One-step hydrothermal synthesis of a cellulose-derived zirconium catalyst for efficient transfer hydrogenation of methyl levulinate to γ-valerolactone.

Abstract

The design of simple, efficient, and cost-effective catalysts for catalytic transfer hydrogenation (CTH) of biomass-derived levulinic acid derivatives remains a key research focus. Herein, a cellulose-derived zirconium catalyst (Cel-Zr) was synthesized via a one-step hydrothermal method using cellulose and zirconium tetrachloride. Cel-Zr exhibited excellent catalytic performance in the CTH conversion of methyl levulinate (ML) to γ-valerolactone (GVL). At 170 °C for 8 h with 0.05 g catalyst, Cel-Zr afforded 99.2% ML conversion and 98.6% GVL selectivity. Cel-Zr showed broad substrate applicability toward biomass-derived compounds, including ethyl levulinate, butyl levulinate, levulinic acid, and furfural. Recycling experiments demonstrated good stability, with ML conversion and GVL yield remaining at 94.2% and 90.1%, respectively, after ten consecutive runs. Leaching experiments supported the heterogeneous nature of Cel-Zr, with minimal zirconium leaching. Characterization results revealed that highly dispersed amorphous Zr species were firmly immobilized on the cellulose-derived support through Zr-O-C/Zr-O interfacial interactions, generating abundant Lewis acid sites and excellent thermal stability. The facile synthesis strategy, low-cost feedstocks, high catalytic activity, and durability make Cel-Zr a promising catalyst for biomass valorization and sustainable GVL production.

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