Improving Cyclability of All‐Solid‐State Batteries via Stabilized Electrolyte–Electrode Interface with Additive in Poly(propylene carbonate) Based Solid Electrolyte

In this study, tetraethylene glycol dimethyl ether (TEGDME) is demonstrated as an effective additive in poly(propylene carbonate) (PPC) polymers for the enhancement of ionic conductivity and interfacial stability and a tissue membrane is used as a backbone to maintain the mechanical strength of the solid polymer electrolytes (SPEs). TEGDME in the PPC allows the uniform distribution of conductive LiF species throughout the cathode electrolyte interface (CEI) layer which plays a critically important role in the formation of a stable and efficient CEI. In addition, the high modulus of SPEs suppresses the formation of a protrusion‐type CEI on the cathode. The SPE with the optimized TEGDME content exhibits a high ionic conductivity of 0.89 mS cm(−1), an adequate potential stability of up to 4.89 V, and a high Li‐ion transference number of 0.81 at 60 °C. Moreover, the Li/SPE/Li cell demonstrates excellent cycling stability for 1650 h, and the Li/SPE/LFP full cell exhibits an initial reversible capacity of 103 mAh g(−1) and improved stability over 500 cycles at a rate of 1 C. The TEGDME additive improves the electrochemical properties of the SPEs and promotes the creation of a stable interface, which is crucial for ASSLIBs.