Si particle size blends to improve cycling performance as negative electrode for all-solid-state lithium-ion battery

Silicon negative electrodes dramatically increase the energy density of lithium-ion batteries (LIBs), but there are still many challenges in their practical application due to the limited cycle performance of conventional liquid electrolyte systems. In this study, we clarified that the use of an inorganic solid electrolyte improves the cycle performance of the LIB with the Si negative electrode and the size of Si particles influenced the properties of the all-solid-state LIB. The all-solid-state LIB using micro-sized silicon (mSi) particles as the negative electrode active material showed a large initial discharge capacity (2400 mAh g -1 ), but the discharge capacity decreased as charge/discharge cycles increased. In contrast, the all-solid-state LIB using nano-sized silicon (nSi) particles showed a low initial discharge capacity (1000 mAh g -1 ), but the discharge capacity increased for the initial 20 charge/discharge cycles. The cross-sectional images analyzed by scanning electron microscopy showed that for mSi particles, cracks and voids occurred due to volumetric changes during charging and discharging, interrupting the flow path of ions and electrons, whereas for nSi particles, the contact with the solid electrolyte and conductive material was improved. Moreover, the all-solid-state LIB using the negative electrode of nSi: mSi = 7: 3 (mass ratio) showed higher initial discharge capacity and longer cycle performance than that using mSi and nSi.