類水滑石復(fù)合材料的合成及其在環(huán)境毒物方面的應(yīng)用
發(fā)布時間:2018-08-04 21:24
【摘要】:類水滑石(Layered Double Hydroxides,LDHs),由于其特殊的層狀結(jié)構(gòu),在催化,光催化,吸附,電化學(xué),生物技術(shù)等方面引起研究者們極大的興趣。作為一種無機層狀材料,LDHs是由層間陰離子及帶正電荷層板堆積而成的化合物。而層間作用力為一種弱作用力,因此LDHs展現(xiàn)出了優(yōu)秀的層間陰離子交換能力。由于類水滑石的陰離子可交換性和生物相容性使他們能夠插入具有高載荷能力陰離子活性分子,這在藥物輸送方面有很好的應(yīng)用。另外,因為LDHs層板間金屬離子的可調(diào)性,可以在晶體結(jié)構(gòu)中摻雜一些功能性離子,例如稀土金屬離子,使其材料帶有熒光性能。目前,應(yīng)用LDHs作為一種吸附劑選擇性吸附陰離子環(huán)境污染物已經(jīng)引起極大的關(guān)注。另外LDHs還可以作為一種優(yōu)秀的半導(dǎo)體載體,在其表面負載上AgX(X=Br,Cl)和Ag3PO4等半導(dǎo)體。把這種復(fù)合材料應(yīng)用到環(huán)境中可以達到吸附和降解污染物的雙重效果。本文以LDHs為模板,利用其陰離子交換能力和層板間金屬離子的可調(diào)性,分別合成了納米Ag和萬古霉素,AgCl,Ag3PO4和Eu2+摻雜的復(fù)合材料,并將其應(yīng)用于熒光標(biāo)記和殺滅細菌,光催化降解環(huán)境有機污染物。具體工作主要分為以下三個方面:(1)以Zn-Al LDHs納米片為基底材料,通過葡萄糖還原Ag+和陰離子交換法,成功在Zn-Al LDHs表面上修飾上納米銀和萬古霉素分子;所制備的萬古霉素和納米銀修飾的類水滑石納米片不僅對細菌具有選擇性吸附富集,而且還具有很好的殺菌性能。對所得產(chǎn)物用透射電子顯微鏡,EDS能譜,FT-IR光譜進行表征。結(jié)果表明,30納米的銀顆粒及萬古霉素分子均勻的附著在類水滑石層狀結(jié)構(gòu)的表面上。由于它們的特性,復(fù)合材料可以同時有效的捕獲和殺滅細菌。與LDHs,Van/LDHs,Ag/LDHs對大腸桿菌(革蘭氏陰性菌)和金黃色葡萄球菌(革蘭氏陽性菌)殺菌性能比較,Van-Ag/LDHs表現(xiàn)出更優(yōu)異的殺菌性能。結(jié)合上Van和Ag的LDHs復(fù)合材料克服了萬古霉素只對陽性細菌具有殺菌作用和納米銀分散性、穩(wěn)定性差的缺點。合成的納米復(fù)合材料在滅菌方面具有廣泛的應(yīng)用前景。(2)通過兩步合成法成功制備了Van和TA修飾的Eu摻雜的LDHs復(fù)合材料。首先,通過陰離子交換法制備了對苯二甲酸鈉改性的銪摻雜Zn-Al LDHs,然后再在材料表面修飾上能夠識別捕獲細菌的萬古霉素分子。對所得產(chǎn)物用X射線粉末衍射,高分辨透射顯微鏡,傅里葉變換紅外光譜,熒光光譜進行了表征。結(jié)果表明萬古霉素改性的銪摻雜類水滑石納米片層材料的粒徑在50 nm左右而且材料具有較好的熒光性能。由于萬古霉素分子對細菌的識別捕獲能力,Van和TA修飾的銪摻雜的類水滑石展現(xiàn)出了較好的熒光標(biāo)記細菌性能。因此,Van-TA-Eu-LDHs復(fù)合納米材料可能在生物領(lǐng)域如生物分子標(biāo)記和細胞成像方面有廣泛的應(yīng)用。(3)通過核殼結(jié)構(gòu)的設(shè)計,成功合成了一種新型的可見光催化劑Fe3O4@LDHs@Ag/Ag3PO4。以層間插入PO43-的LDHs磁性微球作為媒介,然后再在Fe3O4@LDHs上面合成Ag3PO4納米顆粒。對所得產(chǎn)物用X射線粉末衍射,X射線光電子能譜,電感耦合等離子體原子發(fā)射光譜,高分辨率透射電鏡,場發(fā)射掃描電子顯微鏡進行了表征。實驗結(jié)果表明,LDHs和Ag/Ag3PO4納米材料成功包覆到Fe3O4表面上。其中,在Fe3O4@LDHs表面上合成Ag/Ag3PO4過程中,PO43-插層的LDHs起到了重要的作用。通過光催化降解有機染料亞甲基藍的實驗表明,在可見光的激發(fā)下,光催化劑Fe3O4@LDH@Ag/Ag3PO4對有機污染物具有優(yōu)異的光催化降解性能,并且利用復(fù)合材料中Fe3O4的磁性特征,通過外加磁場的方式從廢水中回收復(fù)合材料。制備的Fe3O4@LDHs@Ag3PO4/Ag是一種性能優(yōu)異可回收的復(fù)合光催劑。
[Abstract]:Layered Double Hydroxides (LDHs), due to its special layered structure, has aroused great interest in catalysis, photocatalysis, adsorption, electrochemistry, and biotechnology. As an inorganic layered material, LDHs is a compound of interlayer anions and positive charge laminates. The interlayer force is a kind of compound. Weak forces, so LDHs shows excellent interlayer anion exchange ability. Because of the anion exchangeability and biocompatibility of the hydrotalcite, they can insert high load capacity anionic active molecules, which have good application in drug delivery. In addition, because of the tunability of LDHs interplate metal ions, it can be used. The crystal structure is doped with some functional ions, such as rare earth metal ions, which make the materials with fluorescent properties. At present, the application of LDHs as an adsorbent to selectively adsorb anionic environmental pollutants has attracted great attention. In addition, LDHs can also be used as an excellent semi conductor carrier, AgX (X=Br, Cl) and Ag3 on its surface load. PO4 and other semiconductors. The application of this composite material to the environment can achieve the dual effect of adsorption and degradation of pollutants. In this paper, the composite materials of nano Ag and vancomycin, vancomycin, AgCl, Ag3PO4 and Eu2+ are synthesized by using LDHs as a template, and the composite materials are synthesized by the anion exchange capacity and the interlaminar metal ions. Light labeling and killing bacteria and photocatalytic degradation of environmental organic pollutants. The main work is divided into three aspects: (1) the nano silver and vancomycin are successfully modified on the surface of Zn-Al LDHs by glucose reduction Ag+ and anion exchange method, with Zn-Al LDHs nanoscale as the base material; and the prepared vancomycin and nanosilver are prepared. The ornament hydrotalcite nanoparticles not only have selective adsorption and enrichment, but also have good bactericidal properties. The obtained products are characterized by transmission electron microscopy, EDS spectrum and FT-IR spectra. The results show that the 30 nanometer silver particles and vancomycin molecules are uniformly attached to the surface of the layered structure of hydrotalcite. Compared with LDHs, Van/LDHs, Ag/LDHs for the bactericidal performance of Escherichia coli (Gram-negative bacteria) and Staphylococcus aureus (Gram-positive bacteria), Van-Ag/LDHs showed better bactericidal performance compared with LDHs, Van/LDHs, and Staphylococcus aureus (Gram-positive bacteria). The LDHs composite on Van and Ag overcame vancomycin only against the bactericidal performance. The positive bacteria have the disadvantages of bactericidal action and dispersion of nano silver and poor stability. The synthesized nanocomposites have extensive application prospects in sterilization. (2) the LDHs composite doped with Van and TA modified by Eu was successfully prepared by two step synthesis. The Zn-Al LDHs is doped and then the vancomycin molecules can be identified on the surface of the material. The obtained products are characterized by X ray powder diffraction, high resolution transmission microscopy, Fourier transform infrared spectroscopy, and fluorescence spectra. The results show that the particle size of the vancomycin modified europium doped hydrotalcite nanomaterials is in the particle size. It is about 50 nm and the material has good fluorescent properties. The Van and TA modified europium like hydrotalcite exhibits better fluorescent labeling bacteria because of the ability of vancomycin molecules to identify bacteria. Therefore, Van-TA-Eu-LDHs composite nanomaterials may have a biological domain, such as biomolecular markers and cell imaging. 3. (3) through the design of nuclear shell structure, a new type of visible light catalyst Fe3O4@LDHs@Ag/Ag3PO4. was successfully synthesized by inserting PO43- LDHs magnetic microspheres between layers as medium, and then synthesizing Ag3PO4 nanoparticles on Fe3O4@LDHs. The obtained products were diffracted by X ray powder, X ray photoelectron spectroscopy, inductively coupled and so on. The plasma atomic emission spectroscopy, high resolution transmission electron microscopy, and field emission scanning electron microscopy were characterized. The results showed that the LDHs and Ag/Ag3PO4 nanomaterials were successfully coated on the Fe3O4 surface. In the process of synthesizing Ag/Ag3PO4 on the Fe3O4@LDHs surface, the PO43- intercalated LDHs played an important role. The photocatalytic degradation was achieved by photocatalytic degradation. The experimental dye methylene blue experiment shows that the photocatalyst Fe3O4@LDH@Ag/Ag3PO4 has excellent photocatalytic degradation performance on organic pollutants under the excitation of visible light, and uses the magnetic properties of Fe3O4 in the composite material to recover the composite materials from the wastewater by the external magnetic field. The prepared Fe3O4@LDHs@Ag3PO4/Ag is a kind of performance. Excellent recoverable compound light accelerating agent.
【學(xué)位授予單位】:山東農(nóng)業(yè)大學(xué)
【學(xué)位級別】:碩士
【學(xué)位授予年份】:2015
【分類號】:TB33;O643.36
本文編號:2165202
[Abstract]:Layered Double Hydroxides (LDHs), due to its special layered structure, has aroused great interest in catalysis, photocatalysis, adsorption, electrochemistry, and biotechnology. As an inorganic layered material, LDHs is a compound of interlayer anions and positive charge laminates. The interlayer force is a kind of compound. Weak forces, so LDHs shows excellent interlayer anion exchange ability. Because of the anion exchangeability and biocompatibility of the hydrotalcite, they can insert high load capacity anionic active molecules, which have good application in drug delivery. In addition, because of the tunability of LDHs interplate metal ions, it can be used. The crystal structure is doped with some functional ions, such as rare earth metal ions, which make the materials with fluorescent properties. At present, the application of LDHs as an adsorbent to selectively adsorb anionic environmental pollutants has attracted great attention. In addition, LDHs can also be used as an excellent semi conductor carrier, AgX (X=Br, Cl) and Ag3 on its surface load. PO4 and other semiconductors. The application of this composite material to the environment can achieve the dual effect of adsorption and degradation of pollutants. In this paper, the composite materials of nano Ag and vancomycin, vancomycin, AgCl, Ag3PO4 and Eu2+ are synthesized by using LDHs as a template, and the composite materials are synthesized by the anion exchange capacity and the interlaminar metal ions. Light labeling and killing bacteria and photocatalytic degradation of environmental organic pollutants. The main work is divided into three aspects: (1) the nano silver and vancomycin are successfully modified on the surface of Zn-Al LDHs by glucose reduction Ag+ and anion exchange method, with Zn-Al LDHs nanoscale as the base material; and the prepared vancomycin and nanosilver are prepared. The ornament hydrotalcite nanoparticles not only have selective adsorption and enrichment, but also have good bactericidal properties. The obtained products are characterized by transmission electron microscopy, EDS spectrum and FT-IR spectra. The results show that the 30 nanometer silver particles and vancomycin molecules are uniformly attached to the surface of the layered structure of hydrotalcite. Compared with LDHs, Van/LDHs, Ag/LDHs for the bactericidal performance of Escherichia coli (Gram-negative bacteria) and Staphylococcus aureus (Gram-positive bacteria), Van-Ag/LDHs showed better bactericidal performance compared with LDHs, Van/LDHs, and Staphylococcus aureus (Gram-positive bacteria). The LDHs composite on Van and Ag overcame vancomycin only against the bactericidal performance. The positive bacteria have the disadvantages of bactericidal action and dispersion of nano silver and poor stability. The synthesized nanocomposites have extensive application prospects in sterilization. (2) the LDHs composite doped with Van and TA modified by Eu was successfully prepared by two step synthesis. The Zn-Al LDHs is doped and then the vancomycin molecules can be identified on the surface of the material. The obtained products are characterized by X ray powder diffraction, high resolution transmission microscopy, Fourier transform infrared spectroscopy, and fluorescence spectra. The results show that the particle size of the vancomycin modified europium doped hydrotalcite nanomaterials is in the particle size. It is about 50 nm and the material has good fluorescent properties. The Van and TA modified europium like hydrotalcite exhibits better fluorescent labeling bacteria because of the ability of vancomycin molecules to identify bacteria. Therefore, Van-TA-Eu-LDHs composite nanomaterials may have a biological domain, such as biomolecular markers and cell imaging. 3. (3) through the design of nuclear shell structure, a new type of visible light catalyst Fe3O4@LDHs@Ag/Ag3PO4. was successfully synthesized by inserting PO43- LDHs magnetic microspheres between layers as medium, and then synthesizing Ag3PO4 nanoparticles on Fe3O4@LDHs. The obtained products were diffracted by X ray powder, X ray photoelectron spectroscopy, inductively coupled and so on. The plasma atomic emission spectroscopy, high resolution transmission electron microscopy, and field emission scanning electron microscopy were characterized. The results showed that the LDHs and Ag/Ag3PO4 nanomaterials were successfully coated on the Fe3O4 surface. In the process of synthesizing Ag/Ag3PO4 on the Fe3O4@LDHs surface, the PO43- intercalated LDHs played an important role. The photocatalytic degradation was achieved by photocatalytic degradation. The experimental dye methylene blue experiment shows that the photocatalyst Fe3O4@LDH@Ag/Ag3PO4 has excellent photocatalytic degradation performance on organic pollutants under the excitation of visible light, and uses the magnetic properties of Fe3O4 in the composite material to recover the composite materials from the wastewater by the external magnetic field. The prepared Fe3O4@LDHs@Ag3PO4/Ag is a kind of performance. Excellent recoverable compound light accelerating agent.
【學(xué)位授予單位】:山東農(nóng)業(yè)大學(xué)
【學(xué)位級別】:碩士
【學(xué)位授予年份】:2015
【分類號】:TB33;O643.36
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