Understanding of Lithium 4,5-Dicyanoimidazolate-Poly(ethylene oxide) System: Influence of the Architecture of the Solid Phase on the Conductivity

Solid polymer electrolytes (SPEs) with high lithium conductivity are very beneficial as a safe material for lithium battery applications. Herein we present new set of a SPEs based on lithium 2-trifluoromethyl-4,5-dicyanoimidazolate (LiTDI) with wide range of ether oxygen to lithium molar ratios. The phase composition was characterized in detail with thermal, diffraction, and spectroscopic techniques, and its influence on conductivity behavior was examined. Two detected crystalline phases of LiTDI poly(ethylene oxide) (PEO) were simulated with computational methods. The obtained results allowed insight into the structure of these electrolytes and helped us to understand on the molecular level factors influencing electrochemical properties and phase behavior. It was shown that ability to form a low-melting phase can be used to lower the temperature window of operation. That made it possible to keep such SPEs amorphous at 30 degrees C during 80 days. The thermal stability of the samples was checked to prove the safety of the electrolytes