In this work, the formation of levulinic acid (LA) as one of the top-twelve chemical building blocks from glucose was studied. In particular, the formulations of heterogeneous acid catalysts based on SBA-15, MCM-41 mesoporous silica was carried out and their performance in catalytic conversion of glucose to LA were assessed and compared with commercial H-Beta-25 (SiO2/Al2O3 = 25) microporous zeolite. The high surface area, suitable porosity, balanced acid sites were considered as the main factors of a proper catalytic performance. Thus, essential modification of mesoporous SBA-15 and MCM-41 materials was carried out by introducing Al in their structures for Lewis acid sites improvement. Alumina was introduced to SBA-15 by post synthesis evaporation impregnation method while it was embedded inside the MCM-41 mesoporous material during the synthesis. In addition, Bronsted acidity was introduced via post-synthesis grafting of sulfonic acid groups. The textural and morphological features and acidity of the materials were investigated using N-2 physisorption, SEM, EDX, TEM, XRD and pyridine-FTIR. All catalysts were tested for aqueous glucose conversion in an autoclave at 180 degrees C. Al-MCM-SO3H has shown the best performance with 54% of LA yield after 4 h reaction. According to Py-FTIR introduction of alumina and sulfonic acid groups improved weak and medium Lewis and Bronsted acid sites. However, the Bronsted to Lewis acid site ratio (B/L) was higher for Al-MCM-SO3H compared to SBA-Al-SO3H leading the reaction pathway to LA. H-Beta-25 zeolite displayed a poor performance because of harsh medium and strong acid sites catalyzing humins formation.[GRAPHICS]

Levulinic Acid Production: Comparative Assessment of Al-Rich Ordered Mesoporous Silica and Microporous Zeolite

Cruciani, Giuseppe
Investigation
;
2023

Abstract

In this work, the formation of levulinic acid (LA) as one of the top-twelve chemical building blocks from glucose was studied. In particular, the formulations of heterogeneous acid catalysts based on SBA-15, MCM-41 mesoporous silica was carried out and their performance in catalytic conversion of glucose to LA were assessed and compared with commercial H-Beta-25 (SiO2/Al2O3 = 25) microporous zeolite. The high surface area, suitable porosity, balanced acid sites were considered as the main factors of a proper catalytic performance. Thus, essential modification of mesoporous SBA-15 and MCM-41 materials was carried out by introducing Al in their structures for Lewis acid sites improvement. Alumina was introduced to SBA-15 by post synthesis evaporation impregnation method while it was embedded inside the MCM-41 mesoporous material during the synthesis. In addition, Bronsted acidity was introduced via post-synthesis grafting of sulfonic acid groups. The textural and morphological features and acidity of the materials were investigated using N-2 physisorption, SEM, EDX, TEM, XRD and pyridine-FTIR. All catalysts were tested for aqueous glucose conversion in an autoclave at 180 degrees C. Al-MCM-SO3H has shown the best performance with 54% of LA yield after 4 h reaction. According to Py-FTIR introduction of alumina and sulfonic acid groups improved weak and medium Lewis and Bronsted acid sites. However, the Bronsted to Lewis acid site ratio (B/L) was higher for Al-MCM-SO3H compared to SBA-Al-SO3H leading the reaction pathway to LA. H-Beta-25 zeolite displayed a poor performance because of harsh medium and strong acid sites catalyzing humins formation.[GRAPHICS]
2023
Taghavi, Somayeh; Pizzolitto, Cristina; Ghedini, Elena; Menegazzo, Federica; Cruciani, Giuseppe; Peurla, Markus; Eränen, Kari; Heinmaa, Ivo; Aho, Atte...espandi
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Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/11392/2539417
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