Despite the theoretical promise of attaining high energy densities, practical applications of lithium metal batteries (LMBs) remain hindered by the inadequacies of the electrode/electrolyte interface and unsatisfied cycling stability. Herein, a self-adsorption molecule with polar groups was designed and introduced in ether electrolyte, aiming to form a high-density and ordered molecular layer occupying active sites on the electrode surface, while restricting electrolyte molecule penetration into the interface. This self-adsorption molecule favors the formation of a robust anion-rich cathode/anode electrolyte interphase due to the change of the interfacial solvation structure, thus inhibiting solvent decomposition and enhancing interfacial stability. Consequently, the addition of this molecule into low-concentration ether electrolytes notably upgrades the electrochemical performance of the LiNi_0.8Co_0.1Mn_0.1O₂ (NCM811)||Li battery, which enables a high capacity retention of 87.2% after 250 cycles at 4.5 V. Moreover, the NMC811||Li pouch cells achieve stable cycling over 150 cycles with a capacity retention of 92.9% at a low negative/positive capacity ratio of 2.7 with a lean electrolyte. This interface passivation design strategy provides a promising path toward high-energy, durable, and safe rechargeable LMBs.

中文翻译：

---

自吸附分子钝化界面可实现高效稳定的锂金属电池


尽管理论上有望实现高能量密度，但锂金属电池 （LMB） 的实际应用仍然受到电极/电解质界面不足和循环稳定性不满足的阻碍。在此，设计了一种具有极性基团的自吸附分子并将其引入醚电解质中，旨在形成一个高密度有序的分子层，占据电极表面的活性位点，同时限制电解质分子渗透到界面中。由于界面溶剂化结构的变化，这种自吸附分子有利于形成强大的富含阴离子的阴极/阳极电解质界面，从而抑制溶剂分解并增强界面稳定性。因此，将该分子添加到低浓度醚电解质中显着提升了 LiNi_0.8Co_0.1Mn_0.1O₂ （NCM811）||锂电池，在 4.5 V 下循环 250 次后可实现 87.2% 的高容量保持率。此外，NMC811||锂软包电池在 2.7 的负/正容量比和 2.7 的稀电解质下实现了超过 150 次循环的稳定循环，容量保持率为 92.9%。这种界面钝化设计策略为实现高能量、耐用和安全的可充电 LMB 提供了一条有前途的道路。