InPc-modified gel electrolyte based on in situ polymerization in practical high-loading lithium-sulfur batteries

Lithium-sulfur batteries (LSBs) are currently being investigated as a potential candidate for high-energy–density rechargeable batteries. However, the notorious shuttle effect and uncontrolled dendrite growth posed problems for the practical applications of LSBs. Here, a new solid polymer electrolyte (SPE) was developed by in-situ polymerization of 1,3-dioxolane (DOL) in the presence of a multifunctional indium phthalocyanine (PDOL@InPc). The InPc endows the SPE with improved ionic conductivity and merit inhibition of the shuttle effect, in addition to being an effective additive for inducing uniform Li deposition by reconstructing the electric field at the interface. The characteristics of ionic migration in PDOL@InPc were quantified, and agreement between experiment and simulation established a relationship between macroscopic characteristics and molecular-level processes. The interfacial side reaction was controlled by the PDOL@InPc electrolyte, which also improved the distribution of the Li+ flux for dense Li deposition. Li symmetrical batteries designed with PDOL@lnPc can withstand a current density of up to 0.5 mA cm−2 and cycle reliably for 1500 h. The PDOL@InPc electrolyte displayed a high ionic conductivity at room temperature of 3.7 mS cm−1 and a significant Li+ transference number of 0.63. The resulting Li-S battery (Li|PDOL@lnPc|Sulfur) delivered a significant 325.5 Wh kg−1 of energy density at 0.2 C (1 C = 1000 mA g−1) at the level of the multilayer-pouch cell under an extremely low electrolyte of 3.5 g g−1 Sulfur and high loading of 8.0 mg cm−2. This work provides a feasible strategy for the widespread implementation of LSBs with increased safety and a longer lifetime.