Improved cycling stability of silicon thin film electrodes through patterning for high energy density lithium batteries

Abstract The mechanical degradation of electrodes caused by lithiation and delithiation is one of the main factors responsible for the short cycle life of lithium-based batteries employing high capacity electrodes. In this report, we introduced a simple patterning approach to improve the cycling stability of silicon electrode, which is considered as the next generation negative electrode due to its high Coulombic capacity and low cost, but is limited by the mechanical degradation associated with large volume variations during cycling. The pattern design is based on the observation of a critical size for the crack gap in continuous films. An improvement in cycle life was noted when the pattern size was below the critical (7–10 μm) size, in which case the Si electrode patches adhered well to the Cu substrate after many cycles. By taking the plastic deformation in both Si thin film and substrate into consideration, the calculated crack spacing is consistent with experimental observations. Theoretical considerations gave a feasible explanation for the failure of Si pattern above the critical size. These results suggest a new approach to extend the cycle life of Si-based electrode materials using size to control and relax the stress due to lithiation and delithiation.