Understanding the deformation of energy storage electrodes at a local scale and its correlation to electrochemical performance is crucial for designing effective electrode architectures. In this work, the effect of electrolyte cation and electrode morphology on birnessite (δ-MnO) deformation during charge storage in aqueous electrolytes was investigated using a mechanical cyclic voltammetry approach via atomic force microscopy (AFM) and molecular dynamics (MD) simulation. In both KSO and LiSO electrolytes, the δ-MnO host electrode underwent expansion during cation intercalation, but with different potential dependencies. When intercalating Li, the δ-MnO electrode presents a nonlinear correlation between electrode deformation and electrode height, which is morphologically dependent. These results suggest that the stronger cation-birnessite interaction is the reason for higher local stress heterogeneity when cycling in LiSO electrolyte, which might be the origin of the pronounced electrode degradation in this electrolyte.
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