Graphene-Wrapped Composites of Si Nanoparticles, Carbon Nanofibers, and Pyrolytic Carbon as Anode Materials for Lithium-Ion Batteries

Silicon (Si) anode materials have received much attention on account of their unparalleled theoretical specific capacity, but they suffer from huge volumetric expansion and particle pulverization, which leads to rapid capacity fading and poor electrical conductivity as well. In this work, a quaternary silicon/carbon (Si/C) composite anode material is proposed which combines the advantages of both graphene and the three-dimensional carbon framework through rational structural design and simple synthesis methods. Nanosilicon/carbon nanofibers/pyrolytic carbon (SCC) composite particles are first synthesized by spray drying and pyrolysis, which are then wrapped by graphene nanosheets through a second spray drying and pyrolysis process to obtain the final product (SGCC). In this composite, a 3D carbon skeleton composed of carbon nanofibers and pyrolytic carbon serves as an electric conductive matrix that supports and stabilizes Si nanoparticles, while graphene nanosheets wrapped on the surface further improve the conductivity and structure stability of the composite particles, and isolate the particles from direct contact with electrolytes. Meanwhile, the rich pores of the composite particles can effectively provide space for the volume expansion of Si during lithiation. As a consequence, the as-prepared SGCC composite shows a high initial Coulomb efficiency of 84.7%, a high reversible capacity of 2150.8 mA h g–1, and a good capacity retention rate of 83.75% after 100 cycles.