TY - JOUR AU - Jing Xu AU - Meiling Sun AU - Ruimin Qiao AU - Sara E Renfrew AU - Lu Ma AU - Tianpin Wu AU - Sooyeon Hwang AU - Dennis Nordlund AU - Dong Su AU - Khalil Amine AU - Jun Lu AU - Bryan D McCloskey AU - Wanli Yang AU - Wei Tong AB -

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.

BT - Nature Communications DA - 03/2018 DO - 10.1038/s41467-018-03403-9 IS - 1 LA - eng N2 -

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.

PY - 2018 ST - Nat Commun T2 - Nature Communications TI - Elucidating anionic oxygen activity in lithium-rich layered oxides VL - 9 ER -