Supremely elastic gel polymer electrolyte enables a reliable electrode structure for silicon-based anodes

Abstract Silicon-based materials are promising anodes for next-generation lithium-ion batteries, owing to their high specific capacities. However, the huge volume expansion and shrinkage during cycling result in severe displacement of silicon particles and structural collapse of electrodes. Here we report the use of a supremely elastic gel polymer electrolyte to address this problem and realize long-term stable cycling of silicon monoxide anodes. The high elasticity of the gel polymer electrolyte is attributed to the use of a unique copolymer consisting of a soft ether domain and a hard cyclic ring domain. Consequently, the displacement of silicon monoxide particles and volume expansion of the electrode were effectively reduced, and the damage caused by electrode cracking is alleviated. A SiO|LiNi 0.5 Co 0.2 Mn 0.3 O 2 cell shows 70.0% capacity retention in 350 cycles with a commercial-level reversible capacity of 3.0 mAh cm −2 and an average Coulombic efficiency of 99.9%.