Magnetism in Lithium-Oxygen Discharge Product
- Authors
- Lu, Jun; Jung, Hun-Ji; Lau, Kah Chun; Zhang, Zhengcheng; Schlueter, John A.; Du, Peng; Assary, Rajeev S.; Greeley, Jeffrey; Ferguson, Glen A.; Wang, Hsien-Hau; Hassoun, Jusef; Iddir, Hakim; Zhou, Jigang; Zuin, Lucia; Hu, Yongfeng; Sun, Yang Kook; Scrosati, Bruno; Curtiss, Larry A.; Amine, Kahlil
- Issue Date
- Jul-2013
- Publisher
- WILEY-V C H VERLAG GMBH
- Keywords
- batteries; density functional calculations; lithium peroxide; magnetic properties; superoxide
- Citation
- CHEMSUSCHEM, v.6, no.7, pp.1196 - 1202
- Indexed
- SCIE
SCOPUS
- Journal Title
- CHEMSUSCHEM
- Volume
- 6
- Number
- 7
- Start Page
- 1196
- End Page
- 1202
- URI
- https://scholarworks.bwise.kr/hanyang/handle/2021.sw.hanyang/26687
- DOI
- 10.1002/cssc.201300223
- ISSN
- 1864-5631
- Abstract
- Nonaqueous lithium-oxygen batteries have a much superior theoretical gravimetric energy density compared to conventional lithium-ion batteries, and thus could render long-range electric vehicles a reality. A molecular-level understanding of the reversible formation of lithium peroxide in these batteries, the properties of major/minor discharge products, and the stability of the nonaqueous electrolytes is required to achieve successful lithium-oxygen batteries. We demonstrate that the major discharge product formed in the lithium-oxygen cell, lithium peroxide, exhibits a magnetic moment. These results are based on dc-magnetization measurements and a lithium-oxygen cell containing an ether-based electrolyte. The results are unexpected because bulk lithium peroxide has a significant band gap. Density functional calculations predict that superoxide-type surface oxygen groups with unpaired electrons exist on stoichiometric lithium peroxide crystalline surfaces and on nanoparticle surfaces; these computational results are consistent with the magnetic measurement of the discharged lithium peroxide product as well as EPR measurements on commercial lithium peroxide. The presence of superoxide-type surface oxygen groups with spin can play a role in the reversible formation and decomposition of lithium peroxide as well as the reversible formation and decomposition of electrolyte molecules.
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