Fabricating interfacial layers with high lithiophilicity and rapid Li+ transfer function is critical for dendrite-free lithium deposition in lithium-metal batteries (LMBs). Herein, a two-dimensional coordination network NKU-2000 with ordered lithiophilic crown ether sites is applied as an interfacial layer to protect lithium metal anode. The Li||Li symmetrical cells with NKU-2000-based interfacial layer exhibit an ultra-long cycle of 8500 hours at 1 mA cm-2, and can stably cycle for 1700 hours under severe state of 10 mA cm-2 and 10 mAh cm-2. The corresponding LiFePO4 full cell achieves a long lifespan of 2000 cycles at 1 C with a capacity retention rate of 81.8%. A molecular-level mechanism study reveals that the lithiophilic crown ether sites reduce the Li+ desolvation energy barrier, and the crown ether-based channels promote Li+ transfer kinetics. This work provides a facile coordination assembly approach of arranging uniformly distributed lithiophilic sites in efficient Li+ transfer channels of an interfacial layer for achieving dendrite-free lithium deposition in high-performance LMBs.

文章链接：https://www.chinesechemsoc.org/doi/10.31635/ccschem.024.202405325