Dynamic physical network constructed by tripartite H-bonds in artificial SEI to shape ultra-long life dendrite-free lithium-metal anodes

Constructing artificial solid electrolyte interfaces (SEIs) to shape dendrite-free lithium (Li)-metal anodes remains challenges. Herein, we designed dynamic physical network (DPN) with abundant lithiophilic/anionphilic groups through tripartite hydrogen bonds (H-bonds), serving as artificial SEIs in high-loading NCM811-Li metal batteries. The formation and dissociation of DPN endowed by tripartite H-bonds under tension release during Li plating/stripping cycling skillfully balance the contradiction between mechanical robustness and deformability. LiO bonds between lithiophilic sites and Li ions, and extra H-bonds between hydroxyl and electrolyte anions, endow DPN with functions of homogenizing Li-ion flux and accelerating its desolvation, synergistically achieving the uniform Li-ion deposition and weakening the charge shielding. The artificial SEI enhanced Li-anode (DPN@Li) withstood repeated Li ions plating/stripping processes for over 1000 h, which is 5 times longer than pure Li-anodes, and maintained low overpotential at a high current density of 10 mA cm⁻². DPN@Li-based NCM811 full cells deliver high specific capacities and outstanding cycle life over 3000 cycles. Further, DPN@Li possesses excellent electrochemical performance in the high active material loading (7.84 mg cm⁻²) and foldable pouch cells. This work provides a conceptual framework of DPN constructed by multiple weak intermolecular interaction for artificial SEI to shape anode performance, and achieves the idea with a facile manner and simple chemical substances to promote practical applications of LMBs.