Minimizing Inter‐Lattice Strain to Stabilize Li‐Rich Cathode by Order–Disorder Control

Xu, Shenyang; Gao, Zhihai; Chen, Hao; Chang, Liang; Zhang, Nian; Zhou, Dong; Li, Tianyi; Wang, Tony; Lin, Cong; Xue, Haoyu; Lai, Qinghao; Huang, Weiyuan; Yang, Luyi; Liu, Jiajie; Liu, Tongchao; He, Lunhua; Zhang, Mingjian; Lun, Zhengyan; Pan, Feng

doi:10.1002/adma.202418580

Minimizing Inter‐Lattice Strain to Stabilize Li‐Rich Cathode by Order–Disorder Control

Journal Article · Wed May 21 00:00:00 EDT 2025 · Advanced Materials

DOI:https://doi.org/10.1002/adma.202418580· OSTI ID:2588402

^[1]; Gao, Zhihai ^[1]; Chen, Hao ^[2]; Chang, Liang ^[3]; Zhang, Nian ^[4]; Zhou, Dong ^[5]; Li, Tianyi ^[6]; Wang, Tony ^[7]; Lin, Cong ^[8]; Xue, Haoyu ^[1]; Lai, Qinghao ^[1]; Huang, Weiyuan ^[6]; Yang, Luyi ^[1]; Liu, Jiajie ^[1]; Liu, Tongchao ^[6]; He, Lunhua ^[9]; Zhang, Mingjian ^[10]; Lun, Zhengyan ^[2]; ^[1]

Peking University, Shenzhen (China)
University of Chinese Academy of Sciences, Beijing (China)
Tsinghua University, Shenzhen (China)
Chinese Academy of Sciences (CAS), Shanghai (China)
Institute of Advanced Science Facilities, Shenzhen (China)
Argonne National Laboratory (ANL), Argonne, IL (United States)
Queensland University of Technology, Brisbane, QLD (Australia)
Hong Kong Polytechnic University, Kowloon (Hong Kong)
China Spallation Neutron Source, Dongguan (China)
The Chinese University of Hong Kong, Ma Liu Shui, Shatin (Hong Kong)

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.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: National Natural Science Foundation of China (NSFC); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Science (SC)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 2588402

Journal Information:: Advanced Materials, Journal Name: Advanced Materials Journal Issue: 32 Vol. 37; ISSN 1521-4095; ISSN 0935-9648

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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