【摘要】：本文利用含膨脹晶層礦物及其有機插層納米復合物對水溶液中的鄰苯二甲酸酯進行了吸附實驗研究。根據(jù)含膨脹晶層礦物層間水化陽離子層的可交換性和吸附性,采用水解-插層復合法,用具有相同結構但不同烷基碳鏈長度的系列季銨鹽制備CnTA+/蒙脫石納米復合物和CnTA+/蛭石納米復合物,并對水溶液中4種鄰苯二甲酸酯類物質進行吸附實驗。通過XRD、FT-IR等分析測試手段及物理性能測試對CnTA+/蒙脫石、蛭石納米復合物進行分析表征,考察了吸附反應時間、初始p H值和反應溫度對吸附效果的影響,并探討了季銨鹽烷基碳鏈鏈長和用量對制得的CnTA+/蒙脫石、蛭石納米復合物吸附水溶液中鄰苯二甲酸酯類物質效果的影響。通過對吸附結果進行吸附熱力學和動力學方程擬合,揭示吸附反應機理。結果表明:相同用量的季銨鹽制備的CnTA+/蒙脫石、蛭石納米復合物的層間距d0 0 1值隨季銨鹽的鏈長增長而增大;相同鏈長的季銨鹽制備的CnTA+/蒙脫石、蛭石納米復合的層間距d0 0 1值隨用量的增加而增大。季銨鹽陽離子在蒙脫石、蛭石層間因用量及烷基碳鏈長度的不同而形成不同的排布模式。經(jīng)有機插層后的CnTA+/蒙脫石、蛭石納米復合物對PAEs的吸附能力大于原蒙脫石、蛭石。隨著季銨鹽的用量和季銨鹽烷基碳鏈鏈長的增加,CnTA+/蒙脫石納米復合物和CnTA+/蛭石納米復合物對PAEs的去除率先增加后減小。經(jīng)1.0CEC季銨鹽用量插層后的納米復合物對PAEs的吸附效果最好。PAEs在CnTA+/蒙脫石納米復合物和CnTA+/蛭石納米復合物上的吸附與PAEs物質分子大小及疏水性有關。其中吸附量隨著吸附時間的增加而增加,CnTA+/蒙脫石納米復合物和Cn TA+/蛭石納米復合物對PAEs的吸附作用基本不會受到初始p H的影響。溫度對吸附效果有一定影響,但影響不大。隨著溫度的升高吸附去除率減小。采用Langmuir吸附等溫模型以及Freundlich吸附等溫模型對吸附結果進行擬合,兩種等溫吸附模型均對吸附過程進行擬合。PAEs在鈉蒙脫石和蛭石原樣上的吸附主要是以表面吸附為主,其中還包括離子交換吸附等化學吸附。在CnTA+/蒙脫石、蛭石納米復合物上的吸附主要是有機質的分配作用,表面吸附也是吸附的機制之一。吸附過程不能用擬一級動力學吸附模型進行擬合,但符合擬二級動力學吸附模型。
[Abstract]:In this paper, the adsorption of phthalates in aqueous solution was studied by using expanded crystal layer minerals and their organic intercalation nanocomposites. According to the exchangeability and adsorbability of the hydrated cationic layer between the mineral layers containing expanded crystal layer, the hydrolysis-intercalation composite method was adopted. CnTA / montmorillonite nanocomposites and CnTA / vermiculite nanocomposites were prepared by using a series of quaternary ammonium salts with the same structure but different alkyl carbon chain lengths. The adsorption experiments of four phthalate esters in aqueous solution were carried out. CnTA / montmorillonite and vermiculite nanocomposites were characterized by XRD,FT-IR and physical properties. The effects of adsorption time, initial pH value and reaction temperature on the adsorption were investigated. The effects of alkyl chain length and amount of quaternary ammonium salt on the adsorption of phthalates in aqueous solution by CnTA / montmorillonite and vermiculite nanocomposites were investigated. The adsorption reaction mechanism was revealed by fitting the adsorption thermodynamic and kinetic equations. The results showed that the interlayer spacing of CnTA / montmorillonite prepared with the same amount of quaternary ammonium salt increased with the increase of chain length of quaternary ammonium salt. For CnTA / montmorillonite prepared by quaternary ammonium salt with the same chain length, the interlayer spacing of vermiculite nanocomposite increased with the increase of dosage. Quaternary ammonium salt cations in montmorillonite and vermiculite layers have different distribution patterns due to different dosage and length of alkyl carbon chain. After organic intercalation of CnTA / montmorillonite, the adsorption ability of vermiculite nanocomposites to PAEs was higher than that of original montmorillonite and vermiculite. With the increase of quaternary ammonium salt content and alkyl chain length of quaternary ammonium salt, the removal of PAEs by CnTA / montmorillonite nanocomposites and CnTA / vermiculite nanocomposites increased first and then decreased. The adsorption of PAEs on CnTA / montmorillonite nanocomposites and CnTA / vermiculite nanocomposites was related to the molecular size and hydrophobicity of PAEs. The adsorption capacity increased with the increase of adsorption time. The adsorption of PAEs by CnTA / montmorillonite nanocomposites and Cn TA / vermiculite nanocomposites was not affected by the initial pH. Temperature has a certain effect on adsorption, but it has little effect. The adsorption removal rate decreases with the increase of temperature. Langmuir adsorption isotherm model and Freundlich adsorption isotherm model were used to fit the adsorption results. The adsorption process was fitted by two isothermal adsorption models. The adsorption of PAEs on sodium montmorillonite and vermiculite samples was mainly surface adsorption. It also includes chemical adsorption such as ion exchange adsorption. In CnTA / montmorillonite, the adsorption on vermiculite nanocomposites is mainly due to the distribution of organic matter, and surface adsorption is one of the mechanisms of adsorption. The adsorption process can not be fitted by the pseudo-first-order kinetic adsorption model, but it accords with the pseudo-second-order kinetic adsorption model.
【學位授予單位】：西南科技大學
【學位級別】：碩士
【學位授予年份】：2015
【分類號】：X592;O647.3

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