An artificial interfacial layer with biomimetic ionic channels towards highly stable Li metal anodes

Lithium (Li) metal with low electrochemical potential and high theoretical capacity is a promising anode material for next-generation batteries. However, the low reversibility and safety problems caused by the notorious dendrite growth significantly impede the development of high-energy-density lithium metal batteries (LMBs). Here, to enable a dendrite-free and highly reversible Li metal anode (LMA), we develop a cytomembrane-inspired artificial layer (CAL) with biomimetic ionic channels using a scalable spread coating method. The negatively charged CAL with uniform intraparticle and interparticle ionic channels facilitates the Li-ion transport and redistributes the Li-ion flux, contributing to stable and homogeneous Li stripping and plating. Furthermore, a robust underneath transition layer with abundant lithiophilic inorganic components is in-situ formed through the transformation of CAL during cycling, which promotes Li-ion diffusion and suppresses the continuous side reactions with the electrolyte. Additionally, the resulting cytomembrane-inspired artificial Janus layer (CAJL) displays an ultrahigh Young's modulus (≥10.7 GPa) to inhibit the dendrite growth. Consequently, the CAJL-protected LMA (Li@CAJL) is stably cycled with a high areal capacity of 10 mAh cm⁻² at a high current density of 10 mA cm⁻². More importantly, the effective CAJL modification realizes the stable operation of a practical 429.2 Wh kg⁻¹ lithium-sulfur (Li-S) pouch cell using a low electrolyte/sulfur (E/S) ratio of 3 μL mg⁻¹. The facile yet effective protection strategy of LMAs can promote the practical application of LMBs.