Reversible nature of coke formation on Mo/ZSM-5 methane dehydroaromatization catalysts

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Abstract

Non-oxidative dehydroaromatization of methane over Mo/ZSM-5 zeolite catalysts is a promising reaction for the direct conversion of abundant natural gas into liquid aromatics. Rapid coking deactivation hinders the practical implementation of this technology. Herein, we show that catalyst productivity can be improved by nearly an order of magnitude by raising the reaction pressure to 15 bar. The beneficial effect of pressure was found for different Mo/ZSM-5 catalysts and a wide range of reaction temperatures and space velocities. High-pressure operando X-ray absorption spectroscopy demonstrated that the structure of the active Mo-phase was not affected by operation at elevated pressure. Isotope labeling experiments, supported by mass-spectrometry and 13 C nuclear magnetic resonance spectroscopy, indicated the reversible nature of coke formation. The improved performance can be attributed to faster coke hydrogenation at increased pressure, overall resulting in a lower coke selectivity and better utilization of the zeolite micropore space.

Original languageEnglish
Pages (from-to)7068-7072
Number of pages5
JournalAngewandte Chemie - International Edition
Volume58
Issue number21
DOIs
Publication statusPublished - 20 May 2019

Fingerprint

Methane
Coke
Catalysts
Zeolites
X ray absorption spectroscopy
Coking
Isotopes
Labeling
Nuclear magnetic resonance spectroscopy
Hydrogenation
Mass spectrometry
Natural gas
Productivity
Liquids
Experiments
Temperature

Keywords

  • deactivation
  • heterogeneous catalysis
  • methane dehydroaromatization
  • operando spectroscopy
  • zeolites

Cite this

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title = "Reversible nature of coke formation on Mo/ZSM-5 methane dehydroaromatization catalysts",
abstract = "Non-oxidative dehydroaromatization of methane over Mo/ZSM-5 zeolite catalysts is a promising reaction for the direct conversion of abundant natural gas into liquid aromatics. Rapid coking deactivation hinders the practical implementation of this technology. Herein, we show that catalyst productivity can be improved by nearly an order of magnitude by raising the reaction pressure to 15 bar. The beneficial effect of pressure was found for different Mo/ZSM-5 catalysts and a wide range of reaction temperatures and space velocities. High-pressure operando X-ray absorption spectroscopy demonstrated that the structure of the active Mo-phase was not affected by operation at elevated pressure. Isotope labeling experiments, supported by mass-spectrometry and 13 C nuclear magnetic resonance spectroscopy, indicated the reversible nature of coke formation. The improved performance can be attributed to faster coke hydrogenation at increased pressure, overall resulting in a lower coke selectivity and better utilization of the zeolite micropore space.",
keywords = "deactivation, heterogeneous catalysis, methane dehydroaromatization, operando spectroscopy, zeolites",
author = "Nikolay Kosinov and Uslamin, {Evgeny A.} and Lingqian Meng and Alexander Parastaev and Yujie Liu and Hensen, {Emiel J.M.}",
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T1 - Reversible nature of coke formation on Mo/ZSM-5 methane dehydroaromatization catalysts

AU - Kosinov, Nikolay

AU - Uslamin, Evgeny A.

AU - Meng, Lingqian

AU - Parastaev, Alexander

AU - Liu, Yujie

AU - Hensen, Emiel J.M.

PY - 2019/5/20

Y1 - 2019/5/20

N2 - Non-oxidative dehydroaromatization of methane over Mo/ZSM-5 zeolite catalysts is a promising reaction for the direct conversion of abundant natural gas into liquid aromatics. Rapid coking deactivation hinders the practical implementation of this technology. Herein, we show that catalyst productivity can be improved by nearly an order of magnitude by raising the reaction pressure to 15 bar. The beneficial effect of pressure was found for different Mo/ZSM-5 catalysts and a wide range of reaction temperatures and space velocities. High-pressure operando X-ray absorption spectroscopy demonstrated that the structure of the active Mo-phase was not affected by operation at elevated pressure. Isotope labeling experiments, supported by mass-spectrometry and 13 C nuclear magnetic resonance spectroscopy, indicated the reversible nature of coke formation. The improved performance can be attributed to faster coke hydrogenation at increased pressure, overall resulting in a lower coke selectivity and better utilization of the zeolite micropore space.

AB - Non-oxidative dehydroaromatization of methane over Mo/ZSM-5 zeolite catalysts is a promising reaction for the direct conversion of abundant natural gas into liquid aromatics. Rapid coking deactivation hinders the practical implementation of this technology. Herein, we show that catalyst productivity can be improved by nearly an order of magnitude by raising the reaction pressure to 15 bar. The beneficial effect of pressure was found for different Mo/ZSM-5 catalysts and a wide range of reaction temperatures and space velocities. High-pressure operando X-ray absorption spectroscopy demonstrated that the structure of the active Mo-phase was not affected by operation at elevated pressure. Isotope labeling experiments, supported by mass-spectrometry and 13 C nuclear magnetic resonance spectroscopy, indicated the reversible nature of coke formation. The improved performance can be attributed to faster coke hydrogenation at increased pressure, overall resulting in a lower coke selectivity and better utilization of the zeolite micropore space.

KW - deactivation

KW - heterogeneous catalysis

KW - methane dehydroaromatization

KW - operando spectroscopy

KW - zeolites

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JO - Angewandte Chemie - International Edition

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