General construction of lithiophilic 3D skeleton for dendrite-free lithium metal anode via a versatile MOF-derived route

The pursuit of high-mileage models results in the recurrence of lithium metal batteries (LMBs) to researchers’ horizon. However, the lithium (Li) metal anode for LMBs undergoes the uncontrollable formation of Li dendrites and infinite volume change during cycling, impeding its practical application. To overcome these challenges, we developed a metal-organic framework (MOF)-derived pathway to construct lithiophilic three-dimensional (3D) skeleton using different substrates (e.g., carbon cloth (CC) and Cu mesh) for dendrite-free lithium metal anodes. As a typical example, the MOF-derived ZnO/nitrogen-doped carbon (NC) nanosheet-modified 3D CC was well-constructed as a lithiophilic hierarchical host (CC@ZnO/NC@Li) for molten Li infiltration. Benefiting from the lithiophilic N-functional groups and LiZn alloy, the synthesized CC@ZnO/NC@Li composite anode promoted the uniform distribution of Li, resulting in a dendrite-free morphology. Meanwhile, the 3D conductive carbon skeleton enhanced the reaction kinetics and buffered the volume change of the electrode. The CC@ZnO/NC@Li composite anode presented a prolonged lifespan of over 1000 cycles at 5 mA cm−2 with a low overpotential of 19 mV. Coupled with a LiFePO4 cathode, the CC@ZnO/NC@Li composite anode also exhibited superior electrochemical properties in the full-cell system. This versatile strategy may open up the channel of designing multi-functional lithiophilic 3D hosts for the Li metal anode.