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Absorptive Hydrogen Scavenging for Enhanced Aromatics Yield During Non‐oxidative Methane Dehydroaromatization on Mo/H‐ZSM‐5 Catalysts
Author(s) -
Kumar Anurag,
Song Kepeng,
Liu Lingmei,
Han Yu,
Bhan Aditya
Publication year - 2018
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.201809433
Subject(s) - dehydrogenation , catalysis , chemistry , yield (engineering) , methane , selectivity , hydrogen , absorption (acoustics) , thermodynamic equilibrium , zeolite , inorganic chemistry , chemical engineering , organic chemistry , materials science , thermodynamics , metallurgy , composite material , physics , engineering
Addition of Zr metal particles to MoC x /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 H 2 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. H 2 uptake experiments demonstrate formation of bulk ZrH 1.75 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.