Regulating the nanoscale interfacial solvation structure involving ion coordination in the electric double layer is of significant importance for the construction of a stable and rapid ion-transport solid–electrolyte interface for revolutionary lithium metal batteries (LMBs) operated under low-temperature serving conditions. Herein, an efficient strategy involving the use of PMETAC polymer brushes to regulate the nanoscale interfacial solvation structure is proposed, which is universal to different electrolyte chemistries and operating temperatures. Combined attenuated total reflection analysis and theoretical simulations revealed the unique interfacial solvation structure and the underlying synergistic mechanism. Owing to the electrostatic interaction between the quaternary amino nitrogen of the polymer brushes and electrolyte anions, as well as the unique steric hindrance effect originating from the polymer brushes, solvent molecules were excluded from the first inner solvation shell and more anions entered the electric double layer to participate in Li-ion coordination, thus prompting the formation of a stable inorganic-rich SEI with favorable ion transport. With the unique nanoscale interfacial solvation structure, the assembled LMBs achieved stable operation at room temperature for over 1.7 years and at a low temperature of −20 °C. More excitingly, the strategy could support the industrial manufacturing of Ah-level anode-free Li metal pouch cells. This work reveals the importance of regulating the nanoscale interfacial solvation structure, promoting the realistic applications of high-energy LMBs for operation under various service conditions.

中文翻译：

---

低温锂金属电池定制纳米级界面溶剂化结构


调控双电层中涉及离子配位的纳米级界面溶剂化结构对于在低温使用条件下运行的革命性锂金属电池（LMB）构建稳定且快速的离子传输固体电解质界面具有重要意义。在此，提出了一种使用 PMETAC 聚合物刷来调节纳米级界面溶剂化结构的有效策略，该策略适用于不同的电解质化学和工作温度。衰减全反射分析和理论模拟相结合揭示了独特的界面溶剂化结构和潜在的协同机制。由于聚合物刷的季氨基氮与电解质阴离子之间的静电相互作用，以及聚合物刷独特的空间位阻效应，溶剂分子被排除在第一内溶剂化壳之外，更多的阴离子进入双电层参与锂离子配位，从而促进形成具有有利离子传输的稳定的富含无机物的SEI。凭借独特的纳米级界面溶剂化结构，组装的LMB在室温和-20℃的低温下实现了超过1.7年的稳定运行。更令人兴奋的是，该策略可以支持Ah级无阳极锂金属​​软包电池的工业制造。这项工作揭示了调控纳米级界面溶剂化结构的重要性，促进了高能LMB在各种使用条件下的实际应用。