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Titanium Substitution Facilitating Oxygen and Manganese Redox in Sodium Layered Oxide Cathode
Advanced Materials Interfaces ( IF 5.4 ) Pub Date : 2024-04-10 , DOI: 10.1002/admi.202400190
Junhua Zhou 1, 2 , Huimin Hu 1, 2 , Jiaqi Wang 1, 2 , Qitao Shi 1, 2 , Xueyu Lian 1, 2 , Lijun Liu 3 , Alicja Bachmatiuk 4 , Jingyu Sun 1, 2 , Ruizhi Yang 1, 2 , Jin‐Ho Choi 1, 2 , Mark H. Rümmeli 1, 2, 5, 6, 7
Affiliation  

Sodium layered oxide with anion redox activity (SLO‐A) stands out as a promising cathode material for sodium‐ion batteries due to its impressive capacity and high voltage resulting from Mn‐ and O‐redox processes. However, the SLO‐A faces significant challenges in cycling stability and rate performance, primarily due to the poor reversibility and sluggish kinetics of the O‐redox. In this study,a novel Ti‐doped material, Na2/3Li2/9Mn53/72Ti1/24O2 (NLMTO), exhibiting remarkable characteristics such as a notable rate capacity (130 mAh g−1 at 3C, where 1C equals 200 mA g−1) and excellent cycling retention (85.4% after 100 cycles at 0.5C) is introduced. Employing electrochemical differential analyses, the contributions to the superior performance arising from the Mn‐ and O‐redox processes are quantitatively delineated. The optimized performance of NLMTO is attributed, in part, to the enhanced stability of both bulk and interface structures. The introduction of Ti through substitution not only contributes to this stability but also allows for the fine‐tuning of the material's electron configurations. This is achieved by augmenting the density of states near the Fermi energy level, as well as elevating the O 2p and Mn 3d orbits. This research advances sodium‐ion battery technology.

中文翻译:

钠层状氧化物阴极中钛的替代促进氧和锰的氧化还原

具有阴离子氧化还原活性的钠层状氧化物(SLO-A)因其锰和氧氧化还原过程产生的令人印象深刻的容量和高电压而成为钠离子电池有前途的正极材料。然而,SLO-A 在循环稳定性和倍率性能方面面临重大挑战,这主要是由于 O-氧化还原的可逆性差和动力学缓慢。在这项研究中,一种新型的钛掺杂材料Na2/32/953/721/242(NLMTO),表现出显着的特性,例如显着的倍率容量(130 mAh g−13C 时,其中 1C 等于 200 mA g−1)和出色的循环保持率(0.5C 下 100 次循环后为 85.4%)。采用电化学微分分析,定量描述了锰和氧氧化还原过程对优异性能的贡献。 NLMTO 的优化性能部分归因于体结构和界面结构稳定性的增强。通过取代引入钛不仅有助于这种稳定性,而且还可以微调材料的电子构型。这是通过增加费米能级附近的态密度以及提升 O 2p 和 Mn 3d 轨道来实现的。这项研究推进了钠离子电池技术。
更新日期:2024-04-10
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