An interconnected and scalable hollow Si-C nanospheres/graphite composite for high-performance lithium-ion batteries

Abstract

Silicon (Si) anode is the most promising alternative for next generation lithium-ion batteries (LIBs) owing to large theoretical capacity, low working voltage and abundant natural resources. However, tremendous volume change of Si during the (de)lithiation processes causes repetitive formation of solid electrolyte interphase (SEI) layers, loss of electrical contact and electrodes pulverization, limiting its commercial application. Herein, we fabricate an interconnected hollow Si-C nanospheres/graphite composite via a facile and scalable approach. Notably, hollow Si-C nanospheres and graphite are homogeneously combined by using the surfactants as surface modifiers of graphite and introducing carbon dioxide (CO2) into magnesiothermic reduction reaction, resulting in the enhanced compatibility between hollow Si-C nanospheres and graphite, and the well-established electrical conductive network. The resultant Si-C nanospheres/graphite composite anode with carbon content of 59 wt% delivers a large reversible specific capacity of 662 mAh g−1 and a high capacity retention of 65.7% at 0.5 A g−1 after 200 cycles. Such excellent rate performance and superior cycling performance are attributed to high electrical conductivity and buffering effect of graphite, superior compatibility between hollow Si-C spheres and graphite, uniform distribution of both Si-C nanospheres with a unique hollow architecture and graphite flakes inside the composites and well-established interconnected electrical conductive carbon networks, which can effectively alleviate Si volume expansion and maintain good electrical contact during cycling. This strategy provides insights into designing Si-based anodes for practical LIBs.