摘要

A high-performance Pd/Fe3O4 catalyst for aqueous-phase reforming (APR) of ethylene glycol (EG) to H-2 was prepared facilely by the co-precipitation method. After proper activation, the Pd was present as highly dispersed metallic nanoparticles with dimension of <3 nm, and the Fe was present as magnetite. When compared to Pd catalyst supported on Fe2O3, NiO, Cr2O3, Al2O3, or ZrO2 prepared by incipient wetness impregnation, the Pd/Fe3O4 catalyst displayed superior catalytic performance in terms of activity, selectivity, and stability. The intrinsic activity of the Pd/Fe3O4 catalyst was about three times of that of the second most active Pd/Fe2O3 catalyst under the same reaction conditions. In addition, the Pd/Fe3O4 catalyst retained similar to 80% of its initial activity after reaching the steady-state. Notably, the Pd/Fe3O4 catalyst possessed the highest turnover frequency of H-2 (109 min(-1)) reported so far, showing its promise as a new practical catalyst for APR of biomass-derived oxygenates to H-2. The excellent catalytic performance of the Pd/Fe3O4 catalyst was attributed to the enhanced synergistic effect between small Pd nanoparticles and magnetite in promoting the water-gas shift reaction, the rate-determining step in APR of EG over Pd-based catalysts.