Xiaoming Lin, Jia Lin, Xiaomeng Lu, Xiaohong Tan, Hao Li, Wanxin Mai, Yuhong Luo, Yongbo Wu, Shuangqiang Chen, Chao Yang, Yong Wang. Vacancy-engineered LiMn2O4 embedded in dual-heteroatom-doped carbon via metal-organic framework-mediated synthesis towards longevous lithium ion battery[J]. Materials Futures, 2025, 4(2): 025101. DOI: 10.1088/2752-5724/ad9e08
Citation: Xiaoming Lin, Jia Lin, Xiaomeng Lu, Xiaohong Tan, Hao Li, Wanxin Mai, Yuhong Luo, Yongbo Wu, Shuangqiang Chen, Chao Yang, Yong Wang. Vacancy-engineered LiMn2O4 embedded in dual-heteroatom-doped carbon via metal-organic framework-mediated synthesis towards longevous lithium ion battery[J]. Materials Futures, 2025, 4(2): 025101. DOI: 10.1088/2752-5724/ad9e08
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Vacancy-engineered LiMn2O4 embedded in dual-heteroatom-doped carbon via metal-organic framework-mediated synthesis towards longevous lithium ion battery

© 2025 The Author(s). Published by IOP Publishing Ltd on behalf of the Songshan Lake Materials Laboratory
Materials Futures, Volume 4, Number 2
  • Received Date: September 19, 2024
  • Revised Date: November 20, 2024
  • Accepted Date: December 07, 2024
  • Available Online: December 12, 2024
  • Published Date: March 02, 2025
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  • Spinel LiMn2O4 (LMO) is deemed to be a promising cathode material for commercial lithium-ion batteries (LIBs) in prospect of its cost-effectiveness, nontoxicity, fabulous rate capability, and high energy density. Nevertheless, the LMO is inevitably confronted with sluggish diffusion kinetics and drastic capacity degradation triggered by multiple issues, including Jahn–Teller distortion, Mn dissolution, and structural attenuation. Thereinto, a metal-organic framework (MOF) chemistry engineering for hierarchical micro-/nano-structural F, O-dual-doped carbon embedded oxygen vacancy enriched LiMn2O4 cathode (OV-LMO@FOC) is proposed for longevous LIBs. Bestowed by experimental and theoretical implementations, systematic investigations of OV-LMO@FOC endow that the meticulous integration of F, O-dual-doped carbon and oxygen vacancy in LMO-based cathode reconfigures the electronic structure, boosts electronic conductivity, expedites diffusion capability, facilitates energetically preferable Li+ adsorption, and suppresses Mn dissolution in the electrolyte, consequently achieving fabulous long-term cycling stability. As expected, the OV-LMO@FOC behaves with compelling electrochemical performance with prosperous reversible capacity (130.2 mAh g-1 at 0.2 C upon 200 cycles), exceptional rate capacity (93.7 mAh g-1 even at 20 C), and pronounced long-term cyclability (112.5 mAh g-1 after 1200 cycles with 77.6% capacity retention at 1 C). Even at the ultrahigh current density of 5 C, the OV-LMO@FOC bears a brilliant capacity of 96.9 mAh g-1 upon 1000 cycles with an extraordinary capacity retention of 90.7%, and maintains a discharge capacity of 70.9 mAh g-1 upon 4000 cycles. This work envisions the MOF-chemistry in surface modification and electronic modulation engineering of high-performance cathode materials towards industrialization in automotive market.
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    1. Ou, H., Mo, Q., Chen, Y. et al. Achieving fast lithium/sodium storage reaction kinetics through semiconductor hetero-interface construction derived from metal-organic framework. Journal of Colloid and Interface Science, 2025. DOI:10.1016/j.jcis.2025.138333
    2. Lu, Y., Guo, M., Zhang, Z. et al. Carbon-encapsulated Sb-based nanotubes enable advanced lithium storage anode. Sustainable Materials and Technologies, 2025. DOI:10.1016/j.susmat.2025.e01463
    3. Zhang, Y., Peng, J., Zhao, M. et al. Turning waste into treasure: a dual-modulation strategy for Ni-rich cathode towards moderate Li/Ni mixing and Li2CO3 encapsulation to enhance lithium storage. Journal of Energy Chemistry, 2025. DOI:10.1016/j.jechem.2025.05.044
    4. Chen, S.-J., Guo, X.-W., Wang, J.-H. et al. Cross-Dimensional Control of Topological Defects and Critical Size Effect in Lead-Free Thin Films. Journal of Physical Chemistry C, 2025, 129(26): 12175-12183. DOI:10.1021/acs.jpcc.5c02540
    5. Zhang, Y., Chen, Y., Mai, W. et al. Mn-Ni bimetallic microporous sulfide electrode materials for efficient supercapacitor conversion. Flatchem, 2025. DOI:10.1016/j.flatc.2025.100877
    6. Huang, Q., Xie, T., Luo, Y. et al. A Comprehensive Review on Zinc-Based MOFs and Their Derivatives for Alkali-Ion Batteries: Synthesis, Applications, and Future Prospects. Advanced Functional Materials, 2025. DOI:10.1002/adfm.202508749

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