Full Energy Range Resonant Inelastic X-ray Scattering of O2 and CO2 : Direct Comparison with Oxygen Redox State in Batteries

The Journal of Physical Chemistry Letters
Zengqing ZhuoWanli Yang

Abstract

The evolving oxygen state plays key roles in the performance and stability of high-energy batteries involving oxygen redox reactions. Here, high-efficiency full energy range O-K mapping of resonant inelastic X-ray scattering (mRIXS) was collected from O2 (O0) and CO2 (O2- with strong covalency) molecules and compared directly with Li2O2 (O-) and the oxidized oxygen state in representative Na/Li-ion battery electrodes. Our results confirm again that the critical mRIXS feature around the 523.7 eV emission energy is from intrinsically oxidized oxygen, but not from the highly covalent oxygen state (CO2). The comparison of the mRIXS profile of the four different oxygen states, i.e., O2-, O-, On- (0 < n < 2), and O0, reveals that oxygen redox states in batteries have distinct widths and positions along the excitation energy compared with Li2O2 and O2. The nature of the oxidized oxygen state in oxide electrodes is thus beyond a simple molecular configuration of either peroxide or O2.

References

Apr 1, 1996·Physical Review Letters·P GlansE Rotenberg
Sep 28, 2010·Physical Review Letters·Franz HenniesJan-Erik Rubensson
Jan 23, 2016·Nature Materials·A GrimaudJ-M Tarascon
Feb 6, 2017·The Review of Scientific Instruments·Yi-De ChuangZahid Hussain
Apr 5, 2017·The Review of Scientific Instruments·Ruimin QiaoWanli Yang
Apr 22, 2017·Nature Chemistry·Alexis GrimaudYang Shao-Horn
Mar 7, 2018·Nature Communications·Jing XuWei Tong
Oct 26, 2018·The Journal of Physical Chemistry Letters·Zengqing ZhuoWanli Yang
Feb 8, 2020·Angewandte Chemie·Gi-Hyeok LeeYong-Mook Kang

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Citations

Aug 14, 2020·Dalton Transactions : an International Journal of Inorganic Chemistry·Jue WuWanli Yang
Jan 22, 2021·The Journal of Physical Chemistry Letters·Qingtian LiWanli Yang
Oct 27, 2020·Frontiers in Chemistry·Jinpeng WuWanli Yang
Dec 16, 2020·Journal of the American Chemical Society·Ryan SharpeM Saiful Islam

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