A Triply‐Periodic‐Minimal‐Surface Structured Interphase based on Fluorinated Polymers Strengthening High‐energy Lithium Metal Batteries

Abstract

AbstractThe challenge of constructing a mechanically robust yet lightweight artificial solid‐electrolyte interphase layer on lithium (Li) anodes highlights a trade‐off between high battery safety and high energy density. Inspired by the intricate microstructure of the white sea urchin, we first develop a polyvinyl fluoride‐hexafluoropropylene (PVDF‐HFP) interfacial layer with a triple periodic minimal surface structure (TPMS) that could offer maximal modulus with minimal weight. This design endows high mechanical strength to an ordered porous structure, effectively reduces local current density, polarization, and internal resistance, and stabilizes the anode interface. At a low N/P ratio of ~3, using LiFePO4 as the cathode, Li anodes protected by TPMS‐structured PVDF‐HFP achieve an extremely low capacity‐fading‐rate of approximately 0.002 % per cycle over 200 cycles at 1 C, with an average discharge capacity of 142 mAh g−1. Meanwhile, the TPMS porous structure saves 50 wt % of the interfacial layer mass, thereby enhancing the energy density of the battery. The TPMS structure is conducive to large‐scale additive manufacturing, which will provide a reference for the future development of lightweight, high‐energy‐density secondary batteries.