Dual-ion regulation of coordination chemistry for high-voltage stabilized P2-type cathode

阴极 材料科学 电化学 钠离子电池 密度泛函理论 离子 过渡金属 相变 空位缺陷 化学物理 分析化学(期刊) 结晶学 电极 化学 计算化学 物理化学 热力学 有机化学 法拉第效率 物理 催化作用 生物化学 色谱法
作者
Jiangnan Huang,Jinqiang Gao,Ningyun Hong,Baichao Zhang,Haoji Wang,Fangjun Zhu,Lianshan Ni,Guoqiang Zou,Hongshuai Hou,Hongyi Chen,Wentao Deng,Xiaobo Ji
出处
期刊:Nano Energy [Elsevier BV]
卷期号:126: 109676-109676 被引量:7
标识
DOI:10.1016/j.nanoen.2024.109676
摘要

P2-Na2/3Ni1/3Mn2/3O2 has shown great potential as cathode material for sodium-ion batteries with its high theoretical capacity and energy density. However, severe structural changes are induced by charging P2-Na2/3Ni1/3Mn2/3O2 above 4.2 V, resulting in rapid capacity decay and poor kinetic capability. In this study, we propose a Zn/Ti synergistic modification strategy to stabilize the P2-type cathode under high voltage. It is found that the P2-O2 phase transition with large volume change is replaced by a milder P2-Z phase transition with the noteworthy improvement in structural stability and Na+ diffusion kinetics, due to the disordered Na+/vacancy and the suppressed of the sliding of transition metal layers, as disclosed by density functional theory calculations and in-situ X-ray diffraction. Concurrently, The phenomenon of Ni and O reductive coupling is inhibited by regulating local O coordination owing to the incorporation of a strong Ti−O covalence bond, leading to the more reversible charge compensation mechanism and the inhibited lattice O evolution, as clearly revealed by ex-situ X-ray absorption spectroscopy and Differential Electrochemical Mass Spectrometry. Consequently, we obtained a stable P2-Na0.67Zn0.05Ni0.28Mn0.52Ti0.15O2 cathode, achieving an average discharge voltage of 3.62 V at 0.1 C and a capacity retention of 80% after 500 cycles at 2 C. This research provides valuable insights into the enhancement of sodium-ion battery cathode materials by utilizing different functional ions in synergy.
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