Chemical Interplay of Silicon and Graphite in a Composite Electrode in SEI Formation.

Abstract

We investigated the effect of the Si/graphite weight ratio in half-cells on the solid electrolyte interphase (SEI) layer's chemistry. The nominal concentrations of active materials were (wt % Si/wt % Gr) 15/73, 30/58, 60/28, and 80/0. The electrolyte in the cells consisted of either 1.2 M LiPF6 in ethylene carbonate/ethyl methyl carbonate (3:7 by wt) or 1.2 M LiPF6 in ethylene carbonate:ethyl methyl carbonate (3:7 by wt) + 10 wt % fluoroethylene carbonate. These coin cells were cycled five times at the C/10 rate. As expected, the addition of silicon to the electrode significantly increased the measured capacity. Examination of the aged composite material showed that the electrolyte influenced the concentration of chemical environments on the surface. Depth profiling revealed that these concentrations of surface environments changed with sputtering time. A statistics-of-mixtures model was used to deconvolute how silicon and graphite interacted during the formation of these species and how the interaction changed with depth.