Abstract
Different from graphene with the highly stable sp2 -hybridized carbon atoms, which shows poor controllability for constructing strong interactions between graphene and guest metal, graphdiyne has a great potential to be engineered because its high-reactive acetylene linkages can effectively chelate metal atoms. Herein, a hydrogen-substituted graphdiyne (HsGDY) supported metal catalyst system through in situ growth of Cu3 Pd nanoalloys on HsGDY surface is developed. Benefiting from the strong metal-chelating ability of acetylenic linkages, Cu3 Pd nanoalloys are intimately anchored on HsGDY surface that accordingly creates a strong interaction. The optimal HsGDY-supported Cu3 Pd catalyst (HsGDY/Cu3 Pd-750) exhibits outstanding electrocatalytic activity for the oxygen reduction reaction (ORR) with an admirable half-wave potential (0.870 V), an impressive kinetic current density at 0.75 V (57.7 mA cm-2 ) and long-term stability, far outperforming those of the state-of-the-art Pt/C catalyst (0.859 V and 15.8 mA cm-2 ). This excellent performance is further highlighted by the Zn-air battery using HsGDY/Cu3 Pd-750 as cathode. Density function theory calculations show that such electrocatalytic performance is attributed to the strong interaction between Cu3 Pd and CC bonds of HsGDY, which causes the asymmetric electron distribution on two carbon atoms of CC bond and the strong charge transfer to weaken the shoulder-to-shoulder π conjugation, eventually facilitating the ORR process.
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