Achieving Uniform Li Plating/Stripping at Ultrahigh Currents and Capacities by Optimizing 3D Nucleation Sites and Li₂Se‐Enriched SEI

Abstract

Lithium (Li) has garnered considerable attention as an alternative anodes of next-generation high-performance batteries owing to its prominent theoretical specific capacity. However, the commercialization of Li metal anodes (LMAs) is significantly compromised by non-uniform Li deposition and inferior electrolyte-anode interfaces, particularly at high currents and capacities. Herein, a hierarchical three-dimentional structure with CoSe₂ -nanoparticle-anchored nitrogen-doped carbon nanoflake arrays is developed on a carbon fiber cloth (CoSe₂ -NC@CFC) to regulate the Li nucleation/plating process and stabilize the electrolyte-anode interface. Owing to the enhanced lithiophilicity endowed by CoSe₂ -NC, in situ-formed Li₂ Se and Co nanoparticles during initial Li nucleation, and large void space, CoSe₂ -NC@CFC can induce homogeneous Li nucleation/plating, optimize the solid electrolyte interface, and mitigate volume change. Consequently, the CoSe₂ -NC@CFC can accommodate Li with a high areal capacity of up to 40 mAh cm^-2 . Moreover, the Li/CoSe₂ -NC@CFC anodes possess outstanding cycling stability and lifespan in symmetric cells, particularly under ultrahigh currents and capacities (1600 h at 10 mA cm^-2 /10 mAh cm^-2 and 5 mA cm^-2 /20 mAh cm^-2 ). The Li/CoSe₂ -NC@CFC//LiFePO₄ full cell delivers impressive long-term performance and favorable flexibility. The developed CoSe₂ -NC@CFC provides insights into the development of advanced Li hosts for flexible and stable LMAs.