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Catalytic oxidation of methacrolein to methacrylic acid over silica-supported 11-molybdo-1-vanadophosphoric acid with different heteropolyacid loadings

机译:不同杂多酸负载量的二氧化硅负载的11-钼-1-钒磷酸催化甲基丙烯醛催化氧化为甲基丙烯酸

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摘要

Catalytic oxidation of methacrolein (MAL) to methacrylic acid (MAA) over SiO2-supported H4PMo11VO40 with different H4PMo11VO40 loadings was investigated. H4PMo11VO40/SiO2 showed high activity in comparison with unsupported H4PMo11VO40, and 3.3 mol% H4PMo11VO40/SiO2 (50 wt% H4PMo11VO40) had the highest activity, which was five-times larger than that of unsupported H4PMo11VO40 due to high dispersion of H4PMo11VO40 on SiO2, as determined by temperature-programmed desorption of benzonitrile. On the other hand, the supported catalysts were less selective towards the formation of MAA. From X-ray diffraction and Raman spectroscopy, it was determined that H4PMo11VO40 decomposed to form MoO3 on SiO2 during the catalytic reaction. Since SiO2-supported MoO3 and unsupported MoO3 had only very low selectivity toward the formation of MAA in the oxidation of MAL, it was concluded that the formation of MoO3 caused the decrease in the catalytic performance of the supported catalysts.
机译:研究了在不同负载量的SiO2负载的H4PMo11VO40上,甲基丙烯醛(MAL)催化氧化为甲基丙烯酸(MAA)。与未负载的H4PMo11VO40相比,H4PMo11VO40 / SiO2表现出较高的活性,而3.3 mol%的H4PMo11VO40 / SiO2(50 wt%H4PMo11VO40)的活性最高,这是未负载的H4PMo11VO40的五倍,因为H4PMo11VO40在SiO2上的高度分散,由程序控制的苄腈脱附确定。另一方面,负载型催化剂对MAA形成的选择性较低。从X射线衍射和拉曼光谱法确定,在催化反应期间,H4PMo11VO40分解而在SiO2上形成MoO3。由于SiO 2负载的MoO 3和未负载的MoO 3在MAL的氧化中对MAA的形成仅具有非常低的选择性,因此得出结论,MoO 3的形成导致负载的催化剂的催化性能下降。

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