期刊
ENERGY & ENVIRONMENTAL SCIENCE
卷 13, 期 11, 页码 4322-4333出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d0ee02168g
关键词
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资金
- Center for Mesoscale Transport Properties, an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Basic Energy Sciences [DE-SC0012673]
- Department of Energy, Office of Electricity [1955692]
- U.S. Department of Energy (DOE), Office of Basic Energy Sciences [DE-SC0012704]
- U.S. DOE Office of Science Facility, at Brookhaven National Laboratory [DE-SC0012704]
- William and Jane Knapp Chair in Energy and the Environment
Rechargeable aqueous Zn/alpha-MnO2 batteries are a possible alternative to lithium ion batteries for scalable stationary energy storage applications due to their low cost, safety and environmentally benign components. A critical need for advancement of this battery system is a full understanding of the electrochemical reaction mechanisms, which remain unclear. In this report, operando, spatiotemporal resolved synchrotron X-ray fluorescence mapping measurements on a custom aqueous Zn/alpha-MnO2 cell provided direct evidence of a Mn dissolution-deposition faradaic mechanism that governs the electrochemistry. Simultaneous visualization and quantification of the Mn distribution in the electrolyte revealed the formation of aqueous Mn species during discharge and depletion on charge. The findings are supported by ex situ transmission electron microscopy (TEM), X-ray diffraction, Mn K-edge X-ray absorption near edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) measurements. The elucidated mechanism is fundamentally different from the previously proposed Zn2+ insertion or conversion reactions. These findings provide a foundation for developing dissolution- deposition chemistries suitable for scalable stationary energy storage with aqueous electrolyte.
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