Structure Regulation of Electric Double Layer via Hydrogen Bonding Effect to Realize High‐Stability Lithium‐Metal Batteries

The interfacial chemistry of solid electrolyte interphases (SEI) on lithium (Li) electrode is directly determined by the structural electric double layer (EDL) at interface. Herein, a strategy for regulating EDL via introduction intermolecular hydrogen bonds has been proposed (p-hydroxybenzoic acid (pHA) selected as proof-of-concept). According to molecular dynamics (MD) simulation and density functional theory (DFT) calculation results, existence realizes anion rearrangement in EDL, reduces lowest unoccupied orbital (LUMO) energy level anions number free solvent molecules, which promotes formation inorganic species-enriched SEI eventually achieves dendrite-free Li deposition. Based this strategy, Li||Cu cells can stably run over 185 cycles with an accumulated active loss only 2.27 mAh cm−2, long-term cycle stability Li||Li increased 1200 h. In addition, full cell pairing commercial LiFePO4 (LFP) cathodes exhibits stable cycling performance 1C, capacity retention close 90% after 200 cycles.