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Dynamically lithium-compensated polymer artificial SEI to assist highly stable lithium-rich manganese-based anode-free lithium metal batteries

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Abstract

Owing to the unique structure, anode-free lithium metal batteries (AFLMBs) have higher energy density and lower production cost than traditional lithium metal batteries (LMBs) or lithium-ion batteries (LIBs). However, AFLMBs suffer from an inherently finite Li reservoir and exhibit poor cycle stability, low Coulombic efficiency (CE) and severe dendrite growth. In this work, polydiallyl lithium disulfide (PDS-Li) was successfully synthesized and coated on Cu current collector by electrochemical polymerization. The PDS-Li acts as an additional lithium resource to compensate for the irreversible loss of lithium during cycling. In addition, the special structure and lithiophilicity of PDS-Li contribute to lower nucleation overpotential and uniform lithium deposition. When coupled with Li-rich manganese-based (LRM) cathode of Li1.2Mn0.54Ni0.13Co0.13O2, the anode-free full cell exhibits significantly improved cycle stability over 100 cycles and capacity retention of 63.3% and 57% after 80 and 100 cycles, respectively. We believe that PDS-Li can be used to ensure stable cycling performance and high-energy–density in AFLMBs.

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摘要

由于无负极锂金属电池独特的结构，无负极锂金属电池比传统的锂金属电池或锂离子电池具有更高的能量密度和更低的生产成本。然而，无负极锂金属电池受到固有的有限锂存储的影响，表现出差的循环稳定性，低的库仑效率和严重的枝晶生长。本文成功地合成了聚二烯丙基二硫化锂，并通过电化学聚合将其包覆在铜集流体上。聚二烯丙基二硫化锂中的锂作为额外的锂资源可以补偿循环过程中不可逆的锂损失。此外，聚二烯丙基二硫化锂的特殊结构和亲锂性有助于降低成核过电位和均匀的锂沉积。当与富锂锰基正极Li1.2Mn0.54Ni0.13Co0.13O2配对时，无负极锂金属全电池在100圈循环的循环稳定性显著提高，第80圈和100圈循环后的容量保持率分别为63.3%和57%。我们相信聚二烯丙基二硫化锂可以用于保证无负极锂金属电池稳定的循环性能和高能量密度。

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Acknowledgements

This study was financially supported by the National Natural Science Foundations of China (Nos. 52071226, 51872193 and U21A20332), the Natural Science Foundations of Jiangsu Province (Nos. BK20181168, BK20201171 and BK20220061), the Key R&D Project funded by Department of Science and Technology of Jiangsu Province (No. BE2020003-3), the Natural Science Foundation of Jiangsu Higher Education Institutions of China (No. 19KJA210004) and the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD).

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  1. Ming-Ji Peng and Jin-Qiu Zhou have contributed equally to this work.

Authors and Affiliations

  1. Key Laboratory of Core Technology of High Specific Energy Battery and Key Materials for Petroleum and Chemical Industry, College of Energy, Soochow University, Suzhou, 215006, China

    Ming-Ji Peng, Yang Zhou, Zhen-Kang Wang & Cheng-Lin Yan

  2. School of Chemistry and Chemical Engineering, Nantong University, Nantong, 226019, China

    Jin-Qiu Zhou & Jie Liu

  3. State Key Laboratory of Space Power-Sources Technology, Shanghai Institute of Space Power-Sources, Shanghai, 200245, China

    Ting-Ting Han

  4. Centre Énergie, Matériaux et Télécommunications, Institut National de la Recherche Scientifique, Varennes, QC, J3X 1S2, Canada

    Na Xu

  5. Light Industry Institute of Electrochemical Power Sources, Suzhou, 215006, China

    Ming-Ji Peng, Zhen-Kang Wang & Cheng-Lin Yan

  6. Zhangjiagang Industrial Technologies, Soochow University, Suzhou, 215006, China

    Wen-Bin Lin

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  1. Ming-Ji Peng
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Peng, MJ., Zhou, JQ., Han, TT. et al. Dynamically lithium-compensated polymer artificial SEI to assist highly stable lithium-rich manganese-based anode-free lithium metal batteries. Rare Met. 43, 2527–2535 (2024). https://doi.org/10.1007/s12598-023-02609-1

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