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Liquid-phase pulsed laser ablation synthesis of graphitized carbon-encapsulated palladium core-shell nanospheres for catalytic reduction of nitrobenzene to aniline

机译:液相脉冲激光烧蚀石墨化碳包覆钯核壳纳米球催化硝基苯还原为苯胺

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Graphitized carbon-encapsulated palladium (Pd) core-shell nanospheres were produced via pulsed laser ablation of a solid Pd foil target submerged in acetonitrile. The microstructural features and optical properties of these nanospheres were characterized via high resolution transmission electron microscopy (HRTEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and UV-visible spectroscopy. Microstructural analysis indicated that the core-shell nano structures consisted of single-crystalline cubic metallic Pd spheres that serve as the core material, over which graphitized carbon was anchored as a heterogeneous shell. The absorbance spectrum of the synthesized nanostructures exhibited a broad (absorption) band at similar to 264 nm; this band corresponded to the typical inter-band transition of a metallic system and resulted possibly from the absorbance of the ionic Pd2+. The catalytic properties of the Pd and Pd@C core-shell nanostructures were investigated using the reduction of nitrobenzene to aniline by an excess amount of NaBH4 in an aqueous solution at room temperature, as a model reaction. Owing to the graphitized carbon-layered structure and the high specific surface area, the resulting Pd@C nanostructures exhibited higher conversion efficiencies than their bare Pd counterparts. In fact, the layered structure provided access to the surface of the Pd nanostructures for the hydrogenation reaction, owing to the synergistic effect between graphitized carbon and the nanostructures. Their unique structure and excellent catalytic performance render Pd@C core-shell nanostructures highly promising candidates for catalysis applications. (C) 2015 Elsevier B.V. All rights reserved.
机译:通过对浸没在乙腈中的固体Pd箔靶进行脉冲激光烧蚀来生产石墨化的碳囊封钯(Pd)核壳纳米球。这些纳米球的微观结构特征和光学性质通过高分辨率透射电子显微镜(HRTEM),X射线衍射(XRD),X射线光电子能谱(XPS)和紫外可见光谱来表征。微观结构分析表明,核-壳纳米结构由充当核心材料的单晶立方金属Pd球组成,其上固定了石墨化碳作为异质壳。合成的纳米结构的吸收光谱在类似于264 nm处显示了一个宽的(吸收)带。该带对应于金属系统的典型带间跃迁,可能是由于离子Pd2 +的吸收引起的。在室温下,使用水溶液中过量的NaBH4将硝基苯还原为苯胺,研究了Pd和Pd @ C核壳纳米结构的催化特性,作为模型反应。由于石墨化的碳层结构和高比表面积,所得到的Pd @ C纳米结构比其裸露的Pd对应物具有更高的转化效率。实际上,由于石墨化碳与纳米结构之间的协同作用,层状结构提供了进入Pd纳米结构表面以进行氢化反应的通道。它们独特的结构和出色的催化性能使Pd @ C核壳纳米结构成为催化应用中极有希望的候选者。 (C)2015 Elsevier B.V.保留所有权利。

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