A core shell structured C@MoxTi1-xO2-δnanocrystal with a functionalized interface(C@MTNC-FI)was fabricated via the hydrothermal method with subsequent annealing derived from tetrabutyl orthotitanate.The formation of ...A core shell structured C@MoxTi1-xO2-δnanocrystal with a functionalized interface(C@MTNC-FI)was fabricated via the hydrothermal method with subsequent annealing derived from tetrabutyl orthotitanate.The formation of anatase TiO2 was inhibited by the simultaneous presence of the hydrothermal etching/regrowth process,infiltration of Mo dopants and carbon coating,which endows the C@MTNC-FI with an ultrafine crystalline architecture that has a Mo-functionalized interface and carbon-coated shell.Pt Ru nanoparticles(NPs)were supported on C@MTNC-FI by employing a microwave-assisted polyol process(MAPP).The obtained Pt Ru/C@MTNC-FI catalyst has 2.68 times higher mass activity towards methanol electrooxidation than that of the un-functionalized catalyst(Pt Ru/C@TNC)and 1.65 times higher mass activity than that of Pt Ru/C catalyst with over 25%increase in durability.The improved catalytic performance is due to several aspects including ultrafine crystals of TiO2 with abundant grain boundaries,Mofunctionalized interface with enhanced electron interactions,and core shell architecture with excellent electrical transport properties.This work suggests the potential application of an interface-functionalized crystalline material as a sustainable and clean energy solution.展开更多
Supported PtRu/C catalysts used in direct methanol fuel cells (DMFCs) were prepared by a new modified polyol method. Transmission electron microscopy (TEM), X-ray diffraction (XRD) and cyclic voltammograms (CVs) were ...Supported PtRu/C catalysts used in direct methanol fuel cells (DMFCs) were prepared by a new modified polyol method. Transmission electron microscopy (TEM), X-ray diffraction (XRD) and cyclic voltammograms (CVs) were carried out to characterize the morphology, composition and the electrochemical properties of the PtRu/C catalyst. The results revealed that the PtRu nanoparticles with small average particle size (≈2.5 nm), and highly dispersed on the carbon support. The PtRu/C catalyst exhibited high catalytic activity and anti poisoned performance than that of the JM PtRu/C. It is imply that the modified polyol method is efficient for PtRu/C catalyst preparation.展开更多
Wormholelike mesoporous carbons (WMCs) with three different pore diameters (D-P), namely WMC-F7 (D-p = 8.5 nm), WMC-F30 (D-p =4.4 nm), and WMC-F0 (D-p =3.1 nm) are prepared via a modified sol-gel process. Then PtRu na...Wormholelike mesoporous carbons (WMCs) with three different pore diameters (D-P), namely WMC-F7 (D-p = 8.5 nm), WMC-F30 (D-p =4.4 nm), and WMC-F0 (D-p =3.1 nm) are prepared via a modified sol-gel process. Then PtRu nanoparticles with the particle size (40 of 3.2 nm supported on WMCs are synthesized with a modified pulse microwave-assisted polyol method. It is found that the pore diameter of WMCs plays an important role in the electrochemical activity of PtRu toward alcohol electrooxidation reaction. PtRu/WMC-F7 with D-p > 2d(pt) exhibits the largest electrochemical surface area (ESA) and the highest activity toward methanol electrooxidation. With the decrease in Dp, PtRu/WMC-F30 and PtRu/WMC-F0 have much lower ESA and electrochemical activity, especially for the isopropanol electrooxidation with a larger molecular size. When D-p is more than twice d(pt), the mass transfer of reactants and electrolyte are easier, and thus more PtRu nanoparticles can be utilized and the catalysts activity can be enhanced. (C) 2016 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights reserved.展开更多
PtRu supported on TiO2-embedded carbon nanofibers(PtRu/TECNF),which was recently reported as a highly-active catalyst for methanol oxidation,was applied to a direct methanol fuel cell(DMFC),and the power generation pe...PtRu supported on TiO2-embedded carbon nanofibers(PtRu/TECNF),which was recently reported as a highly-active catalyst for methanol oxidation,was applied to a direct methanol fuel cell(DMFC),and the power generation performance was compared to that using the commercial PtRu/C.Before the comparison,the effect of the catalyst loading on the power density of the DMFC was investigated using PtRu(18 wt%)/TECNF.The DMFC power density showed a maximum at about a 1.5 mg cm2 PtRu loading that corresponds to about an 80 mm layer thickness.A catalyst layer thicker than this value reduced the power density probably due to the concentration overvoltage.The PtRu content in the PtRu/TECNF was then increased to 30 wt%or more to reduce the layer thickness and to increase the power density.The DMFC performance was compared to that of different anode catalysts at a 1 mg cm2 PtRu loading.The power density was maximized using the PtRu30 wt%/TECNF,which showed a 173 mW cm2 at 353 K and had 66 mm layer thick,that was 26%higher than that of commercial PtRu/C.The current–voltage curve of the DMFC with the PtRu/TECNF suggested an improved mass transport overvoltage,but a little improvement in the activation one despite using the catalyst with about a 2 times higher activity compared to that of the commercial PtRu/C.This was attributed to the lower Pt utilization of the nanofiber catalyst layer.展开更多
基金the National Natural Science Foundation of China (Grant Nos. 21273058, 21673064, 51802059 and 21503059)China Postdoctoral Science Foundation (Grant Nos. 2018M631938, 2018T110307 and 2017M621284)+1 种基金Heilongjiang Postdoctoral Fund (LBH-Z17074)Fundamental Research Funds for the Central Universities (Grant No. HIT. NSRIF. 2019040 and 2019041)
文摘A core shell structured C@MoxTi1-xO2-δnanocrystal with a functionalized interface(C@MTNC-FI)was fabricated via the hydrothermal method with subsequent annealing derived from tetrabutyl orthotitanate.The formation of anatase TiO2 was inhibited by the simultaneous presence of the hydrothermal etching/regrowth process,infiltration of Mo dopants and carbon coating,which endows the C@MTNC-FI with an ultrafine crystalline architecture that has a Mo-functionalized interface and carbon-coated shell.Pt Ru nanoparticles(NPs)were supported on C@MTNC-FI by employing a microwave-assisted polyol process(MAPP).The obtained Pt Ru/C@MTNC-FI catalyst has 2.68 times higher mass activity towards methanol electrooxidation than that of the un-functionalized catalyst(Pt Ru/C@TNC)and 1.65 times higher mass activity than that of Pt Ru/C catalyst with over 25%increase in durability.The improved catalytic performance is due to several aspects including ultrafine crystals of TiO2 with abundant grain boundaries,Mofunctionalized interface with enhanced electron interactions,and core shell architecture with excellent electrical transport properties.This work suggests the potential application of an interface-functionalized crystalline material as a sustainable and clean energy solution.
文摘Supported PtRu/C catalysts used in direct methanol fuel cells (DMFCs) were prepared by a new modified polyol method. Transmission electron microscopy (TEM), X-ray diffraction (XRD) and cyclic voltammograms (CVs) were carried out to characterize the morphology, composition and the electrochemical properties of the PtRu/C catalyst. The results revealed that the PtRu nanoparticles with small average particle size (≈2.5 nm), and highly dispersed on the carbon support. The PtRu/C catalyst exhibited high catalytic activity and anti poisoned performance than that of the JM PtRu/C. It is imply that the modified polyol method is efficient for PtRu/C catalyst preparation.
基金supported by the National Natural Science Foundation of China (no. 91434106)
文摘Wormholelike mesoporous carbons (WMCs) with three different pore diameters (D-P), namely WMC-F7 (D-p = 8.5 nm), WMC-F30 (D-p =4.4 nm), and WMC-F0 (D-p =3.1 nm) are prepared via a modified sol-gel process. Then PtRu nanoparticles with the particle size (40 of 3.2 nm supported on WMCs are synthesized with a modified pulse microwave-assisted polyol method. It is found that the pore diameter of WMCs plays an important role in the electrochemical activity of PtRu toward alcohol electrooxidation reaction. PtRu/WMC-F7 with D-p > 2d(pt) exhibits the largest electrochemical surface area (ESA) and the highest activity toward methanol electrooxidation. With the decrease in Dp, PtRu/WMC-F30 and PtRu/WMC-F0 have much lower ESA and electrochemical activity, especially for the isopropanol electrooxidation with a larger molecular size. When D-p is more than twice d(pt), the mass transfer of reactants and electrolyte are easier, and thus more PtRu nanoparticles can be utilized and the catalysts activity can be enhanced. (C) 2016 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights reserved.
基金the Element Innovation Project,Ministry of Education,Japan,and by KAKENHI(26289300).
文摘PtRu supported on TiO2-embedded carbon nanofibers(PtRu/TECNF),which was recently reported as a highly-active catalyst for methanol oxidation,was applied to a direct methanol fuel cell(DMFC),and the power generation performance was compared to that using the commercial PtRu/C.Before the comparison,the effect of the catalyst loading on the power density of the DMFC was investigated using PtRu(18 wt%)/TECNF.The DMFC power density showed a maximum at about a 1.5 mg cm2 PtRu loading that corresponds to about an 80 mm layer thickness.A catalyst layer thicker than this value reduced the power density probably due to the concentration overvoltage.The PtRu content in the PtRu/TECNF was then increased to 30 wt%or more to reduce the layer thickness and to increase the power density.The DMFC performance was compared to that of different anode catalysts at a 1 mg cm2 PtRu loading.The power density was maximized using the PtRu30 wt%/TECNF,which showed a 173 mW cm2 at 353 K and had 66 mm layer thick,that was 26%higher than that of commercial PtRu/C.The current–voltage curve of the DMFC with the PtRu/TECNF suggested an improved mass transport overvoltage,but a little improvement in the activation one despite using the catalyst with about a 2 times higher activity compared to that of the commercial PtRu/C.This was attributed to the lower Pt utilization of the nanofiber catalyst layer.