Journal
CHEM
Volume 8, Issue 10, Pages 2817-2830Publisher
CELL PRESS
DOI: 10.1016/j.chempr.2022.07.023
Keywords
-
Categories
Funding
- National Key Research and Development Program of China
- National Natural Science Foundation of China
- Sichuan Science and Tech- nology Program
- Haihe Laboratory of Sustainable Chemical Transformations
- [2021YFB2500300]
- [2021YFB3800300]
- [52072185]
- [22008154]
- [2021JDRC0015]
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This study demonstrates a Li-enrichment strategy to revive lithium nickel oxide (LNO), a high-energy cathode with poor cycle performance and thermal instability. By forming vacancy clusters in the near-surface lattice, the Li-rich LNO cathode effectively suppresses lattice oxygen release and outperforms traditional Li-deficient LNO cathodes modified by conventional approaches.
Lattice oxygen release (LOR), which promotes surface structural degradation and electrolyte decomposition, is a major contributor to capacity fade and thermal runaway in layered oxide cathodes. Despite decades of research, it is still a great challenge to stabilize the lattice oxygen, especially in deeply delithiated cathodes. Here, we demon-strate an Li-enrichment strategy to revive lithium nickel oxide (LNO), a high-energy cathode (>900 Wh kg_1) long plagued by poor cycle performance and thermal instability. In a slightly Li-enriched LNO (Li1.04Ni0.96O2) prepared by a specially designed molten-salt synthesis, spatially resolved (operando) characterizations reveal intralayer Ni migration upon delithiation, and this leads to the formation of vacancy clusters to trap the electrochemically oxidized oxygen in the near -sur-face lattice. Thus, the detrimental effects of LOR are effectively sup-pressed. The Li-rich LNO cathode greatly outperforms the traditional Li-deficient LNO cathodes modified by conventional approaches such as doping and surface coating. Our findings open up new oppor-tunities for building better batteries.
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