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Understanding voltage decay in lithium-excess layered cathode materials through oxygen-centred structural arrangement
Seungjun Myeong1, Woongrae Cho1, Wooyoung Jin1
1Department of Energy Engineering and School of Energy and Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan, 689-798, South Korea.
Nature Communications
|August 18, 2018
Summary
Lithium-excess layered oxides show voltage decay due to cation arrangement. Understanding this structure-property relationship is key to developing high-energy density cathode materials for batteries.
Area of Science:
- Materials Science
- Electrochemistry
- Solid-State Chemistry
Background:
- Lithium-excess 3d-transition-metal layered oxides (Li1+xNiyCozMn1-x-y-zO2) offer high energy density (>250 mAh g-1).
- Severe voltage decay during cycling limits their practical application and impedes further development.
- The underlying degradation mechanisms remain poorly understood due to the material's complex chemistry and structure.
Purpose of the Study:
- To elucidate the fundamental reason for voltage decay in lithium-excess layered oxides.
- To investigate the influence of cation arrangement on material properties and degradation.
- To provide insights for designing stable, high-energy density cathode materials.
Main Methods:
- Comparative study of ordered and cation-disordered materials.
- Advanced characterization using X-ray absorption spectroscopy (XAS).
- High-resolution imaging with transmission electron microscopy (TEM).
Main Results:
- Cation arrangement significantly impacts transition metal-oxygen covalency and structural reversibility.
- Identified de-lithiated oxygen-centered octahedra as a key structural feature.
- Observed interactions between octahedra influence oxygen stability and transition metal mobility.
Conclusions:
- The cation ordering in layered oxides is critical for mitigating voltage decay.
- Understanding these structural-property relationships offers a pathway to improved cathode material stability.
- This research provides fundamental insights into the degradation chemistry of advanced battery materials.
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