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V2O5-SiO2 systems prepared by flame pyrolysis as catalysts for the oxidative dehydrogenation of propane

机译:通过火焰热解制备的V2O5-SiO2系统作为丙烷氧化脱氢的催化剂

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摘要

VOx/SiO2 catalysts were prepared through an innovative flame pyrolysis (FP) technique and tested for the oxidative dehydrogenation of propane. The samples, of different V loadings, were characterized by electron paramagnetic resonance (EPR), micro-Raman, and FT-IR spectroscopy to assess the nature of the vanadium active sites in comparison with a sample prepared by impregnation. The active sites of the FP-prepared catalysts appeared as highly dispersed V5+O groups partly incorporated into the silica matrix and interacting poorly with one another. Lower dispersion can be achieved at the same V loading with the catalyst prepared by impregnation. EPR revealed V4+O groups pointing out normally from the catalyst surface and sitting in the center of a surface array of oxygen atoms. These V4+ groups helped demonstrate the difference in catalytic behavior of the various samples. Catalytic activity measured under both aerobic and anaerobic conditions revealed a promisingly high selectivity with the FP-prepared samples. The best results were obtained with a 10 wt% V loading, which provided the best propylene yield among the samples, especially under anaerobic conditions (up to 80% selectivity at 10% propane conversion). This is likely related to the much higher dispersion of the VOx species in the FP-prepared samples, which also helps reduce the coke formation triggered by exposed surface acid sites. (C) 2008 Elsevier Inc. All rights reserved.
机译:VOx / SiO2催化剂是通过创新的火焰热解(FP)技术制备的,并经过丙烷氧化脱氢测试。通过电子顺磁共振(EPR),显微拉曼光谱和FT-IR光谱对具有不同V负载的样品进行表征,以与通过浸渍制备的样品相比,评估钒活性位点的性质。 FP制备的催化剂的活性位点显示为高度分散的V5 + O基团,部分结合到二氧化硅基质中并且彼此之间的相互作用较弱。通过浸渍制备的催化剂在相同的V负载下可以实现较低的分散度。 EPR显示,V4 + O基团通常从催化剂表面指向并位于氧原子表面阵列的中心。这些V4 +基团有助于证明各种样品在催化行为上的差异。在好氧和厌氧条件下测定的催化活性均显示出用FP制备的样品具有很高的选择性。在10 wt%的V负载下可获得最佳结果,这在样品中提供了最佳的丙烯收率,尤其是在厌氧条件下(丙烷转化率10%时选择性高达80%)。这可能与VOx物质在FP制备的样品中的分散度高得多有关,这也有助于减少由暴露的表面酸位触发的焦炭形成。 (C)2008 Elsevier Inc.保留所有权利。

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