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A well-defined crystalline cyano-functionalized graphdiyne (CN-GDY) is synthesized at a liquid/liquid interface through alkyne–alkyne coupling reactions. The configurations and nanostructures of CN-GDY were well characterized by TEM, SEM, AFM, XPS, and Raman spectroscopy. HR-TEM and selected area electron diffraction (SAED) in combination with structure simulation firmly revealed a 9-fold stacking mode for CN-GDY.

Graphical abstract: Interfacial synthesis of crystalline two-dimensional cyano-graphdiyne

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