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Vanadium-doped porous silica materials with high catalytic activity and stability for propane dehydrogenation reaction
Applied Catalysis A: General ( IF 5.5 ) Pub Date : 2018-01-17 , DOI: 10.1016/j.apcata.2018.01.014
Ping Hu , Wan-Zhong Lang , Xi Yan , Xing-Fan Chen , Ya-Jun Guo

Novel V-based catalysts, vanadium-doped porous silica materials (V-SiO2), have been successfully prepared by a facile one-pot synthetic method for propane dehydrogenation (PDH). The structure-activity relationships of V-SiO2 with different vanadium contents have been well elucidated through several state-of-the-art characterization techniques. The results indicate that vanadium species are highly dispersed in the channels of the porous silica materials, and that both monomeric and low-polymerized V species are the main active sites for PDH reaction. V-SiO2 catalysts with moderate vanadium doping display a mesoporous structure with high specific surface area and large pore volume, whereas excessively high vanadium doping will disrupt the mesoporous structure due to the formation of bulk V2O5 crystallites. Catalytic tests have shown that V(2)-SiO2 catalyst with a V/Si mass ratio of 1:12 exhibits optimal catalytic activity and stability for PDH reaction, achieving a superior propane conversion that decreases from 64% to 30% and stable propylene selectivity of ∼90% over 21 h at 580 °C. Its regeneration leads to an 8% decrease in propane conversion and about 94% propylene selectivity within 6 h after a second PDH cycle, demonstrating that this V(2)-SiO2 catalyst has excellent long-term catalytic stability. This work may expedite the development of vanadium-doped porous silica materials obtained by an one-pot method for use in catalysis.



中文翻译:

具有高催化活性和丙烷脱氢反应稳定性的钒掺杂多孔二氧化硅材料

新型的钒基催化剂,即钒掺杂的多孔二氧化硅材料(V-SiO 2),已通过一种简便的一锅法丙烷脱氢(PDH)合成方法成功制备。通过几种最新的表征技术已经很好地阐明了钒含量不同的V-SiO 2的结构活性关系。结果表明,钒物质高度分散在多孔二氧化硅材料的通道中,单体和低聚合的V物质都是PDH反应的主要活性部位。V-的SiO 2具有中等钒掺杂量的催化剂显示出具有高比表面积和大孔体积的介孔结构,而过高的钒掺杂量会由于形成大量V 2 O 5晶体而破坏介孔结构。催化测试表明,V / Si质量比为1:12的V (2) -SiO 2催化剂表现出最佳的催化活性和对PDH反应的稳定性,实现了出色的丙烷转化率(从64%降至30%)和稳定的丙烯在580°C下21 h选择性达到〜90%。在第二个PDH循环后的6小时内,其再生导致丙烷转化率降低8%,丙烯选择性降低约94%,表明该V (2) -SiO2催化剂具有优异的长期催化稳定性。这项工作可以加速通过一锅法获得的钒掺杂的多孔二氧化硅材料的开发,以用于催化。

更新日期:2018-01-17
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