Predicting Capacity Fade in Silicon Anode-Based Li-Ion Batteries

Abstract

While silicon anodes hold promise for use in lithium-ion batteries owing to their very high theoretical storage capacity and relatively low discharge potential, they possess a major problem related to their large volume expansion that occurs with battery aging. The resulting stress and strain can lead to mechanical separation of the anode from the current collector and an unstable solid electrolyte interphase (SEI), resulting in capacity fade. Since capacity loss is in part dependent on the cell materials, two different electrodes, Lithium Nickel Oxide or LiNi0.8Co0.15Al0.05O2 (NCA) and LiNi1/3Mn1/3Co1/3O2 (NMC 111), were used in combination with silicon to study capacity fade effects using simulations in COMSOL version 5.5. The results of these studies provide insight into the effects of anode particle size and electrolyte volume fraction on the behavior of silicon anode-based batteries with different positive electrodes. It was observed that the performance of a porous matrix of solid active particles of silicon anode could be improved when the active particles were 150 nm or smaller. The range of optimized values of volume fraction of the electrolyte in the silicon anode were determined to be between 0.55 and 0.40. The silicon anode behaved differently in terms of cell time with NCA and NMC. However, NMC111 gave a high relative capacity in comparison to NCA and proved to be a better working electrode for the proposed silicon anode structure.