Elucidating anionic oxygen activity in lithium-rich layered oxides

Jing Xu, Meiling Sun, Ruimin Qiao, Sara E. Renfrew, Lu Ma, Tianpin Wu, Sooyeon Hwang, Dennis Nordlund, Dong Su, Khalil Amine, Jun Lu, Bryan D. McCloskey (), Wanli Yang () and Wei Tong ()
Additional contact information
Jing Xu: Lawrence Berkeley National Laboratory
Meiling Sun: Lawrence Berkeley National Laboratory
Ruimin Qiao: Lawrence Berkeley National Laboratory
Sara E. Renfrew: University of California
Lu Ma: X-ray Sciences Division, Argonne National Laboratory
Tianpin Wu: X-ray Sciences Division, Argonne National Laboratory
Sooyeon Hwang: Brookhaven National Laboratory
Dennis Nordlund: SLAC National Accelerator Laboratory
Dong Su: Brookhaven National Laboratory
Khalil Amine: Argonne National Laboratory
Jun Lu: Argonne National Laboratory
Bryan D. McCloskey: Lawrence Berkeley National Laboratory
Wanli Yang: Lawrence Berkeley National Laboratory
Wei Tong: Lawrence Berkeley National Laboratory

Nature Communications, 2018, vol. 9, issue 1, 1-10

Abstract: Abstract Recent research has explored combining conventional transition-metal redox with anionic lattice oxygen redox as a new and exciting direction to search for high-capacity lithium-ion cathodes. Here, we probe the poorly understood electrochemical activity of anionic oxygen from a material perspective by elucidating the effect of the transition metal on oxygen redox activity. We study two lithium-rich layered oxides, specifically lithium nickel metal oxides where metal is either manganese or ruthenium, which possess a similar structure and discharge characteristics, but exhibit distinctly different charge profiles. By combining X-ray spectroscopy with operando differential electrochemical mass spectrometry, we reveal completely different oxygen redox activity in each material, likely resulting from the different interaction between the lattice oxygen and transition metals. This work provides additional insights into the complex mechanism of oxygen redox and development of advanced high-capacity lithium-ion cathodes.

Date: 2018
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DOI: 10.1038/s41467-018-03403-9

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