Origin of additional capacities in metal oxide lithium-ion battery electrodes

Hu, Yan-Yan and Liu, Zigeng and Nam, Kyung-Wan and Borkiewicz, Olaf J. and Cheng, Jun and Hua, Xiao and Dunstan, Matthew T. and Yu, Xiqian and Wiaderek, Kamila M. and Du, Lin-Shu and Chapman, Karena W. and Chupas, Peter J. and Yang, Xiao-Qing and Grey, Clare P. (2013) Origin of additional capacities in metal oxide lithium-ion battery electrodes. Nature Materials, 12. pp. 1130-1136. ISSN 1476-1122

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Metal fluorides/oxides (MFx/MxOy) are promising electrodes for lithium-ion batteries that operate through conversion reactions. These reactions are associated with much higher energy densities than intercalation reactions. The fluorides/oxides also exhibit additional reversible capacity beyond their theoretical capacity through mechanisms that are still poorly understood, in part owing to the difficulty in characterizing structure at the nanoscale, particularly at buried interfaces. This study employs high-resolution multinuclear/multidimensional solid-state NMR techniques, with in situ synchrotron-based techniques, to study the prototype conversion material RuO2. The experiments, together with theoretical calculations, show that a major contribution to the extra capacity in this system is due to the generation of LiOH and its subsequent reversible reaction with Li to form Li2O and LiH. The research demonstrates a protocol for studying the structure and spatial proximities of nanostructures formed in this system, including the amorphous solid electrolyte interphase that grows on battery electrodes.

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Journal Article
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Nature Materials
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07 Jun 2022 13:25
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22 Nov 2022 11:31