Self‐Compartmented Electrolyte Design for Stable Cycling of Lithium Metal Batteries under Extreme Conditions
Year: 2025
Type: article
Abstract: Electrolyte is the key component dictating lithium battery performance, especially under extreme conditions such as fast cycling and low temperatures. However, conventional electrolyte design principles, which generally rely on a homogeneous mixture of solvents, salts, and functional additives, fail to simultaneously meet the requirements for both anodic/cathodic interfacial stability and bulk ion‐transport kinetics in lithium metal batteries. Herein, we present a self‐compartmented electrolyte design methodology. Lithium 4,5‐dicyano‐2‐(trifluoromethyl)imidazol‐1‐ide (LiTDI), featuring the ability to selectively self‐assemble on the cathode/electrolyte interface, compartmented the electrolyte into a heterogonous one. Close to the cathode side, LiTDI could induce an interfacial high‐concentration region, where the anion‐rich solvation structure facilitates the formation of a stable cathode–electrolyte interphase (CEI). In the bulk, the electrolyte maintains a low concentration with low viscosity, ensuring fast ion transport and superior rate performance. Li||NCM811 cells achieve over 500 stable cycles with 80.3% capacity retention and deliver 169.3 mAh g −1 at a 10C discharge rate. Under low‐temperature conditions (−20 °C), the cells maintained outstanding stability over 700 cycles at 0.5C charge/discharge, achieving capacity retention of 96.6% and an average Coulombic efficiency of 99.2%. This work provides a new electrolyte design paradigm, addressing the critical challenges of LMBs for high‐voltage and low‐temperature applications.
Language: English
Subfield: Electrical and Electronic Engineering
Field: Engineering
Domain: Physical Sciences
Open Access status: bronze
OpenAlex ID: W4409214609