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Issue 42, 2018
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Role of disorder in limiting the true multi-electron redox in ε-LiVOPO4

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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.

Graphical abstract: Role of disorder in limiting the true multi-electron redox in ε-LiVOPO4

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Supplementary files

Article information


Submitted
05 Jul 2018
Accepted
07 Sep 2018
First published
17 Sep 2018

J. Mater. Chem. A, 2018,6, 20669-20677
Article type
Paper
Author version available

Role of disorder in limiting the true multi-electron redox in ε-LiVOPO4

J. Rana, Y. Shi, M. J. Zuba, K. M. Wiaderek, J. Feng, H. Zhou, J. Ding, T. Wu, G. Cibin, M. Balasubramanian, F. Omenya, N. A. Chernova, K. W. Chapman, M. S. Whittingham and L. F. J. Piper, J. Mater. Chem. A, 2018, 6, 20669
DOI: 10.1039/C8TA06469E

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