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Determination of highly active and selective surface for the oxidative dehydrogenation of ethane over phase-pure M1 MoVNbTeOx catalyst
Journal of Catalysis ( IF 6.5 ) Pub Date : 2022-11-11 , DOI: 10.1016/j.jcat.2022.11.011
Yuxin Chen , Shuairen Qian , Kai Feng , Zhengwen Li , Binhang Yan , Yi Cheng

The original phase-pure M1 MoVNbTeOx catalyst was mechanically treated with stirring water for several days under ambient conditions to obtain particles with different sizes. The catalytic performance was significantly improved and stabilized after about 7 days of treatment. Among all the catalysts, the sample treated in water for 7 days can obtain 57.6 % ethane conversion and 0.79 kgC2H4/kgcat/h ethylene productivity while the original phase-pure M1 catalyst was only 19.2 % and 0.27 kgC2H4/kgcat/h at reaction temperature of 400 °C and contact time of 18.5 gcat·h/molC2H6. Meanwhile, the catalyst was systematically characterized and the results showed that there was essentially no difference in microstructure between the original and treated catalysts. TEM and SEM morphological characterizations presented that the particle size and aspect ratio of the catalysts changed significantly, in which the particle size of the catalyst become smaller and the proportion of basal surface was enhanced. The activity and selectivity of the catalysts exhibited a correlation with the amount and proportion of basal surface. It can be deducted that the basal surface is the most active and selective surface during oxidative dehydrogenation of ethane (ODHE) process, and the intrinsic activity based on the basal (0 0 1) plane of the catalyst remains stable after the mechanical treatment. Samples treated in water for 7 days showed excellent long-term stability in a 200 h stability test at reaction temperature of 440 °C and contact time of 9.3 gcat·h/molC2H6. The present work demonstrated that the differences in the catalytic properties of different M1 samples depend mainly on the amount and proportion of exposed basal surface, and the possibility of enhancing the activity of orthorhombic M1 phase by fragmentation method.



中文翻译:

相纯 M1 MoVNbTeOx 催化剂上乙烷氧化脱氢高活性和选择性表面的测定

原始相纯 M1 MoVNbTeO x催化剂在环境条件下用搅拌水机械处理数天,以获得不同尺寸的颗粒。经过约7天的处理后,催化性能得到显着改善和稳定。在所有催化剂中,在水中处理 7 天的样品可获得 57.6% 的乙烷转化率和 0.79 kg C2H4 /kg cat /h 的乙烯生产率,而原始相纯 M1 催化剂仅为 19.2% 和 0.27 kg C2H4 /kg cat / h 在 400 °C 的反应温度和 18.5 g cat ·h/mol C2H6的接触时间. 同时,对催化剂进行了系统表征,结果表明,原始催化剂和处理后的催化剂在微观结构上基本没有差异。TEM和SEM形貌表征表明,催化剂的粒径和纵横比发生了显着变化,其中催化剂的粒径变小,基面比例增加。催化剂的活性和选择性与基底表面的量和比例相关。可以推断,在乙烷氧化脱氢(ODHE)过程中,基底表面是最活跃和选择性最强的表面,而基于基底的本征活性(0  0 1)机械处理后催化剂平面保持稳定。在 440 °C 的反应温度和 9.3 g cat ·h/mol C2H6的接触时间下进行的 200 小时稳定性测试中,在水中处理 7 天的样品显示出出色的长期稳定性。目前的工作表明,不同M1样品催化性能的差异主要取决于暴露基底表面的数量和比例,以及通过碎裂方法增强正交M1相活性的可能性。

更新日期:2022-11-11
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