Novel cellulose reinforcement for polymer electrolyte membranes with outstanding mechanical properties

► UV-cured methacrylic-based composite gel-polymer electrolyte membranes for rechargeable lithium batteries. ► Excellent mechanical stability by reinforcement with classical cellulose handsheets. ► Fast and environmentally friendly preparation process, green and low cost cellulose reinforcement. ► Good electrochemical behaviour, stable cyclability and long-term performances in real battery configuration. Methacrylic-based thermo-set gel-polymer electrolytes obtained by an easy and reliable free radical photo-polymerisation process demonstrate good behaviour in terms of ionic conductivity, interfacial stability with the Li-metal electrode and cyclability in lithium cells. Though the obtained membranes are flexible, self standing and easy to handle, there is room for improving mechanical strength. In this respect, a novel approach is adopted in this work, in which a cellulose hand-sheet (paper), specifically designed for the specific application, is used as a composite reinforcing agent. To enhance its compatibility with the polymer matrix, cellulose is modified by UV-grafting of poly(ethylene glycol) methyl ether methacrylate on it. Excellent mechanical properties are obtained and good overall electrochemical performances are maintained; highlighting that such specific approach would make these hybrid organic, green, cellulose-based composite polymer electrolyte systems a strong contender in the field of thin and flexible Li-based power sources.