Xu Ruizhe, Hu Anjun, Xu Wang, Yang Wei, Li Fei, Li Yuanjian, Mu Yongbiao, Zeng Lin, Long Jianping, Chen Shimou
College of Materials and Chemistry & Chemical Engineering (College of Lithium Resources and Lithium Battery Industry), Chengdu University of Technology, Chengdu, 610059, P.R. China.
School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu, 610054, P.R. China.
Angew Chem Int Ed Engl. 2025 Sep 10:e202513321. doi: 10.1002/anie.202513321.
Lithium metal batteries (LMBs) have emerged as the most promising candidate for next-generation high-energy-density energy storage systems. However, their practical implementation is hindered by the inability of conventional carbonate electrolytes to simultaneously stabilize the lithium metal anode and LiNiCoMnO (NCM811) cathode interfaces, particularly under extreme operating conditions. Herein, we present a transformative molecular design using 3,5-difluorophenylboronic acid neopentyl glycol ester (DNE), which uniquely integrates dual interfacial stabilization mechanisms in a single molecule. Unlike conventional additives, DNE's Lewis acidic B─O bonds chemically anchor PF anions, reconstructing the Li solvation sheath to enable a lithium fluoride-rich solid electrolyte interphase that suppresses dendrites and lithium dendrite growth. Simultaneously, its cyclic borate ester undergoes in situ polymerization on the cathode surface, forming a transition metal ion-trapping network that optimizes the cathode electrolyte interphase and mitigates structural degradation in NCM811 cathodes. This synergistic dual-action mechanism endows Li||NCM811 cells with exceptional cycling stability under extreme conditions (4.7 V, 60 °C, and 5 C). Furthermore, a 1 Ah pouch cell with an energy density of 331 Wh kg maintains 98.8% capacity retention after 100 cycles. This dual-interface molecular anchoring strategy establishes a design paradigm for developing high-performance LMBs suitable for operations in extreme conditions.
锂金属电池（LMBs）已成为下一代高能量密度储能系统最有前景的候选者。然而，传统碳酸盐电解质无法同时稳定锂金属负极和LiNiCoMnO（NCM811）正极界面，这阻碍了它们的实际应用，尤其是在极端操作条件下。在此，我们提出了一种使用3,5-二氟苯硼酸新戊二醇酯（DNE）的变革性分子设计，它在单个分子中独特地整合了双重界面稳定机制。与传统添加剂不同，DNE的路易斯酸性B─O键化学锚定PF阴离子，重构锂溶剂化鞘层，形成富含氟化锂的固体电解质界面层，抑制枝晶和锂枝晶生长。同时，其环状硼酸酯在正极表面原位聚合，形成过渡金属离子捕获网络，优化正极电解质界面，减轻NCM811正极的结构退化。这种协同双作用机制使Li||NCM811电池在极端条件（4.7 V、60°C和5 C）下具有出色的循环稳定性。此外，一个能量密度为331 Wh kg的1 Ah软包电池在100次循环后保持98.8%的容量保持率。这种双界面分子锚定策略为开发适用于极端条件下运行的高性能LMBs建立了一种设计范例。
