Tuning the Properties of Graphdiyne by Introducing Electron‐Withdrawing/Donating Groups

Abstract

Herein, properties of graphdiyne (GDY) such as energy gap, conductivity, morphology, and affinity to alkalis metals are efficiently adjusted through including electron withdrawing/donating groups. The experimental and theoretical results indicate that the push‐pull electron ability and size differences of groups play a key role on the property adjusting of as‐prepared GDY derivatives named MeGDY, HGDY, and CNGDY. Typically, cyano group with electron withdrawing ability and methyl group with electron donating characteristic have successfully reduced the band gaps and increased the conductivity of the GDY network within an obvious range. Meanwhile, the inclusion of cyano and methyl groups affects the aggregation of GDY, thus providing a higher number of micropores and specific surface area. Moreover, the fascinating properties of these groups endow the original GDY additional advantages in following aspects: the stronger electronegativity of cyano groups increase the affinity of GDY frameworks to lithium atoms; the larger atomic volume of methyl groups increases the interlayer distance and provide more storage space and diffusion tunnels. These results provide an inspiring idea to design and synthesize novel functionalized GDY based materials for high stability, high conductivity and controllable functionality.