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Lignin-reinforced PVDF electrolyte for dendrite-free quasi-solid-state Li metal battery

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Abstract

Quasi-solid-state lithium metal batteries (QSSLMBs) assembled with polyvinylidene fluoride (PVDF) are a promising class of next-generation rechargeable batteries due to their safety, high energy density, and superior interfacial properties. However, PVDF has a series of inherent drawbacks such as low ionic conductivity, ease of crystallization, and hydrophobic character that leading to poor cell properties. To tackle these issues, a lignin-reinforced PVDF electrolyte is proposed in this work to solve these drawbacks of PVDF and enhance the comprehensive performance of QSSBs. The lithophilic polar groups of lignin can promote uniform deposition of Li on the electrodes. Cooperating with the improved mechanical properties can efficiently prevent Li dendrites penetration through the separator. In addition, more active sites provided by lignin can also enhance Li+ transport and lead to a faster electrochemical reaction kinetic. Benefitting from the ingenious design, Li symmetric cells with 5% lignin-PVDF quasi-solid-state electrolyte can operate for 900 h at a high current density/capacity of 5 mA·cm−2/5 mAh·cm−2, while short-circuiting occurs after 56 h for the counterpart (pure PVDF). Moreover, a full cell of Li/5% lignin-PVDF/LFP cell demonstrates a high capacity of 96.2 mAh·g−1 after 2000 cycles at 10 C. This work is expected to open up promising opportunities to develop other high-energy/power-density QSSLMBs.

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摘要

用聚偏二氟乙烯 (PVDF) 组装的准固态锂金属电池 (QSSLMBs) 由于其安全性、高能量密度和优越的界面特性, 是一种有前景的下一代可充电电池。然而, PVDF有一系列固有的缺点, 如离子电导率低、易结晶和疏水等, 导致电池性能差。为了解决这些问题, 本工作提出了一种木质素增强的PVDF电解质, 以解决PVDF的这些缺点, 并提高QSSB的综合性能。木质素的亲锂性极性基团可以促进锂在电极上的均匀沉积。与改善的机械性能相配合, 可以有效地防止锂枝晶穿透隔膜。此外, 木质素提供的更多的活性位点也可以增强锂离子的传输, 并导致更快的电化学反应动力学。受益于这种巧妙的设计, 掺杂了5%木质素-PVDF准固态电解质的锂离子对称电池可以在5 mA·cm−2/5 mAh·cm−2的高电流密度/容量下运行900h, 而对应的电池 (纯PVDF) 在56h后发生短路。此外, 在10C条件下进行2000次循环后, 5%木质素-PVDF/LFP的全电池表现出96.2 mAh·g−1的高容量。这项工作有望为开发其他高能量/高功率密度的QSSLMB提供机会。

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Acknowledgements

This research was financially supported by the National Natural Science Foundation of China (No. 22208039), the Basic Scientific Research Project of the Educational Department of Liaoning Province (No. LJKMZ20220878), the Dalian Science and Technology Talent Innovation Support Plan (No. 2022RQ036) and Dalian Polytechnic University (No. 222002023044, No. 6102072202).

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  1. Center for Lignocellulosic Chemistry and Biomaterials, College of Light Industry and Chemical Engineering, Dalian Polytechnic University, Dalian, 116034, China

    Xin-Yang Chen, Xue-Jie Gao, Han-Yan Wu & Run-Cang Sun

  2. Division of Energy Storage, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China

    Xiao-Fei Yang

  3. School of Chemistry, Northeast Normal University, Changchun, 130024, China

    Yu-Long Liu

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Chen, XY., Gao, XJ., Wu, HY. et al. Lignin-reinforced PVDF electrolyte for dendrite-free quasi-solid-state Li metal battery. Rare Met. 43, 1006–1016 (2024). https://doi.org/10.1007/s12598-023-02444-4

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