Abstract

Due to its excellent capacity, around 4000 mA h g−1, silicon has been recognized as one of the most promising lithium-ion battery anodes, especially for future large-scale applications including electrical vehicles and utility power grids. Nevertheless, Si suffers from a short cycle life as well as limitations for scalable electrode fabrication. Herein, we report a novel design for highly robust and scalable Si anodes: Si nanoparticles embedded in porous nitrogen-doped carbon spheres (NCSs). The porous nature of NCSs buffers the volume changes of Si nanoparticles and thus resolves critical issues of Si anode operations, such as pulverization, vulnerable contacts between Si and carbon conductors, and an unstable solid-electrolyte interphase. The unique electrode structure exhibits outstanding performance with a gravimetric capacity as high as 1579 mA h g−1 at a C/10 rate based on the mass of both Si and C, a cycle life of 300 cycles with 94% capacity retention, as well as a discharge rate capability of 6 min while retaining a capacity of 702 mA h g−1. Significantly, the coulombic efficiencies of this structure reach 99.99%. The assembled structure suggests a design principle for high capacity alloying electrodes that suffer from volume changes during battery operations.