Large-Scale Electric-Field Confined Silicon with Optimized Charge-Transfer Kinetics and Structural Stability for High-Rate Lithium-Ion Batteries.

The stereospecific design of the interface effects can optimize the electron/Li-ion migration kinetics for energy-storage materials. In this study, an electric field was introduced to silicon-based materials (C-SiOx@Si/rGO) through the rational construction of multi-heterostructures. This was achieved by manipulating the physicochemical properties at the atomic level of advanced Li-ion batteries (LIBs). The experimental and density functional theory calculations showed that the unbalanced charge distribution generated a large potential difference, which in turn induced a large-scale electric-field response with a boosted interfacial charge transfer in the composite. The as-prepared C-SiOx@Si/rGO anode showed advanced rate capability (i.e., 1579.0 and 906.5 mAh g-1 at 1000 and 8000 mA g-1, respectively) when the migration paths of the Li-ion/electrons hierarchically optimized the large electric field. Furthermore, the C-SiOx@Si/rGO composite with a high SiOx@Si mass ratio (73.5 wt %) demonstrated a significantly enhanced structural stability with a 40% volume expansion. Additionally, when coupled with the LiNi0.8Co0.1Mn0.1O2 (NCM) cathode, the NCM//C-SiOx@Si/rGO full cell delivers superior Li-ion storage properties with high reversible capacities of 157.6 and 101.4 mAh g-1 at 500 and 4000 mA g-1, respectively. Therefore, the electric-field introduction using optimized electrochemical reaction kinetics can assist in the construction of other high-performance LIB materials.