Beyond Mechanical Protection: The Electron-Shielding Effect of SWCNT for the Stabilized SiO Interface.

ABSTRACT

The single-walled carbon nanotube (SWCNT) commonly serves as a conductive additive for SiO-based anode materials due to the excellent conductivity and mechanical properties. However, the potential action mechanisms for the SWCNT beyond conductivity and mechanical features have rarely been studied. Herein, an interfacial electron-shielding effect and preferential adsorption to the electrolyte components for the SWCNT are revealed through a series of advanced characterizations and density functional theory (DFT) simulations. It can be determined that SWCNT networks could restrict the transmission of the electron from SiO interface to electrolyte with the reduced decomposition, because of the typical axial conductivity of the SWCNT. Moreover, the SWCNT shows stronger adsorption energy for LiPF6 and ethylene carbonate (EC) molecules, rather than nonselectivity of traditional carbon additives, facilitating the generation of inorganic-rich and denser solid electrolyte interface (SEI) film. As a result, benefiting from the electron-shielding effect, preferential adsorption, and mechanical protection, the SWCNT endows the SiO@C anode with a higher average Coulombic efficiency (CE) value of 99.4% over 100 cycles and a long cycling stability.