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Nat Commun. 2018 Mar 5;9(1):947. doi: 10.1038/s41467-018-03403-9.

Elucidating anionic oxygen activity in lithium-rich layered oxides.

Author information

1
Energy Storage and Distributed Resources Division, Lawrence Berkeley National Laboratory, Berkeley, CA, 94720, USA.
2
Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, CA, 94720, USA.
3
Department of Chemical and Biomolecular Engineering, University of California, Berkeley, CA, 94720, USA.
4
X-ray Sciences Division, Argonne National Laboratory, Argonne, IL, 60439, USA.
5
Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, NY, 11973, USA.
6
Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, CA, 94025, USA.
7
Chemical Sciences and Engineering Division, Argonne National Laboratory, Argonne, IL, 60439, USA.
8
Energy Storage and Distributed Resources Division, Lawrence Berkeley National Laboratory, Berkeley, CA, 94720, USA. bmcclosk@berkeley.edu.
9
Department of Chemical and Biomolecular Engineering, University of California, Berkeley, CA, 94720, USA. bmcclosk@berkeley.edu.
10
Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, CA, 94720, USA. wlyang@lbl.gov.
11
Energy Storage and Distributed Resources Division, Lawrence Berkeley National Laboratory, Berkeley, CA, 94720, USA. weitong@lbl.gov.

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.

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