Bivalence Mn<sub>5</sub>O<sub>8</sub> with hydroxylated interphase for high-voltage aqueous sodium-ion storage.

Shan, Xiaoqiang; Charles, Daniel S; Lei, Yinkai; Qiao, Ruimin; Wang, Guofeng; Yang, Wanli; Feygenson, Mikhail; Su, Dong et al. · Nat Commun · 2016

basic_science · Level V

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Abstract

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 Mn5O8 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 Mn5O8 suppresses the gas evolution reactions, offers a two-electron charge transfer via Mn2+/Mn4+ redox couple, and provides facile pathway for Na-ion transport via intra-/inter-layer defects of Mn5O8.