Enabling stable high lithium storage of Si anode via synergistic effects of nanosized Fe3C and partially graphitized porous carbon

Abstract

Si is considered as a promising anode for high-energy lithium-ion batteries (LIBs) because of its ultrahigh theoretical specific capacity and desired working potential. However, the main problems of Si as an anode are still faced with low conductivity and inevitable structure damage caused by large volume change during cycle. Although design of Si/C composites effectively mitigates the above problems, their preparation usually involves complex methods. This work demonstrates a very simple ball milling and subsequent carbonization approach for the preparation of high-performance Si NPs@Fe3C@PC anode, which integrates partially hollow Fe3C nanoparticles (Fe3C) and partially graphitized porous carbon (PC) into Si nanoparticles (Si NPs)-based composite. It is found that Fe3C with catalysis is favorable not only to formation of a graphitized porous carbon during material preparation but also to formation of a stable solid electrolyte interfaces (SEI) on electrode surface during cycle. With Fe3C, the Si NPs@Fe3C@PC shows smaller Li+ adsorption energy, lower activation energy, higher electric conductivity, larger Li+ diffusion coefficient and a thinner SEI film than Si NPs and Si NPs@PC counterparts. The findings verify that the synergistic effects of the Fe3C and PC provide fast kinetics, high capacitive contribution, improved structure stability and a stable LiF-rich SEI film for Si NPs@Fe3C@PC during cycle. Therefore, Si NPs@Fe3C@PC shows excellent electrochemical performance, gaining 1786, 1211.4 and 411.5 mAh/g after 210, 650 and 840 cycles at 100, 1000 and 5000 mA g−1, respectively. Finally, this contribution proposes a simple and effective strategy for improving Si NPs performance and hence obtaining a high-performance of Si-based anode for LIBs.