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Integrated rocksalt–polyanion cathodes with excess lithium and stabilized cycling
Nature Energy ( IF 49.7 ) Pub Date : 2024-08-23 , DOI: 10.1038/s41560-024-01615-6
Yimeng Huang , Yanhao Dong , Yang Yang , Tongchao Liu , Moonsu Yoon , Sipei Li , Baoming Wang , Ethan Yupeng Zheng , Jinhyuk Lee , Yongwen Sun , Ying Han , Jim Ciston , Colin Ophus , Chengyu Song , Aubrey Penn , Yaqi Liao , Haijin Ji , Ting Shi , Mengyi Liao , Zexiao Cheng , Jingwei Xiang , Yu Peng , Lu Ma , Xianghui Xiao , Wang Hay Kan , Huaican Chen , Wen Yin , Lingling Guo , Wei-Ren Liu , Rasu Muruganantham , Chun-Chuen Yang , Yuntong Zhu , Qingjie Li , Ju Li

Co- and Ni-free disordered rocksalt cathodes utilize oxygen redox to increase the energy density of lithium-ion batteries, but it is challenging to achieve good cycle life at high voltages >4.5 V (versus Li/Li+). Here we report a family of Li-excess Mn-rich cathodes that integrates rocksalt- and polyanion-type structures. Following design rules for cation filling and ordering, we demonstrate the bulk incorporation of polyanion groups into the rocksalt lattice. This integration bridges the two primary families of lithium-ion battery cathodes—layered/spinel and phosphate oxides—dramatically enhancing the cycling stability of disordered rocksalt cathodes with 4.8 V upper cut-off voltage. The cathode exhibits high gravimetric energy densities above 1,100 Wh kg−1 and >70% retention over 100 cycles. This study opens up a broad compositional space for developing battery cathodes using earth-abundant elements such as Mn and Fe.



中文翻译:


具有过量锂和稳定循环的集成岩盐-聚阴离子阴极



不含钴和镍的无序岩盐正极利用氧氧化还原来提高锂离子电池的能量密度,但在高电压>4.​​5 V(相对于Li/Li + )下实现良好的循环寿命具有挑战性。在这里,我们报告了一系列集成了岩盐型和聚阴离子型结构的过量锂富锰正极。遵循阳离子填充和排序的设计规则,我们演示了聚阴离子基团大量掺入岩盐晶格中。这种集成连接了锂离子电池阴极的两个主要系列——层状/尖晶石和磷酸盐氧化物——极大地提高了无序岩盐阴极的循环稳定性,上限截止电压为 4.8 V。该阴极表现出高于1,100 Wh kg -1的高重量能量密度和超过100次循环的>70%保留率。这项研究为使用地球上丰富的元素(例如锰和铁)开发电池阴极开辟了广阔的成分空间。

更新日期:2024-08-23
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