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Role of disorder in limiting the true multi-electron redox in ε-LiVOPO4
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Rana, Jatinkumar, Shi, Yong, Zuba, Mateusz J., Wiaderek, Kamila M., Feng, Jun, Zhou, Hui, Ding, Jia, Wu, Tianpin, Cibin, Giannantonio, Balasubramanian, Mahalingam, Omenya, Fredrick, Chernova, Natasha A., Chapman, Karena W., Whittingham, M. Stanley and Piper, Louis F. J. (2018) Role of disorder in limiting the true multi-electron redox in ε-LiVOPO4. Journal of Materials Chemistry A, 6 (42). pp. 20669-20677. doi:10.1039/C8TA06469E ISSN 2050-7488.
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Official URL: http://dx.doi.org/10.1039/C8TA06469E
Abstract
Recent advances in materials syntheses have enabled ε-LiVOPO4 to deliver capacities approaching, and in some cases exceeding the theoretical value of 305 mA h g−1 for 2Li intercalation, despite its poor electronic and ionic conductivity. However, not all of the capacity corresponds to the true electrochemical intercalation/deintercalation reactions as evidenced upon systematic tracking of V valence through combined operando and rate-dependent ex situ X-ray absorption study presented herein. Structural disorder and defects introduced in the material by high-energy ball milling impede kinetics of the high-voltage V5+/V4+ redox more severely than the low-voltage V4+/V3+ redox, promoting significant side reaction contributions in the high-voltage region, irrespective of cycling conditions. The present work emphasizes the need for nanoengineering of active materials without compromising their bulk structural integrity in order to fully utilize high-energy density of multi-electron cathode materials.
Item Type: | Journal Article | ||||||||
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Divisions: | Faculty of Science, Engineering and Medicine > Engineering > WMG (Formerly the Warwick Manufacturing Group) | ||||||||
Journal or Publication Title: | Journal of Materials Chemistry A | ||||||||
Publisher: | Royal Society of Chemistry | ||||||||
ISSN: | 2050-7488 | ||||||||
Official Date: | 2018 | ||||||||
Dates: |
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Volume: | 6 | ||||||||
Number: | 42 | ||||||||
Page Range: | pp. 20669-20677 | ||||||||
DOI: | 10.1039/C8TA06469E | ||||||||
Status: | Peer Reviewed | ||||||||
Publication Status: | Published | ||||||||
Access rights to Published version: | Restricted or Subscription Access |
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