Formation of Hierarchical Zn/N‐doped Carbon Hollow Nanofibers towards Dendrite‐Free Zn Metal Anodes

Abstract Rechargeable aqueous Zn metal batteries are considered as promising next‐generation energy storage device because of their intrinsic safety and low cost. Nonetheless, the poor lifespan stemming from uncontrollable dendrite growth and inevitable parasitic reactions of metallic Zn impede their large‐scale application. Herein, the formation of the hierarchical lotus root‐like Zn/N‐doped carbon hollow nanofibers‐based paper is reported decorated with interconnected Zn/N‐doped carbon nanocages (denoted as LRZCF@ZCC) as a freestanding host with multifunctionality for Zn metal anode. Of note, the interconnected porous structure mitigates the internal stress to ensure robust structure. Besides, the concave surface of inner LRZCF@ZCC channel facilitates the nucleation of Zn²⁺ to geometrically guide the Zn deposition. Meanwhile, the well‐distributed metallic Zn and N‐doped carbon species can serve as the zincophilic sites to reduce the nucleation overpotential and avoid the evolution of hydrogen bubbles. As expected, the LRZCF@ZCC exhibits low polarization for the controllable Zn deposition with small voltage hysteresis. Both the symmetric cell and the full cell using this unique host demonstrate long‐term cycling duration and enhanced rate capability.