Reprecipitation: A Rapid Synthesis of Micro-Sized Silicon-Graphene Composites for Long-lasting Lithium-Ion Batteries

Silicon microparticles (SiMPs) have gained significant attention as a lithium-ion battery anode material due to their 10 times higher theoretical capacity compared to conventional graphite anodes as well as their much lower production cost than silicon nanoparticles (SiNPs). However, SiMPs have suffered from poorer cycle life relative to SiNPs because their larger size makes them more susceptible to volume changes during charging and discharging. Creating a wrapping structure in which SiMPs are enveloped by carbon layers has proven to be an effective strategy to significantly improve the cycling performance of SiMPs. However, the synthesis processes are complex and time-/energy-consuming and therefore not scalable. In this study, a wrapping structure is created by using a simple, rapid, and scalable "modified reprecipitation method". Graphene oxide (GO) and SiMP dispersion in tetrahydrofuran is injected into n-hexane, in which GO and SiMP by themselves cannot disperse. GO and SiMP therefore aggregate and precipitate immediately after injection to form a wrapping structure. The resulting SiMP/GO film is laser scribed to reduce GO to a laser-scribed graphene (LSG). Simultaneously, SiO_x and SiC protection layers form on the SiMPs through the laser process, which alleviates severe volume change. Owing to these desirable characteristics, the modified reprecipitation method successfully doubles the cycle life of SiMP/graphene composites compared to the simple physically mixing method (50.2% vs. 24.0% retention at the 100th cycle). The modified reprecipitation method opens a new synthetic strategy for SiMP/carbon composites.