Ionic conductivity enhancement in solid polymer electrolytes by electrochemical in situ formation of an interpenetrating network

Various overoxidized poly(1H-pyrrole) (PPy), poly(N-methylpyrrole) (PMePy) or poly(3,4-ethylenedioxythiophene) (PEDOT) membranes incorporated into an acrylate-based solid polymer electrolyte matrix (SPE) were directly electrosynthesized by a two-step in situ procedure. The aim was to extend and improve fundamental properties of pure SPE materials. The polymer matrix is based on the cross-linking of glycerol propoxylate (1PO/OH) triacrylate (GPTA) with poly(ethylene glycol) diacrylate (PEGDA) and lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) as a conducting salt. A self-standing and flexible polymer electrolyte film is formed during the UV-induced photopolymerization of the acrylate precursors, followed by an electrochemical polymerization of the conducting polymers to form a 3D-IPN. The electrical conductivity of the conducting polymer is destroyed by electrochemical overoxidation in order to convert the conducting polymer into an ion-exchange membrane by introduction of electron-rich groups onto polymer units. The resulting polymer films were characterized by scanning electron microscopy, cyclic voltammetry, electrochemical impedance spectroscopy, differential scanning calorimetry, thermal analysis and infrared spectroscopy. The results of this study show that the combination of a polyacrylate-matrix with ion selective properties of overoxidized CPs leads to new 3D materials with higher ionic conductivity than SPEs and separator or selective ion-exchange membrane properties with good stability by facile fabrication.