Facile synthesis of highly stable and well-dispersed mesoporous ZrO2/carbon composites with high performance in oxidative dehydrogenation of ethylbenzene
文献情報
Qiang Li, Jie Xu, Zhangxiong Wu, Dan Feng, Jianping Yang, Jing Wei, Qingling Wu, Bo Tu, Yong Cao, Dongyuan Zhao
Highly ordered mesoporous ZrO2/carbon (FDU-15) composites have been synthesized via a facile evaporation induced triconstituent co-assembly (EISA) approach by using Pluronic F127 as a template and zirconium oxychloride octahydrate and resol as Zr and carbon sources. The synthesized mesoporous composites exhibit a highly ordered two-dimensional (2-D) hexagonal mesostructure with relatively high specific surface areas (up to 947 m2 g−1), pore sizes around 3.8 nm and high pore volumes (up to 0.71 cm3 g−1). The results clearly show that the crystalline zirconia nanoparticles (ca. 1.9–3.9 nm) are well-dispersed in amorphous matrices of the ordered mesoporous carbon FDU-15 materials, which construct the nanocomposites. The ordered mesostructures of the obtained ZrO2/FDU-15 composites can be well-retained even at the high pyrolysis temperature (up to 900 °C), suggesting a high thermal stability. The zirconia content of the ZrO2/FDU-15 composites can be tunable in a wide range (up to 47%). Moreover, the resultant mesoporous ZrO2/FDU-15 composites exhibit high catalytic activity in oxidative dehydrogenation (ODH) of ethylbenzene (EB) to styrene (ST), with high ethylbenzene conversion (59.6%) and styrene selectivity (90.4%), which is mainly attributed to the synergistic catalytic effect between the oxygen-containing groups located on the carbon pore walls and weakly basic sites of the nanocrystalline ZrO2. Furthermore, the high specific surface areas and opening pore channels are also responsible for their high catalytic activity. Therefore, it is a very promising catalyst material in styrene production on an industrial scale.
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