Highly reversible oxygen redox in layered compounds enabled by surface polyanions

Qing Chen, Yi Pei, Houwen Chen, Yan Song, Liang Zhen, Cheng-Yan Xu (), Penghao Xiao () and Graeme Henkelman ()
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Qing Chen: Harbin Institute of Technology
Yi Pei: Harbin Institute of Technology
Houwen Chen: Chongqing University
Yan Song: Harbin Institute of Technology (Weihai)
Liang Zhen: Harbin Institute of Technology
Cheng-Yan Xu: Harbin Institute of Technology
Penghao Xiao: The University of Texas at Austin
Graeme Henkelman: The University of Texas at Austin

Nature Communications, 2020, vol. 11, issue 1, 1-12

Abstract: Abstract Oxygen-anion redox in lithium-rich layered oxides can boost the capacity of lithium-ion battery cathodes. However, the over-oxidation of oxygen at highly charged states aggravates irreversible structure changes and deteriorates cycle performance. Here, we investigate the mechanism of surface degradation caused by oxygen oxidation and the kinetics of surface reconstruction. Considering Li2MnO3, we show through density functional theory calculations that a high energy orbital (lO2p’) at under-coordinated surface oxygen prefers over-oxidation over bulk oxygen, and that surface oxygen release is then kinetically favored during charging. We use a simple strategy of turning under-coordinated surface oxygen into polyanionic (SO4)2−, and show that these groups stabilize the surface of Li2MnO3 by depressing gas release and side reactions with the electrolyte. Experimental validation on Li1.2Ni0.2Mn0.6O2 shows that sulfur deposition enhances stability of the cathode with 99.0% capacity remaining (194 mA h g−1) after 100 cycles at 1 C. Our work reveals a promising surface treatment to address the instability of highly charged layered cathode materials.

Date: 2020
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DOI: 10.1038/s41467-020-17126-3

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