Tailoring Graphite Interlayers with Electron‐Acceptor Bridges Raises Ion Diffusion Kinetics for Ultrafast Charging Batteries

Abstract

Abstract Sluggish solid‐state diffusion kinetics of lithium ions is among the primary bottlenecks limiting the fast‐charging performance of graphite anodes. Pre‐intercalating molecules in graphite interlayers can tune the valence π‐electrons, but there are few systematic studies in designing such structures by electron coupling to optimize the charge transfer kinetics. Herein, deliberately guided by simulations, the present study identifies and develops a class of electron‐acceptor aluminum chloride species for intercalation into graphite (AC‐G), aiming to accelerate lithium ions charge transfer to the intercalated graphite through the formation of electron‐acceptor bridges within the graphite interlayers. Consequently, the AC‐G achieves a two‐order‐of‐magnitude enhancement in lithium ions diffusion coefficient (5.85 × 10 −7 cm 2 s −1 ) compared to that in pristine graphite. It delivers stable cycling over 2000 cycles with a high areal capacity retention of 3.84 mAh cm −2 at 1C and maintains 500‐cycle stability at 5C. Furthermore, an Ah‐level pouch cell assembled with AC‐G and cathode achieves an energy density of 285 Wh kg −1 at 3C. The present work provides a new design strategy for graphite by introducing interlayer electron‐bridging structures, offering valuable insights for next‐generation fast‐charging lithium‐ion batteries