Cathode Interfacial Layer Formation via in Situ Electrochemically Charging in Aqueous Zinc-Ion Battery

The issue of material dissolution is common in aqueous batteries, leading to serious performance deterioration. However, it is difficult to be solved so far. In this study, a single component cathode solid electrolyte interface (SEI) layer (CaSO₄·2H₂O) is observed via in situ electrochemically charging process, as demonstrated in a Ca₂MnO₄ cathode for an aqueous zinc-ion battery. Density functional theory calculation confirms its electronic insulation and ionic conductor properties, indicating that it is an appropriate SEI film. The material dissolution seems to be effectively suppressed by the presence of the SEI layer on the cathode side. Meanwhile, this in situ formed interface layer is advantageous for lowering impedance, ameliorating interface, and reducing activation energy. As a result, significantly superior rate performance and cycle stability are exhibited. The observation of a protective SEI layer in an aqueous system may provide an insight into the development of high stability aqueous batteries.