Abstract
We utilize the domain-limiting effect of the porous graphdiyne (GDY) hexagonal ring to control synthesis of single-nickel-atom-alloyed platinum hexagonal nanocrystals (NiPtSAA/GDY) with uniform size approximate to 2.18 nm and atomically lattice distortion. The structure of NiPtSAA/GDY was confirmed by high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) and detail characterized and theoretical calculations. The hexagonal nanocrystals showed an excellent mass activity of 4.40 A mg Pt+Ni−1 and specific activity (136.78 mA cm−2) and exhibited the greatly enhancement in the durability and activity in MOR. In situ XAFS and XPS measurements indicated that low valence states of Pt in NiPtSAA/GDY were highly resistant to CO poisoning and demonstrated that the valence states were the origin of the activity. Our results provide a solid foundation for the design and synthesis with high dependence on valence and reactivity, while avoiding synergistic CO-poisoning, and also provide a general route for the design of new model catalysts.
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