模板法水滑石微球的可控制备及其性能研究
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摘要
随着材料科学与技术的发展,结构可控的复合材料由于其一系列可调的优异性能,从而在新型催化剂载体、大分子聚合物分离膜、生物医药材料和药物载体等新功能材料开发中显示出诱人的应用前景。在各种复合材料的制备方法中,模板法因其具有众多优点而被广泛采用。层状双羟基复合金属氧化物(LDHs)是一类可人工合成的、具有二维结构的阴离子型层状功能材料,它们由带有正电荷的主体层板、平衡正电荷的层间阴离子客体和部分水分子组成。其层板元素组成和层间阴离子种类可调的特点能够衍生出很多具有不同物理化学特性的功能性组装体,因此有可能作为高性能催化材料、分离材料、吸附材料、功能性助剂材料等获得应用。目前,在该研究领域的工作中,LDHs类材料通常是以粉体或薄膜形式使用,这样就会在实际应用过程中产生很多问题。因此,关于LDHs类材料的形貌可控制备具有明显的科学意义和实际应用价值。
本论文以模板法制备LDHs复合微球材料为目的,重点研究了不同模板制备LDHs的形貌控制,以及对所得到的MgAl-LDHs材料在吸附及药物缓释性能方面的初步研究。具体的研究内容和实验结果如下：
1.以高电荷、磺酸根改性的聚苯乙烯为模板,表面原位生长MgAl-LDHs壳层,其壳层可表现出花状结构,LDHs包覆层的片状结构大小可通过不同制备方法进行调控；
2.通过共沉淀方法制备得到MgAl-LDHs@sPS,初步研究其对阴离子的吸附性能；
3.将磁性纳米粒子包覆于MgAl-LDHs@sPS复合材料内,最后得到的异质复合微球磁性大小为10.23 emu／g,通过离子交换作用,将布洛芬(IBU)插入MgAl-LDHs@Fe3O4层间,初步研究了IBU在pH6.8的PBS中的释放行为,随着释放时间的增加,样品的累积释放量逐渐增加直至达到平衡；
4.以SiO2为模板,通过模板表面羟基与MgAl-LDHs层板羟基的氢键作用,原位生长MgAl-LDHs壳层,包覆层粒子大小通过不同制备方法调控。
Well-controlled nanostructures obtained via template-directed synthesis have generated diverse scientific and technological interests, since the tunable morphology is of utmost importance for optimization in many potential areas of applications such as energy conversion, electronics, catalysis, optics, chemical sensing, and medicine. The ability to control morphologies of hierarchical spheres often combines fascinating shapes with remarkable properties, which requires a high level of control of structure, size, morphology, and orientation by assembly at template surfaces. Layered double hydroxides (LDHs), also known as hydrotalcite-like layered clays, have widely been investigated as a class of anionic lamellar multifunctional materials. Important advances in LDH morphology have been made in the past, mainly focusing on microsized LDHs such as spheres, curved belts, and hydrothermally synthesized LDH films with microsized LDH platelets oriented perpendicularly or horizontally to the underlying metal or surface-modified substrates. Spherical structures are of particular interest for a number of different applications, such as catalysts, sorbents, lithium-ion battery electrodes, and carriers for cellular drug and gene delivery. Reports of the deliberate control of colloidal LDH micro/nanostructures are, however, still quite scarce.
In this present study, we report on preparation of LDH shell spheres with controllable morphologies using a protocol combining typical coprecipitation and hard template. Preliminary investigations on the drug's absorption and releasing properties of the obtained shell spheres were also performed. MgAl-LDHs. The obtained results are presented as follows.
1. Flower-like MgAl-LDH microsphere was prepared using sulfonated polystyrene beads. Controllable morphology of LDH shell sphere is achieved readily by varying preparation conditions such as aging durations and temperatures. Removal toxical heavy metal anion was further investigation with the as-prepared flower-like MgAl-LDH microsphere.
2. IBU drug molecule containing MgAl-LDHs@sPS microsphere was prepared with Fe3O4 magnetic core. Evluation of drug releasing shows that the release of IBU in PBS (pH=6.8) is increased with the increasing releasing time and gradually reachs the balance.
3. Using SiO2 as the template, MgAl-LDHs@SiO2 compostie microsphere was synthesized using a scalable procedure. The dimentional size and layer metal types were tuned on the basis of the flexibility to vary LDH composition.
本论文以模板法制备LDHs复合微球材料为目的,重点研究了不同模板制备LDHs的形貌控制,以及对所得到的MgAl-LDHs材料在吸附及药物缓释性能方面的初步研究。具体的研究内容和实验结果如下：
1.以高电荷、磺酸根改性的聚苯乙烯为模板,表面原位生长MgAl-LDHs壳层,其壳层可表现出花状结构,LDHs包覆层的片状结构大小可通过不同制备方法进行调控；
2.通过共沉淀方法制备得到MgAl-LDHs@sPS,初步研究其对阴离子的吸附性能；
3.将磁性纳米粒子包覆于MgAl-LDHs@sPS复合材料内,最后得到的异质复合微球磁性大小为10.23 emu／g,通过离子交换作用,将布洛芬(IBU)插入MgAl-LDHs@Fe3O4层间,初步研究了IBU在pH6.8的PBS中的释放行为,随着释放时间的增加,样品的累积释放量逐渐增加直至达到平衡；
4.以SiO2为模板,通过模板表面羟基与MgAl-LDHs层板羟基的氢键作用,原位生长MgAl-LDHs壳层,包覆层粒子大小通过不同制备方法调控。
Well-controlled nanostructures obtained via template-directed synthesis have generated diverse scientific and technological interests, since the tunable morphology is of utmost importance for optimization in many potential areas of applications such as energy conversion, electronics, catalysis, optics, chemical sensing, and medicine. The ability to control morphologies of hierarchical spheres often combines fascinating shapes with remarkable properties, which requires a high level of control of structure, size, morphology, and orientation by assembly at template surfaces. Layered double hydroxides (LDHs), also known as hydrotalcite-like layered clays, have widely been investigated as a class of anionic lamellar multifunctional materials. Important advances in LDH morphology have been made in the past, mainly focusing on microsized LDHs such as spheres, curved belts, and hydrothermally synthesized LDH films with microsized LDH platelets oriented perpendicularly or horizontally to the underlying metal or surface-modified substrates. Spherical structures are of particular interest for a number of different applications, such as catalysts, sorbents, lithium-ion battery electrodes, and carriers for cellular drug and gene delivery. Reports of the deliberate control of colloidal LDH micro/nanostructures are, however, still quite scarce.
In this present study, we report on preparation of LDH shell spheres with controllable morphologies using a protocol combining typical coprecipitation and hard template. Preliminary investigations on the drug's absorption and releasing properties of the obtained shell spheres were also performed. MgAl-LDHs. The obtained results are presented as follows.
1. Flower-like MgAl-LDH microsphere was prepared using sulfonated polystyrene beads. Controllable morphology of LDH shell sphere is achieved readily by varying preparation conditions such as aging durations and temperatures. Removal toxical heavy metal anion was further investigation with the as-prepared flower-like MgAl-LDH microsphere.
2. IBU drug molecule containing MgAl-LDHs@sPS microsphere was prepared with Fe3O4 magnetic core. Evluation of drug releasing shows that the release of IBU in PBS (pH=6.8) is increased with the increasing releasing time and gradually reachs the balance.
3. Using SiO2 as the template, MgAl-LDHs@SiO2 compostie microsphere was synthesized using a scalable procedure. The dimentional size and layer metal types were tuned on the basis of the flexibility to vary LDH composition.
引文
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