Diagnosing the SEI Layer in a Potassium Ion Battery Using Distribution of Relaxation Time

Understanding the solid electrolyte interphase (SEI) formation process in novel battery systems is of primary importance. Alongside increasingly powerful in situ techniques, searching for readily accessible, noninvasive, and low-cost tools to probe battery chemistry is highly demanded. Here, we applied distribution of relaxation time analysis to interpret in situ electrochemical impedance spectroscopy results during cycling, which is able to distinguish various electrochemical processes based on their time constants. By building a direct link between the SEI layer and the cell performances, it allows us to track the formation and evolution process of the SEI layer, diagnose the failure of the cell, and unveil the reaction mechanisms. For instance, in a K-ion cell using a SnS₂/N-doped reduced graphene oxide composite electrode, we found that the worsened mass transport in the electrolyte phase caused by the weak SEI layer is the main reason for cell deterioration. In the electrolyte with potassium bis(fluorosulfonyl)imide, the porous structure of the composite electrode was reinforced by rapid formation of a robust SEI layer at the SnS₂/electrolyte interface, and thus, the cell delivers a high capacity and good cyclability. This method lowers the barrier of in situ EIS analysis and helps public researchers to explore high-performance electrode materials.