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Zinc‐based batteries offer good volumetric energy densities and are compatible with environmentally friendly aqueous electrolytes. Zinc‐ion batteries (ZIBs) rely on a lithium‐ion‐like Zn 2+ ‐shuttle, which enables higher roundtrip efficiencies and better cycle life than zinc‐air batteries. Manganese‐oxide cathodes in near‐neutral zinc sulfate electrolytes are the most prominent candidates for ZIBs. Zn 2+ ‐insertion, H + ‐insertion, and Mn 2+ ‐dissolution are proposed to contribute to the charge‐storage mechanism. During discharge and charge, two distinct phases are observed. Notably, the pH‐driven precipitation of zinc‐sulfate‐hydroxide is detected during the second discharge phase. However, a complete and consistent understanding of the two‐phase mechanism of these ZIBs is still missing. This paper presents a continuum full cell model supported by density functional theory (DFT) calculations to investigate the implications of these observations. The complex‐formation reactions of near‐neutral aqueous electrolytes are integrated into the battery model and, in combination with the DFT calculations, draw a consistent picture of the cycling mechanism. The interplay between electrolyte pH and reaction mechanisms is investigated at the manganese‐oxide cathodes and the dominant charge‐storage mechanism is identified. The model is validated with electrochemical cycling data, cyclic voltammograms, and in situ pH measurements. This allows to analyze the influence of cell design and electrolyte composition on cycling and optimize the battery performance.

The Cycling Mechanism of Manganese‐Oxide Cathodes in Zinc Batteries: A Theory‐Based Approach