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 H 2 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 H 2 chemisorption and spillover. Crucially, this interface imposes a stable η 1 -(O)-aldehyde adsorption configuration for both furfural and its furfuryl alcohol intermediate, effectively suppressing ring-hydrogenation-inducing flat η 2 -(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.