Abstract
AbstractLewis acidic and/or basic sites are typically clarified to play a positive role in the cascade hydrogen transfer and lactonization process, while the influence of Brønsted acid species on the catalyst activity and stability is rarely studied. In this work, a new acid‐base bifunctional hybrid BPhZr with augmented average pore diameter was prepared from the assembly of ([1, 1’‐biphenyl]‐4,4’‐diylbis(methylene))diphosphonic acid with zirconium via a facile solvothermal method. The effects of reaction parameters, substrate scope, and metal ion type were investigated. Besides the promotional effect of moderate Lewis acid/base sites and improved texture properties, the presence of Brønsted acidic species (e. g., –OH) in BPhZr was demonstrated to positively promote the synthesis of γ‐valerolactone (GVL; ca. 95% yield) from levulinates via cascade transfer hydrogenation and lactonization. In comparison with previously reported catalysts, the BPhZr hybrid exhibited a superior activity in terms of TOF (3.2 h−1) and activation energy (21 kJ/mol) for the reaction. Moreover, BPhZr was found to be highly stable and recyclable in five consecutive cycles, showing no significant decrease in GVL yield and selectivity.
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