Ordered Lithium-Ion Conductive Interphase with Gradient Desolvation Effects for Fast-Charging Lithium Metal Batteries

Efficient desolvation and fast lithium ion (Li+) transport are key factors for fast-charging Li metal batteries (LMBs). Here, we report a self-assembled interphase (SAI) with ordered Li+ transport pathways to enable high Li+ conductivity and fast Li+ desolvation for fast-charging LMBs. A self-assembled structure originating from the intermolecular π–π stacking endows SAI with ordered Li+ transport pathways. The regular molecular stacking and a gradient distribution of functional groups of SAI contribute to a spatially confined gradient desolvation of Li+. Thereby, a stable Li metal anode (LMA) with durable solid-electrolyte interphase, accelerated Li+ transfer, and homogeneous Li plating/stripping is achieved at high rates. A full-cell battery of SAI protected LMA|LiNi0.8Co0.1Mn0.1O2 delivers a high capacity of 147 mAh g–1 with an improved capacity retention for 500 cycles at 3 C (1 C = 210 mA g–1), and the full cell can deliver over 71% of its capacity in 12 min.