General Strategy for Fabricating Sandwich-like Graphene-Based Hybrid Films for Highly Reversible Lithium Storage

We report a general strategy for the fabrication of freestanding sandwich-like graphene-based hybrid films by electrostatic adsorption and following reduction reaction. We demonstrate that by rational control of pH value in precursors, graphene oxide (GO) sheets can form three-dimensional (3D) sandwich frameworks with nanoparticles decorated between the layers of graphene. In our proof-of-concept study, we prepared the graphene/Si/graphene (G@Si@G) sandwich-like films. When used as negative electrode materials for lithium-ion batteries, it exhibits superior lithium-ion storage performance (∼1800 mA h g^-1 after 40 cycles at 100 mA g^-1). Importantly, with this simple and general method, we also successfully synthesized graphene/Fe₂O₃/graphene and graphene/TiO₂/graphene hybrid films, showing improved electrochemical performance. The good electrochemical property results from the enhanced electron transport rate, and the 3D flexible matrix to buffer volume changes during cycling. In addition, the porous sandwich structure consisting of plate-like graphene with high surface area provides effective electrolyte infiltration and promotes diffusion rate of Li⁺, leading to an improved rate capability. (Graph Presented).