Multi‐scale Polyvinylidene Fluoride/Magnesium‐Aluminum Layered Double Hydroxide Gel Electrolytes for Lithium Batteries

An multi‐scale of porous polyvinylidene fluoride‐hexafluoropropylene copolymer (PVDF‐HFP)/magnesium‐aluminum layered double hydroxides (MgAl‐LDHs) composite gel polymer electrolyte is prepared by phase separation method. It is discovered that the ionic conductivity of the electrolyte reaches a maximum value of 1.36×10‐3 S/cm, the lithium ions mobility is 0.66, and the chemical performance is steady within the 4.85 V window along with the concentration of MgAl‐LDHs up to 0.4 wt% at room temperature.The DFT calculations show that the adsorption energy of Li+ with MgAl‐LDH is ‐3.59 eV and the diffusion potential barrier is 0.37 eV, which is favorable for the dissociation and transport of Li+. Moreover, the anode’s initial discharge capacity at 0.1C achieves 144 mAh/g, keeping 84.7% of the theoretical capacity of 170 mAh/g, and the capacity retention and the columbic efficiency maintain 92.4% and 95.7% after 100 cycles at 0.2C, respectively, through assembling into a Li/PVP‐MgAl/LiFePO4 battery.This article is protected by copyright. All rights reserved.