can better simulate the relationship tetracycline adsorption in the soil and time.
Adsorption and desorption of antibiotic tetracyclines in two soils. Tetracycline and oxytetracycline were both strongly absorbed in soils. In this study, more than 80.00% antibiotic tetracyclines added in the solution were absorbed by soils under all condition. And the absorption of soils on tetracycline was stronger than oxytetracycline. Freundlich equation was better non-linear fitting to the antibiotics adsorption isotherm in soils. As the removal of soil organic matter and soil oxides, the absorption capacity of Soil on such antibiotics declined. Under Ca2+、K+、Na + medium, the adsorption of antibiotics in the soil was the weakest in Ca2+ medium. With the increasing of the soil-to-solution ratio, soil absorption capacity and absorption intensity of antibiotics decreased. When pH is above 5.5, soil absorption of tetracycline decreased with the increasing of pH in the final soil solution.
Hysteresis index (HI) of desorption of anyibiotic in cinnamon soil was higher than in red soil, and HI of oxytetracycline was higher than tetracycline in same soil. Removal of soil organic matter is basically able to increase HI of desorption of such antibiotics in the soil. Under Ca2+、K+、Na + medium, HI of tetracycline in Ca2+ medium and oxytetracycline in K+ medium were higher than other condition. There was obvious effect of temperature on the absorption of antibiotics in soil. The adsorption of antibiotic tetracyclines in the soils mainly was physical adsorption.
The degradation of antibiotic tetracyclines in two soils. The degradation of tetracycline and oxytetracycline in soils gradually slowed with the increasing of time. According to the half-life of antibiotic, tetracycline was easier to degrade and oxytetracycline was middle-easier to degrade. The degradation of tetracycline in cinnamon soil was faster than in red soil, and oxytetracycline was on the contrary. Removal of soil organic matter can decreased the degradation of tetracycline and oxytetracycline in soils. The effect of soil organic matter on tetracycline degradation was stronger than oxytetracycline. Indigenous soil microorganisms can not affect the antibiotics degradation in soil.
The eco-toxicity of tetracycline antibiotics to wheat. The inhibition rate of root elongation was the most appropriate eco-toxicity index in following three parameters including seed germinating, root elongation and shoot elongation. Soil on tetracycline antibiotics pollution has an important buffer. Soil buffer on oxytetracycline was stronger than on tetracycline. In different medium, there was a significant logarithmic relationship between the concentration of antibiotics and the inhibition rates of root elongation (or inhibition rates of shoot elongation) of wheat. IC10 of tetracycline and oxytetracycline in water was 25.88mg/kg and 24.22mg/kg, respectively, however, their IC10 values were increased largely in soil with 377.8mg/kg and 717.6mg/kg, respectively. Aboved results showed that medium can strongly affect IC10 values.
引文
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