Integrated rocksalt–polyanion cathodes with excess lithium and stabilized cycling

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 and Ju Li ()
Additional contact information
Yimeng Huang: Massachusetts Institute of Technology
Yanhao Dong: Tsinghua University
Yang Yang: The Pennsylvania State University
Tongchao Liu: Argonne National Laboratory
Moonsu Yoon: Massachusetts Institute of Technology
Sipei Li: Massachusetts Institute of Technology
Baoming Wang: Massachusetts Institute of Technology
Ethan Yupeng Zheng: Massachusetts Institute of Technology
Jinhyuk Lee: McGill University
Yongwen Sun: The Pennsylvania State University
Ying Han: The Pennsylvania State University
Jim Ciston: Lawrence Berkeley National Laboratory
Colin Ophus: Lawrence Berkeley National Laboratory
Chengyu Song: Lawrence Berkeley National Laboratory
Aubrey Penn: Massachusetts Institute of Technology
Yaqi Liao: Huazhong University of Science and Technology
Haijin Ji: Huazhong University of Science and Technology
Ting Shi: Huazhong University of Science and Technology
Mengyi Liao: Huazhong University of Science and Technology
Zexiao Cheng: Huazhong University of Science and Technology
Jingwei Xiang: Huazhong University of Science and Technology
Yu Peng: Fudan University
Lu Ma: Brookhaven National Laboratory
Xianghui Xiao: Brookhaven National Laboratory
Wang Hay Kan: Spallation Neutron Source Science Center
Huaican Chen: Spallation Neutron Source Science Center
Wen Yin: Spallation Neutron Source Science Center
Lingling Guo: Chinese Academy of Sciences
Wei-Ren Liu: Chung Yuan Christian University
Rasu Muruganantham: Chung Yuan Christian University
Chun-Chuen Yang: National Central University
Yuntong Zhu: Massachusetts Institute of Technology
Qingjie Li: Massachusetts Institute of Technology
Ju Li: Massachusetts Institute of Technology

Nature Energy, 2024, vol. 9, issue 12, 1497-1505

Abstract: Abstract 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.

Date: 2024
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DOI: 10.1038/s41560-024-01615-6

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