Controlling the atomic arrangement of elemental atoms in intermetallic catalysts to govern their surface and subsurface properties is a crucial but challenging endeavor in electrocatalytic reactions.In hydrogen evolut...Controlling the atomic arrangement of elemental atoms in intermetallic catalysts to govern their surface and subsurface properties is a crucial but challenging endeavor in electrocatalytic reactions.In hydrogen evolution reaction(HER),adjusting the d-band center of the conventional noble-metallic Pt by introducing Fe enables the optimization of catalytic performance.However,a notable gap exists in research on the effective transition from disordered Fe/Pt alloys to highly ordered intermetallic compounds(IMCs)such as FePt_(3)in the alkaline HER,hampering their broader application.In this study,a series of catalysts FePt_(3-x)H(x=5,6,7,8 and 9)supported on carbon nanotubes(CNTs)were synthesized via a simple impregnation method,along with a range of heat treatment processes,including annealing in a reductive atmosphere,to regulate the order degree of the arrangement of Fe/Pt atoms within the FePt_(3)catalyst.By using advanced microscopy and spectroscopy techniques,we systematically explored the impact of the order degree of FePt_(3)in the HER.The as-prepared FePt_(3)-8H exhibited notable HER catalytic activity with low overpotentials(η=37 mV in 1.0 mol L^(-1)KOH)at j=10 mA cm^(-2).The surface of the L1_(2)FePt_(3)-8H catalyst was demonstrated to be Pt-rich.The Pt on the surface was not easily oxidized due to the unique Fe/Pt coordination,resulting in significant enhancement of HER performance.展开更多
基金supported by the National Natural Science Foundation of China(51872115 and 52101256)Beijing Synchrotron Radiation Facility(BSRF)4B9A。
文摘Controlling the atomic arrangement of elemental atoms in intermetallic catalysts to govern their surface and subsurface properties is a crucial but challenging endeavor in electrocatalytic reactions.In hydrogen evolution reaction(HER),adjusting the d-band center of the conventional noble-metallic Pt by introducing Fe enables the optimization of catalytic performance.However,a notable gap exists in research on the effective transition from disordered Fe/Pt alloys to highly ordered intermetallic compounds(IMCs)such as FePt_(3)in the alkaline HER,hampering their broader application.In this study,a series of catalysts FePt_(3-x)H(x=5,6,7,8 and 9)supported on carbon nanotubes(CNTs)were synthesized via a simple impregnation method,along with a range of heat treatment processes,including annealing in a reductive atmosphere,to regulate the order degree of the arrangement of Fe/Pt atoms within the FePt_(3)catalyst.By using advanced microscopy and spectroscopy techniques,we systematically explored the impact of the order degree of FePt_(3)in the HER.The as-prepared FePt_(3)-8H exhibited notable HER catalytic activity with low overpotentials(η=37 mV in 1.0 mol L^(-1)KOH)at j=10 mA cm^(-2).The surface of the L1_(2)FePt_(3)-8H catalyst was demonstrated to be Pt-rich.The Pt on the surface was not easily oxidized due to the unique Fe/Pt coordination,resulting in significant enhancement of HER performance.