Directional Regulation of Zinc Deposition Through Constructing Hierarchical Janus Carbon Matrix with Organic‐Decorated Multi‐Channels

The development of rechargeable aqueous zinc-ion battery (AZIB) has been hampered by parasitic reactions, despite the low cost, high safety, and environmental friendliness. Here, we design an artificial interfacial layer using a hierarchical Janus carbon matrix on Zn anodes to direct Zn deposition behavior. By covalently anchoring zincophilic organic sulfonic groups within the inner pores of the hierarchical multi-channel structure of CMK-5 (CMK-5/PS), we establish a charge gradient between the grafted inner and unmodified outer surfaces that promotes Zn2+ diffusion and deposition. The negatively charged inner surface facilitates fast Zn2+ adsorption and uniform nucleation, while the interconnected porous structure facilitates fast Zn2+ transport. The confinement effect localizes Zn deposition exclusively within the tubular pores and reduces direct contact with electrolytes, thereby suppressing parasitic reactions and improving the plating/stripping efficiency. As a result, CMK-5/PS@Zn anode achieves a high Coulombic efficiency of 99.2% and stability over 8000 h. When paired with an NH4V4O10 cathode, the CMK-5/PS@Zn delivers a high reversible capacity of 213.8 mAh g-1 after 1000 cycles at 1 A g-1. This work provides a new paradigm for interfacial engineering of Zn metal anodes through carbon-organic composite architectures, advancing the design of durable and high-performance AZIB technologies.