Unexpectedly Large Contribution of Oxygen to Charge Compensation Triggered by Structural Disordering: Detailed Experimental and Theoretical Study on a Li<sub>3</sub>NbO<sub>4</sub>–NiO Binary System
Ryutaro Fukuma, Maho Harada, Wenwen Zhao, Miho Sawamura, Yusuke Noda, Masanobu Nakayama, Masato Goto, Daisuke Kan, Yuichi Shimakawa, Masao Yonemura, Naohiro Ikeda, Ryuta Watanuki, H.L. Andersen, Anita M. D’Angelo, Neeraj Sharma, Jiwon Park, Hye Ryung Byon, Sayuri Fukuyama, Zhen‐Ji Han, Hitoshi Fukumitsu, M. Schulz‐Dobrick, Keisuke Yamanaka, Hirona Yamagishi, Toshiaki Ohta, Naoaki Yabuuchi
Abstract
with a cation-disordered Li/Ni arrangement. Further Li enrichment in the structure destabilizes anionic redox and leads to irreversible oxygen loss due to the disappearance of the linear Ni-O-Ni configuration and the formation of unstable Ni ions with high oxidation states. On the basis of these results, we discuss the possibility of using σ-type interactions for anionic redox to design advanced electrode materials for high-energy lithium-ion batteries.