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. 2025 Jan;37(1):e2412673.
doi: 10.1002/adma.202412673. Epub 2024 Nov 7.

Dynamic Transition Metal Network via Orbital Population Design Stabilizes Lattice Oxygen Redox in Stoichiometric Layered Cathodes

Ang Gao  1   2   3 , Xinyan Li  4 , Qinghua Zhang  5 , Ting Lin  6 , Yichi Wang  6 , Yujie Chen  6 , Weiguang Lin  5 , Shiyu Wang  5 , Pengxiang Ji  5 , Zhu Luo  1   2   3 , Jinlong Wang  1   2   3 , Yanbing Guo  1   2   3 , Lin Gu  6
Affiliations

Dynamic Transition Metal Network via Orbital Population Design Stabilizes Lattice Oxygen Redox in Stoichiometric Layered Cathodes

Ang Gao et al. Adv Mater. 2025 Jan.

Abstract

Li-ion batteries employing stoichiometric layered Li metal oxides as cathodes are now reaching the energy density limits due to single cationic redox chemistry. Lattice oxygen redox (LOR) has been discovered in these materials, as a high-energy-density paradigm observed in Li-rich materials. Nevertheless, the origin of this process is not understood, preventing the rational design of better cathode materials. Here, employing stoichiometric Ni-based cathodes, it is demonstrated that LOR originates from a dynamic transition metal (TM) network caused by ion migration during the electrochemical process. This network is confirmed to be ribbon through both ex- and in-situ STEM observations, facilitating reversible LOR. Finally, a t2g orbital population rule is proposed to guide the design of ordered TM networks, supported by calculated structures and the synthesized ordered TM oxides reported. This work explains the mechanism of LOR in stoichiometric layered cathode materials, and sets a promising direction for the design of high-energy-density cathodes through the regulation of TM ordering.

Keywords: Li‐ion batteries; lattice oxygen redox; orbital population; stoichiometric layered oxides; transition metal network.

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References

    1. a) W. Huang, T. Liu, L. Yu, J. Wang, T. Zhou, J. Liu, T. Li, R. Amine, X. Xiao, M. Ge, L. Ma, S. N. Ehrlich, M. V. Holt, J. Wen, K. Amine, ScienceScience 2024, 384, 912;
    1. b) Q. Wang, Z. Yao, J. Wang, H. Guo, C. Li, D. Zhou, X. Bai, H. Li, B. Li, M. Wagemaker, C. Zhao, NatureNature 2024, 629, 341.
    1. a) T. Liu, J. Liu, L. Li, L. Yu, J. Diao, T. Zhou, S. Li, A. Dai, W. Zhao, S. Xu, Y. Ren, L. Wang, T. Wu, R. Qi, Y. Xiao, J. Zheng, W. Cha, R. Harder, I. Robinson, J. Wen, J. Lu, F. Pan, K. Amine, NatureNature 2022, 606, 305;
    1. b) J.‐J. Marie, R. A. House, G. J. Rees, A. W. Robertson, M. Jenkins, J. Chen, S. Agrestini, M. Garcia‐Fernandez, K.‐J. Zhou, P. G. Bruce, Nat. Mater. 2024, 23, 818.
    1. D. H. Seo, J. Lee, A. Urban, R. Malik, S. Kang, G. Ceder, Nat. Chem. 2016, 8, 692.

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