Si/a-C Nanocomposites with a Multiple Buffer Structure via One-Step Magnetron Sputtering for Ultrahigh-Stability Lithium-Ion Battery Anodes.

Large volume expansion and serious pulverization of silicon are two major challenges for Si-based anode batteries. Herein, a high-mass-load (3.0 g cm-3) silicon-doped amorphous carbon (Si/a-C) nanocomposite with a hierarchical buffer structure is prepared by one-step magnetron sputtering. The uniform mixing of silicon and carbon is realized on the several-nanometer scale by cosputter deposition of silicon and carbon. The boundary of the primary particles, made up of nanocarbon and nanosilicon, and the boundary of the secondary particles aggregated by the primary particles can provide accommodation space for the volume expansion of silicon and effectively buffer the volume expansion of silicon. Meanwhile, the continuous and uniformly distributed amorphous carbon enhances the conductivity of the Si/a-C nanocomposites. Typically, the 20% Si/a-C cell shows a superior initial discharge capacity of 845.3 mAh g-1 and achieves excellent cycle performance of up to 1000 cycles (609.4 mAh g-1) at the current density of 1 A g-1. Furthermore, the 20% Si/a-C cell exhibits a high capacity of 602.8 mAh g-1 with the stable discharge/charge rate performance in several extreme conditions (-40-70 °C). In view of the validity and mass productivity of the magnetron sputtering, a potential route for the industrial preparation of the Si/a-C anode nanocomposites is therefore highlighted by this study.