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Nb2CTx MXene boosting PEO polymer electrolyte for all-solid-state Li-S batteries: two birds with one stone strategy to enhance Li+ conductivity and polysulfide adsorptivity

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Abstract

All-solid-state lithium-sulfur (Li-S) battery is regarded as next-generation high energy density and safety battery system. The key challenge is to develop a compatible high-performance solid-state electrolyte. Herein, a two birds with one stone strategy is proposed to simultaneously enhance Li+ conductivity and polysulfide adsorptivity of poly(ethylene oxide) (PEO)-based polymer electrolyte via the integration of Nb2CTx MXene. Moreover, the sheet size of Nb2CTx MXene is crucial for the enhancement of Li+ conductivity and polysulfide adsorptivity, attributing to the difference in a specific surface area related to the percolation effect. By tuning the sheet size of Nb2CTx MXene from 500–300 nm to below 100 nm, the ionic conductivity of the PEO electrolyte is increased to 2.62 × 10−4 S·cm−1 with improved Li+ transference number of 0.37 at 60 °C. Furthermore, theoretical calculation and X-ray photoelectron spectroscopy (XPS) conjointly prove that polysulfides could be effectively adsorbed by Nb2CTx nanosheets via forming Nb−S bonding to inhibit their shuttle in the PEO framework. As a result, the all-solid-state Li-S cell exhibits an initial capacity of 1149 mAh·g−1 at 0.5C and good cycling stability with 491 mAh·g−1 after 200 cycles. The results demonstrate the necessity of polysulfide inhibition and the application of Nb2CTx MXene in PEO-based electrolytes for all-solid-state Li-S batteries.

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摘要

全固态锂硫电池兼具高能量密度和高安全性，有望成为下一代新型电池体系。聚环氧乙烷(PEO)固态电解质加工性能好、解离锂盐能力强、电压窗口能很好兼容锂硫电池，但PEO室温离子电导率低，电池运行需要在熔融温度下，造成部分多硫离子的溶解与穿梭。本文提出了一种“一石二鸟”的策略，通过二维Nb2CTx MXene纳米片填充PEO电解质，同时提高PEO传导Li+和吸附多硫离子抑制其穿梭的能力。二维Nb2CTx纳米片的尺寸大小对渗流效应具有重要影响，进而决定了Li+传导能力和多硫离子吸附的改善效果。通过真空条件下高功率超声处理调节Nb2CTx纳米片尺寸，随着片径从500 nm减小到100 nm以下，60℃下PEO/ Nb2CTx 复合电解质的离子电导率提高到了2.62×10−4 S·cm−1, Li+迁移数提高到0.37。此外，理论计算和X射线光电子能谱(XPS)分析表明Nb2CTx纳米片通过形成Nb‒S键有效吸附多硫离子，抑制其在熔融PEO中的穿梭。所组装全固态锂硫扣式电池在0.5C下的初始容量为1149 mA·g−1，循环200圈后的可逆容量为491 mAh·g−1，与未改性的PEO电解质相比改善明显。

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Acknowledgements

This work was financially supported by the State Key Laboratory of Powder Metallurgy, Hunan Provincial Natural Science Foundation of China (No. 2020JJ4107), the Innovation-Driven Project of Central South University (No. 2020CX037), the Postgraduate Scientific Research Innovation Project of Hunan Province (No. QL20220021), the National Natural Science Foundation of China (No. 51802352) and the Science and Technology Innovation Leading Project of High-Tech Industry of Hunan Province, China (No. 2020GK2067).

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  1. Si-Ming Liu and Meng-Xun Chen have contributed equally to this work.

Authors and Affiliations

  1. State Key Laboratory for Powder Metallurgy, College of Chemistry and Chemical Engineering, Central South University, Changsha, 410083, China

    Si-Ming Liu, Meng-Xun Chen, Ying Xie, Xiang Xiong & Kai Han

  2. Shinghwa Advanced Material Group Co., Ltd, Dongying, 257500, China

    Deng-Hua Liu

  3. School of Physics and Electronics, Central South University, Changsha, 410083, China

    Jin-Fei Zheng & Heng Luo

  4. Department of Chemistry, Oregon State University, Corvallis, OR 97331-4003, USA

    Heng Jiang

  5. School of Geosciences and Info-Physics, Central South University, Changsha, 410083, China

    Li-Chang Wang

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Liu, SM., Chen, MX., Xie, Y. et al. Nb2CTx MXene boosting PEO polymer electrolyte for all-solid-state Li-S batteries: two birds with one stone strategy to enhance Li+ conductivity and polysulfide adsorptivity. Rare Met. 42, 2562–2576 (2023). https://doi.org/10.1007/s12598-022-02260-2

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