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Resolving the degradation pathways in high-voltage oxides for high-energy-density lithium-ion batteries; Alternation in chemistry, composition and crystal structures [electronic resource].

Published
Washington, D.C. : United States. Office of the Assistant Secretary of Energy Efficiency and Renewable Energy, 2017.
Oak Ridge, Tenn. : Distributed by the Office of Scientific and Technical Information, U.S. Dept. of Energy
Physical Description
pages 76-84 : digital, PDF file
Additional Creators
Oak Ridge National Laboratory, United States. Office of the Assistant Secretary of Energy Efficiency and Renewable Energy, United States. Department of Energy. Office of Basic Energy Sciences, and United States. Department of Energy. Office of Scientific and Technical Information
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Summary
Our development of stable high-voltage (HV), high capacity (HC) cathode oxides is indispensable to enhancing the performance of current high-energy-density (HED) lithium-ion batteries. Overstoichiometric, layered Li- and Mn-rich (LMR) composite oxides are promising materials for HV-HC cathodes for HED batteries; however, their practical use is limited. By probing the crystal structure, magnetic structure, and microstructure of the Li1.2Mn0.55Ni0.15Co0.1O2 LMR oxide, we demonstrate that the oxide loses its pristine chemistry, structure, and composition during the first charge-discharge cycle and that it proceeds through a series of progressive events that introduce impediments on the ion mobility pathways. Here, we discovered i) the presence of tetrahedral Mn3+, interlayer cation intermixing, interface of layered-spinel, and structurally rearranged domains, cation segregation at an HV charged state, and ii) the loss of Li ions, inhomogeneous distribution of Li/Ni, and structurally transformed domains after the first discharge. Our results will advance our fundamental understanding of the obstacles related to ion migration pathways in HV-HC cathode systems and will enable us to formulate design rules for use of such materials in high-energy-density electrochemical-energy-storage devices.
Report Numbers
E 1.99:1362204
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Note
Published through SciTech Connect.
04/05/2017.
"VT1201000"
"CEVT110"
Nano Energy 36 C ISSN 2211-2855 AM
Debasish Mohanty; Baishakhi Mazumder; Arun Devaraj; Athena S. Sefat; Ashfia Huq; Lamuel A. David; E. Andrew Payzant; Jianlin Li; David L. Wood; Claus Daniel.
Funding Information
AC05-00OR22725
AC05-76RL01830
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