Properties and activity of zn-ta-tud-1 in the lebedev process - Université de Lille Accéder directement au contenu
Article Dans Une Revue Green Chemistry Année : 2020

Properties and activity of zn-ta-tud-1 in the lebedev process

Résumé

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.

Domaines

Catalyse
Fichier principal
Vignette du fichier
d0gc00103a.pdf (5.12 Mo) Télécharger le fichier
Origine Publication financée par une institution
Licence

Dates et versions

hal-04250906 , version 1 (23-10-2023)

Licence

Identifiants

Citer

Guillaume Pomalaza Raez, Pardis Simon, Ahmed Addad, Mickael Capron, Franck Dumeignil. Properties and activity of zn-ta-tud-1 in the lebedev process. Green Chemistry, 2020, Green chemistry an international journal and green chemistry resource GC, 22, pp.2558-2574. ⟨10.1039/d0gc00103a⟩. ⟨hal-04250906⟩
6 Consultations
2 Téléchargements

Altmetric

Partager

Gmail Mastodon Facebook X LinkedIn More