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

Journal Article · · Angewandte Chemie (International Edition)
 [1];  [2];  [2]; ORCiD logo [2]; ORCiD logo [3]
  1. University of Minnesota, Minneapolis, MN (United States); University of Minnesota
  2. King Abdullah University of Science and Technology (KAUST), Thuwal (Saudi Arabia)
  3. University of Minnesota, Minneapolis, MN (United States)
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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. Here, 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.

Research Organization:
University of Minnesota, Minneapolis, MN (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division
Grant/Contract Number:
SC0019028
OSTI ID:
1658234
Journal Information:
Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 47 Vol. 57; ISSN 1433-7851
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

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Cited By (3)

Reversible Nature of Coke Formation on Mo/ZSM‐5 Methane Dehydroaromatization Catalysts journal April 2019
Direct Imaging of Atomically Dispersed Molybdenum that Enables Location of Aluminum in the Framework of Zeolite ZSM‐5 journal December 2019
Direct Imaging of Atomically Dispersed Molybdenum that Enables Location of Aluminum in the Framework of Zeolite ZSM-5 journal December 2019

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03 NATURAL GAS
Carbides
heterogeneous catalysis
metal additives
methane dehydroaromatization
polyfunctional catalysis