Elucidating Zeolite Channel Geometry–Reaction Intermediate Relationships for the Methanol‐to‐Hydrocarbon Process
Abstract: The chemical industry has exploited zeolite shape selectivity for more than 50 years, yet our fundamental understanding remains incomplete. Herein, the zeolite channel geometry–reactive intermediate relationships are studied in detail using anisotropic zeolite ZSM‐5 crystals for the methanol‐to‐hydrocarbon (MTH) process, and advanced magic‐angle spinning solid‐state NMR (ssNMR) spectroscopy. The utilization of anisotropic ZSM‐5 crystals enabled the preferential formation of reaction intermediates in single‐orientation zeolite channels, as revealed by molecular dynamics simulations and in situ UV/Vis diffuse‐reflectance spectroscopy. The ssNMR results show that the slightly more constrained sinusoidal zeolite channels favor the olefin cycle by promoting the homologation of alkanes, whereas the more extended straight zeolite channels facilitate the aromatic cycle with a higher degree of alkylation of aromatics. Dynamic nuclear polarization experiments further indicate the preferential formation of heavy aromatics at the zeolite surface dominated by the sinusoidal channels, providing further insight into catalyst deactivation.
- Location
-
Deutsche Nationalbibliothek Frankfurt am Main
- Extent
-
Online-Ressource
- Language
-
Englisch
- Bibliographic citation
-
Elucidating Zeolite Channel Geometry–Reaction Intermediate Relationships for the Methanol‐to‐Hydrocarbon Process ; volume:59 ; number:45 ; year:2020 ; pages:20024-20030 ; extent:7
Angewandte Chemie / International edition. International edition ; 59, Heft 45 (2020), 20024-20030 (gesamt 7)
- Creator
-
Fu, Donglong
Lucini Paioni, Alessandra
Lian, Cheng
van der Heijden, Onno
Baldus, Marc
Weckhuysen, Bert
- DOI
-
10.1002/anie.202009139
- URN
-
urn:nbn:de:101:1-2022061907060340724498
- Rights
-
Open Access; Der Zugriff auf das Objekt ist unbeschränkt möglich.
- Last update
-
15.08.2025, 7:23 AM CEST
Data provider
Deutsche Nationalbibliothek. If you have any questions about the object, please contact the data provider.
Associated
- Fu, Donglong
- Lucini Paioni, Alessandra
- Lian, Cheng
- van der Heijden, Onno
- Baldus, Marc
- Weckhuysen, Bert
Other Objects (12)
Effect of Steaming on Waste‐Derived Zeolite ZSM‐5 as Methanol‐To‐Hydrocarbons Catalyst
Template–Framework Interactions in Tetraethylammonium‐Directed Zeolite Synthesis
Template–Framework Interactions in Tetraethylammonium‐Directed Zeolite Synthesis
Separation and Purification of Hydrocarbons with Porous Materials
Separation and Purification of Hydrocarbons with Porous Materials
Thermally Stable TiO 2 ‐ and SiO 2 ‐Shell‐Isolated Au Nanoparticles for In Situ Plasmon‐Enhanced Raman Spectroscopy of Hydrogenation Catalysts
Carbon Pathways, Sodium‐Sulphur Promotion and Identification of Iron Carbides in Iron‐based Fischer‐Tropsch Synthesis
Bridging the Gap between the Direct and Hydrocarbon Pool Mechanisms of the Methanol‐to‐Hydrocarbons Process
Bridging the Gap between the Direct and Hydrocarbon Pool Mechanisms of the Methanol‐to‐Hydrocarbons Process
Influence of Levulinic Acid Hydrogenation on Aluminum Coordination in Zeolite‐Supported Ruthenium Catalysts: A 27 Al 3QMAS Nuclear Magnetic Resonance Study †
Diagnosing the Internal Architecture of Zeolite Ferrierite
Carbon Deposit Analysis in Catalyst Deactivation, Regeneration, and Rejuvenation
Effect of Steaming on Waste‐Derived Zeolite ZSM‐5 as Methanol‐To‐Hydrocarbons Catalyst
Template–Framework Interactions in Tetraethylammonium‐Directed Zeolite Synthesis
Template–Framework Interactions in Tetraethylammonium‐Directed Zeolite Synthesis
Separation and Purification of Hydrocarbons with Porous Materials
Separation and Purification of Hydrocarbons with Porous Materials
Thermally Stable TiO 2 ‐ and SiO 2 ‐Shell‐Isolated Au Nanoparticles for In Situ Plasmon‐Enhanced Raman Spectroscopy of Hydrogenation Catalysts
Carbon Pathways, Sodium‐Sulphur Promotion and Identification of Iron Carbides in Iron‐based Fischer‐Tropsch Synthesis
Bridging the Gap between the Direct and Hydrocarbon Pool Mechanisms of the Methanol‐to‐Hydrocarbons Process
Bridging the Gap between the Direct and Hydrocarbon Pool Mechanisms of the Methanol‐to‐Hydrocarbons Process
Influence of Levulinic Acid Hydrogenation on Aluminum Coordination in Zeolite‐Supported Ruthenium Catalysts: A 27 Al 3QMAS Nuclear Magnetic Resonance Study †
Diagnosing the Internal Architecture of Zeolite Ferrierite
Carbon Deposit Analysis in Catalyst Deactivation, Regeneration, and Rejuvenation
Effect of Steaming on Waste‐Derived Zeolite ZSM‐5 as Methanol‐To‐Hydrocarbons Catalyst
Template–Framework Interactions in Tetraethylammonium‐Directed Zeolite Synthesis
Template–Framework Interactions in Tetraethylammonium‐Directed Zeolite Synthesis
Separation and Purification of Hydrocarbons with Porous Materials
Separation and Purification of Hydrocarbons with Porous Materials
Thermally Stable TiO 2 ‐ and SiO 2 ‐Shell‐Isolated Au Nanoparticles for In Situ Plasmon‐Enhanced Raman Spectroscopy of Hydrogenation Catalysts
Carbon Pathways, Sodium‐Sulphur Promotion and Identification of Iron Carbides in Iron‐based Fischer‐Tropsch Synthesis
Bridging the Gap between the Direct and Hydrocarbon Pool Mechanisms of the Methanol‐to‐Hydrocarbons Process
Bridging the Gap between the Direct and Hydrocarbon Pool Mechanisms of the Methanol‐to‐Hydrocarbons Process
Influence of Levulinic Acid Hydrogenation on Aluminum Coordination in Zeolite‐Supported Ruthenium Catalysts: A 27 Al 3QMAS Nuclear Magnetic Resonance Study †
Diagnosing the Internal Architecture of Zeolite Ferrierite