Bo Peng, Zihao Zhou, Ji Shi, Sheng Xu, Jie Yang, Chengrong Xu, Daxian Zuo, Jie Xu, Lianbo Ma, Shaohua Guo, Haoshen Zhou
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引用次数: 0
摘要
高电压 P2-Na0.67Ni0.33Mn0.67O2 层状氧化物正极在钠离子电池中具有巨大潜力,因为其工作电压和理论能量密度均高于磷酸铁锂,但大体积相变是其致命弱点。目前,这种正极仍然存在稳定性和容量权衡的困境。为解决上述问题,本文提出了一种通过多种成岩元素微量掺杂的定制策略概念。定制的掺杂镁-铝-钛微量元素阴极可保持 140.3 mAh g - 1 的显著容量,能量密度接近 500 Wh kg - 1,并显示出良好的循环稳定性,在 0.1C 下循环 50 次后仍能保持 89.0% 的容量。此外,与硬碳阳极配对的全电池还实现了 303.3 Wh kg-1 的先进能量密度。多重表征揭示了对比样品的失效机理,包括严重的粒内裂纹以及层到岩盐的转变,这减少了活性物质并增加了电荷转移电阻。而掺杂后滑动能垒增加的样品则很好地抑制了这一现象。令人印象深刻的是,这种定制策略可扩展到镁-铁-钛体系。这项研究为高能钠离子阴极的设计提供了一个新概念。
A Customized Strategy Realizes Stable Cycle of Large-Capacity and High-Voltage Layered Cathode for Sodium-Ion Batteries
High-voltage P2-Na0.67Ni0.33Mn0.67O2 layered oxide cathode exhibits significant potential for sodium-ion batteries, owing to the elevated operating voltage and theoretical energy density beyond lithium iron phosphate, but the large-volume phase transition is the devil. Currently, this type cathode still suffers from stability–capacity trade-off dilemma. Herein, a concept of customized strategy via multiple rock-forming elements trace doping is presented to address the mentioned issue. The customized Mg-Al-Ti trace doped cathode maintains a notable capacity of 140.3 mAh g − 1 with an energy density approaching 500 Wh kg − 1, and shows good cycle stability, retaining 89.0% of its capacity after 50 cycles at 0.1C. Additionally, the full cell, paired with a hard carbon anode, achieves an advanced energy density of 303.3 Wh kg−1. The multiple characterizations reveal the failure mechanism of contrast sample involving severe intragranular cracks coupled with layer to rock salt transformation, which reduces active substance and increases charge transfer resistance. The doped sample with increased sliding energy barrier well suppresses this phenomenon. Impressively, the customized strategy can be extended to Mg-Fe-Ti system. This research provides a novel concept for the design of high energy sodium-ion cathode.
期刊介绍:
Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.