Dendrite-free Mg-MOF-based all-solid-state lithium metal batteries with superior cycle life

Dendrite-free Mg-MOF-based all-solid-state lithium metal batteries with superior cycle life

Rare Metals

10.1007/s12598-024-03049-1

https://doi.org/10.1007/s12598-024-03049-1

Xu-Dong Chen, Si Zhao, Xin-Fu Feng, Jin Huang, Yan Wang, Zhen-Chun Qiu, Jian-Biao Wang, Yi-Yin Huang, Li-Tuo Zheng, Ming-Deng Wei, Zhen-Sheng Hong

General Materials Science

09 January 2025

Chen, X.-D., Zhao, S., Feng, X.-F., Huang, J., Wang, Y., Qiu, Z.-C., Wang, J.-B., Huang, Y.-Y., Zheng, L.-T., Wei, M.-D., & Hong, Z.-S. (2025). Dendrite-free Mg-MOF-based all-solid-state lithium metal batteries with superior cycle life. Rare Metals, 44(4), 2805–2814. https://doi.org/10.1007/s12598-024-03049-1

The widespread application of solid-state polymer electrolytes (SPEs) is impeded due to their limited ionic conductivity, narrow electrochemical window and lithium dendrite problem. In this work, Mg-metal–organic frameworks (MOF) is incorporated into a polyethylene oxide (PEO)-based polymer solid electrolyte, leading to the insitu formation of LiF and other compounds at the electrolyte interface. This modification significantly improves lithium-ion transport capabilities and regulates lithium deposition behavior, suppressing the formation of lithium dendrites. Mg-MOF serves as a Lewis acid site, facilitating anion adsorption and promoting the dissociation of lithium bis(trifluoromethanesulfonyl) imide (LiTFSI), also providing additional sites for complexation/decomplexation of lithium ions. As a result, symmetric Li//Li cells demonstrate stable plating/stripping performance for over 3000 h with a low overpotential of 35 mV at 0.1 mAcm-2 . SPE@Mg-MOF exhibits high ionic conductivity (5.2 9 10-4 Scm-1 at 60 C) and a high lithium-ion migration number (0.64). Consequently, Li/SPE@MgMOF/LiFePO4 full cell demonstrates a high discharge capacity of 169.4 mAhg-1 at 0.1C, a significantly improved rate capability with 145.7 mAhg-1 at 5C, and an impressive capacity retention rate of 80% after stable cycling for 500 cycles at 1C. Lithium-ion batteries (LIBs) have recently garnered great attention due to their costefficiency and high energy density [1–3]. It is expected that lithium metal batteries (LMBs) with Li metal as an anode are a promising candidate in realizing high energy density battery, due to their high theoretical capacity (3860 mAhg-1 ) and low standard electrode potential (3.04 V (vs. SHE)) [4–12]. However, conventional organic liquid electrolytes comprise flammable and volatile solvents, exhibiting instability and safety concerns. In contrast, SPEs show enhanced thermal and electrochemical stability, and are recognized as potential electrolyte candidates for next generation lithium batteries

Publisher Copyright

There was no specific funding for the research done

This is a post-peer-review, pre-copyedit version of an article published in Rare Metals. The final authenticated version is available online at: http://dx.doi.org/10.1007/s12598-024-03049-1.

https://oar.a-star.edu.sg/communities-collections/articles/22326

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