土壤中典型抗生素与镉的二元竞争吸附—解吸行为研究
摘要
本课题以典型抗生素(3种四环素类抗生素)为研究对象,结合2种典型土壤即褐土和红壤,通过振荡平衡法研究了此类抗生素与镉在2种土壤上的二元竞争吸附、解吸行为,同时利用红外光谱方法探讨了此类抗生素与镉复合后在上壤中的吸附机理,研究结果表明：
四环素类抗生素在土壤环境中的吸附和解吸行为：四环素类抗生素均能被土壤强烈的吸附,在本研究所有的环境条件下,土壤吸附了>80%的添加在溶液中的四环素类抗生素。Freundlich方程对此类抗生素在土壤中的吸附解吸等温线具有良好的非线性拟合效果。随着镉的加入,除了红壤对土霉素的吸附减少外,四环素类抗生素在土壤中的吸附都是增加的,且2种土壤对金霉素的吸附强于四环素和土霉素；当登陆顺序发生改变时,除了红壤对金霉素和土霉素的吸附减少外,四环素类抗生素在土壤中的吸附容量(Kf)都是增加的,其中对土霉素的影响最小；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；温度对此类抗生素吸附解吸的影响并不明显。此类抗生素在褐土中的解吸滞后系数高于红壤,镉能够增加此类抗生素在土壤中的滞后性；不同登陆顺序下,先加入抗生素后加入镉的解吸滞后系数增加,而先加入镉后加入抗生素则有所减少；不同土壤有机质对四环素类抗生素的解吸滞后系数影响不同,去除有机质红壤会增加其滞后性,而去除有机质褐土则会减少；去除土壤氧化物基本上能够增加此类抗生素在土壤中的滞后性,且有机质、氧化物对四环素解吸滞后的影响比其他抗生素强烈。除了金霉素在红壤中的吸附以化学吸附为主其它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中的吸附机理研究：通过对四环素类抗生素以及其与镉复合在土壤上的红外光谱图分析,发现四环素类抗生素中起作用的基团,主要是羟基、环B中的羰基和环D中的胺基以及酰胺中的羰基和氨基。四环素类抗生素与镉的复合作用可能发生在O1-O17,O13-O15,N4-O3这些官能团上
Heavy metals and antibiotics often coexist in agricultural soils and their concentrations are increasing due to land application of wasters generated from concentrated animal feeding operations. This study aims at evaluating the interaction of widely-used veterinary antibiotic tetracyclines (TCs) and cadmium (Cd) regarding to their adsorption and desorption in two tested soils (cinnamon soil and red soil) using the batch experiments. The sorption mechanisms of TCs and Cd interaction in tested soils are proposed based on the results from Fourier transform-infrared (FT-IR) analyses. The results were abstracted as follows:
Adsorption and desorption of antibiotic tetracyclines in two soils. TCs were strongly absorbed in two tested soils. In this study, more than 80.00% antibiotic TCs added in the solution were absorbed by soils under all condition. The adsorption and desorption isotherms of TCs on the two soils were well fitted with Freundlich equation. The presence of Cd increased TCs adsorption on tested soils in addition to oxytetracycline (OTC) adsorption on red soil. When using different loading methods, the sorption Kf values of TCs increased except for the sorption Kf values of chlortetracycline (CTC) and OTC on red soil.The impact of loading methods on oxytetracycline was weakest. As the removal of soil organic matter and soil oxide, the absorption capacity of soils on such antibiotics declined. There was unobvious effect of temperature on the absorption of TCs in two soils. The apparent sorption-desorption hysteresis of TCs was found in soil, which will probably pose a threat to soil-environmental quality and human health. Hysteresis index (HI) of desorption of TCs in cinnamon soil was higher than in red soil. The present of Cd enhanced the hysteresis effect. HI of desorption TCs were increased when TCs loaded before Cd and removal of red soil organic matter. On the contrary, HI of desorption TCs were decreased when Cd loaded before TCs and removal of cinnamon soil organic matter. Removal of soil organic matter is basically able to increase HI of desorption TCs in the soil. HI of tetratracycline (TC) in soils without soil organic matter and soil oxide were higher than other antibiotic TCs. The adsorption of TCs in the soils mainly was physical adsorption in addition to CTC adsorption on red soil.
Sorption mechanisms of antibiotic tetracyclines in two soils. Base on the results from the spectra of TCs equilibrated with Cd in two soils, it can be found that hydroxyl groups, carbonyl groups in B and D rings, carbonyl and amino groups of the amide in ring D played a significant role in retaining TCs in soils. From the FTIR results, it indicated that TC complexation with Cd could be occurring at the 01-017, O13-O15 and N4-O3.
四环素类抗生素在土壤环境中的吸附和解吸行为：四环素类抗生素均能被土壤强烈的吸附,在本研究所有的环境条件下,土壤吸附了>80%的添加在溶液中的四环素类抗生素。Freundlich方程对此类抗生素在土壤中的吸附解吸等温线具有良好的非线性拟合效果。随着镉的加入,除了红壤对土霉素的吸附减少外,四环素类抗生素在土壤中的吸附都是增加的,且2种土壤对金霉素的吸附强于四环素和土霉素；当登陆顺序发生改变时,除了红壤对金霉素和土霉素的吸附减少外,四环素类抗生素在土壤中的吸附容量(Kf)都是增加的,其中对土霉素的影响最小；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；温度对此类抗生素吸附解吸的影响并不明显。此类抗生素在褐土中的解吸滞后系数高于红壤,镉能够增加此类抗生素在土壤中的滞后性；不同登陆顺序下,先加入抗生素后加入镉的解吸滞后系数增加,而先加入镉后加入抗生素则有所减少；不同土壤有机质对四环素类抗生素的解吸滞后系数影响不同,去除有机质红壤会增加其滞后性,而去除有机质褐土则会减少；去除土壤氧化物基本上能够增加此类抗生素在土壤中的滞后性,且有机质、氧化物对四环素解吸滞后的影响比其他抗生素强烈。除了金霉素在红壤中的吸附以化学吸附为主其它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中的吸附机理研究：通过对四环素类抗生素以及其与镉复合在土壤上的红外光谱图分析,发现四环素类抗生素中起作用的基团,主要是羟基、环B中的羰基和环D中的胺基以及酰胺中的羰基和氨基。四环素类抗生素与镉的复合作用可能发生在O1-O17,O13-O15,N4-O3这些官能团上
Heavy metals and antibiotics often coexist in agricultural soils and their concentrations are increasing due to land application of wasters generated from concentrated animal feeding operations. This study aims at evaluating the interaction of widely-used veterinary antibiotic tetracyclines (TCs) and cadmium (Cd) regarding to their adsorption and desorption in two tested soils (cinnamon soil and red soil) using the batch experiments. The sorption mechanisms of TCs and Cd interaction in tested soils are proposed based on the results from Fourier transform-infrared (FT-IR) analyses. The results were abstracted as follows:
Adsorption and desorption of antibiotic tetracyclines in two soils. TCs were strongly absorbed in two tested soils. In this study, more than 80.00% antibiotic TCs added in the solution were absorbed by soils under all condition. The adsorption and desorption isotherms of TCs on the two soils were well fitted with Freundlich equation. The presence of Cd increased TCs adsorption on tested soils in addition to oxytetracycline (OTC) adsorption on red soil. When using different loading methods, the sorption Kf values of TCs increased except for the sorption Kf values of chlortetracycline (CTC) and OTC on red soil.The impact of loading methods on oxytetracycline was weakest. As the removal of soil organic matter and soil oxide, the absorption capacity of soils on such antibiotics declined. There was unobvious effect of temperature on the absorption of TCs in two soils. The apparent sorption-desorption hysteresis of TCs was found in soil, which will probably pose a threat to soil-environmental quality and human health. Hysteresis index (HI) of desorption of TCs in cinnamon soil was higher than in red soil. The present of Cd enhanced the hysteresis effect. HI of desorption TCs were increased when TCs loaded before Cd and removal of red soil organic matter. On the contrary, HI of desorption TCs were decreased when Cd loaded before TCs and removal of cinnamon soil organic matter. Removal of soil organic matter is basically able to increase HI of desorption TCs in the soil. HI of tetratracycline (TC) in soils without soil organic matter and soil oxide were higher than other antibiotic TCs. The adsorption of TCs in the soils mainly was physical adsorption in addition to CTC adsorption on red soil.
Sorption mechanisms of antibiotic tetracyclines in two soils. Base on the results from the spectra of TCs equilibrated with Cd in two soils, it can be found that hydroxyl groups, carbonyl groups in B and D rings, carbonyl and amino groups of the amide in ring D played a significant role in retaining TCs in soils. From the FTIR results, it indicated that TC complexation with Cd could be occurring at the 01-017, O13-O15 and N4-O3.
引文
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