4.7 Article

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

Journal

INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
Volume 43, Issue 15, Pages 7317-7325

Publisher

PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.ijhydene.2018.02.156

Keywords

Hydrogen storage; Liquid organic hydrogen carrier; Dehydrogenation; Graphene; Kinetics

Funding

  1. National Natural Science Foundation of China [21376186]
  2. China Postdoctoral Science Foundation [2016M592794]
  3. Fundamental Research Funds for the Central Universities (Creative Team Plan in Xi'an Jiaotong University) [cxtd2017004]
  4. Natural Science Basic Research Plan in Shaanxi Province of China [2017JQ2030]
  5. National Science Foundation of U.S. [NSF/CHE-1346572]
  6. U.S. DOE [DE-AC02-06CH11357]

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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. (C) 2018 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.

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