Catalytic Conversion & Processes Division, CSIR-Indian Institute of Petroleum, Dehradun 248005, India.
Nanoscale. 2015 Oct 7;7(37):15197-208. doi: 10.1039/c5nr02510a.
A halide ion promoted two dimensional silver tungsten-based nanomaterial was synthesized by a facile one-pot synthesis protocol at room temperature. The 2D morphology features high activity and selectivity for the oxidation of a wide range of tertiary N-compounds to their corresponding N-oxides. The morphology of Ag/WO3 materials can be varied by changing the synthesis parameters. The unique 2D plate like morphology of tungsten oxide increases adsorption sites of the support, leading to less sintering and higher dispersion of silver nanoparticles, resulting in significantly enhanced activity for the reaction. The influence of reaction parameters such as temperature, substrate to oxidant molar ratio, reaction time, etc. was investigated in detail. The catalyst was characterized by XRD, XPS, ICP-AES, TGA, FT-IR, UV-vis, Raman, SEM, TEM and STEM. Raman studies further provide mechanistic insight which proves that the formation of peroxo tungsten species is responsible for the N-oxidation reaction. High stability and recyclability of the 2D Ag/WO3 nanoplates are also observed under the investigated conditions.
一种卤化物离子促进的二维银钨基纳米材料通过在室温下的一种简便的一锅合成法合成。这种二维形态具有高活性和对广泛的叔 N-化合物氧化为相应的 N-氧化物的选择性。通过改变合成参数可以改变 Ag/WO3 材料的形态。氧化钨的独特的二维片状形态增加了载体的吸附位,导致银纳米粒子的烧结和分散性更高,从而显著提高了反应的活性。详细研究了反应参数如温度、底物与氧化剂摩尔比、反应时间等的影响。通过 XRD、XPS、ICP-AES、TGA、FT-IR、UV-vis、拉曼、SEM、TEM 和 STEM 对催化剂进行了表征。拉曼研究进一步提供了机理见解,证明了过氧钨物种的形成是 N-氧化反应的原因。在研究条件下,二维 Ag/WO3 纳米板还表现出高稳定性和可回收性。