Uniform Li‐deposition induced by Ni‐catalyzing graphitization of natural carbon materials in lithium metal batteries

Abstract Lithium metal batteries are known as the most prospecting recyclable accumulation system owing to the high specific capacity of 3860 mAh g⁻¹. Nevertheless, Li‐dendrites formed by the charge‐discharge process would lead to poor performances and severe safety problems. In this work, we proposed a new silk‐film with a composite network that was full of the Ni‐containing functionalized nanoparticles to induce the uniform Li‐deposition and prevent the wanton growth of lithium dendrite. As a result, the as‐designed flexible fiber materials (Ni‐silks) were successfully prepared by utilizing degradable silks as the substrates and Ni‐particles as the catalyzer for graphitization of carbon materials. The Ni‐silk‐Li (NSL) as anodes were constructed by Ni‐silk and Li metals, which exhibited the long‐term cycle of 800 h and high coulombic efficiency of 98.35% for the half cells. In addition, the NSL anodes also showed outstanding electrochemical performances in full cells using LiFePO₄ as the cathode with an outstanding specific capacity of 155 mAh g⁻¹. To further explore the working mechanism of the NSL electrode, Density functional theory (DFT) computations were analyzed. Our findings provide a new idea for evoking uniform Li‐nucleation by introducing graphitization of flexible Ni‐silks, which is not to be ignored for reducing Li‐dendrite formation.