摘要
过渡金属氧化物因其多样性的价电子结构,使其具有丰富物理和化学性质,并显示出在光学、磁学、催化和电池等领域广泛的应用前景。通过对过渡金属氧化物纳米材料的有效合成,探索其合成机制,进而实现对目标纳米结构的尺寸、化学组成及物性的有效调控,对于进一步探索结构与物性的关联具有重要作用。通过一系列的化学手段,将纳米晶“自下而上”的集成,即组装成具有更高级结构的功能体,对实现按照人们的意愿设计合成功能材料具有重要意义。本论文在过渡金属氧化物纳米结构合成新方法的设计、合成机制,功能组装及物性等方面进行了系统的探索研究。
基于相转移和相分离的机制,成功制备了尺寸均匀的水合磷酸钇纳米晶;对纳米晶的形貌和尺寸进行了调控,并探讨了纳米晶形成和形貌演化的机理,丰富和发展了稀土纳米结构的合成方法。通过利用纳米晶表面有机长链的交叠产生的相互作用,实现了对纳米晶的2维组装,为从纳米晶向高级超结构的组装奠定了实验基础。
基于硝酸铈铵具有稳定的二十面体结构,以其前驱物,发展了液相大量合成3nm氧化铈纳米晶的方法,并研究了其负载金后的催化性能;通过增加体系中反应物的浓度,直接制备了具有有序超结构的胶体纳米粒子,观察到了纳米晶在合成过程中的3维组装行为,为探讨具有有序超结构胶体粒子的形成和应用提供了实验依据。
设计了液相合成不同形貌二氧化钛纳米晶的方法;通过利用水油体系形成的正相胶束,对纳米晶进行了组装,并研究了其催化和电池性能。
设计了基于层状结构的有机分子与无机物复合双分子层,发展出了通用的合成超细(2 nm以下)过渡金属及其氧化纳米结构的方法;在实验上方法上,实现了纳米晶合成与组装的结合,成功的构建了具有应用前景的功能组装体。
Owing to variety of electronic structures, nanostructured transition metal oxides have exhibited strongly potential applications in optics, magnetics, catalysis and batteries. Preparing nanostructured transition metal oxides, investigating their possible formation mechanism and consequent controlling the size, composition and physical properties could be of the key importance. Apart from the synthesis, the organization of the as-obtained nanostructures towards advanced and complex superstructures also play a very important role in materials science, which would help the design of functional materials as the corresponding requirement. In this dissertation, systematic explorations have been carried out on synthetic strategies of nanostructured transition metal oxides, formation mechanisms, controllable organization and their properties.
Based on the phase transfer and separation, the uniform yttrium phosphate hydrate nanocrystals with controllable size and shape have successfully prepared via a solution-base path way. Based on experimental facts, a possible formation mechanism was also proposed and applied to the preparation of the other lanthanide phosphates nanocrystals. By utilizing the multiple interactions between the long chain alkyl molecules, which absorbed on the surface of the nanocrystals, the 2 dimensional (2D) assembled superstructures were readily formed.
Based on the special crystal structure of ammonium cerium nitrate, a novel method for synthesis of monodisperse 3nm cerium oxides nanocrystal in large scale was developed rationally. Furthermore, 3D assembled colloidal particles with high ordered internal secondary structures were also prepared in one step through increasing the concentration of the precursor in the synthetic system.
A facile method was established for the synthesis of uniform titanium oxide nanocrystals with different shapes and sizes. Based on the constructed positive micelle, the as-obtained nanocrystals were organized into functional colloidal nanospheres. Systematical studies of their electronchemistry and catalytic properties indicated promising applications of the assembled products materials in catalysis and Li-ion battery.
A general method for synthesis of ultrathin nanostructures was developed based on the rational artificial lamellar mesostructure. The as-obtained products can be organized into various ordered superstructures, which indicated that the synthesis and organization was couple together successfully.
引文
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