打破恶性螺旋以抑制丰富氧化物阴极材料中的氧气损失
Zhenjie Zhang1,2, Yixin Li1,3, Xi Shen4
1Key Laboratory for Renewable Energy, Chinese Academy of Sciences, Beijing Key Laboratory for New Energy Materials and Devices, Institute of Physics, Chinese Academy of Sciences, Beijing, 100190, China.
Advanced materials (Deerfield Beach, Fla.)
|June 3, 2025
概括
澄清了电池阴极中不可逆转的氧气损失. 在Li4Mn5O12中稳定的螺旋结构防止了氧的释放,使高能电池的可逆氧氧氧化还原成为可能.
科学领域:
- 材料科学 材料科学 材料科学
- 电化学 电化学 电化学
- 固态化学 固态化学
背景情况:
- 氧氧还氧 (O-redox) 阴极材料为/离子电池提供高能量密度.
- 不可逆转的氧气损失 (O-loss) 是一个主要的限制,阻碍了实际应用.
- 除了简单的表面现象之外,O-loss的精确机制仍然不太了解.
研究的目的:
- 在分层Li2MnO3和螺旋Li4Mn5O12中比较研究O-loss和O-redox行为.
- 阐明导致O损失和结构退化的潜在机制.
- 为了指导先进的O-redox阴极材料的设计.
主要方法:
- 对Li2MnO3和Li4Mn5O12的实验研究.
- 密度函数理论 (DFT) 的计算.
- Li4Mn5O12的原子组成与LiNi0.5Mn1.5O4.5的原子组成.
主要成果:
- 在Li2MnO3中,O-损失是由O-O二元化和Mn迁移的循环驱动的,导致空洞生长,结构崩和O2释放.
- 4Mn5O12表现出稳定的旋转框架和惰性氧气,阻止了这个循环,并将O2困在散装中,以获得可逆的O-redox.
- 通过将Li4Mn5O12与LiNi0.5Mn1.5O4合成,合成了一种新型的Co-free Li-rich spinel oxide (LRSO),实现了高能量密度 (>1000 Wh kg-1).
结论:
- 结构重组,特别是O-O二分化和阴离子迁移,与O-损失和O-redox活性直接相关.
- Li4Mn5O12的稳定螺旋结构有效抑制O损失,确保可逆的O-redox.
- 这项研究为设计下一代电池的稳定和高性能O-redox阴极材料提供了基本的见解.
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