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Enhanced performance of boron nitride catalysts with induction period for the oxidative dehydrogenation of ethane to ethylene
Journal of Catalysis ( IF 6.5 ) Pub Date : 2018-06-28 , DOI: 10.1016/j.jcat.2018.05.023
Yanliang Zhou , Jian Lin , Lin Li , Xiaoli Pan , Xiucheng Sun , Xiaodong Wang

Hexagonal boron nitride (h-BN) has recently aroused continuous interest in the oxidative dehydrogenation (ODH) of light alkanes. Here we found that commercial h-BN exhibits an induction period during the ODH of ethane to ethylene. It can achieve better performance only on activated BN after the first cycle run of ODH or treatment of reactants together. The conversion of ethane was 36% at a selectivity of 79% on the activated BN at 570 °C, which nearly tripled that on the fresh BN (12% conversion with 84% selectivity). An excellent productivity of 110 μmol gcat−1 s−1 was obtained, which was one order of magnitude higher than that on most previous catalysts. Various methods of characterization such as infrared spectroscopy, O2 adsorption microcalorimetry, and transient analysis of products by mass spectroscopy indicated the formation of B–OH species on BN after the induction period. There was a linear relationship between the reaction rate of ethane and the quantity of OH species. It is suggested that B–OH species can facilitate the adsorption of O2 and then be transformed to B–O species, which would react with ethane to produce ethylene with the assistance of O2, thus resulting in a higher reaction rate and a lower activation energy.



中文翻译:

具有诱导期的氮化硼催化剂增强性能,可将乙烷氧化脱氢为乙烯

六方氮化硼(h-BN)最近引起了人们对轻质烷烃的氧化脱氢(ODH)的持续关注。在这里,我们发现商业化的h-BN在乙烷ODH转化为乙烯的过程中表现出诱导期。仅在ODH的第一个循环运行或一起处理反应物后,才能在活化的BN上实现更好的性能。在570°C下,活化的BN的乙烷转化率为36%,选择性为79%,几乎是新鲜BN的三倍(转化率为12%,选择性为84%)。获得了110μmolg cat -1  s -1的优异生产率,比大多数以前的催化剂高出一个数量级。各种表征方法,例如红外光谱法,O 2吸附微量量热法和质谱对产物的瞬态分析表明,诱导期后BN上形成了B–OH物种。乙烷的反应速率与OH的数量之间存在线性关系。有人认为,B-OH种类可以促进O 2的吸附,然后转化为B-O种类,它们在O 2的帮助下会与乙烷反应生成乙烯,从而导致更高的反应速率和更低的反应速率。活化能。

更新日期:2018-06-28
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