Solid Silicon Nanosheet Sandwiched by Self-Assembled Honeycomb Silicon Nanosheets Enabling Long Life at High Current Density for a Lithium-Ion Battery Anode.

A two-dimensional silicon nanosheet (2D Si NS) is promising as a lithium-ion battery anode. However, insufficient cycling life at high current density hampers its practical applications due to its easy fragileness. Rationally engineering the Si micro/nanostructure is promising to address this issue. Unfortunately, the precise construction of a dedicated micro/nanostructure into 2D Si NS meets serious challenges. Herein, a facile strategy is developed to synthesize a sandwich-like honeycomb Si NS/solid Si NS/honeycomb Si NS (h/s/h-Si NS) anode through self-assembled preparation of a sandwich-like honeycomb SiO NS/solid SiO NS/honeycomb SiO NS template, followed by magnesiothermic reduction. This unique structure effectively enhances the mechanical strength, enlarges the specific surface area, and reserves sufficient space to accommodate the anode volume change. A conductive carbon layer is further coated on the h/s/h-Si NS (h/s/h-Si@C NS) to construct a stable electrode/electrolyte interface. The optimal h/s/h-Si@C NS displays outstanding performance with high initial Coulombic efficiency (86%), high reversible capacity (1624 mAh g after 100 cycles at 1000 mA g), good rate capability (over 1000 mAh g at 4000 mA g), and long cycling life even at 4000 mA g (93% retained capacity after 1000 cycles). This work provides a new strategy for constructing high-performance Si electrodes for lithium-ion battery applications.