Lithium‐metal batteries (LMBs) with high energy densities are highly desirable for energy storage, but generally suffer from dendrite growth and side reactions in liquid electrolytes; thus the need for solid electrolytes with high mechanical strength, ionic conductivity, and compatible interface arises. Herein, a thiol‐branched solid polymer electrolyte (SPE) is introduced featuring high Li⁺ conductivity (2.26 × 10⁻⁴ S cm⁻¹ at room temperature) and good mechanical strength (9.4 MPa)/toughness (≈500%), thus unblocking the tradeoff between ionic conductivity and mechanical robustness in polymer electrolytes. The SPE (denoted as M‐S‐PEGDA) is fabricated by covalently cross‐linking metal–organic frameworks (MOFs), tetrakis (3‐mercaptopropionic acid) pentaerythritol (PETMP), and poly(ethylene glycol) diacrylate (PEGDA) via multiple CSC bonds. The SPE also exhibits a high electrochemical window (>5.4 V), low interfacial impedance (<550 Ω), and impressive Li⁺ transference number (t_Li+ = 0.44). As a result, Li||Li symmetrical cells with the thiol‐branched SPE displayed a high stability in a >1300 h cycling test. Moreover, a Li|M‐S‐PEGDA|LiFePO₄ full cell demonstrates discharge capacity of 143.7 mAh g⁻¹ and maintains 85.6% after 500 cycles at 0.5 C, displaying one of the most outstanding performances for SPEs to date.

中文翻译：

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硫醇支化的固体聚合物电解质，具有高强度，韧性和锂离子电导率，适用于锂金属电池。

高能量密度的锂金属电池（LMB）非常适合用于储能，但通常会出现枝晶生长和液体电解质中的副反应的问题。因此，需要具有高机械强度，离子电导率和相容界面的固体电解质。本文介绍了具有高Li ⁺电导率（2.26×10 ^-4 S cm ^-1）的硫醇支化固体聚合物电解质（SPE）在室温下）和良好的机械强度（9.4 MPa）/韧性（≈500％），从而消除了离子电导率与聚合物电解质机械强度之间的折衷。SPE（表示为M‐S‐PEGDA）是通过金属-有机骨架（MOF），四（3-巯基丙酸）季戊四醇（PETMP）和聚（乙二醇）二丙烯酸酯（PEGDA）共价交联制备的ç 小号 C键。SPE还具有较高的电化学窗口（> 5.4 V），较低的界面阻抗（<550Ω）和令人印象深刻的Li ⁺迁移数（t _{Li +} = 0.44）。结果，具有硫醇支化SPE的Li || Li对称电池在> 1300 h的循环测试中显示出很高的稳定性。此外，Li | M‐S‐PEGDA | LiFePO_4个完整电池的放电容量为143.7 mAh g ^-1，在0.5 C下经过500次循环后仍保持85.6％，这是迄今为止SPE最杰出的性能之一。