Unraveling the Dissolution-Mediated Reaction Mechanism of α-MnO2 Cathodes for Aqueous Zn-Ion Batteries

Sung Joo Kim; Daren Wu; Nahian Sadique; Calvin D. Quilty; Lijun Wu; Amy C. Marschilok; Kenneth J. Takeuchi; Esther S. Takeuchi; Yimei Zhu

doi:10.1002/smll.202005406

Unraveling the Dissolution-Mediated Reaction Mechanism of α-MnO₂ Cathodes for Aqueous Zn-Ion Batteries

Sung Joo Kim
, Daren Wu
, Nahian Sadique
, Calvin D. Quilty
, Lijun Wu
, Amy C. Marschilok
, Kenneth J. Takeuchi
, Esther S. Takeuchi
, Yimei Zhu

Brookhaven National Laboratory Condensed Matter Physics and Materials Science Department
Brookhaven National Laboratory
Stony Brook University

Research output: Contribution to journal › Article › peer-review

122 Scopus citations

Abstract

Aqueous Zn/α-MnO₂ batteries have attracted immense interest owing to their high energy density, low cost, and safety, making them desirable for future large-scale energy application. Despite these merits, the comprehensive understanding of their reaction mechanism has been elusive due to the limitations of standard bulk characterization. Here, via transmission electron microscopy, the dissolution-mediated reaction mechanism of a Zn/α-MnO₂ system is discovered and explored in full scope to involve reversible formation of Zn₄SO₄(OH)₆·xH₂O and “birnessite-like” Zn-MnO_x phase upon cycling. Overall, α-MnO₂ acts primarily as a source for cell activation through dissolution and thus is not directly involved in the Zn redox chemistry. This microscopic study offers a unique knowledge on the unconventional reaction chemistry of Zn/α-MnO₂ batteries.

Original language	English
Article number	2005406
Journal	Small
Volume	16
Issue number	48
DOIs	https://doi.org/10.1002/smll.202005406
State	Published - Dec 3 2020

Keywords

aqueous zinc-ion batteries
manganese oxides
scanning transmission electron microscopy

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10.1002/smll.202005406

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title = "Unraveling the Dissolution-Mediated Reaction Mechanism of α-MnO2 Cathodes for Aqueous Zn-Ion Batteries",

abstract = "Aqueous Zn/α-MnO2 batteries have attracted immense interest owing to their high energy density, low cost, and safety, making them desirable for future large-scale energy application. Despite these merits, the comprehensive understanding of their reaction mechanism has been elusive due to the limitations of standard bulk characterization. Here, via transmission electron microscopy, the dissolution-mediated reaction mechanism of a Zn/α-MnO2 system is discovered and explored in full scope to involve reversible formation of Zn4SO4(OH)6·xH2O and “birnessite-like” Zn-MnOx phase upon cycling. Overall, α-MnO2 acts primarily as a source for cell activation through dissolution and thus is not directly involved in the Zn redox chemistry. This microscopic study offers a unique knowledge on the unconventional reaction chemistry of Zn/α-MnO2 batteries.",

keywords = "aqueous zinc-ion batteries, manganese oxides, scanning transmission electron microscopy",

author = "Kim, \{Sung Joo\} and Daren Wu and Nahian Sadique and Quilty, \{Calvin D.\} and Lijun Wu and Marschilok, \{Amy C.\} and Takeuchi, \{Kenneth J.\} and Takeuchi, \{Esther S.\} and Yimei Zhu",

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year = "2020",

month = dec,

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doi = "10.1002/smll.202005406",

language = "English",

volume = "16",

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T1 - Unraveling the Dissolution-Mediated Reaction Mechanism of α-MnO2 Cathodes for Aqueous Zn-Ion Batteries

AU - Kim, Sung Joo

AU - Wu, Daren

AU - Sadique, Nahian

AU - Quilty, Calvin D.

AU - Wu, Lijun

AU - Marschilok, Amy C.

AU - Takeuchi, Kenneth J.

AU - Takeuchi, Esther S.

AU - Zhu, Yimei

PY - 2020/12/3

Y1 - 2020/12/3

N2 - Aqueous Zn/α-MnO2 batteries have attracted immense interest owing to their high energy density, low cost, and safety, making them desirable for future large-scale energy application. Despite these merits, the comprehensive understanding of their reaction mechanism has been elusive due to the limitations of standard bulk characterization. Here, via transmission electron microscopy, the dissolution-mediated reaction mechanism of a Zn/α-MnO2 system is discovered and explored in full scope to involve reversible formation of Zn4SO4(OH)6·xH2O and “birnessite-like” Zn-MnOx phase upon cycling. Overall, α-MnO2 acts primarily as a source for cell activation through dissolution and thus is not directly involved in the Zn redox chemistry. This microscopic study offers a unique knowledge on the unconventional reaction chemistry of Zn/α-MnO2 batteries.

AB - Aqueous Zn/α-MnO2 batteries have attracted immense interest owing to their high energy density, low cost, and safety, making them desirable for future large-scale energy application. Despite these merits, the comprehensive understanding of their reaction mechanism has been elusive due to the limitations of standard bulk characterization. Here, via transmission electron microscopy, the dissolution-mediated reaction mechanism of a Zn/α-MnO2 system is discovered and explored in full scope to involve reversible formation of Zn4SO4(OH)6·xH2O and “birnessite-like” Zn-MnOx phase upon cycling. Overall, α-MnO2 acts primarily as a source for cell activation through dissolution and thus is not directly involved in the Zn redox chemistry. This microscopic study offers a unique knowledge on the unconventional reaction chemistry of Zn/α-MnO2 batteries.

KW - aqueous zinc-ion batteries

KW - manganese oxides

KW - scanning transmission electron microscopy

UR - https://www.scopus.com/pages/publications/85096774952

U2 - 10.1002/smll.202005406

DO - 10.1002/smll.202005406

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ER -

Unraveling the Dissolution-Mediated Reaction Mechanism of α-MnO₂ Cathodes for Aqueous Zn-Ion Batteries

Abstract

Keywords

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