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

23 Scopus citations

Abstract

The 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 ~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 hydrogen removal by Zr while retaining the cumulative aromatic product selectivity. The absorptive function of the polyfunctional catalyst formulation can be regenerated by thermal treatment in helium flow at 973 K yielding above equilibrium methane conversion in successive regeneration cycles. Hydrogen uptake experiments demonstrate formation of bulk ZrH₁.₇₅ on hydrogen absorption by zirconium 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 - Oct 30 2018

Bibliographical note

KAUST Repository Item: Exported on 2020-10-01
Acknowledged KAUST grant number(s): OSR Ref. 3325
Acknowledgements: 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.

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