摘要
In this study, a series of novel Pt-Ni bimetallic catalysts supported on LaFeO_3/SiO_2 with different amounts of Ni were prepared by the lattice atomic-confined reduction of LaFe_(1-x)(Ni, Pt)_xO_3/SiO_2 perovskite precursors and applied in isobutane dehydrogenation to isobutene reaction. The catalysts were characterized by X-ray diffraction, H_2-temperature-programmed reduction, Brunauer-Emmett-Teller analysis, transmission electron microscopy, energy dispersive X-ray, CO chemisorption, X-ray photoelectron spectroscopy, and thermogravimetric analysis. The as-synthesized Pt-Ni bimetallic catalysts possessed smaller most probable particle size with tunable Pt-Ni interaction, depending on the Ni content. The catalyst with Ni content of 3.0 wt% showed excellent activity and stability(the isobutane conversion and isobutene selectivity remained at about 38% and 92%, respectively, after 310 min) for the isobutane dehydrogenation reaction. It also provided approximately six times turnover frequency of the catalyst without Ni. The excellent activity and stability of the 3.0 wt% Ni-containing catalyst can be attributed to its small metal nanoparticles with high dispersion and suitable Pt-Ni interaction. Moreover, the Pt(Ni)-LaFeO_3/SiO_2 catalyst with Ni content of 3.0 wt% had been run for more than 35 h without obvious loss of activity,indicating its long-term stability, and the decrease in the Pt-Ni interaction that accompanied the formation of the FeNi alloy phase was thought to be responsible for the slight decrease in activity.
In this study, a series of novel Pt-Ni bimetallic catalysts supported on LaFeO_3/SiO_2 with different amounts of Ni were prepared by the lattice atomic-confined reduction of LaFe_(1-x)(Ni, Pt)_xO_3/SiO_2 perovskite precursors and applied in isobutane dehydrogenation to isobutene reaction. The catalysts were characterized by X-ray diffraction, H_2-temperature-programmed reduction, Brunauer-Emmett-Teller analysis, transmission electron microscopy, energy dispersive X-ray, CO chemisorption, X-ray photoelectron spectroscopy, and thermogravimetric analysis. The as-synthesized Pt-Ni bimetallic catalysts possessed smaller most probable particle size with tunable Pt-Ni interaction, depending on the Ni content. The catalyst with Ni content of 3.0 wt% showed excellent activity and stability(the isobutane conversion and isobutene selectivity remained at about 38% and 92%, respectively, after 310 min) for the isobutane dehydrogenation reaction. It also provided approximately six times turnover frequency of the catalyst without Ni. The excellent activity and stability of the 3.0 wt% Ni-containing catalyst can be attributed to its small metal nanoparticles with high dispersion and suitable Pt-Ni interaction. Moreover, the Pt(Ni)-LaFeO_3/SiO_2 catalyst with Ni content of 3.0 wt% had been run for more than 35 h without obvious loss of activity,indicating its long-term stability, and the decrease in the Pt-Ni interaction that accompanied the formation of the FeNi alloy phase was thought to be responsible for the slight decrease in activity.
基金
supported by National Natural Science Foundation of China (No. 21776214)
State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, China
