A core–shell additive with anionic Keggin-type polyoxometalate (POM) cluster as core and N-containing cation of ionic liquid (IL) as shell is proposed to stabilize Li-metal batteries (LMBs). The suspended POM derived complex in ether-based electrolyte is absorbed around the protuberances of anode and triggers a lithiophobic repulsion mechanism for the homogenization of Li⁺ redistribution. The gradually released POM cores with negative charge then enrich Li⁺ and co-assemble with Li. The Li⁺ repulsion-enrichment synergism can compact Li deposition and reinforce solid electrolyte interphase. This sustained-release additive enables Li∥Li symmetric cells with a long lifetime over 500 h and 300 h at high current densities of 3 and 5 mA cm⁻² respectively. The complex additive is also compatible with high-voltage Li∥LiNi_0.8Co_0.15Al_0.05O₂ (NCA) cells. Even with a NCA loading as high as ca. 20 mg cm⁻², the additive contained Li∥NCA cell can still cycle for over 100 cycles at 2.6 mA cm⁻².

中文翻译：

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核壳离子复合物诱导的锂离子排斥-富集协同作用使高负载锂金属电池成为可能

提出了一种以阴离子 Keggin 型多金属氧酸盐 (POM) 簇为核、离子液体 (IL) 的含氮阳离子为壳的核壳添加剂，以稳定锂金属电池 (LMB)。醚基电解质中悬浮的 POM 衍生复合物被吸收在阳极的突起周围，并触发疏锂排斥机制，使 Li ⁺再分布均质化。逐渐释放的带负电荷的 POM 核富集 Li ⁺并与 Li 共组装。Li ⁺排斥-富集协同作用可以压缩锂沉积并增强固体电解质界面。这种缓释添加剂使 Li∥Li 对称电池在 3 和 5 mA cm ^{-2 的}高电流密度下具有超过 500 小时和 300 小时的长寿命分别。该复合添加剂还与高压 Li∥LiNi _0.8 Co _0.15 Al _0.05 O ₂ (NCA) 电池兼容。即使 NCA 负载高达约。20 mg cm ^{-2 时}，含有添加剂的 Li∥NCA 电池仍可在 2.6 mA cm ^{-2 下}循环超过 100 个循环。