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Lithium metal anodes (LMAs) possess the largest energy density among all anode candidates, while dendrite growth is a huge barrier in the direct application of LMAs in batteries. Herein, an ultrathin graphitic C3N4–poly(1,3-dioxolane) (CN–PDOL) composite interlayer was in situ synthesized by cationic ring-opening polymerization upon lithium metal anodes. Flexible PDOL could isolate electrolytes, remitting the corrosion reactions and consumption of electrolytes, while g-C3N4 nanoflakes could reduce the crystallinity of PDOL, increase ion-conductivity and uniform Li-ion fluxes. At a current density of 3 mA cm−2, the synergistic effect of CN and PDOL could enable 850 h stable Li plating/stripping behavior at an overpotential of 70 mV. In this work, a facile and accessible design of a composite buffer layer was developed for lithium metal anodes, which might be of interest to a broad community investigating surface modifications.

Lithium metal anode (LMA) possesses the largest energy density among all anode candidates, while dendrite growth is a huge barrier in the direct application of LMA in batteries. Herein, metal-organic framework (MOF) derived Zn-CxNy nanoparticle arrays are newly grown onto carbon cloth as an effective host toward lithium metal anode. The N and Zn species are lithiophilic to Li-ions, resulting in a stable Li plating/stripping process of up to 2200 hrs without running into a dendrite issue when operating at a current density of 10 mA cm-2. The newly developed ZNCC-Li anode also exhibits an ultralow voltage hysteresis of only 6.4 mV at the end of the operating process. This work creates an effective design of MOF derived lithium metal anode suitable for high-energy batteries.