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Article Dans Une Revue Green Chemistry Année : 2020

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


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.


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




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⟩
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