Extracting the Redox Orbitals in Li Battery Materials with High-Resolution X-Ray Compton Scattering Spectroscopy

K. Suzuki, B. Barbiellini, Y. Orikasa, N. Go, H. Sakurai, S. Kaprzyk, M. Itou, K. Yamamoto, Y. Uchimoto, Yung Jui Wang, H. Hafiz, A. Bansil, and Y. Sakurai
Phys. Rev. Lett. 114, 087401 – Published 25 February 2015
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Abstract

We present an incisive spectroscopic technique for directly probing redox orbitals based on bulk electron momentum density measurements via high-resolution x-ray Compton scattering. Application of our method to spinel LixMn2O4, a lithium ion battery cathode material, is discussed. The orbital involved in the lithium insertion and extraction process is shown to mainly be the oxygen 2p orbital. Moreover, the manganese 3d states are shown to experience spatial delocalization involving 0.16±0.05 electrons per Mn site during the battery operation. Our analysis provides a clear understanding of the fundamental redox process involved in the working of a lithium ion battery.

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  • Received 27 May 2014

DOI:https://doi.org/10.1103/PhysRevLett.114.087401

© 2015 American Physical Society

Authors & Affiliations

K. Suzuki1,*, B. Barbiellini2, Y. Orikasa3, N. Go1, H. Sakurai1, S. Kaprzyk2,4, M. Itou5, K. Yamamoto3, Y. Uchimoto3, Yung Jui Wang2,6, H. Hafiz2, A. Bansil2, and Y. Sakurai5

  • 1Faculty of Science and Technology, Gunma University, Tenjin-cho, Kiryu, Gunma 376-8515, Japan
  • 2Physics Department, Northeastern University, Boston, Massachusetts 02115, USA
  • 3Graduate School of Human and Environmental Studies, Kyoto University, Yoshida-nihonmatsu-cho, Sakyo-ku, Kyoto 606-8501, Japan
  • 4Faculty of Physics and Applied Computer Science, AGH University of Science and Technology, aleja Mickiewicza 30, 30-059 Krakow, Poland
  • 5Japan Synchrotron Radiation Research Institute, SPring-8, 1-1-1 Kouto, Sayo, Sayo, Hyogo 679-5198, Japan
  • 6Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA

  • *kosuzuki@gunma-u.ac.jp

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Issue

Vol. 114, Iss. 8 — 27 February 2015

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