Extracting the redox orbitals in Li battery materials with high-resolution x-ray compton scattering spectroscopy

Physical Review Letters
K SuzukiY Sakurai

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 Li_{x}Mn_{2}O_{4}, 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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Citations

Sep 22, 2015·Physical Chemistry Chemical Physics : PCCP·Xiaosong LiuWanli Yang
Oct 17, 2015·Journal of Physics. Condensed Matter : an Institute of Physics Journal·S KamaliY Sakurai
Sep 5, 2019·Microscopy and Microanalysis : the Official Journal of Microscopy Society of America, Microbeam Analysis Society, Microscopical Society of Canada·Zhenbao FengDangsheng Su
Jun 11, 2021·Nature·Hasnain HafizVenkatasubramanian Viswanathan
Oct 26, 2018·The Journal of Physical Chemistry Letters·Zengqing ZhuoWanli Yang

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