Absorptive Hydrogen Scavenging for Enhanced Aromatics Yield During Non-oxidative Methane Dehydroaromatization on Mo/H-ZSM-5 Catalysts

Anurag Kumar, Kepeng Song, Lingmei Liu, Yu Han, Aditya Bhan

Research output: Contribution to journalArticlepeer-review

11 Scopus citations

Abstract

Addition of Zr metal particles to MoCx/ZSM-5 in interpellet mixtures (2:1 weight ratio) resulted in maximum single-pass methane conversion of 27 % for dehydroaromatization at 973 K (in significant excess of the equilibrium prescribed circa 10 % conversion at these conditions) and a concurrent 1.4–5.6-fold increase in aromatic product yields due to circumvention of thermodynamic equilibrium limitations by absorptive H2 removal by Zr while retaining cumulative aromatic product selectivity. The absorptive function of the polyfunctional catalyst formulation can be regenerated by thermal treatment in He flow at 973 K, yielding above-equilibrium methane conversion in successive regeneration cycles. H2 uptake experiments demonstrate formation of bulk ZrH1.75 on hydrogen absorption by Zr at 973 K. Cooperation between absorption and catalytic centers distinct in location and function enables circumvention of persistent thermodynamic challenges in non-oxidative methane dehydrogenation.

Original languageEnglish (US)
Pages (from-to)15577-15582
Number of pages6
JournalAngewandte Chemie - International Edition
Volume57
Issue number47
DOIs
StatePublished - Nov 19 2018

Bibliographical note

Funding Information:
We acknowledge financial support from KAUST (OSR Ref. 3325) and Office of Basic Energy Sciences, U.S. Department of Energy (Award DE-SC0019028) and thank Dr. Seema Thakral for XRD measurements as part of Characterization Facility, University of Minnesota, which receives partial support from NSF through MRSEC program.

Publisher Copyright:
© 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

Keywords

  • carbides
  • heterogeneous catalysis
  • metal additives
  • methane dehydroaromatization
  • polyfunctional catalysis

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