Xu Nuo, Song Xingchen, Sun Guolin, Zhang Jinping, Quan Zuhao, Lou Genglin, Li Aihong, Li Chenxi, Zhang Hongtao, Chen Yongsheng
The Centre of Nanoscale Science and Technology and Key Laboratory of Functional Polymer Materials, Institute of Polymer Chemistry, College of Chemistry, Nankai University, Tianjin 300071, China.
Renewable Energy Conversion and Storage Center (RECAST), Nankai University, Tianjin 300071, China.
J Am Chem Soc. 2026 Jan 21;148(2):2471-2480. doi: 10.1021/jacs.5c17294. Epub 2026 Jan 6.
Lithium metal batteries (LMBs) are regarded as the "holy grail" of next-generation energy storage systems due to their potential for high energy density. However, uncontrolled lithium dendrite growth on lithium metal anodes leads to poor cycling stability and serious safety risks, hindering their practical deployment. Herein, we design an polymerized POSS-based gel polymer electrolyte (POSS-GPE) that exhibits high ionic conductivity (3.04 mS cm at room temperature), excellent oxidative stability (>4.9 V vs Li/Li), broad compatibility with diverse electrode materials, and intrinsic flame retardancy. The POSS-GPE establishes an anion-rich solvation environment that promotes the formation of robust, anion-derived electrode-electrolyte interphase on both the cathode and anode, thus mitigating interfacial degradation. As a result, LiNiCoMnO|POSS-GPE|Li (50 μm) full cell delivers long-term cycling stability of 500 cycles with 87.3% capacity retention. Furthermore, a 6.08 Ah pouch cell with lean electrolyte (1.40 g Ah) achieves a remarkable energy density of 511.2 Wh kg and cycles stably for 70 cycles at 4.6 V, representing the best balance between cycling performance and energy density for polymer-electrolyte-based LMBs. The high-energy-density pouch cells also demonstrate superior safety in nail-penetration tests. This work presents a promising strategy for developing practical high-energy-density and high-safety LMBs.
锂金属电池（LMBs）因其具有高能量密度的潜力，被视为下一代储能系统的“圣杯”。然而，锂金属阳极上不受控制的锂枝晶生长会导致循环稳定性差和严重的安全风险，阻碍了它们的实际应用。在此，我们设计了一种基于聚合倍半硅氧烷（POSS）的凝胶聚合物电解质（POSS-GPE），它具有高离子电导率（室温下为3.04 mS cm）、优异的氧化稳定性（相对于Li/Li>4.9 V）、与多种电极材料的广泛兼容性以及固有的阻燃性。POSS-GPE建立了一个富含阴离子的溶剂化环境，促进了在阴极和阳极上形成坚固的、源自阴离子的电极-电解质界面，从而减轻了界面降解。结果，LiNiCoMnO|POSS-GPE|Li（50μm）全电池在500次循环中具有长期循环稳定性，容量保持率为87.3%。此外，一个具有贫电解质（1.40 g Ah）的6.08 Ah软包电池实现了511.2 Wh kg的显著能量密度，并在4.6 V下稳定循环70次，代表了基于聚合物电解质的LMBs在循环性能和能量密度之间的最佳平衡。高能量密度软包电池在针刺测试中也表现出卓越的安全性。这项工作为开发实用的高能量密度和高安全性LMBs提出了一种有前景的策略。
