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Aqueous electrochemical energy storage devices have attracted significant attention owing to their high safety, low cost and environmental friendliness. However, their applications have been limited by a narrow potential window (∼1.23 V), beyond which the hydrogen and oxygen evolution reactions occur. Here we report the formation of layered Mn 5 O 8 pseudocapacitor electrode material with a well-ordered hydroxylated interphase. A symmetric full cell using such electrodes demonstrates a stable potential window of 3.0 V in an aqueous electrolyte, as well as high energy and power performance, nearly 100% coulombic efficiency and 85% energy efficiency after 25,000 charge–discharge cycles. The interplay between hydroxylated interphase on the surface and the unique bivalence structure of Mn 5 O 8 suppresses the gas evolution reactions, offers a two-electron charge transfer via Mn 2+ /Mn 4+ redox couple, and provides facile pathway for Na-ion transport via intra-/inter-layer defects of Mn 5 O 8 . Rechargeable aqueous electrochemical energy storage is a promising technology but suffers from a narrow potential window. Here the authors report a surface hydroxylated Mn 5 O 8 pseudocapacitor electrode with bivalence structure that expands the potential window to deliver high energy and power performance.

Aqueous electrochemical energy storage devices have attracted significant attention owing to their high safety, low cost and environmental friendliness. However, their applications have been limited by a narrow potential window (1/41.23 V), beyond which the hydrogen and oxygen evolution reactions occur. Here we report the formation of layered Mn 5 O 8 pseudocapacitor electrode material with a well-ordered hydroxylated interphase. A symmetric full cell using such electrodes demonstrates a stable potential window of 3.0 V in an aqueous electrolyte, as well as high energy and power performance, nearly 100% coulombic efficiency and 85% energy efficiency after 25,000 charge-discharge cycles. The interplay between hydroxylated interphase on the surface and the unique bivalence structure of Mn 5 O 8 suppresses the gas evolution reactions, offers a two-electron charge transfer via Mn 2+ /Mn 4+ redox couple, and provides facile pathway for Na-ion transport via intra-/inter-layer defects of Mn 5 O 8.