SiO_x microparticles embedded into 3D wrinkled N, S co-doped multilayer graphene sheets as a high-performance anode for long-life full lithium-ion batteries

Silicon oxide (SiO_x) emerges as one of the most promising anodes for lithium-ion batteries (LIBs). However, the severe capacity fading arising from the structural degradation and low electronic conductivity still hinders its practical application. Herein, a novel SiO_x anode material is constructed by embedding the SiO_x microparticles into the 3D wrinkled multilayer graphene sheets with the heteroatoms of N, S co-doping. The proposed stable 3D conductive architecture can effectively facilitate the electronic and ionic transportation as well as buffer the volume changes of SiO_x to maintain the structural integrity during cycling. Moreover, the first principles calculations confirm the synergistic effect of N, S co-doping, which introduces more heteroatomic defects, lowers the band gap and leads to more negative Li adsorption energies to further promote the electron transfer and improve the Li storage capability. Consequently, the fabricated anode material exhibits a high reversible capacity of 1150 mA h g⁻¹ after 500 cycles. When paired with the commercial LiCoO₂ cathode, the fabricated full LIB delivers the excellent long-life cycling stability, showing a high reversible capacity of 151 mA h g⁻¹ and a superior energy density up to 501 W h kg⁻¹ after 330 cycles, among the best of the recently reported work.