【摘要】：隨著抗生素的大量使用,越來越多的抗生素通過各種途徑進(jìn)入環(huán)境介質(zhì)。由于抗生素本身的難降解性加上處理工藝的有限性,大大增加了其對(duì)環(huán)境和人體及動(dòng)物體的危害。磺胺類抗生素因生產(chǎn)成本低、化學(xué)性質(zhì)穩(wěn)定、抗菌譜廣等優(yōu)勢(shì)而被大量應(yīng)用。近年來我國(guó)的地表水、地下水及污水處理廠進(jìn)出水中均能檢測(cè)到磺胺類抗生素,嚴(yán)重威脅環(huán)境安全和人類健康,尋求高效的磺胺類抗生素去除技術(shù)刻不容緩。碳質(zhì)材料以其高比表面積、豐富的孔結(jié)構(gòu)以及強(qiáng)相互作用,常被用于解決環(huán)境污染問題,但同時(shí)利用多種碳質(zhì)材料(包括凈水廠用活性炭、家用凈水設(shè)備濾芯活性炭、石墨烯、氧化石墨烯等)對(duì)磺胺類抗生素的吸附特性和機(jī)理進(jìn)行對(duì)比研究的較少。本實(shí)驗(yàn)以十五種碳質(zhì)材料為吸附劑研究了其對(duì)磺胺類抗生素的吸附去除性能與機(jī)理。以磺胺甲基嘧啶(SM1)、磺胺二甲基嘧啶(SM2)和磺胺甲惡唑(SMX)為吸附質(zhì)。通過研究吸附劑吸附磺胺甲惡唑的平衡時(shí)間、平衡吸附量、動(dòng)力學(xué)和等溫線參數(shù)確定出各類材料中性能好的四種碳質(zhì)材料。通過掃描電鏡(SEM)、比表面積和孔體積分析及紅外光譜(FT-IR)等手段對(duì)吸附劑進(jìn)行了表征。對(duì)單一吸附體系,研究了碳質(zhì)材料對(duì)SMX的吸附解吸特性,包括不同水化學(xué)條件(溫度、pH值、離子強(qiáng)度、吸附劑投加量、污染物溶液初始濃度和反應(yīng)時(shí)間等)、動(dòng)力學(xué)、等溫線、熱力學(xué)等對(duì)吸附效果的影響,分析了碳質(zhì)材料的吸附機(jī)理。對(duì)共吸附體系,通過固定競(jìng)爭(zhēng)物質(zhì)濃度,研究了不同溫度下競(jìng)爭(zhēng)物質(zhì)SM1和SM2對(duì)主要物質(zhì)SMX吸附等溫線的影響。通過以上研究,得出了吸附反應(yīng)的最佳因子組合,并從多個(gè)角度對(duì)吸附機(jī)理進(jìn)行解釋。實(shí)驗(yàn)結(jié)果表明大部分碳質(zhì)材料的吸附過程符合Freundlich等溫吸附模型,根據(jù)模型參數(shù)知,碳質(zhì)材料對(duì)SMX的吸附容易進(jìn)行;通過動(dòng)力學(xué)實(shí)驗(yàn)得出,實(shí)驗(yàn)數(shù)據(jù)符合擬二級(jí)動(dòng)力學(xué)模型和顆粒內(nèi)擴(kuò)散模型;通過熱力學(xué)實(shí)驗(yàn)得出,吸附反應(yīng)自發(fā)進(jìn)行。以氫氧化鈉為解吸液,對(duì)吸附劑進(jìn)行的一系列解吸再吸實(shí)驗(yàn),結(jié)果表明活性炭的解吸效果很好,解吸之后的吸附性能變化不大,為實(shí)際環(huán)境中吸附劑的再生回收、循環(huán)利用提供了依據(jù)。共吸附體系SMX等溫線結(jié)果表明,主要物質(zhì)高濃度時(shí)加入競(jìng)爭(zhēng)物質(zhì)可提高吸附劑對(duì)主要物質(zhì)的吸附量,更好的發(fā)揮吸附劑的吸附性能,為多種污染物的同時(shí)高效去除提供了新思路。
[Abstract]:With the extensive use of antibiotics, more and more antibiotics enter environmental media through various channels. Because the antibiotic itself is difficult to degrade and the treatment process is limited, the harm to the environment, human body and animal body is greatly increased. Sulfonamides are widely used because of their low production cost, stable chemical properties and wide antibacterial spectrum. In recent years, sulfanilamide antibiotics can be detected in the surface water, groundwater and sewage treatment plant in China, which is a serious threat to environmental safety and human health. It is urgent to seek efficient removal technology of sulfanilamide antibiotics. Carbon materials, with their high specific surface area, rich pore structure and strong interaction, are often used to solve environmental pollution problems, but at the same time, many kinds of carbon materials (including activated carbon for water purification plant, filter activated carbon for household water purification equipment, graphene) are used. The adsorption characteristics and mechanism of sulfanilamides were seldom studied. Fifteen carbon materials were used as adsorbents to study the adsorption and removal mechanism of sulfanilamides. Sulfamethazine (SM1), sulfamethazine (SM2) and sulfamethoxazole (SMX) were used as adsorbents. By studying the equilibrium time, equilibrium adsorption capacity, kinetics and isotherm parameters of adsorption of sulfamethoxazole with adsorbent, four kinds of carbonaceous materials with good properties were determined. The adsorbent was characterized by scanning electron microscope (SEM) (SEM), surface area and pore volume analysis and infrared spectroscopy (FT-IR). For a single adsorption system, the adsorption and desorption characteristics of carbon materials to SMX were studied, including different hydrochemical conditions (temperature, pH value, ionic strength, adsorbent dosage, initial concentration of pollutant solution and reaction time, etc.), kinetics, etc. The adsorption mechanism of carbon materials was analyzed by the influence of isotherm, thermodynamics and so on. The effects of SM1 and SM2 on the adsorption isotherms of the main compounds SMX at different temperatures were studied by fixing the concentration of competitive substances in the co-adsorption system. Through the above research, the best combination of factors for adsorption reaction was obtained, and the adsorption mechanism was explained from several angles. The experimental results show that the adsorption process of most carbon materials accords with the Freundlich isothermal adsorption model. According to the model parameters, the adsorption of SMX on carbon materials is easy. According to the kinetic experiments, the experimental data are in accordance with the pseudo-second-order kinetic model and the intraparticle diffusion model, and the thermodynamic experiments show that the adsorption reaction proceeds spontaneously. A series of desorption and readsorption experiments were carried out with sodium hydroxide as desorption solution. The results showed that the desorption effect of activated carbon was very good, and the adsorption performance of activated carbon after desorption had little change, which was the regeneration and recovery of adsorbent in actual environment. The basis of recycling is provided. The results of SMX isotherm showed that the amount of adsorbent could be increased when the main substances were high concentration, and the adsorption properties of the adsorbent could be improved. It provides a new idea for the efficient removal of various pollutants at the same time.
【學(xué)位授予單位】：華北電力大學(xué)(北京)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：X703

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