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New Multicomponent MoVSbNbCeOx/SiO2 Catalyst with Enhanced Catalytic Activity for Oxidative Dehydrogenation of Ethane to Ethylene
ChemCatChem ( IF 4.5 ) Pub Date : 2020-05-04 , DOI: 10.1002/cctc.202000489
Galina A. Zenkovets 1 , Alexey A. Shutilov 1 , Valentina M. Bondareva 1 , Vladimir I. Sobolev 1 , Alexander S. Marchuk 1 , Sergey V. Tsybulya 1 , Igor P. Prosvirin 1 , Arcady V. Ishchenko 1 , Vladimir Yu. Gavrilov 1
Affiliation  

In our study, we have obtained a multicomponent MoVSbNbCeOx/SiO2 catalyst with high catalytic activity for oxidative dehydrogenation of ethane (ODE) to ethylene. To date, multicomponent MoVTe(Sb)NbOx catalysts, which have been intensively studied during the last years, were found as very promising for the ODE to produce ethylene. It was generally agreed that the MoVTeNbOx catalyst was more efficient than MoVSbNbOx. The major drawback of using Te‐containing catalysts is the presence of environmentally harmful, toxic tellurium, and its volatility during the catalyst preparation and catalytic reaction conditions. In our work, the Mo1V0.24Sb0.23Nb0.08Ce0.01Ox/50 wt. % SiO2 catalyst was prepared via the spray‐dry method of aqueous solutions of the starting components, followed by heat‐treatment in He at 350 and 600 °C. For comparative purpose, one of the best Te‐containing catalysts Mo1V0.3Te0.23Nb0.12Ox was also tested in this reaction under the similar reaction conditions. A comparison of the catalytic properties of Sb− and Te− containing catalysts at the reaction temperature of 400–450 °C illustrates for both catalysts relatively high catalytic properties for ODE. The yield of ethylene of ca. 74 % was obtained for these catalysts, which exceeds the best yield reported in literature for Sb‐containing catalysts. The two main phases – M1 and M2 were revealed by XRD in the Sb‐containing catalyst. Intergrowth between the crystals of M1 and M2 phases with the formation of the interphase boundary in the highly active and selective Sb‐containing catalyst can be proposed from HRTEM results. The nature of the active state in this catalyst is discussed.

中文翻译:

新型具有增强催化活性的乙烷氧化脱氢制乙烯的多组分MoVSbNbCeOx / SiO2催化剂

在我们的研究中,我们获得了具有高催化活性的多组分MoVSbNbCeO x / SiO 2催化剂,可将乙烷(ODE)氧化脱氢为乙烯。迄今为止,发现在过去的几年中已进行了深入研究的多组分MoVTe(Sb)NbO x催化剂对于ODE生产乙烯非常有希望。人们普遍认为,MoVTeNbO x催化剂比MoVSbNbO x更有效。使用含Te的催化剂的主要缺点是对环境有害,有毒的碲的存在,及其在催化剂制备和催化反应条件下的挥发性。在我们的工作中,Mo 1 V 0.24 Sb 0.23Nb 0.08 Ce 0.01 O x / 50 wt。通过喷雾干燥起始成分的水溶液的方法制备%SiO 2催化剂,然后在350和600°C的He中进行热处理。为了比较,最好的含Te催化剂之一Mo 1 V 0.3 Te 0.23 Nb 0.12 O x在相似的反应条件下也对该反应进行了测试。在400–450°C的反应温度下,含Sb-和Te-的催化剂的催化性能比较表明,两种催化剂对ODE的催化性能都较高。乙烯的产率约为。这些催化剂获得了74%的产率,超过了文献中报道的含Sb催化剂的最佳收率。XRD在含Sb的催化剂中揭示了两个主要相– M1和M2。可以从HRTEM结果提出M1和M2相晶体之间的共生以及在高活性和选择性的含Sb催化剂中形成相间边界的方法。讨论了该催化剂中活性态的性质。
更新日期:2020-05-04
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