Freely deformable and free-standing electrodes together with high capacity are crucial to realizing flexible Li-ion batteries. Herein, a lamellar graphene/nanocellulose/silicon (GN/NC/Si) film assembled by interpenetrated GN nanosheets is synthesized via a facile vacuum-assisted filtration approach accompanied by the covalent cross-linking effect of glutaraldehyde. The hybrid film consists of the highly conductive GN matrix as an effective current collector, hydroxylated silicon nanoparticles (Si NPs) embedded uniformly within GN interlayer and NC as adhesive to cross-link GN and Si NPs. When applied as anode, the GN/NC/Si film exhibits a high reversible capacity of 1251 mA h g-1 at 100 mA g-1 after 100 cycles and superior rate capability. More importantly, in the stress-strain test, this film represents robust mechanical strength, which not only provides good flexibility but also accommodates volume change of Si during cycling. By coupling with lithium cobalt oxide as the cathode, the full cell successfully powers a light-emitting diode, even bended and folded, indicating the deformation-tolerant GN/NC/Si film electrode for flexible Li-ion batteries. Therefore, the design of layered nanocomposites will offer the possibility closer to the application of flexible batteries.
Keywords: Si-based anode; flexible Li-ion batteries; free-standing electrode; graphene nanosheets; nanocellulose.