TY - JOUR
T1 - The high activity of mesoporous Ga-SiO2 catalysts in the upgrading of glycerol to solketal explained by in-depth characterization
AU - Vivian, Alvise
AU - Soumoy, Loraine
AU - Fusaro, Luca
AU - Louette, Pierre
AU - Felten, Alexandre
AU - Fiorilli, Sonia
AU - Debecker, Damien P.
AU - Aprile, Carmela
N1 - Funding Information:
Authors acknowledge the ‘Communauté française de Belgique’ – including the PhD fellowship of A. Vivian – through the ARC programme (15/20-069) and the FNRS through the FNRS-EQP-U.N034.17F for the financial support. L. Soumoy thanks the FNRS for the financial support in the context of her FRIA PhD grant. This research used resources of the “Technology Platform 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. D.P. Debecker thanks the Francqui Foundation for his “Francqui Research Professor” chair. F. Devred is acknowledged for the technical and logistical support.
Funding Information:
Authors acknowledge the ‘Communauté française de Belgique’ – including the PhD fellowship of A. Vivian – through the ARC programme (15/20-069) and the FNRS through the FNRS-EQP-U.N034.17F for the financial support. L. Soumoy thanks the FNRS for the financial support in the context of her FRIA PhD grant. This research used resources of the “Technology Platform Physico-Chemical Characterization” – PC 2 , the SIAM platform (Synthesis, Irradiation & Analysis of Materials) and the MORPH-IM platform (Morphology & Imaging) located at the University of Namur. D.P. Debecker thanks the Francqui Foundation for his “Francqui Research Professor” chair. F. Devred is acknowledged for the technical and logistical support.
Publisher Copyright:
© 2021 Elsevier Inc.
PY - 2021/8
Y1 - 2021/8
N2 - Mesoporous Ga-silicates were prepared using a sustainable and continuous aerosol synthesis procedure. The novel solids showed record activity in the synthesis of solketal from glycerol and acetone. Three different Si/Ga ratios of 34, 74 and 148 were investigated and all materials displayed favorable features for catalytic applications such as high surface area and calibrated mesoporosity. An in-depth characterization allowed to elucidate the remarkable catalytic performance. The insertion of Ga predominantly as single site in tetrahedral coordination in the silica framework was highlighted by X-ray photoelectron spectroscopy (XPS), using the Auger parameter of Ga in a Wagner plot representation. The speciation of Ga was further clarified using solid state 71Ga NMR spectroscopy, confirming the formation of mainly isolated Ga species. Consistently, the aerosol-made Ga-silicates displayed outstanding turnover frequencies (up to 677 h−1) and selectivity, markedly outcompeting other reference metallosilicate catalysts reported in literature. Moreover, the most active catalyst was successfully reused in multiple catalytic cycles thus proving its stability under the selected reaction conditions.
AB - Mesoporous Ga-silicates were prepared using a sustainable and continuous aerosol synthesis procedure. The novel solids showed record activity in the synthesis of solketal from glycerol and acetone. Three different Si/Ga ratios of 34, 74 and 148 were investigated and all materials displayed favorable features for catalytic applications such as high surface area and calibrated mesoporosity. An in-depth characterization allowed to elucidate the remarkable catalytic performance. The insertion of Ga predominantly as single site in tetrahedral coordination in the silica framework was highlighted by X-ray photoelectron spectroscopy (XPS), using the Auger parameter of Ga in a Wagner plot representation. The speciation of Ga was further clarified using solid state 71Ga NMR spectroscopy, confirming the formation of mainly isolated Ga species. Consistently, the aerosol-made Ga-silicates displayed outstanding turnover frequencies (up to 677 h−1) and selectivity, markedly outcompeting other reference metallosilicate catalysts reported in literature. Moreover, the most active catalyst was successfully reused in multiple catalytic cycles thus proving its stability under the selected reaction conditions.
KW - Aerosol-assisted sol–gel
KW - Glycerol valorization, Ga NMR
KW - Mesoporous materials
KW - XPS Wagner plot
UR - http://www.scopus.com/inward/record.url?scp=85107693080&partnerID=8YFLogxK
U2 - 10.1016/j.jcat.2021.05.017
DO - 10.1016/j.jcat.2021.05.017
M3 - Article
AN - SCOPUS:85107693080
SN - 0021-9517
VL - 400
SP - 83
EP - 92
JO - Journal of Catalysis
JF - Journal of Catalysis
ER -