電廠飛灰對水體中典型抗生素的吸附特性研究
發(fā)布時間：2018-08-22 21:13
【摘要】：我國是抗生素生產(chǎn)和使用大國,抗生素不合理使用或濫用現(xiàn)象嚴重。抗生素的作用時間和代謝時間較長,在自然環(huán)境中難以實現(xiàn)有效降解,一旦進入環(huán)境將嚴重威脅人類健康和生態(tài)安全,目前抗生素已成為水環(huán)境中最重要的污染物之一。吸附法作為處理水體中抗生素的重要方法之一,吸附材料的選擇、吸附條件的優(yōu)化以及吸附機制的探究已成為研究的熱點。燃煤飛灰是燃煤顆粒中所含礦物質(zhì)經(jīng)一系列變化而形成,具有比表面積大、表面能高及多活性點的特殊物理化學(xué)性質(zhì)。我國是以煤炭為主要能源的發(fā)展中國家,燃煤飛灰作為火力發(fā)電廠的一種工業(yè)固體廢物,年產(chǎn)生量巨大,實現(xiàn)飛灰的綜合利用、提高其再利用率,從而減少灰場飛灰貯存量,已成為當(dāng)務(wù)之急。飛灰具有性能穩(wěn)定、價格低廉的特點,為實現(xiàn)其作為吸附劑處理水體中的污染物提供了可能。本課題分別以電廠燃煤飛灰及其主要成分——氧化鋁為吸附劑,在改變吸附劑初始投加量、振蕩頻率、溫度和溶液pH值等條件下,研究了其對水溶液中三種典型抗生素——磺胺(SA)、四環(huán)素(TC)和諾氟沙星(NOR)的吸附特性,分析了各吸附體系的動力學(xué)、熱力學(xué),并在理論上通過分子動力學(xué)(Molecular dynamics, MD)簡化模型模擬研究了其作用機制,從而為水體中抗生素吸附材料的選擇提供了新的方法,也為實現(xiàn)電廠飛灰的資源化利用提供了新的途徑。研究結(jié)果表明：(1)氧化鋁及電廠飛灰吸附去除水體中抗生素的過程,吸附效果受多種因素的影響。在本實驗初始投加濃度范圍內(nèi)(0.1～5.0 g·L-1),吸附劑投加質(zhì)量濃度越高,吸附效果越明顯且平衡吸附量越低；在所研究的溫度范圍(15、25和35℃)內(nèi),吸附過程溫度控制在25℃時三種抗生素的吸附效果最佳；高頻率的振蕩可促進吸附；不同pH值條件下吸附劑對各種抗生素的吸附效果差異較大,SA、TC和NOR三種抗生素的吸附過程對應(yīng)不同的最佳pH值,分析認為這與溶液中不同pH值下抗生素和電廠飛灰中各種成分的溶解度、存在形態(tài)及表面電荷種類有關(guān)。(2)氧化鋁及電廠飛灰吸附三種典型抗生素的機制可通過吸附等溫線模型、動力學(xué)及熱力學(xué)分析解釋。不同吸附體系對Langmuir和Freundlich吸附等溫線模型復(fù)合情況不一致,吸附體系整體符合狀況不佳,可能與實際飛灰中的成分較為復(fù)雜及氧化鋁與抗生素的作用機制有關(guān)。三種抗生素所對應(yīng)的體系均較符合準(zhǔn)二級動力學(xué)模型,表明吸附過程的吸附速率與吸附質(zhì)濃度的平方成正比。所有吸附體系均符合顆粒內(nèi)擴散模型,表明氧化鋁、電廠飛灰吸附抗生素的過程受膜擴散和內(nèi)擴散的共同控制,且內(nèi)擴散速率常數(shù)kint隨著吸附劑質(zhì)量濃度的增加而遞減,這與傳質(zhì)過程的推動力及抗生素分子的擴散趨勢有關(guān)。(3)對于氧化鋁和電廠飛灰吸附水體中抗生素的體系,均有以下規(guī)律：同樣吸附劑投加濃度下,吸附劑對TC去除效果最佳,對NOR其次,對SA去除效果最不理想。MD模擬計算的能量數(shù)據(jù)也與這一結(jié)果相符,表明所設(shè)計的模擬體系具有合理性及可靠性。
[Abstract]:China is a big country in the production and use of antibiotics, and the irrational use or abuse of antibiotics is serious. Antibiotics have a long acting time and metabolism time. It is difficult to achieve effective degradation in the natural environment. Once entering the environment, it will seriously threaten human health and ecological safety. At present, antibiotics have become one of the most important pollutants in the water environment. Adsorption is one of the most important methods to treat antibiotics in water. The selection of adsorptive materials, the optimization of adsorptive conditions and the study of adsorptive mechanism have become the focus of research. China is a developing country with coal as the main energy source, Coal-fired Fly Ash as a kind of industrial solid waste of thermal power plant, the annual output is huge, realize the comprehensive utilization of fly ash, improve its reuse rate, thereby reducing the fly ash storage in ash yard, has become an urgent matter of the moment. It is possible to use it as an adsorbent for the treatment of pollutants in water. In this paper, three typical antibiotics, sulfonamide (SA) and tetra-sulfonamide (IV), were studied under the conditions of changing the initial dosage of adsorbent, oscillation frequency, temperature and pH value of solution. The adsorption characteristics of cyclinE (TC) and norfloxacin (NOR) were analyzed. The kinetics and thermodynamics of each adsorption system were analyzed. The mechanism of action was simulated by molecular dynamics (MD) simplified model. Thus a new method was provided for the selection of antibiotic adsorbent materials in water and the resource of fly ash from power plant was realized. The results show that: (1) the adsorption efficiency of alumina and fly ash is affected by many factors in the process of removing antibiotics from water. Within the temperature range (15, 25 and 35 degrees), when the temperature of the adsorption process is controlled at 25 degrees, the adsorption effect of the three antibiotics is the best; the high frequency oscillation can promote the adsorption; the adsorption effect of the adsorbent on various antibiotics under different pH conditions is quite different; the adsorption process of SA, TC and NOR three antibiotics corresponds to different optimal pH values, points. The mechanism of adsorption of Three Typical Antibiotics on alumina and fly ash can be explained by adsorption isotherm model, kinetic and thermodynamic analysis. Langmuir and Freundlic in different adsorption systems. The results show that the adsorption rate of the three antibiotics is equal to that of the adsorbate concentration. All adsorption systems conform to the intraparticle diffusion model, indicating that the process of adsorption of antibiotics by alumina and fly ash is controlled by both membrane diffusion and internal diffusion, and the internal diffusion rate constant kint decreases with the increase of adsorbent concentration, which is related to the driving force of mass transfer process and the diffusion trend of antibiotic molecules. 3) For the system of adsorbing antibiotics in water by fly ash of alumina and power plant, there are the following rules: under the same concentration of adsorbent, the adsorbent has the best effect on TC removal, and the second is NOR, and the effect on SA removal is the least ideal. The energy data calculated by MD simulation is also consistent with this result, which shows that the simulation system designed is reasonable and feasible. By sex.
【學(xué)位授予單位】：南京師范大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2015
【分類號】：X773
本文編號：2198315
[Abstract]:China is a big country in the production and use of antibiotics, and the irrational use or abuse of antibiotics is serious. Antibiotics have a long acting time and metabolism time. It is difficult to achieve effective degradation in the natural environment. Once entering the environment, it will seriously threaten human health and ecological safety. At present, antibiotics have become one of the most important pollutants in the water environment. Adsorption is one of the most important methods to treat antibiotics in water. The selection of adsorptive materials, the optimization of adsorptive conditions and the study of adsorptive mechanism have become the focus of research. China is a developing country with coal as the main energy source, Coal-fired Fly Ash as a kind of industrial solid waste of thermal power plant, the annual output is huge, realize the comprehensive utilization of fly ash, improve its reuse rate, thereby reducing the fly ash storage in ash yard, has become an urgent matter of the moment. It is possible to use it as an adsorbent for the treatment of pollutants in water. In this paper, three typical antibiotics, sulfonamide (SA) and tetra-sulfonamide (IV), were studied under the conditions of changing the initial dosage of adsorbent, oscillation frequency, temperature and pH value of solution. The adsorption characteristics of cyclinE (TC) and norfloxacin (NOR) were analyzed. The kinetics and thermodynamics of each adsorption system were analyzed. The mechanism of action was simulated by molecular dynamics (MD) simplified model. Thus a new method was provided for the selection of antibiotic adsorbent materials in water and the resource of fly ash from power plant was realized. The results show that: (1) the adsorption efficiency of alumina and fly ash is affected by many factors in the process of removing antibiotics from water. Within the temperature range (15, 25 and 35 degrees), when the temperature of the adsorption process is controlled at 25 degrees, the adsorption effect of the three antibiotics is the best; the high frequency oscillation can promote the adsorption; the adsorption effect of the adsorbent on various antibiotics under different pH conditions is quite different; the adsorption process of SA, TC and NOR three antibiotics corresponds to different optimal pH values, points. The mechanism of adsorption of Three Typical Antibiotics on alumina and fly ash can be explained by adsorption isotherm model, kinetic and thermodynamic analysis. Langmuir and Freundlic in different adsorption systems. The results show that the adsorption rate of the three antibiotics is equal to that of the adsorbate concentration. All adsorption systems conform to the intraparticle diffusion model, indicating that the process of adsorption of antibiotics by alumina and fly ash is controlled by both membrane diffusion and internal diffusion, and the internal diffusion rate constant kint decreases with the increase of adsorbent concentration, which is related to the driving force of mass transfer process and the diffusion trend of antibiotic molecules. 3) For the system of adsorbing antibiotics in water by fly ash of alumina and power plant, there are the following rules: under the same concentration of adsorbent, the adsorbent has the best effect on TC removal, and the second is NOR, and the effect on SA removal is the least ideal. The energy data calculated by MD simulation is also consistent with this result, which shows that the simulation system designed is reasonable and feasible. By sex.
【學(xué)位授予單位】：南京師范大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2015
【分類號】：X773
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，本文編號：2198315
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