Abstract
Silicon microparticles (SiMPs) show considerable promise as an anode material in high-performance lithium-ion batteries (LIBs) because of their low-cost starting material and high capacity. The failure issues associated with the intrinsically low conductivity and significant volume expansion of Si have largely been resolved by designing silicon/carbon composites using carbon nanotubes (CNTs). The CNTs are important in terms of stress dissipation and the conductive network in Si/CNT composites. Here, we synthesized a SiMP/2D CNT sheet wrapping composite (SiMP/CNT wrapping) via a facile freeze-drying method with the use of highly dispersed single-walled CNTs. In this work, the well-dispersed CNTs are easily mixed with Si, resulting in effective CNT wrapping on the SiMP surface. During freeze-drying, the CNTs are self-assembled into a segregated 2D CNT sheet morphology via van der Waals interactions. The resulting CNT wrapping shows a unique wide range of conductive networks and mesh-like CNT sheets with void spaces. The SiMP/CNT wrapping 9 : 1 electrode exhibits good rate and cycle performance. The first charge/discharge capacity of SiMP/CNT wrapping 9 : 1 is 3160.7 mA h g-1/3469.1 mA h g-1 at 0.1 A g-1 with superior initial coulombic efficiency of 91.11%. After cycling, the SiMP/CNT wrapping electrode shows good structural integrity with preserved electrical conductivity. The superior electrochemical performance of the SiMP/CNT wrapping composite can be explained by an extensive conductive CNT network on the SiMPs and facile lithium-ion diffusion via mesh-like CNT wrapping.