학위논문(박사) - 한국과학기술원 : 화학과, 2014.8, [ xi, 115 p ]The development of novel synthetic methods and morphology control for nanoscale metal and metal-oxide particles has attracted a great deal of attention owing to their unique properties and wide catalytic applications. However, the catalytic activity of the heterogeneous nanoparticles often drops as a result of particle aggregation and decreased metal surface area during the catalytic processes. Hybrid nanostructures integrating two or more discrete nanomaterials, especially with functional metal-oxide supports, can provide superior catalytic performance such as higher catalytic activity, structural stability and further recyclability. The resulting hybrid nanocatalysts show unique physico-chemical properties and tailored properties directly influence on their catalytic activity and reusability.
In chapter I, we offer a comprehensive introduction into the synthesis of metal/metal-oxide hybrid nanostructures with characteristic functionalities and a study of their physical and catalytic properties. In chapter II, we present the fabrication of three different bifunctional palladium nanocomposites with silica(SiO2)-based supports for catalytic reactions. The Pd/SiO2 nanobeads that tiny Pd clusters are deposited inside porous silica (SiO2) network, and the porosity-controlled Pd@Niphy (Ni3Si2O5(OH)4, nickel phyllosilicate) yolk-shell nanoparticles exhibit enhanced catalytic activities in Suzuki cross-coupling reactions due to easy transport of reaction molecules inward and outward active sites. In addition, surface-activated Pd@SiO2 yolk-shell nanoparticles by an oxidant, PhICl2, catalyze the homogeneous hydroalkoxylation reaction showing the homogeneity of heterogeneous catalyst. In chapter III, we introduce a hybrid system comprising metal (Pd or Au) and iron oxide (Fe3O4) components. The structural anisotropy and crystallinity of metal−Fe3O4 structures are precisely controlled producing as yolk-shell, irregular core-shell, and dumbb...한국과학기술원 : 화학과