四環(huán)素與含水層中常見鐵氧化物礦物的相互作用機(jī)理研究
本文選題:四環(huán)素 + 鐵氧化物礦物。 參考:《中國(guó)地質(zhì)大學(xué)(北京)》2017年碩士論文
【摘要】:四環(huán)素類抗生素由于具有抗菌廣譜性和高效價(jià)廉的特點(diǎn),已經(jīng)成為目前使用最廣泛、用量最大的抗生素種類之一。近年來,對(duì)其的濫用以及機(jī)體不完全吸收部分排出體外的現(xiàn)狀使其在環(huán)境中不斷積累,導(dǎo)致耐藥基因的產(chǎn)生并對(duì)生物體造成危害,抗生素污染的高危害性引起了國(guó)際上的普遍關(guān)注。四環(huán)素是四環(huán)素類抗生素中元素組成較簡(jiǎn)單,具有代表性的一類,本文著眼于四環(huán)素在土水環(huán)境中的遷移轉(zhuǎn)化,選取了三種土壤常見礦物針鐵礦、水鐵礦和赤鐵礦作為研究對(duì)象,通過靜態(tài)吸附批實(shí)驗(yàn)描述各礦物與四環(huán)素的吸附過程,輔以多種表征手段(XRD、SEM、TEM、BET、BJH、XPS、FTIR)刻畫了相互作用前后礦物理化性質(zhì)的差異性并進(jìn)行分析,旨在研究四環(huán)素與不同類型常見鐵氧化物礦物的相互作用機(jī)理。實(shí)驗(yàn)結(jié)果表明:(1)針鐵礦和水鐵礦對(duì)四環(huán)素的吸附平衡時(shí)間為4 d,其中水鐵礦因其比表面積的絕對(duì)優(yōu)勢(shì),吸附速率最快且平衡吸附量大于針鐵礦,而赤鐵礦由于晶體形態(tài)缺陷較多,在吸附過程中不斷裂解,動(dòng)力學(xué)曲線呈階梯狀,在實(shí)驗(yàn)時(shí)間4 d內(nèi)未達(dá)到平衡;針鐵礦和水鐵礦的等溫吸附量隨初始濃度升高而增大直至飽和,赤鐵礦因多階段吸附,未達(dá)平衡,但實(shí)驗(yàn)時(shí)間4 d內(nèi),與針鐵礦和水鐵礦相比,其吸附量最大。(2)實(shí)驗(yàn)所采用的鐵礦物均為三價(jià)鐵,反應(yīng)后上清液中可檢測(cè)出二價(jià)鐵,表明在鐵礦吸附四環(huán)素的過程中,鐵礦表面發(fā)生了化學(xué)反應(yīng)導(dǎo)致了鐵的還原,其中針鐵礦反應(yīng)體系的二價(jià)鐵含量很低,化學(xué)反應(yīng)所占比例有限。對(duì)反應(yīng)前后的礦物表面進(jìn)行紅外光譜測(cè)試,發(fā)現(xiàn)其界面官能團(tuán)有變化,證明三種鐵礦與四環(huán)素相互作用過程中均存在絡(luò)合作用。推測(cè)二價(jià)鐵為四環(huán)素絡(luò)合至礦物表面后發(fā)生電子轉(zhuǎn)移而產(chǎn)生。(3)在水化學(xué)參數(shù)對(duì)吸附的影響研究中,隨著離子強(qiáng)度的升高吸附量略有升高,表明四環(huán)素在此三種鐵礦上的吸附主要為專性吸附;在pH的影響下,四環(huán)素在鐵礦上的吸附量在某個(gè)pH值附近出現(xiàn)最大值,證明吸附過程中存在靜電作用;常見陽離子類型對(duì)吸附無顯著影響,而Cu2+作為鍵橋?qū)λ沫h(huán)素在三種鐵礦物上的吸附量影響不同,推測(cè)與鐵礦物結(jié)晶程度有關(guān)。
[Abstract]:Tetracycline antibiotics have become one of the most widely used and used antibiotics because of their wide spectrum and high efficiency and low price. In recent years, its abuse and incomplete absorption of the body have resulted in its accumulation in the environment, leading to the production of drug-resistant genes and causing harm to organisms, The high harmfulness of antibiotic contamination has aroused widespread concern in the world. Tetracycline is a simple and representative class of tetracycline antibiotics. Based on the migration and transformation of tetracycline in soil-water environment, three common minerals, goethite, are selected. The sorption process of each mineral with tetracycline was described by static adsorption batch experiments, and the physicochemical properties of minerals before and after interaction were characterized and analyzed by various means of characterization. The purpose of this study is to study the interaction mechanism of tetracycline with different types of iron oxide minerals. The experimental results show that the adsorption equilibrium time of tetracycline for goethite and water ore is 4 days, in which the adsorption rate of pyrite is the fastest and the equilibrium adsorption capacity is larger than that of goethite because of its absolute advantage of specific surface area. However, hematite, due to many defects in crystal morphology, cleavage continuously during the adsorption process, and the kinetic curve is in the form of a ladder, and the equilibrium is not reached within 4 days of the experimental time. The isothermal adsorption capacity of goethite and pyrite increases until saturation with the increase of initial concentration. Hematite is not balanced due to multi-stage adsorption, but the experimental time is 4 days, compared with that of goethite and pyrite. The divalent iron can be detected in the supernatant after the reaction, which indicates that the chemical reaction on the surface of iron ore resulted in the reduction of iron during the process of adsorption of tetracycline. The divalent iron content of goethite reaction system is very low and the proportion of chemical reaction is limited. The surface of the minerals before and after the reaction was tested by infrared spectroscopy, and it was found that the interfacial functional groups changed, which proved that the interaction between the three kinds of iron ores and tetracycline existed complexation. It is inferred that the divalent iron is produced by electron transfer after tetracycline complexing to the mineral surface. In the study of the effect of hydrochemical parameters on adsorption, the adsorption capacity increases slightly with the increase of ionic strength. The results show that the adsorption of tetracycline on these three kinds of iron ores is mainly specific adsorption, and the adsorption capacity of tetracycline on iron ore is maximum near a certain pH value under the influence of pH, which proves that electrostatic action exists in the adsorption process. The common cations have no significant effect on the adsorption, but Cu _ 2 acts as a bond bridge for different amounts of tetracycline adsorbed on the three kinds of iron ores, which may be related to the degree of crystallization of iron minerals.
【學(xué)位授予單位】:中國(guó)地質(zhì)大學(xué)(北京)
【學(xué)位級(jí)別】:碩士
【學(xué)位授予年份】:2017
【分類號(hào)】:X505;P579
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