High-performance Si@C anode for lithium-ion batteries enabled by a novel structuring strategy

Abstract

Si anode has drawn growing attention because of its features of large specific capacity, low electrochemical potential, and high natural abundance. However, it suffers from severe electrochemical irreversibility due to its large volume change during cycling. In spite of the achievement of improved electrochemical performance after compositing with carbon materials, most of the reported Si/C composite anodes lack a simple preparation process. To obtain a promising Si-based anode material, both simple preparation process and improved performance are necessary. Herein, inspired by the structure of shock proof foam, a novel structure of Si-based composite (Si@FeNO@P), consisting of Si nanoparticles embedded within a highly graphitized Fe₃C/Fe₃O₄ hybrid nanoparticle-interspersed foam-like porous carbon matrix, has been constructed using a simple method, consisting of simple mixing, drying, and carbonization processes. Thus, the well-designed composite structure effectively mitigates issues resulting from volumetric change of the Si during cycle and hence improves its performance significantly. The research results confirm outstanding performance of the Si@FeNO@P anode in the aspects of cycle durability, specific capacity, and rate capability, with 1116.1 (250^th cycle), 858.1 (500^th cycle), and 503.1 (500^th cycle) mA h g⁻¹ at 100, 1000, and 5000 mA g⁻¹, respectively. By comparing the performance and structure of Si@FeNO@P with other control samples, it was substantiated that the outstanding performances of the Si@FeNO@P anode depend on the synergistic effects of the well-designed unique carbon matrix, conductive Fe₃C, and Fe₃O₄-in situ derived metallic Fe nanoparticles during cycling. The outstanding electrochemical performance and simple preparation route make the Si@FeNO@P anode promising for lithium-ion battery applications. This work also gives useful insights into the development of high-performance Si-based anodes with simple practical methods.