Selective C = C Hydrogenation of α,β-Unsaturated Aldehydes Over Intermetallic Ni3Sb Catalysts
摘要
Selective hydrogenation of α,β-unsaturated aldehydes to saturated aldehydes is a transformation of considerable industrial relevance, providing intermediates for pharmaceutical, fragrance, and food additive applications. Conventional nickel-based catalysts, however, often cause over-hydrogenation of the target saturated aldehydes to saturated alcohols, thereby requiring relatively stringent kinetic control. Herein, we report a facile sol-gel route for preparing intermetallic Ni3Sb catalysts that achieve 97.1% butenal conversion and 97.5% selectivity toward butanal under mild conditions (25 ℃, 2 MPa H2). Mechanistic studies reveal that Sb atoms electronically modulate surface Ni sites, reducing the adsorption strength of saturated aldehyde intermediates while simultaneously elevating the activation barrier of undesired C = O bond hydrogenation. This electronic modulation suppresses over-hydrogenation without compromising C = C bond activation efficiency, offering a promising approach for the design of non-noble metal catalysts for the selective hydrogenation of α,β-unsaturated aldehydes.
Graphical Abstract