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Effect of the nature and the distribution of vanadium Species on the catalytic behavior of vanadium-based silica catalysts

机译:钒种质的作用与钒种对钒基二氧化硅催化剂催化行为的影响

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V-containing hexagonal mesoporous silica catalysts were prepared by direct synthesis and impregnation method in a wide range of V loading (0.68 - 7.8 wt. %). Investigation of VOx complex distribution by means of H2-TPR reveals that direct synthesis method led predominantly to formation of material with very narrow distribution of VOx complexes, whereas impregnation methods resulted in materials with broad distribution of VOx species including VOx units with a lower degree of dispersion. The catalytic results in propane ODH (Oxidative dehydrogenation) were much better for synthesized catalysts compared to impregnated catalysts. Synthesized samples exhibited higher activity as well as selectivity to propene. This activity and selectivity of synthesized catalysts was ascribed to well-dispersed VOx units characterized by low-temperature reduction peak in H2-TPR. Presence of more polymeric or bulk-like vanadium oxide species, reflected in high-temperature reduction peak, led to decrease in selectivity and/or activity of the catalysts in C3-ODH reaction.
机译:通过直接合成和浸渍方法在宽范围的V负载(0.68-7.8重量%)中,制备含V含六方介孔二氧化硅催化剂。通过H2-TPR调查VOX综合分布显示,直接合成方法主要用于形成具有非常窄的VOX配合物分布的材料,而浸渍方法导致材料具有广泛的VOX物种,包括较低程度的VOX物种分散。与浸渍催化剂相比,催化剂在丙烷ODH(氧化脱氢)中的结果较多。合成样品表现出更高的活性以及对丙烯的选择性。合成催化剂的这种活性和选择性均匀于分散的VOX单元,其特征在于H2-TPR中的低温还原峰。在高温降低峰值中反映的更多聚合物或块状氧化钒物质的存在导致C3- ODH反应中催化剂的选择性和/或活性降低。

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