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 Zn²⁺ 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 Zn²⁺. 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.