Self‐Expanding Ion‐Transport Channels on Anodes for Fast‐Charging Lithium‐Ion Batteries

We propose self‐expanding lithium‐ion transport channels to construct a fast‐charging anode and realize high‐performance fast‐charging Li‐ion batteries. The self‐expanded Li‐ion transport channels can be enabled by a self‐reversible conversion of chemical bonds with different bond lengths in the anode driven by the interactions with Li ions during cycling, reduce the energy barrier of Li‐ion transport and allow a fast Li‐ion solid‐state diffusion, whereby the severe voltage polarization and Li metal plating are effectively eliminated. Our proof‐of‐concept demonstration of the self‐reversible conversion of chemical bonds on the surface of graphdiyne successfully verifies the self‐expanded Li‐ion transport channels, self‐accelerated Li in‐plane/out‐of‐plane migration, and superior fast‐charging capability with a high capacity (342 mA h g −1 ) and an ultra‐long lifespan (22 000 cycles) under extremely fast‐charging conditions (6 C rate, 1 C=744 mA g −1 ), even at low temperatures (−10 °C).