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Mildly acidic aluminosilicate catalysts for stable performance in ethanol dehydration

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Résumé

Ethanol dehydration is effectively catalyzed by strongly acidic zeolites which, however, exhibit poor time-on-stream stability. For example, HZSM-5 features strong acid sites, catalyzes ethylene oligomerization, and is prone to coking. Alumina and silica-alumina on the other hand have lower acidity, are relatively stable, but reach only low activity. Here, a series of mesoporous aluminosilicate catalysts was prepared by non-hydrolytic sol-gel (NHSG) and are shown to feature an intermediate level of acidity (both in strength and nature), resulting in intermediate catalytic performance. Importantly, the best NHSG-made samples were very stable with time on stream, did not produce any traces of ethylene oligomers, did not show any trace of coke formation, and their texture was unaffected. Characterization (ICP-OES, N2-physisorption, TEM, XPS, IR-pyridine, Raman and solid state NMR spectroscopies) revealed that this behavior must be correlated with the remarkable degree of homogeneity in the NHSG-made aluminosilicate (only tetrahedrally coordinated Al species).

langue originaleAnglais
Numéro d'article118926
journalApplied Catalysis. B: Environmental
Volume271
Les DOIs
Etat de la publicationPublié - 15 août 2020

Financement

A.S. acknowledges funding from the European Union´s Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie grant agreement No 751774. F.R.S.–F.N.R.S. is thanked for the acquisition of the physi-chemisorption equipment used here (project “EQP U.N030.18”). Authors acknowledge the ‘Communauté française de Belgique’ for the financial support through the ARC programme (15/20-069). François Devred and Jean-François Statsyns are acknowledged for the technical and logistical support. This research used resources of the “Plateforme Technologique Physico-Chemical Characterization” – PC2, the SIAM platform (Synthesis, Irradiation & Analysis of Materials) and the MORPH-IM platform (Morphology & Imaging) located at the University of Namur. Authors thank L. Simonikova for performing ICP-OES analyses. CIISB research infrastructure project LM2015043 funded by MEYS CR is gratefully acknowledged for the financial support of the measurements at the CF Cryo-electron Microscopy and Tomography. This research has been financially supported by the MEYS CR under the project CEITEC 2020 (LQ1601) and by the Czech Science Foundation under the project GJ20-03636Y. A.S. acknowledges funding from the European Union´s Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie grant agreement No 751774 . F.R.S.–F.N.R.S. is thanked for the acquisition of the physi-chemisorption equipment used here (project "EQP U.N030.18"). Authors acknowledge the ‘Communauté française de Belgique’ for the financial support through the ARC programme ( 15/20-069 ). François Devred and Jean-François Statsyns are acknowledged for the technical and logistical support. This research used resources of the “Plateforme Technologique Physico-Chemical Characterization” – PC2, the SIAM platform (Synthesis, Irradiation & Analysis of Materials) and the MORPH-IM platform (Morphology & Imaging) located at the University of Namur. Authors thank L. Simonikova for performing ICP-OES analyses. CIISB research infrastructure project LM2015043 funded by MEYS CR is gratefully acknowledged for the financial support of the measurements at the CF Cryo-electron Microscopy and Tomography. This research has been financially supported by the MEYS CR under the project CEITEC 2020 ( LQ1601 ) and by the Czech Science Foundation under the project GJ20-03636Y.

Bailleurs de fondsNuméro du bailleur de fonds
European Union´s Horizon 2020 research and innovation programme
H2020 Marie Skłodowska-Curie Actions751774
Australian Government, Australian Research Council15/20-069, LM2015043
Ministerstvo Školství, Mládeže a TělovýchovyLQ1601
Grantová Agentura České RepublikyGJ20-03636Y
Fonds de la Recherche Scientifique F.R.S.-FNRSEQP U.N030.18
Fédération Wallonie-Bruxelles

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