High-Performance MnO₂/Al Battery with In Situ Electrochemically Reformed Al_xMnO₂ Nanosphere Cathode

Aqueous Al–ion battery (AAIB) is regarded as a promising candidate for large-scale energy storage systems due to its high capacity, high safety, and low cost, with MnO₂ proved to be a high-performance cathode. However, the potential commercial application of this type of battery is plagued by the frequent structural collapse of MnO₂. Herein, an in situ, electrochemically reformed, urchin-like Al_xMnO₂ cathode is developed for water-in-salt electrolyte-based AAIBs. Benefiting from its unique α-MnO₂ coated Mn₂AlO₄ structure, a high Al ion storage capacity is achieved together with a high discharge voltage plateau of 1.9 V by reversible MnO₂ electrolysis. Consequently, the battery exhibits a high specific capacity of 285 mAh g^–1 and a high energy density of 370 Wh kg^–1 at a high current density of 500 mA g^–1. Improved stability with record capacity retention is also obtained at an ultrahigh current density of 5 A g^–1 after 500 cycles. Such a high-capacity and high-stability Al_xMnO₂ cathode would pave the way for in situ electrochemical transformation of cathode design and thus boost the practical application of AAIBs.