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Demonstrating Oxygen Loss and Associated Structural Reorganization in the Lithium Battery Cathode Li[Ni0.2Li0.2Mn0.6]O2
Abstract
The cathode in rechargeable lithium-ion batteries operates by conventional intercalation; Li+ is extracted from LiCoO2 on charging accompanied by oxidation of Co3+ to Co4+; the process is reversed on discharge. In contrast, Li+ may be extracted from Mn4+-based solids, e.g., Li2MnO3, without oxidation of Mn4+. A mechanism involving simultaneous Li and O removal is often proposed. Here, we demonstrate directly, by in situ differential electrochemical mass spectrometry (DEMS), that O2 is evolved from such Mn4+ -containing compounds, Li[Ni(0.2)Li(0.2)Mn(0.6)]O2, on charging and using powder neutron diffraction show that O loss from the surface is accompanied by diffusion of transition metal ions from surface to bulk where they occupy vacancies created by Li removal. The composition of the compound moves toward MO(2). Understanding such unconventional Li extraction is important because Li-Mn-Ni-O compounds, irrespective of whether they contain Co, can, after O loss, store 200 mAhg(-1) of charge compared with 140 mAhg(-1) for LiCoO(2).
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Citations
Cited by
Thackeray, M. M., Wolverton, C., & Isaacs, E. D. (2012) · Energy & Environmental Science · doi:10.1039/c2ee21892e · Cited by 2,515
Self-citationAn Outlook on Lithium Ion Battery Technology
Manthiram, A. (2017) · ACS Central Science · doi:10.1021/acscentsci.7b00288 · Cited by 1,771
Reversible anionic redox chemistry in high-capacity layered-oxide electrodes
Sathiya, M., Rousse, G., Ramesha, K., Laisa, C. P., Vezin, H., Sougrati, M. T., Doublet, M.-L., Foix, D., Gonbeau, D., Walker, W., et al. (2013) · Nature Materials · doi:10.1038/nmat3699 · Cited by 1,539
Visualization of O-O peroxo-like dimers in high-capacity layered oxides for Li-ion batteries
McCalla, E., Abakumov, A. M., Saubanère, M., Foix, D., Berg, E. J., Rousse, G., Doublet, M.-L., Gonbeau, D., Novák, P., Van Tendeloo, G., et al. (2015) · Science · doi:10.1126/science.aac8260 · Cited by 854
Self-citationQiu, B., Zhang, M., Wu, L., Wang, J., Xia, Y., Qian, D., Liu, H., Hy, S., Chen, Y., An, K., et al. (2016) · Nature Communications · doi:10.1038/ncomms12108 · Cited by 734
Metadata
- Authors
- Armstrong, A. R., Holzapfel, M., Novák, P., Johnson, C. S., Kang, S.-H., Thackeray, M. M., & Bruce, P. G.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2006-06-13
- Volume
- 128
- Issue
- 26
- Pages
- 8694-8698
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W1988921362
- Cited by
- 1,588
- References
- 0
- FWCI
- 16.87
- Type
- journal article
- Language
- en
- Open access
- closed
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- Armstrong, A. R., Holzapfel, M., Novák, P., Johnson, C. S., Kang, S.-H., Thackeray, M. M., & Bruce, P. G. (2006). Demonstrating Oxygen Loss and Associated Structural Reorganization in the Lithium Battery Cathode Li[Ni0.2Li0.2Mn0.6]O2. Journal of the American Chemical Society. https://doi.org/10.1021/ja062027%2B
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