TiO2‐supported Pd‐Sb bimetallic catalysts were prepared and evaluated for the direct synthesis of H2O2 at ambient pressure.The addition of Sb to Pd significantly enhanced catalytic performance,and a Pd50Sb catalyst ...TiO2‐supported Pd‐Sb bimetallic catalysts were prepared and evaluated for the direct synthesis of H2O2 at ambient pressure.The addition of Sb to Pd significantly enhanced catalytic performance,and a Pd50Sb catalyst showed the greatest selectivity of up to 73%.Sb promoted the dispersion of Pd on TiO2,as evidenced by transmission electron microscopy and X‐ray diffraction.X‐ray photoelectron spectroscopy indicated that the oxidation of Pd was suppressed by Sb.In addition,Sb2O3 layers were formed and partially wrapped the surfaces of Pd catalysts,thus suppressing the activation of H2 and subsequent hydrogenation of H2O2.In situ diffuse reflection infrared Fourier transform spectroscopy for CO adsorption suggested that Sb homogenously located on the surface of Pd‐Sb catalysts and isolated contiguous Pd sites,resulting in the rise of the ratio of Pd monomer sites that are favorable for H2O2 formation.As a result,the Sb modified Pd surfaces significantly enhanced the non‐dissociative activation of O2 and H2O2 selectivity.展开更多
A series of bimetallic Pd-Pb catalysts with a constant Pd content of 1 wt%and Pb/Pd atomic ratio from 0 to 1.6 supported on γ-Al2O3 were prepared and used for glycerol oxidation with H2O2 as the oxidizing agent at at...A series of bimetallic Pd-Pb catalysts with a constant Pd content of 1 wt%and Pb/Pd atomic ratio from 0 to 1.6 supported on γ-Al2O3 were prepared and used for glycerol oxidation with H2O2 as the oxidizing agent at atmospheric pressure,45℃ and pH =11.The morphology and dispersion of the catalysts were characterized by scanning electron microscopy-energy dispersive X-ray spectroscopy（SEM-EDX） and transmission electron microscopy（TEM）.The presence of an alloy phase in the bimetallic catalyst was detected by X-ray photoelectron spectroscopy（XPS）.Glycerol conversion obtained with the monometallic Pd catalyst was 19%,which was increased to 100%with the addition of Pb.The four bimetallic PdPb catalysts were able to oxidize glycerol to dihydroxyacetone（DIHA） and the selectivity to DIHA reached 59%,58%,34%and 25%for PdPb0.25,PdPb0.50,PdPb1.00 and PdPbl.60 catalysts,respectively.展开更多
Bimetallic palladium-gold （PdAu） catalysts have better catalytic performance than monometallic catalysts for many applications. PdAu catalysts with controlled nanostructures and enhanced activi- ties have been exten...Bimetallic palladium-gold （PdAu） catalysts have better catalytic performance than monometallic catalysts for many applications. PdAu catalysts with controlled nanostructures and enhanced activi- ties have been extensively studied but their syntheses require multiple and occasionally complicated steps, In this work, we demonstrated that supported PdAu catalysts could be simply prepared by doping a supported Pd catalyst with gold through wet impregnation and calcination. Resulting PdAu-on-carbon （PdAu/C） catalysts were tested for the room-temperature, aqueous-phase hydro- dech/orination of trichloroethene. The most active PdAu/C catalyst （Pd 1.0 wt%, Au 1.1 wt%, dried/air/H2 process] had an initial turnover frequency （TOF] of 34.0×10^-2 mOITcE mOled-1 S-1, which was 〉15 times higher than monometallic Pd/C （Pd 1,0 wt%, initial TOF of 2.2 ×10^-2 molTCE molpd^-1s^-1）. Through X-ray absorption spectroscopy, the gold kept Pd from oxidizing under calcination at 400℃. Probable nanostructure evolution pathways are proposed to explain the observed catalysis,展开更多
A simple and efficient solution-based method for the synthesis of Pd-Ni bimetallic nanoparticles （NPs） has been developed. A series of Pd-Ni bimetallic NPs were readily achieved by reduction of PdC12 and Ni（acac）2...A simple and efficient solution-based method for the synthesis of Pd-Ni bimetallic nanoparticles （NPs） has been developed. A series of Pd-Ni bimetallic NPs were readily achieved by reduction of PdC12 and Ni（acac）2 （acac = acetyl- acetonate） in the presence of oleylamine （OAm）, oleic acid （OA） and benzyl alcohol. Furthermore, by using high-resolution transmission electron microscopy （HRTEM）, energy-dispersive spectrometry （EDS） mapping and X-ray diffraction （XRD）, we demonstrate that the as-prepared Pd-Ni bimetallic NPs have core-shell structures with a Pd-rich core and a Ni-rich shell. In addition, the as-obtained Pd-Ni bimetallic NPs with varying compositions show excellent catalytic activities in the Miyaura-Suzuki reaction. When the nickel molar percentage was 0.23 to 0.65, the conversion with the as-obtained Pd-Ni bimetallic catalysts was above 90%. It is believed that this strategy can be employed to produce a variety of other well-defined core-shell type multimetallic nanostructures.展开更多
Less-expensive but efficient electrocatalysts are essential to accelerate the commercialization of fuel cells.Herein,ultrathin PdPb nanowires(PdPb NWs)with a diameter of around 3.5 nm were prepared by using a one-step...Less-expensive but efficient electrocatalysts are essential to accelerate the commercialization of fuel cells.Herein,ultrathin PdPb nanowires(PdPb NWs)with a diameter of around 3.5 nm were prepared by using a one-step hydrothermal method.The introduction of Pb in Pd-based bimetallic nanostructures produced high differences in the morphology from Pd nanoparticles(NPs)to various PdPb NWs.All the as-prepared PdPb NWs exhibited better electrocatalytic activity and durability than Pd NPs due to the synergistic effect.Especially,Pd65Pb35 possessed the highest current density of about 3460 mA mgPd^−1 for the ethanol electrooxidation which was around 6.3 times higher than commercial Pd/C.The high-performance of Pd65Pb35 is attributed to the defect-rich and stable nanowire structure with optimized surface atomic arrangement,as evidenced by high resolution transmission electron microscopy measurements and long-time treatment in an acidic media.The differences in the morphologies and electrocatalytic activities of PdPb NWs with varied Pb contents have also been discussed and analyzed.展开更多
基金supported by the National Basic Research Program of China(973 Program,2011CB201400)the National Natural Science Foundation of China(21173008,21373019,21433001)~~
基金supported by the National Natural Science Foundation of China(91534127,U1463205)the Innovation Scientists and Technicians Troop Construction Projects of Henan Provincethe Chinese Education Ministry 111 Project(B08021)~~
文摘TiO2‐supported Pd‐Sb bimetallic catalysts were prepared and evaluated for the direct synthesis of H2O2 at ambient pressure.The addition of Sb to Pd significantly enhanced catalytic performance,and a Pd50Sb catalyst showed the greatest selectivity of up to 73%.Sb promoted the dispersion of Pd on TiO2,as evidenced by transmission electron microscopy and X‐ray diffraction.X‐ray photoelectron spectroscopy indicated that the oxidation of Pd was suppressed by Sb.In addition,Sb2O3 layers were formed and partially wrapped the surfaces of Pd catalysts,thus suppressing the activation of H2 and subsequent hydrogenation of H2O2.In situ diffuse reflection infrared Fourier transform spectroscopy for CO adsorption suggested that Sb homogenously located on the surface of Pd‐Sb catalysts and isolated contiguous Pd sites,resulting in the rise of the ratio of Pd monomer sites that are favorable for H2O2 formation.As a result,the Sb modified Pd surfaces significantly enhanced the non‐dissociative activation of O2 and H2O2 selectivity.
基金supported by CONICET(PIP 0276)UNLP(Projects X 700)+1 种基金UNNOBA(SIB 2924/14)Ministry of Education and Sports(Call "Jorge Sabato" Project 44-144-415),Argentina
文摘A series of bimetallic Pd-Pb catalysts with a constant Pd content of 1 wt%and Pb/Pd atomic ratio from 0 to 1.6 supported on γ-Al2O3 were prepared and used for glycerol oxidation with H2O2 as the oxidizing agent at atmospheric pressure,45℃ and pH =11.The morphology and dispersion of the catalysts were characterized by scanning electron microscopy-energy dispersive X-ray spectroscopy（SEM-EDX） and transmission electron microscopy（TEM）.The presence of an alloy phase in the bimetallic catalyst was detected by X-ray photoelectron spectroscopy（XPS）.Glycerol conversion obtained with the monometallic Pd catalyst was 19%,which was increased to 100%with the addition of Pb.The four bimetallic PdPb catalysts were able to oxidize glycerol to dihydroxyacetone（DIHA） and the selectivity to DIHA reached 59%,58%,34%and 25%for PdPb0.25,PdPb0.50,PdPb1.00 and PdPbl.60 catalysts,respectively.
基金supported by the National Science Foundation,United States(EEC-0647452)the Welch Foundation(C-1676)~~
文摘Bimetallic palladium-gold （PdAu） catalysts have better catalytic performance than monometallic catalysts for many applications. PdAu catalysts with controlled nanostructures and enhanced activi- ties have been extensively studied but their syntheses require multiple and occasionally complicated steps, In this work, we demonstrated that supported PdAu catalysts could be simply prepared by doping a supported Pd catalyst with gold through wet impregnation and calcination. Resulting PdAu-on-carbon （PdAu/C） catalysts were tested for the room-temperature, aqueous-phase hydro- dech/orination of trichloroethene. The most active PdAu/C catalyst （Pd 1.0 wt%, Au 1.1 wt%, dried/air/H2 process] had an initial turnover frequency （TOF] of 34.0×10^-2 mOITcE mOled-1 S-1, which was 〉15 times higher than monometallic Pd/C （Pd 1,0 wt%, initial TOF of 2.2 ×10^-2 molTCE molpd^-1s^-1）. Through X-ray absorption spectroscopy, the gold kept Pd from oxidizing under calcination at 400℃. Probable nanostructure evolution pathways are proposed to explain the observed catalysis,
文摘A simple and efficient solution-based method for the synthesis of Pd-Ni bimetallic nanoparticles （NPs） has been developed. A series of Pd-Ni bimetallic NPs were readily achieved by reduction of PdC12 and Ni（acac）2 （acac = acetyl- acetonate） in the presence of oleylamine （OAm）, oleic acid （OA） and benzyl alcohol. Furthermore, by using high-resolution transmission electron microscopy （HRTEM）, energy-dispersive spectrometry （EDS） mapping and X-ray diffraction （XRD）, we demonstrate that the as-prepared Pd-Ni bimetallic NPs have core-shell structures with a Pd-rich core and a Ni-rich shell. In addition, the as-obtained Pd-Ni bimetallic NPs with varying compositions show excellent catalytic activities in the Miyaura-Suzuki reaction. When the nickel molar percentage was 0.23 to 0.65, the conversion with the as-obtained Pd-Ni bimetallic catalysts was above 90%. It is believed that this strategy can be employed to produce a variety of other well-defined core-shell type multimetallic nanostructures.
基金This work was financially supported by the National Natural Science Foundation of China(21773133)Taishan Scholars Advantageous and Distinctive Discipline Program for supporting the research team of energy storage materials of Shandong Province,China.
文摘Less-expensive but efficient electrocatalysts are essential to accelerate the commercialization of fuel cells.Herein,ultrathin PdPb nanowires(PdPb NWs)with a diameter of around 3.5 nm were prepared by using a one-step hydrothermal method.The introduction of Pb in Pd-based bimetallic nanostructures produced high differences in the morphology from Pd nanoparticles(NPs)to various PdPb NWs.All the as-prepared PdPb NWs exhibited better electrocatalytic activity and durability than Pd NPs due to the synergistic effect.Especially,Pd65Pb35 possessed the highest current density of about 3460 mA mgPd^−1 for the ethanol electrooxidation which was around 6.3 times higher than commercial Pd/C.The high-performance of Pd65Pb35 is attributed to the defect-rich and stable nanowire structure with optimized surface atomic arrangement,as evidenced by high resolution transmission electron microscopy measurements and long-time treatment in an acidic media.The differences in the morphologies and electrocatalytic activities of PdPb NWs with varied Pb contents have also been discussed and analyzed.
