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

Jatinkumar Rana | Zendy; Yong Shi | Zendy; Mateusz Zuba | Zendy; Kamila M. Wiaderek | Zendy; Jun Feng | Zendy; Hui Zhou | Zendy; Jia Ding | Zendy; Tianpin Wu | Zendy; Giannantonio Cibin | Zendy; Mahalingam Balasubramanian | Zendy; Fredrick Omenya | Zendy; Natasha A. Chernova | Zendy; Karena W. Chapman | Zendy; M. Stanley Whittingham | Zendy; Louis F. J. Piper | Zendy

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

Author(s) -

Jatinkumar Rana,

Yong Shi,

Mateusz Zuba,

Kamila M. Wiaderek,

Jun Feng,

Hui Zhou,

Jia Ding,

Tianpin Wu,

Giannantonio Cibin,

Mahalingam Balasubramanian,

Fredrick Omenya,

Natasha A. Chernova,

Karena W. Chapman,

M. Stanley Whittingham,

Louis F. J. Piper

Publication year - 2018

Publication title -

journal of materials chemistry a

Language(s) - English

Resource type - Journals

SCImago Journal Rank - 3.637

H-Index - 212

eISSN - 2050-7488

pISSN - 2050-7496

DOI - 10.1039/c8ta06469e

Subject(s) - redox , limiting , electron , materials science , chemistry , inorganic chemistry , physics , quantum mechanics , engineering , mechanical engineering

Recent advances in materials syntheses have enabled e-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.

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