Nanoporous Triazine-Framework-Assembled Electrolyte Interphase Layer as a Lithiophilic Gridding for Uniform Lithium Deposition and Dendrite Inhibition

Lithium metal is widely utilized due to its high theoretical capacity and low electrochemical potential. However, the growth of uncontrollable lithium dendrites and increased voltage polarization during lithium stripping and plating can severely impact cycling stability. In this study, we propose a nitrogen-rich triazinyl nanoporous organic polymer (DCP-CTF) as an artificial solid–electrolyte interphase (SEI) for a lithium-metal anode. The spatial distribution of the porous layered array structure enables the gradient migration of Li+. Meanwhile, the rigid nanochannels can also restrict the excessive growth of Li depositions through the steric confinement effect and reduce the generation of lithium dendrites. By combining density functional theory calculations with Fourier transform infrared spectroscopy, we demonstrate the functional lithiophilic coordination of DCP-CTF. The electron-rich triazine ring acts as a donor to attract Li+, and the pyridine nitrogen group serves as an effective lithium anchoring site. The abundant distribution of these lithiophilic sites can regulate Li+ transfer, thereby ensuring smooth lithium deposition and inhibiting dendrite formation. As a result, the DCP-CTF-modified lithium-metal anode exhibits exceptional electrochemical stability of more than 2500 h of cycling in an ether-based electrolyte at a high current density of 20 mA cm–2.