Quantification of aging mechanisms of carbon-coated and uncoated silicon thin film anodes in lithium metal and lithium ion cells

In this work, a comprehensive investigation of the effect of carbon-coating on the aging mechanism of silicon thin films in lithium metal and lithium ion cells is presented. In Li||Si cells with sufficient lithium excess, 92% of the total capacity loss of the silicon film was attributed to a loss of active material and 8% was attributed to an increased cell resistance. Carbon-coating reduces the loss of active material by improving the mechanical integrity of the silicon thin film, leading to a 67% reduction of capacity loss per cycle. In Si||LiFePO4 lithium ion cells, 86% of the total capacity loss was attributed to a loss of lithium inventory and 14% attributed to an increase in cell resistance. Furthermore, a loss of 69% of silicon active material was observed. Carbon-coating reduces the capacity loss per cycle by 28%. After aging of the lithium ion cells, the negative electrode of the carbon-coated silicon retained double the capacity compared to the uncoated silicon electrode. Hence, carbon-coating is an effective measure to improve mechanical stability of silicon thin film electrodes, but it must be coupled with additional strategies to reduce lithium consumption in order to increase the overall effectiveness of the coating in lithium ion cells.