Lian Shuang, Wang Yu, Ji Haifeng, Zhang Xiaojie, Shi Jingjing, Feng Yi, Qu Xiongwei
Hebei Key Laboratory of Functional Polymers, Department of Polymer Materials and Engineering, Hebei University of Technology, 8 Guangrong Street, Tianjin 300130, China.
School of Science, Nantong University, Nantong 226019, Jiangsu, China.
Nanomaterials (Basel). 2021 Sep 29;11(10):2562. doi: 10.3390/nano11102562.
The development of solid-state polymer electrolytes is an effective way to overcome the notorious shuttle effect of polysulfides in traditional liquid lithium sulfur batteries. In this paper, cationic cyclopropenium based cross-linked polymer was firstly prepared with the one pot method, and then the counter ion was replaced by TFSI anion using simple ion replacement. Cationic cyclopropenium hyper-crosslinked polymer (HP) was introduced into a polyethylene oxide (PEO) matrix with the solution casting method to prepare a composite polymer electrolyte membrane. By adding HP@TFSI to the PEO-based electrolyte, the mechanical and electrochemical properties of the solid-state lithium-sulfur batteries were significantly improved. The PEO-20%HP@TFSI electrolyte shows the highest Li ionic conductivity at 60 °C (4.0 × 10 S·cm) and the highest mechanical strength. In the PEO matrix, uniform distribution of HP@TFSI inhibits crystallization and weakens the interaction between each PEO chain. Compared with pure PEO/LiTFSI electrolyte, the PEO-20%HP@TFSI electrolyte shows lower interface resistance and higher interface stability with lithium anode. The lithium sulfur battery based on the PEO-20%HP@TFSI electrolyte shows excellent electrochemical performance, high Coulombic efficiency and high cycle stability. After 500 cycles, the capacity of the lithium-sulfur battery based on PEO-20%HP@TFSI electrolytes keeps approximately 410 mAh·g at 1 C, the Coulomb efficiency is close to 100%, and the cycle capacity decay rate is 0.082%.
固态聚合物电解质的发展是克服传统液态锂硫电池中多硫化物臭名昭著的穿梭效应的有效途径。本文首先采用一锅法制备了基于阳离子环丙烯鎓的交联聚合物，然后通过简单的离子置换将抗衡离子替换为TFSI阴离子。采用溶液浇铸法将阳离子环丙烯鎓超交联聚合物（HP）引入聚环氧乙烷（PEO）基体中，制备了复合聚合物电解质膜。通过向基于PEO的电解质中添加HP@TFSI，固态锂硫电池的机械性能和电化学性能得到了显著改善。PEO-20%HP@TFSI电解质在60℃时表现出最高的锂离子电导率（4.0×10 S·cm）和最高的机械强度。在PEO基体中，HP@TFSI的均匀分布抑制了结晶并削弱了各PEO链之间的相互作用。与纯PEO/LiTFSI电解质相比，PEO-20%HP@TFSI电解质与锂负极的界面电阻更低，界面稳定性更高。基于PEO-20%HP@TFSI电解质的锂硫电池表现出优异的电化学性能、高库仑效率和高循环稳定性。经过500次循环后，基于PEO-20%HP@TFSI电解质的锂硫电池在1 C下的容量保持在约410 mAh·g，库仑效率接近100%，循环容量衰减率为0.082%。
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