Solid-state polymer lithium batteries have great potential in flexible/wearable electronics, however, it still has been struggling with insufficient mechanical properties of polymer electrolytes, which have great possibility to result in safety issues in the abuse condition. Herein, we present a poly(vinylene carbonate)-based cross-linked network as a promising polymer platform via a rigid-flexible coupling polymer design for lithium battery applications, which is versatile for high performance electrolyte and binder. The as-prepared cross-linked network polymer is prepared by the nucleophilic attack of flexible polyoxyethylene bis(amine) and oxidation-resistant aminopropionitrile to rigid poly(vinylene carbonate) framework. This reaction chemistry shows a facile, fast solidification of electrolyte precursor solutions without the employment of any initiators. It is demonstrated that the resultant solid polymer electrolyte with this cross-linked network polymer presents excellent mechanical properties without any supporting materials, with a tensile strength of 22 MPa and an elongation-at-break value of 350%. Furthermore, it exhibits excellent thermal stabilities, decent ionic conductivities, good compatibility with electrodes especially lithium metal anode. Benefited from these merits, excellent cycling performance of 4.3 V-class LiCoO₂/Li cell under 60 °C can be achieved, with a capacity retention of 80% after 150 cycles at 0.5 C. More striking, employing this cross-linked network polymer as both the electrolyte host and electrode binder, lithium batteries exhibit superior cycle performance at both ambient and high temperatures. This work indicates that the as-prepared cross-linked network polymer can serve as a polymer platform, which can provide high performance electrolyte and binder that are urgently needed for lithium batteries.

固态聚合物锂电池在柔性/可穿戴电子产品领域具有巨大的潜力，但其仍面临聚合物电解质机械性能不足的问题，在滥用状态下极有可能导致安全问题。在这里，我们通过用于锂电池应用的刚柔耦合聚合物设计，提出了一种基于聚（碳酸亚乙烯酯）的交联网络作为一种有前途的聚合物平台，该聚合物可用于高性能电解质和粘合剂。所制备的交联网络聚合物是通过柔性聚氧乙烯双胺和抗氧化氨基丙腈对刚性聚碳酸亚乙烯酯骨架的亲核攻击而制备的。这种反应化学显示出一种简单的、电解质前体溶液的快速凝固，无需使用任何引发剂。结果表明，使用这种交联网络聚合物制备的固体聚合物电解质在没有任何支撑材料的情况下表现出优异的机械性能，拉伸强度为 22 MPa，断裂伸长率为 350%。此外，它还表现出优异的热稳定性、良好的离子电导率、与电极特别是锂金属负极的良好相容性。得益于这些优点，4.3 V 级 LiCoO 的优异循环性能 此外，它还表现出优异的热稳定性、良好的离子电导率、与电极特别是锂金属负极的良好相容性。得益于这些优点，4.3 V 级 LiCoO 的优异循环性能 此外，它还表现出优异的热稳定性、良好的离子电导率、与电极特别是锂金属负极的良好相容性。得益于这些优点，4.3 V 级 LiCoO 的优异循环性能₂ /Li 电池可在 60 °C 下实现，在 0.5 C 下循环 150 次后容量保持率为 80%。更引人注目的是，采用这种交联网络聚合物作为电解质主体和电极粘合剂，锂电池表现出优异的循环性能在环境和高温下的性能。这项工作表明，所制备的交联网络聚合物可以作为聚合物平台，可以提供锂电池急需的高性能电解质和粘合剂。