Unraveling the Cationic and Anionic Redox Reactions in a Conventional Layered Oxide CathodeUnraveling the Cationic and Anionic Redox Reactions in a Conventional Layered Oxide Cathode

Date Published
10/2019
Publication Type
Journal Article
Authors
DOI
10.1021/acsenergylett.9b02147
Abstract

Increasing interest in high-energy lithium-ion batteries has triggered the demand to clarify the reaction mechanism in battery cathodes during high-potential operation. However, the reaction mechanism often involves both transition-metal and oxygen activities that remain elusive. Here we report a comprehensive study of both cationic and anionic redox mechanisms of LiNiO2 nearly full delithiation. Selection of pure LiNiO2 removes the complication of multiple transition metals. Using combined X-ray absorption spectroscopy, resonant inelastic X-ray scattering, and operando differential electrochemical mass spectrometry, we are able to clarify the redox reactions of transition metals in the bulk and at the surface, reversible lattice oxygen redox, and irreversible oxygen release associated with surface reactions. Many findings presented here bring attention to different types of oxygen activities and metal–oxygen interactions in layered oxides, which are of crucial importance to the advancement of a Ni-rich layered oxide cathode for high capacity and long cycling performance.

Journal
ACS Energy Letters
Volume
4
Year of Publication
2019
Issue
12
Pagination
2836 - 2842
ISSN Number
2380-8195
Short Title
ACS Energy Lett.
Refereed Designation
Refereed
Organizations
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