Silicotungstic acid-derived WO_(3) composited with ZrO_(2) supported on SBA-15 as a highly efficient mesoporous solid acid catalyst for the alkenylation of p-xylene with phenylacetylene  

作　　者：Xueting Bai Yongle Guo Zhongkui Zhao 

机构地区：[1]State Key Laboratory of Fine Chemicals,Department of Catalysis Chemistry and Engineering,School of Chemical Engineering,Dalian University of Technology,Dalian 116024,China

出　　处：《Chinese Chemical Letters》2022年第3期1325-1330,共6页中国化学快报（英文版）

基　　金：financially supported by the National Natural Science Foundation of China (No. 21276041);Chinese Ministry of Education via the Program for New Century Excellent Talents in University (No. NCET-12-0079)。

摘　　要：Highly dispersed silicotungstic acid-derived WO_(3) composited with ZrO_(2) supported on SBA-_(15) (WZ/SBA-_(15)) as an ordered mesoporous solid acid catalyst was prepared via a facile incipient wetness impregnation (IWI) method that active ingredients, ZrO_(2) and WO_(3), were impregnated into the channels of SBA-_(15) simultaneously with a subsequent calcination process. The relationship between catalyst nature and performance was explored by high resolution transmission electron microscopy (HRTEM), high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), FT-IR, X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), N_(2) adsorption-desorption, NH_(3) temperature-programmed desorption (NH_(3)-TPD), and FT-IR of pyridine adsorption (Py-IR) characterization techniques. The catalytic performance of W_(12)Z_(15)/SBA-_(15) is not only greater than that of single component solid acid catalysts, WO_(3)/SBA-_(15) and ZrO_(2)/SBA-_(15), but also W_(12)/Z_(15)/SBA-_(15) prepared by impregnating active ingredients, ZrO_(2) and WO_(3), into SBA-_(15) in sequence. The outstanding performance of W_(12)Z_(15)/SBA-_(15) is derived from the strong interaction between ZrO_(2) and WO_(3), which results in more acid sites, and relatively high specific surface area, large pore volume, and ordered mesoporous structure of SBA-_(15). The characterization and reaction results clearly demonstrate that the synergy of ZrO_(2) and WO_(3) has a clear boost for the alkenylation. The optimized W_(12)Z_(15)/SBA-_(15)-500 achieves a 99.4% conversion of phenylacetylene and a 92.3% selectivity of main product α-arylstyrene for the alkenylation of p-xylene with phenylacetylene, with very low level of oligomers producing at the same time. Moreover, W_(12)Z_(15)/SBA-_(15)-500 shows excellent catalytic stability and regeneration. Therefore, W_(12)Z_(15)/SBA-_(15)-500 is a promising solid acid catalyst for the alkenylation.

关 键 词：ALKENYLATION SBA-15 Zirconium dioxide Tungsten trioxide Silicotungstic acid Solid acid 

分 类 号：O621.251[理学—有机化学] O643.36[理学—化学]