本文選題：Fe_3O_4@SiO_2 + 功能化��； 參考：《浙江大學》2015年碩士論文

【摘要】：利用新穎、高效和易分離的功能化Fe304磁性納米材料去除水中的重金屬,已越來越受到研究者的關(guān)注。本文采用化學氧化法將問苯二胺單體(mPD)和對苯二胺鄰磺酸單體(SP)共聚包覆在納米Fe304@Si02表面上,制備出氨基、亞氨基、磺酸基等修飾的功能化磁性納米復合材料(Fe3O4@SiO2-mPD/SP).通過改變mPD/SP單體的比例進行共聚包覆,分別篩選出針對Pb(Ⅱ)和Cr(Ⅵ)去除的Fe3O4@SiO2-mPD/SP,并通過TEM、XRD、FTIR等手段對功能化改性前后的磁性納米復合材料進行表征,了解其形貌、結(jié)構(gòu)、化學組成、磁性特性及耐酸耐堿性等特征；考察了Fe3O4@SiO2-mPD/SP對Pb(Ⅱ)、Cr(Ⅵ)的選擇性吸附性能和影響因素,深入探討了Fe3O4@SiO2-mPD/SP對Pb(Ⅱ)、Cr(Ⅵ)重金屬離子的吸附機理；最后探索了Fe3O4@SiO2-mPD/SP的分離和重復利用性。通過X射線衍射、透射電鏡、紅外、熱重分析等表征手段,考察了功能化改性前后磁性納米復合材料的形貌、結(jié)構(gòu)、化學組成和磁性特性。通過表征發(fā)現(xiàn)Fe3O4@SiO2-mPD/SP保持了Fe3O4的尖晶石結(jié)構(gòu),具有良好的熱穩(wěn)定性和耐酸耐堿性,且磁響應(yīng)強度大,僅需30s就可從廢水中有效分離。磁性納米Fe3O4顆粒主要為粒徑20-30 nm的均勻球形顆粒,包裹在Fe3O4@SiO2表面的聚合物為mPD-SP的共聚物,而不是]mPD-mPD聚合物和SP-SP聚合物的簡單混合。通過調(diào)整mPD/S P比例對重金屬離子去除效果的研究,得出Pb(Ⅱ)和Cr(Ⅵ)去除的最優(yōu)mPD/SP共聚比例分別為95：5和50：50,Fe3O4@SiO2-mPD/SP(95:5)和Fe3O4@SiO2-mPD/SP(50:50)對Pb(Ⅱ)和Cr(Ⅵ)的飽和吸附量分別為83.23和119.06 mg g-1。Fe3O4@SiO2-mPD/SP(95:5)對Pb(Ⅱ)的吸附速率較快,反應(yīng)5min即可達到吸附平衡；而Fe3O4@SiO2-mPD/SP(50:50)對Cr(Ⅵ)的吸附在前30 min較快,但需要6 h左右才逐漸達到吸附平衡。Fe3O4@SiO2-mPD/SP(95:5)和Fe3O4@SiO2-mPD/SP(50:50)對Pb(Ⅱ)和 Cr(Ⅵ)的吸附過程均符合準二級動力學方程和Freundlich模型；熱力學研究表明,Fe3O4@SiO2-mPD/SP(95:5)和Fe3O4@SiO2-mPD/SP(50:50)對Pb(Ⅱ)和 Cr(Ⅵ)的吸附過程均為自發(fā)的吸熱過程；溶液pH值對Fe3O4@SiO2-mPD/SP(95:5)和Fe3O4@SiO2-mPD/SP(50:50)的吸附作用均有顯著的影響；而天然有機物、競爭性離子對Fe3O4@SiO2-mPD/SP(95:5)和Fe3O4@SiO2-mPD/SP(50:50)的吸附作用無顯著影響；Fe3O4@SiO2-mPD/SP(95:5)和Fe3O4@SiO2-mPD/SP(50:50)均具有較好的分離再生和循環(huán)使用性能。功能化磁性納米復合材料Fe3O4@SiO2-mPD/SP(95:5)和Fe3O4@SiO2-mPD/SP(50:50)可分別從多種重金屬離子共存的廢水中選擇性地將Pb(Ⅱ)和Cr(Ⅵ)高效去除。通過測量Fe3O4@SiO2-mPD/SP(95:5) 和 Fe3O4@SiO2-mPD/SP(50:50)吸附Pb(Ⅱ)和Cr(Ⅵ)前后溶液pH值的變化,對吸附Pb(Ⅱ)和Cr(Ⅵ)前后的功能化磁性納米Fe3O4材料進行FTR和XPS表征,考察Fe3O4@SiO2-mPD/SP(50:50)吸附Cr(Ⅵ)過程中剩余總Cr和Cr(Ⅵ)濃度隨吸附時間的變化,可以得出Fe3O4@SiO2-mPD/SP對 Pb(Ⅱ)和Cr(Ⅵ)的吸附機理主要包括：離子交換、絡(luò)合吸附、氧化還原反應(yīng)、靜電吸引和物理吸附等過程。其中Fe3O4@SiO2-mPD/SP(95:5)對Pb(Ⅱ)的吸附過程,絡(luò)合吸附占主導作用,而Fe3O4@SiO2-mPD/SP(50:50)對 Cr(Ⅵ)的吸附過程,絡(luò)合吸附和氧化還原反應(yīng)占主導作用。
[Abstract]:The use of novel, efficient and easy separation functional Fe304 magnetic nanomaterials to remove heavy metals in water has attracted more and more attention. In this paper, a chemical oxidation method was used to encapsulate two amines (mPD) and phenylene two amine o sulfonic acid monomer (SP) on the surface of nanoscale Fe304@ Si02 to prepare amino, subamino, sulfonic acid groups and so on. Functionalized Magnetic Nanocomposites (Fe3O4@SiO2-mPD/SP). By modifying the proportion of mPD/SP monomers to encapsulate, the Fe3O4@SiO2-mPD/SP for the removal of Pb (II) and Cr (VI) was screened, and the Magnetic Nanocomposites before and after functional modification were characterized by TEM, XRD, FTIR and so on, and their morphology, structure and chemistry were understood. The composition, magnetic properties, acid resistance and alkali resistance, the selective adsorption properties and influence factors of Fe3O4@SiO2-mPD/SP on Pb (II), Cr (VI), and the adsorption mechanism of Fe3O4@SiO2-mPD/SP on Pb (II), Cr (VI) heavy metal ions, and the separation and reutilization of Fe3O4@SiO2-mPD/SP are explored. Through X ray diffraction, through the X-ray diffraction, and through the X ray diffraction. The morphology, structure, chemical composition and magnetic properties of the Magnetic Nanocomposites before and after functional modification were investigated by means of electron microscopy, infrared and thermogravimetric analysis. It was found that Fe3O4@SiO2-mPD/SP maintained the spinel structure of Fe3O4, and had good thermal stability, acid resistance and alkali resistance, and the magnetic response intensity was great, only 30s could be used. The magnetic nano Fe3O4 particles are mainly homogeneous spherical particles with a particle size of 20-30 nm, and the polymer of the Fe3O4@SiO2 surface is a copolymer of mPD-SP, not a simple mixture of]mPD-mPD and SP-SP polymers. By adjusting the ratio of mPD/S P to the removal of heavy metal ions, Pb (II) and Cr (VI) are obtained. The optimal mPD/SP copolymerization ratio is 95:5 and 50:50 respectively. The adsorption capacity of Pb (95:5) and Fe3O4@SiO2-mPD/SP (50:50) to Pb (II) and Cr (VI) is 83.23 and 119.06 mg g-1.Fe3O4@SiO2-mPD/SP (95:5) has a faster adsorption rate. The adsorption of (VI) is faster in the front 30 min, but it takes about 6 h to gradually reach the adsorption equilibrium.Fe3O4@SiO2-mPD/SP (95:5) and Fe3O4@SiO2-mPD/SP (50:50) for Pb (II) and Cr (VI) adsorption processes that conform to the quasi two kinetic equation and Freundlich model. The adsorption process of and Cr (VI) were both spontaneous endothermic processes, and the pH value of the solution had a significant effect on the adsorption of Fe3O4@SiO2-mPD/SP (95:5) and Fe3O4@SiO2-mPD/SP (50:50), while the natural organic matter, the competitive ions had no significant influence on the adsorption of Fe3O4@SiO2-mPD/SP (95:5) and Fe3O4@ SiO2-mPD/SP (50:50); P (95:5) and Fe3O4@SiO2-mPD/SP (50:50) have good separation and recycling performance. Functional magnetic nanocomposites, Fe3O4@SiO2-mPD/SP (95:5) and Fe3O4@SiO2-mPD/SP (50:50), can selectively remove Pb (II) and Cr (VI) from a variety of heavy metal ions. By measuring Fe3O4@SiO2-mPD/SP (95:5) The changes in the pH value of the solution before and after the adsorption of Pb (II) and Cr (VI) with Fe3O4@SiO2-mPD/SP (50:50) and the adsorption of Pb (II) and Cr (VI) on the functional magnetic nanoscale Fe3O4 materials before and after the adsorption of Cr (VI) are characterized by FTR and XPS, and the changes in the concentration of residual total and (VI) in the process of Fe3O4@SiO2-mPD/SP (50:50) adsorption (VI) can be obtained. The adsorption mechanism of /SP on Pb (II) and Cr (VI) mainly includes the processes of ion exchange, complex adsorption, redox reaction, electrostatic attraction and physical adsorption. The adsorption process of Fe3O4@SiO2-mPD/SP (95:5) to Pb (II), the dominant effect of complex adsorption, and the adsorption process of Fe3O4@ SiO2-mPD/SP (50:50) to Cr (VI), complex adsorption and oxidation The primary reaction is dominant.
【學位授予單位】：浙江大學
【學位級別】：碩士
【學位授予年份】：2015
【分類號】：TB33;X703

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