Lithium (Li) metal has been considered as an important substitute for the graphite anode to further boost the energy density of Li‐ion batteries. However, Li dendrite growth during Li plating/stripping causes safety concern and poor lifespan of Li metal batteries (LMB). Herein, fluoroethylene carbonate (FEC) additives are used to form a LiF‐rich solid electrolyte interphase (SEI). The FEC‐induced SEI layer is compact and stable, and thus beneficial to obtain a uniform morphology of Li deposits. This uniform and dendrite‐free morphology renders a significantly improved Coulombic efficiency of 98% within 100 cycles in a Li | Cu half‐cell. When the FEC‐protected Li metal anode matches a high‐loading LiNi0.5Co0.2Mn0.3O2 (NMC) cathode (12 mg cm−2), a high initial capacity of 154 mAh g−1 (1.9 mAh cm−2) at 180.0 mA g−1 is obtained. This LMB with conversion‐type Li metal anode and intercalation‐type NMC cathode affords an emerging energy storage system to probe the energy chemistry of Li metal protection and demonstrates the material engineering of batteries with very high energy density.

Lithium (Li) metal is the most promising electrode for next-generation rechargeable batteries. However, the challenges induced by Li dendrites on a working Li metal anode hinder the practical applications of Li metal batteries. Herein, nitrogen (N) doped graphene was adopted as the Li plating matrix to regulate Li metal nucleation and suppress dendrite growth. The N-containing functional groups, such as pyridinic and pyrrolic nitrogen in the N-doped graphene, are lithiophilic, which guide the metallic Li nucleation causing the metal to distribute uniformly on the anode surface. As a result, the N-doped graphene modified Li metal anode exhibits a dendrite-free morphology during repeated Li plating and demonstrates a high Coulombic efficiency of 98 % for near 200 cycles.

Lithium (Li) metal is among the most promising anode materials for nextgeneration high-energy-density batteries. However, both dendrite growth and unstable solid electrolyte interphases have hindered its practical applications. Herein, we propose a coralloid carbon fiber-based composite lithium anode, which is an initially Li-containing structured anode. Such electrode design renders dendrite-free morphology during repeated stripping/plating cycles and extraordinary electrochemical performance in Li-LiFePO 4 and Li-sulfur cells.

The performance of lithium-ion battery is highly dependent on its interfacial chemistry, which is regulated by electrolytes. Conventional electrolyte typically contains polar solvents to dissociate Li salts. Here, we report a novel weakly-solvating electrolyte (WSE) that consists of a pure non-polar solvent, which leads to a peculiar solvation structure where ion pairs and aggregates prevail under a low salt concentration of 1.0 M. Importantly, WSE forms unique anion-derived interphases on graphite electrodes that exhibit fast-charging and long-term cycling characteristics. First-principles calculations unravel a general principle that the competitive coordination between anions and solvents to Li ion is the origin of different interfacial chemistries. By bridging the gap between solution thermodynamics and interfacial chemistry in batteries, this work opens a brand-new way towards precise electrolyte engineering for energy storage devices with desired properties.