期刊
CATALYSIS TODAY
卷 363, 期 -, 页码 73-84出版社
ELSEVIER
DOI: 10.1016/j.cattod.2019.06.001
关键词
Catalytic selective oxidation; Mixed oxides; Toluene; Benzaldehyde; Uranium; Molybdenum; Tungsten
资金
- BNFL
Various mixed metal bi-component oxide catalysts were prepared, characterized and evaluated for gas phase selective toluene oxidation. Among these catalysts, Fe/Mo showed the highest benzaldehyde yield, while U/Mo and U/W also exhibited selective toluene oxidation activity. Different catalysts led to the formation of various by-products.
Mixed metal bi-component oxide catalysts, including Fe/Mo, U/Mo, U/W, Fe/U, U/V and U/Sb have been prepared, characterised and evaluated for gas phase selective toluene oxidation. Selective toluene oxidation activity to form benzaldehyde was exhibited by Fe/Mo, U/Mo and U/W mixed oxide catalysts. The Fe/Mo catalyst produced the highest benzaldehyde yield. Catalysts that formed benzaldehyde also produced a range of by-products, these were other partial oxidation and coupling products, and preliminary studies of benzaldehyde oxidation suggests they were formed from secondary reactions of benzaldehyde. The Fe/U, Sb/U and U/V catalysts produced only total oxidation to carbon oxides. Catalysts were characterised by X-ray diffraction, laser Raman spectroscopy and temperature programmed reduction. Single molybdate phases were identified for the Fe/Mo and U/Mo catalysts, and a mixture of uranium molybdate and WO3 was identified for the U/W catalyst. Results suggest that the formation of a molybdate phase is important for the selective oxidation of toluene. In contrast, the U/Fe catalyst was a mixture of U3O8 and V2O5, whilst the Fe/U catalyst was comprised of highly dispersed iron oxide on UO3. The presence of U3O8 was responsible for toluene total oxidation. The U/Sb catalyst did not exhibit selective toluene oxidation, but previous studies have demonstrated that the catalyst exhibits high activity for selective propene oxidation. Similar behaviour has been observed for the other catalysts in this study, and it is apparent that catalysts that were selective for toluene oxidation were not selective for propene/propane oxidation and vice versa.
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