Tunnel-structured manganese dioxides (MnO ), also known as octahedral molecule sieves (OMS), are widely studied in geochemistry, deionization, energy storage and (electro)catalysis. These functionalities originate from their characteristic sub-nanoscale tunnel framework, which, with a high degree of structural polymorphism and rich surface chemistry, can reversibly absorb and transport various ions. An intensive understanding of their structure-property relationship is prerequisite for functionality optimization, which has been recently approached by implementation of advanced (in situ) characterizations providing significant atomistic sciences. This review will thus timely cover recent advancements related to OMS and their energy storage applications, with a focus on the atomistic insights pioneered by researchers including our group: the origins of structural polymorphism and heterogeneity, the evolution of faceted OMS crystals and its effect on electrocatalysis, the ion transport/storage properties and their implication for processing OMS. These studies represent a clear rational behind recent endeavors investigating the historically applied OMS materials, the summary of which is expected to deepen the scientific understandings and guide material engineering for functionality control.
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