Aromatization of ethylene over zeolite-based catalysts

Uslamin, Evgeny A.; Saito, Hikaru; Kosinov, Nikolay; Pidko, Evgeny A.; Sekine, Yasushi; Hensen, Emiel J. M.

doi:10.1039/c9cy02108f

Cited by 88 publications

(66 citation statements)

References 48 publications

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“…Recently, a similar hydrocarbon pool type mechanism was proposed for the conversion of ethane to benzene over Mo/ZSM‐5, whereas ethane aromatization over Ga/ZSM‐5 proceeded via a different mechanism and metal‐free HZSM‐5 was not active for the reaction. [ 78 ] This finding indicates that even in case of C 2 compounds, being the main initial products of methane activation, the hydrocarbon pool‐like mechanism would still be a valid explanation for the reactivity of Mo‐zeolite catalysts.…”

Section: Reaction Mechanismmentioning

confidence: 99%

Reactivity, Selectivity, and Stability of Zeolite‐Based Catalysts for Methane Dehydroaromatization

2020

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strong C-H bonds complicates the selective conversion of methane to higher hydrocarbons and oxygenates. Currently, the main industrial method to use methane as a material feedstock involves the transformation to syngas by steam reforming, followed by processes such as methanol synthesis and Fischer-Tropsch synthesis to obtain liquid fuels and other useful chemicals. A disadvantage of this indirect technology is the high capital cost of reforming plants, making it only economically attractive at a very large scale. An efficient direct process for the conversion of methane to higher hydrocarbons or oxygenates remains one of the "holy grails" of chemistry. [6,7] The approaches to directly convert methane can be categorized into oxidative and non-oxidative methods. Oxidative processes are often met with low product selectivity because of the higher reactivity of targeted products as compared to methane itself, resulting in overoxidation to CO 2. Non-oxidative methods are generally more atom-efficient, because, in addition to valuable hydrocarbon products, pure CO xfree hydrogen gas (H 2) is obtained, which can be used for instance in fuel cells. [8] Among several alternatives, including non-oxidative coupling of methane to ethylene and deep methane dehydrogenation to solid carbon and hydrogen, [9-12] methane dehydroaromatization (MDA) remains one of the most promising non-oxidative reactions for the direct valorization of natural gas. MDA involves the selective conversion of methane to a mixture of easily transportable aromatics, that is, benzene (predominantly), naphthalene, and toluene. As all other non-oxidative methane conversion reactions, MDA is a highly endothermic process: 6CH C H 9H 532 kJ mol Non-oxidative dehydroaromatization is arguably the most promising process for the direct upgrading of cheap and abundant methane to liquid hydrocarbons. This reaction has not been commercialized yet because of the suboptimal activity and swift deactivation of benchmark Mo-zeolite catalysts. This progress report represents an elaboration on the recent developments in understanding of zeolite-based catalytic materials for high-temperature non-oxidative dehydroaromatization of methane. It is specifically focused on recent studies, relevant to the materials chemistry and elucidating i) the structure of active species in working catalysts; ii) the complex molecular pathways underlying the mechanism of selective conversion of methane to benzene; iii) structure, evolution and role of coke species; and iv) process intensification strategies to improve the deactivation resistance and overall performance of the catalysts. Finally, unsolved challenges in this field of research are outlined and an outlook is provided on promising directions toward improving the activity, stability, and selectivity of methane dehydroaromatization catalysts.

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Section: Reaction Mechanismmentioning

confidence: 99%

Reactivity, Selectivity, and Stability of Zeolite‐Based Catalysts for Methane Dehydroaromatization

2020

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“…15,18 Olefins such as ethene and propene directly formed from the furan species can be considered the primary origin of BTX aromatics. 55 To broaden understanding of how 2,5-dmf is transformed upon adsorption and how olefin and BTX formation are related temperature programmed desorption experiments were carried out.…”

Section: Desorption Products From Preadsorbed 25-dmfmentioning

confidence: 99%

Valorisation of 2,5-dimethylfuran over zeolite catalysts studied by on-line FTIR-MS gas phase analysis

Sauer

Lorén

Schaëfer

et al. 2022

Catal. Sci. Technol.

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“…5,6 This mechanism involves organocatalytic intermediates of aromatic and olefinic nature, resulting in two catalytic cycles interconnected through hydrogen transfer reactions. The generality of the HCP chemistry is evident from similar mechanistic proposals for the zeolite-catalyzed conversion of methyl halides to higher hydrocarbons, 7 conversion of furanics, 8,9 and the dehydroaromatization of methane. 10 The fact that similar chemistry can arise from different starting reactants prompted us to investigate methanethiol (CH 3 SH) substrate.…”

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confidence: 92%

Selective methanethiol-to-olefins conversion over HSSZ-13 zeolite

Tormene

Bolshakov

et al. 2021

Chem. Commun.

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Aromatization of ethylene over zeolite-based catalysts

Abstract: Elucidating the role of metal modification and confined hydrocarbon species in the aromatization of ethylene on zeolite catalysts.

Cited by 88 publications

References 48 publications

Reactivity, Selectivity, and Stability of Zeolite‐Based Catalysts for Methane Dehydroaromatization

Reactivity, Selectivity, and Stability of Zeolite‐Based Catalysts for Methane Dehydroaromatization

Valorisation of 2,5-dimethylfuran over zeolite catalysts studied by on-line FTIR-MS gas phase analysis

Selective methanethiol-to-olefins conversion over HSSZ-13 zeolite

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