A layered multifunctional framework based on polyacrylonitrile and MOF derivatives for stable lithium metal anode

Composite Li metal anodes based on three-dimensional (3D) porous frameworks have been considered as an effective material for achieving stable Li metal batteries with high energy density. However, uneven Li deposition behavior still occurs at the top of 3D frameworks owing to the local accumulation of Li ions. To promote uniform Li deposition without top dendrite growth, herein, a layered multifunctional framework based on oxidation-treated polyacrylonitrile (OPAN) and metal-organic framework (MOF) derivatives was proposed for rationally regulating the distribution of Li ions flux, nucleation sites, and electrical conductivity. Profiting from these merits, the OPAN/carbon nano fiber-MOF (CMOF) composite framework demonstrated a reversible Li plating/stripping behavior for 500 cycles with a stable Coulombic efficiency of around 99.0% at the current density of 2 mA/cm2. Besides, such a Li composite anode exhibited a superior cycle lifespan of over 1300 h under a low polarized voltage of 18 mV in symmetrical cells. When the Li composite anode was paired with LiFePO4 (LFP) cathode, the obtained full cell exhibited a stable cycling over 500 cycles. Moreover, the COMSOL Multiphysics simulation was conducted to reveal the effects on homogeneous Li ions distribution derived from the above-mentioned OPAN/CMOF framework and electrical insulation/conduction design. These electrochemical and simulated results shed light on the difficulties of designing stable and safe Li metal anode via optimizing the 3D frameworks.