Modulating the Inner Helmholtz Plane towards Stable Solid Electrolyte Interphase by Anion‐π Interactions for High‐Performance Anode‐Free Lithium Metal Batteries

Anode-free lithium (Li) metal batteries (AFLBs) featured high energy density are viewed as the viable future energy storage technology. However, the irregular Li deposition and unstable solid electrolyte interphase (SEI) on anode current collectors reduce their cycling performance. Here, we propose a concept of anion-recognition electrodes enabled by anion-π interactions to regulate the inner Helmholtz plane (IHP) and electrolyte solvation chemistry for high-performance AFLBs. By engineering the electrodes with electron-deficient aromatic-π systems that possess high permanent quadrupole moment (Q