Interfacial self-healing polymer electrolytes for long-cycle solid-state lithium-sulfur batteries

Interfacial self-healing polymer electrolytes for long-cycle solid-state lithium-sulfur batteries

08 January 2024 | Fei Pei, Lin Wu, Yi Zhang, Yaqi Liao, Qi Kang, Yan Han, Huangwei Zhang, Yue Shen, Henghui Xu, Zhen Li & Yunhui Huang
A poly(ether-urethane)-based solid-state polymer electrolyte with self-healing capability is developed to enhance the performance of solid-state lithium-sulfur (Li-S) batteries. This electrolyte, composed of dynamic covalent disulfide bonds and hydrogen bonds, exhibits excellent interfacial self-healing properties, reducing interfacial resistance and improving the stability of the battery. The self-healing ability enables the electrolyte to repair defects at the interface between the solid-state polymer electrolyte and the electrodes, leading to better interfacial contact and enhanced electrochemical performance. The electrolyte is integrated with the electrodes to form a dual-integrated structure, which significantly improves the cycling stability and rate performance of the battery. The Li||Li symmetric cells exhibit stable long-term cycling for over 6000 hours, and the solid-state Li-S battery shows a prolonged cycling life of 700 cycles at 0.3 C. The use of ultrasound imaging technology confirms that the interfacial contact in the integrated structure is much better than in traditional laminated structures. The electrolyte also demonstrates high ionic conductivity, a high Li+ transference number, and excellent electrochemical stability. The self-healing electrolyte effectively suppresses Li dendrite growth and polysulfide shuttling, leading to improved cycling stability and capacity retention. The study provides a promising strategy for designing high-performance solid-state Li-S batteries with enhanced safety and energy density.A poly(ether-urethane)-based solid-state polymer electrolyte with self-healing capability is developed to enhance the performance of solid-state lithium-sulfur (Li-S) batteries. This electrolyte, composed of dynamic covalent disulfide bonds and hydrogen bonds, exhibits excellent interfacial self-healing properties, reducing interfacial resistance and improving the stability of the battery. The self-healing ability enables the electrolyte to repair defects at the interface between the solid-state polymer electrolyte and the electrodes, leading to better interfacial contact and enhanced electrochemical performance. The electrolyte is integrated with the electrodes to form a dual-integrated structure, which significantly improves the cycling stability and rate performance of the battery. The Li||Li symmetric cells exhibit stable long-term cycling for over 6000 hours, and the solid-state Li-S battery shows a prolonged cycling life of 700 cycles at 0.3 C. The use of ultrasound imaging technology confirms that the interfacial contact in the integrated structure is much better than in traditional laminated structures. The electrolyte also demonstrates high ionic conductivity, a high Li+ transference number, and excellent electrochemical stability. The self-healing electrolyte effectively suppresses Li dendrite growth and polysulfide shuttling, leading to improved cycling stability and capacity retention. The study provides a promising strategy for designing high-performance solid-state Li-S batteries with enhanced safety and energy density.
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