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生物炭對土壤中四環(huán)素類抗生素的有效性和形態(tài)轉(zhuǎn)化的影響

發(fā)布時間:2018-10-22 07:39
【摘要】:隨著養(yǎng)殖業(yè)和醫(yī)藥業(yè)的迅猛發(fā)展,進(jìn)入環(huán)境中的抗生素日益增多,四環(huán)素類抗生素(Tetracyclines)就是其中主要的一類抗生素。研究表明,土壤中殘留的四環(huán)素類抗生素可通過食物鏈傳輸并累積風(fēng)險,給人類健康和環(huán)境帶來嚴(yán)重的威脅。因生物炭具有經(jīng)濟(jì)、安全以及高效等優(yōu)點,近年來被廣泛關(guān)注,利用生物炭增強(qiáng)土壤對四環(huán)素類抗生素的吸附等研究已取得諸多進(jìn)展,但生物炭對四環(huán)素類抗生素有效性的影響和老化過程中四環(huán)素類抗生素各形態(tài)之間的轉(zhuǎn)化等關(guān)鍵問題仍不明確,亟待研究探討。本文研究了改性核桃殼基生物炭的制備及其對土霉素(Oxytetracycline)、四環(huán)素(Tetracycline)和金霉素(Chlortetracycline)為代表的四環(huán)素類抗生素的吸附性能;向土壤添加生物炭,探究生物炭對土壤吸附四環(huán)素類抗生素的強(qiáng)化作用及生物炭對四環(huán)素類抗生素有效性影響;進(jìn)行土壤老化實驗,探討生物炭對四環(huán)素類抗生素在老化過程中形態(tài)轉(zhuǎn)化的影響。取得的主要成果如下:(1)以系列濃度的KOH、H3PO4、ZnCl2為改性劑,核桃殼為原料制備核桃殼基生物炭,并對其進(jìn)行表征,選擇吸附性能較好的一種生物炭用于四環(huán)素類抗生素的吸附。結(jié)果表明:當(dāng)四環(huán)素類抗生素初始濃度均為20 mg·L-1、生物炭用量為0.010 g時,反應(yīng)24 h后基本達(dá)到平衡,土霉素、四環(huán)素和金霉素的吸附率分別為97.56%、91.14%和96.01%,吸附作用強(qiáng)弱順序為土霉素金霉素四環(huán)素。該吸附動力學(xué)服從準(zhǔn)二級動力學(xué)方程,吸附平衡類型與Langmuir等溫吸附模型相似,且從熱力學(xué)數(shù)據(jù)可以確定此吸附為放熱反應(yīng)。(2)添加生物炭能夠增強(qiáng)黃棕壤對四環(huán)素類抗生素的吸附。對于吸附動力學(xué)實驗,當(dāng)土樣均為1.00 g時,含1%生物炭的實驗組的吸附速率遠(yuǎn)比不含生物炭的對照組要快;吸附平衡時,實驗組的平衡吸附量分別為對照組的1.18、1.14和1.15倍,吸附能力強(qiáng)弱順序為:土霉素金霉素四環(huán)素。反應(yīng)均屬于準(zhǔn)二級動力學(xué)方程,吸附平衡類型接近Langmuir等溫吸附方程,回歸系數(shù)R2均大于0.99,并且添加生物炭能夠大大提高對四環(huán)素類抗生素的吸附,降低有效性。(3)當(dāng)含炭量為1%的黃棕壤中土霉素濃度分別為10、20、50 mg·kg-1時,隨著老化時間的增加,部分可脫附態(tài)逐漸轉(zhuǎn)化為結(jié)合態(tài),并且隨著土霉素初始濃度的增大,轉(zhuǎn)化為結(jié)合態(tài)的量逐漸增大,但其結(jié)合態(tài)占總土霉素含量的比例卻逐漸減小。生物炭含量分別為0%、1%和2%時,隨著生物炭含量的增加,土樣對土霉素的吸附能力增強(qiáng),一定程度上能減少被吸附土霉素的脫附,也能降低土霉素的可提取態(tài)含量,減小其有效性。對于土霉素、四環(huán)素和金霉素這3種四環(huán)素類抗生素,可提取態(tài)轉(zhuǎn)化為結(jié)合態(tài)的轉(zhuǎn)化率大小順序為:金霉素土霉素四環(huán)素。
[Abstract]:With the rapid development of aquaculture and medicine industry, the number of antibiotics entering the environment is increasing day by day. Tetracycline antibiotic (Tetracyclines) is one of the main antibiotics. Studies have shown that tetracycline antibiotics in soil can be transported through the food chain and accumulate risks, which pose a serious threat to human health and the environment. Because biochar has the advantages of economy, safety and high efficiency, it has been paid more and more attention in recent years. The study of using biochar to enhance the adsorption of tetracycline antibiotics has made a lot of progress. However, the effects of biochar on the availability of tetracycline antibiotics and the transformation of tetracycline antibiotics in different forms during aging are still unclear. The preparation of modified walnut shell based biochar and its adsorption on tetracycline antibiotics represented by oxytetracycline (Oxytetracycline),) tetracycline (Tetracycline) and chlortetracycline (Chlortetracycline) were studied. To explore the enhancement effect of biochar on the adsorption of tetracycline antibiotics and the effect of biochar on the availability of tetracycline antibiotics, and to investigate the effect of biochar on the morphological transformation of tetracycline antibiotics during aging. The main results are as follows: (1) A series of KOH,H3PO4,ZnCl2 was used as modifier and walnut shell was used as raw material to prepare walnut shell based biochar, which was characterized and used to adsorb tetracycline antibiotics. The results showed that when the initial concentration of tetracycline antibiotics was 20 mg L ~ (-1) and the amount of biochar was 0.010 g, the equilibrium of tetracycline antibiotics was basically achieved after 24 h reaction. The adsorption rates of tetracycline and chlortetracycline were 97.56% and 96.01% respectively. The order of adsorption was oxytetracycline. The adsorption kinetics was derived from the quasi-second-order kinetic equation, and the adsorption equilibrium type was similar to that of the Langmuir isothermal adsorption model. The thermodynamic data showed that the adsorption was an exothermic reaction. (2) addition of biochar could enhance the adsorption of tetracycline antibiotics in yellow brown soil. For adsorption kinetics experiment, when soil sample is 1.00 g, the adsorption rate of experimental group containing 1% biochar is much faster than that of control group without biochar, and the equilibrium adsorption capacity of experimental group is 1.18 ~ 1.14 and 1.15 times of that of control group respectively. The order of adsorption ability was: tetracycline oxytetracycline. The adsorption equilibrium type is close to the Langmuir isotherm adsorption equation, and the regression coefficient R2 is greater than 0.99, and the adsorption of tetracycline antibiotics can be greatly improved by adding biochar. (3) when the concentration of oxytetracycline in yellow brown soil with 1% carbon content was 10 ~ 20 ~ 50 mg kg-1, with the aging time increasing, part of the desorption state was gradually transformed into a bound state, and the initial concentration of oxytetracycline increased with the increase of the initial concentration of oxytetracycline. The amount of conversion to binding state increased gradually, but the ratio of bound state to total oxytetracycline content decreased gradually. When the content of biochar was 0% and 2%, the adsorption ability of oxytetracycline was enhanced with the increase of biochar content, which could reduce the desorption of oxytetracycline and the extractable content of oxytetracycline to some extent. Reduce its effectiveness. For three tetracycline antibiotics, oxytetracycline, tetracycline and chlortetracycline, the order of conversion of extractable state to bound state is as follows: chlortetracycline tetracycline.
【學(xué)位授予單位】:南京農(nóng)業(yè)大學(xué)
【學(xué)位級別】:碩士
【學(xué)位授予年份】:2015
【分類號】:X53

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