Liquid Gallium Nanoislands on Zeolite: A Dynamic Confinement Strategy to Break the Catalytic Trade-Off in Hydrodeoxygenation

Abstract Breaking the pervasive activity–selectivity–stability trade-off in catalytic hydrodeoxygenation (HDO) remains a formidable challenge. Herein, we report a bifunctional nanoisland catalyst (GaNPs-Pt/Beta) that overcomes this limitation by utilizing liquid gallium nanodroplets anchored on Beta zeolite as mobile nanoislands. These islands effectively restrict platinum single-atom migration and agglomeration. Concurrently, Brønsted acid sites provided by the zeolite sea facilitate the dehydration-etherification process. This synergy enables highly efficient transfer hydrogenation at the gallium–platinum interface, achieving selective C–O bond cleavage while preserving C═C bonds under mild conditions. Benefiting from this island-sea architecture, the GaNPs-Pt/Beta catalyst delivers high catalytic activity, achieving >99% cinnamyl alcohol conversion and 93.8% β-methylstyrene selectivity within 6 h at 160 °C, with recyclability demonstrated over nine cycles involving intercycle regeneration. This strategy is scalable to diverse α,β-unsaturated aldehyde/alcohol chemicals, demonstrating that zeolite-based liquid metal nanoislands provide a versatile platform for the sustainable synthesis of high-value chemicals.