University of Sydney – Cascade response engineering on zirconia-supported mesoporous MFI zeolites with tunable Lewis–Brønsted acid web sites: a case of the one-pot conversion of furfural to γ-valerolactone

University of Sydney –

Cascade response engineering on zirconia-supported mesoporous MFI zeolites with tunable Lewis–Brønsted acid web sites: a case of the one-pot conversion of furfural to γ-valerolactone†

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Catalytic cascade reactions are strongly desired as a doubtless job of combining multistep reactions into a single catalytic reactor. Acceptable catalysts serene of multi-reactive web sites to catalyze cascade reactions in a sequential style are central to such efforts. Right here, we elaborate a bifunctional zeolite catalyst with terminate proximity of Brønsted and Lewis acid web sites via the synthesis of a mesoporous ZrO₂[Al]MFI nanosponge (NS). The uncommon mesopores of the MFI-NS allow the confinement of zirconium oxide clusters (Lewis acid web sites, LA) for the length of the few-unit-cell-thin MFI aluminosilicate zeolite wall (Brønsted acid web sites, BA). This type of construction is clearly obvious from the conventional MFI zeolite, where the agglomeration of zirconium oxide clusters onto the exterior surface dwelling for the length of the crystal bulk will not be that you may per chance well well presumably possess, leading to segregated BA and LA web sites on the interior and exterior zeolite, respectively. By bringing the BA and LA within ZrO₂[Al]MFI-NS 30, we uncovered a more surroundings pleasant catalytic route for the conversion of furfural (100% within 2 h) to γ-valerolactone (GVL) (83%). This route is finest evident when the prolonged molecular diffusion direction, in essentially the most crude case of physically blended ZrO₂-(LA) and Al-zeolites (BA) (45% of GVL yield), is eliminated. Unlike the bifunctional ZrO₂–Al-beta (GVL yield of 75%), where the BA concentration is very much compromised on the expense of LA formation, we also indicate that the ZrO₂[Al]MFI-NS is able to help a excessive density and upright balance of every forms of acids.