AA‐Stacked Hydrogen‐Substituted Graphdiyne for Enhanced Lithium Storage

Graphdiyne (GDY) has been considered a promising electrode material for application in electrochemical energy storage. However, studies on GDY featuring an ordered interlayer stacking are lacking, which is supposed to be another effective way to increase lithium binding sites and diffusion pathways. Herein, we synthesized a hydrogen‐substituted GDY (HsGDY) with a highly‐ordered AA‐stacking structure via a facile alcohol‐thermal method. Such unique architecture enables a rapid lithium transfer through the well‐organized pore channels and endows a stronger adsorption capability to lithium atom as compared to the arbitrarily‐stacked mode. The resultant HsGDY exhibits a reversible capacity of 1040 mA h g‐1 at 0.05 A g‐1 ranking among the most powerful GDY‐based electrode materials, and an excellent rate performance as well as a long‐term cycling stability. The successful preparation of gram‐level high‐quality HsGDY products in batches implies the potential for large‐scale lithium‐storage applications.