A comparative study of catalytic dehydrogenation of perhydro-N-ethylcarbazole over noble metal catalysts

A comparative study of catalytic dehydrogenation of perhydro-N-ethylcarbazole over noble metal catalysts
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全氢-N-乙基咔唑与贵金属催化剂催化脱氢的比较研究

DOI:
10.1016/j.ijhydene.2014.09.123
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发表时间:
2014-11
影响因子:
7.2
通讯作者:
Hansong
Hansong
中科院分区:
工程技术2区
文献类型:
--
作者:
Yang;Ming;Dong;Yuan;Fei;Shunxin;Ke;Hanzhong;Cheng;Hansong

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N-乙基咔唑是最有前途的液体有机氢载体之一,因为它可以在相对温和的温度下催化氢化和脱氢。在本工作中,我们报告了一个系统的研究,全氢-N-乙基咔唑脱氢在几个重要的负载贵金属催化剂,以确定最佳的催化剂的温度控制脱氢。反应分三步进行,中间产物为八氢-N-乙基咔唑和四氢-N-乙基咔唑。所选贵金属催化剂的初始脱氢活性顺序为Pd > Pt > Ru > Rh。在负载型Pt和Pd催化剂上,N-乙基咔唑的最终产物的选择性达到100%,并且完全脱氢。研究了催化剂上三段脱氢过程的动力学,求出了反应速率常数。结果表明,对于所有贵金属催化剂,脱氢反应速率均随反应阶段的增加而显著降低,四氢-N-乙基咔唑向N-乙基咔唑的转化是整个反应过程的限速步骤.
N-ethylcarbazole is one of the most promising liquid organic hydrogen carriers (LOHCs) as it can be catalytically hydrogenated and dehydrogenated at relatively moderate temperatures. In the present work, we report a systematic study on dehydrogenation of perhydro-N-ethylcarbazole over several important supported noble metal catalysts to identify the optimal catalyst for temperature-controlled dehydrogenation. The reaction takes three consecutive stages with two intermediates of octahydro-N-ethylcarbazole and tetrahydro-N-ethylcarbazole. The initial catalytic activity of the selected noble metal catalysts for the dehydrogenation process was found to follow the order of Pd > Pt > Ru > Rh. 100% selectivity toward the final product of N-ethylcarbazole and fully dehydrogenation was achieved over the supported Pt and Pd catalysts. The kinetics of the three stage dehydrogenation processes over the catalysts was studied and the rate constants were derived. The results indicate that the dehydrogenation reaction rate decreases significantly with the reaction stage for all the selected noble catalysts and the conversion from tetrahydro-N-ethylcarbazole to N-ethylcarbazole was found to be the rate-limiting step of the entire reaction process.
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