Rechargeable magnesium batteries (RMBs) have emerged as one of the promising energy storage devices, and polymer electrolytes with high safety, stability, and structural flexibility are the ideal choice for RMBs. Herein, a novel in situ crosslinked gel polymer electrolyte, PDTE is reported, via facile ring‐opening polymerization in RMBs. The electrolyte exhibits a remarkable room‐temperature ionic conductivity of 2.8 × 10−4 S cm−1 and highly reversible Mg plating/stripping behavior (98.9% Coulombic efficiency, 2000 cycles) with a low overpotential (<0.1 V). Mo6S8||PDTE||Mg coin cells demonstrate exceptional cycling stability and rate capability at a wide temperature range (−20 to 50 °C), characterizing an average discharge capacity of 81.6 mAh g−1 at 10 C for 7500 cycles at room temperature, and 97.4 and 111.7 mAh g−1 at 0.2 C for 400 and 50 cycles at −20 and 50 °C, respectively. The pouch cell exhibits a high energy density of 204 Wh kg−1 with a high retention of 90.6% at 0.2 C for 350 cycles, along with significantly improved safety and remarkable flexibility. Additionally, good compatibility with conversion‐type cathode Cu3Se2 validates the application versatility of PDTE. The development of this gel polymer electrolyte provides a feasible approach for the research on semi‐solid‐state electrolytes for RMBs.

中文翻译：

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基于简单的原位开环聚合的凝胶聚合物电解质可实现高性能可充电镁电池


可充电镁电池（RMB）已成为最有前途的储能装置之一，而具有高安全性、稳定性和结构灵活性的聚合物电解质是RMB的理想选择。本文报道了一种新型原位交联凝胶聚合物电解质，PDTE，通过在人民币中进行轻松的开环聚合。该电解质表现出显着的室温离子电导率（2.8 × 10−4 S cm−1）和高度可逆的镁电镀/剥离行为（98.9％库仑效率，2000次循环）和低过电势（<0.1 V）。 Mo6S8||PDTE||Mg纽扣电池在较宽的温度范围（-20至50°C）下表现出出色的循环稳定性和倍率性能，在室温下10 C下7500次循环的平均放电容量为81.6 mAh g−1 ，0.2 C 下分别为 97.4 和 111.7 mAh g−1，在 -20 和 50 °C 下循环 400 次和 50 次。该软包电池具有 204 Wh kg−1 的高能量密度，在 0.2 C 下循环 350 次后仍具有 90.6% 的高保留率，同时显着提高了安全性和显着的灵活性。此外，与转换型阴极 Cu3Se2 的良好兼容性验证了 PDTE 的应用多功能性。这种凝胶聚合物电解质的开发为人民币半固态电解质的研究提供了可行的途径。