Improving Cycle Life and Capacity Retention in PVMPO‖Li Dual-Ion Lithium-Organic Batteries Using an EC-Free and FEC...

Electrolytes critically influence the electrochemical performance and cycle life of lithium ion batteries (LIBs). This holds especially for organic redox polymer-based batteries, such as those employing poly(3-vinyl-N-methylphenoxazine) (PVMPO), where solubility limits performance in conventional ethylene carbonate (EC)/ dimethyl carbonate (DMC)-based electrolytes. Reducing EC content has shown solubility suppression when using ethyl methyl carbonate (EMC) as a co-solvent, however, capacity fading persists due to PVMPO electrode degradation. To address this degradation, this study explores the use of EC-free electrolytes, with and without fluoroethylene carbonate (FEC). Electrochemical investigations, UltraViolet/Visible (UV/Vis) spectroscopy, post-cycling Scanning Electron Microscopy (SEM), Energy Dispersive X-ray Spectroscopy (EDS) mapping, and X-ray Photoelectron Spectroscopy (XPS) analyses are employed to evaluate solubility, interfacial properties, and electrode integrity. The EC-free electrolyte system with FEC retains 95 mAh g^‒1, while that without FEC retains 86 mAh g^‒1, outperforming the 76 mAh g^‒1 observed in EC-based systems after 500 cycles at 1C. FEC containing electrolyte systems display reduced interfacial resistance, fewer surface cracks, and minimal electrode degradation. These findings demonstrate that EC-free electrolytes, particularly with FEC, effectively suppress electrode degradation and enhance the cycle life of organic LIBs.