Understanding W/H-ZSM-5 catalysts for the dehydroaromatization of methane

Çağlayan, Mustafa; Nassereddine, Abdallah; Nastase, Stefan A. F.; Tapia, Antonio Aguilar; Dikhtiarenko, Alla; Chung, Sang K.; Shterk, Genrikh; Shoinkhorova, Tuiana; Hazemann, Jean‐Louis; Martínez, Javier Rúiz; Cavallo, Luigi Maria; Ould‐Chikh, Samy; Gascón, Jorge

doi:10.1039/d3cy00103b

Catal. Sci. Technol.

2023

DOI: 10.1039/d3cy00103b

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Understanding W/H-ZSM-5 catalysts for the dehydroaromatization of methane

Mustafa Çağlayan

Abdallah Nassereddine

Stefan A. F. Nastase

et al.

Abstract: Tungsten is the most interesting and promising metal to replace molybdenum in methane dehydroaromatization (MDA) catalysis. Located in the same column of the periodic table, tungsten displays similar chemical features...

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2024

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Cited by 3 publications

References 63 publications

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Direct conversion of methane to aromatics and hydrogen via a heterogeneous trimetallic synergistic catalyst

Zhu,

Bian,

Liu

et al. 2024

Nat Commun

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Non-oxidative methane dehydro-aromatization reaction can co-produce hydrogen and benzene effectively on a molybdenum-zeolite based thermochemical catalyst, which is a very promising approach for natural-gas upgrading. However, the low methane conversion and aromatics selectivity and weak durability restrain the realistic application for industry. Here, a mechanism for enhancing catalysis activity on methane activation and carbon-carbon bond coupling has been found to promote conversion and selectivity simultaneously by adding platinum–bismuth alloy cluster to form a trimetallic catalyst on zeolite (Pt-Bi/Mo/ZSM-5). This bimetallic alloy cluster has synergistic interaction with molybdenum: the formed CH3* from Mo2C on the external surface of zeolite can efficiently move on for C-C coupling on the surface of Pt-Bi particle to produce C2 compounds, which are the key intermediates of oligomerization. This pathway is parallel with the catalysis on Mo inside the cage. This catalyst demonstrated 18.7% methane conversion and 69.4% benzene selectivity at 710 °C. With 95% methane/5% nitrogen feedstock, it exhibited robust stability with slow deactivation rate of 9.3% after 2 h and instant recovery of 98.6% activity after regeneration in hydrogen. The enhanced catalytic activity is strongly associated with synergistic interaction with Mo and ligand effects of alloys by extensive mechanism studies and DFT calculation.

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Direct conversion of methane to aromatics and hydrogen via a heterogeneous trimetallic synergistic catalyst

Zhu,

Bian,

Liu

et al. 2024

Nat Commun

View full text Add to dashboard Cite

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Novel high-pressure/high-temperature reactor cell for in situ and operando x-ray absorption spectroscopy studies of heterogeneous catalysts at synchrotron facilities

Nassereddine,

Prat,

Ould-Chikh

et al. 2024

Review of Scientific Instruments

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This paper presents the development of a novel high-pressure/high-temperature reactor cell dedicated to the characterization of catalysts using synchrotron x-ray absorption spectroscopy under operando conditions. The design of the vitreous carbon reactor allows its use as a plug-flow reactor, monitoring catalyst samples in a powder form with a continuous gas flow at high-temperature (up to 1000 °C) and under high pressure (up to 1000 bar) conditions, depending on the gas environment. The high-pressure/high-temperature reactor cell incorporates an automated gas distribution system and offers the capability to operate in both transmission and fluorescence detection modes. The operando x-ray absorption spectroscopy results obtained on a bimetallic InCo catalyst during CO2 hydrogenation reaction at 300 °C and 50 bar are presented, replicating the conditions of a conventional microreactor. The complete setup is available for users and permanently installed on the Collaborating Research Groups French Absorption spectroscopy beamline in Material and Environmental (CRG-FAME) sciences and French Absorption spectroscopy beamline in Material and Environmental sciences at ultra-high dilution (FAME-UHD) beamlines (BM30 and BM16) at the European Synchrotron Radiation Facility in Grenoble, France.

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Elusive supported surface M2Ox dimer active site (M = Re, W, Mo, Cr, V, Nb, and Ta)

Wachs

2024

Journal of Vacuum Science &Amp; Technology A

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Supported transition metal oxide catalysts are extensively used as heterogeneous catalysts for various energy, chemical, and environmental applications. The molecular structures of dehydrated surface metal oxide phases are crucial for understanding structure-activity/selectivity relationships that guide the design of enhanced catalysts. Some early studies suggested that dimeric (aka binuclear) surface metal oxide sites were more active/selective than monomeric (aka mononuclear) sites, prompting interest in synthesizing catalysts with supported dimeric metal oxide structures. This review examines the literature on dehydrated silica-based supported group 7-5 MOx catalysts (ReOx, WOx, MoOx, CrOx, VOx, NbOx, and TaOx on SiO2, MCM-41, AlOx/SiO2, and H-ZSM-5) for their surface metal oxide structures. In situ Raman, extended x-ray absorption fine structure, and ultraviolet-visible spectroscopy indicate that monomeric surface MOx structures predominate in all such catalysts. Therefore, the cursory use of dimeric surface M2Ox sites in catalytic mechanisms and reaction models in heterogeneous catalysis by supported metal oxides is questionable, and moving forward, the invoking of supporting dimeric surface M2Ox sites should be critically examined and backed up with direct spectroscopic methods.

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Understanding W/H-ZSM-5 catalysts for the dehydroaromatization of methane

Abstract: Tungsten is the most interesting and promising metal to replace molybdenum in methane dehydroaromatization (MDA) catalysis. Located in the same column of the periodic table, tungsten displays similar chemical features...

Cited by 3 publications

References 63 publications

Direct conversion of methane to aromatics and hydrogen via a heterogeneous trimetallic synergistic catalyst

Direct conversion of methane to aromatics and hydrogen via a heterogeneous trimetallic synergistic catalyst

Novel high-pressure/high-temperature reactor cell for in situ and operando x-ray absorption spectroscopy studies of heterogeneous catalysts at synchrotron facilities

Elusive supported surface M2Ox dimer active site (M = Re, W, Mo, Cr, V, Nb, and Ta)

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