Tuning the Unloading and Infiltrating Behaviors of Li-Ion by a Multiphases Gradient Interphase for High-Rate Lithium...

The random distribution of organic-phases (OPs) and inorganic-phases (IOPs) in native solid electrolyte interface (SEI) derived a sluggish Li-ion de-solvation and transmission, impairing the high-rate performance of lithium metal anodes (LMAs). Herein, a multiphases gradient distribution hybrid interface is constructed on metallic Li by surface chemical reconstruction. Theoretical simulations and experiments verify that the Li-ion unloading and infiltrating behaviors are tuned by functional complementary effects, enabling speedy kinetics. The upper OPs with polar functional group (─COO^-) convert near-surface solvation structure, pushing Li-ion to unload the solvation cluster. Simultaneously, the bottom IOPs with plenty of crystal boundary accelerates Li-ion infiltration. Moreover, flexible OPs cooperate with rigid IOPs to buffer volume fluctuation and suppress dendritic Li growth. Consequently, the lifespan of the composited electrode is significantly prolonged over 520 h at 5 mA cm^-2. The full cells also exhibit an exhilarated rate performance and capacity retention even under a low N/P ratio (≈2.5). This work offers a characteristic insight for the rational design of gradient hybrid interface on the practical LMAs.