Atomic Scale Account of the Surface Effect on Ionic Transport in Silver Hollandite

Xiaobing Hu, Jianping Huang, Lijun Wu, Merzuk Kaltak, Maria Victoria Fernandez-Serra, Qingping Meng, Lei Wang, Amy C. Marschilok, Esther S. Takeuchi, Kenneth J. Takeuchi, Mark S. Hybertsen, Yimei Zhu

Research output: Contribution to journalArticle

Abstract

Nanosized electrodes for Li-ion batteries typically display improved electrochemical properties, which are generally attributed to the reduced dimensionality for lithiation. However, the intriguing roles of surface defects and disorder associated with the nanosized materials are often overlooked. Here, combining atomically resolved structural analysis with density functional theory calculations, we reveal that the formation of intrinsic oxygen vacancies near surface in silver hollandite nanorods modifies the local atomic structure and valence state. These surface reconstructions resulted from oxygen vacancies can significantly affect the diffusion pathways in what are otherwise one-dimensional (1D) tunneled structures. On the basis of energy barrier calculations, we demonstrate that the oxygen vacancies boost ionic transport through the edge sharing MnO 6 polyhedra in the a-b plane. Thus, within a single rod different from the inherent 1D tunnel diffusion in the interior, the ionic transport at oxygen vacancy decorated surfaces likely adopts a three-dimensional diffusion pathway including both tunnel and planar diffusion.

Original languageEnglish (US)
Pages (from-to)6124-6133
Number of pages10
JournalChemistry of Materials
Volume30
Issue number17
DOIs
StatePublished - Sep 11 2018

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Oxygen vacancies
Silver
Tunnels
Surface reconstruction
Energy barriers
Surface defects
Nanorods
Electrochemical properties
Structural analysis
Density functional theory
Electrodes

ASJC Scopus subject areas

  • Chemistry(all)
  • Chemical Engineering(all)
  • Materials Chemistry

Cite this

Hu, X., Huang, J., Wu, L., Kaltak, M., Fernandez-Serra, M. V., Meng, Q., ... Zhu, Y. (2018). Atomic Scale Account of the Surface Effect on Ionic Transport in Silver Hollandite. Chemistry of Materials, 30(17), 6124-6133. https://doi.org/10.1021/acs.chemmater.8b02575
Hu, Xiaobing ; Huang, Jianping ; Wu, Lijun ; Kaltak, Merzuk ; Fernandez-Serra, Maria Victoria ; Meng, Qingping ; Wang, Lei ; Marschilok, Amy C. ; Takeuchi, Esther S. ; Takeuchi, Kenneth J. ; Hybertsen, Mark S. ; Zhu, Yimei. / Atomic Scale Account of the Surface Effect on Ionic Transport in Silver Hollandite. In: Chemistry of Materials. 2018 ; Vol. 30, No. 17. pp. 6124-6133.
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Hu, X, Huang, J, Wu, L, Kaltak, M, Fernandez-Serra, MV, Meng, Q, Wang, L, Marschilok, AC, Takeuchi, ES, Takeuchi, KJ, Hybertsen, MS & Zhu, Y 2018, 'Atomic Scale Account of the Surface Effect on Ionic Transport in Silver Hollandite' Chemistry of Materials, vol. 30, no. 17, pp. 6124-6133. https://doi.org/10.1021/acs.chemmater.8b02575

Atomic Scale Account of the Surface Effect on Ionic Transport in Silver Hollandite. / Hu, Xiaobing; Huang, Jianping; Wu, Lijun; Kaltak, Merzuk; Fernandez-Serra, Maria Victoria; Meng, Qingping; Wang, Lei; Marschilok, Amy C.; Takeuchi, Esther S.; Takeuchi, Kenneth J.; Hybertsen, Mark S.; Zhu, Yimei.

In: Chemistry of Materials, Vol. 30, No. 17, 11.09.2018, p. 6124-6133.

Research output: Contribution to journalArticle

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AU - Meng, Qingping

AU - Wang, Lei

AU - Marschilok, Amy C.

AU - Takeuchi, Esther S.

AU - Takeuchi, Kenneth J.

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AU - Zhu, Yimei

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