We have investigated the local electronic and atomic structure of the LiMn0.5Ni0.5O2 electrode during the first charge and discharge process using in situ X-ray absorption spectroscopy (XAS) of the Mn and Ni K-edges. The Ni K-edge structure in the XANES spectrum shifts to higher energy during charge and shifts back reversibly during discharge in the higher voltage region of similar to4 V, whereas the Mn K-edge structure does not appear to exhibit a rigid edge shift. Further Li-ion intercalation during extended discharge in the 1-V plateau leads to the reduction of Mn4+ ions suggesting that the charge compensation in this region is achieved via the reduction of Mn4+ ions to Mn2+. Mn K-edge EXAFS results indicate that a small amount of Li is found in the Ni2+/Mn4+ layers. These Li ions in the transition metal layers are primarily present in the second coordination shell of Mn and not around Ni. Ni K-edge EXAFS fitting results suggest that the oxidation process upon Li deintercalation takes place in two steps: Ni2+ to Ni3+ first, and then Ni3+ to Ni4+.
机构:
Brookhaven Natl Lab, Dept Appl Sci, Div Mat & Chem Sci, Upton, NY 11973 USABrookhaven Natl Lab, Dept Appl Sci, Div Mat & Chem Sci, Upton, NY 11973 USA
Balasubramanian, M
Sun, X
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Brookhaven Natl Lab, Dept Appl Sci, Div Mat & Chem Sci, Upton, NY 11973 USABrookhaven Natl Lab, Dept Appl Sci, Div Mat & Chem Sci, Upton, NY 11973 USA
Sun, X
Yang, XQ
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Brookhaven Natl Lab, Dept Appl Sci, Div Mat & Chem Sci, Upton, NY 11973 USABrookhaven Natl Lab, Dept Appl Sci, Div Mat & Chem Sci, Upton, NY 11973 USA
Yang, XQ
McBreen, J
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Brookhaven Natl Lab, Dept Appl Sci, Div Mat & Chem Sci, Upton, NY 11973 USABrookhaven Natl Lab, Dept Appl Sci, Div Mat & Chem Sci, Upton, NY 11973 USA
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Brookhaven Natl Lab, Dept Appl Sci, Div Chem & Mat Sci, Upton, NY 11973 USABrookhaven Natl Lab, Dept Appl Sci, Div Chem & Mat Sci, Upton, NY 11973 USA
Balasubramanian, M
Sun, X
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Brookhaven Natl Lab, Dept Appl Sci, Div Chem & Mat Sci, Upton, NY 11973 USABrookhaven Natl Lab, Dept Appl Sci, Div Chem & Mat Sci, Upton, NY 11973 USA
Sun, X
Yang, XQ
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Brookhaven Natl Lab, Dept Appl Sci, Div Chem & Mat Sci, Upton, NY 11973 USABrookhaven Natl Lab, Dept Appl Sci, Div Chem & Mat Sci, Upton, NY 11973 USA
Yang, XQ
McBreen, J
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Brookhaven Natl Lab, Dept Appl Sci, Div Chem & Mat Sci, Upton, NY 11973 USABrookhaven Natl Lab, Dept Appl Sci, Div Chem & Mat Sci, Upton, NY 11973 USA
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Brookhaven Natl Lab, Div Mat & Chem Sci, Dept Energy Sci & Technol, Upton, NY 11973 USABrookhaven Natl Lab, Div Mat & Chem Sci, Dept Energy Sci & Technol, Upton, NY 11973 USA
Balasubramanian, M
McBreen, J
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机构:Brookhaven Natl Lab, Div Mat & Chem Sci, Dept Energy Sci & Technol, Upton, NY 11973 USA
McBreen, J
Davidson, IJ
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Davidson, IJ
Whitfield, PS
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Whitfield, PS
Kargina, I
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机构:Brookhaven Natl Lab, Div Mat & Chem Sci, Dept Energy Sci & Technol, Upton, NY 11973 USA
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Brookhaven Natl Lab, Dept Appl Sci, Div Mat & Chem Sci, Upton, NY 11973 USABrookhaven Natl Lab, Dept Appl Sci, Div Mat & Chem Sci, Upton, NY 11973 USA
Balasubramanian, M
Sun, X
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Brookhaven Natl Lab, Dept Appl Sci, Div Mat & Chem Sci, Upton, NY 11973 USABrookhaven Natl Lab, Dept Appl Sci, Div Mat & Chem Sci, Upton, NY 11973 USA
Sun, X
Yang, XQ
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Brookhaven Natl Lab, Dept Appl Sci, Div Mat & Chem Sci, Upton, NY 11973 USABrookhaven Natl Lab, Dept Appl Sci, Div Mat & Chem Sci, Upton, NY 11973 USA
Yang, XQ
McBreen, J
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Brookhaven Natl Lab, Dept Appl Sci, Div Mat & Chem Sci, Upton, NY 11973 USABrookhaven Natl Lab, Dept Appl Sci, Div Mat & Chem Sci, Upton, NY 11973 USA
机构:
Brookhaven Natl Lab, Dept Appl Sci, Div Chem & Mat Sci, Upton, NY 11973 USABrookhaven Natl Lab, Dept Appl Sci, Div Chem & Mat Sci, Upton, NY 11973 USA
Balasubramanian, M
Sun, X
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Brookhaven Natl Lab, Dept Appl Sci, Div Chem & Mat Sci, Upton, NY 11973 USABrookhaven Natl Lab, Dept Appl Sci, Div Chem & Mat Sci, Upton, NY 11973 USA
Sun, X
Yang, XQ
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Brookhaven Natl Lab, Dept Appl Sci, Div Chem & Mat Sci, Upton, NY 11973 USABrookhaven Natl Lab, Dept Appl Sci, Div Chem & Mat Sci, Upton, NY 11973 USA
Yang, XQ
McBreen, J
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Brookhaven Natl Lab, Dept Appl Sci, Div Chem & Mat Sci, Upton, NY 11973 USABrookhaven Natl Lab, Dept Appl Sci, Div Chem & Mat Sci, Upton, NY 11973 USA
机构:
Brookhaven Natl Lab, Div Mat & Chem Sci, Dept Energy Sci & Technol, Upton, NY 11973 USABrookhaven Natl Lab, Div Mat & Chem Sci, Dept Energy Sci & Technol, Upton, NY 11973 USA
Balasubramanian, M
McBreen, J
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机构:Brookhaven Natl Lab, Div Mat & Chem Sci, Dept Energy Sci & Technol, Upton, NY 11973 USA
McBreen, J
Davidson, IJ
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机构:Brookhaven Natl Lab, Div Mat & Chem Sci, Dept Energy Sci & Technol, Upton, NY 11973 USA
Davidson, IJ
Whitfield, PS
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机构:Brookhaven Natl Lab, Div Mat & Chem Sci, Dept Energy Sci & Technol, Upton, NY 11973 USA
Whitfield, PS
Kargina, I
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机构:Brookhaven Natl Lab, Div Mat & Chem Sci, Dept Energy Sci & Technol, Upton, NY 11973 USA