A First-Cycle Coulombic Efficiency Higher than 100% Observed for a Li sub(2)MO sub(3) (M=Mo or Ru) Electrode

The lithiation/de-lithiation behavior of a ternary oxide (Li sub(2)MO sub(3), where M=Mo or Ru) is examined. In the first lithiation, the metal oxide (MO sub(2)) component in Li sub(2)MO sub(3) is lithiated by a conversion reaction to generate nano-sized metal (M) particles and two equivalents of Li...

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Published inAngewandte Chemie International Edition Vol. 53; no. 40; pp. 10654 - 10657
Main Authors Jang, Jihyun, Kim, Youngjin, Chae, Oh B, Yoon, Taeho, Kim, Sang-Mo, Kim, Hyun-seung, Park, Hosang, Ryu, Ji Heon, Oh, Seung M
Format Journal Article
LanguageEnglish
Published 01.09.2014
Subjects
Computational efficiency
Computing time
Consumption
Electrodes
Electrolytes
Equivalence
Metal oxides
Nanostructure
Oxides
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Summary:The lithiation/de-lithiation behavior of a ternary oxide (Li sub(2)MO sub(3), where M=Mo or Ru) is examined. In the first lithiation, the metal oxide (MO sub(2)) component in Li sub(2)MO sub(3) is lithiated by a conversion reaction to generate nano-sized metal (M) particles and two equivalents of Li sub(2)O. As a result, one idling Li sub(2)O equivalent is generated from Li sub(2)MO sub(3). In the de-lithiation period, three equivalents of Li sub(2)O react with M to generate MO sub(3). The first-cycle Coulombic efficiency is theoretically 150% since the initial Li sub(2)MO sub(3) takes four Li super(+) ions and four electrons per formula unit, whereas the M component is oxidized to MO sub(3) by releasing six Li super(+) ions and six electrons. In practice, the first-cycle Coulombic efficiency is less than 150% owing to an irreversible charge consumption for electrolyte decomposition. The as-generated MO sub(3) is lithiated/de-lithiated from the second cycle with excellent cycle performance and rate capability. More out than in: Nano-sized metallic components (Mo or Ru), generated from Li sub(2)MO sub(3) (M=Mo or Ru) by consuming four Li super(+) ions and four electrons, react with Li sub(2)O even just as a physical mixture. In the reaction with Li sub(2)O the theoretical first-cycle Coulombic efficiency is 150% because the metallic component is oxidized to MO sub(3) by the release of six Li super(+) ions and six electrons per formula unit.
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ISSN:1433-7851
1521-3773
DOI:10.1002/anie.201404510