Tailored N‐Doped Micro‐Mesoporous Carbon‐Based Artificial Protective Layer With Uniform Electric Field and Desolvation for Dendrite‐Free Zn Anodes

Zinc dendrite growth and interfacial side reactions severely restrict the practical application of aqueous zinc‐ion batteries (AZIBs). Therefore, we propose a tailored structural construction strategy for artificial protective layer of Zn anode. A tailored N‐doped micro‐mesoporous carbon material (ZMC2) artificial protective layer with 81.4% micropores and 18.6% mesopores is successfully prepared through uniform in situ growth of ZIF‐8 nanoparticles on medulla tetrapanacis (MT) skeleton followed by high‐temperature pyrolysis. Combining molecular dynamics (MD), density functional theory (DFT) calculations, and experimental verification, this work clarifies the synergistic mechanism of micro‐mesoporous structures, conductive carbon substrate, and N‐doped active sites in ZMC2. The optimized micro‐mesoporous structure of ZMC2 accelerates hydrated Zn 2+ desolvation and homogenizes the interfacial electric field and regulates ion flux through the conductive carbon substrate and porous network. Meanwhile, the N‐doped sites of ZMC2 induce uniform adsorption and stable deposition of Zn 2+ . Benefiting from above synergistic effect, the ZMC2 artificial protective layer effectively inhibits zinc dendrite growth and alleviates interfacial side reactions. Furthermore, the symmetric, half and full cells assembled with ZMC2@Zn electrode all exhibit outstanding cycling stability and electrochemical reversibility, fully verifying that the strategy of constructing a tailored N‐doped micro‐mesoporous structure based on biomass‐derived carbon has promising feasibility for high‐performance AZIBs.