Properties and activity of zn-ta-tud-1 in ...
Document type :
Article dans une revue scientifique: Article original
DOI :
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Title :
Properties and activity of zn-ta-tud-1 in the lebedev process
Author(s) :
Pomalaza Raez, Guillaume [Auteur]
Unité de Catalyse et Chimie du Solide - UMR 8181 [UCCS]
Simon, Pardis [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Addad, Ahmed [Auteur]
Unité Matériaux et Transformations (UMET) - UMR 8207
Capron, Mickael [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Dumeignil, Franck [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Unité de Catalyse et Chimie du Solide - UMR 8181 [UCCS]
Simon, Pardis [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Addad, Ahmed [Auteur]
Unité Matériaux et Transformations (UMET) - UMR 8207
Capron, Mickael [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Dumeignil, Franck [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Journal title :
Green chemistry . an international journal and green chemistry resource . GC
Abbreviated title :
Green Chem.
Volume number :
22
Pages :
2558-2574
Publication date :
2020-04-21
ISSN :
1463-9262
HAL domain(s) :
Chimie/Catalyse
English abstract : [en]
A zinc and tantalum-containing mesoporous silica catalyst highly active and selective in the Lebedev process has been prepared using the one-pot TUD-1 methodology. Selectivity towards butadiene reached 60–70%, making ...
Show more >A zinc and tantalum-containing mesoporous silica catalyst highly active and selective in the Lebedev process has been prepared using the one-pot TUD-1 methodology. Selectivity towards butadiene reached 60–70%, making Zn–Ta-TUD-1 one of the best performing catalysts in the literature. To rationalize these results and establish a structure–activity relationship, a series of similar catalysts was prepared and characterized. Nitrogen physisorption, XPS, ICP-AES, XRD, TEM, UV-vis spectroscopy, TGA NH3-TPD, H2-TPR and FT-IR techniques were used. The most active samples were found to possess a large specific surface area and highly dispersed metal oxide phase incorporated within the mesoporous silica matrix. In combination with catalytic testing, characterization also showed a direct correlation between the number of Lewis acid sites and butadiene yield, confirming the structure–activity relationship theory prevalent for the Lebedev process. Deactivation of Zn–Ta-TUD-1 was also studied using the same techniques to characterize the properties of spent catalysts. It was found that the accumulation of heavy carbonaceous species caused a reduction of specific surface area and pore size coinciding with the observed loss in activity. Nevertheless, the pores of TUD-1 were large enough to avoid total pore blockage and a high selectivity could be maintained for 72 hours.Show less >
Show more >A zinc and tantalum-containing mesoporous silica catalyst highly active and selective in the Lebedev process has been prepared using the one-pot TUD-1 methodology. Selectivity towards butadiene reached 60–70%, making Zn–Ta-TUD-1 one of the best performing catalysts in the literature. To rationalize these results and establish a structure–activity relationship, a series of similar catalysts was prepared and characterized. Nitrogen physisorption, XPS, ICP-AES, XRD, TEM, UV-vis spectroscopy, TGA NH3-TPD, H2-TPR and FT-IR techniques were used. The most active samples were found to possess a large specific surface area and highly dispersed metal oxide phase incorporated within the mesoporous silica matrix. In combination with catalytic testing, characterization also showed a direct correlation between the number of Lewis acid sites and butadiene yield, confirming the structure–activity relationship theory prevalent for the Lebedev process. Deactivation of Zn–Ta-TUD-1 was also studied using the same techniques to characterize the properties of spent catalysts. It was found that the accumulation of heavy carbonaceous species caused a reduction of specific surface area and pore size coinciding with the observed loss in activity. Nevertheless, the pores of TUD-1 were large enough to avoid total pore blockage and a high selectivity could be maintained for 72 hours.Show less >
Language :
Anglais
Audience :
Internationale
Popular science :
Non
Administrative institution(s) :
CNRS
Centrale Lille
ENSCL
INRA
Univ. Artois
Université de Lille
Centrale Lille
ENSCL
INRA
Univ. Artois
Université de Lille
Collections :
Research team(s) :
Valorisation des alcanes et de la biomasse (VAALBIO)
Submission date :
2022-03-02T07:13:20Z
2023-10-20T07:39:22Z
2023-10-20T07:39:22Z
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