Publication date: 15th December 2025
Aqueous Zn–MnO₂ batteries with mildly acidic electrolytes are emerging as a promising alternative to Li-ion systems for large-scale energy storage, offering low cost, high safety, and competitive energy density. These advantages stem from the high capacity and reversibility of Zn metal in aqueous electrolytes, combined with the abundance and environmental benefits of MnO₂, a material long used in primary alkaline batteries. Recent demonstrations of rechargeability in mildly acidic media have expanded the potential of Zn/MnO₂ chemistry for sustainable energy storage.
Despite this progress, the underlying mechanisms remain debated. Our operando (XAS, XRD) and ex situ (TEM, SEM, TXM) studies indicate that electrolytic MnO₂ dissolution–precipitation dominates over intercalation, although voltage profiles and capacities vary with active material and electrolyte composition, as well as cell architecture [1]. The precipitated Mn phases are highly defective and poorly crystalline, with properties strongly influenced by pH, additives, and electrode texture. These insights enable the rational design of cells that exploit Mn oxide precipitation and dissolution as the primary charge-storage mechanism.
Building on this understanding, we present a Zn–MnO₂ flow cell architecture where cycling induces dynamic porosity changes within the electrode, impacting mass transport and reaction distribution. Experimental results are complemented by a 2D COMSOL model based on a porous electrode framework, exploring the effects of diffusion coefficients, electrode thickness, porosity gradients, and Zn geometry on voltage profiles, efficiency, and rate capability. This modelling approach provides design guidelines that are challenging to obtain experimentally and demonstrates the value of macro-scale simulation for optimizing Zn–MnO₂ battery performance. Our findings highlight the potential of aqueous Zn-based systems as safe, cost-effective solutions for grid-scale storage and beyond.
Cheng Liu is very grateful for financial support from the China Scholarship Council (CSC no.: 202106370079). This study was also implemented within the framework of the doctoral program in Materials Science at the Universitat Auto`noma de Barcelona (UAB, Spain). This research was funded by the Spanish Agency for Research (AEI) co-funded with ERDF through the ‘‘Severo Ochoa’’ Programme for Centers of Excel- lence in R&D (CEX2023-001263-S) and the projects PID2021- 124681OB-I00 and TED2021-132707B-I00. This research was partially developed within the CSIC Interdisciplinary Thematic Platform PTI-TRANSENER+ as part of the CSIC programme for the Spanish Recovery, Transformation, and Resilience Plan funded by the Recovery and Resilience Facility of the European Union, established by Regulation (EU) 2020/2094.
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