From a batch to a continuous supported ionic liquid phase (silp) process: anhydrous synthesis of oxymethylene dimethyl ethers
Abstract: Oxymethylene dimethyl ethers (OMEn; CH3(−OCH2)n−OCH3) are promising sustainable synthetic fuels when produced from CO2 and green H2. The synthesis pathway presented here overcomes synthetic problems and includes the reaction of dimethoxymethane (OME1) with molecular gaseous formaldehyde in a novel continuous, anhydrous reaction setup. An initially performed wide batch-catalyst screening highlighted the salts M[NTf2]x with M=Cu+, Co2+ and Mg2+ as especially interesting catalysts (NTf2=N(SO2CF3)2). Supported ionic liquid phase (SILP)-catalysts were prepared on this basis and demonstrated the successful synthesis of OMEn in a continuous process. The SILP-catalysts immobilized in the IL EMIM[BF4] showed a fast and strong deactivation, but those with the IL EMIM[NTf2] showed excellent catalytic performance and stable results in continuous operations exceeding 19 h. The influence of the weight hourly space velocity (WHSV), the reaction temperature as well as the storage conditions of the catalysts (inert vs non-inert) were investigated. 90 °C was identified as ideal reaction temperature. High feed-gas flows (WHSV=15.8 h−1) are preferable in terms of product selectivity SOME2-5>90 mol- % with an OME1 conversion XOME1=5.10 mol- % at the same time. We also demonstrated that the catalysts can be stored in air for 50 days without loss of activity. The SILP-catalysts were analyzed by NMR and IR spectroscopy. Furthermore, the thermodynamics of the reaction mechanism of some selected catalysts was calculated by DFT theory to this reaction
- Location
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Deutsche Nationalbibliothek Frankfurt am Main
- Extent
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Online-Ressource
- Language
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Englisch
- Notes
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ChemCatChem. - 15, 20 (2023) , e202300844, ISSN: 1867-3899
- Classification
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Chemie
- Event
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Veröffentlichung
- (where)
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Freiburg
- (who)
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Universität
- (when)
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2023
- Creator
- DOI
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10.1002/cctc.202300844
- URN
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urn:nbn:de:bsz:25-freidok-2400148
- Rights
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Open Access; Der Zugriff auf das Objekt ist unbeschränkt möglich.
- Last update
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25.03.2025, 1:53 PM CET
Data provider
Deutsche Nationalbibliothek. If you have any questions about the object, please contact the data provider.
Associated
- Billion, Andreas
- Vogel, Andreas
- Schulte, Jonas
- Scherer, Harald
- Krossing, Ingo
- Universität
Time of origin
- 2023
Other Objects (12)
CO2 hydrogenation to methanol and dimethyl ether
Continuous anhydrous synthesis of oxymethylene dimethyl ethers by reaction of dimethyl ether with molecular formaldehyde
Beiträge zur Chemie des Aluminiums : Synthese, Struktur und Reaktivität monomerer Aminoalane, Additionsverbindungen der Aluminiumhalogenide
Chemie mit schwach koordinierenden Anionen : Synthese einer neuen Klasse schwach koordinierender Anionen des Typs Al(ORF)-4, Lewis-Säure-Base-Addukte der sehr schwachen Lewis-Basen S8, P4 und P4S3 mit dem Ag+-Kation von Ag[Al(ORF)4], von homopolyatomaren Phosphorkationen zu Al(ORF)-4-Salzen neuer binärer Phosphor-Halogen-Kationen mit Polyphosphorskelett
On the anhydrous synthesis of oxymethylene dimethyl ether by the reaction of dimethoxymethane with gaseous molecular formaldehyde
Does direct dimethyl ether synthesis from carbon dioxide and hydrogen yield more valuable products than the equivalent methanol production? A review on recent work
Thermodynamic properties of ionic liquids
Boron ionic liquids as potential hydrogen storage materials : = Bor-ionische Flüssigkeiten als potentielle Wasserstoffspeicher-Materialien
Chemistry in ionic liquids and prediction of their transport properties : = Chemie in ionischen Flüssigkeiten und die Vorhersage ihrer Transporteigenschaften
Investigations on dynamic properties of ionic liquids towards their application as electrolytes : = Untersuchungen der dynamischen Eigenschaften Ionischer Flüssigkeiten im Hinblick auf ihre Anwendung als Elektrolyte
Synthesis of the weakly coordinating anion [Al(OC10F15)4]− and continuous anhydrous synthesis of oxymethylene dimethyl ethers with gaseous molecular formaldehyde
The contribution of molecular interaction potentials to properties and activities of ionic liquid ions in solution
CO2 hydrogenation to methanol and dimethyl ether
Continuous anhydrous synthesis of oxymethylene dimethyl ethers by reaction of dimethyl ether with molecular formaldehyde
Beiträge zur Chemie des Aluminiums : Synthese, Struktur und Reaktivität monomerer Aminoalane, Additionsverbindungen der Aluminiumhalogenide
Chemie mit schwach koordinierenden Anionen : Synthese einer neuen Klasse schwach koordinierender Anionen des Typs Al(ORF)-4, Lewis-Säure-Base-Addukte der sehr schwachen Lewis-Basen S8, P4 und P4S3 mit dem Ag+-Kation von Ag[Al(ORF)4], von homopolyatomaren Phosphorkationen zu Al(ORF)-4-Salzen neuer binärer Phosphor-Halogen-Kationen mit Polyphosphorskelett
On the anhydrous synthesis of oxymethylene dimethyl ether by the reaction of dimethoxymethane with gaseous molecular formaldehyde
Does direct dimethyl ether synthesis from carbon dioxide and hydrogen yield more valuable products than the equivalent methanol production? A review on recent work
Thermodynamic properties of ionic liquids
Boron ionic liquids as potential hydrogen storage materials : = Bor-ionische Flüssigkeiten als potentielle Wasserstoffspeicher-Materialien
Chemistry in ionic liquids and prediction of their transport properties : = Chemie in ionischen Flüssigkeiten und die Vorhersage ihrer Transporteigenschaften
Investigations on dynamic properties of ionic liquids towards their application as electrolytes : = Untersuchungen der dynamischen Eigenschaften Ionischer Flüssigkeiten im Hinblick auf ihre Anwendung als Elektrolyte
Synthesis of the weakly coordinating anion [Al(OC10F15)4]− and continuous anhydrous synthesis of oxymethylene dimethyl ethers with gaseous molecular formaldehyde
The contribution of molecular interaction potentials to properties and activities of ionic liquid ions in solution
CO2 hydrogenation to methanol and dimethyl ether
Continuous anhydrous synthesis of oxymethylene dimethyl ethers by reaction of dimethyl ether with molecular formaldehyde
Beiträge zur Chemie des Aluminiums : Synthese, Struktur und Reaktivität monomerer Aminoalane, Additionsverbindungen der Aluminiumhalogenide
Chemie mit schwach koordinierenden Anionen : Synthese einer neuen Klasse schwach koordinierender Anionen des Typs Al(ORF)-4, Lewis-Säure-Base-Addukte der sehr schwachen Lewis-Basen S8, P4 und P4S3 mit dem Ag+-Kation von Ag[Al(ORF)4], von homopolyatomaren Phosphorkationen zu Al(ORF)-4-Salzen neuer binärer Phosphor-Halogen-Kationen mit Polyphosphorskelett
On the anhydrous synthesis of oxymethylene dimethyl ether by the reaction of dimethoxymethane with gaseous molecular formaldehyde
Does direct dimethyl ether synthesis from carbon dioxide and hydrogen yield more valuable products than the equivalent methanol production? A review on recent work
Thermodynamic properties of ionic liquids
Boron ionic liquids as potential hydrogen storage materials : = Bor-ionische Flüssigkeiten als potentielle Wasserstoffspeicher-Materialien
Chemistry in ionic liquids and prediction of their transport properties : = Chemie in ionischen Flüssigkeiten und die Vorhersage ihrer Transporteigenschaften
Investigations on dynamic properties of ionic liquids towards their application as electrolytes : = Untersuchungen der dynamischen Eigenschaften Ionischer Flüssigkeiten im Hinblick auf ihre Anwendung als Elektrolyte
Synthesis of the weakly coordinating anion [Al(OC10F15)4]− and continuous anhydrous synthesis of oxymethylene dimethyl ethers with gaseous molecular formaldehyde