Silicon (Si) is considered a promising anode active material to enhance energy density of lithium-ion batteries. Many studies have focused on new structures and the electrochemical performance, but only a few investigated the particulate properties in detail. Therefore, a comprehensive study on the impact of Si content (5, 10, 15 wt.%) and particle size (120, 160, 250 nm) of core–shell structured Si@Gr composites on particulate and electrode properties was conducted. It was shown that both parameters had significant impact on the specific surface area (SSA) of particles, which was later correlated to the initial capacities and coulombic efficiencies (ICEs). Furthermore, changes in pore size distribution and electrical conductivity were found. The built full cells showed high initial capacities (>150 mAh g−1), good rate capability (75% at 1 C, 50% at 2 C) and ICEs (>80%). The energy density was found to increase by 32% at 15 wt.% Si compared to graphite (Gr), indicating the future potential of Si. In addition, the impact of a carbon coating was investigated (Si@Gr/C), which led to a reduction in SSA, improved particle stability and higher capacity retention. Consequently, this study emphasizes the importance of also investigating the particulate properties of Si anodes.
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