功能化碳纳米管材料体系的构建及其生物医学基础与吸附应用研究

发布时间：2018-03-24 23:27

本文选题：碳纳米管　切入点：功能化　出处：《南京航空航天大学》2015年博士论文

【摘要】：以碳纳米管为典型的纳米材料因其独特的结构以及奇异的性质,在各产业领域内创造了巨大的应用前景,正潜移默化地推动着一场新产业革命,逐渐渗透进入并改变了人们的生活。如在生物医学领域中,基于碳纳米管发展起来的生物成像、载药、检测等纳米医学技术,有望为肿瘤的早期诊断与治疗方法的突破提供新的思路;另外,碳纳米管作为吸附材料显示出相较于传统吸附剂更加高效的应用效率,有望为目前日益严重的各类废物处置提供帮助。然而,在碳纳米管等纳米材料大规模用于产业化应用的道路中,仍然有许多问题亟待解决或加以改进。本论文正是在这样一个大背景下,针对某些具体应用中的特定问题,设计构建了功能化的碳纳米管材料体系,主要研究了其在生物医学应用中的一些基础问题以及作为吸附材料方向上的初步应用,同时也从纳米材料的构建方法角度作了讨论。具体研究内容与结果阐述如下:(1)发展了以水溶性壳聚糖修饰为基础的碳纳米管生物功能化方法,一方面改善了碳纳米管的固有缺点,为其在生物医学领域的应用提供前提条件;另一方面,基于壳聚糖的修饰,在碳纳米管体系中可以后续引入多种生物功能性分子,如荧光标记物、肿瘤靶向分子,以及各类药物等。经壳聚糖修饰的碳纳米管具有良好的生物相容性,可以有效地被细胞摄入,有利于该体系在生物医学中的各类应用。(2)构建了以壳聚糖修饰的碳纳米管为载体,茶多酚为负载药物的纳米载药体系,研究了以主动方式调控药物释放的方法,分别以溶液p H、温度、γ射线照射为触发器,探讨了在上述外界条件影响下水溶液中茶多酚/碳纳米管载药体系中的药物释放行为,从光谱分析的层面验证了药物的释放,为后续的细胞及活体内应用提供研究基础。(3)设计了双荧光标记的碳纳米管探针,将其应用于亚细胞层次的胞内示踪,分别从碳纳米管与细胞的相互作用以及载药体系在细胞内部的作用机制两个科学问题角度进行了讨论。利用多功能荧光标记的方法以及灵敏的共聚焦显微成像技术,首次从直观成像的角度示踪了碳纳米管在细胞内的小泡运输过程,以及碳纳米管载药体系在细胞内部转运过程中药物的特定释放过程。该结果为碳纳米管与生物体系的相互作用机制提供了信息,同时也为载药体系的机制理解与新设计提供了思路。(4)构建了两类以碳纳米管为基础的功能性吸附材料,初步探讨了其对于水体中特定物质的吸附应用。主要针对碳纳米管本身作为吸附材料在实际应用中的固有缺点,如难于分离或成型等限制因素,提出了磁性碳纳米管吸附材料以及碳纳米管宏观体吸附材料的改进设计概念,分别从磁分离方法的角度和块状材料成型的角度出发,拓展了碳纳米管作为吸附材料在实际应用中的可操作性与实用性。(5)制备了多功能的碳纳米管宏观体吸附材料,讨论了其在放射性废水处理中的应用前景。以碳纳米管海绵状骨架材料为模板,在孔壁中引入了具有离子交换性能的普鲁士蓝类化合物,得到了多功能的吸附材料,在保留了纳米材料的优秀特性的同时改善了其单独使用时的缺陷。该吸附材料在对多种金属离子混合溶液的吸附实验中表现出对铯、锶等常见放射性离子较高的吸附能力与选择性,并且因其块状多孔的宏观材料特点,有望后续加工成实用装置,在当前日益受关切的大规模放射性废水处理中得到应用。(6)发展了以水溶性壳聚糖为分子模板的γ辐照合成纳米粒子的方法,构建了纳米金、纳米银等具有表面等离子激元共振性质的功能纳米材料,并将γ辐照方法的“绿色”特点与纳米粒子的生物成像应用相结合,在暗场环境下粒子呈现出良好的散射光成像效果。γ辐照方法的诸多优点使其在制备用于生物医学方向的纳米材料上具有很好的应用前景,并且加以改进和扩展,有望高效制备出如纳米粒子与碳纳米管结合的功能性纳米复合材料体系。
[Abstract]:Using carbon nanotubes as typical nano materials because of its unique structure and special properties, in the industry to create a great prospect, are subtly driving a new industrial revolution, gradually penetrated into and changed people's lives. Such as in the field of biomedicine, drug biological imaging, carbon nanotubes based on the development of nano technology in medicine, testing, is expected to provide new ideas for early diagnosis and treatment methods of tumor breakthrough; in addition, carbon nanotubes as adsorption materials show the application efficiency compared with the traditional adsorbent is more efficient, is expected to present all kinds of waste disposal serious help. However, in carbon carbon nanotubes were used for large-scale industrial application of the road, there are still many problems to be solved or improved. This paper is in such a background, the Some specific problems in the specific application, design and construct the system of functional carbon nanotube materials, mainly studies some basic problems in biomedical applications as well as the application of adsorption materials on the direction, but also from the perspective of construction method of nano materials are discussed. The specific research contents and results of this thesis are as follows: (1) developed with water-soluble chitosan modified carbon nanotubes biofunctionalization method based on one hand, improve the inherent disadvantages of carbon nanotubes, provide the prerequisite for its application in the biomedical field; on the other hand, modified chitosan based on carbon nanotubes in the system can follow the introduction of a variety of biological functional molecules, such as fluorescent markers, tumor targeting molecules, and all kinds of drugs. The chitosan modified carbon nanotubes have good biocompatibility, can effectively be cellular uptake, This system is conducive to applications in various applications. (2) constructed using chitosan modified carbon nanotubes as the carrier, tea polyphenols as drug loaded nanoparticle drug delivery system, studied the method of drug release control in active mode, respectively in P solution H, temperature, gamma ray irradiation as a trigger, discussed in the above conditions under the influence of tea polyphenols solution / carbon nanotube supported drug release behavior in the system, from the spectral analysis to verify the level of drug release, and provide basis for the study of living cells and subsequent application. (3) the design of carbon nanotube probe double fluorescence labeling and its application in subcellular level intracellular tracer, from the angles of mechanism of interaction between carbon nanotubes and cell and drug carrier system in the interior of the cell of the two scientific problems are discussed. By using the method of fluorescence labeling and sensitive function The confocal microscopic imaging technique, for the first time from the perspective of the intuitive imaging tracer vesicular transport of carbon nanotubes in cells, the specific process and release of carbon nanotubes as drug delivery system of drugs inside cells in the transport process. The results of carbon nanotubes and the interaction mechanism of biological system to provide information, but also provides ideas for understanding the mechanism of drug delivery system and new design. (4) based on two kinds of carbon nanotube based functional adsorption material, discusses its application for the adsorption of specific substances in water. Mainly for the carbon nano tube itself as adsorption material in the practical application of the inherent disadvantages, such as difficulty to separation or molding and other limiting factors, put forward the adsorption material of magnetic carbon nanotubes and carbon nanotube macrostructures adsorption materials to improve the design concept, from the angle of magnetic separation method and bulk material The type of point of view, expand the carbon nanotubes as adsorption material in the practical application of the maneuverability and practicability. (5) carbon nanotube macrostructures multifunctional adsorption material was prepared and discussed its application prospect in the treatment of radioactive wastewater. The carbon nanotube sponge skeleton material as a template in Kong Bizhong introduces a Prussian blue ion exchange performance, obtained the adsorption material function, improve the separate use of defects in keep the excellent properties of nanometer materials at the same time. The adsorbent in the adsorption experiment of various metal ions in the mixed solution showed the adsorption capacity and selectivity of strontium and cesium, etc. common radioactive ion is high, and because of its characteristics of macroscopic material of porous block, is expected to further processing into practical devices, obtained in the current increasingly concern about the massive radioactive waste treatment Application. (6) the development of methods for gamma irradiation synthesis of nanoparticles with water-soluble chitosan as the template molecule, constructed gold nanoparticles, functional nano materials nano silver with surface plasmon resonance properties, and gamma irradiation method of "green" characteristics of nano particles and biological imaging applications combine in the dark environment particle scattering light shows good imaging effect. Has a good application prospect of nano materials has many advantages in the gamma irradiation method for the preparation of biomedical direction, and to be improved and extended, prepared with nanoparticles and carbon nanotubes functional nano composite system is expected to be efficient.

【学位授予单位】：南京航空航天大学
【学位级别】：博士
【学位授予年份】：2015
【分类号】：TQ127.11;TB383.1

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