Abstract
The oxygen redox reaction in lithium-rich layered oxide battery cathode materials generates extra capacity at high cell voltages (i.e., >4.5 V). However, the irreversible oxygen release causes transition metal (TM) dissolution, migration and cell voltage decay. To circumvent these issues, we introduce a strategy for tuning the Coulombic interactions in a model Li-rich positive electrode active material, i.e., Li1.2Mn0.6Ni0.2O2. In particular, we tune the Coulombic repulsive interactions to obtain an adaptable crystal structure that enables the reversible distortion of TMO6 octahedron and mitigates TM dissolution and migration. Moreover, this strategy hinders the irreversible release of oxygen and other parasitic reactions (e.g., electrolyte decomposition) commonly occurring at high voltages. When tested in non-aqueous coin cell configuration, the modified Li-rich cathode material, combined with a Li metal anode, enables a stable cell discharge capacity of about 240 mAh g−1 for 120 cycles at 50 mA g−1 and a slower voltage decay compared to the unmodified Li1.2Mn0.6Ni0.2O2.
| Original language | English |
|---|---|
| Article number | 1123 |
| Journal | Nature Communications |
| Volume | 13 |
| Issue number | 1 |
| DOIs | |
| State | Published - Dec 2022 |
Funding
This work was supported by the International Partnership Program (grant no. 211211KYSB20170060) of the Chinese Academy of Sciences, the National Natural Science Foundation of China (grant nos. 11975238 and 11575192), the Scientific Instrument Developing Project (grant no. ZDKYYQ20170001), and the Strategic Priority Research Program (grant no. XDB28000000) of the Chinese Academy of Sciences. This work was also supported by the Fundamental Research Funds for the Central Universities. The neutron experiments at the SNS user facilities (VULCAN beamline) were sponsored by the Office of Basic Energy Sciences (BES) and the Office of Science of the U.S. DOE. The authors thank Dr. Dmitry Smirnov at the Russian–German Beamline at BESSY-II, HZB, Germany. The authors also thank the staff at beamline 20A1 of the TLS at HsinChu. The authors thank Dr. Hui Fu and the Analytical Instrumentation Centre of Peking University for help with ssNMR testing and analysis and Dr. Jicheng Zhang and Weijin Kong from the University of Chinese Academy of Sciences for help with article revision. This work was supported by the International Partnership Program (grant no. 211211KYSB20170060) of the Chinese Academy of Sciences, the National Natural Science Foundation of China (grant nos. 11975238 and 11575192), the Scientific Instrument Developing Project (grant no. ZDKYYQ20170001), and the Strategic Priority Research Program (grant no. XDB28000000) of the Chinese Academy of Sciences. This work was also supported by the Fundamental Research Funds for the Central Universities. The neutron experiments at the SNS user facilities (VULCAN beamline) were sponsored by the Office of Basic Energy Sciences (BES) and the Office of Science of the U.S. DOE. The authors thank Dr. Dmitry Smirnov at the Russian–German Beamline at BESSY-II, HZB, Germany. The authors also thank the staff at beamline 20A1 of the TLS at HsinChu. The authors thank Dr. Hui Fu and the Analytical Instrumentation Centre of Peking University for help with ssNMR testing and analysis and Dr. Jicheng Zhang and Weijin Kong from the University of Chinese Academy of Sciences for help with article revision.