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Employing the Dynamics of the Electrochemical Interface in Aqueous Zinc‐Ion Battery Cathodes
Author(s) -
Becknell Nigel,
Lopes Pietro P.,
Hatsukade Toru,
Zhou Xiuquan,
Liu Yuzi,
Fisher Brandon,
Chung Duck Young,
Kanatzidis Mercouri G.,
Markovic Nenad M.,
Tepavcevic Sanja,
Stamenkovic Vojislav R.
Publication year - 2021
Publication title -
advanced functional materials
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 6.069
H-Index - 322
eISSN - 1616-3028
pISSN - 1616-301X
DOI - 10.1002/adfm.202102135
Subject(s) - dissolution , materials science , electrolyte , electrochemistry , chemical engineering , tetragonal crystal system , cathode , aqueous solution , battery (electricity) , phase (matter) , energy storage , ion , nanotechnology , electrode , chemistry , power (physics) , physics , organic chemistry , quantum mechanics , engineering
Intrinsically stable materials are desirable for constructing energy storage devices, which aim to demonstrate durability under the harsh electrochemical conditions that are detrimental to their lifespan. However, it is demonstrated here that the intrinsic instability of an electrochemical interface can be converted from an obstacle into an advantage. In aqueous zinc‐ion batteries, manganese oxide (MnO 2 ) exhibits considerable dissolution even in electrolyte containing Mn 2+ salt. Balancing with redeposition alleviates the harmful impact of dissolution on performance and alters the trajectory of the active phase. Inclusion of Mn 2+ salt in the electrolyte induces MnO 2 deposition on all conductive surfaces, requiring that distracting side reactions be eliminated to isolate the dynamics of the active phase. Under conditions favoring dissolution, capacity decreases dramatically and a highly crystalline tetragonal ZnMn 2 O 4 phase forms, while redeposition helps maintain capacity and promotes a disordered cubic Zn‐rich phase. Ultimately, this work aims to illuminate a path forward to unlock the potential of batteries made with materials that are fundamentally unstable in their operating environment.

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