Next-generation batteries demand solid polymer electrolytes (SPEs) with rapid ion transport and robust mechanical properties. However, many SPEs with liquid-like Li⁺ transport mechanisms suffer a fundamental trade-off between conductivity and strength. Dynamic polymer networks can improve bulk mechanics with minimal impact to segmental relaxation or ionic conductivity. This study demonstrates a system where a single polymer-bound ligand simultaneously dissociates Li⁺ and forms long-lived Ni²⁺ networks. The polymer comprises an ethylene oxide backbone and imidazole (Im) ligands, blended with Li⁺ and Ni²⁺ salts. Ni²⁺–Im dynamic cross-links result in the formation of a rubbery plateau resulting in, consequently, storage modulus improvement by a factor of 133× with the introduction of Ni²⁺ at r_Ni = 0.08, from 0.014 to 1.907 MPa. Even with Ni²⁺ loading, the high Li⁺ conductivity of 3.7 × 10^–6 S/cm is retained at 90 °C. This work demonstrates that decoupling of ion transport and bulk mechanics can be readily achieved by the addition of multivalent metal cations to polymers with chelating ligands.

中文翻译：

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提高机械强度而不牺牲聚合物电解质中的锂离子传输


下一代电池需要具有快速离子传输和强大机械性能的固体聚合物电解质（SPE）。然而，许多具有类液体Li ⁺ 传输机制的SPE在电导率和强度之间存在根本性的权衡。动态聚合物网络可以改善整体力学，同时对链段弛豫或离子电导率的影响最小。这项研究展示了一个系统，其中单个聚合物结合的配体同时解离 Li ⁺ 并形成长寿命的 Ni ²⁺ 网络。该聚合物包含环氧乙烷主链和咪唑(Im)配体，并与Li ⁺ 和Ni ²⁺ 盐混合。 Ni ²⁺ –Im 动态交联导致橡胶平台的形成，因此，随着在 r 处引入 Ni ²⁺ ，储能模量提高了 133 倍 _Ni = 0.08，从 0.014 到 1.907 MPa。即使负载了 Ni ²⁺ ，在 90 °C 时仍保持 3.7 × 10 ^–6 S/cm 的高 Li ⁺ 电导率。这项工作表明，通过将多价金属阳离子添加到具有螯合配体的聚合物中，可以轻松实现离子传输和体积力学的解耦。