Regulating the electronic and geometric structures of electrocatalysts is an effective strategy to boost their catalytic properties.Herein,a coral-like nanostructure is assembled with Mo-doped Pt clusters to form a hi...Regulating the electronic and geometric structures of electrocatalysts is an effective strategy to boost their catalytic properties.Herein,a coral-like nanostructure is assembled with Mo-doped Pt clusters to form a highly active catalyst toward the oxygen reduction reaction(ORR).The advantages of a Mo-doped porous skeleton,grain boundaries,and MoOx species on the Pt cluster surfaces synergistically boost the electrocatalytic performance.This unique architecture delivers 3.5-and 2.8-fold higher mass and specific activities,respectively,than commercial Pt/C.Density functional theory calculations reveal that the Mo-doped Pt clusters have an optimized Pt–O bond length of 2.110Å,which weakens the adsorption energy of the intermediate O*to yield great ORR activity.Moreover,the catalyst shows a decay in the half-wave potential of only 8 mV after 10,000 cycles of accelerated durability testing.The high stability arises from the increased dissociation energy of Pt atoms and the stable architecture of the coral-like structure of clusters.展开更多
基金the financial support from the National Natural Science Foundation of China(22379078).
文摘Regulating the electronic and geometric structures of electrocatalysts is an effective strategy to boost their catalytic properties.Herein,a coral-like nanostructure is assembled with Mo-doped Pt clusters to form a highly active catalyst toward the oxygen reduction reaction(ORR).The advantages of a Mo-doped porous skeleton,grain boundaries,and MoOx species on the Pt cluster surfaces synergistically boost the electrocatalytic performance.This unique architecture delivers 3.5-and 2.8-fold higher mass and specific activities,respectively,than commercial Pt/C.Density functional theory calculations reveal that the Mo-doped Pt clusters have an optimized Pt–O bond length of 2.110Å,which weakens the adsorption energy of the intermediate O*to yield great ORR activity.Moreover,the catalyst shows a decay in the half-wave potential of only 8 mV after 10,000 cycles of accelerated durability testing.The high stability arises from the increased dissociation energy of Pt atoms and the stable architecture of the coral-like structure of clusters.