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Unlocking the Acidity-Reactivity Correlation of Metal(IV)-Doped Silica Nanotubes in the Conversion of Ethyl Levulinate

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Résumé

Metal-doped hollow silica nanotubes (M-NT, where M = Ti, Zr, Hf) were successfully synthesized via a straightforward impregnation of pristine hollow silica nanotubes with M-acetylacetonate solutions. After their characterization, the materials were tested as heterogeneous catalysts for the conversion of ethyl levulinate (EL) into γ-valerolactone (GVL) revealing highly promising activity for the target reaction. Special emphasis was given on disclosing the influence of the nature of the acid sites (Lewis or Brønsted) and their strength on the catalytic performances. Ammonia temperature programmed desorption (NH3-TPD), 31P solid-state nuclear magnetic resonance (31P-ssNMR) of trimethylphosphine and FT-IR of adsorbed ammonia, were the key techniques to evaluate the structure–activity correlation. The best solid exceeds the activity of other reference catalysts reported in the literature and tested under similar reaction conditions. The efficient recyclability of the best catalyst of the series was evaluated as well. The low E-factor obtained further confirmed the overall sustainability of the process.

langue originaleAnglais
journalChemCatChem
Les DOIs
Etat de la publicationAccepté/sous presse - 2025

Financement

Authors acknowledge the FNRS for the financial support in the context of the FRIA PhD grants of A. Maertens and L. Soumoy and the EOS funding scheme for the PhD grant of M. Saitta. This project received funding from the FWO and F.R.S.-FNRS (Belgium) under the Excellence of Science (EOS) program (“PHOSPORE” – EOS reference number: 40,007,504) as well as from the FNRS via a PdR project (ref: T.0004.21). This research used resources of PC2 (Physico-Chemical Characterization), MORPH-IM (Morphology & Imaging), and SIAM (Synthesis, Irradiation & Analysis of Materials) technology platforms located at the University of Namur. This research also used resources of the Institute of Condensed Matter and Nanosciences (IMCN) at Université catholique de Louvain (UCLouvain) to conduct the ammonia temperature-programmed desorption coupled with mass spectrometry analysis. The IR measurements were performed at the Polytechnic of Turin. Authors acknowledge the FNRS for the financial support in the context of the FRIA PhD grants of A. Maertens and L. Soumoy and the EOS funding scheme for the PhD grant of M. Saitta. This project received funding from the FWO and F.R.S.‐FNRS (Belgium) under the Excellence of Science (EOS) program (“PHOSPORE” – EOS reference number: 40,007,504) as well as from the FNRS via a PdR project (ref: T.0004.21). This research used resources of PC (Physico‐Chemical Characterization), MORPH‐IM (Morphology & Imaging), and SIAM (Synthesis, Irradiation & Analysis of Materials) technology platforms located at the University of Namur. This research also used resources of the Institute of Condensed Matter and Nanosciences (IMCN) at Université catholique de Louvain (UCLouvain) to conduct the ammonia temperature‐programmed desorption coupled with mass spectrometry analysis. The IR measurements were performed at the Polytechnic of Turin.

Bailleurs de fondsNuméro du bailleur de fonds
Université Catholique de Louvain
Fonds Wetenschappelijk Onderzoek - Vlaanderen (FWO)
MORPH-IM
Fonds De La Recherche Scientifique - FNRS
Excellence of ScienceT.0004.21, 40,007,504

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