Catalytic dehydrogenation study of dodecahydro-N-ethylcarbazole by noble metal supported on reduced graphene oxide

• Published in: International journal of hydrogen energy 2018-04, Vol.43 (15), p.7317-7325
• Main Authors: Wang, Bin, Chang, Tie-yan, Jiang, Zhao, Wei, Jin-jia, Zhang, Yong-hai, Yang, Sen, Fang, Tao
• Format: Article
• Language: English
• Subjects: Dehydrogenation; Graphene; Hydrogen storage; Kinetics; Liquid organic hydrogen carrier
• ISSN: 0360-3199; 1879-3487
• DOI: 10.1016/j.ijhydene.2018.02.156

Through systematical experiments, a comparative study was conducted concerning several graphene-supported noble metal catalysts for dehydrogenation of dodecahydro-N-ethylcarbazole (12H-NEC). It was found that the catalytic activity of the prepared graphene-supported noble metal catalysts was following the order of Pd > Pt > Rh > Ru > Au for the dehydrogenation process. Pd supported on reduced graphene oxide (rGO) prepared by one-pot in situ synthesis has much more excellent catalytic performance than other kinds of catalysts investigated for comparison, simultaneously the using amount of noble metals can obviously be decreased. To be specific, at 453 K, the final dehydrogenation product catalyzed by the novel catalyst of Pd/rGO is N-ethylcarbazole (NEC) and the process selectivity was increased from 44.77% (commercial Pd/Al2O3) to 97.65%, as well as the dehydrogenation ratio reached 99.14%. In addition, the novel catalyst is also superior to other reported catalysts in terms of dehydrogenation performance of 12H-NEC. Its dehydrogenation activity at 443 and 433 K of Pd/rGO was tested and the catalytic performance keeps stable at the two temperatures. Based on the experimental data, kinetic calculation was carried out and some fundamental parameters regarding reaction kinetics was obtained. [Display omitted] •Dealing with five kinds of noble metals for comparative dehydrogenation studies.•Synchrotron X-ray Diffraction was used to reveal the crystal structure of Pd on rGO.•The prepared Pd/rGO catalyst exhibits a dramatically enhanced dehydrogenation activity state-of-the-art.•A more accurate kinetic calculation of the dehydrogenation reaction was performed.