Lithiophilic anchor points enabling endogenous symbiotic Li3N interface for homogeneous and stable lithium electrodeposition

The safety hazards and short lifecycles caused by uncontrollable dendrite growth and infinite volume expansion hamper the widespread deployment of Li metal anodes. To address these issues, it is critical to regulate the nucleation and electrodeposition behaviors of Li. Herein, tetraaminophthalocyanine (TAPC) as lithiophilic anchor points modified on three-dimensional (3D) carbon skeleton (denoted as [email protected]) as both current collector and host material, is rationally designed for stabilizing Li metal anodes. Li3N spontaneously generated from the reaction between TAPC and Li enables upgraded electrochemical kinetics. Moreover, density functional theory (DFT) results reveal that the evenly distributed TAPC nanoparticles can effectively guide the homogeneous smooth deposition of metallic Li via strong affinity between Li and conjugation groups. Symmetrical cells containing [email protected] anodes afford a stable cycling for 3500 h at 10 mA cm−2. Further, coupled with a high-loading LiFePO4 cathode (15.0 mg cm−2), the stability and feasibility of the modified electrode in practical cells are proved.