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Dual Active Sites of Ni and FeNi3 Constructed from Layered Double Hydroxides for One-Pot Hydrogenation of Furfural to Tetrahydrofurfuryl Alcohol

Rongrong Li,Wenqi Liu,Huibin Liu,Hongyu Niu,Quan Zhou,Changhai Liang,Xiao Chen

One-pot hydrogenation of biomass-derived furfural with multiple reduction sites requires suitable metal sites to achieve a high value-added chemical in high yield. In this work, nonprecious Ni–Fe bimetallic catalysts with high efficiency derived from FexNiy/MgAl-LDH hydrotalcite precursors are prepared for one-pot sequential hydrogenation of furfural to tetrahydrofurfuryl alcohol at mild conditions. Through fine adjustment of metallic Fe/Ni molar ratios in hydrotalcite precursors, bimetallic FexNiy/MgAlO catalysts can be constructed. The topological transformation of hydrotalcite precursors provides a mesoporous structure for bimetallic supported catalysts. Due to the formation of the Ni–Fe alloy, there is an electron transfer from Fe to Ni in the catalyst due to the higher electronegativity of Ni than that of Fe, which greatly influences the adsorption of furfural on the surface of catalysts. Comparing the structures and catalytic performances of monometallic Ni/MgAlO and Fe/MgAlO catalysts, the Ni-rich Fe1Ni4/MgAlO catalyst with the dual active sites of metallic Ni and FeNi3 alloy presents high efficiency in sequential hydrogenation of the C═O bonds and C═C bonds of furfural to tetrahydrofurfuryl alcohol with the yield of 90.3% under 3 MPa H2 and 80 °C for 3 h, which can be an alternative for noble metal catalysts. Additionally, the Ni-rich Fe1Ni4/MgAlO catalyst presents excellent cycling stability. This design strategy for nonprecious NiFe bimetallic catalysts not only provide promising candidates for effective utilization of biobased furfural but also extend the application of bimetallic catalysts derived from hydrotalcite precursors for one-pot hydrogenation reactions.