DOE OSTI · 2588402
Minimizing Inter‐Lattice Strain to Stabilize Li‐Rich Cathode by Order–Disorder Control
Abstract
Li-rich Mn-based layered (LMR) cathodes with anionic redox chemistry show great potential for next-generation sustainable Li-ion battery (LIB) applications due to the low cost and high energy density. However, the asynchronous structural evolutions with cycling in the heterogeneous composite structure of LMR lead to serious lattice strain and thus fast electrochemical decay, which hinders the commercialization of LMR cathodes. Here, in this study, an order–disorder coherent LMR cathode is demonstrated that exhibits a higher average voltage (by 0.25 V), negligible voltage decay (97.6% voltage retention after 100 cycles at 100 mA g −1 ), and enhanced cycling stability (98% capacity retention after 200 cycles at 100 mA g −1 ) compared to its layered oxide counterparts. It is proposed that this order–disorder coherent structure design can promote a more synchronous and homogeneous structure evolution during charge and discharge, thus minimizing lattice strain, which significantly prevents layer collapse and collective degradation at high voltage, improving the electrochemical stability. The study displays the feasibility of optimizing the performance of Li-rich cathode materials through a dedicated order–disorder structure control for sustainable energy storage.
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Xu, Shenyang [Peking University, Shenzhen (China)] (ORCID:000000021124484X), Gao, Zhihai [Peking University, Shenzhen (China)], Chen, Hao [University of Chinese Academy of Sciences, Beijing (China)], Chang, Liang [Tsinghua University, Shenzhen (China)], Zhang, Nian [Chinese Academy of Sciences (CAS), Shanghai (China)], Zhou, Dong [Institute of Advanced Science Facilities, Shenzhen (China) ], Li, Tianyi [Argonne National Laboratory (ANL), Argonne, IL (United States)], Wang, Tony [Queensland University of Technology, Brisbane, QLD (Australia)], Lin, Cong [Hong Kong Polytechnic University, Kowloon (Hong Kong)], Xue, Haoyu [Peking University, Shenzhen (China)], Lai, Qinghao [Peking University, Shenzhen (China)], Huang, Weiyuan [Argonne National Laboratory (ANL), Argonne, IL (United States)], Yang, Luyi [Peking University, Shenzhen (China)], Liu, Jiajie [Peking University, Shenzhen (China)], Liu, Tongchao [Argonne National Laboratory (ANL), Argonne, IL (United States)], He, Lunhua [China Spallation Neutron Source, Dongguan (China)], Zhang, Mingjian [The Chinese University of Hong Kong, Ma Liu Shui, Shatin (Hong Kong)], Lun, Zhengyan [University of Chinese Academy of Sciences, Beijing (China)], Pan, Feng [Peking University, Shenzhen (China)] (ORCID:0000000213624336). 2025-05-21. Minimizing Inter‐Lattice Strain to Stabilize Li‐Rich Cathode by Order–Disorder Control. https://doi.org/10.1002/adma.202418580
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