Free-Standing Stable Silicon-Based Anode with Exceptional Flexibility Realized by a Multifunctional Structure Design in Multiple Dimensions

Cyclized polyacrylonitrile (cPAN) with decently flexible, elastic, and conductive properties is a promising substrate or binder material for flexible devices. However, it is infeasible to accommodate the large volume expansion and contribute the exceptional rate capability of silicon anodes in lithium-ion batteries only counting on the limited elasticity and conductivity of cPAN. Herein, we report a robust silicon/carbon-cPAN-graphene (SC-CP-G) composite membrane with excellent flexibility based on a multifunctional structure design in multiple dimensions, which can be used as a free-standing integrated anode for lithium ion batteries. In this integrated electrode, silicon nanoparticles are encapsulated in porous carbon with in situ formed confined space, and the silicon/carbon particles are further embedded in cPAN nanofibers, which are inextricably interwoven with a reduced graphene oxide film, forming an interpenetrating network architecture. The unique hierarchical and functional structure design greatly improves the mechanical performance, cycling stability, and capacity accessibility of silicon electrodes, delivering a specific capacity of 1847 mA h g–1 at 2 A g–1 and a capacity retention of 87% after 150 cycles.