Hydrogen-Bonded Organic Framework as Superior Separator with High Lithium Affinity C═N Bond for Low N/P Ratio Lithium Metal Batteries

Lithium dendrite and side reactions are two major challenges for lithium metal anode. Here, the highly lithophilic triazine ring in the hydrogen-bonded organic framework is recommended to accelerate the desolvation process of lithium ions. Among them, the formation of Li–N bonds between lithium ions and the triazine ring in CAM reduces the diffusion energy barrier of Li+ crossing the SEI interface and the desolvation energy barrier of Li+ exiting from the solvent sheath so that the rapid and homogeneous deposition of lithium-ion can be achieved. Meanwhile, the lithium-ion migration coefficient can be as high as 0.70. CAM separator is used to assemble lithium metal batteries with nickel-rich cathodes (NCM 622). When N/P = 8 and 5, the capacity retention rates of Li-NCM 622 full cell are 78.2% and 80.5% after 200 and 110 cycles, respectively, and the Coulomb efficiency can be maintained at 99.5%, showing excellent cycle stability.