Single Iron Atom Anchored on ZIF‐8 Derived Carbon Framework to Directionally Regulate Lithium Deposition with Minimum Nucleation Overpotential

Abstract Lithium (Li) metal has earned valuable status among the most auspicious anodes for the assembly of next‐generation rechargeable batteries. However, the dendritic growth and infinite change in volume of metallic Li anode strongly hinder its use for practical applications. Here, the preparation of atomically dispersed iron doped ZIF‐8 through pyrolysis (Fe@NC) to lower the Li nucleation overpotential and control the Li deposition on specific positions is reported. Thermodynamic and kinetic simulations show that the doped single Fe atoms can improve the atomic structure, increase the adsorption energy and enhance the diffusion capacity of Li. Moreover, the specific framework structure of Fe@NC can induce Li metal to nucleate in interior space of the material which can hinder the Li growth along one direction and restrain its volume expansion. As‐fabricated electrode displays nearly no nucleation overpotential at current density of 2 mA cm –2 and offers higher average Coulombic efficiency up to 99.0% for 100 cycles at current density 2 mA cm –2 , and higher areal capacity up to 5 mAh cm –2 . Also, the fabricated Fe@NC/LiFePO 4 based full cells exhibit a longer lifespan of 100 cycles at 0.5 C. The results provide new insights for future rechargeable Li metal batteries.