Combining the advantages of both heterogeneous and homogeneous catalysts,single-atom catalysts(SACs)with unique electronic properties have shown excellent catalytic properties.Herein,we report single-atom Pd dispersed...Combining the advantages of both heterogeneous and homogeneous catalysts,single-atom catalysts(SACs)with unique electronic properties have shown excellent catalytic properties.Herein,we report single-atom Pd dispersed on nanoscale TiO2 prepared by self-assembly method as efficient and selective catalysts for the hydrogenation of phenylacetylene to styrene.The catalysts were characterized by N2 adsorption/desorption,X-ray diffraction(XRD),transmission electron microscopy(TEM),X-ray photoelectron spectroscopy(XPS),diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)and X-ray absorption spectroscopy(XAS).0.2 Pd-TiO2(150℃)possessing dominant single-atom Pd species,exhibited a turnover frequency(TOF)of over 8000 h^-1 with 91%selectivity towards styrene at room temperature.Further increasing Pd loading from 0.2%to 0.5%and 1.5%resulted in the decrease of activity probably due to the formation of Pd nanoparticles.Besides,the 0.2 Pd-TiO2 prepared by self-assembly strategy showed better catalytic performance than commercial 10%Pd/C and0.2 Pd-TiO2 synthesized by using impregnation method.展开更多
基金supported by the National University of Singapore Flagship Green Energy Program (#R-279-000-553-646 and R-279-000-553-731)the National Natural Science Foundation of China (21908085)the Natural Science Foundation of Jiangsu Province,China (BK20190961)
文摘Combining the advantages of both heterogeneous and homogeneous catalysts,single-atom catalysts(SACs)with unique electronic properties have shown excellent catalytic properties.Herein,we report single-atom Pd dispersed on nanoscale TiO2 prepared by self-assembly method as efficient and selective catalysts for the hydrogenation of phenylacetylene to styrene.The catalysts were characterized by N2 adsorption/desorption,X-ray diffraction(XRD),transmission electron microscopy(TEM),X-ray photoelectron spectroscopy(XPS),diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)and X-ray absorption spectroscopy(XAS).0.2 Pd-TiO2(150℃)possessing dominant single-atom Pd species,exhibited a turnover frequency(TOF)of over 8000 h^-1 with 91%selectivity towards styrene at room temperature.Further increasing Pd loading from 0.2%to 0.5%and 1.5%resulted in the decrease of activity probably due to the formation of Pd nanoparticles.Besides,the 0.2 Pd-TiO2 prepared by self-assembly strategy showed better catalytic performance than commercial 10%Pd/C and0.2 Pd-TiO2 synthesized by using impregnation method.
