Highly active and robust electrocatalysts are desired for proton exchange membrane fuel cells.Pt-based intermetallic compounds(IMCs) have been recognized as one of the most promising low-platinum catalysts for fuel ce...Highly active and robust electrocatalysts are desired for proton exchange membrane fuel cells.Pt-based intermetallic compounds(IMCs) have been recognized as one of the most promising low-platinum catalysts for fuel cells(FCs).Herein,we report a high-performance IMCs by anchoring ordered PtCoNi ternary nanoparticles on the N,Co and Ni co-doped dodecahedral mesoporous carbon(DMC).While the introduced Co and Ni participate in the formation of PtCoNi IMCs,some of them are doped in the mesoporous carbon and coordinated by N to form Co-N_(y)/Ni-N_(z)dual active centers,which further enhances the electrocatalytic activity towards oxygen reduction reaction.Moreover,the addition of Ni results in a negative shift of the d-band center of Pt as compared to the Pt/DMC and Pt_(3)Co/DMC,making it easier to adsorb oxygen on the surface.As expected,our optimal sample Pt_(3)Co_(0.7)Ni_(0.3)/DMC exhibits excellent performance with mass activity and specific activity of 1.32 A mgPt-1and 1.98 mA cm^(-2)at 0.9 V,which are 7.33and 6.19 times that of commercial Pt/C,respectively.The Pt_(3)Co_(0.7)Ni_(0.3)/DMC also reveals much better cathodic performance in an H2-air single fuel cell than commercial Pt/C catalyst with a power density of0.802 W cm^(-2).This work provides critical sights into constructing efficient catalysts by ternary intermetallic strategy and synergetic effect between active components and support.展开更多
The crystal structures and magnetic properties of novel Eu TrGa3-r （T=Pd, It, Rh） in termetallic compounds are investigated by using powder x-ray diffraction and magnetic measurements. EuTrGa3-r crystallizes in orth...The crystal structures and magnetic properties of novel Eu TrGa3-r （T=Pd, It, Rh） in termetallic compounds are investigated by using powder x-ray diffraction and magnetic measurements. EuTrGa3-r crystallizes in orthorhombic structure with space group of Cmcm and Z = 4. There are four kinds of nonequivalent 4c crystal positions in EuTrGaa-r unit cell, which are occupied by 4Eu, 4GaⅠ, 4（GaⅡ, T） and 4GaⅢ, respectively. EuTrGa3-r ex- hibits the complex magnetic states in low-temperature regime, with the three-, two- and one-antiferromagnetic transitions occurring for T=Ir, T=Rh and T=Pd, respectively. It might be due to the Kondo effect： a localized antiferromagnetic interaction of the isolated impurity spins with the surrounding conduction electrons at low-temperature regime.展开更多
基金supported by the National Key Research and Development Program of China(2017YFB0102900 and 2016YFB0101201)the National Natural Science Foundation of China(51971094,21476088 and 21776104)the Guangdong Provincial Department of Science and Technology(2015A030312007)。
文摘Highly active and robust electrocatalysts are desired for proton exchange membrane fuel cells.Pt-based intermetallic compounds(IMCs) have been recognized as one of the most promising low-platinum catalysts for fuel cells(FCs).Herein,we report a high-performance IMCs by anchoring ordered PtCoNi ternary nanoparticles on the N,Co and Ni co-doped dodecahedral mesoporous carbon(DMC).While the introduced Co and Ni participate in the formation of PtCoNi IMCs,some of them are doped in the mesoporous carbon and coordinated by N to form Co-N_(y)/Ni-N_(z)dual active centers,which further enhances the electrocatalytic activity towards oxygen reduction reaction.Moreover,the addition of Ni results in a negative shift of the d-band center of Pt as compared to the Pt/DMC and Pt_(3)Co/DMC,making it easier to adsorb oxygen on the surface.As expected,our optimal sample Pt_(3)Co_(0.7)Ni_(0.3)/DMC exhibits excellent performance with mass activity and specific activity of 1.32 A mgPt-1and 1.98 mA cm^(-2)at 0.9 V,which are 7.33and 6.19 times that of commercial Pt/C,respectively.The Pt_(3)Co_(0.7)Ni_(0.3)/DMC also reveals much better cathodic performance in an H2-air single fuel cell than commercial Pt/C catalyst with a power density of0.802 W cm^(-2).This work provides critical sights into constructing efficient catalysts by ternary intermetallic strategy and synergetic effect between active components and support.
基金Supported by the National Natural Science Foundation of China under Grant No 11274110
文摘The crystal structures and magnetic properties of novel Eu TrGa3-r （T=Pd, It, Rh） in termetallic compounds are investigated by using powder x-ray diffraction and magnetic measurements. EuTrGa3-r crystallizes in orthorhombic structure with space group of Cmcm and Z = 4. There are four kinds of nonequivalent 4c crystal positions in EuTrGaa-r unit cell, which are occupied by 4Eu, 4GaⅠ, 4（GaⅡ, T） and 4GaⅢ, respectively. EuTrGa3-r ex- hibits the complex magnetic states in low-temperature regime, with the three-, two- and one-antiferromagnetic transitions occurring for T=Ir, T=Rh and T=Pd, respectively. It might be due to the Kondo effect： a localized antiferromagnetic interaction of the isolated impurity spins with the surrounding conduction electrons at low-temperature regime.
