Energy Storage Materials ( IF 18.9 ) Pub Date : 2023-02-12 , DOI: 10.1016/j.ensm.2023.02.012
Jie Zhu , Jinping Zhang , Ruiqi Zhao , Yang Zhao , Jie Liu , Nuo Xu , Xiangjian Wan , Chenxi Li , Yanfeng Ma , Hongtao Zhang , Yongsheng Chen
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The commercialization of lithium metal batteries (LMBs) highly relies on developing high-performance solid electrolytes, which should possess high Li+ conductivity comparable to liquid electrolytes, efficient suppression of dendrite growth, nonflammability, intimate electrode/electrolyte contact, and compatibility with the state-of-art lithium batteries industrial fabrication. Herein, we develop an in situ crosslinking method via cationic ring-opening polymerization (CROP) using a four-armed cross-linker and fabricate a crosslinked gel polymer electrolyte (c-GPE), where the more densely and efficiently three-dimensional (3D) crosslinked polymer network renders the c-GPE high solvent uptake and improved oxidative stability. Moreover, the strong interaction between the crosslinked polymer network and the solvent is proved to reduce the desolvation energy barrier of Li+, which facilitates homogeneous Li+ deposition. Thus, the Li||LiFePO4 battery with this in situ fabricated c-GPE demonstrates one of the longest lifespans among polymer electrolyte-based batteries at high rate (2C) so far (2000 cycles with 78% retention). Furthermore, when this in situ 3D crosslinked gel polymer electrolyte is applied together with high voltage cathode material Ni0.6Mn0.2Co0.2O2, the Li|c-GPE|Ni0.6Mn0.2Co0.2O2 battery could deliver the best cycling performance with high nonflammability among CROP-based batteries so far (300 cycles with 80% retention). These results demonstrate that by the dedicated design of in situ polymerization, a high-performance c-GPE could be achieved to meet the requirements for practical, safe, and high-energy-density LMBs.
中文翻译:
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用于超长循环、高电压和高安全性锂金属电池的原位 3D 交联凝胶聚合物电解质
锂金属电池 (LMB) 的商业化高度依赖于开发高性能固体电解质,其应具有与液体电解质相当的高 Li +电导率、有效抑制枝晶生长、不易燃、电极/电解质接触紧密以及与状态相容-最先进的锂电池工业制造。在这里,我们开发了一个原位使用四臂交联剂通过阳离子开环聚合 (CROP) 交联方法并制造交联凝胶聚合物电解质 (c-GPE),其中更密集和更有效的三维 (3D) 交联聚合物网络呈现 c -GPE 高溶剂吸收和改进的氧化稳定性。此外,交联聚合物网络与溶剂之间的强相互作用被证明可以降低 Li +的去溶剂化能垒,从而促进 Li + 的均匀沉积。因此,具有这种原位的Li||LiFePO 4电池制造的 c-GPE 展示了迄今为止高倍率 (2C) 聚合物电解质电池中寿命最长的电池之一(2000 次循环,保留率为 78%)。此外,当这种原位3D 交联凝胶聚合物电解质与高压正极材料 Ni 0.6 Mn 0.2 Co 0.2 O 2一起应用时,Li|c-GPE|Ni 0.6 Mn 0.2 Co 0.2 O 2电池可提供最佳循环性能迄今为止,在基于 CROP 的电池中具有较高的不易燃性(300 次循环,保留率为 80%)。这些结果表明,通过原位的专门设计通过聚合,可以获得高性能的c-GPE,以满足实用、安全和高能量密度LMBs的要求。