Construction of Synergistic Cu–Zn Alloy Interfaces within Hierarchical Zeolite Nanosheets for High-Efficiency Production of 2-Methylfuran from Furfural

The hydrodeoxygenation of furfural to 2-methylfuran represents a critical route for biomass valorization, although hindered by slow kinetics and undesired side reactions. Key challenges involve designing catalytic sites that enable enhanced H2 activation and vertically oriented furfural adsorption. Herein, we engineer a self-pillared silicalite-1 nanosheet-supported Cu–Zn bimetallic catalyst to overcome these limitations. The hierarchically porous silicalite-1 architecture serves dual functions: (1) stabilizing highly dispersed Cu–Zn alloy interfaces and (2) inducing electronic modulation that synergistically enhances dissociative H2 chemisorption and spillover. Crucially, this interface imposes a stable η1-(O)-aldehyde adsorption configuration for both furfural and its furfuryl alcohol intermediate, effectively suppressing ring-hydrogenation-inducing flat η2-(C,O) adsorption modes. At a moderate 180 °C, this integrated catalyst design achieves a 2-methylfuran turnover frequency (TOF) of 20.6 h–1 with near-quantitative selectivity (99.2% yield) after one hour of reaction.