Tailorable electron distribution of the active sites is widely regarded as the key issue to boost the catalytic activity and provide mechanistic insights into the structure-property-performance relationship. Here, a selective metal atom in situ growth strategy to construct highly active interface of mixed metal atom with different Nby RhOx species on sp-/sp2 -cohybridized graphdiyne (Nby RhOx /GDY) is reported. With this innovative idea implemented, experimental results show that the asymmetric electron distribution and the variation of coordination environment of bimetallic species significantly improve the electrocatalytic activity of Nby RhOx /GDY. Optimal hydrogen evolution reaction (HER) activity is achieved at the Nb/Rh ratio of 0.23, exhibiting excellent HER activity with the small overpotentials of 14 and 10 mV at 10 mA cm-2 in alkaline and neutral electrolytes. The data show the strong potential for real-system application of such catalysts, which outperform commercial Pt/C (20 wt%). These results shown in this study represent a platform for designing novel catalytic materials by selectively introducing metal atoms on different supports, which can be used as a general method extended to other catalytic systems.
Keywords: 2D carbon allotrope; electrocatalysis; graphdiyne; hydrogen energy conversion; regulation of metal valence.
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