The preparation of mass producible, highly-cycling stable Si/C anode materials with nano-sized silicon crystals embedded in highly amorphous silicon matrix

Abstract

sThe commercial applications of silicon nanomaterials as anode in lithium-ion batteries must solve two important problems, namely low expansion and long-term cycle stability. The former is related to nano-silicon structure, while the latter depends on silicon/carbon composite structure and preparation process. In order to suppress volume expansion appeared during lithiation, this paper selects a kind of silicon nanoparticles (SiNPs) with a high degree of amorphization (81.9%), and designs a stable silicon/carbon composite material structure. Inside this structure, graphite nanoflakes (GNFs) with high specific surface are used as the skeleton, which can provide enough surface area for SiNPs to adhere and avoid the local accumulation of SiNPs. Outside this structure is uniformly coated with a layer of amorphous carbon. Raman and x-ray diffraction results show that after the high-temperature carbonization, the nano-silicon in the composite material still maintains a high degree of amorphization (67.1%) and the average crystallite size of Si has only increased from 3.7 to 9.5 nm. The initial Coulombic efficiency and reversible specific capacity of the composite material are 86.7% and 1374.8 mAh g−1, respectively. After mixing with commercial graphite, the initial Coulombic efficiency and reversible specific capacity are 93.7% and 426.4 mAh g−1, respectively. LiNi0.8Co0.1Mn0.1O2 (NCM811) is used as the cathode to produce a soft-pack battery. After 900 cycles at room temperature, the capacity remains 86.2%. The silicon/carbon anode material reported in this paper is of great potential for commercialization.