High ionic conductivity is a prerequisite for the application of solid-state polymer electrolyte towards the safe and high energy density electrochemical devices. Here we report the preparation and properties of an in-situ polymerized comb-like copolymer-based SPE (PLA/PEG-SPE) with high ionic conductivity from methyl acrylate functionalized poly(D,L-Lactide) (PLAMA) and poly(ethylene glycol) methyl ether methacrylate (PEGMA). A remarkably high ionic conductivity value of 6.9 × 10⁻⁵ S cm⁻¹ at ambient temperature and a maximum ionic conductivity of 4.3 × 10⁻⁴ S cm⁻¹ at 60°C were detected, with an activation energy of 0.2 eV and a Li⁺ transference number (t_Li⁺) of 0.36. The PLA/PEG-SPE exhibits a wide electrochemical stability window up to 4.6 vs. Li/Li⁺ and very good lithium metal electrode compatibility. Solid-state LiFePO₄/SPE/Li cells with integrated cathode and lithium metal deliver superior cycling stability with high discharge capacities (149 mAh g⁻¹ as the initial specific capacity) and high capacity retention (exceeded 82% of its initial specific capacity) at 0.2 C at 60°C. The solid-state cells are also capable of being cycled at room temperature at 0.2 C. This work highlights a facile, in-situ fabrication strategy involving a vinyl-functionalized PLA precursor that yields a high-performance ion-conducting membrane attractive for lithium metal battery applications.

中文翻译：

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用于锂金属电池的原位聚合梳状PLA / PEG基固体聚合物电解质

高离子电导率是将固态聚合物电解质应用于安全和高能量密度电化学装置的先决条件。在这里，我们报道了由丙烯酸甲酯官能化的聚（D，L-丙交酯）（PLAMA）和聚（乙烯）组成的具有高离子电导率的原位聚合的梳状共聚物基固相萃取（PLA / PEG-SPE）的制备和性能二醇）甲基丙烯酸甲酯（PEGMA）。在室温下的离子电导率值非常高，为6.9×10 ^-5 S cm ^-1，在60°C时的最大离子电导率是4.3×10 ^-4 S cm ^-1，活化能为0.2 eV，且Li ⁺转移数（t _Li ⁺）的0.36。与Li / Li ⁺相比，PLA / PEG-SPE具有高达4.6的宽电化学稳定性窗口，并且与锂金属电极的相容性非常好。具有集成阴极和锂金属的固态LiFePO ₄ / SPE / Li电池具有出色的循环稳定性，具有高放电容量（初始比容量149 mAh g ^-1）和高容量保持率（超过其初始比容量的82％）在60°C下于0.2 C下。固态电池还能够在室温下于0.2 C循环。这项工作强调了一种简便的原位制造策略，该策略涉及乙烯基官能化的PLA前驱体，该前驱体产生了对锂金属有吸引力的高性能离子导电膜电池应用。